Correlation-Enabled Beatings in Two-Dimensional Electronic Spectroscopy
Fuente:
arXiv
Saved in:
| Main Authors: | , |
|---|---|
| Format: | Preprint |
| Published: |
2026
|
| Subjects: | |
| Online Access: | |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1866908811502026752 |
|---|---|
| author | Chen, Sirui Davidović, Dragomir |
| author_facet | Chen, Sirui Davidović, Dragomir |
| contents | 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. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2602_04061 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Correlation-Enabled Beatings in Two-Dimensional Electronic Spectroscopy Chen, Sirui Davidović, Dragomir Quantum Physics 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. |
| title | Correlation-Enabled Beatings in Two-Dimensional Electronic Spectroscopy |
| topic | Quantum Physics |
| url | https://arxiv.org/abs/2602.04061 |