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Electronic structure and optical properties of quantum crystals from first principles calculations in the Born-Oppenheimer approximation
- Source :
- The Journal of Chemical Physics, The Journal of Chemical Physics, AIP, 2020, ⟨10.1063/5.0031843⟩, Journal of Chemical Physics, Journal of Chemical Physics, 2020, ⟨10.1063/5.0031843⟩
- Publication Year :
- 2020
- Publisher :
- HAL CCSD, 2020.
-
Abstract
- International audience; We develop a formalism to accurately account for the renormalization of electronic structure due to quantum and thermal nuclear motions within the Born-Oppenheimer approximation. We focus on the fundamental energy gap obtained from electronic addition and removal energies from Quantum Monte Carlo calculations in either the canonical or grand canonical ensembles. The formalism applies as well to effective single electron theories such as those based on Density Functional Theory. We show that electronic (Bloch) crystal momentum can be restored by marginalizing the total electron-ion wave function with respect to the nuclear equilibrium distribution, and we describe an explicit procedure to establish the band structure of electronic excitations for quantum crystals within the Born-Oppenheimer approximation. Based on the Kubo-Greenwood equation, we discuss the effects of nuclear motion on optical conductivity. Our methodology applies to the low temperature regime where nuclear motion is quantized and in general differs from the semi-classical approximation. We apply our method to study the electronic structure of C2/c-24 crystalline hydrogen at 200K and 250 GPa and discuss the optical absorption profile of hydrogen crystal at 200K and carbon diamond at 297K.
- Subjects :
- Quantum Monte Carlo
Born–Oppenheimer approximation
FOS: Physical sciences
General Physics and Astronomy
Electronic structure
010402 general chemistry
01 natural sciences
Renormalization
symbols.namesake
Quantum mechanics
0103 physical sciences
Physical and Theoretical Chemistry
[PHYS.COND]Physics [physics]/Condensed Matter [cond-mat]
Wave function
Electronic band structure
Physics
Condensed Matter - Materials Science
010304 chemical physics
Materials Science (cond-mat.mtrl-sci)
Computational Physics (physics.comp-ph)
0104 chemical sciences
Crystal momentum
symbols
Density functional theory
Physics - Computational Physics
[PHYS.COND] Physics [physics]/Condensed Matter [cond-mat]
Subjects
Details
- Language :
- English
- ISSN :
- 00219606 and 10897690
- Database :
- OpenAIRE
- Journal :
- The Journal of Chemical Physics, The Journal of Chemical Physics, AIP, 2020, ⟨10.1063/5.0031843⟩, Journal of Chemical Physics, Journal of Chemical Physics, 2020, ⟨10.1063/5.0031843⟩
- Accession number :
- edsair.doi.dedup.....9ef2b4e3a87c494a234696cc752a8337
- Full Text :
- https://doi.org/10.1063/5.0031843⟩