Time dependent Vibrational Electronic Coupled Cluster (VECC) theory for non-adiabatic nuclear dynamics

• URL: http://arxiv.org/abs/2312.14164v1
• Date: Sat, 2 Dec 2023 20:53:22 GMT
• Title: Time dependent Vibrational Electronic Coupled Cluster (VECC) theory for non-adiabatic nuclear dynamics
• Authors: Songhao Bao, Neil Raymond, Marcel Nooijen
• Abstract summary: A time-dependent vibrational electronic coupled-cluster approach is proposed to simulate photoelectron/ UV-VIS absorption spectra. A detailed derivation of the equations of motion and a motivation of the ansatz is presented. To illustrate the capabilities the VECC method is also applied successfully to a large vibronic model for hexahelicene.
• Score: 0.0
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: A time-dependent vibrational electronic coupled-cluster (VECC) approach is proposed to simulate photoelectron/ UV-VIS absorption spectra, as well as time-dependent properties for non-adiabatic vibronic models, going beyond the Born-Oppenheimer approximation. A detailed derivation of the equations of motion and a motivation of the ansatz are presented. The VECC method employs second-quantized bosonic construction operators and a mixed linear and exponential ansatz to form a compact representation of the time-dependent wave-function. Importantly, the method does not require a basis set, has only few user-defined inputs, and has a classical (polynomial) scaling with respect to the number of degrees of freedom (of the vibronic model), resulting in a favourable computational cost. In benchmark applications to small models and molecules the VECC method provides accurate results, compared to Multi-Configurational Time-dependent Hartree (MCTDH) calculations when predicting short-time dynamical properties (i.e. photo-elecron / UV-VIS absorption spectra) for non-adiabatic vibronic models. To illustrate the capabilities the VECC method is also applied successfully to a large vibronic model for hexahelicene with 14 electronic states and 63 normal modes, developed in the group by Santoro.

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