Thermodynamics of technetium: Reconciling theory and experiment using density functional perturbation analysis
Abstract
The structure, lattice dynamics and thermodynamic properties of bulk technetium were investigated within the framework of density functional theory. The phonon density of states spectrum computed with density functional perturbation theory closely matches inelastic coherent neutron scattering measurements. The thermal properties of technetium were derived from phonon frequencies calculated within the quasi-harmonic approximation (QHA), which introduces a volume dependence of phonon frequencies as a part of the anharmonic effect. As a result, the predicted thermal expansion and isobaric heat capacity of technetium are in excellent agreement with available experimental data for temperatures up to ~1600 K.
- Authors:
-
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
- Univ. of Nevada, Las Vegas, NV (United States)
- Publication Date:
- Research Org.:
- Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1235368
- Report Number(s):
- SAND-2015-3444J
Journal ID: ISSN 1477-9226; ICHBD9; 583604
- Grant/Contract Number:
- AC04-94AL85000
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Dalton Transactions
- Additional Journal Information:
- Journal Volume: 44; Journal Issue: 28; Journal ID: ISSN 1477-9226
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Weck, Philippe F., and Kim, Eunja. Thermodynamics of technetium: Reconciling theory and experiment using density functional perturbation analysis. United States: N. p., 2015.
Web. doi:10.1039/c5dt01639h.
Weck, Philippe F., & Kim, Eunja. Thermodynamics of technetium: Reconciling theory and experiment using density functional perturbation analysis. United States. https://doi.org/10.1039/c5dt01639h
Weck, Philippe F., and Kim, Eunja. Thu .
"Thermodynamics of technetium: Reconciling theory and experiment using density functional perturbation analysis". United States. https://doi.org/10.1039/c5dt01639h. https://www.osti.gov/servlets/purl/1235368.
@article{osti_1235368,
title = {Thermodynamics of technetium: Reconciling theory and experiment using density functional perturbation analysis},
author = {Weck, Philippe F. and Kim, Eunja},
abstractNote = {The structure, lattice dynamics and thermodynamic properties of bulk technetium were investigated within the framework of density functional theory. The phonon density of states spectrum computed with density functional perturbation theory closely matches inelastic coherent neutron scattering measurements. The thermal properties of technetium were derived from phonon frequencies calculated within the quasi-harmonic approximation (QHA), which introduces a volume dependence of phonon frequencies as a part of the anharmonic effect. As a result, the predicted thermal expansion and isobaric heat capacity of technetium are in excellent agreement with available experimental data for temperatures up to ~1600 K.},
doi = {10.1039/c5dt01639h},
journal = {Dalton Transactions},
number = 28,
volume = 44,
place = {United States},
year = {Thu Jun 11 00:00:00 EDT 2015},
month = {Thu Jun 11 00:00:00 EDT 2015}
}
Web of Science
Works referenced in this record:
Radioactive Isotopes of Element 43
journal, July 1937
- Perrier, C.; SegrÈ, E.
- Nature, Vol. 140, Issue 3535
α-Manganese Phases containing Technetium-99
journal, November 1961
- Lam, D. J.; Darby, J. B.; Downey, J. W.
- Nature, Vol. 192, Issue 4804
Crystal chemistry of some technetium-containing oxides
journal, December 1964
- Muller, O.; White, W. B.; Roy, R.
- Journal of Inorganic and Nuclear Chemistry, Vol. 26, Issue 12
The thermal conductivity of technetium
journal, June 1965
- Baker, D. E.
- Journal of the Less Common Metals, Vol. 8, Issue 6
Über die Existenz eines Technetiumcarbides
journal, May 1962
- Trzebiatowski, W.; Rudziński, J.
- Zeitschrift für Chemie, Vol. 2, Issue 5
An investigation of the vanadium-technetium alloy system
journal, May 1968
- Koch, C. C.; Love, G. R.
- Journal of the Less Common Metals, Vol. 15, Issue 1
A low temperature X-ray investigation of technetium and the TcMo A-15 compound
journal, October 1972
- Marples, J. A. C.; Koch, C. C.
