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Attosecond physics

Attosecond physics, also known as attophysics, or more generally attosecond science, is a branch of physics that deals with light-matter interaction phenomena wherein attosecond (10−18 s) photon pulses are used to unravel dynamical processes in matter with unprecedented time resolution.

High harmonic generation in krypton. This technology is one of the most used techniques to generate attosecond bursts of light.

Attosecond science mainly employs pump–probe spectroscopic methods to investigate the physical process of interest. Due to the complexity of this field of study, it generally requires a synergistic interplay between state-of-the-art experimental setup and advanced theoretical tools to interpret the data collected from attosecond experiments.[1]

The main interests of attosecond physics are:

  1. Atomic physics: investigation of electron correlation effects, photo-emission delay and ionization tunneling.[2]
  2. Molecular physics and molecular chemistry: role of electronic motion in molecular excited states (e.g. charge-transfer processes), light-induced photo-fragmentation, and light-induced electron transfer processes.[3]
  3. Solid-state physics: investigation of exciton dynamics in advanced 2D materials, petahertz charge carrier motion in solids, spin dynamics in ferromagnetic materials.[4]

One of the primary goals of attosecond science is to provide advanced insights into the quantum dynamics of electrons in atoms, molecules and solids with the long-term challenge of achieving real-time control of the electron motion in matter.[5]

The advent of broadband solid-state titanium-doped sapphire based (Ti:Sa) lasers (1986),[6] chirped pulse amplification (CPA)[7] (1988), spectral broadening of high-energy pulses[8] (e.g. gas-filled hollow-core fiber via self-phase modulation) (1996), mirror-dispersion-controlled technology (chirped mirrors)[9] (1994), and carrier envelop offset stabilization[10] (2000) had enabled the creation of isolated-attosecond light pulses (generated by the non-linear process of high harmonic generation in a noble gas)[11][12] (2004, 2006), which have given birth to the field of attosecond science.[13]

The current world record for the shortest light-pulse generated by human technology is 43 as.[14]

In 2022, Anne L'Huillier, Paul Corkum, Ferenc Krausz were awarded with the Wolf prize in physics for their pioneering contributions to ultrafast laser science and attosecond physics. This was followed by the 2023 Nobel Prize in Physics, where L'Huillier, Krausz and Pierre Agostini were rewarded “for experimental methods that generate attosecond pulses of light for the study of electron dynamics in matter.”

Introduction edit

"Electron motion" in a hydrogen atom. The period of this states superposition (1s-2p) is around 400 as.

Motivation edit

The natural time scale of electron motion in atoms, molecules, and solids is the attosecond (1 as= 10−18 s). This fact is a direct consequence of quantum mechanics.

Indeed, for simplicity, consider a quantum particle in superposition between ground-level, of energy  , and the first excited level, of energy  :

 

with   and   chosen as the square roots of the quantum probability of observing the particle in the corresponding state.

 

are the time-dependent ground   and excited state   respectively, with   the reduced Planck constant.

The expectation value of a generic hermitian and symmetric operator,[15]  , can be written as  , as a consequence the time evolution of this observable is:

 

While the first two terms do not depend on time, the third, instead, does. This creates a dynamic for the observable   with a characteristic time,  , given by  .

 
Evolution of the angular probability density of the superposition between 1s and 2p state in hydrogen atoms. The color bar indicates the angular density (orientation of the wavepacket) as a function of the polar angle from 0 to π (x-axis), at which one can find the particle, and time (y-axis).

As a consequence, for energy levels in the range of   10 eV, which is the typical electronic energy range in matter,[5] the characteristic time of the dynamics of any associated physical observable is approximately 400 as.

To measure the time evolution of  , one needs to use a controlled tool, or a process, with an even shorter time-duration that can interact with that dynamic.

This is the reason why attosecond light pulses are used to disclose the physics of ultra-fast phenomena in the few-femtosecond and attosecond time-domain.[16]

Generation of attosecond pulses edit

To generate a traveling pulse with an ultrashort time duration, two key elements are needed: bandwidth and central wavelength of the electromagnetic wave.[17]

From Fourier analysis, the more the available spectral bandwidth of a light pulse, the shorter, potentially, is its time duration.

There is, however, a lower-limit in the minimum duration exploitable for a given pulse central wavelength. This limit is the optical cycle.[18]

Indeed, for a pulse centered in the low-frequency region, e.g. infrared (IR)  800 nm, its minimum time duration is around  2.67 fs, where   is the speed of light; whereas, for a light field with central wavelength in the extreme ultraviolet (XUV) at  30 nm the minimum duration is around  100 as.[18]

Thus, a smaller time duration requires the use of shorter, and more energetic wavelength, even down to the soft-X-ray (SXR) region.

For this reason, standard techniques to create attosecond light pulses are based on radiation sources with broad spectral bandwidths and central wavelength located in the XUV-SXR range.[19]

The most common sources that fit these requirements are free-electron lasers (FEL) and high harmonic generation (HHG) setups.

Physical observables and experiments edit

Once an attosecond light source is available, one has to drive the pulse towards the sample of interest and, then, measure its dynamics.

The most suitable experimental observables to analyze the electron dynamics in matter are:

Pump-probe techniques are used to image ultra-fast processes occurring in matter.

