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Physical Review Applied

Molecular Rovibrational Spectroscopy with Undetected Photons via Single-Photon Interferometry

Sun Kyung Lee, Tai Hyun Yoon, Minhaeng Cho

Published Jul 15, 2020• 9 citations
Publisher

Abstract

Interferometric spectroscopy with undetected photons (ISUP) utilizing quantum mechanically path-entangled photon pairs has received considerable attention as an optical-measurement platform. Recently, we carried out a proof-of-concept experiment to show that ISUP can be used to measure the transmission spectrum of a Fabry-Perot resonator. Here, we demonstrate that ISUP with dual stimulated parametric down-conversion (StPDC) processes, which allows us to perform infrared rovibrational spectroscopy with visible photons. In our ISUP method, quantum coherence between two independent signal photons from each StPDC crystal is induced by the indistinguishability of conjugate idler fields and results in high visibility of the signal single-photon interferometry at the nondegenerate wavelength. If the seed-beam intensity is imbalanced due to the sample absorption, the corresponding envelope modulation of the interference fringe as a function of the seed-beam frequency reveals the absorption spectrum of the optical sample. As a proof-of-principle experiment, the full rovibrational transmission spectrum at 1550 nm of the hydrogen cyanide (${\mathrm{H}}^{13}{\mathrm{C}}^{14}\mathrm{N}$) molecules in a gas cell is measured from the single-photon interference fringe of the signal fields at 807 nm. We thus anticipate that the single-photon ISUP technique with dual StPDC crystals will find broad use for the development of high-resolution atomic and molecular spectroscopy with undetected photons.

DOI
10.1103/physrevapplied.14.014045

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Interferometric spectroscopy with undetected photons (ISUP) utilizing quantum mechanically path-entangled photon pairs has received considerable attention as an optical-measurement platform. Recently, we carried out a proof-of-concept experiment to show that ISUP can be used to measure the transmission spectrum of a Fabry-Perot resonator. Here, we demonstrate that ISUP with dual stimulated parametric down-conversion (StPDC) processes, which allows us to perform infrared rovibrational spectroscopy with visible photons. In our ISUP method, quantum coherence between two independent signal photons from each StPDC crystal is induced by the indistinguishability of conjugate idler fields and results in high visibility of the signal single-photon interferometry at the nondegenerate wavelength. If the seed-beam intensity is imbalanced due to the sample absorption, the corresponding envelope modulation of the interference fringe as a function of the seed-beam frequency reveals the absorption spectrum of the optical sample. As a proof-of-principle experiment, the full rovibrational transmission spectrum at 1550 nm of the hydrogen cyanide (H13C14N{\mathrm{H}}^{13}{\mathrm{C}}^{14}\mathrm{N}H13C14N) molecules in a gas cell is measured from the single-photon interference fringe of the signal fields at 807 nm. We thus anticipate that the single-photon ISUP technique with dual StPDC crystals will find broad use for the development of high-resolution atomic and molecular spectroscopy with undetected photons.
We present a novel technique of molecular vibration spectroscopy with undetected photons (MSUP) with dual stimulated parametric down-conversion crystals. In our MSUP, quantum coherence between independent signal photons is induced by the path indistinguishability of the conjugate idler single-photon-added coherent states and results in perfect visibility under the same pump and seed beam intensities. If the seed beam intensity is imbalanced by the sample absorption, the modulated interference fringe reveals the absorption spectrum as a function of seed beam frequency. As a proof-of-principle experiment, a rovibrational absorption spectrum of hydrogen cyanide (H13C14N) molecules in a gas cell at approximately 1550 nm is successfully measured by analyzing the single-photon interference fringe of the signal field at 807 nm.
Quantum spectroscopy with undetected photons (QSUP) utilizing the quantum entanglement of parametrically down-converted photons has emerged as a new spectroscopic platform. Here, we demonstrate a high-resolution and remote-measurement QSUP, where light-matter interactions and photon detections are performed in spectrally and spatially different regions. A dual-stimulated parametric down-conversion scheme with an optical frequency-comb pump and ultra-narrow coherent seed beam in an idler mode is used to generate path-entangled pairs of the undetected idler and measured frequency-comb signal photons. To demonstrate the frequency resolution of this scheme, a Fabry-Pérot cavity with a narrow bandwidth is used as a sample that modulates the distinguishability of one-photon-added coherent idler beams, which directly affects the interference fringe visibility of the entangled signal photons. We thus anticipate that the remote QSUP whose frequency resolution is determined by the linewidth of the coherent seed laser will enable the development of quantum spectroscopy featuring high resolution.
Abstract Due to their frequency scaling and long-term coherence, frequency combs at the single-photon level can provide a fascinating platform for developments in quantum technology. Here we demonstrate frequency comb single-photon interferometry in an unheralded manner. We are able to induce coherence by erasing the which-way information of path-entangled photon pairs. The photon pairs are prepared using a dual parametric down-conversion pumped by a highly stable frequency comb laser and an ultra-narrow seed laser. This is conducted at the extremely low-conversion efficiency regime. The unique feature of our quantum interferometer is that the induced one-photon interference of the path-encoded single photons (signal), with multiple frequency components, is observed with a unit visibility without heralding conjugate photons (idler). We demonstrate that quantum information and frequency comb technology can be combined to realize quantum information platforms. We expect this will contribute to the application of quantum information and optical measurements beyond the classical limit.
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.
Abstract Quantum interferometry based on induced-coherence phenomena has demonstrated the possibility of undetected-photon measurements. Perturbation in the optical path of probe photons can be detected by interference signals generated by quantum mechanically correlated twin photons propagating through a different path, possibly at a different wavelength. To the best of our knowledge, this work demonstrates for the first time a hybrid-type induced-coherence interferometer that incorporates a Mach–Zehnder-type interferometer for near-visible photons and a Michelson-type interferometer for infrared (IR) photons, based on double-pass-pumped spontaneous parametric down-conversion. This configuration enables IR optical measurements via the detection of near-visible photons and provides methods for optimizing the quality of measurements by identifying photon pairs of different origins. We theoretically identify that the induced-coherence interference visibility is approximately the same as the heralding efficiency between twin photons along the relevant spatial modes, and experimentally maximize the visibility by setting up a common reference spatial mode for IR photons. Applications to both time-domain and frequency-domain quantum optical induced-coherence tomography for three-dimensional test structures are demonstrated. The results prove the feasibility of practical undetected-photon sensing and imaging techniques based on the presented structure.