Extended Mixed-Reference Spin-Flip Time-Dependent Density Functional Theory for Charge-Transfer State

Oh, Minseok

doi:10.1021/acs.jctc.6c00454

Extended Mixed-Reference Spin-Flip Time-Dependent Density Functional Theory for Charge-Transfer State

2026-06-09

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AI

O

Oh, Minseok

N

Nakhyun Kim

Y

YounJoon Jung *

C

Cheol Ho Choi *

S

Seunghoon Lee *

DOI：10.1021/acs.jctc.6c00454

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We propose a novel extended mixed-reference spin-flip time-dependent density functional theory (EMRSF-TDDFT). This approach extends MRSF-TDDFT by incorporating electronic configurations present in linear-response TDDFT but absent in conventional MRSF-TDDFT. The formulation is based on the connection between linear-response and MRSF time-dependent Hartree–Fock theories and is extended to TDDFT. Benchmark calculations for representative molecular systems show that the newly introduced configurations capture a major contribution to orbital relaxation effects. This stabilizes both ground and excited states described in the triplet-reference orbital basis and improves agreement with reference theoretical best estimates. We expect that the new EMRSF-TDDFT model is applicable to photochemical processes involving charge transfer.

Extended Mixed-Reference Spin-Flip Time-Dependent Density Functional Theory for Charge-Transfer State

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