Fully consistent density functional theory determination of the insulator-metal transition boundary in warm dense hydrogen
Abstract
Using conceptually and procedurally consistent density functional theory (DFT) calculations with an advanced meta-GGA exchange-correlation functional in ab initio (Born-Oppenheimer, BO) molecular dynamics simulations, we determine the insulator-metal transition (IMT) of warm dense fluid hydrogen from 50 to 300 GPa, to be in better agreement with experiment than previous DFT predictions. Inclusion of nuclear quantum effects via path-integral molecular dynamics (PIMD) sharpens the transition and lowers its temperature relative to BOMD results. A rapid decrease in the molecular character of the system, as observed via the ionic pair correlation function, coincides with an abrupt conductivity increase, confirming a metallic transition due to molecular hydrogen dissociation that is coincident with abrupt band gap closure. Comparison of the PIMD and BOMD results clearly demonstrates an isotope effect on the IMT. Exploitation of differing methodologies for using the orbital-dependent and de-orbitalized versions of the meta-GGA enables us to quantify exchange-correlation approximation effects. Distinct from stochastic simulations, these results do 2 not depend upon any clever but uncontrolled combination of ground-state and finite-T methodologies and should provide a reliable benchmark for further studies.
- Publication Date:
- Research Org.:
- Univ. of Rochester, NY (United States)
- Sponsoring Org.:
- USDOE National Nuclear Security Administration (NNSA); National Science Foundation (NSF)
- Contributing Org.:
- Laboratory for Laser Energetics, University of Rochester
- OSTI Identifier:
- 1659363
- Alternate Identifier(s):
- OSTI ID: 1668795
- Report Number(s):
- 2019-257, 1585, 2540
Journal ID: ISSN 2643-1564; PPRHAI; 032065
- Grant/Contract Number:
- SC0002139; NA0003856; 1802964
- Resource Type:
- Published Article
- Journal Name:
- Physical Review Research
- Additional Journal Information:
- Journal Name: Physical Review Research Journal Volume: 2 Journal Issue: 3; Journal ID: ISSN 2643-1564
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Electrical conductivity; First-principle calculations
Citation Formats
Hinz, Joshua, Karasiev, Valentin V., Hu, S. X., Zaghoo, Mohamed, Mejía-Rodríguez, Daniel, Trickey, S. B., and Calderín, L. Fully consistent density functional theory determination of the insulator-metal transition boundary in warm dense hydrogen. United States: N. p., 2020.
Web. doi:10.1103/PhysRevResearch.2.032065.
Hinz, Joshua, Karasiev, Valentin V., Hu, S. X., Zaghoo, Mohamed, Mejía-Rodríguez, Daniel, Trickey, S. B., & Calderín, L. Fully consistent density functional theory determination of the insulator-metal transition boundary in warm dense hydrogen. United States. https://doi.org/10.1103/PhysRevResearch.2.032065
Hinz, Joshua, Karasiev, Valentin V., Hu, S. X., Zaghoo, Mohamed, Mejía-Rodríguez, Daniel, Trickey, S. B., and Calderín, L. Thu .
"Fully consistent density functional theory determination of the insulator-metal transition boundary in warm dense hydrogen". United States. https://doi.org/10.1103/PhysRevResearch.2.032065.
@article{osti_1659363,
title = {Fully consistent density functional theory determination of the insulator-metal transition boundary in warm dense hydrogen},
author = {Hinz, Joshua and Karasiev, Valentin V. and Hu, S. X. and Zaghoo, Mohamed and Mejía-Rodríguez, Daniel and Trickey, S. B. and Calderín, L.},
abstractNote = {Using conceptually and procedurally consistent density functional theory (DFT) calculations with an advanced meta-GGA exchange-correlation functional in ab initio (Born-Oppenheimer, BO) molecular dynamics simulations, we determine the insulator-metal transition (IMT) of warm dense fluid hydrogen from 50 to 300 GPa, to be in better agreement with experiment than previous DFT predictions. Inclusion of nuclear quantum effects via path-integral molecular dynamics (PIMD) sharpens the transition and lowers its temperature relative to BOMD results. A rapid decrease in the molecular character of the system, as observed via the ionic pair correlation function, coincides with an abrupt conductivity increase, confirming a metallic transition due to molecular hydrogen dissociation that is coincident with abrupt band gap closure. Comparison of the PIMD and BOMD results clearly demonstrates an isotope effect on the IMT. Exploitation of differing methodologies for using the orbital-dependent and de-orbitalized versions of the meta-GGA enables us to quantify exchange-correlation approximation effects. Distinct from stochastic simulations, these results do 2 not depend upon any clever but uncontrolled combination of ground-state and finite-T methodologies and should provide a reliable benchmark for further studies.},
doi = {10.1103/PhysRevResearch.2.032065},
journal = {Physical Review Research},
number = 3,
volume = 2,
place = {United States},
year = {Thu Sep 10 00:00:00 EDT 2020},
month = {Thu Sep 10 00:00:00 EDT 2020}
}
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