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Quantum dot

March 28, 2023

Quantum dots (QDs) - also called semiconductor nanocrystals, are semiconductor particles a few nanometres in size, having optical and electronic properties that differ from those of larger particles as a result of quantum mechanics. They are a central topic in nanotechnology and materials science. When the quantum dots are illuminated by UV light, an electron in the quantum dot can be excited to a state of higher energy. In the case of a semiconducting quantum dot, this process corresponds to the transition of an electron from the valence band to the conductance band. The excited electron can drop back into the valence band releasing its energy as light. This light emission (photoluminescence) is illustrated in the figure on the right. The color of that light depends on the energy difference between the conductance band and the valence band, or the transition between discrete energy states when the band structure is no longer well-defined in QDs.

Colloidal quantum dots irradiated with a UV light. Different sized quantum dots emit different colors of light due to quantum confinement.

Nanoscale semiconductor materials tightly confine either electrons or electron holes. The confinement is similar to a three-dimensional particle in a box model. The quantum dot absorption and emission features correspond to transitions between discrete quantum mechanically allowed energy levels in the box that are reminiscent of atomic spectra. For these reasons, quantum dots are sometimes referred to as artificial atoms,[1] emphasizing their bound and discrete electronic states, like naturally occurring atoms or molecules.[2][3] It was shown that the electronic wave functions in quantum dots resemble the ones in real atoms.[4] By coupling two or more such quantum dots, an artificial molecule can be made, exhibiting hybridization even at room temperature.[5]

Quantum dots have properties intermediate between bulk semiconductors and discrete atoms or molecules. Their optoelectronic properties change as a function of both size and shape.[6][7] Larger QDs of 5–6 nm diameter emit longer wavelengths, with colors such as orange, or red. Smaller QDs (2–3 nm) emit shorter wavelengths, yielding colors like blue and green. However, the specific colors vary depending on the exact composition of the QD.[8]

Potential applications of quantum dots include single-electron transistors, solar cells, LEDs, lasers,[9] single-photon sources,[10][11][12] second-harmonic generation, quantum computing,[13] cell biology research,[14] microscopy,[15] and medical imaging.[16] Their small size allows for some QDs to be suspended in solution, which may lead to their use in inkjet printing, and spin coating.[17] They have been used in Langmuir-Blodgett thin films.[18][19][20] These processing techniques result in less expensive and less time-consuming methods of semiconductor fabrication.

Production

 
Quantum Dots with gradually stepping emission from violet to deep red

There are several ways to fabricate quantum dots. Possible methods include colloidal synthesis, self-assembly, and electrical gating.

Colloidal synthesis

Colloidal semiconductor nanocrystals are synthesized from solutions, much like traditional chemical processes. The main difference is the product neither precipitates as a bulk solid nor remains dissolved.[6] Heating the solution at high temperature, the precursors decompose forming monomers which then nucleate and generate nanocrystals. Temperature is a critical factor in determining optimal conditions for the nanocrystal growth. It must be high enough to allow for rearrangement and annealing of atoms during the synthesis process while being low enough to promote crystal growth. The concentration of monomers is another critical factor that has to be stringently controlled during nanocrystal growth. The growth process of nanocrystals can occur in two different regimes: "focusing" and "defocusing". At high monomer concentrations, the critical size (the size where nanocrystals neither grow nor shrink) is relatively small, resulting in growth of nearly all particles. In this regime, smaller particles grow faster than large ones (since larger crystals need more atoms to grow than small crystals) resulting in the size distribution focusing, yielding an improbable distribution of nearly monodispersed particles. The size focusing is optimal when the monomer concentration is kept such that the average nanocrystal size present is always slightly larger than the critical size. Over time, the monomer concentration diminishes, the critical size becomes larger than the average size present, and the distribution defocuses.

 
Cadmium sulfide quantum dots on cells

There are colloidal methods to produce many different semiconductors. Typical dots are made of binary compounds such as lead sulfide, lead selenide, cadmium selenide, cadmium sulfide, cadmium telluride, indium arsenide, and indium phosphide. Dots may also be made from ternary compounds such as cadmium selenide sulfide. Further, recent advances have been made which allow for synthesis of colloidal perovskite quantum dots.[21] These quantum dots can contain as few as 100 to 100,000 atoms within the quantum dot volume, with a diameter of ≈10 to 50 atoms. This corresponds to about 2 to 10 nanometers, and at 10 nm in diameter, nearly 3 million quantum dots could be lined up end to end and fit within the width of a human thumb.

 
Idealized image of colloidal nanoparticle of lead sulfide (selenide) with complete passivation by oleic acid, oleyl amine, and hydroxyl ligands (size ≈5nm)

Large batches of quantum dots may be synthesized via colloidal synthesis. Due to this scalability and the convenience of benchtop conditions, colloidal synthetic methods are promising for commercial applications.

Plasma synthesis

Plasma synthesis has evolved to be one of the most popular gas-phase approaches for the production of quantum dots, especially those with covalent bonds.[22][23][24] For example, silicon (Si) and germanium (Ge) quantum dots have been synthesized by using nonthermal plasma. The size, shape, surface and composition of quantum dots can all be controlled in nonthermal plasma.[25][26] Doping that seems quite challenging for quantum dots has also been realized in plasma synthesis.[27][28][29] Quantum dots synthesized by plasma are usually in the form of powder, for which surface modification may be carried out. This can lead to excellent dispersion of quantum dots in either organic solvents[30] or water[31] (i. e., colloidal quantum dots).

Fabrication

The electrostatic potential needed to create a quantum dot can be realized with several methods. These include external electrodes,[32] doping, strain,[33] or impurities. Self-assembled quantum dots are typically between 5 and 50 nm in size. Quantum dots defined by lithographically patterned gate electrodes, or by etching on two-dimensional electron gases in semiconductor heterostructures can have lateral dimensions between 20 and 100 nm.

  • Some quantum dots are small regions of one material buried in another with a larger band gap. These can be so-called core–shell structures, e.g., with CdSe in the core and ZnS in the shell, or from special forms of silica called ormosil. Sub-monolayer shells can also be effective ways of passivating the quantum dots, such as PbS cores with sub-monolayer CdS shells.[34]
  • Quantum dots sometimes occur spontaneously in quantum well structures due to monolayer fluctuations in the well's thickness.
 
Atomic resolution scanning transmission electron microscopy image of an indium gallium arsenide (InGaAs) quantum dot buried in gallium arsenide (GaAs)
  • Self-assembled quantum dots nucleate spontaneously under certain conditions during molecular beam epitaxy (MBE) and metalorganic vapour-phase epitaxy (MOVPE), when a material is grown on a substrate to which it is not lattice matched. The resulting strain leads to the formation of islands on top of a two-dimensional wetting layer. This growth mode is known as Stranski–Krastanov growth.[35] The islands can be subsequently buried to form the quantum dot. A widely used type of quantum dots grown with this method are indium gallium arsenide (InGaAs) quantum dots in gallium arsenide (GaAs).[36] Such quantum dots have the potential for applications in quantum cryptography (i.e. single-photon sources) and quantum computation. The main limitations of this method are the cost of fabrication and the lack of control over positioning of individual dots.
  • Individual quantum dots can be created from two-dimensional electron or hole gases present in remotely doped quantum wells or semiconductor heterostructures called lateral quantum dots. The sample surface is coated with a thin layer of resist and a lateral pattern is then defined in the resist by electron beam lithography. This pattern can then be transferred to the electron or hole gas by etching, or by depositing metal electrodes (lift-off process) that allow the application of external voltages between the electron gas and the electrodes. Such quantum dots are mainly of interest for experiments and applications involving electron or hole transport and they are also used as spin qubits.[37] A strength of this type of quantum dots is that their energy spectrum can be engineered by controlling the geometrical size, shape, and the strength of the confinement potential with gate electrodes. These quantum dots can be easily connected by tunnel barriers to conducting leads, which allows the application of the techniques of tunneling spectroscopy for their investigation.
  • Complementary metal–oxide–semiconductor (CMOS) technology can be employed to fabricate silicon quantum dots. Ultra small (L=20 nm, W=20 nm) CMOS transistors behave as single electron quantum dots when operated at cryogenic temperature over a range of −269 °C (4 K) to about −258 °C (15 K). The transistor displays Coulomb blockade due to progressive charging of electrons (holes) one by one. The number of electrons (holes) confined in the channel is driven by the gate voltage, starting from an occupation of zero electrons (holes), and it can be set to 1 or many.[38]

Viral assembly

Genetically engineered M13 bacteriophage viruses allow preparation of quantum dot biocomposite structures.[39] It had previously been shown that genetically engineered viruses can recognize specific semiconductor surfaces through the method of selection by combinatorial phage display.[40] Additionally, it is known that liquid crystalline structures of wild-type viruses (Fd, M13, and TMV) are adjustable by controlling the solution concentrations, solution ionic strength, and the external magnetic field applied to the solutions. Consequently, the specific recognition properties of the virus can be used to organize inorganic nanocrystals, forming ordered arrays over the length scale defined by liquid crystal formation. Using this information, Lee et al. (2000) were able to create self-assembled, highly oriented, self-supporting films from a phage and ZnS precursor solution. This system allowed them to vary both the length of bacteriophage and the type of inorganic material through genetic modification and selection.

