Nuclear isomer

A nuclear isomer is a metastable state of an atomic nucleus, in which one or more nucleons (protons or neutrons) occupy excited state (higher energy) levels. "Metastable" describes nuclei whose excited states have half-lives 100 to 1000 times longer than the half-lives of the excited nuclear states that decay with a "prompt" half life (ordinarily on the order of 10⁻¹² seconds). The term "metastable" is usually restricted to isomers with half-lives of 10⁻⁹ seconds or longer. Some references recommend 5 × 10⁻⁹ seconds to distinguish the metastable half life from the normal "prompt" gamma-emission half-life.^[1] Occasionally the half-lives are far longer than this and can last minutes, hours, or years. For example, the ^180m
₇₃Ta
nuclear isomer survives so long (at least 10¹⁵ years) that it has never been observed to decay spontaneously. The half-life of a nuclear isomer can even exceed that of the ground state of the same nuclide, as shown by ^180m
₇₃Ta
as well as ^192m2
₇₇Ir
, ^210m
₈₃Bi
, ^242m
₉₅Am
and multiple holmium isomers.

Sometimes, the gamma decay from a metastable state is referred to as isomeric transition, but this process typically resembles shorter-lived gamma decays in all external aspects with the exception of the long-lived nature of the meta-stable parent nuclear isomer. The longer lives of nuclear isomers' metastable states are often due to the larger degree of nuclear spin change which must be involved in their gamma emission to reach the ground state. This high spin change causes these decays to be forbidden transitions and delayed. Delays in emission are caused by low or high available decay energy.

The first nuclear isomer and decay-daughter system (uranium X₂/uranium Z, now known as ^234m
₉₁Pa
/²³⁴
₉₁Pa
) was discovered by Otto Hahn in 1921.^[2]

Nuclei of nuclear isomers

The nucleus of a nuclear isomer occupies a higher energy state than the non-excited nucleus existing in the ground state. In an excited state, one or more of the protons or neutrons in a nucleus occupy a nuclear orbital of higher energy than an available nuclear orbital. These states are analogous to excited states of electrons in atoms.

When excited atomic states decay, energy is released by fluorescence. In electronic transitions, this process usually involves emission of light near the visible range. The amount of energy released is related to bond-dissociation energy or ionization energy and is usually in the range of a few to few tens of eV per bond. However, a much stronger type of binding energy, the nuclear binding energy, is involved in nuclear processes. Due to this, most nuclear excited states decay by gamma ray emission. For example, a well-known nuclear isomer used in various medical procedures is ^99m
₄₃Tc
, which decays with a half-life of about 6 hours by emitting a gamma ray of 140 keV of energy; this is close to the energy of medical diagnostic X-rays.

Nuclear isomers have long half-lives because their gamma decay is "forbidden" from the large change in nuclear spin needed to emit a gamma ray. For example, ^180m
₇₃Ta
has a spin of 9 and must gamma-decay to ¹⁸⁰
₇₃Ta
with a spin of 1. Similarly, ^99m
₄₃Tc
has a spin of 1/2 and must gamma-decay to ⁹⁹
₄₃Tc
with a spin of 9/2.

While most metastable isomers decay through gamma-ray emission, they can also decay through internal conversion. During internal conversion, energy of nuclear de-excitation is not emitted as a gamma ray, but is instead used to accelerate one of the inner electrons of the atom. These excited electrons then leave at a high speed. This occurs because inner atomic electrons penetrate the nucleus where they are subject to the intense electric fields created when the protons of the nucleus re-arrange in a different way.

In nuclei that are far from stability in energy, even more decay modes are known.

After fission, several of the fission fragments that may be produced have a metastable isomeric state. These fragments are usually produced in a highly excited state, in terms of energy and angular momentum, and go through a prompt de-excitation. At the end of this process, the nuclei can populate both the ground and the isomeric states. If the half-life of the isomers is long enough, it is possible to measure their production rate and compare it to the one of the ground state, calculating the so-called isomeric yield ratio.^[3]

Metastable isomers

Metastable isomers can be produced through nuclear fusion or other nuclear reactions. A nucleus produced this way generally starts its existence in an excited state that relaxes through the emission of one or more gamma rays or conversion electrons. Sometimes the de-excitation does not completely proceed rapidly to the nuclear ground state. This usually occurs when the formation of an intermediate excited state has a spin far different from that of the ground state. Gamma-ray emission is hindered if the spin of the post-emission state differs greatly from that of the emitting state, especially if the excitation energy is low. The excited state in this situation is a good candidate to be metastable if there are no other states of intermediate spin with excitation energies less than that of the metastable state.

