A general implementation of time-dependent vibrational coupled-cluster theory

Madsen, N.; Jensen, Andreas Buchgraitz; Hansen, Mads Bøttger; Christiansen, Ove

doi:10.1063/5.0034013

Cited by 10 publications

(6 citation statements)

References 53 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Any other wave function propagation methods capable of providing time-dependent reduced one-body densities will also be applicable in this context. In future work, we will use the methodology in conjunction with the time-dependent vibrational coupled cluster with time-dependent modals methods, − offering new attractive compromises between accuracy and efficiency.…”

Section: Discussionmentioning

confidence: 99%

“…The TD-ADGA procedure can generally be used with any time-dependent wave function method as long as a wave function density can be formulated. In future work, we expect to combine the methods with time-dependent vibrational coupled cluster methods. − In this work, we exclusively consider single surface computations. The wave function may be initiated from a wave function obtained on another surface but the simulated time-dependent dynamics and PES construction is restricted to a single surface.…”

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Quasi-direct Quantum Molecular Dynamics: The Time-Dependent Adaptive Density-Guided Approach for Potential Energy Surface Construction

Høyer,

Christiansen

2024

J. Chem. Theory Comput.

Self Cite

View full text Add to dashboard Cite

We present a new quasi-direct quantum molecular dynamics computational method which offers a compromise between quantum dynamics using a precomputed potential energy surface (PES) and fully direct quantum dynamics. This method is termed the time-dependent adaptive density-guided approach (TD-ADGA) and is a method for constructing a PES on the fly during a dynamics simulation. This is achieved by acquisition of new single-point (SP) calculations and refitting of the PES, depending on the need of the dynamics. The TD-ADGA is a further development of the adaptive density-guided approach (ADGA) for PES construction where the placement of SPs is guided by the density of the nuclear wave function. In TD-ADGA, the ADGA framework has been integrated into the time propagation of the time-dependent nuclear wave function and we use the reduced one-mode density of this wave function to guide when and where new SPs are placed. The PES is thus extended or updated if the wave function moves into new areas or if a certain area becomes more important. Here, we derive equations for the reduced one-mode density for the timedependent Hartree (TDH) method and for multiconfiguration time-dependent Hartree (MCTDH) methods, but the TD-ADGA can be used with any time-dependent wave function method as long as a density is available. The TD-ADGA method has been investigated on molecular systems containing single-and double-minimum potentials and on single-mode and multi-mode systems. We explore different approaches to handle the fact that the TD-ADGA involves a PES that changes during the computation and show how results can be obtained that are in very good agreement with results obtained by using an accurate reference PES. Dynamics with TD-ADGA is essentially a black box procedure, where only the initialization of the system and how to compute SPs must be provided. The TD-ADGA thus makes it easier to carry out quantum molecular dynamics and the quasi-direct framework opens up the possibility to compute quantum dynamics accurately for larger molecular systems.

show abstract

Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Quasi-direct Quantum Molecular Dynamics: The Time-Dependent Adaptive Density-Guided Approach for Potential Energy Surface Construction

Høyer,

Christiansen

2024

J. Chem. Theory Comput.

Self Cite

View full text Add to dashboard Cite

show abstract

“…In a follow‐up study, 129 an automated implementation of the full hierarchy of TCVCC[ n ] approximations was presented. Again, the Dormand–Prince 8(5,3) method was the chosen integrator for the numerical studies.…”

Section: Time‐dependent Vibrational Coupled‐cluster Theorymentioning

confidence: 99%

Time‐dependent coupled‐cluster theory

Ofstad

Aurbakken

Schøyen

et al. 2023

WIREs Comput Mol Sci

View full text Add to dashboard Cite

Recent years have witnessed an increasing interest in time‐dependent coupled‐cluster (TDCC) theory for simulating laser‐driven electronic dynamics in atoms and molecules, and for simulating molecular vibrational dynamics. Starting from the time‐dependent bivariational principle, we review different flavors of single‐reference TDCC theory with either orthonormal static, orthonormal time‐dependent, or biorthonormal time‐dependent spin orbitals. The time‐dependent extension of equation‐of‐motion coupled‐cluster theory is also discussed, along with the applications of TDCC methods to the calculation of linear absorption spectra, linear and low‐order nonlinear response functions, highly nonlinear high harmonic generation spectra and ionization dynamics. In addition, the role of TDCC theory in finite‐temperature many‐body quantum mechanics is briefly described along with a few other application areas.This article is categorized under: Electronic Structure Theory > Ab Initio Electronic Structure Methods Theoretical and Physical Chemistry > Spectroscopy Software > Simulation Methods

show abstract

“…4. Instead, the FSMR framework has been used in the small-basis calculations, and the calculations in larger basis sets have been performed using a new general excitation level TDVCC implementation 46 (not covering TDMVCC). The results clearly demonstrate that even in a much larger modal basis, the TDVCC [2] method is still inferior to TDMVCC [2].…”

Section: Intramolecular Vibrational-energy Redistribution Of Watermentioning

confidence: 99%

Time-dependent vibrational coupled cluster with variationally optimized time-dependent basis sets

Madsen

Hansen

Christiansen

et al. 2020

The Journal of Chemical Physics

Self Cite

View full text Add to dashboard Cite

show abstract

A general implementation of time-dependent vibrational coupled-cluster theory

Abstract: A general implementation of timedependent vibrational coupled-cluster theory

Cited by 10 publications

References 53 publications

Quasi-direct Quantum Molecular Dynamics: The Time-Dependent Adaptive Density-Guided Approach for Potential Energy Surface Construction

Quasi-direct Quantum Molecular Dynamics: The Time-Dependent Adaptive Density-Guided Approach for Potential Energy Surface Construction

Time‐dependent coupled‐cluster theory

Time-dependent vibrational coupled cluster with variationally optimized time-dependent basis sets

Contact Info

Product

Resources

About