Electrochemical assembly

Highly ordered arrays of quantum dots may also be self-assembled by electrochemical techniques. A template is created by causing an ionic reaction at an electrolyte-metal interface which results in the spontaneous assembly of nanostructures, including quantum dots, onto the metal which is then used as a mask for mesa-etching these nanostructures on a chosen substrate.[citation needed]

Bulk-manufacture

Quantum dot manufacturing relies on a process called high temperature dual injection which has been scaled by multiple companies for commercial applications that require large quantities (hundreds of kilograms to tons) of quantum dots. This reproducible production method can be applied to a wide range of quantum dot sizes and compositions.

The bonding in certain cadmium-free quantum dots, such as III-V-based quantum dots, is more covalent than that in II-VI materials, therefore it is more difficult to separate nanoparticle nucleation and growth via a high temperature dual injection synthesis. An alternative method of quantum dot synthesis, the molecular seeding process, provides a reproducible route to the production of high-quality quantum dots in large volumes. The process utilises identical molecules of a molecular cluster compound as the nucleation sites for nanoparticle growth, thus avoiding the need for a high temperature injection step. Particle growth is maintained by the periodic addition of precursors at moderate temperatures until the desired particle size is reached.[41] The molecular seeding process is not limited to the production of cadmium-free quantum dots; for example, the process can be used to synthesise kilogram batches of high-quality II-VI quantum dots in just a few hours.

Another approach for the mass production of colloidal quantum dots can be seen in the transfer of the well-known hot-injection methodology for the synthesis to a technical continuous flow system. The batch-to-batch variations arising from the needs during the mentioned methodology can be overcome by utilizing technical components for mixing and growth as well as transport and temperature adjustments. For the production of CdSe based semiconductor nanoparticles this method has been investigated and tuned to production amounts of kg per month. Since the use of technical components allows for easy interchange in regards of maximum throughput and size, it can be further enhanced to tens or even hundreds of kilograms.[42]

In 2011 a consortium of U.S. and Dutch companies reported a milestone in high volume quantum dot manufacturing by applying the traditional high temperature dual injection method to a flow system.[43]

On 23 January 2013 Dow entered into an exclusive licensing agreement with UK-based Nanoco for the use of their low-temperature molecular seeding method for bulk manufacture of cadmium-free quantum dots for electronic displays, and on 24 September 2014 Dow commenced work on the production facility in South Korea capable of producing sufficient quantum dots for "millions of cadmium-free televisions and other devices, such as tablets". Mass production is due to commence in mid-2015.[44] On 24 March 2015 Dow announced a partnership deal with LG Electronics to develop the use of cadmium free quantum dots in displays.[45]

Heavy-metal-free quantum dots

In many[which?] regions of the world there is now a restriction or ban on the use of toxic heavy metals in many household goods, which means that most cadmium-based quantum dots are unusable for consumer-goods applications.

For commercial viability, a range of restricted, heavy-metal-free quantum dots has been developed showing bright emissions in the visible and near-infrared region of the spectrum and have similar optical properties to those of CdSe quantum dots. Among these materials are InP/ZnS, CuInS/ZnS, Si, Ge, and C.

Peptides are being researched as potential quantum dot material.[46]

Health and safety

Main articles: Health and safety hazards of nanomaterials and Nanotoxicology

Some quantum dots pose risks to human health and the environment under certain conditions.[47][48][49] Notably, the studies on quantum dot toxicity have focused on particles containing cadmium and have yet to be demonstrated in animal models after physiologically relevant dosing.[49] In vitro studies, based on cell cultures, on quantum dots (QD) toxicity suggest that their toxicity may derive from multiple factors including their physicochemical characteristics (size, shape, composition, surface functional groups, and surface charges) and their environment. Assessing their potential toxicity is complex as these factors include properties such as QD size, charge, concentration, chemical composition, capping ligands, and also on their oxidative, mechanical, and photolytic stability.[47]

Many studies have focused on the mechanism of QD cytotoxicity using model cell cultures. It has been demonstrated that after exposure to ultraviolet radiation or oxidation by air, CdSe QDs release free cadmium ions causing cell death.[50] Group II–VI QDs also have been reported to induce the formation of reactive oxygen species after exposure to light, which in turn can damage cellular components such as proteins, lipids, and DNA.[51] Some studies have also demonstrated that addition of a ZnS shell inhibits the process of reactive oxygen species in CdSe QDs. Another aspect of QD toxicity is that there are, in vivo, size-dependent intracellular pathways that concentrate these particles in cellular organelles that are inaccessible by metal ions, which may result in unique patterns of cytotoxicity compared to their constituent metal ions.[52] The reports of QD localization in the cell nucleus[53] present additional modes of toxicity because they may induce DNA mutation, which in turn will propagate through future generation of cells, causing diseases.

Although concentration of QDs in certain organelles have been reported in in vivo studies using animal models, no alterations in animal behavior, weight, hematological markers, or organ damage has been found through either histological or biochemical analysis.[54] These findings have led scientists to believe that intracellular dose is the most important determining factor for QD toxicity. Therefore, factors determining the QD endocytosis that determine the effective intracellular concentration, such as QD size, shape, and surface chemistry determine their toxicity. Excretion of QDs through urine in animal models also have demonstrated via injecting radio-labeled ZnS-capped CdSe QDs where the ligand shell was labeled with 99mTc.[55] Though multiple other studies have concluded retention of QDs in cellular levels,[49][56] exocytosis of QDs is still poorly studied in the literature.

While significant research efforts have broadened the understanding of toxicity of QDs, there are large discrepancies in the literature, and questions still remain to be answered. Diversity of this class of material as compared to normal chemical substances makes the assessment of their toxicity very challenging. As their toxicity may also be dynamic depending on the environmental factors such as pH level, light exposure, and cell type, traditional methods of assessing toxicity of chemicals such as LD50 are not applicable for QDs. Therefore, researchers are focusing on introducing novel approaches and adapting existing methods to include this unique class of materials.[49] Furthermore, novel strategies to engineer safer QDs are still under exploration by the scientific community. A recent novelty in the field is the discovery of carbon quantum dots, a new generation of optically-active nanoparticles potentially capable of replacing semiconductor QDs, but with the advantage of much lower toxicity.

Optical properties

 
Fluorescence spectra of CdTe quantum dots of various sizes. Different sized quantum dots emit different color light due to quantum confinement.

In semiconductors, light absorption generally leads to an electron being excited from the valence to the conduction band, leaving behind a hole. The electron and the hole can bind to each other to form an exciton. When this exciton recombines (i.e. the electron resumes its ground state), the exciton's energy can be emitted as light. This is called fluorescence. In a simplified model, the energy of the emitted photon can be understood as the sum of the band gap energy between the highest occupied level and the lowest unoccupied energy level, the confinement energies of the hole and the excited electron, and the bound energy of the exciton (the electron–hole pair):

 

As the confinement energy depends on the quantum dot's size, both absorption onset and fluorescence emission can be tuned by changing the size of the quantum dot during its synthesis. The larger the dot, the redder (lower-energy) its absorption onset and fluorescence spectrum. Conversely, smaller dots absorb and emit bluer (higher-energy) light. Recent articles suggest that the shape of the quantum dot may be a factor in the coloration as well, but as yet not enough information is available[citation needed]. Furthermore, it was shown[57] that the lifetime of fluorescence is determined by the size of the quantum dot. Larger dots have more closely spaced energy levels in which the electron–hole pair can be trapped. Therefore, electron–hole pairs in larger dots live longer causing larger dots to show a longer lifetime.

To improve fluorescence quantum yield, quantum dots can be made with shells of a larger bandgap semiconductor material around them. The improvement is suggested to be due to the reduced access of electron and hole to non-radiative surface recombination pathways in some cases, but also due to reduced Auger recombination in others.

Applications

Quantum dots are particularly promising for optical applications due to their high extinction coefficient[58] and ultrafast optical nonlinearities with potential applications for developing all-optical systems.[59] They operate like a single-electron transistor and show the Coulomb blockade effect. Quantum dots have also been suggested as implementations of qubits for quantum information processing,[60] and as active elements for thermoelectrics.[61][62][63]

Tuning the size of quantum dots is attractive for many potential applications. For instance, larger quantum dots have a greater spectrum-shift toward red compared to smaller dots and exhibit less pronounced quantum properties. Conversely, the smaller particles allow one to take advantage of more subtle quantum effects.

 
A device that produces visible light, through energy transfer from thin layers of quantum wells to crystals above the layers.[64]

Being zero-dimensional, quantum dots have a sharper density of states than higher-dimensional structures. As a result, they have superior transport and optical properties. They have potential uses in diode lasers, amplifiers, and biological sensors.[65] Quantum dots may be excited within a locally enhanced electromagnetic field produced by gold nanoparticles, which then can be observed from the surface plasmon resonance in the photoluminescent excitation spectrum of (CdSe)ZnS nanocrystals. High-quality quantum dots are well suited for optical encoding and multiplexing applications due to their broad excitation profiles and narrow/symmetric emission spectra. The new generations of quantum dots have far-reaching potential for the study of intracellular processes at the single-molecule level, high-resolution cellular imaging, long-term in vivo observation of cell trafficking, tumor targeting, and diagnostics.

