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arXiv:2205.11554 · Physical Review Letters

Electro-Optic Fourier Transform Chronometry of Pulsed Quantum Light

Ali Golestani, Alex O. C. Davis, Filip Sośnicki, Michał Mikołajczyk, Nicolas Treps, Michał Karpiński

Published Sep 16, 2022• 9 citations
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Abstract

The power spectrum of an optical field can be acquired without a spectrally resolving detector by means of Fourier-transform spectrometry, based on measuring the temporal autocorrelation of the optical field. Analogously, we here perform temporal envelope measurements of ultrashort optical pulses without time resolved detection. We introduce the technique of Fourier transform chronometry, where the temporal envelope is acquired by measuring the frequency autocorrelation of the optical field in a linear interferometer. We apply our technique, which is the time-frequency conjugate measurement to Fourier-transform spectrometry, to experimentally measure the pulse envelope of classical and single-photon light pulses.

DOI
10.1103/physrevlett.129.123605

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•Aug 3, 2016•0 citations
The power spectrum of an optical field can be acquired without a spectrally resolving detector by means of Fourier-transform spectrometry, based on measuring the temporal autocorrelation of the optical field. Analogously, we here perform temporal envelope measurements of ultrashort optical pulses without time resolved detection. We introduce the technique of Fourier transform chronometry, where the temporal envelope is acquired by measuring the frequency autocorrelation of the optical field in a linear interferometer. We apply our technique, which is the time-frequency conjugate measurement to Fourier-transform spectrometry, to experimentally measure the pulse envelope of classical and single-photon light pulses.
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.
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.
Despite the multitude of available methods, the characterization of ultrafast pulses remains a challenging endeavor, especially at the single-photon level. We introduce a pulse characterization scheme that maps the magnitude of its short-time Fourier transform. Contrary to many well-known solutions it does not require nonlinear effects and is therefore suitable for single-photon-level measurements. Our method is based on introducing a series of controlled time and frequency shifts, where the latter is performed via an electro-optic modulator allowing a fully-electronic experimental control. We characterized the full spectral and temporal width of a classical and single-photon-level pulse and successfully tested the applicability of the reconstruction algorithm of the spectral phase and amplitude. The method can be extended by implementing a phase-sensitive measurement and is naturally well-suited to partially-incoherent light.
Spectral-temporal manipulation of optical pulses has enabled numerous developments within a broad range of research topics, ranging from fundamental science to practical applications. Within quantum optics spectral-temporal degree of freedom of light offers a promising platform for integrated photonic quantum information processing. An important challenge in experimentally realizing spectral-temporal manipulation of quantum states of light is the need for highly efficient manipulation tools. In this context the intrinsically deterministic electro-optic methods show great promise for quantum applications. We experimentally demonstrate application of electro-optic platform for spectral-temporal manipulation of ultrashort pulsed quantum light. Using techniques analogous to serrodyne frequency shifting we show active spectral translation of few-picosecond single photon pulses by up to 0.5 THz. By employing an approach based on an electro-optic time lens we demonstrate up to 6-fold spectral compression of heralded single photon pulses with efficiency that enables us to significantly increase single photon flux through a narrow bandpass filter. We realize the required temporal phase manipulation by driving a lithium niobate waveguided electrooptic modulator with 33 dBm sinusoidal RF field at the frequency of either 10 GHz or 40 GHz. We use a phase lock loop to temporally lock the RF field to the 80 MHz repetition rate of approximately 1 ps long optical pulses. Heralded single photon wavepackets are generated by means of spontaneous parametric down-conversion in potassium dihydrogen phosphate (KDP) crystal, which enables preparation of spectrally pure single photon wavepackets without the need for spectral filtering. Spectral shifting is achieved by locking single-photon pulses to the linear slope of sinusoidal 40 GHz RF phase modulation. We verify the spectral shift by performing spectrally resolved heralded single photon counting, using frequency-to-time conversion by means of a highly dispersive chirped fiber Bragg grating. We verify the non-classicality of spectrally shifted single photons by measuring high-visibility Hong-Ou-Mandel interference using a reference single photon pulse. Spectral compression is based on the time lens principle, which requires locking optical pulses to approximately quadratic region of sinusoidal phase modulation. We utilize both 10 GHz and 40 GHz RF driving frequencies. Bandwidth compression is achieved by chirping the single photon pulse using an appropriate length of single-mode fibre and subsequently subjecting it to the action of the time lens. We verify spectral compression directly using the aforementioned spectrally-resolved heralded single photon counting method. We achieve 3-fold spectral compression of 2 nm bandwidth single photon pulses using 40 GHZ modulation frequency, and 6-fold spectral compression of 0.9 nm bandwidth single photon pulses using 10 GHz modulation frequency. Overall transmission of our set-up exceeding 30% enables practical usability of our spectral compression method which we demonstrate experimentally by showing an increased photon flux through a narrowband filter. Our results present an important contribution towards implementing quantum information processing in the spectral-temporal degree of freedom of a photon. In the context of quantum networks they present an enabling tool towards efficient photonic interfacing of different quantum information processing platforms.