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arXiv · 2606.30569

Revisiting crossed-correlated baths in open quantum systems simulated by HEOM or T-TEDOPA

Brieuc Le Dé·Etienne Mangaud·Alex W. Chin·Michèle Desouter-Lecomte
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Abstract

Excited-state dynamics of open quantum systems is analyzed by the hierarchical equations of motion (HEOM) or the thermalized time-evolving density operator with orthogonal polynomials algorithm (T-TEDOPA) method when a discrete $ab$ $initio$ linear vibronic model is parametrized by continuous temperature-dependent spectral densities leading to crossed correlation functions, i.e. correlated fluctuations of the energy gap collective modes. We focus on a conical intersection involving two collective modes tuning the energy of each excited state and we revisit the transformation of the initial correlated tuning baths to de-correlated shared baths in order to reduce the computational resources. While a completely frequency-dependent transformation poses problems for HEOM, we find that in some particular cases, an optimal approximate frequency-independent transformation may be derived. On the contrary, T-TEDOPA is very efficient and allows to use this frequency-dependent transformation at the price of managing long-range couplings in the tensor chain. An illustrative application is shown by using the linear vibronic coupling model of a planar symmetrical (phenylethynyl)benzene dimer.

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Brieuc Le Dé, Etienne Mangaud, Alex W. Chin, Michèle Desouter-Lecomte. 2026-06-29. Revisiting crossed-correlated baths in open quantum systems simulated by HEOM or T-TEDOPA. https://arxiv.org/abs/2606.30569

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