CdSe nanocrystals are efficient triplet photosensitizers.[66] Laser excitation of small CdSe nanoparticles enables the extraction of the excited state energy from the quantum dots into bulk solution, thus opening the door to a wide range of potential applications such as photodynamic therapy, photovoltaic devices, molecular electronics, and catalysis.

Subcutaneous record-keeping

In December 2019, Robert S. Langer and his team developed and patented a technique whereby transdermal patches could be used to apply an identification tattoo to people with invisible ink to store information subcutaneously. This was presented as a boon to "developing nations" where lack of infrastructure means an absence of medical records.[67][68] The technology, which is assigned to the Massachusetts Institute of Technology,[68] uses a "quantum dot dye that is delivered, in this case along with a vaccine, by a microneedle patch." The research "was funded by the Bill and Melinda Gates Foundation and the Koch Institute for Integrative Cancer Research."[67]

Biology

In modern biological analysis, various kinds of organic dyes are used. However, as technology advances, greater flexibility in these dyes is sought.[69] To this end, quantum dots have quickly filled in the role, being found to be superior to traditional organic dyes on several counts, one of the most immediately obvious being brightness (owing to the high extinction coefficient combined with a comparable quantum yield to fluorescent dyes[14]) as well as their stability (allowing much less photobleaching).[70] It has been estimated that quantum dots are 20 times brighter and 100 times more stable than traditional fluorescent reporters.[69] For single-particle tracking, the irregular blinking of quantum dots is a minor drawback. However, there have been groups which have developed quantum dots which are essentially nonblinking and demonstrated their utility in single-molecule tracking experiments.[71][72]

The use of quantum dots for highly sensitive cellular imaging has seen major advances.[73] The improved photostability of quantum dots, for example, allows the acquisition of many consecutive focal-plane images that can be reconstructed into a high-resolution three-dimensional image.[74] Another application that takes advantage of the extraordinary photostability of quantum dot probes is the real-time tracking of molecules and cells over extended periods of time.[75] Antibodies, streptavidin,[76] peptides,[77] DNA,[78] nucleic acid aptamers,[79] or small-molecule ligands[80] can be used to target quantum dots to specific proteins on cells. Researchers were able to observe quantum dots in lymph nodes of mice for more than 4 months.[81]

Quantum dots can have antibacterial properties similar to nanoparticles and can kill bacteria in a dose-dependent manner.[82] One mechanism by which quantum dots can kill bacteria is through impairing the functions of antioxidative system in the cells and down regulating the antioxidative genes. In addition, quantum dots can directly damage the cell wall. Quantum dots have been shown to be effective against both gram- positive and gram-negative bacteria.[83]

Semiconductor quantum dots have also been employed for in vitro imaging of pre-labeled cells. The ability to image single-cell migration in real time is expected to be important to several research areas such as embryogenesis, cancer metastasis, stem cell therapeutics, and lymphocyte immunology.

One application of quantum dots in biology is as donor fluorophores in Förster resonance energy transfer, where the large extinction coefficient and spectral purity of these fluorophores make them superior to molecular fluorophores[84] It is also worth noting that the broad absorbance of QDs allows selective excitation of the QD donor and a minimum excitation of a dye acceptor in FRET-based studies.[85] The applicability of the FRET model, which assumes that the Quantum Dot can be approximated as a point dipole, has recently been demonstrated[86]

The use of quantum dots for tumor targeting under in vivo conditions employ two targeting schemes: active targeting and passive targeting. In the case of active targeting, quantum dots are functionalized with tumor-specific binding sites to selectively bind to tumor cells. Passive targeting uses the enhanced permeation and retention of tumor cells for the delivery of quantum dot probes. Fast-growing tumor cells typically have more permeable membranes than healthy cells, allowing the leakage of small nanoparticles into the cell body. Moreover, tumor cells lack an effective lymphatic drainage system, which leads to subsequent nanoparticle-accumulation.

Quantum dot probes exhibit in vivo toxicity. For example, CdSe nanocrystals are highly toxic to cultured cells under UV illumination, because the particles dissolve, in a process known as photolysis, to release toxic cadmium ions into the culture medium. In the absence of UV irradiation, however, quantum dots with a stable polymer coating have been found to be essentially nontoxic.[81][48] Hydrogel encapsulation of quantum dots allows for quantum dots to be introduced into a stable aqueous solution, reducing the possibility of cadmium leakage. Then again, only little is known about the excretion process of quantum dots from living organisms.[87]

In another potential application, quantum dots are being investigated as the inorganic fluorophore for intra-operative detection of tumors using fluorescence spectroscopy.

Delivery of undamaged quantum dots to the cell cytoplasm has been a challenge with existing techniques. Vector-based methods have resulted in aggregation and endosomal sequestration of quantum dots while electroporation can damage the semi-conducting particles and aggregate delivered dots in the cytosol. Via cell squeezing, quantum dots can be efficiently delivered without inducing aggregation, trapping material in endosomes, or significant loss of cell viability. Moreover, it has shown that individual quantum dots delivered by this approach are detectable in the cell cytosol, thus illustrating the potential of this technique for single-molecule tracking studies.[88]

Photovoltaic devices

Main article: Quantum dot solar cell

The tunable absorption spectrum and high extinction coefficients of quantum dots make them attractive for light harvesting technologies such as photovoltaics. Quantum dots may be able to increase the efficiency and reduce the cost of today's typical silicon photovoltaic cells. According to an experimental report from 2004,[89] quantum dots of lead selenide (PbSe) can produce more than one exciton from one high-energy photon via the process of carrier multiplication or multiple exciton generation (MEG). This compares favorably to today's photovoltaic cells which can only manage one exciton per high-energy photon, with high kinetic energy carriers losing their energy as heat. On the other hand, the quantum-confined ground-states of colloidal quantum dots (e.g. lead sulfide, PbS) incorporated in wider-bandgap host semiconductors (e.g. perovskite) can allow the generation of photocurrent from photons with energy below the host bandgap, via a two-photon absorption process, offering another approach (termed intermediate band, IB) to exploit a broader range of the solar spectrum and thereby achieve higher photovoltaic efficiency.[90][91]

Colloidal quantum dot photovoltaics would theoretically be cheaper to manufacture, as they can be made using simple chemical reactions.

Quantum dot only solar cells

Aromatic self-assembled monolayers (SAMs) (e.g. 4-nitrobenzoic acid) can be used to improve the band alignment at electrodes for better efficiencies. This technique has provided a record power conversion efficiency (PCE) of 10.7%.[92] The SAM is positioned between ZnO-PbS colloidal quantum dot (CQD) film junction to modify band alignment via the dipole moment of the constituent SAM molecule, and the band tuning may be modified via the density, dipole and the orientation of the SAM molecule.[92]

Quantum dot in hybrid solar cells

Colloidal quantum dots are also used in inorganic/organic hybrid solar cells. These solar cells are attractive because of the potential for low-cost fabrication and relatively high efficiency.[93] Incorporation of metal oxides, such as ZnO, TiO2, and Nb2O5 nanomaterials into organic photovoltaics have been commercialized using full roll-to-roll processing.[93] A 13.2% power conversion efficiency is claimed in Si nanowire/PEDOT:PSS hybrid solar cells.[94]

Quantum dot with nanowire in solar cells

Another potential use involves capped single-crystal ZnO nanowires with CdSe quantum dots, immersed in mercaptopropionic acid as hole transport medium in order to obtain a QD-sensitized solar cell. The morphology of the nanowires allowed the electrons to have a direct pathway to the photoanode. This form of solar cell exhibits 50–60% internal quantum efficiencies.[95]

Nanowires with quantum dot coatings on silicon nanowires (SiNW) and carbon quantum dots. The use of SiNWs instead of planar silicon enhances the antiflection properties of Si.[96] The SiNW exhibits a light-trapping effect due to light trapping in the SiNW. This use of SiNWs in conjunction with carbon quantum dots resulted in a solar cell that reached 9.10% PCE.[96]

Graphene quantum dots have also been blended with organic electronic materials to improve efficiency and lower cost in photovoltaic devices and organic light emitting diodes (OLEDs) compared to graphene sheets. These graphene quantum dots were functionalized with organic ligands that experience photoluminescence from UV-Vis absorption.[97]

Light emitting diodes

See also: Light-emitting diode § Quantum-dot LEDs, and Quantum dot display

Several methods are proposed for using quantum dots to improve existing light-emitting diode (LED) design, including quantum dot light-emitting diode (QD-LED or QLED) displays, and quantum dot white-light-emitting diode (QD-WLED) displays. Because quantum dots naturally produce monochromatic light, they can be more efficient than light sources which must be color filtered. QD-LEDs can be fabricated on a silicon substrate, which allows them to be integrated onto standard silicon-based integrated circuits or microelectromechanical systems.[98]

Quantum dot displays

Main article: Quantum dot display

Quantum dots are valued for displays because they emit light in very specific gaussian distributions. This can result in a display with visibly more accurate colors.

A conventional color liquid crystal display (LCD) is usually backlit by fluorescent lamps (CCFLs) or conventional white LEDs that are color filtered to produce red, green, and blue pixels. Quantum dot displays use blue-emitting LEDs rather than white LEDs as the light sources. The converting part of the emitted light is converted into pure green and red light by the corresponding color quantum dots placed in front of the blue LED or using a quantum dot infused diffuser sheet in the backlight optical stack. Blank pixels are also used to allow the blue LED light to still generate blue hues. This type of white light as the backlight of an LCD panel allows for the best color gamut at lower cost than an RGB LED combination using three LEDs.[99]

Another method by which quantum dot displays can be achieved is the electroluminescent (EL) or electro-emissive method. This involves embedding quantum dots in each individual pixel. These are then activated and controlled via an electric current application.[100] Since this is often light emitting itself, the achievable colors may be limited in this method.[101] Electro-emissive QD-LED TVs exist in laboratories only.