The general strategy is to use a pump-probe scheme to "image" through one of the aforementioned observables the ultra-fast dynamics occurring in the material under investigation.[1]

Few-femtosecond IR-XUV/SXR attosecond pulse pump-probe experiments edit

As an example, in a typical pump-probe experimental apparatus, an attosecond (XUV-SXR) pulse and an intense (  W/cm2) low-frequency infrared pulse with a time duration of few to tens femtoseconds are collinearly focused on the studied sample.

At this point, by varying the delay of the attosecond pulse, which could be pump/probe depending on the experiment, with respect to the IR pulse (probe/pump), the desired physical observable is recorded.[24]

The subsequent challenge is to interpret the collected data and retrieve fundamental information on the hidden dynamics and quantum processes occurring in the sample. This can be achieved with advanced theoretical tools and numerical calculations.[25][26]

By exploiting this experimental scheme, several kinds of dynamics can be explored in atoms, molecules and solids; typically light-induced dynamics and out-of-equilibrium excited states within attosecond time-resolution.[20][21][23]

Quantum mechanics foundations edit

Attosecond physics typically deals with non-relativistic bounded particles and employs electromagnetic fields with a moderately high intensity (  W/cm2).[27]

This fact allows to set up a discussion in a non-relativistic and semi-classical quantum mechanics environment for light-matter interaction.

Atoms edit

Resolution of time dependent Schrödinger equation in an electromagnetic field edit

The time evolution of a single electronic wave function in an atom,   is described by the Schrödinger equation (in atomic units):

 

where the light-matter interaction Hamiltonian,  , can be expressed in the length gauge, within the dipole approximation, as:[28][29]

 

where   is the Coulomb potential of the atomic species considered;   are the momentum and position operator, respectively; and   is the total electric field evaluated in the neighbor of the atom.

The formal solution of the Schrödinger equation is given by the propagator formalism:

 

where  , is the electron wave function at time  .

This exact solution cannot be used for almost any practical purpose.

However, it can be proved, using Dyson's equations[30][31] that the previous solution can also be written as:

 

where,

 

is the bounded Hamiltonian and

 

is the interaction Hamiltonian.

The formal solution of Eq.  , which previously was simply written as Eq.  , can now be regarded in Eq.   as a superposition of different quantum paths (or quantum trajectory), each one of them with a peculiar interaction time   with the electric field.

In other words, each quantum path is characterized by three steps:

  1. An initial evolution without the electromagnetic field. This is described by the left-hand side   term in the integral.
  2. Then, a "kick" from the electromagnetic field,   that "excite" the electron. This event occurs at an arbitrary time that uni-vocally characterizes the quantum path  .
  3. A final evolution driven by both the field and the Coulomb potential, given by  .

In parallel, you also have a quantum path that do not perceive the field at all, this trajectory is indicated by the right-hand side term in Eq.  .

This process is entirely time-reversible, i.e. can also occur in the opposite order.[30]

Equation   is not straightforward to handle. However, physicists use it as the starting point for numerical calculation, more advanced discussion or several approximations.[31][32]

For strong-field interaction problems, where ionization may occur, one can imagine to project Eq.   in a certain continuum state (unbounded state or free state)  , of momentum  , so that:

 

where  is the probability amplitude to find at a certain time  , the electron in the continuum states  .

If this probability amplitude is greater than zero, the electron is photoionized.

For the majority of application, the second term in   is not considered, and only the first one is used in discussions,[31] hence:

 

Equation   is also known as time reversed S-matrix amplitude[31] and it gives the probability of photoionization by a generic time-varying electric field.

Strong field approximation (SFA) edit

Strong field approximation (SFA), or Keldysh-Faisal-Reiss theory is a physical model, started in 1964 by the Russian physicist Keldysh,[33] is currently used to describe the behavior of atoms (and molecules) in intense laser fields.

SFA is the starting theory for discussing both high harmonic generation and attosecond pump-probe interaction with atoms.

The main assumption made in SFA is that the free-electron dynamics is dominated by the laser field, while the Coulomb potential is regarded as a negligible perturbation.[34]

This fact re-shapes equation   into:

 

where,   is the Volkov Hamiltonian, here expressed for simplicity in the velocity gauge,[35] with  ,  , the electromagnetic vector potential.[36]

At this point, to keep the discussion at its basic level, lets consider an atom with a single energy level  , ionization energy   and populated by a single electron (single active electron approximation).

We can consider the initial time of the wave function dynamics as  , and we can assume that initially the electron is in the atomic ground state  .

So that,

  and  

Moreover, we can regard the continuum states as plane-wave functions state,  .

This is a rather simplified assumption, a more reasonable choice would have been to use as continuum state the exact atom scattering states.[37]

The time evolution of simple plane-wave states with the Volkov Hamiltonian is given by:

 

here for consistency with Eq.   the evolution has already been properly converted into the length gauge.[38]

As a consequence, the final momentum distribution of a single electron in a single-level atom, with ionization potential  , is expressed as:

 

where,

 

is the dipole expectation value (or transition dipole moment), and

 

is the semiclassical action.

