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arXiv:2211.09083 · Optics Express

Probing ultra-fast dephasing via entangled photon pairs

Xinghua Liu, Tian Li, Jiaxuan Wang, Mrunal Kamble, Aleksei M. Zheltikov, G. S. Agarwal

Published Dec 6, 2022• 8 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1364/oe.480300

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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.
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.
The Hong-Ou-Mandel (HOM) effect ranks among the most notable quantum interference phenomena, and is central to many applications in quantum technologies. The fundamental effect appears when two independent and indistinguishable photons are superimposed on a beam splitter, which achieves a complete suppression of coincidences between the two output ports. Much less studied, however, is when the fields share coherence (continuous-wave lasers) or mode envelope properties (pulsed lasers). In this case, we expect the existence of two distinct and concurrent HOM interference regimes: the traditional HOM dip on the coherence length time scale, and a structured HOM interference pattern on the pulse length scale. We develop a theoretical framework that describes HOM interference for laser fields having arbitrary temporal waveforms and only partial overlap in time. We observe structured HOM interference from a continuous-wave laser via fast polarization modulation and time-resolved single photon detection fast enough to resolve these structured HOM dips.
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.
Two-photon interference, commonly known as Hong-Ou-Mandel (HOM) interference [1] , has attracted a great deal of interest in quantum sensing, including the precision timing measurements [2] and quantum optical coherence tomography [3] . While the dip of the HOM interference is the direct measure of the purity of the single-photon, the width of the HOM dip relates to the coherence time of the interfering photons. The broad consensus for using the HOM interferometer for sensing application remained the HOM dip width as the limiting factor for the precision measurements. As a consequence, the ultra-broadband photon sources have long been hailed as a vital prerequisite for ultra-precise HOM interferometry. Here, we have studied the variation in the width of the HOM dip with the crystal length for the continuous-wave pump laser and measured the HOM dip as low as 8.2 ± 0.2 µm corresponding to the spectral width of the single-photon source of 79.6±1.9 nm useful for sensitive sensing applications.
Entanglement swapping enables the distribution of quantum states over long distances. In this protocol, a Bell state measurement projects photons, which were created in separate entangled photon sources, into an entangled state when their corresponding pairs interfere at a beamsplitter. This process is optimally realized when the photons are indistinguishable in all degrees of freedom, resulting in Hong-Ou-Mandel (HOM) interference. Since its initial proposal by [1], several experimental realizations have used pulsed, synchronized pumps, as in [2] to achieve temporal indistiguishability. In the case of continuous wave (CW) pumping, the sources are not synchronized, requiring post-selection of the coincidence events after detection. This requires detectors with a temporal resolution greater than the coherence time of the photons. Previous experiments have successfully observed HOM interference using periodically poled Lithium Niobate (ppLN) waveguides and superconducting nanowire single-photon detectors (SNSPDs) [3], also with hybrid sources to improve coincidence rates and HOM visibility [4], [5].
Due to the simplicity of Hong-Ou-Mandel (HOM) interferometer setup, it becomes very important in various quantum-based applications, especially when the photon indistinguishability is required such as measurement device independent quantum key distribution (MDI-QKD). In the present work, the HOM experiment setup is designed to study the quantum interference between two indistinguishable photons (frequency, time of arrival and polarization should be same for both photons) coming from two independent laser sources (attenuated laser). The aim is to achieve high visibility as it indicates the photon indistinguishability from two independent sources. Theoretically, the visibility is 50%50 \%50% for indistinguishable photons from attenuated laser sources but in the experiment, due to various devices imperfections and other factors it is less than 50%. The HOM visibility achieved from our setup is 40%40 \%40% tested for a distance of 20 km over standard single mode fiber (SMF). The main point to be noticed in this work is that, this experiment is performed using single photon avalanche diode.