The ability of QDs to precisely convert and tune a spectrum makes them attractive for LCD displays. Previous LCD displays can waste energy converting red-green poor, blue-yellow rich white light into a more balanced lighting. By using QDs, only the necessary colors for ideal images are contained in the screen. The result is a screen that is brighter, clearer, and more energy-efficient. The first commercial application of quantum dots was the Sony XBR X900A series of flat panel televisions released in 2013.[102]

In June 2006, QD Vision announced technical success in making a proof-of-concept quantum dot display and show a bright emission in the visible and near infrared region of the spectrum. A QD-LED integrated at a scanning microscopy tip was used to demonstrate fluorescence near-field scanning optical microscopy (NSOM) imaging.[103]

Photodetector devices

Quantum dot photodetectors (QDPs) can be fabricated either via solution-processing,[104] or from conventional single-crystalline semiconductors.[105] Conventional single-crystalline semiconductor QDPs are precluded from integration with flexible organic electronics due to the incompatibility of their growth conditions with the process windows required by organic semiconductors. On the other hand, solution-processed QDPs can be readily integrated with an almost infinite variety of substrates, and also postprocessed atop other integrated circuits. Such colloidal QDPs have potential applications in visible- and infrared-light cameras,[106] machine vision, industrial inspection, spectroscopy, and fluorescent biomedical imaging.

Photocatalysts

Main article: Photocatalysis

Quantum dots also function as photocatalysts for the light driven chemical conversion of water into hydrogen as a pathway to solar fuel. In photocatalysis, electron hole pairs formed in the dot under band gap excitation drive redox reactions in the surrounding liquid. Generally, the photocatalytic activity of the dots is related to the particle size and its degree of quantum confinement.[107] This is because the band gap determines the chemical energy that is stored in the dot in the excited state. An obstacle for the use of quantum dots in photocatalysis is the presence of surfactants on the surface of the dots. These surfactants (or ligands) interfere with the chemical reactivity of the dots by slowing down mass transfer and electron transfer processes. Also, quantum dots made of metal chalcogenides are chemically unstable under oxidizing conditions and undergo photo corrosion reactions.

Theory

Quantum dots are theoretically described as a point-like, or zero dimensional (0D) entity. Most of their properties depend on the dimensions, shape, and materials of which QDs are made. Generally, QDs present different thermodynamic properties from their bulk materials. One of these effects is melting-point depression. Optical properties of spherical metallic QDs are well described by the Mie scattering theory.

Quantum confinement in semiconductors

 
3D confined electron wave functions in a quantum dot. Here, rectangular and triangular-shaped quantum dots are shown. Energy states in rectangular dots are more s-type and p-type. However, in a triangular dot the wave functions are mixed due to confinement symmetry. (Click for animation)
Main article: Potential well

The energy levels of a single particle in a quantum dot can be predicted using the particle in a box model in which the energies of states depend on the length of the box. For an exciton inside a quantum dot, there is also the Coulomb interaction between the negatively charged electron and the positively charged hole. By comparing the quantum dot's size to the exciton Bohr radius, three regimes can be defined. In the 'strong confinement regime', the quantum dot's radius is much smaller than the exciton Bohr radius, respectively the confinement energy dominates over the Coulomb interactions.[108] In the 'weak confinement' regime, the quantum dot is larger than the exciton Bohr radius, respectively the confinement energy is smaller than the Coulomb interactions between electron and hole. The regime where the exciton Bohr radius and confinement potential are comparable is called the 'intermediate confinement regime'.[109]

 
Splitting of energy levels for small quantum dots due to the quantum confinement effect. The horizontal axis is the radius, or the size, of the quantum dots and ab* is the Exciton Bohr radius.
Band gap energy
The band gap can become smaller in the strong confinement regime as the energy levels split up. The exciton Bohr radius can be expressed as:
 
where aB=0.053 nm is the Bohr radius, m is the mass, μ is the reduced mass, and εr is the size-dependent dielectric constant (relative permittivity). This results in the increase in the total emission energy (the sum of the energy levels in the smaller band gaps in the strong confinement regime is larger than the energy levels in the band gaps of the original levels in the weak confinement regime) and the emission at various wavelengths. If the size distribution of QDs is not enough peaked, the convolution of multiple emission wavelengths is observed as a continuous spectra.
Confinement energy
The exciton entity can be modeled using the particle in the box. The electron and the hole can be seen as hydrogen in the Bohr model with the hydrogen nucleus replaced by the hole of positive charge and negative electron mass. Then the energy levels of the exciton can be represented as the solution to the particle in a box at the ground level (n = 1) with the mass replaced by the reduced mass. Thus by varying the size of the quantum dot, the confinement energy of the exciton can be controlled.
Bound exciton energy
There is Coulomb attraction between the negatively charged electron and the positively charged hole. The negative energy involved in the attraction is proportional to Rydberg's energy and inversely proportional to square of the size-dependent dielectric constant[110] of the semiconductor. When the size of the semiconductor crystal is smaller than the Exciton Bohr radius, the Coulomb interaction must be modified to fit the situation.

Therefore, the sum of these energies can be represented as:

 

where μ is the reduced mass, a is the radius of the quantum dot, me is the free electron mass, mh is the hole mass, and εr is the size-dependent dielectric constant.

Although the above equations were derived using simplifying assumptions, they imply that the electronic transitions of the quantum dots will depend on their size. These quantum confinement effects are apparent only below the critical size. Larger particles do not exhibit this effect. This effect of quantum confinement on the quantum dots has been repeatedly verified experimentally[111] and is a key feature of many emerging electronic structures.[112]

The Coulomb interaction between confined carriers can also be studied by numerical means when results unconstrained by asymptotic approximations are pursued.[113]

Besides confinement in all three dimensions (i.e., a quantum dot), other quantum confined semiconductors include:

  • Quantum wires, which confine electrons or holes in two spatial dimensions and allow free propagation in the third.
  • Quantum wells, which confine electrons or holes in one dimension and allow free propagation in two dimensions.

Models

A variety of theoretical frameworks exist to model optical, electronic, and structural properties of quantum dots. These may be broadly divided into quantum mechanical, semiclassical, and classical.

Quantum mechanics

Quantum mechanical models and simulations of quantum dots often involve the interaction of electrons with a pseudopotential or random matrix.[114]

Semiclassical

Semiclassical models of quantum dots frequently incorporate a chemical potential. For example, the thermodynamic chemical potential of an N-particle system is given by

 

whose energy terms may be obtained as solutions of the Schrödinger equation. The definition of capacitance,

 ,

with the potential difference

 

may be applied to a quantum dot with the addition or removal of individual electrons,

  and  .

Then

 

is the quantum capacitance of a quantum dot, where we denoted by I(N) the ionization potential and by A(N) the electron affinity of the N-particle system.[115]

Classical mechanics

Classical models of electrostatic properties of electrons in quantum dots are similar in nature to the Thomson problem of optimally distributing electrons on a unit sphere.

The classical electrostatic treatment of electrons confined to spherical quantum dots is similar to their treatment in the Thomson,[116] or plum pudding model, of the atom.[117]

The classical treatment of both two-dimensional and three-dimensional quantum dots exhibit electron shell-filling behavior. A "periodic table of classical artificial atoms" has been described for two-dimensional quantum dots.[118] As well, several connections have been reported between the three-dimensional Thomson problem and electron shell-filling patterns found in naturally-occurring atoms found throughout the periodic table.[119] This latter work originated in classical electrostatic modeling of electrons in a spherical quantum dot represented by an ideal dielectric sphere.[120]

History

The term quantum dot was coined in 1986.[121] They were first synthesized in a glass matrix by Alexey Ekimov in 1981[122][123][124][125] and in colloidal suspension[126] by Louis Brus in 1983.[127][128] They were first theorized by Alexander Efros in 1982.[129]

See also

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Further reading

  • Delerue, C. & Lannoo, M. (2004). Nanostructures: Theory and Modelling. Springer. p. 47. ISBN 978-3-540-20694-1.</ref> Methods to produce quantum-confined semiconductor structures (quantum wires, wells, and dots via grown by advanced epitaxial techniques), nanocrystals by gas-phase, liquid-phase, and solid-phase approaches.
  • Norris, D. J. (1995). "Measurement and Assignment of the Size-Dependent Optical Spectrum in Cadmium Selenide (CdSe) Quantum Dots, PhD thesis, MIT". hdl:1721.1/11129. Photoluminescence of a QD vs. particle diameter.

