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arXiv:1611.02415 · Scientific Reports

Quantum interference in the presence of a resonant medium

Dmitry A. Kalashnikov, Elizaveta Melik-Gaykazyan, А. А. Калачев, Yefeng Yu, Arseniy I. Kuznetsov, Leonid A. Krivitsky

Published Sep 7, 2017• 37 citations
arXivHTMLPDF

Abstract

Interaction of light with media often occurs with a femtosecond response time. Its measurement by conventional techniques requires the use of femtosecond lasers and sophisticated time-gated optical detection. Here we demonstrate that by exploiting quantum interference of entangled photons it is possible to measure the dephasing time of a resonant media on the femtosecond time scale (down to 100 fs) using accessible continuous wave laser and single-photon counting. We insert a sample in the Hong-Ou-Mandel interferometer and observe the modification of the two-photon interference pattern, which is driven by the coherent response of the medium, determined by the dephasing time. The dephasing time is then inferred from the observed pattern. This effect is distinctively different from the basic effect of spectral filtering, which was studied in earlier works. In addition to its ease of use, our technique does not require compensation of group velocity dispersion and does not induce photo-damage of the samples. Our technique will be useful for characterization of ultrafast phase relaxation processes in material science, chemistry, and biology.

DOI
10.1038/s41598-017-11694-z

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Interaction of light with media often occurs with a femtosecond response time. Its measurement by conventional techniques requires the use of femtosecond lasers and sophisticated time-gated optical detection. Here we demonstrate that by exploiting quantum interference of entangled photons it is possible to measure the dephasing time of a resonant media on the femtosecond time scale (down to 100 fs) using accessible continuous wave laser and single-photon counting. We insert a sample in the Hong-Ou-Mandel interferometer and observe the modification of the two-photon interference pattern, which is driven by the coherent response of the medium, determined by the dephasing time. The dephasing time is then inferred from the observed pattern. This effect is distinctively different from the basic effect of spectral filtering, which was studied in earlier works. In addition to its ease of use, our technique does not require compensation of group velocity dispersion and does not induce photo-damage of the samples. Our technique will be useful for characterization of ultrafast phase relaxation processes in material science, chemistry, and biology.
We demonstrate how the Hong-Ou-Mandel (HOM) interference with polarization-entangled photons can be used to probe ultrafast dephasing. We can infer the optical properties like the real and imaginary parts of the complex susceptibility of the medium from changes in the position and the shape of the HOM dip. From the shift of the HOM dip, we are able to measure 22 fs dephasing time using a continuous-wave (CW) laser even with optical loss > 97 %, while the HOM dip visibility is maintained at 92.3 % (which can be as high as 96.7 %). The experimental observations, which are explained in terms of a rigorous theoretical model, demonstrate the utility of HOM interference in probing ultrafast dephasing.
Entangled photon pairs have been used for molecular spectroscopy in the form of entangled two-photon absorption and in quantum interferometry for precise measurements of light source properties and time delays. We present an experiment that combines molecular spectroscopy and quantum interferometry by utilizing the correlations of entangled photons in a Hong-Ou-Mandel (HOM) interferometer to study molecular properties. We find that the HOM signal is sensitive to the presence of a resonant organic sample placed in one arm of the interferometer, and the resulting signal contains information pertaining to the light-matter interaction. We can extract the dephasing time of the coherent response induced by the excitation on a femtosecond time scale. A dephasing time of 102 fs is obtained, which is relatively short compared to times found with similar methods and considering line width broadening and the instrument entanglement time As the measurement is done with coincidence counts as opposed to simply intensity, it is unaffected by even-order dispersion effects, and because interactions with the molecular state affect the photon correlation, the observed measurement contains only these effects and no other classical losses. The experiments are accompanied by theory that predicts the observed temporal shift and captures the entangled photon joint spectral amplitude and the molecule's transmission in the coincidence counting rate. Thus, we present a proof-of-concept experimental method based of entangled photon interferometry that can be used to characterize optical properties in organic molecules and can in the future be expanded on for more complex spectroscopic studies of nonlinear optical properties.
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.
We theoretically investigate the quantum interference of entangled two-photon states generated in a nonlinear crystal pumped by femtosecond optical pulses. Interference patterns generated by the polarization analog of the Hong-Ou-Mandel interferometer are studied. Attention is devoted to the effects of the pump-pulse profile (pulse duration and chirp) and the second-order dispersion in both the nonlinear crystal and the interferometer's optical elements. Dispersion causes the interference pattern to have an asymmetric shape. Dispersion cancellation occurs in some cases.
We report two-photon interference with continuous-wave multi-mode coherent light. We show that the two-photon interference, in terms of the detection time difference, reveals two-photon beating fringes with the visibility V = 0.5. While scanning the optical delay of the interferometer, Hong-Ou-Mandel dips or peaks are measured depending on the chosen detection time difference. The HOM dips/peaks are repeated when the optical delay and the first-order coherence revival period of the multi-mode coherent light are the same. These results help to understand the nature of two-photon interference and also can be useful for quantum information science.
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.