- Physical Review Journals
All JournalsPhysics Magazine

Physical Review Research

Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Letter
  • Open Access

Resonance Raman optical cycling for high-fidelity fluorescence detection of molecules

J. C. Shaw, J. C. Schnaubelt, and D. J. McCarron*

  • Department of Physics, University of Connecticut, 196A Auditorium Road, Unit 3046, Storrs, Connecticut 06269, USA

  • *daniel.mccarron@uconn.edu
PDF

Phys. Rev. Research 3, L042041 – Published 15 December, 2021

DOI: https://doi.org/10.1103/PhysRevResearch.3.L042041

Abstract

We propose and demonstrate a 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 ≈20 spontaneously emitted photons per molecule, limited by the interaction time, while using a bandpass filter to suppress detected scattered laser light by ∼106. This general technique represents a powerful tool for high-fidelity fluorescence detection of molecules and is particularly well suited to molecular laser cooling and trapping experiments.

View figure in article

Physics Subject Headings (PhySH)

Article Text

References (53)

  1. L. Carr, D. DeMille, R. Krems, and J. Ye, Cold and ultracold molecules: Science, technology and applications, New J. Phys. 11, 055049 (2009).
  2. A. Prehn, M. Ibrügger, R. Glöckner, G. Rempe, and M. Zeppenfeld, Optoelectrical Cooling of Polar Molecules to Submillikelvin Temperatures, Phys. Rev. Lett. 116, 063005 (2016).
  3. E. B. Norrgard, D. J. McCarron, M. H. Steinecker, M. R. Tarbutt, and D. DeMille, Submillikelvin Dipolar Molecules in a Radio-Frequency Magneto-Optical Trap, Phys. Rev. Lett. 116, 063004 (2016).
  4. D. J. McCarron, M. H. Steinecker, Y. Zhu, and D. DeMille, Magnetic Trapping of an UltraCold Gas of Polar Molecules, Phys. Rev. Lett. 121, 013202 (2018).
  5. M.-G. Hu, Y. Liu, D. D. Grimes, Y.-W. Lin, A. H. Gheorghe, R. Vexiau, N. Bouloufa-Maafa, O. Dulieu, T. Rosenband, and K.-K. Ni, Direct observation of bimolecular reactions of ultracold KRb molecules, Science 366, 1111 (2019).
  6. S. Truppe, R. J. Hendricks, S. K. Tokunaga, H. J. Lewandowski, M. G. Kozlov, C. Henkel, E. A. Hinds, and M. R. Tarbutt, A search for varying fundamental constants using hertz-level frequency measurements of cold CH molecules, Nat. Commun. 4, 2600 (2013).
  7. R. Mitra, V. S. Prasannaa, R. F. Garcia Ruiz, T. K. Sato, M. Abe, Y. Sakemi, B. P. Das, and B. K. Sahoo, Towards CP-violation studies on superheavy molecules: Theoretical and experimental perspectives, Phys. Rev. A 104, 062801 (2021).
  8. M. Zeppenfeld, Nondestructive detection of polar molecules via Rydberg atoms, Europhys. Lett. 118, 13002 (2017).
  9. L. W. Cheuk, L. Anderegg, B. L. Augenbraun, Y. Bao, S. Burchesky, W. Ketterle, and J. M. Doyle, Λ-Enhanced Imaging of Molecules in an Optical Trap, Phys. Rev. Lett. 121, 083201 (2018).
  10. Q. Guan, M. Highman, E. Meier, G. Williams, V. Scarola, B. DeMarco, S. Kotochigova, and B. Gadway, Nondestructive dispersive imaging of rotationally excited ultracold molecules, Phys. Chem. Chem. Phys. 22, 20531 (2020).
  11. D. J. McCarron, Laser cooling and trapping molecules, J. Phys. B: At. Mol. Opt. Phys. 51, 212001 (2018).
  12. D. Wang, B. Neyenhuis, M. H. G. de Miranda, K.-K. Ni, S. Ospelkaus, D. S. Jin, and J. Ye, Direct absorption imaging of ultracold polar molecules, Phys. Rev. A 81, 061404(R) (2010).
  13. E. S. Shuman, J. F. Barry, D. R. Glenn, and D. DeMille, Radiative Force from Optical Cycling on a Diatomic Molecule, Phys. Rev. Lett. 103, 223001 (2009).
  14. J. F. Barry, D. J. McCarron, E. N. Norrgard, M. H. Steinecker, and D. DeMille, Magneto-optical trapping of a diatomic molecule, Nature (London) 512, 286 (2014).
