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arXiv · 2602.04061

Correlation-Enabled Beatings in Two-Dimensional Electronic Spectroscopy

Sirui Chen·Dragomir Davidović
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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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Sirui Chen, Dragomir Davidović. 2026-02-03. Correlation-Enabled Beatings in Two-Dimensional Electronic Spectroscopy. https://doi.org/10.1103/w496-d4b8

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