Correlation-Enabled Beatings in Two-Dimensional Electronic Spectroscopy
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.
Cite
@article{arxiv.2602.04061,
title = {Correlation-Enabled Beatings in Two-Dimensional Electronic Spectroscopy},
author = {Sirui Chen and Dragomir Davidović},
journal= {arXiv preprint arXiv:2602.04061},
year = {2026}
}