External links

  • Quantum Dots: Technical Status and Market Prospects
  • Quantum dot on arxiv.org
  • Quantum Dots Research and Technical Data

March 28, 2023
quantum, also, called, semiconductor, nanocrystals, semiconductor, particles, nanometres, size, having, optical, electronic, properties, that, differ, from, those, larger, particles, result, quantum, mechanics, they, central, topic, nanotechnology, materials, . Quantum dots QDs also called semiconductor nanocrystals are semiconductor particles a few nanometres in size having optical and electronic properties that differ from those of larger particles as a result of quantum mechanics They are a central topic in nanotechnology and materials science When the quantum dots are illuminated by UV light an electron in the quantum dot can be excited to a state of higher energy In the case of a semiconducting quantum dot this process corresponds to the transition of an electron from the valence band to the conductance band The excited electron can drop back into the valence band releasing its energy as light This light emission photoluminescence is illustrated in the figure on the right The color of that light depends on the energy difference between the conductance band and the valence band or the transition between discrete energy states when the band structure is no longer well defined in QDs Colloidal quantum dots irradiated with a UV light Different sized quantum dots emit different colors of light due to quantum confinement Nanoscale semiconductor materials tightly confine either electrons or electron holes The confinement is similar to a three dimensional particle in a box model The quantum dot absorption and emission features correspond to transitions between discrete quantum mechanically allowed energy levels in the box that are reminiscent of atomic spectra For these reasons quantum dots are sometimes referred to as artificial atoms 1 emphasizing their bound and discrete electronic states like naturally occurring atoms or molecules 2 3 It was shown that the electronic wave functions in quantum dots resemble the ones in real atoms 4 By coupling two or more such quantum dots an artificial molecule can be made exhibiting hybridization even at room temperature 5 Quantum dots have properties intermediate between bulk semiconductors and discrete atoms or molecules Their optoelectronic properties change as a function of both size and shape 6 7 Larger QDs of 5 6 nm diameter emit longer wavelengths with colors such as orange or red Smaller QDs 2 3 nm emit shorter wavelengths yielding colors like blue and green However the specific colors vary depending on the exact composition of the QD 8 Potential applications of quantum dots include single electron transistors solar cells LEDs lasers 9 single photon sources 10 11 12 second harmonic generation quantum computing 13 cell biology research 14 microscopy 15 and medical imaging 16 Their small size allows for some QDs to be suspended in solution which may lead to their use in inkjet printing and spin coating 17 They have been used in Langmuir Blodgett thin films 18 19 20 These processing techniques result in less expensive and less time consuming methods of semiconductor fabrication Contents 1 Production 1 1 Colloidal synthesis 1 2 Plasma synthesis 1 3 Fabrication 1 4 Viral assembly 1 5 Electrochemical assembly 1 6 Bulk manufacture 1 7 Heavy metal free quantum dots 2 Health and safety 3 Optical properties 4 Applications 4 1 Subcutaneous record keeping 4 2 Biology 4 3 Photovoltaic devices 4 3 1 Quantum dot only solar cells 4 3 2 Quantum dot in hybrid solar cells 4 3 3 Quantum dot with nanowire in solar cells 4 4 Light emitting diodes 4 5 Quantum dot displays 4 6 Photodetector devices 4 7 Photocatalysts 5 Theory 6 Quantum confinement in semiconductors 6 1 Models 6 2 Quantum mechanics 6 2 1 Semiclassical 6 2 2 Classical mechanics 7 History 8 See also 9 References 10 Further reading 11 External linksProduction Edit Quantum Dots with gradually stepping emission from violet to deep red There are several ways to fabricate quantum dots Possible methods include colloidal synthesis self assembly and electrical gating Colloidal synthesis Edit Colloidal semiconductor nanocrystals are synthesized from solutions much like traditional chemical processes The main difference is the product neither precipitates as a bulk solid nor remains dissolved 6 Heating the solution at high temperature the precursors decompose forming monomers which then nucleate and generate nanocrystals Temperature is a critical factor in determining optimal conditions for the nanocrystal growth It must be high enough to allow for rearrangement and annealing of atoms during the synthesis process while being low enough to promote crystal growth The concentration of monomers is another critical factor that has to be stringently controlled during nanocrystal growth The growth process of nanocrystals can occur in two different regimes focusing and defocusing At high monomer concentrations the critical size the size where nanocrystals neither grow nor shrink is relatively small resulting in growth of nearly all particles In this regime smaller particles grow faster than large ones since larger crystals need more atoms to grow than small crystals resulting in the size distribution focusing yielding an improbable distribution of nearly monodispersed particles The size focusing is optimal when the monomer concentration is kept such that the average nanocrystal size present is always slightly larger than the critical size Over time the monomer concentration diminishes the critical size becomes larger than the average size present and the distribution defocuses Cadmium sulfide quantum dots on cells There are colloidal methods to produce many different semiconductors Typical dots are made of binary compounds such as lead sulfide lead selenide cadmium selenide cadmium sulfide cadmium telluride indium arsenide and indium phosphide Dots may also be made from ternary compounds such as cadmium selenide sulfide Further recent advances have been made which allow for synthesis of colloidal perovskite quantum dots 21 These quantum dots can contain as few as 100 to 100 000 atoms within the quantum dot volume with a diameter of 10 to 50 atoms This corresponds to about 2 to 10 nanometers and at 10 nm in diameter nearly 3 million quantum dots could be lined up end to end and fit within the width of a human thumb Idealized image of colloidal nanoparticle of lead sulfide selenide with complete passivation by oleic acid oleyl amine and hydroxyl ligands size 5nm Large batches of quantum dots may be synthesized via colloidal synthesis Due to this scalability and the convenience of benchtop conditions colloidal synthetic methods are promising for commercial applications Plasma synthesis Edit Plasma synthesis has evolved to be one of the most popular gas phase approaches for the production of quantum dots especially those with covalent bonds 22 23 24 For example silicon Si and germanium Ge quantum dots have been synthesized by using nonthermal plasma The size shape surface and composition of quantum dots can all be controlled in nonthermal plasma 25 26 Doping that seems quite challenging for quantum dots has also been realized in plasma synthesis 27 28 29 Quantum dots synthesized by plasma are usually in the form of powder for which surface modification may be carried out This can lead to excellent dispersion of quantum dots in either organic solvents 30 or water 31 i e colloidal quantum dots Fabrication Edit The electrostatic potential needed to create a quantum dot can be realized with several methods These include external electrodes 32 doping strain 33 or impurities Self assembled quantum dots are typically between 5 and 50 nm in size Quantum dots defined by lithographically patterned gate electrodes or by etching on two dimensional electron gases in semiconductor heterostructures can have lateral dimensions between 20 and 100 nm Some quantum dots are small regions of one material buried in another with a larger band gap These can be so called core shell structures e g with CdSe in the core and ZnS in the shell or from special forms of silica called ormosil Sub monolayer shells can also be effective ways of passivating the quantum dots such as PbS cores with sub monolayer CdS shells 34 Quantum dots sometimes occur spontaneously in quantum well structures due to monolayer fluctuations in the well s thickness Atomic resolution scanning transmission electron microscopy image of an indium gallium arsenide InGaAs quantum dot buried in gallium arsenide GaAs Self assembled quantum dots nucleate spontaneously under certain conditions during molecular beam epitaxy MBE and metalorganic vapour phase epitaxy MOVPE when a material is grown on a substrate to which it is not lattice matched The resulting strain leads to the formation of islands on top of a two dimensional wetting layer This growth mode is known as Stranski Krastanov growth 35 The islands can be subsequently buried to form the quantum dot A widely used type of quantum dots grown with this method are indium gallium arsenide InGaAs quantum dots in gallium arsenide GaAs 36 Such quantum dots have the potential for applications in quantum cryptography i e single photon sources and quantum computation The main limitations of this method are the cost of fabrication and the lack of control over positioning of individual dots Individual quantum dots can be created from two dimensional electron or hole gases present in remotely doped quantum wells or semiconductor heterostructures called lateral quantum dots The sample surface is coated with a thin layer of resist and a lateral pattern is then defined in the resist by electron beam lithography This pattern can then be transferred to the electron or hole gas by etching or by depositing metal electrodes lift off process that allow the application of external voltages between the electron gas and the electrodes Such quantum dots are mainly of interest for experiments and applications involving electron or hole transport and they are also used as spin qubits 37 A strength of this type of quantum dots is that their energy spectrum can be engineered by controlling the geometrical size shape and the strength of the confinement potential with gate electrodes These quantum dots can be easily connected by tunnel barriers to conducting leads which allows the application of the techniques of tunneling spectroscopy for their investigation Complementary metal oxide semiconductor CMOS technology can be employed to fabricate silicon quantum dots Ultra small L 20 nm W 20 nm CMOS transistors behave as single electron quantum dots when operated at cryogenic temperature over a range of 269 C 4 K to about 258 C 15 K The transistor displays Coulomb blockade due to progressive charging of electrons holes one by one The number of electrons holes confined in the channel is driven by the gate voltage starting from an occupation of zero electrons holes and it can be set to 1 or many 38 Viral assembly Edit Genetically engineered M13 bacteriophage viruses allow preparation of quantum dot biocomposite structures 39 It had previously been shown that genetically engineered viruses can recognize specific semiconductor surfaces through the method of selection by combinatorial phage display 40 Additionally it is known that liquid crystalline structures of wild type viruses Fd M13 and TMV are adjustable by controlling the solution concentrations solution ionic strength and the external magnetic field applied to the solutions Consequently the specific recognition