Solving Response Expressions in the ADC/ISR Framework

Scheurer, Maximilian; Papapostolou, Antonia; Fransson, Thomas; Norman, Patrick; Dreuw, Andreas; Rehn, Dirk

doi:10.26434/chemrxiv-2022-tcb7t

Cited by 1 publication

(1 citation statement)

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“…12−14 Therefore, the so-called sum-overstates (SOS) expressions or spectral representations of the response functions are reformulated into closed matrix expressions represented in the intermediate states that provide a convenient way to calculate them. This ansatz has already been successfully used in the computation of static and dynamic polarizabilities of the ground state, 15,16 complex excited-state polarizabilities, 17 two-photon absorption (TPA) transition moments, 18 resonant inelastic X-ray scattering (RIXS) amplitudes, 19 and electronic as well as magnetic circular dichroism (ECD and MCD). 20,21 Moreover, this general formalism is also applicable to those higher-order molecular properties required for the CME.…”

Section: ■ Introductionmentioning

confidence: 99%

Cotton-Mouton Effect Using Algebraic Diagrammatic Construction Schemes in the Intermediate State Representation Formalism

Schneider,

Papapostolou,

Leitner

et al. 2023

J. Phys. Chem. A

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The Cotton-Mouton effect is theoretically investigated for a selected set of molecules by using a novel computational methodology based on algebraic diagrammatic construction (ADC) schemes in the intermediate state representation (ISR) formulation. Therefore, the electronic contributions to the frequency-dependent polarizabilities and, for the first time, to the magnetizabilities as well as mixed electric and magnetic hypermagnetizabilities have been computed in the ADC/ISR framework. In addition to calculation of the Cotton-Mouton constant and the birefringence, the gauge origin dependence of the computed tensors and the applied methodology are thoroughly investigated. The new ADC/ISR methodology, employing the recently presented package, is applied to a test set of Ne and small molecules (H2, HF, O2, CO2, and benzene) and compared to data from the experiment as well as other ab initio methods. The presented theoretical ab initio ADC/ISR approach is a substantial extension of the available computational methods for the investigation of complex nonlinear properties, however, with a gauge origin dependence inherent to the method that decreases with increasing perturbation order.

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