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Correlation-Enabled Beatings in Two-Dimensional Electronic Spectroscopy

arXiv
Authors: Sirui Chen, Dragomir Davidović

Year

2026

Paper ID

2899

Status

Preprint

Abstract Read

~2 min

Abstract Words

109

Citations

N/A

Abstract

Long-lived beatings in two-dimensional electronic spectroscopy (2DES) remain difficult to interpret within standard excitonic open-system models, which typically assume factorized initialization and predict rapid coherence decay. We show that persistent beatings can arise from a correlation-driven mechanism that requires both slow bath memory and ultrafast pulse sequences that propagate system-bath correlations across optical interactions. In this regime, the pulse sequence unitarily dresses the bath-memory contribution and activates nonsecular population-coherence transfer during field-free evolution, sustaining coherence signatures far beyond factorized or weak-memory descriptions. Rather than addressing what is oscillating (excitonic versus vibronic) or quantum-versus-classical semantics, this work reframes long-lived beatings as a protocol-level dynamical effect: correlation-mediated retrieval under ultrafast control.

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  • Long-lived beatings in two-dimensional electronic spectroscopy (2DES) remain difficult to interpret within standard excitonic open-system models, which typically assume...

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