properties of the virus can be used to organize inorganic nanocrystals forming ordered arrays over the length scale defined by liquid crystal formation Using this information Lee et al 2000 were able to create self assembled highly oriented self supporting films from a phage and ZnS precursor solution This system allowed them to vary both the length of bacteriophage and the type of inorganic material through genetic modification and selection Electrochemical assembly Edit Highly ordered arrays of quantum dots may also be self assembled by electrochemical techniques A template is created by causing an ionic reaction at an electrolyte metal interface which results in the spontaneous assembly of nanostructures including quantum dots onto the metal which is then used as a mask for mesa etching these nanostructures on a chosen substrate citation needed Bulk manufacture Edit Quantum dot manufacturing relies on a process called high temperature dual injection which has been scaled by multiple companies for commercial applications that require large quantities hundreds of kilograms to tons of quantum dots This reproducible production method can be applied to a wide range of quantum dot sizes and compositions The bonding in certain cadmium free quantum dots such as III V based quantum dots is more covalent than that in II VI materials therefore it is more difficult to separate nanoparticle nucleation and growth via a high temperature dual injection synthesis An alternative method of quantum dot synthesis the molecular seeding process provides a reproducible route to the production of high quality quantum dots in large volumes The process utilises identical molecules of a molecular cluster compound as the nucleation sites for nanoparticle growth thus avoiding the need for a high temperature injection step Particle growth is maintained by the periodic addition of precursors at moderate temperatures until the desired particle size is reached 41 The molecular seeding process is not limited to the production of cadmium free quantum dots for example the process can be used to synthesise kilogram batches of high quality II VI quantum dots in just a few hours Another approach for the mass production of colloidal quantum dots can be seen in the transfer of the well known hot injection methodology for the synthesis to a technical continuous flow system The batch to batch variations arising from the needs during the mentioned methodology can be overcome by utilizing technical components for mixing and growth as well as transport and temperature adjustments For the production of CdSe based semiconductor nanoparticles this method has been investigated and tuned to production amounts of kg per month Since the use of technical components allows for easy interchange in regards of maximum throughput and size it can be further enhanced to tens or even hundreds of kilograms 42 In 2011 a consortium of U S and Dutch companies reported a milestone in high volume quantum dot manufacturing by applying the traditional high temperature dual injection method to a flow system 43 On 23 January 2013 Dow entered into an exclusive licensing agreement with UK based Nanoco for the use of their low temperature molecular seeding method for bulk manufacture of cadmium free quantum dots for electronic displays and on 24 September 2014 Dow commenced work on the production facility in South Korea capable of producing sufficient quantum dots for millions of cadmium free televisions and other devices such as tablets Mass production is due to commence in mid 2015 44 On 24 March 2015 Dow announced a partnership deal with LG Electronics to develop the use of cadmium free quantum dots in displays 45 Heavy metal free quantum dots Edit In many which regions of the world there is now a restriction or ban on the use of toxic heavy metals in many household goods which means that most cadmium based quantum dots are unusable for consumer goods applications For commercial viability a range of restricted heavy metal free quantum dots has been developed showing bright emissions in the visible and near infrared region of the spectrum and have similar optical properties to those of CdSe quantum dots Among these materials are InP ZnS CuInS ZnS Si Ge and C Peptides are being researched as potential quantum dot material 46 Health and safety EditMain articles Health and safety hazards of nanomaterials and Nanotoxicology Some quantum dots pose risks to human health and the environment under certain conditions 47 48 49 Notably the studies on quantum dot toxicity have focused on particles containing cadmium and have yet to be demonstrated in animal models after physiologically relevant dosing 49 In vitro studies based on cell cultures on quantum dots QD toxicity suggest that their toxicity may derive from multiple factors including their physicochemical characteristics size shape composition surface functional groups and surface charges and their environment Assessing their potential toxicity is complex as these factors include properties such as QD size charge concentration chemical composition capping ligands and also on their oxidative mechanical and photolytic stability 47 Many studies have focused on the mechanism of QD cytotoxicity using model cell cultures It has been demonstrated that after exposure to ultraviolet radiation or oxidation by air CdSe QDs release free cadmium ions causing cell death 50 Group II VI QDs also have been reported to induce the formation of reactive oxygen species after exposure to light which in turn can damage cellular components such as proteins lipids and DNA 51 Some studies have also demonstrated that addition of a ZnS shell inhibits the process of reactive oxygen species in CdSe QDs Another aspect of QD toxicity is that there are in vivo size dependent intracellular pathways that concentrate these particles in cellular organelles that are inaccessible by metal ions which may result in unique patterns of cytotoxicity compared to their constituent metal ions 52 The reports of QD localization in the cell nucleus 53 present additional modes of toxicity because they may induce DNA mutation which in turn will propagate through future generation of cells causing diseases Although concentration of QDs in certain organelles have been reported in in vivo studies using animal models no alterations in animal behavior weight hematological markers or organ damage has been found through either histological or biochemical analysis 54 These findings have led scientists to believe that intracellular dose is the most important determining factor for QD toxicity Therefore factors determining the QD endocytosis that determine the effective intracellular concentration such as QD size shape and surface chemistry determine their toxicity Excretion of QDs through urine in animal models also have demonstrated via injecting radio labeled ZnS capped CdSe QDs where the ligand shell was labeled with 99mTc 55 Though multiple other studies have concluded retention of QDs in cellular levels 49 56 exocytosis of QDs is still poorly studied in the literature While significant research efforts have broadened the understanding of toxicity of QDs there are large discrepancies in the literature and questions still remain to be answered Diversity of this class of material as compared to normal chemical substances makes the assessment of their toxicity very challenging As their toxicity may also be dynamic depending on the environmental factors such as pH level light exposure and cell type traditional methods of assessing toxicity of chemicals such as LD50 are not applicable for QDs Therefore researchers are focusing on introducing novel approaches and adapting existing methods to include this unique class of materials 49 Furthermore novel strategies to engineer safer QDs are still under exploration by the scientific community A recent novelty in the field is the discovery of carbon quantum dots a new generation of optically active nanoparticles potentially capable of replacing semiconductor QDs but with the advantage of much lower toxicity Optical properties Edit Fluorescence spectra of CdTe quantum dots of various sizes Different sized quantum dots emit different color light due to quantum confinement In semiconductors light absorption generally leads to an electron being excited from the valence to the conduction band leaving behind a hole The electron and the hole can bind to each other to form an exciton When this exciton recombines i e the electron resumes its ground state the exciton s energy can be emitted as light This is called fluorescence In a simplified model the energy of the emitted photon can be understood as the sum of the band gap energy between the highest occupied level and the lowest unoccupied energy level the confinement energies of the hole and the excited electron and the bound energy of the exciton the electron hole pair As the confinement energy depends on the quantum dot s size both absorption onset and fluorescence emission can be tuned by changing the size of the quantum dot during its synthesis The larger the dot the redder lower energy its absorption onset and fluorescence spectrum Conversely smaller dots absorb and emit bluer higher energy light Recent articles suggest that the shape of the quantum dot may be a factor in the coloration as well but as yet not enough information is available citation needed Furthermore it was shown 57 that the lifetime of fluorescence is determined by the size of the quantum dot Larger dots have more closely spaced energy levels in which the electron hole pair can be trapped Therefore electron hole pairs in larger dots live longer causing larger dots to show a longer lifetime To improve fluorescence quantum yield quantum dots can be made with shells of a larger bandgap semiconductor material around them The improvement is suggested to be due to the reduced access of electron and hole to non radiative surface recombination pathways in some cases but also due to reduced Auger recombination in others Applications EditQuantum dots are particularly promising for optical applications due to their high extinction coefficient 58 and ultrafast optical nonlinearities with potential applications for developing all optical systems 59 They operate like a single electron transistor and show the Coulomb blockade effect Quantum dots have also been suggested as implementations of qubits for quantum information processing 60 and as active elements for thermoelectrics 61 62 63 Tuning the size of quantum dots is attractive for many potential applications For instance larger quantum dots have a greater spectrum shift toward red compared to smaller dots and exhibit less pronounced quantum properties Conversely the smaller particles allow one to take advantage of more subtle quantum effects A device that produces visible light through energy transfer from thin layers of quantum wells to crystals above the layers 64 Being zero dimensional quantum dots have a sharper density of states than higher dimensional structures As a result they have superior transport and optical properties They have potential uses in diode lasers amplifiers and biological sensors 65 Quantum dots may be excited within a locally enhanced electromagnetic field produced by gold nanoparticles which then can be observed from the surface plasmon resonance in the photoluminescent excitation spectrum of CdSe ZnS nanocrystals High quality quantum dots are well suited for optical encoding and multiplexing applications due to their broad excitation profiles and narrow symmetric emission spectra The new generations of