The result of Eq.   is the basic tool to understand phenomena like:

  • The high harmonic generation process,[39] which is typically the result of strong field interaction of noble gases with an intense low-frequency pulse,
  • Attosecond pump-probe experiments with simple atoms.[40]
  • The debate on tunneling time.[41][42]
Weak attosecond pulse-strong-IR-fields-atoms interactions edit

Attosecond pump-probe experiments with simple atoms is a fundamental tool to measure the time duration of an attosecond pulse[43] and to explore several quantum proprieties of matter.[40]

 
Scheme of a strong IR field and a delayed attosecond XUV pulse interacting with a single electron in a single-level atom. The XUV can ionize the electron, which "jumps" in the continuum by direct ionization (blue path in the figure). The IR pulse, later, "streaks" up and down in energy the photo-electron. After the interaction, the electron has final energy which can be subsequently detected and measured (e.g. time-of-flight apparatus). The multi-photon ionization process (red path in the figure) is also possible, but, since it is relevant in different energetic region, it can be disregarded.

This kind of experiments can be easily described within strong field approximation by exploiting the results of Eq.  , as discussed below.

As a simple model, consider the interaction between a single active electron in a single-level atom and two fields: an intense femtosecond infrared (IR) pulse ( ,

and a weak attosecond pulse (centered in the extreme ultraviolet (XUV) region)  .

Then, by substituting these fields to   it results

 

with

 .

At this point, we can divide Eq.   in two contributions: direct ionization and strong field ionization (multiphoton regime), respectively.

Typically, these two terms are relevant in different energetic regions of the continuum.

Consequently, for typical experimental condition, the latter process is disregarded, and only direct ionization from the attosecond pulse is considered.[31]

Then, since the attosecond pulse is weaker than the infrared one, it holds  . Thus,   is typically neglected in Eq.  .

In addition to that, we can re-write the attosecond pulse as a delayed function with respect to the IR field,  .

Therefore, the probability distribution,  , of finding an electron ionized in the continuum with momentum  , after the interaction has occurred (at  ), in a pump-probe experiments,

with an intense IR pulse and a delayed-attosecond XUV pulse, is given by:

 

with

 

Equation   describes the photoionization phenomenon of two-color interaction (XUV-IR) with a single-level atom and single active electron.

This peculiar result can be regarded as a quantum interference process between all the possible ionization paths, started by a delayed XUV attosecond pulse, with a following motion in the continuum states driven by a strong IR field.[31]

The resulting 2D photo-electron (momentum, or equivalently energy, vs delay) distribution is called streaking trace.[44]

Techniques edit

Here are listed and discussed some of the most common techniques and approaches pursued in attosecond research centers.

Metrology with photo-electron spectroscopy (FROG-CRAB) edit

 
Simulation of a streaking trace in Neon. The attosecond pulse duration is 350 as, with central wavelength at the 33 harmonics of an 800 nm laser. The 800 nm pulse, which has the role of streaking up and down the photoelectron trace, has a duration of 7 fs with a peak intensity of 5 TW/cm2.[45]

A daily challenge in attosecond science is to characterize the temporal proprieties of the attosecond pulses used in any pump-probe experiments with atoms, molecules or solids.

The most used technique is based on the frequency-resolved optical gating for a complete reconstruction of attosecond bursts (FROG-CRAB).[43]

The main advantage of this technique is that it allows to exploit the corroborated frequency-resolved optical gating (FROG) technique,[46] developed in 1991 for picosecond-femtosecond pulse characterization, to the attosecond field.

Complete reconstruction of attosecond bursts (CRAB) is an extension of FROG and it is based on the same idea for the field reconstruction.

In other words, FROG-CRAB is based on the conversion of an attosecond pulse into an electron wave-packet that is freed in the continuum by atomic photoionization, as already described with Eq. .

The role of the low-frequency driving laser pulse( e.g. infra-red pulse) is to behave as gate for the temporal measurement.

Then, by exploring different delays between the low-frequency and the attosecond pulse a streaking trace (or streaking spectrogram) can be obtained.[44]

This 2D-spectrogram is later analyzed by a reconstruction algorithm with the goal of retrieving both the attosecond pulse and the IR pulse, with no need of a prior knowledge on any of them.

However, as Eq.   pinpoints, the intrinsic limits of this technique is the knowledge on atomic dipole proprieties, in particular on the atomic dipole quantum phase.[40][47]

The reconstruction of both the low-frequency field and the attosecond pulse from a streaking trace is typically achieved through iterative algorithms, such as:

  • Principal component generalized projections algorithm (PCGPA).[48]
  • Volkov transform generalized projection algorithm (VTGPA).[49]
  • extended ptychographic iterative engine (ePIE).[50]

See also edit

References edit

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  46. ^ Trebino R (2003). "FROG". Frequency-Resolved Optical Gating: The Measurement of Ultrashort Laser Pulses. Boston, MA: Springer US. pp. 101–115. doi:10.1007/978-1-4615-1181-6_5. ISBN 978-1-4613-5432-1.
  47. ^ Zhao X, Wei H, Wei C, Lin CD (2017-10-23). "A new method for accurate retrieval of atomic dipole phase or photoionization group delay in attosecond photoelectron streaking experiments". Journal of Optics. 19 (11): 114009. Bibcode:2017JOpt...19k4009Z. doi:10.1088/2040-8986/aa8fb6. ISSN 2040-8978. S2CID 125209544.
  48. ^ Kane DJ (2008-06-01). "Principal components generalized projections: a review [Invited]". JOSA B. 25 (6): A120–A132. Bibcode:2008JOSAB..25A.120K. doi:10.1364/JOSAB.25.00A120. ISSN 1520-8540.
  49. ^ Keathley PD, Bhardwaj S, Moses J, Laurent G, Kaertner FX (2016-07-06). "Volkov transform generalized projection algorithm for attosecond pulse characterization". New Journal of Physics. 18 (7): 073009. Bibcode:2016NJPh...18g3009K. doi:10.1088/1367-2630/18/7/073009. hdl:1721.1/105139. ISSN 1367-2630. S2CID 53077495.
  50. ^ Lucchini M, Brügmann MH, Ludwig A, Gallmann L, Keller U, Feurer T (November 2015). "Ptychographic reconstruction of attosecond pulses". Optics Express. 23 (23): 29502–13. arXiv:1508.07714. Bibcode:2015OExpr..2329502L. doi:10.1364/OE.23.029502. PMID 26698434. S2CID 33845261.

