TY - JOUR
T1 - Spin-flip approach within time-dependent density functional tight-binding method
T2 - Theory and applications
AU - Inamori, Mayu
AU - Yoshikawa, Takeshi
AU - Ikabata, Yasuhiro
AU - Nishimura, Yoshifumi
AU - Nakai, Hiromi
N1 - Funding Information:
Some of the presented calculations were performed at the Research Center for Computational Science (RCCS), Okazaki Research Facilities, National Institutes of Natural Sciences (NINS). This work was supported in part by a Grant-in-Aid for Scientific Research (S) “KAKENHI Grant Number JP18H05264” and Grant-in-Aid for Early-Career Scientists “KAKENHI Grant Number JP18K14184” from the Japan Society for the Promotion of Science (JSPS). This work was also supported by Element Strategy Initiative “JPMXP0112101003” from the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan.
Funding Information:
Some of the presented calculations were performed at the Research Center for Computational Science (RCCS), Okazaki Research Facilities, National Institutes of Natural Sciences (NINS). This work was supported in part by a Grant‐in‐Aid for Scientific Research (S) “KAKENHI Grant Number JP18H05264” and Grant‐in‐Aid for Early‐Career Scientists “KAKENHI Grant Number JP18K14184” from the Japan Society for the Promotion of Science (JSPS). This work was also supported by Element Strategy Initiative “JPMXP0112101003” from the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan.
Publisher Copyright:
© 2020 Wiley Periodicals, Inc.
PY - 2020/6/15
Y1 - 2020/6/15
N2 - A spin-flip time-dependent density functional tight-binding (SF-TDDFTB) method is developed that describes target states as spin-flipping excitation from a high-spin reference state obtained by the spin-restricted open shell treatment. Furthermore, the SF-TDDFTB formulation is extended to long-range correction (LC), denoted as SF-TDLCDFTB. The LC technique corrects the overdelocalization of electron density in systems such as charge-transfer systems, which is typically found in conventional DFTB calculations as well as density functional theory calculations using pure functionals. The numerical assessment of the SF-TDDFTB method shows smooth potential curves for the bond dissociation of hydrogen fluoride and the double-bond rotation of ethylene and the double-cone shape of H3 as the simplest degenerate systems. In addition, numerical assessments of SF-TDDFTB and SF-TDLCDFTB for 39 S0/S1 minimum energy conical intersection (MECI) structures are performed. The SF-TDDFTB and SF-TDLCDFTB methods drastically reduce the computational cost with accuracy for MECI structures compared with SF-TDDFT.
AB - A spin-flip time-dependent density functional tight-binding (SF-TDDFTB) method is developed that describes target states as spin-flipping excitation from a high-spin reference state obtained by the spin-restricted open shell treatment. Furthermore, the SF-TDDFTB formulation is extended to long-range correction (LC), denoted as SF-TDLCDFTB. The LC technique corrects the overdelocalization of electron density in systems such as charge-transfer systems, which is typically found in conventional DFTB calculations as well as density functional theory calculations using pure functionals. The numerical assessment of the SF-TDDFTB method shows smooth potential curves for the bond dissociation of hydrogen fluoride and the double-bond rotation of ethylene and the double-cone shape of H3 as the simplest degenerate systems. In addition, numerical assessments of SF-TDDFTB and SF-TDLCDFTB for 39 S0/S1 minimum energy conical intersection (MECI) structures are performed. The SF-TDDFTB and SF-TDLCDFTB methods drastically reduce the computational cost with accuracy for MECI structures compared with SF-TDDFT.
KW - conical intersection
KW - degenerate phenomena
KW - long-range correction
KW - spin-flip
KW - time-dependent density functional tight-binding method
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U2 - 10.1002/jcc.26197
DO - 10.1002/jcc.26197
M3 - Article
C2 - 32220108
AN - SCOPUS:85082407886
SN - 0192-8651
VL - 41
SP - 1538
EP - 1548
JO - Journal of Computational Chemistry
JF - Journal of Computational Chemistry
IS - 16
ER -