Details

Autor(en) / Beteiligte

• Mosquera, Martín A
• Jones, Leighton O
• Kang, Gyeongwon
• Ratner, Mark A
• Schatz, George C

Titel

Second Linear Response Theory and the Analytic Calculation of Excited-State Properties

Ist Teil von

• The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory, 2021-02, Vol.125 (4), p.1093-1102

Ort / Verlag

United States: American Chemical Society

Erscheinungsjahr

2021

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• We present a method based on second linear response time-dependent density functional theory (TDDFT) to calculate permanent and transition multipoles of excited states, which are required to compute excited-state absorption/emission spectra and multiphoton optical processes, among others. In previous work, we examined computations based on second linear response theory in which linear response TDDFT was employed twice. In contrast, the present methodology requires information from only a single linear response calculation to compute the excited-state properties. These are evaluated analytically through various algebraic operations involving electron repulsion integrals and excitation vectors. The present derivation focuses on full many-body wave functions instead of single orbitals, as in our previous approach. We test the proposed method by applying it to several diatomic and triatomic molecules. This shows that the computed excited-state dipoles are consistent with respect to reference equation-of-motion coupled-cluster calculations.