Further reading edit

  • Bucksbaum PH (February 2003). "Attophysics: Ultrafast control". Nature. 421 (6923): 593–4. Bibcode:2003Natur.421..593B. doi:10.1038/421593a. hdl:2027.42/62570. PMID 12571581. S2CID 12268311.
  • Cerullo G, Nisoli M (March 2019). "Ultrafast lasers: from femtoseconds to attoseconds". Europhysics News. 50 (2): 11–4. Bibcode:2019ENews..50b..11C. doi:10.1051/epn/2019201. S2CID 132721942.
  • Kennedy S, Burdick A (June 2003). "Stopping Time: What can you do in a billionth of a billionth of a second?".
  • Nisoli M (July 2019). "The Birth of Attochemistry". Optics and Photonics News. 30 (7): 32–9. Bibcode:2019OptPN..30...32N. doi:10.1364/OPN.30.7.000032. S2CID 198445481.

attosecond, physics, also, known, attophysics, more, generally, attosecond, science, branch, physics, that, deals, with, light, matter, interaction, phenomena, wherein, attosecond, photon, pulses, used, unravel, dynamical, processes, matter, with, unprecedente. Attosecond physics also known as attophysics or more generally attosecond science is a branch of physics that deals with light matter interaction phenomena wherein attosecond 10 18 s photon pulses are used to unravel dynamical processes in matter with unprecedented time resolution High harmonic generation in krypton This technology is one of the most used techniques to generate attosecond bursts of light Attosecond science mainly employs pump probe spectroscopic methods to investigate the physical process of interest Due to the complexity of this field of study it generally requires a synergistic interplay between state of the art experimental setup and advanced theoretical tools to interpret the data collected from attosecond experiments 1 The main interests of attosecond physics are Atomic physics investigation of electron correlation effects photo emission delay and ionization tunneling 2 Molecular physics and molecular chemistry role of electronic motion in molecular excited states e g charge transfer processes light induced photo fragmentation and light induced electron transfer processes 3 Solid state physics investigation of exciton dynamics in advanced 2D materials petahertz charge carrier motion in solids spin dynamics in ferromagnetic materials 4 One of the primary goals of attosecond science is to provide advanced insights into the quantum dynamics of electrons in atoms molecules and solids with the long term challenge of achieving real time control of the electron motion in matter 5 The advent of broadband solid state titanium doped sapphire based Ti Sa lasers 1986 6 chirped pulse amplification CPA 7 1988 spectral broadening of high energy pulses 8 e g gas filled hollow core fiber via self phase modulation 1996 mirror dispersion controlled technology chirped mirrors 9 1994 and carrier envelop offset stabilization 10 2000 had enabled the creation of isolated attosecond light pulses generated by the non linear process of high harmonic generation in a noble gas 11 12 2004 2006 which have given birth to the field of attosecond science 13 The current world record for the shortest light pulse generated by human technology is 43 as 14 In 2022 Anne L Huillier Paul Corkum Ferenc Krausz were awarded with the Wolf prize in physics for their pioneering contributions to ultrafast laser science and attosecond physics This was followed by the 2023 Nobel Prize in Physics where L Huillier Krausz and Pierre Agostini were rewarded for experimental methods that generate attosecond pulses of light for the study of electron dynamics in matter Contents 1 Introduction 1 1 Motivation 1 2 Generation of attosecond pulses 1 3 Physical observables and experiments 1 3 1 Few femtosecond IR XUV SXR attosecond pulse pump probe experiments 2 Quantum mechanics foundations 2 1 Atoms 2 1 1 Resolution of time dependent Schrodinger equation in an electromagnetic field 2 1 2 Strong field approximation SFA 2 1 2 1 Weak attosecond pulse strong IR fields atoms interactions 3 Techniques 3 1 Metrology with photo electron spectroscopy FROG CRAB 4 See also 5 References 6 Further readingIntroduction edit source source source source source source Electron motion in a hydrogen atom The period of this states superposition 1s 2p is around 400 as Motivation edit The natural time scale of electron motion in atoms molecules and solids is the attosecond 1 as 10 18 s This fact is a direct consequence of quantum mechanics Indeed for simplicity consider a quantum particle in superposition between ground level of energy ϵ 0 displaystyle epsilon 0 nbsp and the first excited level of energy ϵ 1 displaystyle epsilon 1 nbsp PS c g ps g c e ps e displaystyle Psi rangle c g psi g rangle c e psi e rangle nbsp with c e displaystyle c e nbsp and c g displaystyle c g nbsp chosen as the square roots of the quantum probability of observing the particle in the corresponding state ps g t 0 e i ϵ 0 ℏ t ps e t 1 e i ϵ 1 ℏ t displaystyle psi g t rangle 0 rangle e frac i epsilon 0 hbar t qquad psi e t rangle 1 rangle e frac i epsilon 1 hbar t nbsp are the time dependent ground 0 displaystyle 0 rangle nbsp and excited state 1 displaystyle 1 rangle nbsp respectively with ℏ displaystyle hbar nbsp the reduced Planck constant The expectation value of a generic hermitian and symmetric operator 15 P displaystyle hat P nbsp can be written as P t PS P PS displaystyle P t langle Psi hat P Psi