Molecular Rovibrational Spectroscopy with Undetected Photons via Single-Photon Interferometry

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) 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.