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arXiv:2304.07828 · The Journal of Chemical Physics

Measurement principles for quantum spectroscopy of molecular materials with entangled photons

Luca Moretti, Esteban Rojas‐Gatjens, Lorenzo Uboldi, David O. Tiede, Evan J. Kumar, Chiara Trovatello, Fabrizio Preda, Antonio Perri, Cristian Manzoni, Giulio Cerullo, Ajay Ram Srimath Kandada

Published Aug 24, 2023• 10 citations
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Abstract

Nonlinear spectroscopy with quantum entangled photons is an emerging field of research that holds the promise to achieve superior signal-to-noise ratio and effectively isolate many-body interactions. Photon sources used for this purpose, however, lack the frequency tunability and spectral bandwidth demanded by contemporary molecular materials. Here, we present design strategies for efficient spontaneous parametric downconversion to generate biphoton states with adequate spectral bandwidth and at visible wavelengths. Importantly, we demonstrate, by suitable design of the nonlinear optical interaction, the scope to engineer the degree of spectral correlations between the photons of the pair. We also present an experimental methodology to effectively characterize such spectral correlations. Importantly, we believe that such a characterization tool can be effectively adapted as a spectroscopy platform to optically probe system-bath interactions in materials.

DOI
10.1063/5.0156598

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Nonlinear spectroscopy with quantum entangled photons is an emerging field of research that holds the promise to achieve superior signal-to-noise ratio and effectively isolate many-body interactions. Photon sources used for this purpose, however, lack the frequency tunability and spectral bandwidth demanded by contemporary molecular materials. Here, we present design strategies for efficient spontaneous parametric downconversion to generate biphoton states with adequate spectral bandwidth and at visible wavelengths. Importantly, we demonstrate, by suitable design of the nonlinear optical interaction, the scope to engineer the degree of spectral correlations between the photons of the pair. We also present an experimental methodology to effectively characterize such spectral correlations. Importantly, we believe that such a characterization tool can be effectively adapted as a spectroscopy platform to optically probe system-bath interactions in materials.
We introduce an experimental methodology based on spectrally entangled biphoton states as a probe of many-body dynamics in materials. To that end, we present an experimental technique based on the Fourier transform spectroscopy to reliably estimate the spectral correlations between the entangled photons. In a proof-of-principle experiment, we transmit the biphoton state through a strongly coupled microcavity and reliably measure and analyze the variations in the spectral correlations between the photons.
Tailoring spectral properties of photon pairs is of great importance for optical quantum information and measurement applications. High-resolution spectral measurement is a key technique for engineering spectral properties of photons, making them ideal for various quantum applications. Here we demonstrate spectral measurements and optimization of frequency-entangled photon pairs produced via spontaneous parametric downconversion (SPDC), utilizing frequency-resolved sum-frequency generation (SFG), the reverse process of SPDC. A joint phase-matching spectrum of a nonlinear crystal around 1580 nm is captured with a 40 pm resolution and a > 40 dB signal-to-noise ratio, which is significantly improved compared to traditional frequency-resolved coincidence measurements. Moreover, our scheme is applicable to collinear degenerate sources whose characterization is difficult with previously demonstrated stimulated difference frequency generation (DFG). We also illustrate that the observed phase-matching function is useful for finding an optimal pump spectrum to maximize the spectral indistinguishability of SPDC photons. We expect that our precise spectral characterization technique will be useful tool for characterizing and tailoring SPDC sources for a wide range of optical quantum applications.
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.
We report the generation and characterization of a frequency anti-correlated entangled biphoton source at the wavelength of 1560nm via a continuous-wave laser pumped spontaneous parametric down-conversion process. The spectra of the signal and idler photons are measured to have their center wavelength being 1559.7nm and 1559.8nm while their 3-dB bandwidths being 3.2nm and 3.15nm respectively. The joint spectrum of the photon pair is observed to be frequency anti-correlated and have a spectral bandwidth of 0.5nm. 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 6.4. By investigating the relative overlap between the achieved two-photon spectral intensity function and its transpose, the spectral indisinguishablity of the photon pairs is expected to be 90%. Based on a HOM interferometric coincidence measurement setup, a visibility of 89.8% is demonstrated, which shows a good agreement with the expectation.
Spontaneous parametric down-conversion (SPDC) is one of the most important sources for entangled or correlated photon pairs, which are the foundation of the emerging fields of quantum-optical imaging and spectroscopy. Using periodically poled materials as an SPDC-source allows broad emission spectra in widely tunable wavelength ranges in an efficient and walk-off-free process. For applications that employ nonlinear interference setups, maximum interferometric contrast is only achieved when signal and idler modes are overlapped precisely in the second crystal. Thus, accurate knowledge of the spectral-angular characteristic of SPDC is crucial for designing such devices.
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