rangle nbsp as a consequence the time evolution of this observable is P t c g 2 0 P 0 c e 2 1 P 1 2 c e c g 0 P 1 cos ϵ 1 ϵ 0 ℏ t displaystyle P t c g 2 langle 0 hat P 0 rangle c e 2 langle 1 hat P 1 rangle 2c e c g langle 0 hat P 1 rangle cos left frac epsilon 1 epsilon 0 hbar t right nbsp While the first two terms do not depend on time the third instead does This creates a dynamic for the observable P t displaystyle P t nbsp with a characteristic time T c displaystyle T c nbsp given by T c 2 p ℏ ϵ 1 ϵ 0 displaystyle T c frac 2 pi hbar epsilon 1 epsilon 0 nbsp nbsp Evolution of the angular probability density of the superposition between 1s and 2p state in hydrogen atoms The color bar indicates the angular density orientation of the wavepacket as a function of the polar angle from 0 to p x axis at which one can find the particle and time y axis As a consequence for energy levels in the range of ϵ 1 ϵ 0 displaystyle epsilon 1 epsilon 0 approx nbsp 10 eV which is the typical electronic energy range in matter 5 the characteristic time of the dynamics of any associated physical observable is approximately 400 as To measure the time evolution of P t displaystyle P t nbsp one needs to use a controlled tool or a process with an even shorter time duration that can interact with that dynamic This is the reason why attosecond light pulses are used to disclose the physics of ultra fast phenomena in the few femtosecond and attosecond time domain 16 Generation of attosecond pulses edit To generate a traveling pulse with an ultrashort time duration two key elements are needed bandwidth and central wavelength of the electromagnetic wave 17 From Fourier analysis the more the available spectral bandwidth of a light pulse the shorter potentially is its time duration There is however a lower limit in the minimum duration exploitable for a given pulse central wavelength This limit is the optical cycle 18 Indeed for a pulse centered in the low frequency region e g infrared IR l displaystyle lambda nbsp 800 nm its minimum time duration is around t p u l s e l c displaystyle t pulse frac lambda c nbsp 2 67 fs where c displaystyle c nbsp is the speed of light whereas for a light field with central wavelength in the extreme ultraviolet XUV at l displaystyle lambda nbsp 30 nm the minimum duration is around t p u l s e displaystyle t rm pulse nbsp 100 as 18 Thus a smaller time duration requires the use of shorter and more energetic wavelength even down to the soft X ray SXR region For this reason standard techniques to create attosecond light pulses are based on radiation sources with broad spectral bandwidths and central wavelength located in the XUV SXR range 19 The most common sources that fit these requirements are free electron lasers FEL and high harmonic generation HHG setups Physical observables and experiments edit Once an attosecond light source is available one has to drive the pulse towards the sample of interest and then measure its dynamics The most suitable experimental observables to analyze the electron dynamics in matter are Angular asymmetry in the velocity distribution of molecular photo fragment 20 Quantum yield of molecular photo fragments 21 XUV SXR spectrum transient absorption 22 XUV SXR spectrum transient reflectivity 23 Photo electron kinetic energy distribution 2 source source source source source source source source Pump probe techniques are used to image ultra fast processes occurring in matter The general strategy is to use a pump probe scheme to image through one of the aforementioned observables the ultra fast dynamics occurring in the material under investigation 1 Few femtosecond IR XUV SXR attosecond pulse pump probe experiments edit As an example in a typical pump probe experimental apparatus an attosecond XUV SXR pulse and an intense 10 11 10 14 displaystyle 10 11 10 14 nbsp W cm2 low frequency infrared pulse with a time duration of few to tens femtoseconds are collinearly focused on the studied sample At this point by varying the delay of the attosecond pulse which could be pump probe depending on the experiment with respect to the IR pulse probe pump the desired physical observable is recorded 24 The subsequent challenge is to interpret the collected data and retrieve fundamental information on the hidden dynamics and quantum processes occurring in the sample This can be achieved with advanced theoretical tools and numerical calculations 25 26 By exploiting this experimental scheme several kinds of dynamics can be explored in atoms molecules and solids typically light induced dynamics and out of equilibrium excited states within attosecond time resolution 20 21 23 Quantum mechanics foundations editAttosecond physics typically deals with non relativistic bounded particles and employs electromagnetic fields with a moderately high intensity 10 11 10 14 displaystyle 10 11 10 14 nbsp W cm2 27 This fact allows to set up a discussion in a non relativistic and semi classical quantum mechanics environment for light matter interaction Atoms edit Resolution of time dependent Schrodinger equation in an electromagnetic field edit The time evolution of a single electronic wave function in an atom ps t displaystyle psi t rangle nbsp is described by the Schrodinger equation in atomic units H ps t i t ps t 1 0 displaystyle hat H psi t rangle i dfrac partial partial