  15. E. B. Norrgard, N. Sitaraman, J. F. Barry, D. J. McCarron, M. H. Steinecker, and D. DeMille, In-vacuum scattered light reduction with black cupric oxide surfaces for sensitive fluorescence detection, Rev. Sci. Instrum. 87, 053119 (2016).
  16. S. A. Meek, H. Conrad, and G. Meijer, Trapping molecules on a chip, Science (NY) 324, 1699 (2009).
  17. G. Santambrogio, Trapping molecules on chips, EPJ Techn. Instrum. 2, 14 (2015).
  18. S. Hou, B. Wei, L. Deng, and J. Yin, Chip-based microtrap arrays for cold polar molecules, Phys. Rev. A 96, 063416 (2017).
  19. A. André, D. DeMille, J. M. Doyle, M. D. Lukin, S. E. Maxwell, P. Rabl, R. J. Schoelkopf, and P. Zoller, A coherent all-electrical interface between polar molecules and mesoscopic superconducting resonators, Nat. Phys 2, 636 (2006).
  20. M. Chalfie, Y. Tu, G. Euskirchen, W. Ward, and D. Prasher, Green fluorescent protein as a marker for gene expression, Science 263, 802 (1994).
  21. J. R. Lakowicz, Fluorophores, in Principles of Fluorescence Spectroscopy (Springer US, Boston, MA, 1999), pp. 63–93.
  22. B. K. Stuhl, B. C. Sawyer, D. Wang, and J. Ye, A Magneto-Optical Trap for Polar Molecules, Phys. Rev. Lett. 101, 243002 (2008).
  23. S. E. Galica, L. Aldridge, D. J. McCarron, E. E. Eyler, and P. L. Gould, Deflection of a molecular beam using the bichromatic stimulated force, Phys. Rev. A 98, 023408 (2018).
  24. J. C. Shaw and D. J. McCarron, Bright, continuous beams of cold free radicals, Phys. Rev. A 102, 041302(R) (2020).
  25. H. J. Williams, S. Truppe, M. Hambach, L. Caldwell, N. J. Fitch, E. A. Hinds, B. E. Sauer, and M. R. Tarbutt, Characteristics of a magneto-optical trap of molecules, New J. Phys. 19, 113035 (2017).
  26. C. J. Foot, Atomic Physics, Oxford master series in atomic, optical, and laser physics (Oxford University Press, Oxford, England, 2007).
  27. M. R. Tarbutt, B. E. Sauer, J. J. Hudson, and E. A. Hinds, Design for a fountain of YbF molecules to measure the electron's electric dipole moment, New J. Phys. 15, 053034 (2013).
  28. S. Truppe, H. J. Williams, M. Hambach, L. Caldwell, N. J. Fitch, E. A. Hinds, B. E. Sauer, and M. R. Tarbutt, Molecules cooled below the Doppler limit, Nat. Phys. 13, 1173 (2017).
  29. J. F. Barry, E. S. Shuman, E. B. Norrgard, and D. DeMille, Laser Radiation Pressure Slowing of a Molecular Beam, Phys. Rev. Lett. 108, 103002 (2012).
  30. B. Hemmerling, E. Chae, A. Ravi, L. Anderegg, G. Drayna, N. R. Hutzler, A. Collopy, J. Ye, W. Ketterle, and J. M. Doyle, Laser slowing of CAF molecules to near the capture velocity of a molecular MOT, J. Phys. B 49, 174001 (2016).
  31. B. L. Augenbraun, Z. D. Lasner, A. Frenett, H. Sawaoka, C. Miller, T. C. Steimle, and J. M. Doyle, Laser-cooled polyatomic molecules for improved electron electric dipole moment searches, New J. Phys. 22, 022003 (2020).
  32. R. F. G. Ruiz, R. Berger, J. Billowes, C. L. Binnersley, M. L. Bissell, A. A. Breier, A. J. Brinson, K. Chrysalidis, T. E. Cocolios, B. S. Cooper, K. T. Flanagan, T. F. Giesen, R. P. de Groote, S. Franchoo, F. P. Gustafsson, T. A. Isaev, A. Koszorús, G. Neyens, H. A. Perrett, C. M. Ricketts et al., Spectroscopy of short lived radioactive molecules, Nature (London) 581, 396 (2020).
  33. T. Chen, W. Bu, and B. Yan, Radiative deflection of a BaF molecular beam via optical cycling, Phys. Rev. A 96, 053401 (2017).
  34. R. Albrecht, M. Scharwaechter, T. Sixt, L. Hofer, and T. Langen, Buffer-gas cooling, high-resolution spectroscopy, and optical cycling of barium monofluoride molecules, Phys. Rev. A 101, 013413 (2020).