quantum dots have far reaching potential for the study of intracellular processes at the single molecule level high resolution cellular imaging long term in vivo observation of cell trafficking tumor targeting and diagnostics CdSe nanocrystals are efficient triplet photosensitizers 66 Laser excitation of small CdSe nanoparticles enables the extraction of the excited state energy from the quantum dots into bulk solution thus opening the door to a wide range of potential applications such as photodynamic therapy photovoltaic devices molecular electronics and catalysis Subcutaneous record keeping Edit In December 2019 Robert S Langer and his team developed and patented a technique whereby transdermal patches could be used to apply an identification tattoo to people with invisible ink to store information subcutaneously This was presented as a boon to developing nations where lack of infrastructure means an absence of medical records 67 68 The technology which is assigned to the Massachusetts Institute of Technology 68 uses a quantum dot dye that is delivered in this case along with a vaccine by a microneedle patch The research was funded by the Bill and Melinda Gates Foundation and the Koch Institute for Integrative Cancer Research 67 Biology Edit In modern biological analysis various kinds of organic dyes are used However as technology advances greater flexibility in these dyes is sought 69 To this end quantum dots have quickly filled in the role being found to be superior to traditional organic dyes on several counts one of the most immediately obvious being brightness owing to the high extinction coefficient combined with a comparable quantum yield to fluorescent dyes 14 as well as their stability allowing much less photobleaching 70 It has been estimated that quantum dots are 20 times brighter and 100 times more stable than traditional fluorescent reporters 69 For single particle tracking the irregular blinking of quantum dots is a minor drawback However there have been groups which have developed quantum dots which are essentially nonblinking and demonstrated their utility in single molecule tracking experiments 71 72 The use of quantum dots for highly sensitive cellular imaging has seen major advances 73 The improved photostability of quantum dots for example allows the acquisition of many consecutive focal plane images that can be reconstructed into a high resolution three dimensional image 74 Another application that takes advantage of the extraordinary photostability of quantum dot probes is the real time tracking of molecules and cells over extended periods of time 75 Antibodies streptavidin 76 peptides 77 DNA 78 nucleic acid aptamers 79 or small molecule ligands 80 can be used to target quantum dots to specific proteins on cells Researchers were able to observe quantum dots in lymph nodes of mice for more than 4 months 81 Quantum dots can have antibacterial properties similar to nanoparticles and can kill bacteria in a dose dependent manner 82 One mechanism by which quantum dots can kill bacteria is through impairing the functions of antioxidative system in the cells and down regulating the antioxidative genes In addition quantum dots can directly damage the cell wall Quantum dots have been shown to be effective against both gram positive and gram negative bacteria 83 Semiconductor quantum dots have also been employed for in vitro imaging of pre labeled cells The ability to image single cell migration in real time is expected to be important to several research areas such as embryogenesis cancer metastasis stem cell therapeutics and lymphocyte immunology One application of quantum dots in biology is as donor fluorophores in Forster resonance energy transfer where the large extinction coefficient and spectral purity of these fluorophores make them superior to molecular fluorophores 84 It is also worth noting that the broad absorbance of QDs allows selective excitation of the QD donor and a minimum excitation of a dye acceptor in FRET based studies 85 The applicability of the FRET model which assumes that the Quantum Dot can be approximated as a point dipole has recently been demonstrated 86 The use of quantum dots for tumor targeting under in vivo conditions employ two targeting schemes active targeting and passive targeting In the case of active targeting quantum dots are functionalized with tumor specific binding sites to selectively bind to tumor cells Passive targeting uses the enhanced permeation and retention of tumor cells for the delivery of quantum dot probes Fast growing tumor cells typically have more permeable membranes than healthy cells allowing the leakage of small nanoparticles into the cell body Moreover tumor cells lack an effective lymphatic drainage system which leads to subsequent nanoparticle accumulation Quantum dot probes exhibit in vivo toxicity For example CdSe nanocrystals are highly toxic to cultured cells under UV illumination because the particles dissolve in a process known as photolysis to release toxic cadmium ions into the culture medium In the absence of UV irradiation however quantum dots with a stable polymer coating have been found to be essentially nontoxic 81 48 Hydrogel encapsulation of quantum dots allows for quantum dots to be introduced into a stable aqueous solution reducing the possibility of cadmium leakage Then again only little is known about the excretion process of quantum dots from living organisms 87 In another potential application quantum dots are being investigated as the inorganic fluorophore for intra operative detection of tumors using fluorescence spectroscopy Delivery of undamaged quantum dots to the cell cytoplasm has been a challenge with existing techniques Vector based methods have resulted in aggregation and endosomal sequestration of quantum dots while electroporation can damage the semi conducting particles and aggregate delivered dots in the cytosol Via cell squeezing quantum dots can be efficiently delivered without inducing aggregation trapping material in endosomes or significant loss of cell viability Moreover it has shown that individual quantum dots delivered by this approach are detectable in the cell cytosol thus illustrating the potential of this technique for single molecule tracking studies 88 Photovoltaic devices Edit Main article Quantum dot solar cell The tunable absorption spectrum and high extinction coefficients of quantum dots make them attractive for light harvesting technologies such as photovoltaics Quantum dots may be able to increase the efficiency and reduce the cost of today s typical silicon photovoltaic cells According to an experimental report from 2004 89 quantum dots of lead selenide PbSe can produce more than one exciton from one high energy photon via the process of carrier multiplication or multiple exciton generation MEG This compares favorably to today s photovoltaic cells which can only manage one exciton per high energy photon with high kinetic energy carriers losing their energy as heat On the other hand the quantum confined ground states of colloidal quantum dots e g lead sulfide PbS incorporated in wider bandgap host semiconductors e g perovskite can allow the generation of photocurrent from photons with energy below the host bandgap via a two photon absorption process offering another approach termed intermediate band IB to exploit a broader range of the solar spectrum and thereby achieve higher photovoltaic efficiency 90 91 Colloidal quantum dot photovoltaics would theoretically be cheaper to manufacture as they can be made using simple chemical reactions Quantum dot only solar cells Edit Aromatic self assembled monolayers SAMs e g 4 nitrobenzoic acid can be used to improve the band alignment at electrodes for better efficiencies This technique has provided a record power conversion efficiency PCE of 10 7 92 The SAM is positioned between ZnO PbS colloidal quantum dot CQD film junction to modify band alignment via the dipole moment of the constituent SAM molecule and the band tuning may be modified via the density dipole and the orientation of the SAM molecule 92 Quantum dot in hybrid solar cells Edit Colloidal quantum dots are also used in inorganic organic hybrid solar cells These solar cells are attractive because of the potential for low cost fabrication and relatively high efficiency 93 Incorporation of metal oxides such as ZnO TiO2 and Nb2O5 nanomaterials into organic photovoltaics have been commercialized using full roll to roll processing 93 A 13 2 power conversion efficiency is claimed in Si nanowire PEDOT PSS hybrid solar cells 94 Quantum dot with nanowire in solar cells Edit Another potential use involves capped single crystal ZnO nanowires with CdSe quantum dots immersed in mercaptopropionic acid as hole transport medium in order to obtain a QD sensitized solar cell The morphology of the nanowires allowed the electrons to have a direct pathway to the photoanode This form of solar cell exhibits 50 60 internal quantum efficiencies 95 Nanowires with quantum dot coatings on silicon nanowires SiNW and carbon quantum dots The use of SiNWs instead of planar silicon enhances the antiflection properties of Si 96 The SiNW exhibits a light trapping effect due to light trapping in the SiNW This use of SiNWs in conjunction with carbon quantum dots resulted in a solar cell that reached 9 10 PCE 96 Graphene quantum dots have also been blended with organic electronic materials to improve efficiency and lower cost in photovoltaic devices and organic light emitting diodes OLEDs compared to graphene sheets These graphene quantum dots were functionalized with organic ligands that experience photoluminescence from UV Vis absorption 97 Light emitting diodes Edit See also Light emitting diode Quantum dot LEDs and Quantum dot display Several methods are proposed for using quantum dots to improve existing light emitting diode LED design including quantum dot light emitting diode QD LED or QLED displays and quantum dot white light emitting diode QD WLED displays Because quantum dots naturally produce monochromatic light they can be more efficient than light sources which must be color filtered QD LEDs can be fabricated on a silicon substrate which allows them to be integrated onto standard silicon based integrated circuits or microelectromechanical systems 98 Quantum dot displays Edit Main article Quantum dot display Quantum dots are valued for displays because they emit light in very specific gaussian distributions This can result in a display with visibly more accurate colors A conventional color liquid crystal display LCD is usually backlit by fluorescent lamps CCFLs or conventional white LEDs that are color filtered to produce red green and blue pixels Quantum dot displays use blue emitting LEDs rather than white LEDs as the light sources The converting part of the emitted light is converted into pure green and red light by the corresponding color quantum dots placed in front of the blue LED or using a quantum dot infused diffuser sheet in the backlight optical stack Blank pixels are also used to allow the blue LED light to still generate blue hues This type of white light as the backlight of an LCD panel allows for the best color gamut at lower cost than an RGB LED combination using three LEDs 99 Another method by which quantum dot displays can be achieved is the electroluminescent EL or electro emissive method This involves embedding quantum dots in each individual pixel These are then activated and controlled via an electric current application 100 Since this is often light emitting itself the achievable colors may be limited in this method 