t psi t rangle quad 1 0 nbsp where the light matter interaction Hamiltonian H displaystyle hat H nbsp can be expressed in the length gauge within the dipole approximation as 28 29 H 1 2 p 2 V C r E t displaystyle hat H frac 1 2 hat textbf p 2 V C hat textbf r cdot textbf E t nbsp where V C displaystyle V C nbsp is the Coulomb potential of the atomic species considered p r displaystyle hat textbf p hat textbf r nbsp are the momentum and position operator respectively and E t displaystyle textbf E t nbsp is the total electric field evaluated in the neighbor of the atom The formal solution of the Schrodinger equation is given by the propagator formalism ps t e i t 0 t H d t ps t 0 1 1 displaystyle psi t rangle e i int t 0 t hat H dt psi t 0 rangle qquad 1 1 nbsp where ps t 0 displaystyle psi t 0 rangle nbsp is the electron wave function at time t t 0 displaystyle t t 0 nbsp This exact solution cannot be used for almost any practical purpose However it can be proved using Dyson s equations 30 31 that the previous solution can also be written as ps t i t 0 t d t e i t t H t d t H I t e i t 0 t H 0 t d t ps t 0 e i t 0 t H 0 t d t ps t 0 1 2 displaystyle psi t rangle i int t 0 t dt Big e i int t t hat H t dt hat H I t e i int t 0 t hat H 0 t dt psi t 0 rangle Big e i int t 0 t hat H 0 t dt psi t 0 rangle qquad 1 2 nbsp where H 0 1 2 p 2 V C displaystyle hat H 0 frac 1 2 hat textbf p 2 V C nbsp is the bounded Hamiltonian and H I r E t displaystyle hat H I hat textbf r cdot textbf E t nbsp is the interaction Hamiltonian The formal solution of Eq 1 0 displaystyle 1 0 nbsp which previously was simply written as Eq 1 1 displaystyle 1 1 nbsp can now be regarded in Eq 1 2 displaystyle 1 2 nbsp as a superposition of different quantum paths or quantum trajectory each one of them with a peculiar interaction time t displaystyle t nbsp with the electric field In other words each quantum path is characterized by three steps An initial evolution without the electromagnetic field This is described by the left hand side H 0 displaystyle hat H 0 nbsp term in the integral Then a kick from the electromagnetic field H I t displaystyle hat H I t nbsp that excite the electron This event occurs at an arbitrary time that uni vocally characterizes the quantum path t displaystyle t nbsp A final evolution driven by both the field and the Coulomb potential given by H displaystyle hat H nbsp In parallel you also have a quantum path that do not perceive the field at all this trajectory is indicated by the right hand side term in Eq 1 2 displaystyle 1 2 nbsp This process is entirely time reversible i e can also occur in the opposite order 30 Equation 1 2 displaystyle 1 2 nbsp is not straightforward to handle However physicists use it as the starting point for numerical calculation more advanced discussion or several approximations 31 32 For strong field interaction problems where ionization may occur one can imagine to project Eq 1 2 displaystyle 1 2 nbsp in a certain continuum state unbounded state or free state p displaystyle textbf p rangle nbsp of momentum p displaystyle textbf p nbsp so that c p t p ps t i t 0 t d t p e i t t H t d t H I t e i t 0 t H 0 t d t ps t 0 p e i t 0 t H 0 t d t ps t 0 1 3 displaystyle c textbf p t langle textbf p psi t rangle i int t 0 t dt langle textbf p e i int t t hat H t dt hat H I t e i int t 0 t hat H 0 t dt psi t 0 rangle langle textbf p e i int t 0 t hat H 0 t dt psi t 0 rangle quad 1 3 nbsp where c p t 2 displaystyle c textbf p t 2 nbsp is the probability amplitude to find at a certain time t displaystyle t nbsp the electron in the continuum states p displaystyle textbf p rangle nbsp If this probability amplitude is greater than zero the electron is photoionized For the majority of application the second term in 1 3 displaystyle 1 3 nbsp is not considered and only the first one is used in discussions 31 hence a p t i t 0 t d t p e i t t H t d t H I t e i t 0 t H 0 t d t ps t 0 1 4 displaystyle a textbf p t i int t 0 t dt langle textbf p e i int t t hat H t dt hat H I t e i int t 0 t hat H 0 t dt psi t 0 rangle quad 1 4 nbsp Equation 1 4 displaystyle 1 4 nbsp is also known as time reversed S matrix amplitude 31 and it gives the probability of photoionization by a generic time varying electric field Strong field approximation SFA edit Strong field approximation SFA or Keldysh Faisal Reiss theory is a physical model started in 1964 by the Russian physicist Keldysh 33 is currently used to describe the behavior of atoms and molecules in intense laser fields SFA is the starting theory for discussing both high harmonic generation and attosecond pump probe interaction with atoms The main assumption made in SFA is that the free electron dynamics is dominated by the laser field while the Coulomb potential is regarded as a negligible perturbation 34 This fact re shapes equation 1 4 displaystyle 1 4 nbsp into a p S F A t i t 0 t d t p e i t t H V t d t H I t e i t 0 t H 0 t d t ps t 0 1 4 displaystyle a textbf p SFA t i int t 0 t dt langle textbf p e i int t t hat H V t dt hat H I t e i int t 0 t hat H 0 t dt psi t 0 rangle quad 1 4 nbsp where H V 1 2 p A t 2 displaystyle hat H V frac 1 2 hat textbf p textbf A t 2 nbsp is the Volkov Hamiltonian here expressed for simplicity in the velocity gauge 35 with A t displaystyle textbf A t nbsp E t A t t displaystyle textbf