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Title: Quantum embedding for material chemistry based on domain separation and open subsystems

Journal Article · · International Journal of Quantum Chemistry
DOI:https://doi.org/10.1002/qua.26184· OSTI ID:1598617
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Northwestern Univ., Evanston, IL (United States)
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Our perspective considers two theories we recently proposed to perform quantum embedding calculations for chemical systems: domain-separated density functional theory (DSDFT) and locally coupled open subsystems (LCOS). The development includes both the fundamentals of each theory as well as potential applications, some technical aspects, and related challenges. DS-DFT is suited to study intramolecular effects, where one can apply a high level of theory (based on DFT or wave function theory) to a region of interest inside a molecule or solid, and lower level theory elsewhere, with smooth switching between the regions. LCOS, in contrast, is a fragment-based embedding which offers computational advantages to study intermolecular behavior such as electron hopping, spin-environment interaction, and charge transfer excitations. Yet, both theories can exchange roles when appropriate. In addition, these theories allow for control of computational scaling of their algorithms. We investigate paths to determine the charge-transfer operator used in LCOS, and suggest an auxiliary energy minimization that can provide a practical estimate to this operator. We also briefly discuss how to implement density fitting techniques in domain separation, and how domain separation can be used for pure wavefunction-based embedding.

Research Organization:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
Grant/Contract Number:
SC0004752; FG02‐03ER15457
OSTI ID:
1598617
Alternate ID(s):
OSTI ID: 1600043
Journal Information:
International Journal of Quantum Chemistry, Vol. 120, Issue 21; ISSN 0020-7608
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 3 works
Citation information provided by
Web of Science

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Related Subjects

77 NANOSCIENCE AND NANOTECHNOLOGY
charge transfer
density functional theory
open subsystem
quantum embedding