Correlation-Enabled Beatings in Two-Dimensional Electronic Spectroscopy

TL;DR

This paper reveals that long-lived beatings observed in two-dimensional electronic spectroscopy can be explained by a correlation-driven mechanism involving slow bath memory and ultrafast pulses, challenging standard models.

Contribution

It introduces a new correlation-driven mechanism explaining persistent beatings, emphasizing the role of ultrafast pulse sequences and bath correlations in 2DES.

Findings

Persistent beatings arise from correlation-driven effects.

Ultrafast pulses propagate system-bath correlations.

Long-lived coherence signatures are protocol-level dynamical effects.

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.