- Physics Letters A, Vol. 41, Issue 4
Superconductivity of technetium and technetium carbide
journal, December 1966
- Giorgi, A. L.; Szklarz, E. G.
- Journal of the Less Common Metals, Vol. 11, Issue 6
Superconducting Properties of Technetium
journal, March 1967
- Sekula, S. T.; Kernohan, R. H.; Love, G. R.
- Physical Review, Vol. 155, Issue 2
The electrical resistivity of technetium from 8.0° to 1700° K
journal, January 1967
- Koch, C. C.; Love, G. R.
- Journal of the Less Common Metals, Vol. 12, Issue 1
Heat capacity of technetium
journal, December 1975
- Trainor, R. J.; Brodsky, M. B.
- Physical Review B, Vol. 12, Issue 11
Current Status of the Thermodynamic Data for Technetium and Its Compounds and Aqueous Species
journal, January 2005
- Rard, Joseph A.
- Journal of Nuclear and Radiochemical Sciences, Vol. 6, Issue 3
Design of targeting ligands in medicinal inorganic chemistry
journal, January 2006
- Storr, Tim; Thompson, Katherine H.; Orvig, Chris
- Chemical Society Reviews, Vol. 35, Issue 6
The preparation of substitution-inert 99Tc metal-fragments: Promising candidates for the design of new 99mTc radiopharmaceuticals
journal, August 2006
- Tisato, Francesco; Porchia, Marina; Bolzati, Cristina
- Coordination Chemistry Reviews, Vol. 250, Issue 15-16
Technetium in the Nuclear Fuel Cycle, in Medicine and in the Environment
journal, January 1993
- Lieser, K. H.
- Radiochimica Acta, Vol. 63, Issue s1
Evidence for the Interaction of Technetium Colloids with Humic Substances by X-ray Absorption Spectroscopy
journal, April 2004
- Maes, A.; Geraedts, K.; Bruggeman, C.
- Environmental Science & Technology, Vol. 38, Issue 7
The heat capacity of Tc0.85Ru0.15 alloy
journal, February 2000
- van der Laan, R. R.; Konings, R. J. M.
- Journal of Alloys and Compounds, Vol. 297, Issue 1-2
Heat capacities of technetium metal and technetium–ruthenium alloy
journal, May 2002
- Shirasu, Yoshiro; Minato, Kazuo
- Journal of Alloys and Compounds, Vol. 337, Issue 1-2
Modeling of heat capacities of metals
journal, September 1989
- Krikorian, Oscar H.; Lai, David Y.
- Journal of Nuclear Materials, Vol. 167
Thermodynamic properties of technetium
journal, March 1989
- Guillermet, Armando Fernández; Grimvall, Göran
- Journal of the Less Common Metals, Vol. 147, Issue 2
The thermodynamic properties of rhenium on ITS-90
journal, September 1996
- Arblaster, J. W.
- Calphad, Vol. 20, Issue 3
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Atoms, molecules, solids, and surfaces: Applications of the generalized gradient approximation for exchange and correlation
journal, September 1992
- Perdew, John P.; Chevary, J. A.; Vosko, S. H.
- Physical Review B, Vol. 46, Issue 11
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Structures of uranyl peroxide hydrates: a first-principles study of studtite and metastudtite
journal, January 2012
- Weck, Philippe F.; Kim, Eunja; Jové-Colón, Carlos F.
- Dalton Transactions, Vol. 41, Issue 32
On the role of strong electron correlations in the surface properties and chemistry of uranium dioxide
journal, January 2013
- Weck, Philippe F.; Kim, Eunja; Jové-Colón, Carlos F.
- Dalton Transactions, Vol. 42, Issue 13
First-principles study of anhydrite, polyhalite and carnallite
journal, February 2014
- Weck, Philippe F.; Kim, Eunja; Jové-Colón, Carlos F.
