Mixed stochastic-deterministic density functional theoretic decomposition of Kubo–Greenwood conductivities in the projector augmented wave formalism

Sharma, Vidushi; Collins, Lee Anthony; White, Alexander James

doi:10.1063/5.0305405

Mixed stochastic-deterministic density functional theoretic decomposition of Kubo–Greenwood conductivities in the projector augmented wave formalism

Journal Article · Mon Jan 26 00:00:00 EST 2026 · Physics of Plasmas

DOI:https://doi.org/10.1063/5.0305405· OSTI ID:3017781

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Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Princeton Plasma Physics Laboratory (PPPL), Princeton, NJ (United States)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Pairing the accuracy of the Kohn–Sham density-functional framework with the efficiency of a stochastic algorithmic approach, mixed stochastic-deterministic density functional theory (mDFT) achieves a favorable computational scaling with system sizes and electronic temperatures. We employ the recently developed mDFT formalism to investigate the dynamic charge-transport properties of systems in the warm dense matter regime. The optical conductivity spectra are computed for single- and multi- component mixtures of carbon, hydrogen, and beryllium using two complementary approaches: Kubo–Greenwood in the mDFT picture and real-time time-dependent mDFT. We further devise a decomposition of the Onsager coefficients leading up to the Kubo–Greenwood spectra to exhibit contributions from the deterministic, stochastic, and mixed electronic state transitions at different incident photon energies.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Princeton Plasma Physics Laboratory (PPPL), Princeton, NJ (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC)

Grant/Contract Number:: 89233218CNA000001; AC02-09CH11466

Other Award/Contract Number:: 20230322ER
20230323ER

OSTI ID:: 3017781

Alternate ID(s):: OSTI ID: 3017856

Report Number(s):: LA-UR--25-29854; 10.1063/5.0305405

Journal Information:: Physics of Plasmas, Journal Name: Physics of Plasmas Journal Issue: 1 Vol. 33; ISSN 1070-664X; ISSN 1089-7674

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (64)