E t frac partial textbf A t partial t nbsp the electromagnetic vector potential 36 At this point to keep the discussion at its basic level lets consider an atom with a single energy level 0 displaystyle 0 rangle nbsp ionization energy I P displaystyle I P nbsp and populated by a single electron single active electron approximation We can consider the initial time of the wave function dynamics as t 0 displaystyle t 0 infty nbsp and we can assume that initially the electron is in the atomic ground state 0 displaystyle 0 rangle nbsp So that H 0 0 I P 0 displaystyle hat H 0 0 rangle I P 0 rangle nbsp and ps t e i t H 0 d t 0 e I P t 0 displaystyle psi t rangle e i int infty t hat H 0 dt 0 rangle e I P t 0 rangle nbsp Moreover we can regard the continuum states as plane wave functions state r p 2 p 3 2 e i p r displaystyle langle textbf r textbf p rangle 2 pi frac 3 2 e i textbf p cdot textbf r nbsp This is a rather simplified assumption a more reasonable choice would have been to use as continuum state the exact atom scattering states 37 The time evolution of simple plane wave states with the Volkov Hamiltonian is given by p e i t t H V t d t p A t e i t t p A t 2 d t displaystyle langle textbf p e i int t t hat H V t dt langle textbf p textbf A t e i int t t textbf p textbf A t 2 dt nbsp here for consistency with Eq 1 4 displaystyle 1 4 nbsp the evolution has already been properly converted into the length gauge 38 As a consequence the final momentum distribution of a single electron in a single level atom with ionization potential I P displaystyle I P nbsp is expressed as a p t S F A i t E t d p A t e i I P t S t t d t 1 5 displaystyle a textbf p t SFA i int infty t textbf E t cdot textbf d textbf p textbf A t e i I P t S t t dt quad 1 5 nbsp where d p A t p A t r 0 displaystyle textbf d textbf p textbf A t langle textbf p textbf A t hat textbf r 0 rangle nbsp is the dipole expectation value or transition dipole moment and S t t t t 1 2 p A t 2 d t displaystyle S t t int t t frac 1 2 textbf p textbf A t 2 dt nbsp is the semiclassical action The result of Eq 1 5 displaystyle 1 5 nbsp is the basic tool to understand phenomena like The high harmonic generation process 39 which is typically the result of strong field interaction of noble gases with an intense low frequency pulse Attosecond pump probe experiments with simple atoms 40 The debate on tunneling time 41 42 Weak attosecond pulse strong IR fields atoms interactions editAttosecond pump probe experiments with simple atoms is a fundamental tool to measure the time duration of an attosecond pulse 43 and to explore several quantum proprieties of matter 40 nbsp Scheme of a strong IR field and a delayed attosecond XUV pulse interacting with a single electron in a single level atom The XUV can ionize the electron which jumps in the continuum by direct ionization blue path in the figure The IR pulse later streaks up and down in energy the photo electron After the interaction the electron has final energy which can be subsequently detected and measured e g time of flight apparatus The multi photon ionization process red path in the figure is also possible but since it is relevant in different energetic region it can be disregarded This kind of experiments can be easily described within strong field approximation by exploiting the results of Eq 1 5 displaystyle 1 5 nbsp as discussed below As a simple model consider the interaction between a single active electron in a single level atom and two fields an intense femtosecond infrared IR pulse E I R t A I R t displaystyle textbf E IR t textbf A IR t nbsp and a weak attosecond pulse centered in the extreme ultraviolet XUV region E X U V t A X U V t displaystyle textbf E XUV t textbf A XUV t nbsp Then by substituting these fields to 1 5 displaystyle 1 5 nbsp it results a p t i t E X U V t E I R t d p A X U V t A I R t e i I P t S t t d t 1 6 displaystyle a textbf p t i int infty t textbf E XUV t textbf E IR t cdot textbf d textbf p textbf A XUV t textbf A IR t e i I P t S t t dt quad 1 6 nbsp with S t t t t 1 2 p A I R t A X U V t 2 d t displaystyle S t t int t t frac 1 2 textbf p textbf A IR t textbf A XUV t 2 dt nbsp At this point we can divide Eq 1 6 displaystyle 1 6 nbsp in two contributions direct ionization and strong field ionization multiphoton regime respectively Typically these two terms are relevant in different energetic regions of the continuum Consequently for typical experimental condition the latter process is disregarded and only direct ionization from the attosecond pulse is considered 31 Then since the attosecond pulse is weaker than the infrared one it holds A I R t gt gt A X U V t displaystyle textbf A IR t gt gt textbf A XUV t nbsp Thus A X U V t displaystyle textbf A XUV t nbsp is typically neglected in Eq 1 6 displaystyle 1 6 nbsp In addition to that we can re write the attosecond pulse as a delayed function with respect to the IR field A I R t E X U V t t displaystyle textbf A IR t textbf E XUV t tau nbsp Therefore the probability distribution a p t 2 displaystyle a textbf p tau 2 nbsp of finding an electron ionized in the continuum with momentum p displaystyle textbf p nbsp after the interaction has occurred at t displaystyle t infty nbsp in a pump probe experiments with an intense IR pulse and a delayed attosecond XUV pulse is given by a p t i E X