Algebraic diagrammatic construction schemes for the simulation of electronic spectroscopies

Dreuw, Andreas; Dempwolff, Adrian L.

doi:10.1016/b978-0-323-91738-4.00012-9

Cited by 4 publications

(1 citation statement)

References 62 publications

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“…Under particular approximations, it is possible to circumvent the direct solution of the time-dependent Schrödinger equation (TDSE) in favor of time-dependent perturbation theory (or “frequency-domain” methods), which aims to implicitly access quantum dynamics through probing the spectral structure of the Hamiltonian operator. In the context of electronic structure theory, these approaches include linear-response, − polarization propagator, − and equation-of-motion − methods, among others. − While these methods can often be a powerful tool for the simulation and prediction of observable phenomena such as spectroscopies, their veracity depends on the applicability of their various approximations to accurately characterize queried physical conditions. Further, the vast majority of these perturbative methods serve to access the equilibrium behavior of electronic dynamics, leaving nonequilibrium phenomena, such as charge migration, inaccessible.…”

Section: Introductionmentioning

confidence: 99%

Approximate Exponential Integrators for Time-Dependent Equation-of-Motion Coupled Cluster Theory

Williams-Young,

Yuwono,

DePrince III

et al. 2023

J. Chem. Theory Comput.

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With a growing demand for time-domain simulations of correlated many-body systems, the development of efficient and stable integration schemes for the time-dependent Schrödinger equation is of keen interest in modern electronic structure theory. In this work, we present two approaches for the formation of the quantum propagator for time-dependent equation-of-motion coupled cluster theory based on the Chebyshev and Arnoldi expansions of the complex, nonhermitian matrix exponential, respectively. The proposed algorithms are compared with the short-iterative Lanczos method of Cooper et al. [ J. Phys. Chem. A 2021 125 , 5438–5447], the fourth-order Runge–Kutta method, and exact dynamics for a set of small but challenging test problems. For each of the cases studied, both of the proposed integration schemes demonstrate superior accuracy and efficiency relative to the reference simulations.

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Section: Introductionmentioning

confidence: 99%

Approximate Exponential Integrators for Time-Dependent Equation-of-Motion Coupled Cluster Theory

Williams-Young,

Yuwono,

DePrince III

et al. 2023

J. Chem. Theory Comput.

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Efficient and Parallel Implementation of Real and Complex Response Functions Employing the Second-Order Algebraic-Diagrammatic Construction Scheme for the Polarization Propagator

Brand,

Dreuw,

Norman

et al. 2023

J. Chem. Theory Comput.

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We present the implementation of an efficient matrix-folded formalism for the evaluation of complex response functions and the calculation of transition properties at the level of the second-order algebraicdiagrammatic construction (ADC(2)) scheme. The underlying algorithms, in combination with the adopted hybrid MPI/OpenMP parallelization strategy, enabled calculations of the UV/vis spectra of a guanine oligomer series ranging up to 1032 contracted basis functions, thereby utilizing vast computational resources from up to 32,768 CPU cores. Further analysis of the convergence behavior of the involved iterative subspace algorithms revealed the superiority of a frequency-separated treatment of response equations even for a large spectral window, including 101 frequencies. We demonstrate the applicability to general quantum mechanical operators by the first reported electronic circular dichroism spectrum calculated with a complex polarization propagator approach at the ADC(2) level of theory.

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In silico photochemistry

Curchod

2024

Photochemistry

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The goal of this Chapter is to provide examples attesting to the maturity of current strategies for simulating the excited-state dynamics and nonradiative processes of molecules in the gas phase. Such progress over the past few decades means that we are approaching the possibility of performing in silico photochemistry, i.e., a photochemical experiment taking place fully on the computer and allowing for the prediction of photochemical processes and observables – at least qualitatively. We provide here a brief survey of nonadiabatic molecular dynamics and the creation of a hierarchy of methods within the multiple spawning framework. We then show how nonadiabatic molecular dynamics techniques can be used in the context of atmospheric photochemistry.

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Algebraic diagrammatic construction schemes for the simulation of electronic spectroscopies

Cited by 4 publications

References 62 publications

Approximate Exponential Integrators for Time-Dependent Equation-of-Motion Coupled Cluster Theory

Approximate Exponential Integrators for Time-Dependent Equation-of-Motion Coupled Cluster Theory

Efficient and Parallel Implementation of Real and Complex Response Functions Employing the Second-Order Algebraic-Diagrammatic Construction Scheme for the Polarization Propagator

In silico photochemistry

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