Correlated-photon time- and frequency-resolved optical spectroscopy

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. Spectroscopy and microscopy schemes that use quantum states of light have been widely described theoretically with fewer experimental demonstrations that typically require very long measurements that can extend for hours or more. Here, we show that time-resolved spectroscopy with quantum light can be performed without compromising measurement time or wavelength tunability, recording a fluorescence lifetime trace in biological samples in less than a second with acceptable signal-to-noise ratio. Starting from spontaneous parametric down-conversion driven by a continuous-wave laser, we exploit the temporal correlation between randomly generated signal/idler pairs to obtain temporal resolution, and their spectral correlation to select the excitation frequency. We also add spectral resolution in detection, using a 'photon-efficient' Fourier transform approach which employs a common-path interferometer. We demonstrate the potential of this approach 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. Our results provide a new approach to ultrafast optical spectroscopy, where experiments are performed under illumination intensity conditions comparable to real-world sunlight illumination.