Many-body Interactions in Ultrafast Spectroscopy

Abstract

Nonlinear spectroscopy is widely used to probe ultrafast dynamics in matter. Signals of higher nonlinear orders encode valuable many-body dynamics but only recently have become individually retrievable. However, their physical interpretation in terms of double-sided Feynman diagrams is cumbersome and non-intuitive. Here, we establish an alternative framework that connects them to the underlying excitation conditions and many-body interactions. This approach predicts two classes of dynamic nonlinearities, due either to direct many-body interactions or to saturable kinetic channels. The method provides a direct physical interpretation of the retrieved signals, explaining their sign, magnitude, and dynamics. It also enables model-free reconstruction of the dynamics of a sub-ensemble of particles starting with a given number of excitons, which we demonstrate to be especially insightful. We validate the framework using colloidal CdSe/CdS core/shell quantum dots, which enable us to model nonlinearities of both classes in isolation and also combined.

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BibTeX RIS

BibTeX

@misc{florio2026manybody,
  title = {{Many-body Interactions in Ultrafast Spectroscopy}},
  author = {Diego Florio and Alessandro Baserga and Sofia Bertuetti and Federico Visentin and Adar Levi and Uri Banin and Giulio Cerullo and Franco V. A. Camargo},
  howpublished = {arXiv},
  year = {2026},
  month = oct,
  doi = {10.48550/arxiv.2610.07213},
  eprint = {2610.07213},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2610.07213},
  note = {CC BY-NC-SA 4.0},
}

RIS

TY  - UNPB
TI  - Many-body Interactions in Ultrafast Spectroscopy
AU  - Diego Florio
AU  - Alessandro Baserga
AU  - Sofia Bertuetti
AU  - Federico Visentin
AU  - Adar Levi
AU  - Uri Banin
AU  - Giulio Cerullo
AU  - Franco V. A. Camargo
PY  - 2026
DA  - 2026/10/05
PB  - arXiv
DO  - 10.48550/arxiv.2610.07213
UR  - https://arxiv.org/abs/2610.07213
AB  - Nonlinear spectroscopy is widely used to probe ultrafast dynamics in matter. Signals of higher nonlinear orders encode valuable many-body dynamics but only recently have become individually retrievable. However, their physical interpretation in terms of double-sided Feynman diagrams is cumbersome and non-intuitive. Here, we establish an alternative framework that connects them to the underlying excitation conditions and many-body interactions. This approach predicts two classes of dynamic nonlinearities, due either to direct many-body interactions or to saturable kinetic channels. The method provides a direct physical interpretation of the retrieved signals, explaining their sign, magnitude, and dynamics. It also enables model-free reconstruction of the dynamics of a sub-ensemble of particles starting with a given number of excitons, which we demonstrate to be especially insightful. We validate the framework using colloidal CdSe/CdS core/shell quantum dots, which enable us to model nonlinearities of both classes in isolation and also combined.
ER  -

Abstract

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