Electronic decoherence along a single nuclear trajectory

We describe an approach to subsystem decoherence without the usual tracing out of the environment. The subsystem of focus is described entirely by a pure state evolving nonunitarily along a single classical trajectory of its environment. The approach is deduced from the exact factorization framework for arbitrary systems of electrons and nuclei. The nonunitarity of the electronic dynamics arises exclusively from nonadiabatic correlations between electrons and nuclei. We demonstrate that the approach correctly describes the coherence gain and the subsequent decoherence for the example of a nuclear trajectory passing through an avoided crossing, the prototypical case where single-trajectory Ehrenfest dynamics fails to produce decoherence.

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Publication Details

Journal
Physical Review Research
Published
2025-10-17
DOI
https://doi.org/10.1103/nnkr-phm5
Primary Topic
Spectroscopy and Quantum Chemical Studies
Type
article
Field-Weighted Citation Impact
0.00
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article

Electronic decoherence along a single nuclear trajectory

E. K. U. Gross, Matisse Wei-Yuan Tu
Physical Review Research
Spectroscopy and Quantum Chemical Studies
article

Electronic decoherence along a single nuclear trajectory

E. K. U. Gross, Matisse Wei-Yuan Tu
article en

Abstract

We describe an approach to subsystem decoherence without the usual tracing out of the environment. The subsystem of focus is described entirely by a pure state evolving nonunitarily along a single classical trajectory of its environment. The approach is deduced from the exact factorization framework for arbitrary systems of electrons and nuclei. The nonunitarity of the electronic dynamics arises exclusively from nonadiabatic correlations between electrons and nuclei. We demonstrate that the approach correctly describes the coherence gain and the subsequent decoherence for the example of a nuclear trajectory passing through an avoided crossing, the prototypical case where single-trajectory Ehrenfest dynamics fails to produce decoherence.

Physical Review ResearchVol. 7(4)
Hebrew University of Jerusalem (IL), Max Planck Institute for the Structure and Dynamics of Matter (DE)
Openalex Percentile: Top 76%
Spectroscopy and Quantum Chemical Studies
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Electronic decoherence along a single nuclear trajectory — E. K. U. Gross, Matisse Wei-Yuan Tu · Physical Review Research (2025) | TGRS Research Map | TGRS