Ab initio simulation of laser-induced electronic and vibrational coherence

• URL: http://arxiv.org/abs/2112.11083v2
• Date: Mon, 20 Jun 2022 15:02:12 GMT
• Title: Ab initio simulation of laser-induced electronic and vibrational coherence
• Authors: Jannis Krumland, Matheus Jacobs, and Caterina Cocchi
• Abstract summary: 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.
• Score: 0.0
• License: http://arxiv.org/licenses/nonexclusive-distrib/1.0/
• Abstract: The atomistic resolution recently achieved by ultrafast spectroscopies demands corresponding theoretical advances. Real-time time-dependent density-functional theory (RT-TDDFT) with Ehrenfest dynamics offers an optimal trade-off between accuracy and computational costs to study electronic and vibrational dynamics of laser-excited materials in the sub-picosecond regime. However, this approach is unable to account for thermal effects or zero-point energies which are crucial in the physics involved. Herein, we adopt a quantum-semiclassical method based on RT-TDDFT+Ehrenfest to simulate laser-induced electronic and vibrational coherences in condensed matter. With the example of carbon-conjugated molecules, we show that ensemble-averaging with initial configurations from a nuclear quantum distribution remedies many shortcomings of single-trajectory RT-TDDFT+Ehrenfest, damping electronic coherence and introducing ultrafast non-adiabatic coupling between excited states. As the number of sampled configurations decreases with size and rigidity of the compounds, computational costs remain moderate for large systems for which mean-field approaches shine. 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 as an independent counterpart to experimental results.

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