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OSA Quantum 2.0 Conference

Molecular Vibration Spectroscopy with Undetected Photons

Tai Hyun Yoon, Sun Kyung Lee, Minhaeng Cho

Published Jan 1, 2020• 0 citations
Publisher

Abstract

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.

DOI
10.1364/quantum.2020.qtu8b.18

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Quantum spectroscopy and imaging with undetected idler photons have been demonstrated by measuring one-photon interference between the corresponding entangled signal fields from two spontaneous parametric down conversion (SPDC) crystals. In this Report, we present a new quantum optical measurement scheme utilizing three SPDC crystals in a cascading arrangement; here, neither the detection of the idler photons which interact with materials of interest nor their conjugate signal photons which do not interact with the sample is required. The coherence of signal beams in a single photon W-type path-entangled state is induced and modulated by indistinguishabilities of the idler beams and crucially the quantum vacuum fields. As a result, the optical properties of materials or objects interacting with the idler beam from the first SPDC crystal can be measured by detecting second-order interference between the signal beams generated by the other two SPDC crystals further down the set-up. This gedankenexperiment illustrates the fundamental importance of vacuum fields in generating an optical tripartite entangled state and thus its crucial role in quantum optical measurements.

Scientific Reports•Jul 20, 2017•12 citations
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.
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.
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.
Parametric down-conversion is a second-order nonlinear optical process annihilating a pump photon and creating a pair of photons in the signal and idler modes. Then, by using two parametric down-converters and introducing a path indistinguishability for the two generated idler modes, a quantum coherence between two conjugate signal beams can be induced. Such a double spontaneous or stimulated parametric down-conversion scheme has been used to demonstrate quantum spectroscopy and imaging with undetected idler photons via measuring one-photon interference between their correlated signal beams. Recently, we considered another quantum optical measurement scheme utilizing W-type tripartite entangled signal photons that can be generated by employing three spontaneous parametric down-conversion crystals and by inducing coherences or path-indistinguishabilities between their correlated idler beams and between quantum vacuum fields. Here, we consider an extended triple stimulated parametric down-conversion scheme for quantum optical measurement of sample properties with undetected idler and photons. Noting the real effect of vacuum field indistinguishability on the fringe visibility as well as the role of zero-point field energy in the interferometry, we show that this scheme is an ideal and efficient way to create a coherent state of W-type entangled signal photons. We anticipate that this scheme would be of critical use in further developing quantum optical measurements in spectroscopy and microscopy with undetected photons.
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.
Absorption spectroscopy is a fundamental tool for probing molecular structure. However, performing absorption spectroscopy on individual molecules is challenging due to the low signal-to-noise ratio. Here, we report on a nondestructive absorption spectroscopy on a mid-infrared vibrational transition in a single molecular ion that is co-trapped with an atomic ion. The absorption of a single photon is detected via the momentum transfer from the absorbed photon onto the molecule. This recoil signal is amplified using a non-classical state of motion of the two-ion crystal and subsequently read out via the atomic ion. We characterize the recoil detection method and use it to investigate the interaction between femtosecond laser pulses and the O-H stretching vibration in individual CaOH+ molecular ions. Furthermore, we present the single-photon absorption spectrum obtained for the vibrational transition. This method represents a milestone towards quantum non-demolition measurements of complex polyatomic molecules, providing high-fidelity methods for preparation and measurement of the quantum state of a wide range of molecular species.
Quantum spectroscopy and imaging with undetected idler photons have been demonstrated by measuring one-photon interference between the corresponding entangled signal fields from two spontaneous parametric down conversion (SPDC) crystals. In this Report, we present a new quantum optical measurement scheme utilizing three SPDC crystals in a cascading arrangement; here, neither the detection of the idler photons which interact with materials of interest nor their conjugate signal photons which do not interact with the sample is required. The coherence of signal beams in a single photon W-type path-entangled state is induced and modulated by indistinguishabilities of the idler beams and crucially the quantum vacuum fields. As a result, the optical properties of materials or objects interacting with the idler beam from the first SPDC crystal can be measured by detecting second-order interference between the signal beams generated by the other two SPDC crystals further down the set-up. This gedankenexperiment illustrates the fundamental importance of vacuum fields in generating an optical tripartite entangled state and thus its crucial role in quantum optical measurements.