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Two-photon-excited fluorescence spectroscopy of Rb atoms in a magneto-optical trap
Phys. Rev. Applied 26, 034067 – Published 28 September, 2026
DOI: https://doi.org/10.1103/c8gq-zp19
Abstract
We report the results of two-photon-excited fluorescence (TPEF) measurements of the transition of and cooled in a magneto-optical trap. We observe TPEF at excitation powers as low as or fluxes as low as () and (). Our results demonstrate that optically cooled Rb is a promising platform for observing sensitive two-photon spectral signatures at low photon fluxes.
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References (73)
- K. W. Martin, G. Phelps, N. D. Lemke, M. S. Bigelow, B. Stuhl, M. Wojcik, M. Holt, I. Coddington, M. W. Bishop, and J. H. Burke, Compact optical atomic clock based on a two-photon transition in rubidium, Phys. Rev. Appl. 9, 014019 (2018).
- C.-H. Chu, P.-C. Chang, Y.-J. Shih, D.-A. Luh, M.-S. Chang, T.-W. Liu, Y.-T. Lin, B.-W. Chen, and W.-Y. Cheng, Measurement of the two-photon clock transition frequency of rubidium-85 in high vacuum, Opt. Lett. 48, 5984 (2023).
- J. Leng, H. Xu, H. Lu, Y. Fan, and J. Zhao, Optical communication frequency standard using a fiber laser to excite cold rubidium two-photon transition, J. Opt. Soc. Am. B 36, 1183 (2019).
- H. Lu, J. Leng, and J. Zhao, The optimization of cold rubidium atom two-photon transition excitation with an erbium-fiber optical frequency comb, Appl. Sci. 9, 921 (2019).
- M. Carey, M. Belal, M. Himsworth, J. Bateman, and T. Freegarde, Matterwave interferometric velocimetry of cold Rb atoms, J. Mod. Opt. 65, 657 (2018).
- G. P. Greve, C. Luo, B. Wu, and J. K. Thompson, Entanglement-enhanced matter-wave interferometry in a high-finesse cavity, Nature (London) 610, 472 (2022).
- Q.-Q. Hu, C. Freier, B. Leykauf, V. Schkolnik, J. Yang, M. Krutzik, and A. Peters, Mapping the absolute magnetic field and evaluating the quadratic Zeeman effect induced systematic error in an atom interferometer gravimeter, Phys. Rev. A 96, 033414 (2017).
- M. Schmidt, A. Senger, M. Hauth, C. Freier, V. Schkolnik, and A. Peters, A mobile high-precision absolute gravimeter based on atom interferometry, Gyrosc. Navigation 2, 170 (2011).
- C. Chen, G. Bornet, M. Bintz, G. Emperauger, L. Leclerc, V. S. Liu, P. Scholl, D. Barredo, J. Hauschild, S. Chatterjee, M. Schuler, A. M. Läuchli, M. P. Zaletel, T. Lahaye, N. Y. Yao, and A. Browaeys, Continuous symmetry breaking in a two-dimensional Rydberg array, Nature (London) 616, 691 (2023).
- C. Luo, H. Zhang, A. Chu, R. Maruko, A. M. Rey, and J. K. Thompson, Hamiltonian engineering of collective spin models in an optical cavity, Nat. Phys. 21, 916 (2025).
- D. Bluvstein, S. J. Evered, A. A. Geim, S. H. Li, H. Zhou, T. Manovitz, S. Ebadi, M. Cain, M. Kalinowski, D. Hangleiter, J. P. B. Ataides, N. Maskara, I. Cong, X. Gao, P. S. Rodriguez, T. Karolyshyn, G. Semeghini, M. J. Gullans, M. Greiner, V. Vuletić, and M. D. Lukin, Logical quantum processor based on reconfigurable atom arrays, Nature (London) 626, 58 (2023).
- C. Drago, A. McLean, R. Jimenez, and J. E. Sipe, Two-photon absorption of squeezed light by rubidium atoms: Will Doppler do us in?, CLEO: Fundam. Sci. JTh2A-5 (2023).
- M. Caracas Núñez, M. A. Gonzalez, and M. Núñez Portela, Theoretical and experimental study of the 6 S-8S two-photon absorption cross-section in cesium atoms, Opt. Express 31, 31749 (2023).
- C. Drago and J. E. Sipe, Fluorescence driven by nonclassical light, arXiv:2508.12037.
- M. Rubart, Two-photon microscopy of cells and tissue, Circ. Res. 95, 1154 (2004).
- F. Helmchen and W. Denk, Deep tissue two-photon microscopy, Nat. Methods 2, 932 (2005).
- J. Bhawalkar, N. Kumar, C.-F. Zhao, and P. Prasad, Two-photon photodynamic therapy, J. Clin. Laser Med. Surg. 15, 201 (1997).
- N. P. Georgiades, E. S. Polzik, and H. J. Kimble, Two-photon spectroscopy of the transition of trapped atomic cesium, Opt. Lett. 19, 1474 (1994).
