Entangled-photon time- and frequency-resolved optical spectroscopy

Fuente: arXiv
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Autores principales: Alvarez-Mendoza, Raul, Uboldi, Lorenzo, Lyons, Ashley, Cogdell, Richard, Cerullo, Giulio, Faccio, Daniele
Formato: Preprint
Publicado: 2025
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author Alvarez-Mendoza, Raul
Uboldi, Lorenzo
Lyons, Ashley
Cogdell, Richard
Cerullo, Giulio
Faccio, Daniele
author_facet Alvarez-Mendoza, Raul
Uboldi, Lorenzo
Lyons, Ashley
Cogdell, Richard
Cerullo, Giulio
Faccio, Daniele
contents Classical time-resolved optical spectroscopy experiments are performed using sequences of ultrashort light pulses, with photon fluxes incident on the sample which are many orders of magnitude higher than real-world conditions corresponding to sunlight illumination. Here we overcome this paradigm by exploiting quantum correlations to perform time-resolved spectroscopy with entangled photons. Starting from spontaneous parametric down-conversion driven by a continuous-wave laser, we exploit the temporal entanglement between randomly generated signal/idler pairs to obtain temporal resolution, and their spectral entanglement to select the excitation frequency. We also add spectral resolution in detection, using a Fourier transform approach which employs a common-path interferometer. We demonstrate the potential of our entangled-photon streak camera by resolving, at the single-photon level, excitation energy transfer cascades from LH2 to LH1 in the photosynthetic membrane and disentangling the lifetimes of two dyes in a mixture. We show that time-resolved spectroscopy with quantum light can be performed without compromising measurement time, recording a fluorescence time trace in less than a minute even for samples with low quantum yield, which can be reduced to sub-second times with acceptable signal-to-noise ratio. Our results provide a new approach to ultrafast optical spectroscopy, where experiments are performed under conditions comparable to real-world sunlight illumination.
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id arxiv_https___arxiv_org_abs_2505_02940
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Entangled-photon time- and frequency-resolved optical spectroscopy
Alvarez-Mendoza, Raul
Uboldi, Lorenzo
Lyons, Ashley
Cogdell, Richard
Cerullo, Giulio
Faccio, Daniele
Quantum Physics
Optics
Classical time-resolved optical spectroscopy experiments are performed using sequences of ultrashort light pulses, with photon fluxes incident on the sample which are many orders of magnitude higher than real-world conditions corresponding to sunlight illumination. Here we overcome this paradigm by exploiting quantum correlations to perform time-resolved spectroscopy with entangled photons. Starting from spontaneous parametric down-conversion driven by a continuous-wave laser, we exploit the temporal entanglement between randomly generated signal/idler pairs to obtain temporal resolution, and their spectral entanglement to select the excitation frequency. We also add spectral resolution in detection, using a Fourier transform approach which employs a common-path interferometer. We demonstrate the potential of our entangled-photon streak camera by resolving, at the single-photon level, excitation energy transfer cascades from LH2 to LH1 in the photosynthetic membrane and disentangling the lifetimes of two dyes in a mixture. We show that time-resolved spectroscopy with quantum light can be performed without compromising measurement time, recording a fluorescence time trace in less than a minute even for samples with low quantum yield, which can be reduced to sub-second times with acceptable signal-to-noise ratio. Our results provide a new approach to ultrafast optical spectroscopy, where experiments are performed under conditions comparable to real-world sunlight illumination.
title Entangled-photon time- and frequency-resolved optical spectroscopy
topic Quantum Physics
Optics
url https://arxiv.org/abs/2505.02940