Quantum-light probe for molecular femtosecond dephasing in dyes
Phys. Rev. A 113, 033725 – Published 17 March, 2026
DOI: https://doi.org/10.1103/2zpv-g7w2
Abstract
We report an experimental method that combines quantum interferometry with molecular spectroscopy using indistinguishable photon pairs generated via spontaneous parametric down-conversion of continuous-wave (cw) pump radiation in a Hong-Ou-Mandel (HOM) setup. Introducing a resonant organic medium into one interferometer arm leads to measurable changes in the coincidence signal due to the coherence response of the medium, from which we determine a molecular dephasing time of for concentrations ranging from 2 to . Unlike classical techniques, this approach leverages photon correlations with low photon flux, making it immune to even-order dispersion and insensitive to classical losses. The results align with a theoretical framework that incorporates the joint spectral properties of the photon pair and the molecular transmission response. This work extends the technique of Eshun et al. [J. Am. Chem. Soc. 143, 9070 (2021)] to the cw domain, demonstrating the potential of cw-pumped HOM interferometry for probing ultrafast molecular dynamics and highlighting its promise as a foundation for advanced quantum-light spectroscopic techniques in organic systems.