Entangled-photon time- and frequency-resolved optical spectroscopy
- URL: http://arxiv.org/abs/2505.02940v1
- Date: Mon, 05 May 2025 18:17:00 GMT
- Title: Entangled-photon time- and frequency-resolved optical spectroscopy
- Authors: Raul Alvarez-Mendoza, Lorenzo Uboldi, Ashley Lyons, Richard Cogdell, Giulio Cerullo, Daniele Faccio,
- Abstract summary: We show that time-resolved spectroscopy with quantum light can be performed without compromising measurement time.<n>Our results provide a new approach to ultrafast optical spectroscopy, where experiments are performed under conditions comparable to real-world sunlight illumination.
- Score: 0.9917784471651826
- License: http://creativecommons.org/licenses/by/4.0/
- Abstract: 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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