Understanding Jupiter's interior: UNDERSTANDING JUPITER'S INTERIOR Militzer, Burkhard; Soubiran, François; Wahl, Sean M. Journal of Geophysical Research: Planets, Vol. 121, Issue 9 https://doi.org/10.1002/2016JE005080	journal	September 2016
Liquid li structure and dynamics: A comparison between OFDFT and second nearest-neighbor embedded-atom method Chen, Mohan; Vella, Joseph R.; Panagiotopoulos, Athanassios Z. AIChE Journal, Vol. 61, Issue 9 https://doi.org/10.1002/aic.14795	journal	April 2015
On the Kubo-Greenwood model for electron conductivity Dufty, James; Wrighton, Jeffrey; Luo, Kai Contributions to Plasma Physics, Vol. 58, Issue 2-3 https://doi.org/10.1002/ctpp.201700102	journal	January 2018
Stochastic density functional theory Fabian, Marcel D.; Shpiro, Ben; Rabani, Eran Wiley Interdisciplinary Reviews: Computational Molecular Science, Vol. 9, Issue 6 https://doi.org/10.1002/wcms.1412	journal	April 2019
Introducing PROFESS: A new program for orbital-free density functional theory calculations Ho, Gregory S.; Lignères, Vincent L.; Carter, Emily A. Computer Physics Communications, Vol. 179, Issue 11 https://doi.org/10.1016/j.cpc.2008.07.002	journal	December 2008
Finite-temperature orbital-free DFT molecular dynamics: Coupling Profess and Quantum Espresso Karasiev, Valentin V.; Sjostrom, Travis; Trickey, S. B. Computer Physics Communications, Vol. 185, Issue 12 https://doi.org/10.1016/j.cpc.2014.08.023	journal	December 2014
Review of the first charged-particle transport coefficient comparison workshop Grabowski, P. E.; Hansen, S. B.; Murillo, M. S. High Energy Density Physics, Vol. 37 https://doi.org/10.1016/j.hedp.2020.100905	journal	November 2020
Current challenges in the physics of white dwarf stars Saumon, Didier; Blouin, Simon; Tremblay, Pier-Emmanuel Physics Reports, Vol. 988 https://doi.org/10.1016/j.physrep.2022.09.001	journal	November 2022
Experimental methods for warm dense matter research Falk, Katerina High Power Laser Science and Engineering, Vol. 6 https://doi.org/10.1017/hpl.2018.53	journal	January 2018
Orbital-Free Density Functional Theory: An Attractive Electronic Structure Method for Large-Scale First-Principles Simulations Mi, Wenhui; Luo, Kai; Trickey, S. B. Chemical Reviews, Vol. 123, Issue 21 https://doi.org/10.1021/acs.chemrev.2c00758	journal	October 2023
Time-dependent quantum-mechanical methods for molecular dynamics Kosloff, Ronnie The Journal of Physical Chemistry, Vol. 92, Issue 8 https://doi.org/10.1021/j100319a003	journal	April 1988
Probing warm dense matter using femtosecond X-ray absorption spectroscopy with a laser-produced betatron source Mahieu, B.; Jourdain, N.; Ta Phuoc, K. Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-05791-4	journal	August 2018
Demonstration of X-ray Thomson scattering as diagnostics for miscibility in warm dense matter Frydrych, S.; Vorberger, J.; Hartley, N. J. Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-16426-y	journal	May 2020
Measurement of interfacial thermal resistance in high-energy-density matter Allen, Cameron H.; Oliver, Matthew; Gericke, Dirk O. Nature Communications, Vol. 16, Issue 1 https://doi.org/10.1038/s41467-025-56051-1	journal	February 2025
Transient absorption of warm dense matter created by an X-ray free-electron laser Mercadier, Laurent; Benediktovitch, Andrei; Krušič, Špela Nature Physics, Vol. 20, Issue 10, p. 1564-1569 https://doi.org/10.1038/s41567-024-02587-w	journal	July 2024
Observing the onset of pressure-driven K-shell delocalization Döppner, T.; Bethkenhagen, M.; Kraus, D. Nature, Vol. 618, Issue 7964 https://doi.org/10.1038/s41586-023-05996-8	journal	May 2023
Superheating gold beyond the predicted entropy catastrophe threshold White, Thomas G.; Griffin, Travis D.; Haden, Daniel Nature, Vol. 643, Issue 8073 https://doi.org/10.1038/s41586-025-09253-y	journal	July 2025
Understanding dense hydrogen at planetary conditions Helled, Ravit; Mazzola, Guglielmo; Redmer, Ronald Nature Reviews Physics, Vol. 2, Issue 10 https://doi.org/10.1038/s42254-020-0223-3	journal	September 2020
Mixture of hydrogen and methane under planetary interior conditions Roy, Argha Jyoti; Bergermann, Armin; Bethkenhagen, Mandy Physical Chemistry Chemical Physics, Vol. 26, Issue 19 https://doi.org/10.1039/D4CP00058G	journal	January 2024
Algorithms and novel applications based on the isokinetic ensemble. II. Ab initio molecular dynamics Minary, Peter; Martyna, Glenn J.; Tuckerman, Mark E. The Journal of Chemical Physics, Vol. 118, Issue 6 https://doi.org/10.1063/1.1534583	journal	January 2003
Unitary quantum time evolution by iterative Lanczos reduction Park, Tae Jun; Light, J. C. The Journal of Chemical Physics, Vol. 85, Issue 10 https://doi.org/10.1063/1.451548	journal	November 1986
Sublinear scaling for time-dependent stochastic density functional theory Gao, Yi; Neuhauser, Daniel; Baer, Roi The Journal of Chemical Physics, Vol. 142, Issue 3 https://doi.org/10.1063/1.4905568	journal	January 2015