Metastable isomers of a particular isotope are usually designated with an "m". This designation is placed after the mass number of the atom; for example, cobalt-58m1 is abbreviated ^58m1
₂₇Co
, where 27 is the atomic number of cobalt. For isotopes with more than one metastable isomer, "indices" are placed after the designation, and the labeling becomes m1, m2, m3, and so on. Increasing indices, m1, m2, etc., correlate with increasing levels of excitation energy stored in each of the isomeric states (e.g., hafnium-178m2, or ^178m2
₇₂Hf
).

A different kind of metastable nuclear state (isomer) is the fission isomer or shape isomer. Most actinide nuclei in their ground states are not spherical, but rather prolate spheroidal, with an axis of symmetry longer than the other axes, similar to an American football or rugby ball. This geometry can result in quantum-mechanical states where the distribution of protons and neutrons is so much further from spherical geometry that de-excitation to the nuclear ground state is strongly hindered. In general, these states either de-excite to the ground state far more slowly than a "usual" excited state, or they undergo spontaneous fission with half-lives of the order of nanoseconds or microseconds—a very short time, but many orders of magnitude longer than the half-life of a more usual nuclear excited state. Fission isomers may be denoted with a postscript or superscript "f" rather than "m", so that a fission isomer, e.g. of plutonium-240, can be denoted as plutonium-240f or ^240f
₉₄Pu
.

Nearly stable isomers

Most nuclear excited states are very unstable and "immediately" radiate away the extra energy after existing on the order of 10⁻¹² seconds. As a result, the characterization "nuclear isomer" is usually applied only to configurations with half-lives of 10⁻⁹ seconds or longer. Quantum mechanics predicts that certain atomic species should possess isomers with unusually long lifetimes even by this stricter standard and have interesting properties. Some nuclear isomers are so long-lived that they are relatively stable and can be produced and observed in quantity.

The most stable nuclear isomer occurring in nature is ^180m
₇₃Ta
, which is present in all tantalum samples at about 1 part in 8,300. Its half-life is at least 10¹⁵ years, markedly longer than the age of the universe. The low excitation energy of the isomeric state causes both gamma de-excitation to the ¹⁸⁰
Ta
ground state (which itself is radioactive by beta decay, with a half-life of only 8 hours) and direct electron capture to hafnium or beta decay to tungsten to be suppressed due to spin mismatches. The origin of this isomer is mysterious, though it is believed to have been formed in supernovae (as are most other heavy elements). Were it to relax to its ground state, it would release a photon with a photon energy of 75 keV.

It was first reported in 1988 by C. B. Collins^[4] that theoretically ^180m
Ta
can be forced to release its energy by weaker X-rays, although at that time this de-excitation mechanism had never been observed. However, the de-excitation of ^180m
Ta
by resonant photo-excitation of intermediate high levels of this nucleus (E ~ 1 MeV) was observed in 1999 by Belic and co-workers in the Stuttgart nuclear physics group.^[5]

^178m2
₇₂Hf
is another reasonably stable nuclear isomer. It possesses a half-life of 31 years and the highest excitation energy of any comparably long-lived isomer. One gram of pure ^178m2
Hf
contains approximately 1.33 gigajoules of energy, the equivalent of exploding about 315 kg (694 lb) of TNT. In the natural decay of ^178m2
Hf
, the energy is released as gamma rays with a total energy of 2.45 MeV. As with ^180m
Ta
, there are disputed reports that ^178m2
Hf
can be stimulated into releasing its energy. Due to this, the substance is being studied as a possible source for gamma-ray lasers. These reports indicate that the energy is released very quickly, so that ^178m2
Hf
can produce extremely high powers (on the order of exawatts). Other isomers have also been investigated as possible media for gamma-ray stimulated emission.^[1][6]

Holmium's nuclear isomer ^166m1
₆₇Ho
has a half-life of 1,200 years, which is nearly the longest half-life of any holmium radionuclide. Only ¹⁶³
Ho
, with a half-life of 4,570 years, is more stable.