101 Electro emissive QD LED TVs exist in laboratories only The ability of QDs to precisely convert and tune a spectrum makes them attractive for LCD displays Previous LCD displays can waste energy converting red green poor blue yellow rich white light into a more balanced lighting By using QDs only the necessary colors for ideal images are contained in the screen The result is a screen that is brighter clearer and more energy efficient The first commercial application of quantum dots was the Sony XBR X900A series of flat panel televisions released in 2013 102 In June 2006 QD Vision announced technical success in making a proof of concept quantum dot display and show a bright emission in the visible and near infrared region of the spectrum A QD LED integrated at a scanning microscopy tip was used to demonstrate fluorescence near field scanning optical microscopy NSOM imaging 103 Photodetector devices Edit Quantum dot photodetectors QDPs can be fabricated either via solution processing 104 or from conventional single crystalline semiconductors 105 Conventional single crystalline semiconductor QDPs are precluded from integration with flexible organic electronics due to the incompatibility of their growth conditions with the process windows required by organic semiconductors On the other hand solution processed QDPs can be readily integrated with an almost infinite variety of substrates and also postprocessed atop other integrated circuits Such colloidal QDPs have potential applications in visible and infrared light cameras 106 machine vision industrial inspection spectroscopy and fluorescent biomedical imaging Photocatalysts Edit Main article Photocatalysis Quantum dots also function as photocatalysts for the light driven chemical conversion of water into hydrogen as a pathway to solar fuel In photocatalysis electron hole pairs formed in the dot under band gap excitation drive redox reactions in the surrounding liquid Generally the photocatalytic activity of the dots is related to the particle size and its degree of quantum confinement 107 This is because the band gap determines the chemical energy that is stored in the dot in the excited state An obstacle for the use of quantum dots in photocatalysis is the presence of surfactants on the surface of the dots These surfactants or ligands interfere with the chemical reactivity of the dots by slowing down mass transfer and electron transfer processes Also quantum dots made of metal chalcogenides are chemically unstable under oxidizing conditions and undergo photo corrosion reactions Theory EditQuantum dots are theoretically described as a point like or zero dimensional 0D entity Most of their properties depend on the dimensions shape and materials of which QDs are made Generally QDs present different thermodynamic properties from their bulk materials One of these effects is melting point depression Optical properties of spherical metallic QDs are well described by the Mie scattering theory Quantum confinement in semiconductors Edit 3D confined electron wave functions in a quantum dot Here rectangular and triangular shaped quantum dots are shown Energy states in rectangular dots are more s type and p type However in a triangular dot the wave functions are mixed due to confinement symmetry Click for animation Main article Potential well The energy levels of a single particle in a quantum dot can be predicted using the particle in a box model in which the energies of states depend on the length of the box For an exciton inside a quantum dot there is also the Coulomb interaction between the negatively charged electron and the positively charged hole By comparing the quantum dot s size to the exciton Bohr radius three regimes can be defined In the strong confinement regime the quantum dot s radius is much smaller than the exciton Bohr radius respectively the confinement energy dominates over the Coulomb interactions 108 In the weak confinement regime the quantum dot is larger than the exciton Bohr radius respectively the confinement energy is smaller than the Coulomb interactions between electron and hole The regime where the exciton Bohr radius and confinement potential are comparable is called the intermediate confinement regime 109 Splitting of energy levels for small quantum dots due to the quantum confinement effect The horizontal axis is the radius or the size of the quantum dots and ab is the Exciton Bohr radius Band gap energy The band gap can become smaller in the strong confinement regime as the energy levels split up The exciton Bohr radius can be expressed as a B e r m m a B displaystyle a rm B varepsilon rm r left frac m mu right a rm B dd where aB 0 053 nm is the Bohr radius m is the mass m is the reduced mass and er is the size dependent dielectric constant relative permittivity This results in the increase in the total emission energy the sum of the energy levels in the smaller band gaps in the strong confinement regime is larger than the energy levels in the band gaps of the original levels in the weak confinement regime and the emission at various wavelengths If the size distribution of QDs is not enough peaked the convolution of multiple emission wavelengths is observed as a continuous spectra Confinement energy The exciton entity can be modeled using the particle in the box The electron and the hole can be seen as hydrogen in the Bohr model with the hydrogen nucleus replaced by the hole of positive charge and negative electron mass Then the energy levels of the exciton can be represented as the solution to the particle in a box at the ground level n 1 with the mass replaced by the reduced mass Thus by varying the size of the quantum dot the confinement energy of the exciton can be controlled Bound exciton energy There is Coulomb attraction between the negatively charged electron and the positively charged hole The negative energy involved in the attraction is proportional to Rydberg s energy and inversely proportional to square of the size dependent dielectric constant 110 of the semiconductor When the size of the semiconductor crystal is smaller than the Exciton Bohr radius the Coulomb interaction must be modified to fit the situation Therefore the sum of these energies can be represented as E confinement ℏ 2 p 2 2 a 2 1 m e 1 m h ℏ 2 p 2 2 m a 2 E exciton 1 ϵ r 2 m m e R y R y E E bandgap E confinement E exciton E bandgap ℏ 2 p 2 2 m a 2 R y displaystyle begin aligned E textrm confinement amp frac hbar 2 pi 2 2a 2 left frac 1 m rm e frac 1 m h right frac hbar 2 pi 2 2 mu a 2 E textrm exciton amp frac 1 epsilon rm r 2 frac mu m rm e R y R y E amp E textrm bandgap E textrm confinement E textrm exciton amp E textrm bandgap frac hbar 2 pi 2 2 mu a 2 R y end aligned where m is the reduced mass a is the radius of the quantum dot me is the free electron mass mh is the hole mass and er is the size dependent dielectric constant Although the above equations were derived using simplifying assumptions they imply that the electronic transitions of the quantum dots will depend on their size These quantum confinement effects are apparent only below the critical size Larger particles do not exhibit this effect This effect of quantum confinement on the quantum dots has been repeatedly verified experimentally 111 and is a key feature of many emerging electronic structures 112 The Coulomb interaction between confined carriers can also be studied by numerical means when results unconstrained by asymptotic approximations are pursued 113 Besides confinement in all three dimensions i e a quantum dot other quantum confined semiconductors include Quantum wires which confine electrons or holes in two spatial dimensions and allow free propagation in the third Quantum wells which confine electrons or holes in one dimension and allow free propagation in two dimensions Models Edit A variety of theoretical frameworks exist to model optical electronic and structural properties of quantum dots These may be broadly divided into quantum mechanical semiclassical and classical Quantum mechanics Edit Quantum mechanical models and simulations of quantum dots often involve the interaction of electrons with a pseudopotential or random matrix 114 Semiclassical Edit Semiclassical models of quantum dots frequently incorporate a chemical potential For example the thermodynamic chemical potential of an N particle system is given by m N E N E N 1 displaystyle mu N E N E N 1 whose energy terms may be obtained as solutions of the Schrodinger equation The definition of capacitance 1 C D V D Q displaystyle 1 over C equiv Delta V over Delta Q with the potential difference D V D m e m N D N m N e displaystyle Delta V Delta mu over e mu N Delta N mu N over e may be applied to a quantum dot with the addition or removal of individual electrons D N 1 displaystyle Delta N 1 and D Q e displaystyle Delta Q e Then C N e 2 m N 1 m N e 2 I N A N displaystyle C N e 2 over mu N 1 mu N e 2 over I N A N is the quantum capacitance of a quantum dot where we denoted by I N the ionization potential and by A N the electron affinity of the N particle system 115 Classical mechanics Edit Classical models of electrostatic properties of electrons in quantum dots are similar in nature to the Thomson problem of optimally distributing electrons 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AI Onushchenko AA 1982 Quantum size effect in the optical spectra of semiconductor micro crystals Soviet Physics Semiconductors USSR 16 7 775 778 Ekimov AI Efros AL Onushchenko AA 1985 Quantum size effect in semiconductor microcrystals Solid State Communications 56 11 921 924 Bibcode 1985SSCom 56 921E doi 10 1016 S0038 1098 85 80025 9 Nanotechnology Timeline National Nanotechnology Initiative Kolobkova E V Nikonorov N V Aseev V A 2012 Optical Technologies Silver Nanoclusters Influence on Formation of Quantum Dots in Fluorine Phosphate Glasses Scientific and Technical Journal of Information Technologies Mechanics and Optics 5 12 Rossetti R Nakahara S Brus L E 15 July 1983 Quantum size effects in the redox potentials resonance Raman spectra and electronic spectra of CdS crystallites in aqueous solution The Journal of Chemical Physics 79 2 1086 1088 Bibcode 1983JChPh 79 1086R doi 10 1063 1 445834 ISSN 0021 9606 Brus L E 1 May 1984 Electron electron and electron hole interactions in small semiconductor crystallites The size dependence of the lowest excited electronic state The Journal of Chemical Physics 80 9 4403 4409 Bibcode 1984JChPh 80 4403B doi 10 1063 1 447218 ISSN 0021 9606 S2CID 54779723 superadmin History of Quantum Dots Nexdot Retrieved 8 October 2020 Further reading EditDelerue C amp Lannoo M 2004 Nanostructures Theory and Modelling Springer p 47 ISBN 978 3 540 20694 1 lt ref gt Methods to produce quantum confined semiconductor structures quantum wires wells and dots via grown by advanced epitaxial techniques nanocrystals by gas phase liquid phase and solid phase approaches Norris D J 1995 Measurement and Assignment of the Size Dependent Optical Spectrum in Cadmium Selenide CdSe Quantum Dots PhD thesis MIT hdl 1721 1 11129 Photoluminescence of a QD vs particle diameter External links EditQuantum Dots Technical Status and Market Prospects Quantum dots that produce white light could be the light bulb s successor Single quantum dots optical properties Quantum dot on arxiv org Quantum Dots Research and Technical Data Simulation and interactive visualization of Quantum Dots wave function Retrieved from https en wikipedia org w index php title Quantum dot amp oldid 1145010770, wikipedia, wiki, book, books, library,

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