DC electrical conductivity of platinum from ab initio simulations Lentz, Meghan K.; Townsend, Joshua P.; Cochrane, Kyle R. AIP Conference Proceedings https://doi.org/10.1063/12.0020403	conference	January 2023
Hotspot conditions achieved in inertial confinement fusion experiments on the National Ignition Facility Patel, P. K.; Springer, P. T.; Weber, C. R. Physics of Plasmas, Vol. 27, Issue 5 https://doi.org/10.1063/5.0003298	journal	May 2020
Observation of a highly conductive warm dense state of water with ultrafast pump–probe free-electron-laser measurements Chen, Z.; Na, X.; Curry, C. B. Matter and Radiation at Extremes, Vol. 6, Issue 5 https://doi.org/10.1063/5.0043726	journal	September 2021
A polar direct drive liquid deuterium–tritium wetted foam target concept for inertial confinement fusion Olson, R. E.; Schmitt, M. J.; Haines, B. M. Physics of Plasmas, Vol. 28, Issue 12 https://doi.org/10.1063/5.0062590	journal	December 2021
Charged particle transport coefficient challenges in high energy density plasmas Haines, Brian M. Physics of Plasmas, Vol. 31, Issue 5 https://doi.org/10.1063/5.0197128	journal	May 2024
A review on charged-particle transport modeling for laser direct-drive fusion Hu, S. X.; Nichols, K. A.; Shaffer, N. R. Physics of Plasmas, Vol. 31, Issue 4 https://doi.org/10.1063/5.0197969	journal	April 2024
Optical and transport properties of plasma mixtures from ab initio molecular dynamics White, Alexander J.; Craven, Galen T.; Sharma, Vidushi Physics of Plasmas, Vol. 31, Issue 4 https://doi.org/10.1063/5.0198003	journal	April 2024
Review of the second charged-particle transport coefficient code comparison workshop Stanek, Lucas J.; Kononov, Alina; Hansen, Stephanie B. Physics of Plasmas, Vol. 31, Issue 5 https://doi.org/10.1063/5.0198155	journal	May 2024
The melting point of lithium: an orbital-free first-principles molecular dynamics study Chen, Mohan; Hung, Linda; Huang, Chen Molecular Physics, Vol. 111, Issue 22-23 https://doi.org/10.1080/00268976.2013.828379	journal	December 2013
A stochastic estimator of the trace of the influence matrix for laplacian smoothing splines Hutchinson, M. F. Communications in Statistics - Simulation and Computation, Vol. 19, Issue 2 https://doi.org/10.1080/03610919008812866	journal	January 1990
The Boltzmann Equation in the Theory of Electrical Conduction in Metals Greenwood, D. A. Proceedings of the Physical Society, Vol. 71, Issue 4 https://doi.org/10.1088/0370-1328/71/4/306	journal	April 1958
Mixed stochastic-deterministic time-dependent density functional theory: application to stopping power of warm dense carbon White, Alexander J.; Collins, Lee A.; Nichols, Katarina Journal of Physics: Condensed Matter, Vol. 34, Issue 17 https://doi.org/10.1088/1361-648X/ac4f1a	journal	February 2022
Electrical conductivity of warm dense hydrogen from ohm’s law and time-dependent density functional theory Ramakrishna, Kushal; Lokamani, Mani; Cangi, Attila Electronic Structure, Vol. 6, Issue 4 https://doi.org/10.1088/2516-1075/ad912b	journal	November 2024
Dynamical structure factors of warm dense matter from time-dependent orbital-free and mixed-stochastic-deterministic density functional theory White, Alexander J. Electronic Structure, Vol. 7, Issue 1 https://doi.org/10.1088/2516-1075/adad24	journal	February 2025
Thermal Properties of the Inhomogeneous Electron Gas Mermin, N. David Physical Review, Vol. 137, Issue 5A https://doi.org/10.1103/PhysRev.137.A1441	journal	March 1965
Transition to metallization in warm dense helium-hydrogen mixtures using stochastic density functional theory within the Kubo-Greenwood formalism Cytter, Yael; Rabani, Eran; Neuhauser, Daniel Physical Review B, Vol. 100, Issue 19 https://doi.org/10.1103/PhysRevB.100.195101	journal	November 2019
Real-space orthogonal projector-augmented-wave method Li, Wenfei; Neuhauser, Daniel Physical Review B, Vol. 102, Issue 19 https://doi.org/10.1103/PhysRevB.102.195118	journal	November 2020
Efficient time-dependent orbital-free density functional theory: Semilocal adiabatic response Jiang, Kaili; Shao, Xuecheng; Pavanello, Michele Physical Review B, Vol. 106, Issue 11 https://doi.org/10.1103/PhysRevB.106.115153	journal	September 2022
Electrical conductivity of iron in Earth's core from microscopic Ohm's law Ramakrishna, Kushal; Lokamani, Mani; Baczewski, Andrew Physical Review B, Vol. 107, Issue 11 https://doi.org/10.1103/PhysRevB.107.115131	journal	March 2023
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Nonlocal orbital-free kinetic energy density functional for semiconductors Huang, Chen; Carter, Emily A. Physical Review B, Vol. 81, Issue 4 https://doi.org/10.1103/PhysRevB.81.045206	journal	January 2010
Electronic transport coefficients from ab initio simulations and application to dense liquid hydrogen Holst, Bastian; French, Martin; Redmer, Ronald Physical Review B, Vol. 83, Issue 23 https://doi.org/10.1103/PhysRevB.83.235120	journal	June 2011
