We propose and demonstrate a novel technique that combines Raman scattering and optical cycling in molecules with diagonal Franck-Condon factors. This resonance Raman optical cycling manipulates molecules to behave like efficient fluorophores with discrete absorption and emission profiles that are readily separated for sensitive fluorescence detection in high background light environments. Using a molecular beam of our test species, SrF, we realize up to an average of $\approx20$ spontaneously emitted photons per molecule, limited by the interaction time, while using a bandpass filter to suppress detected scattered laser light by $\sim10^{6}$. This general technique represents a powerful tool for high-fidelity fluorescence detection of molecules in any setting and is particularly well-suited to molecular laser cooling and trapping experiments.
Photon Cycling and Laser Cooling of an Asymmetric Top Molecule
Harvard University（哈佛大学）；Harvard-MIT Center for Ultracold Atoms（哈佛-麻省理工学院超冷原子中心）；Korea University（高丽大学）；Massachusetts Institute of Technology（麻省理工学院）；University of California, Berkeley（加州大学伯克利分校）；Michigan State University（密歇根州立大学）；University of Southern California（南加州大学）
Optical cycling on thorium monoxide (ThO) for an improved test of fundamental symmetries
Facility for Rare Isotope Beams, Michigan State University（密歇根州立大学稀有同位束设施）；Department of Physics and Astronomy, Michigan State University（密歇根州立大学物理与天文学系）
Raman Transitions in Collinear Laser Spectroscopy for High-Precision Frequency Measurements
Institut für Kernphysik, Technische Universität Darmstadt（达姆施塔特工业大学核物理研究所）；Helmholtz Research Academy Hesse for FAIR, GSI Helmholtzzentrum für Schwerionenforschung（黑森州FAIR亥姆霍兹研究院，GSI重离子研究中心）；Institute for Nuclear and Radiation Physics, KU Leuven（荷语鲁汶大学核与辐射物理研究所）
An N-atom Collective State Atomic Interferometer with Ultra-High Compton Frequency and Ultra-Short de Broglie Wavelength, with root-N Reduction in Fringe Width
Background-free time-resolved coherent Raman spectroscopy (CSRS and CARS): heterodyne detection of low-energy vibrations and recognition of excited-state contributions
