Ultrafast measurement of energy-time entanglement with an optical Kerr shutter
Andrew Cameron, Kate L. Fenwick, Sandra W. L. Cheng, Sacha Schwarz, Benjamin MacLellan, Philip J. Bustard, Duncan G. England, Benjamin Sussman, Kevin J. Resch
Correlations between the temporal and frequency properties of two photons may be exploited for optical quantum technologies, but they can be difficult to measure on ultrafast time scales. In this work, we measure the time-of-arrival correlations of two energy-time entangled photons using an optical Kerr shutter.
The generation of ultrafast laser pulses and the reconstruction of their electric fields is essential for many applications in modern optics. Quantum optical fields can also be generated on ultrafast timescales; however, the tools and methods available for strong laser pulses are not appropriate for measuring the properties of weak, possibly entangled pulses. Here, we demonstrate a method to reconstruct the joint-spectral amplitude of a two-photon energy-time entangled state from joint measurements of the frequencies and arrival times of the photons, and the correlations between them. Our reconstruction method is based on a modified Gerchberg-Saxton algorithm. Such techniques are essential to measure and control the shape of ultrafast entangled photon pulses.
Single photons are a natural platform for quantum technologies as they support entanglement in many degrees of freedom and are inherently well protected from a detrimental type of noise called decoherence. In order to fully exploit photons for quantum technologies, it will be necessary to be able to shape, control, and measure their properties in all degrees of freedom: space, time, frequency, and polarization. \n \n The time-frequency degree of freedom of light is of particular interest for quantum information tasks as it supports various encodings, including frequency bins and time bins, and is intrinsically robust for propagation through long-distance fibre links. Applications which harness quantum correlations in this degree of freedom, referred to as energy-time entanglement, include dispersion cancellation and high-dimensional quantum key distribution. However, detection of this entanglement and observation of these effects requires time resolution beyond the capabilities of current photon detectors. Thus, for operations on ultrafast time scales, more powerful and complex methods are required. \n \n In this thesis, we use a nonlinear technique known as optical gating to surpass the limitations in current detectors and measure single photon pairs, improving the time resolution by two orders of magnitude. When a single photon enters a nonlinear medium at the same time as a strong laser pulse, it may upconvert to a higher energy photon. The strong laser pulse effectively acts as an ultrafast shutter or gate and this creates a high resolution snapshot of the photon in time. Optical gating in conjunction with single photon spectrometers then allow us to measure both the spectral and temporal features of photons on subpicosecond time scales. \n \n These high resolution measurements enable us to explore a host of quantum effects which remained previously inaccessible. First, we directly observe energy-time entanglement, analogous to Einstein-Rosen-Podolsky correlations but \\emph{in frequency and time}. Then, with full control over the dispersion of each photon, we observe nonlocal dispersion cancellation on femtosecond time scales. We also explore ultrafast interferometry in the quantum domain by temporally resolving two-photon interference from a Franson interferometer and observe a violation of the CHSH-Bell inequality. Finally, we show that, using these measurements, it is possible to reconstruct a two-photon energy-time entangled state. Such measurement capabilities will be essential to precisely control both the spectral and temporal shape of entangled photons and to develop new applications in quantum state engineering.
Energy-time entangled photons are critical in many quantum optical phenomena and have emerged as important elements in quantum information protocols. Entanglement in this degree of freedom often manifests itself on ultrafast time scales, making it very difficult to detect, whether one employs direct or interferometric techniques, as photon-counting detectors have insufficient time resolution. Here, we implement ultrafast photon counters based on nonlinear interactions and strong femtosecond laser pulses to probe energy-time entanglement in this important regime. Using this technique and single-photon spectrometers, we characterize all the spectral and temporal correlations of two entangled photons with femtosecond resolution. This enables the witnessing of energy-time entanglement using uncertainty relations and the direct observation of nonlocal dispersion cancellation on ultrafast time scales. These techniques are essential to understand and control the energy-time degree of freedom of light for ultrafast quantum optics.
Many quantum advantages in metrology and communication arise from interferometric phenomena. Such phenomena can occur on ultrafast timescales, particularly when energy-time entangled photons are employed. These have been relatively unexplored as their observation necessitates time resolution much shorter than conventional photon counters. Integrating nonlinear optical gating with conventional photon counters can overcome this limitation and enable subpicosecond time resolution. Here, using this technique and a Franson interferometer, we demonstrate high-visibility quantum interference with two entangled photons, where the one- and two-photon coherence times are both subpicosecond. We directly observe the spectral and temporal interference patterns, measure a visibility in the two-photon coincidence rate of $(85.3\ifmmode\pm\else\textpm\fi{}0.4)%$, and report a Clauser--Horne--Shimony--Holt--Bell parameter of $2.42\ifmmode\pm\else\textpm\fi{}0.02$, violating the local-hidden variable bound by 21 standard deviations. The demonstration of energy-time entanglement with ultrafast interferometry provides opportunities for examining and exploiting entanglement in previously inaccessible regimes.
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.
The time-energy entanglement of down-converted photon pairs is particularly difficult to characterize because direct measurements of photon arrival times are limited by the temporal resolution of photon detection. Here, we explore an alternative possibility of characterizing the temporal coherence of two-photon wave functions using single-photon interference with weak coherent light. Specifically, this method makes use of the fact that down conversion generates a coherent superposition of vacuum and two-photon states, so that the coincidence count rates for photon pairs after interference with weak coherent light are given by a superposition of the two-photon wave function from the down conversion with the product wave function defined by the weak coherent references. By observing the frequency-dependent interference pattern, it is possible to reconstruct the amplitudes and the phases of the two-photon wave function within the bandwidth of the reference pulses used in the single-photon interferences. The correlated single-photon interferences therefore provide a direct map of the entangled two-photon wave function generated in the down-conversion process.