Electronic structure and optical properties of quantum crystals from first principles calculations in the Born–Oppenheimer approximation

Gorelov, Vitaly; Ceperley, David M.; Holzmann, Markus; Pierleoni, Carlo

doi:10.1063/5.0031843

Title: Electronic structure and optical properties of quantum crystals from first principles calculations in the Born–Oppenheimer approximation

Journal Article · Mon Dec 21 00:00:00 EST 2020 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0031843· OSTI ID:1850286

Gorelov, Vitaly ^[1]; Ceperley, David M. ^[2]; Holzmann, Markus ^[3];

^[4]

Univ. Paris-Saclay, Gif-sur-Yvette (France). Centre National de la Recherche Scientifique (CNRS). Commissariat a l'Energie Atomique (CEA). Maison de la Simulation
Univ. of Illinois at Urbana-Champaign, IL (United States). Dept. of Physics
Univ. of Grenoble Alpes, Grenoble (France). Institut Laue Langevin. Centre National de la Recherche Scientifique (CNRS). LPMMC
Univ. Paris-Saclay, Gif-sur-Yvette (France). Centre National de la Recherche Scientifique (CNRS). Commissariat a l'Energie Atomique (CEA). Maison de la Simulation; Univ. of L’Aquila, L’Aquila (Italy). Dept. of Physical and Chemical Sciences

In this work, we develop a formalism to accurately account for the renormalization of the 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 the 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 200 K and 250 GPa and discuss the optical absorption profile of hydrogen crystals at 200 K and carbon diamond at 297 K.

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Research Organization:: Univ. of Illinois at Urbana-Champaign, IL (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); European Union Horizon 2020

Grant/Contract Number:: NA0001789; 676531

OSTI ID:: 1850286

Journal Information:: Journal of Chemical Physics, Vol. 153, Issue 23; ISSN 0021-9606

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

Country of Publication:: United States

Language:: English

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