²²⁹
₉₀Th
has a remarkably low-lying metastable isomer, estimated at only 8.28 ± 0.17 eV above the ground state.^[7] After years of failure and one notable false alarm,^[8][9] this decay was directly observed in 2016, based on its internal conversion decay.^[10][11] This direct detection allowed for a first measurement of the isomer's lifetime under internal-conversion decay,^[12] the determination of the isomer's magnetic dipole and electric quadrupole moment via spectroscopy of the electronic shell^[13] and an improved measurement of the excitation energy.^[7] Due to its low energy, the isomer is expected to allow for direct nuclear laser spectroscopy and the development of a nuclear clock of unprecedented accuracy.^[14][15]

High-spin suppression of decay

The most common mechanism for suppression of gamma decay of excited nuclei, and thus the existence of a metastable isomer, is lack of a decay route for the excited state that will change nuclear angular momentum along any given direction by the most common amount of 1 quantum unit ħ in the spin angular momentum. This change is necessary to emit a gamma photon, which has a spin of 1 unit in this system. Integral changes of 2 and more units in angular momentum are possible, but the emitted photons carry off the additional angular momentum. Changes of more than 1 unit are known as forbidden transitions. Each additional unit of spin change larger than 1 that the emitted gamma ray must carry inhibits decay rate by about 5 orders of magnitude.^[16] The highest known spin change of 8 units occurs in the decay of ^180mTa, which suppresses its decay by a factor of 10³⁵ from that associated with 1 unit. Instead of a natural gamma-decay half-life of 10⁻¹² seconds, it has a half-life of more than 10²³ seconds, or at least 3 × 10¹⁵ years, and thus has yet to be observed to decay.

Gamma emission is impossible when the nucleus begins in a zero-spin state, as such an emission would not conserve angular momentum.^{[citation needed]}

Applications

Hafnium^[17][18] isomers (mainly ^178m2Hf) have been considered as weapons that could be used to circumvent the Nuclear Non-Proliferation Treaty, since it is claimed that they can be induced to emit very strong gamma radiation. This claim is generally discounted.^[19] DARPA had a program to investigate this use of both nuclear isomers.^[20] The potential to trigger an abrupt release of energy from nuclear isotopes, a prerequisite to their use in such weapons, is disputed. Nonetheless a 12-member Hafnium Isomer Production Panel (HIPP) was created in 2003 to assess means of mass-producing the isotope.^[21]

Technetium isomers ^99m
₄₃Tc
(with a half-life of 6.01 hours) and ^95m
₄₃Tc
(with a half-life of 61 days) are used in medical and industrial applications.

Nuclear batteries

 

Nuclear decay pathways for the conversion of lutetium-177^m to hafnium-177

Nuclear batteries use small amounts (milligrams and microcuries) of radioisotopes with high energy densities. In one betavoltaic device design, radioactive material sits atop a device with adjacent layers of P-type and N-type silicon. Ionizing radiation directly penetrates the junction and creates electron–hole pairs. Nuclear isomers could replace other isotopes, and with further development, it may be possible to turn them on and off by triggering decay as needed. Current candidates for such use include ¹⁰⁸Ag, ¹⁶⁶Ho, ¹⁷⁷Lu, and ²⁴²Am. As of 2004, the only successfully triggered isomer was ^180mTa, which required more photon energy to trigger than was released.^[22]

An isotope such as ¹⁷⁷Lu releases gamma rays by decay through a series of internal energy levels within the nucleus, and it is thought that by learning the triggering cross sections with sufficient accuracy, it may be possible to create energy stores that are 10⁶ times more concentrated than high explosive or other traditional chemical energy storage.^[22]

Decay processes

An isomeric transition or internal transition (IT) is the decay of a nuclear isomer to a lower-energy nuclear state. The actual process has two types (modes):^[23][24]

• γ (gamma ray) emission (emission of a high-energy photon),
• internal conversion (the energy is used to eject one of the atom's electrons).