Time evolution of electron structure in femtosecond heated warm dense molybdenum Dorchies, F.; Recoules, V.; Bouchet, J. Physical Review B, Vol. 92, Issue 14 https://doi.org/10.1103/PhysRevB.92.144201	journal	October 2015
Stochastic density functional theory at finite temperatures Cytter, Yael; Rabani, Eran; Neuhauser, Daniel Physical Review B, Vol. 97, Issue 11 https://doi.org/10.1103/PhysRevB.97.115207	journal	March 2018
Time-dependent orbital-free density functional theory for electronic stopping power: Comparison to the Mermin-Kohn-Sham theory at high temperatures White, Alexander J.; Certik, Ondrej; Ding, Y. H. Physical Review B, Vol. 98, Issue 14 https://doi.org/10.1103/PhysRevB.98.144302	journal	October 2018
Stochastic and mixed density functional theory within the projector augmented wave formalism for simulation of warm dense matter Sharma, Vidushi; Collins, Lee A.; White, Alexander J. Physical Review E, Vol. 108, Issue 2 https://doi.org/10.1103/PhysRevE.108.L023201	journal	August 2023
Ionic and electronic transport properties in dense plasmas by orbital-free density functional theory Sjostrom, Travis; Daligault, Jérôme Physical Review E, Vol. 92, Issue 6 https://doi.org/10.1103/PhysRevE.92.063304	journal	December 2015
Self-Averaging Stochastic Kohn-Sham Density-Functional Theory Baer, Roi; Neuhauser, Daniel; Rabani, Eran Physical Review Letters, Vol. 111, Issue 10 https://doi.org/10.1103/PhysRevLett.111.106402	journal	September 2013
X-ray Thomson Scattering in Warm Dense Matter without the Chihara Decomposition Baczewski, A. D.; Shulenburger, L.; Desjarlais, M. P. Physical Review Letters, Vol. 116, Issue 11 https://doi.org/10.1103/PhysRevLett.116.115004	journal	March 2016
Measurements of the K -Shell Opacity of a Solid-Density Magnesium Plasma Heated by an X-Ray Free-Electron Laser Preston, T. R.; Vinko, S. M.; Ciricosta, O. Physical Review Letters, Vol. 119, Issue 8 https://doi.org/10.1103/PhysRevLett.119.085001	journal	August 2017
Ab Initio Studies on the Stopping Power of Warm Dense Matter with Time-Dependent Orbital-Free Density Functional Theory Ding, Y. H.; White, A. J.; Hu, S. X. Physical Review Letters, Vol. 121, Issue 14 https://doi.org/10.1103/PhysRevLett.121.145001	journal	October 2018
Fast and Universal Kohn-Sham Density Functional Theory Algorithm for Warm Dense Matter to Hot Dense Plasma White, A. J.; Collins, L. A. Physical Review Letters, Vol. 125, Issue 5 https://doi.org/10.1103/PhysRevLett.125.055002	journal	July 2020
Group Conductivity and Nonadiabatic Born Effective Charges of Disordered Metals, Warm Dense Matter, and Hot Dense Plasma Sharma, Vidushi; White, Alexander J. Physical Review Letters, Vol. 134, Issue 9 https://doi.org/10.1103/PhysRevLett.134.095102	journal	March 2025
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Carbon ionization at gigabar pressures: An ab initio perspective on astrophysical high-density plasmas Bethkenhagen, Mandy; Witte, Bastian B. L.; Schörner, Maximilian Physical Review Research, Vol. 2, Issue 2 https://doi.org/10.1103/PhysRevResearch.2.023260	journal	June 2020
Accelerating equilibration in first-principles molecular dynamics with orbital-free density functional theory Fiedler, Lenz; Moldabekov, Zhandos A.; Shao, Xuecheng Physical Review Research, Vol. 4, Issue 4 https://doi.org/10.1103/PhysRevResearch.4.043033	journal	October 2022
Physics principles of inertial confinement fusion and U.S. program overview Hurricane, O. A.; Patel, P. K.; Betti, R. Reviews of Modern Physics, Vol. 95, Issue 2 https://doi.org/10.1103/RevModPhys.95.025005	journal	June 2023
Negative differential conductivity in liquid aluminum from real-time quantum simulations Andrade, Xavier; Hamel, Sébastien; Correa, Alfredo A. The European Physical Journal B, Vol. 91, Issue 10 https://doi.org/10.1140/epjb/e2018-90291-5	journal	October 2018
Statistical-Mechanical Theory of Irreversible Processes. I. General Theory and Simple Applications to Magnetic and Conduction Problems Kubo, Ryogo Journal of the Physical Society of Japan, Vol. 12, Issue 6 https://doi.org/10.1143/JPSJ.12.570	journal	June 1957
Electron dynamics in extended systems within real-time time-dependent density-functional theory Kononov, Alina; Lee, Cheng-Wei; dos Santos, Tatiane Pereira MRS Communications, Vol. 12, Issue 6 https://doi.org/10.1557/s43579-022-00273-7	journal	September 2022
Understanding the Transport Properties of Methane–Hydrogen Mixtures under the Interior Conditions of Ice Giants Roy, Argha Jyoti; Bethkenhagen, Mandy; Bergermann, Armin The Astrophysical Journal, Vol. 990, Issue 2 https://doi.org/10.3847/1538-4357/adf5be	journal	September 2025

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Mixed stochastic-deterministic density functional theoretic decomposition of Kubo–Greenwood conductivities in the projector augmented wave formalism

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