  35. S. Vazquez-Carson, Q. Sun, and T. Zelevinsky, Progress towards Laser-Cooled CH Molecules, Bull. Am. Phys. Soc. (unpublished).
  36. L. Baum, N. B. Vilas, C. Hallas, B. L. Augenbraun, S. Raval, D. Mitra, and J. M. Doyle, Establishing a nearly closed cycling transition in a polyatomic molecule, Phys. Rev. A 103, 043111 (2021).
  37. D. Mitra, N. B. Vilas, C. Hallas, L. Anderegg, B. L. Augenbraun, L. Baum, C. Miller, S. Raval, and J. M. Doyle, Direct laser cooling of a symmetric top molecule, Science 369, 1366 (2020).
  38. S. Jurgilas, A. Chakraborty, C. J. H. Rich, B. E. Sauer, M. D. Frye, J. M. Hutson, and M. R. Tarbutt, Collisions in a dual-species magneto-optical trap of molecules and atoms, New J. Phys. 23, 075004 (2021).
  39. L. Anderegg, S. Burchesky, Y. Bao, S. S. Yu, T. Karman, E. Chae, K.-K. Ni, W. Ketterle, and J. M. Doyle, Observation of microwave shielding of ultracold molecules, Science 373, 779 (2021).
  40. J. C. Schnaubelt, J. C. Shaw, and D. J. McCarron, Cold CH radicals for laser cooling and trapping, arXiv:2109.03953 (2021).
  41. P. Wcislo, H. Wu, D. Reens, A. Aeppli, and J. Ye, Detection and manipulation of the transverse motion of neutral molecules in a stark decelerator, Measurement 183, 109888 (2021).
  42. T. K. Langin, V. Jorapur, Y. Zhu, Q. Wang, and D. DeMille, Polarization Enhanced Deep Optical Dipole Trapping of Λ-cooled Polar Molecules, Phys. Rev. Lett. 127, 163201 (2021).
  43. X. Wu, Z. Han, J. Chow, D. G. Ang, C. Meisenhelder, C. D. Panda, E. P. West, G. Gabrielse, J. M. Doyle, and D. DeMille, The metastable q3δ2 state of ThO: A new resource for the ACME electron EDM search, New J. Phys. 22, 023013 (2020).
  44. X. Alauze, J. Lim, M. A. Trigatzis, S. Swarbrick, F. J. Collings, N. J. Fitch, B. E. Sauer, and M. R. Tarbutt, An ultracold molecular beam for testing fundamental physics, Quantum Sci. Technol. 6, 044005 (2021).
  45. Y. Wu, J. J. Burau, K. Mehling, J. Ye, and S. Ding, High phase-space density of laser-cooled molecules in an optical lattice, arXiv:2107.06422.
  46. J. R. Daniel, C. Wang, K. Rodriguez, B. Hemmerling, T. N. Lewis, C. Bardeen, A. Teplukhin, and B. K. Kendrick, Spectroscopy on the a1Π←x1Σ+ transition of buffer-gas-cooled AlCl, Phys. Rev. A 104, 012801 (2021).
  47. J. C. Shaw, J. C. Schnaubelt, and D. J. McCarron, Stable 2 W continuous-wave 261.5 nm laser for cooling and trapping aluminum monochloride, Opt. Express 29, 37140 (2021).
  48. S. Hofsäss, M. Doppelbauer, S. C. Wright, S. Kray, B. G. Sartakov, J. Pérez-Ríos, G. Meijer, and S. Truppe, Optical cycling of AlF molecules, New J. Phys. 23, 075001 (2021).
  49. M. Xia, R. Gu, K. Yan, D. Wu, L. Xu, Y. Xia, and J. Yin, Destabilization of dark states in MgF molecules, Phys. Rev. A 103, 013321 (2021).
  50. L. Anderegg, L. W. Cheuk, Y. Bao, S. Burchesky, W. Ketterle, K.-K. Ni, and J. M. Doyle, An optical tweezer array of ultracold molecules, Science 365, 1156 (2019).
  51. A. Heinz, J. Trautmann, N. Šantić, A. J. Park, I. Bloch, and S. Blatt, Crossed optical cavities with large mode diameters, Opt. Lett. 46, 250 (2021).
  52. S. W. Hell, Toward fluorescence nanoscopy, Nat. Biotechnol. 21, 1347 (2003).
  53. J. Rao, A. Dragulescu-Andrasi, and H. Yao, Fluorescence imaging in vivo: Recent advances, Curr. Opin. Biotechnol. 18, 17 (2007).

Outline

Information

Phys. Rev. Research 3, L042041– Published 15 December, 2021
  • Received 22 August 2021
  • Accepted 26 November 2021
Crossmark - Check for updates button
Creative Commons Logo

Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

Published by the American Physical Society

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation