1. Photo-induced dynamics with continuous and discrete quantum baths
- Author
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Xie, Zhaoxuan, Moroder, Mattia, Schollwöck, Ulrich, and Paeckel, Sebastian
- Subjects
Quantum Physics - Abstract
The ultrafast quantum dynamics of photophysical processes in complex molecules is an extremely challenging computational problem with a wide variety of fascinating applications in quantum chemistry and biology. Inspired by recent developments in open quantum systems, we introduce a pure-state unraveled hybrid-bath method that describes a continuous environment via a set of discrete, effective bosonic degrees of freedom using a Markovian embedding. Our method is capable of describing both, a continuous spectral density and sharp peaks embedded into it. Thereby, we overcome the limitations of previous methods, which either capture long-time memory effects using the unitary dynamics of a set of discrete vibrational modes or use memoryless Markovian environments employing a Lindblad or Redfield master equation. We benchmark our method against two paradigmatic problems from quantum chemistry and biology. We demonstrate that compared to unitary descriptions, a significantly smaller number of bosonic modes suffices to describe the excitonic dynamics accurately, yielding a computational speed-up of nearly an order of magnitude. Furthermore, we take into account explicitly the effect of a $\delta$-peak in the spectral density of a light-harvesting complex, demonstrating the strong impact of the long-time memory of the environment on the dynamics., Comment: Minor changes after publication
- Published
- 2024