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.

Related papers

• Accelerating Electron Dynamics Simulations through Machine Learned Time Propagators [0.9208007322096533]
  We present a novel approach to accelerate real time TDDFT based electron dynamics simulations. By leveraging physics-informed constraints and high-resolution training data, our model achieves superior accuracy and computational speed. This method has potential in enabling real-time, on-the-fly modeling of laser-irradiated molecules and materials.
  arXiv  Detail & Related papers  (2024-07-12T18:29:48Z)
• Single vibronic level fluorescence spectra from Hagedorn wavepacket dynamics [0.0]
  We develop an efficient algorithm to compute the overlaps between two Hagedorn wavepackets. We study the effects of displacement, distortion (squeezing), and Duschinsky rotation on SVL spectra.
  arXiv  Detail & Related papers  (2024-03-01T14:58:07Z)
• Real-Space, Real-Time Approach to Quantum-Electrodynamical Time-Dependent Density Functional Theory [55.41644538483948]
  The equations are solved by time propagating the wave function on a tensor product of a Fock-space and real-space grid. Examples include the coupling strength and light frequency dependence of the energies, wave functions, optical absorption spectra, and Rabi splitting magnitudes in cavities.
  arXiv  Detail & Related papers  (2022-09-01T18:49:51Z)
• Photoinduced prethermal order parameter dynamics in the two-dimensional large-$N$ Hubbard-Heisenberg model [77.34726150561087]
  We study the microscopic dynamics of competing ordered phases in a two-dimensional correlated electron model. We simulate the light-induced transition between two competing phases.
  arXiv  Detail & Related papers  (2022-05-13T13:13:31Z)
• Driving Force and Nonequilibrium Vibronic Dynamics in Charge Separation of Strongly Bound Electron-Hole Pairs [59.94347858883343]
  We study the dynamics of charge separation in one, two and three-dimensional donor-acceptor networks. This allows us to identify the precise conditions in which underdamped vibrational motion induces efficient long-range charge separation.
  arXiv  Detail & Related papers  (2022-05-11T17:51:21Z)
• Ab initio simulation of laser-induced electronic and vibrational coherence [0.0]
  We show that ensemble-averaging with initial configurations from a nuclear quantum distribution remedies many shortcomings of single-trajectory RT-TDDFT+Ehrenfest. The explicit inclusion of a time-dependent pulse in the simulations makes this method a prime advance for first-principles studies of coherent nonlinear spectroscopy.
  arXiv  Detail & Related papers  (2021-12-21T10:30:41Z)
• Gaussian wavepacket model for single-photon generation based on cavity QED in the adiabatic and nonadiabatic conditions [0.0]
  We show how to achieve a high success probability while keeping a short pulse width by optimizing the cavity transmittance parameter. Our formulations provide a practical tool for efficient single-photon generation in a wide variety of experimental platforms.
  arXiv  Detail & Related papers  (2021-12-05T13:34:54Z)
• Simulation of absorption spectra of molecular aggregates: a Hierarchy of Stochastic Pure States approach [68.8204255655161]
  hierarchy of pure states (HOPS) provides a formally exact solution based on local, trajectories. Exploiting the localization of HOPS for the simulation of absorption spectra in large aggregares requires a formulation in terms of normalized trajectories.
  arXiv  Detail & Related papers  (2021-11-01T16:59:54Z)
• Time-resolved Interparticle Coulombic Decay spectra including nuclear degrees of freedom [49.1574468325115]
  We explore the ultra-rapid electronic motion spanning attoseconds to femtoseconds, demonstrating that it is equally integral and relevant to the discipline. The advent of ultrashort attosecond pulse technology has revolutionized our ability to directly observe electronic rearrangements in atoms and molecules.
  arXiv  Detail & Related papers  (2021-02-10T16:51:48Z)
• Fast and differentiable simulation of driven quantum systems [58.720142291102135]
  We introduce a semi-analytic method based on the Dyson expansion that allows us to time-evolve driven quantum systems much faster than standard numerical methods. We show results of the optimization of a two-qubit gate using transmon qubits in the circuit QED architecture.
  arXiv  Detail & Related papers  (2020-12-16T21:43:38Z)
• On-the-fly ab initio semiclassical evaluation of third-order response functions for two-dimensional electronic spectroscopy [0.0]
  We use the single-trajectory semiclassical thawed Gaussian approximation to evaluate two-dimensional electronic spectra. We find that in this molecule, the anharmonicity effects are weak, whereas the Duschinsky rotation and the changes in the mode frequencies must be included in accurate simulations.
  arXiv  Detail & Related papers  (2020-10-06T21:29:11Z)

This list is automatically generated from the titles and abstracts of the papers in this site.

This site does not guarantee the quality of this site (including all information) and is not responsible for any consequences.