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Gentlest ascent dynamics for calculating first excited state and exploring energy landscape of Kohn-Sham density functionals

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.4936411· OSTI ID:1371102
 [1];  [1];  [2]
  1. Duke Univ., Durham, NC (United States)
  2. Duke Univ., Durham, NC (United States); South China Normal Univ., Guangzhou (China)
+ Show Author Affiliations
Here, we develop the gentlest ascent dynamics for Kohn-Sham density functional theory to search for the index-1 saddle points on the energy landscape of the Kohn-Sham density functionals. These stationary solutions correspond to excited states in the ground state functionals. As shown by various examples, the first excited states of many chemical systems are given by these index-1 saddle points. Our novel approach provides an alternative, more robust way to obtain these excited states, compared with the widely used ΔSCF approach. The method can be easily generalized to target higher index saddle points. Our results also reveal the physical interest and relevance of studying the Kohn-Sham energy landscape.
Research Organization:
Energy Frontier Research Centers (EFRC), Washington, D.C. (United States). Center for the Computational Design of Functional Layered Materials (CCDM)
Sponsoring Organization:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
SC0012575
OSTI ID:
1371102
Alternate ID(s):
OSTI ID: 1228787
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 22 Vol. 143; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

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Figures / Tables (5)

FIG. 1(p. 6)figure FIG. 1
TABLE I(p. 6)table TABLE I
TABLE II(p. 7)table TABLE II
TABLE III(p. 8)table TABLE III
TABLE IV(p. 8)table TABLE IV

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