Isomers may decay into other elements, though the rate of decay may differ between isomers. For example, ^177mLu can beta-decay to ¹⁷⁷Hf with a half-life of 160.4 d, or it can undergo isomeric transition to ¹⁷⁷Lu with a half-life of 160.4 d, which then beta-decays to ¹⁷⁷Hf with a half-life of 6.68 d.^[22]

The emission of a gamma ray from an excited nuclear state allows the nucleus to lose energy and reach a lower-energy state, sometimes its ground state. In certain cases, the excited nuclear state following a nuclear reaction or other type of radioactive decay can become a metastable nuclear excited state. Some nuclei are able to stay in this metastable excited state for minutes, hours, days, or occasionally far longer.

The process of isomeric transition is similar to gamma emission from any excited nuclear state, but differs by involving excited metastable states of nuclei with longer half-lives. As with other excited states, the nucleus can be left in an isomeric state following the emission of an alpha particle, beta particle, or some other type of particle.

The gamma ray may transfer its energy directly to one of the most tightly bound electrons, causing that electron to be ejected from the atom, a process termed the photoelectric effect. This should not be confused with the internal conversion process, in which no gamma-ray photon is produced as an intermediate particle.

See also

• Induced gamma emission
• Isomeric shift

References

1. Walker, Philip M.; Carroll, James J. (2007). "Nuclear Isomers: Recipes from the Past and Ingredients for the Future" (PDF). Nuclear Physics News. 17 (2): 11–15. doi:10.1080/10506890701404206. S2CID 22342780.
2. Hahn, Otto (1921). "Über ein neues radioaktives Zerfallsprodukt im Uran". Die Naturwissenschaften. 9 (5): 84. Bibcode:1921NW......9...84H. doi:10.1007/BF01491321. S2CID 28599831.
3. Rakopoulos, V.; Lantz, M.; Solders, A.; Al-Adili, A.; Mattera, A.; Canete, L.; Eronen, T.; Gorelov, D.; Jokinen, A.; Kankainen, A.; Kolhinen, V. S. (13 August 2018). "First isomeric yield ratio measurements by direct ion counting and implications for the angular momentum of the primary fission fragments". Physical Review C. 98 (2): 024612. doi:10.1103/PhysRevC.98.024612. ISSN 2469-9985. S2CID 125464341.
4. C. B. Collins; et al. (1988). (PDF). Physical Review C. 37 (5): 2267–2269. Bibcode:1988PhRvC..37.2267C. doi:10.1103/PhysRevC.37.2267. PMID 9954706. Archived from the original (PDF) on 21 January 2019.
5. D. Belic; et al. (1999). "Photoactivation of ¹⁸⁰Ta^m and Its Implications for the Nucleosynthesis of Nature's Rarest Naturally Occurring Isotope". Physical Review Letters. 83 (25): 5242–5245. Bibcode:1999PhRvL..83.5242B. doi:10.1103/PhysRevLett.83.5242.
6. . UNH Nuclear Physics Group. 1997. Archived from the original on 5 September 2006. Retrieved 1 June 2006.
7. Seiferle, B.; von der Wense, L.; Bilous, P.V.; Amersdorffer, I.; Lemell, C.; Libisch, F.; Stellmer, S.; Schumm, T.; Düllmann, C.E.; Pálffy, A.; Thirolf, P.G. (12 September 2019). "Energy of the ²²⁹Th nuclear clock transition". Nature. 573 (7773): 243–246. arXiv:1905.06308. doi:10.1038/s41586-019-1533-4. PMID 31511684. S2CID 155090121.
8. Shaw, R. W.; Young, J. P.; Cooper, S. P.; Webb, O. F. (8 February 1999). "Spontaneous Ultraviolet Emission from ²³³Uranium/²²⁹Thorium Samples". Physical Review Letters. 82 (6): 1109–1111. Bibcode:1999PhRvL..82.1109S. doi:10.1103/PhysRevLett.82.1109.
9. Utter, S.B.; et al. (1999). "Reexamination of the Optical Gamma Ray Decay in ²²⁹Th". Phys. Rev. Lett. 82 (3): 505–508. Bibcode:1999PhRvL..82..505U. doi:10.1103/PhysRevLett.82.505.