U V t t d p A I R t e i I P t S t d t 1 7 displaystyle a textbf p tau i int infty infty textbf E XUV t tau cdot textbf d textbf p textbf A IR t e i I P t S t dt quad 1 7 nbsp with S t 1 2 p 2 t t p A I R t 1 2 A I R t 2 d t displaystyle S t frac 1 2 textbf p 2 t int t infty textbf p cdot textbf A IR t frac 1 2 textbf A IR t 2 dt nbsp Equation 1 7 displaystyle 1 7 nbsp describes the photoionization phenomenon of two color interaction XUV IR with a single level atom and single active electron This peculiar result can be regarded as a quantum interference process between all the possible ionization paths started by a delayed XUV attosecond pulse with a following motion in the continuum states driven by a strong IR field 31 The resulting 2D photo electron momentum or equivalently energy vs delay distribution is called streaking trace 44 Techniques editHere are listed and discussed some of the most common techniques and approaches pursued in attosecond research centers Metrology with photo electron spectroscopy FROG CRAB edit nbsp Simulation of a streaking trace in Neon The attosecond pulse duration is 350 as with central wavelength at the 33 harmonics of an 800 nm laser The 800 nm pulse which has the role of streaking up and down the photoelectron trace has a duration of 7 fs with a peak intensity of 5 TW cm2 45 A daily challenge in attosecond science is to characterize the temporal proprieties of the attosecond pulses used in any pump probe experiments with atoms molecules or solids The most used technique is based on the frequency resolved optical gating for a complete reconstruction of attosecond bursts FROG CRAB 43 The main advantage of this technique is that it allows to exploit the corroborated frequency resolved optical gating FROG technique 46 developed in 1991 for picosecond femtosecond pulse characterization to the attosecond field Complete reconstruction of attosecond bursts CRAB is an extension of FROG and it is based on the same idea for the field reconstruction In other words FROG CRAB is based on the conversion of an attosecond pulse into an electron wave packet that is freed in the continuum by atomic photoionization as already described with Eq 1 7 displaystyle 1 7 nbsp The role of the low frequency driving laser pulse e g infra red pulse is to behave as gate for the temporal measurement Then by exploring different delays between the low frequency and the attosecond pulse a streaking trace or streaking spectrogram can be obtained 44 This 2D spectrogram is later analyzed by a reconstruction algorithm with the goal of retrieving both the attosecond pulse and the IR pulse with no need of a prior knowledge on any of them However as Eq 1 7 displaystyle 1 7 nbsp pinpoints the intrinsic limits of this technique is the knowledge on atomic dipole proprieties in particular on the atomic dipole quantum phase 40 47 The reconstruction of both the low frequency field and the attosecond pulse from a streaking trace is typically achieved through iterative algorithms such as Principal component generalized projections algorithm PCGPA 48 Volkov transform generalized projection algorithm VTGPA 49 extended ptychographic iterative engine ePIE 50 See also editFemtochemistry Femtotechnology Ultrashort pulse Chirped pulse amplification Free electron laser Attosecond chronoscopyReferences edit a b Krausz F Ivanov M February 2009 Attosecond physics Reviews of Modern Physics 81 1 163 234 Bibcode 2009RvMP 81 163K doi 10 1103 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4613 5432 1 Zhao X Wei H Wei C Lin CD 2017 10 23 A new method for accurate retrieval of atomic dipole phase or photoionization group delay in attosecond photoelectron streaking experiments Journal of Optics 19 11 114009 Bibcode 2017JOpt 19k4009Z doi 10 1088 2040 8986 aa8fb6 ISSN 2040 8978 S2CID 125209544 Kane DJ 2008 06 01 Principal components generalized projections a review Invited JOSA B 25 6 A120 A132 Bibcode 2008JOSAB 25A 120K doi 10 1364 JOSAB 25 00A120 ISSN 1520 8540 Keathley PD Bhardwaj S Moses J Laurent G Kaertner FX 2016 07 06 Volkov transform generalized projection algorithm for attosecond pulse characterization New Journal of Physics 18 7 073009 Bibcode 2016NJPh 18g3009K doi 10 1088 1367 2630 18 7 073009 hdl 1721 1 105139 ISSN 1367 2630 S2CID 53077495 Lucchini M Brugmann MH Ludwig A Gallmann L Keller U Feurer T November 2015 Ptychographic reconstruction of attosecond pulses Optics Express 23 23 29502 13 arXiv 1508 07714 Bibcode 2015OExpr 2329502L doi 10 1364 OE 23 029502 PMID 26698434 S2CID 33845261 Further reading editBucksbaum PH February 2003 Attophysics Ultrafast control Nature 421 6923 593 4 Bibcode 2003Natur 421 593B doi 10 1038 421593a hdl 2027 42 62570 PMID 12571581 S2CID 12268311 Cerullo G Nisoli M March 2019 Ultrafast lasers from femtoseconds to attoseconds Europhysics News 50 2 11 4 Bibcode 2019ENews 50b 11C doi 10 1051 epn 2019201 S2CID 132721942 Kennedy S Burdick A June 2003 Stopping Time What can you do in a billionth of a billionth of a second Nisoli M July 2019 The Birth of Attochemistry Optics and Photonics News 30 7 32 9 Bibcode 2019OptPN 30 32N doi 10 1364 OPN 30 7 000032 S2CID 198445481 Retrieved from https en wikipedia org w index php title Attosecond physics amp oldid 1183996081, wikipedia, wiki, book, books, library,

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