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

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/5.0031843· OSTI ID:1850286
 [1];  [2];  [3];  [4]
  1. 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. Paris-Saclay, Gif-sur-Yvette (France)
  2. Univ. of Illinois at Urbana-Champaign, IL (United States). Dept. of Physics
  3. Univ. of Grenoble Alpes, Grenoble (France). Institut Laue Langevin. Centre National de la Recherche Scientifique (CNRS). LPMMC
  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 L’Aquila, L’Aquila (Italy). Dept. of Physical and Chemical Sciences
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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.
Research Organization:
Univ. of Illinois at Urbana-Champaign, IL (United States)
Sponsoring Organization:
European Union Horizon 2020; USDOE National Nuclear Security Administration (NNSA)
Grant/Contract Number:
NA0001789
OSTI ID:
1850286
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 23 Vol. 153; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
60 APPLIED LIFE SCIENCES
71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
Born-Oppenheimer approximation
Chemistry
Monte Carlo methods
band gap
density functional theory
electronic structure
optical absorption
physics
statistical thermodynamics