10. von der Wense, Lars; Seiferle, Benedict; Laatiaoui, Mustapha; Neumayr, Jürgen B.; Maier, Hans-Jörg; Wirth, Hans-Friedrich; Mokry, Christoph; Runke, Jörg; Eberhardt, Klaus; Düllmann, Christoph E.; Trautmann, Norbert G.; Thirolf, Peter G. (5 May 2016). "Direct detection of the ²²⁹Th nuclear clock transition". Nature. 533 (7601): 47–51. arXiv:1710.11398. Bibcode:2016Natur.533...47V. doi:10.1038/nature17669. PMID 27147026. S2CID 205248786.
11. (Press release). Ludwig Maximilian University of Munich. 6 May 2016. Archived from the original on 27 August 2016. Retrieved 1 August 2016.
12. Seiferle, B.; von der Wense, L.; Thirolf, P.G. (2017). "Lifetime measurement of the ²²⁹Th nuclear isomer". Phys. Rev. Lett. 118 (4): 042501. arXiv:1801.05205. doi:10.1103/PhysRevLett.118.042501. PMID 28186791. S2CID 37518294.
13. Thielking, J.; Okhapkin, M.V.; Przemyslaw, G.; Meier, D.M.; von der Wense, L.; Seiferle, B.; Düllmann, C.E.; Thirolf, P.G.; Peik, E. (2018). "Laser spectroscopic characterization of the nuclear-clock isomer ^229mTh". Nature. 556 (7701): 321–325. arXiv:1709.05325. doi:10.1038/s41586-018-0011-8. PMID 29670266. S2CID 4990345.
14. Peik, E.; Tamm, Chr. (15 January 2003). (PDF). Europhysics Letters. 61 (2): 181–186. Bibcode:2003EL.....61..181P. doi:10.1209/epl/i2003-00210-x. S2CID 250818523. Archived from the original (PDF) on 16 December 2013. Retrieved 12 September 2019.
15. Campbell, C.; Radnaev, A.G.; Kuzmich, A.; Dzuba, V.A.; Flambaum, V.V.; Derevianko, A. (2012). "A single ion nuclear clock for metrology at the 19th decimal place". Phys. Rev. Lett. 108 (12): 120802. arXiv:1110.2490. Bibcode:2012PhRvL.108l0802C. doi:10.1103/PhysRevLett.108.120802. PMID 22540568. S2CID 40863227.
16. Leon van Dommelen, Quantum Mechanics for Engineers 5 April 2014 at the Wayback Machine (Chapter 14).
17. David Hambling (16 August 2003). "Gamma-ray weapons". Reuters EurekAlert. New Scientist. Retrieved 12 December 2010.
18. Jeff Hecht (19 June 2006). "A perverse military strategy". New Scientist. Retrieved 12 December 2010.
19. Davidson, Seay. . Archived from the original on 10 May 2005.{{cite web}}: CS1 maint: bot: original URL status unknown (link)
20. S. Weinberger (28 March 2004). . Washington Post. Archived from the original on 23 August 2011.
21. . San Francisco Chronicle. 28 September 2003. Archived from the original on 15 June 2012.
22. M. S. Litz & G. Merkel (December 2004). "Controlled extraction of energy from nuclear isomers" (PDF). (PDF) from the original on 4 March 2016.
23. Darling, David. "isomeric transition". Encyclopedia of Science. Retrieved 16 August 2019.
24. Gardiner, Steven (12 August 2017). (PDF). University of California. Archived from the original (PDF) on 21 September 2018. Retrieved 16 August 2019.

External links

• Research group which presented initial claims of hafnium nuclear isomer de-excitation control. 25 February 2009 at the Wayback Machine – The Center for Quantum Electronics, The University of Texas at Dallas.
• JASON Defense Advisory Group report on high energy nuclear materials mentioned in the Washington Post story above
• Bertram Schwarzschild (May 2004). "Conflicting Results on a Long-Lived Nuclear Isomer of Hafnium Have Wider Implications". Physics Today. Vol. 57, no. 5. pp. 21–24. Bibcode:2004PhT....57e..21S. doi:10.1063/1.1768663. login required?
• – The Center for Quantum Electronics, The University of Texas at Dallas.
• – The Center for Quantum Electronics, The University of Texas at Dallas.