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arXiv:2104.04656 · The Journal of Chemical Physics

Designing high-power, octave spanning entangled photon sources for quantum spectroscopy

Szilárd Szőke, Manni He, Bryce P. Hickam, Scott K. Cushing

Published Jun 23, 2021• 14 citations
arXivHTMLPDF

Abstract

Entangled photon spectroscopy is a nascent field that has important implications for measurement and imaging across chemical, biology, and materials fields. Entangled photon spectroscopy potentially offers improved spatial and temporal-frequency resolutions, increased cross sections for multiphoton and nonlinear measurements, and new abilities in inducing or measuring quantum correlations. A critical step in enabling entangled photon spectroscopies is the creation of high-flux entangled sources that can use conventional detectors as well as provide redundancy for the losses in realistic samples. Here, we report a periodically poled, chirped, lithium tantalate platform that generates entangled photon pairs with ∼10−7 efficiency. For a near watt level diode laser, this results in a near μW-level flux. The single photon per mode limit that is necessary to maintain non-classical photon behavior is still satisfied by distributing this power over up to an octave-spanning bandwidth. The spectral–temporal photon correlations are observed via a Michelson-type interferometer that measures the broadband Hong–Ou–Mandel two-photon interference. A coherence time of 245 fs for a 10 nm bandwidth in the collinear case and a coherence time of 62 fs for a 125 nm bandwidth in the non-collinear case are measured using a CW pump laser and, essentially, collecting the full photon cone. We outline in detail the numerical methods used for designing and tailoring the entangled photons source, such as changing center wavelength or bandwidth, with the ultimate aim of increasing the availability of high-flux UV–Vis entangled photon sources in the optical spectroscopy community.

DOI
10.1063/5.0053688

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We demonstrate an efficient generation of frequency anti-correlated entangled photon pairs at telecom wavelength. The fundamental laser is a continuous-wave high-power fiber laser at 1560 nm, through an extracavity frequency doubling system, a 780-nm pump with a power as high as 742 mW is realized. After single-passing through a periodically poled KTiOPO4 (PPKTP) crystal, degenerate down-converted photon pairs are generated. With an overall detection efficiency of 14.8 %, the count rates of the single photons and coincidence of the photon pairs are measured to be 370 kHz and 22 kHz, respectively. The spectra of the signal and idler photons are centered at 1560.23 and 1560.04 nm, while their 3-dB bandwidths being 3.22 nm both. The joint spectrum of the photon pair is observed to be frequency anti-correlated and have a spectral bandwidth of 0.52 nm. According to the ratio of the single-photon spectral bandwidth to the joint spectral bandwidth of the photon pairs, the degree of frequency entanglement is quantified to be 6.19. Based on a Hong–Ou–Mandel interferometric coincidence measurement, a frequency indistinguishability of 95 % is demonstrated. The good agreements with the theoretical estimations show that the inherent extra intensity noise in fiber lasers has little influence on frequency entanglement of the generated photon pairs.
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As some of the most promising quantum applications such as high resolution quantum optical coherence tomography (QOCT) [1] with dispersion cancellation as well as quantum key distribution require frequency entanglement. Therefore, frequency entanglement light sources are an essential importance for implement of many quantum optical applications. So Far, the most prominent method used for the entangled photon pair generation is spontaneous parametric down-conversion (SPDC) in nonlinear crystals. Recently, with adopting chirp quasi-phase matching (QPM) PPSLT (periodically poled stoichiometric lithium tantalate) has been used as source of entangled photons with large bandwidth [2]. However, improving the overall system efficiency is still remain challenging.
Broadband quantum light is a vital resource for quantum metrology and spectroscopy applications such as quantum optical coherence tomography or entangled two photon absorption. For entangled two photon absorption in particular, very high photon flux combined with high time-frequency entanglement is crucial for observing a signal. So far these conditions could be met by using high power lasers driving degenerate, type 0 bulk-crystal spontaneous parametric down conversion (SPDC) sources. This naturally limits the available wavelength ranges and precludes deterministic splitting of the generated output photons. In this work we demonstrate an integrated two-colour SPDC source utilising a group-velocity matched lithium niobate waveguide, reaching both exceptional brightness 1.52⋅10 6 pairssmWGHz and large bandwidth (7.8 THz FWHM) while pumped with a few mW of continuous wave (CW) laser light. By converting a narrow band pump to broadband pulses the created photon pairs show correlation times of Δ τ ≈ 120 fs while maintaining the narrow bandwidth Δ ω p ≪ 1 MHz of the CW pump light, yielding strong time-frequency entanglement. Furthermore our process can be adapted to a wide range of central wavelengths.
This thesis describes work on single-photon pair creation, entanglement and entanglement measurement; single-photon spectral narrowing for atomic interaction; and single-photon detection and spectral analysis. The systems developed exploit the interactions of light beams in non-linear crystal materials. Greatly non-degenerate time-bin entangled photon pair sources are implemented based on the quantum process of spontaneous-parametric-down-conversion. The non-degenerate wavelengths correspond to an atomic transition (895 nm) and a telecommunications band (1310 nm). Interference-fringe-visibilities of over 78% are achieved, verifying entanglement. An efficient and low-noise single-photon up-conversion detector based on sum-frequency-generation is implemented. Photons at 1310 nm are converted to the visible region and efficiently detected using a visible single-photon detector. An overall detection efficiency of over 32% is achieved with a dark-count noise rate of 2500 s-1. The detector is further developed to achieve an inter-symbol-interference free detection rate at twice the limit of the type of visible detector used. The detector is adapted into an up-conversion spectrometer for wavelengths near 1310 nm. A sensitivity of -126 dBm is achieved, corresponding to photon fluxes of approximately 500 s-1. The up-conversion spectrometer is further adapted for correlated biphoton spectroscopy by incorporating a frequency entangled and time correlated source. In this scheme, the spectral function near 895 nm of a remote object can be reproduced by locally measuring the 1310 nm with the up-conversion spectrometer and monitoring the coincidence detection rates. To achieve linewidths feasible for atomic interaction, a very narrow linewidth non-degenerate single-photon pair source is implemented based on spontaneous-parametric-down-conversion embedded in a singly-resonant cavity which is locked to and resonating at the frequency corresponding to a target atomic transition. Linewidths as narrow as 28 MHz are achieved. The brightness of the source within the modes is increased by two-orders compared to the single-pass implementations.
Entangled photons could translate complex, ultrafast laser-based spectroscopy and imaging to a chip-sized or distributable platform. The inherent temporal and energy correlations between the two entangled photons created in spontaneous parametric down conversion (SPDC) allow a continuous-wave laser diode source to replicate ultrafast, two-pulse experiments that are usually performed in table-top scale setups. Although entangled photons were originally proposed to enhance multiphoton or nonlinear processes, few entangled experiments to date have outperformed classical photon sources from a full systems perspective. The low pump power criteria and periodically poled nonlinear sources, however, do make entangled photon experiments natural candidates for on-chip photonic circuits and spectroscopy. In our talk, we will discuss experiments that prove that the miniaturization of ultrafast experiments is a key area where entangled photons can compete with or prove superior to classical photon experiments. We will first discuss our progress in creating entangled photon sources in the visible to deep ultraviolet (UV) wavelengths as needed for spectroscopy and imaging, the integration of the subsequent photonic circuitry needed to create on-chip spectrometers, and then experimental results proving that on-chip entangled photon sources can replicate ultrafast pump-probe or be used for fluorescence lifetime imaging microscopy (FLIM) experiments. We will also discuss our increasingly null experiments on topics like entangled two-photon absorption (ETPA) which are equally important for the progressing the field.