- Chemical Physics Letters, Vol. 594
Solar Energy Storage in Phase Change Materials: First-Principles Thermodynamic Modeling of Magnesium Chloride Hydrates
journal, February 2014
- Weck, Philippe F.; Kim, Eunja
- The Journal of Physical Chemistry C, Vol. 118, Issue 9
Layered uranium( vi ) hydroxides: structural and thermodynamic properties of dehydrated schoepite α-UO 2 (OH) 2
journal, January 2014
- Weck, Philippe F.; Kim, Eunja
- Dalton Trans., Vol. 43, Issue 45
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999
- Kresse, G.; Joubert, D.
- Physical Review B, Vol. 59, Issue 3, p. 1758-1775
Matrix Eigenvector Methods
book, January 1983
- Davidson, Ernest R.
- Methods in Computational Molecular Physics
Special points for Brillouin-zone integrations
journal, June 1976
- Monkhorst, Hendrik J.; Pack, James D.
- Physical Review B, Vol. 13, Issue 12, p. 5188-5192
Improved tetrahedron method for Brillouin-zone integrations
journal, June 1994
- Blöchl, Peter E.; Jepsen, O.; Andersen, O. K.
- Physical Review B, Vol. 49, Issue 23
First-principles calculations of the ferroelastic transition between rutile-type and -type at high pressures
journal, October 2008
- Togo, Atsushi; Oba, Fumiyasu; Tanaka, Isao
- Physical Review B, Vol. 78, Issue 13
Interplay between structure, stoichiometry and properties of technetium nitrides
journal, January 2011
- Weck, Philippe F.; Kim, Eunja; Czerwinski, Kenneth R.
- Dalton Transactions, Vol. 40, Issue 25
Origin of the zone-center [001] LO-phonon anomaly in superconducting hcp transition metals
journal, November 1981
- Liu, S. H.; Stassis, C.; Ho, K. -M.
- Physical Review B, Vol. 24, Issue 9
Phonon anomalies and superconductivity in the hcp metals, Tc, Re, and Ru
journal, July 1981
- Smith, H. G.; Wakabayashi, N.
- Solid State Communications, Vol. 39, Issue 2
Finite Elastic Strain of Cubic Crystals
journal, June 1947
- Birch, Francis
- Physical Review, Vol. 71, Issue 11
The Compressibility of Media under Extreme Pressures
journal, September 1944
- Murnaghan, F. D.
- Proceedings of the National Academy of Sciences, Vol. 30, Issue 9
Elastic moduli and Debye temperature of polycrystalline technetium by ultrasonic velocity measurements
journal, January 1970
- Love, G. R.; Koch, C. C.; Whaley, H. L.
- Journal of the Less Common Metals, Vol. 20, Issue 1
Thermal expansions of technetium–ruthenium alloys
journal, March 2002
- Shirasu, Yoshiro; Minato, Kazuo
- Journal of Alloys and Compounds, Vol. 335, Issue 1-2
Superconductivity and the Fermi surface of Tc
journal, June 1980
- Asokamani, R.; Iyakutti, K.
- Journal of Physics F: Metal Physics, Vol. 10, Issue 6
Electronic, superconducting, and optical properties of technetium from its augmented-plane-wave band structure
journal, April 1983
- Chatterjee, Parsathi
- Physical Review B, Vol. 27, Issue 8
Anharmonic lattice vibrations in simple metals
journal, June 1983
- Rosén, J.; Grimvall, G.
- Physical Review B, Vol. 27, Issue 12
Works referencing / citing this record:
Infrared and Raman spectroscopy of α-ZrW 2 O 8 : A comprehensive density functional perturbation theory and experimental study
journal, May 2018
- Weck, Philippe F.; Gordon, Margaret E.; Greathouse, Jeffery A.
- Journal of Raman Spectroscopy, Vol. 49, Issue 8
Reverse-martensitic hcp-to-fcc transformation in technetium under shock compression
journal, July 2018
- Kim, Eunja; Weck, Philippe F.; Mattsson, Thomas R.
- Journal of Applied Physics, Vol. 124, Issue 3