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Title: Quantum many-body effects in x-ray spectra efficiently computed using a basic graph algorithm

Abstract

The mounting interest in using x-ray spectroscopy for refined materials characterization calls for an accurate electronic-structure theory to interpret the x-ray near-edge fine structure. Here, we propose an efficient and unified framework to describe all the many-electron processes in a Fermi liquid after a sudden perturbation (such as a core hole). This problem has been visited by the Mahan-Noziéres-De Dominicis (MND) theory, but it is intractable to implement various Feynman diagrams within first-principles calculations. In our report, we adopt a nondiagrammatic approach and treat all the many-electron processes in the MND theory on an equal footing. Starting from a recently introduced determinant formalism [Phys. Rev. Lett. 118, 096402 (2017)], we exploit the linear dependence of determinants describing different final states involved in the spectral calculations. An elementary graph algorithm, breadth-first search, can be used to quickly identify the important determinants for shaping the spectrum, which avoids the need to evaluate a great number of vanishingly small terms. This search algorithm is performed over the tree-structure of the many-body expansion, which mimics a path-finding process. We demonstrate that the determinantal approach is computationally inexpensive even for obtaining x-ray spectra of extended systems. Using Kohn-Sham orbitals from two self-consistent fields (ground andmore » core-excited state) as input for constructing the determinants, the calculated x-ray spectra for a number of transition metal oxides are in good agreement with experiments. Many-electron aspects beyond the Bethe-Salpeter equation, as captured by this approach, are also discussed, such as shakeup excitations and many-body wave function overlap considered in Anderson's orthogonality catastrophe.« less

Authors:
 [1];  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1544275
Alternate Identifier(s):
OSTI ID: 1438503
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 97; Journal Issue: 20; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Liang, Yufeng, and Prendergast, David. Quantum many-body effects in x-ray spectra efficiently computed using a basic graph algorithm. United States: N. p., 2018. Web. doi:10.1103/PhysRevB.97.205127.
Liang, Yufeng, & Prendergast, David. Quantum many-body effects in x-ray spectra efficiently computed using a basic graph algorithm. United States. doi:10.1103/PhysRevB.97.205127.
Liang, Yufeng, and Prendergast, David. Wed . "Quantum many-body effects in x-ray spectra efficiently computed using a basic graph algorithm". United States. doi:10.1103/PhysRevB.97.205127. https://www.osti.gov/servlets/purl/1544275.
@article{osti_1544275,
title = {Quantum many-body effects in x-ray spectra efficiently computed using a basic graph algorithm},
author = {Liang, Yufeng and Prendergast, David},
abstractNote = {The mounting interest in using x-ray spectroscopy for refined materials characterization calls for an accurate electronic-structure theory to interpret the x-ray near-edge fine structure. Here, we propose an efficient and unified framework to describe all the many-electron processes in a Fermi liquid after a sudden perturbation (such as a core hole). This problem has been visited by the Mahan-Noziéres-De Dominicis (MND) theory, but it is intractable to implement various Feynman diagrams within first-principles calculations. In our report, we adopt a nondiagrammatic approach and treat all the many-electron processes in the MND theory on an equal footing. Starting from a recently introduced determinant formalism [Phys. Rev. Lett. 118, 096402 (2017)], we exploit the linear dependence of determinants describing different final states involved in the spectral calculations. An elementary graph algorithm, breadth-first search, can be used to quickly identify the important determinants for shaping the spectrum, which avoids the need to evaluate a great number of vanishingly small terms. This search algorithm is performed over the tree-structure of the many-body expansion, which mimics a path-finding process. We demonstrate that the determinantal approach is computationally inexpensive even for obtaining x-ray spectra of extended systems. Using Kohn-Sham orbitals from two self-consistent fields (ground and core-excited state) as input for constructing the determinants, the calculated x-ray spectra for a number of transition metal oxides are in good agreement with experiments. Many-electron aspects beyond the Bethe-Salpeter equation, as captured by this approach, are also discussed, such as shakeup excitations and many-body wave function overlap considered in Anderson's orthogonality catastrophe.},
doi = {10.1103/PhysRevB.97.205127},
journal = {Physical Review B},
number = 20,
volume = 97,
place = {United States},
year = {2018},
month = {5}
}

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