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Direct measurement of high-lying vibrational repumping transitions for molecular laser cooling

Nickolas H. Pilgram1,*,†, Arian Jadbabaie2, Chandler J. Conn2, and Nicholas R. Hutzler2

  • 1Division of Engineering and Applied Science, California Institute of Technology, Pasadena, California 91125, USA
  • 2Division of Physics, Mathematics, and Astronomy, California Institute of Technology, Pasadena, California 91125, USA

  • *nickolas.pilgram@nist.gov
  • †Present address: Sensor Sciences Division, National Institute of Standards and Technology, Gaithersburg, MD 20899, USA.
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Phys. Rev. A 107, 062805 – Published 2 June, 2023

DOI: https://doi.org/10.1103/PhysRevA.107.062805

Abstract

Molecular laser cooling and trapping requires addressing all spontaneous decays to excited vibrational states that occur at the ≳10−4–10−5 level, which is accomplished by driving repumping transitions out of these states. However, the transitions must first be identified spectroscopically at high resolution. A typical approach is to prepare molecules in excited vibrational states via optical cycling and pumping, which requires multiple high-power lasers. Here, we demonstrate a general method to perform this spectroscopy without the need for optical cycling. We produce molecules in excited vibrational states by using optically driven chemical reactions in a cryogenic buffer gas cell, and implement frequency-modulated absorption to perform direct, sensitive, high-resolution spectroscopy. We demonstrate this technique by measuring the spectrum of the Ã2Π1/2(1,0,0)–X̃2Σ+(3,0,0) band in YbOH174. We identify the specific vibrational repump transitions needed for photon cycling, and combine our data with previous measurements of the Ã2Π1/2(1,0,0)–X̃2Σ+(0,0,0) band to determine all of the relevant spectral constants of the X̃2Σ+(3,0,0) state. This technique achieves high signal to noise, can be further improved to measure increasingly high-lying vibrational states, and is applicable to other molecular species favorable for laser cooling.

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Phys. Rev. A 107, 062805– Published 2 June, 2023
  • Received 8 March 2023
  • Accepted 10 May 2023
Article part of CHORUS
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