- B. Dayan, A. Pe’er, A. A. Friesem, and Y. Silberberg, Nonlinear interactions with an ultrahigh flux of broadband entangled photons, Phys. Rev. Lett. 94, 043602 (2005).
- D. Tabakaev, M. Montagnese, G. Haack, L. Bonacina, J.-P. Wolf, H. Zbinden, and R. T. Thew, Energy-time-entangled two-photon molecular absorption, Phys. Rev. A 103, 033701 (2021).
- D. Tabakaev, A. Djorović, L. La Volpe, G. Gaulier, S. Ghosh, L. Bonacina, J.-P. Wolf, H. Zbinden, and R. Thew, Spatial properties of entangled two-photon absorption, Phys. Rev. Lett. 129, 183601 (2022).
- J. P. Villabona-Monsalve, O. Varnavski, B. A. Palfey, and T. Goodson III, Two-photon excitation of flavins and flavoproteins with classical and quantum light, J. Am. Chem. Soc. 140, 14562 (2018).
- J. P. Villabona-Monsalve, O. Calderón-Losada, M. Nuñez Portela, and A. Valencia, Entangled two photon absorption cross section on the 808 nm region for the common dyes zinc tetraphenylporphyrin and rhodamine B, J. Phys. Chem. A 121, 7869 (2017).
- O. Varnavski, B. Pinsky, T. Goodson III, Entangled photon excited fluorescence in organic materials: An ultrafast coincidence detector, J. Phys. Chem. Lett. 8, 388 (2017).
- O. Varnavski and T. Goodson III, Two-photon fluorescence microscopy at extremely low excitation intensity: The power of quantum correlations, J. Am. Chem. Soc. 142, 12966 (2020).
- O. Varnavski, C. Gunthardt, A. Rehman, G. D. Luker, and T. Goodson III, Quantum light-enhanced two-photon imaging of breast cancer cells, J. Phys. Chem. Lett. 13, 2772 (2022).
- K. M. Parzuchowski, A. Mikhaylov, M. D. Mazurek, R. N. Wilson, D. J. Lum, T. Gerrits, C. H. Camp, M. J. Stevens, and R. Jimenez, Setting bounds on entangled two-photon absorption cross sections in common fluorophores, Phys. Rev. Appl. 15, 044012 (2021).
- T. Landes, B. J. Smith, and M. G. Raymer, Limitations in fluorescence-detected entangled two-photon-absorption experiments: Exploring the low- to high-gain squeezing regimes, Phys. Rev. A 110, 033708 (2024).
- M. G. Raymer, T. Landes, M. Allgaier, S. Merkouche, B. J. Smith, and A. H. Marcus, How large is the quantum enhancement of two-photon absorption by time-frequency entanglement of photon pairs?, Optica 8, 757 (2021).
- A. Mikhaylov, R. N. Wilson, K. M. Parzuchowski, M. D. Mazurek, C. H. Camp Jr., M. J. Stevens, and R. Jimenez, Hot-band absorption can mimic entangled two-photon absorption, J. Phys. Chem. Lett. 13, 1489 (2022).
- B. P. Hickam, M. He, N. Harper, S. Szoke, and S. K. Cushing, Single-photon scattering can account for the discrepancies among entangled two-photon measurement techniques, J. Phys. Chem. Lett. 13, 4934 (2022).
- S.-Y. Baek and Y.-H. Kim, Spectral properties of entangled photons generated via type-I spontaneous parametric down-conversion, Phys. Rev. A 80, 033814 (2009).
- B. Farella, G. Medwig, R. A. Abrahao, and A. Nomerotski, Spectral characterization of an SPDC source with a fast broadband spectrometer, AIP Adv. 14, 045034 (2024).
- D. Sheng, A. Perez Galvan, and L. A. Orozco, Lifetime measurements of the states of rubidium, Phys. Rev. A 78, 062506 (2008).
- N. P. Georgiades, Nonclassical excitation and quantum interference in a three level atom, PhD thesis, California Institute of Technology, Pasadena, California, 1998.
- K. M. Parzuchowski. Setting experimental bounds on entangled two-photon absorption cross sections, PhD thesis, University of Colorado Boulder, 2023.
- C. Xu and W. W. Webb, Measurement of two-photon excitation cross sections of molecular fluorophores with data from 690 to 1050 nm, J. Opt. Soc. Am. B 13, 481 (1996).
- K. Saha, V. Venkataraman, P. Londero, and A. L. Gaeta, Enhanced two-photon absorption in a hollow-core photonic-band-gap fiber, Phys. Rev. A 83, 033833 (2011).
- W. Zapka, M. D. Levenson, F. M. Schellenberg, A. C. Tam, and G. C. Bjorklund, Continuous-wave Doppler-free two-photon frequency-modulation spectroscopy in Rb vapor, Opt. Lett. 8, 27 (1983).
- B. Hoekstra, High-density trapping of rubidium-85 with a temporal dark magneto-optical trap, Master’s thesis, Eindhoven University of Technology, 2017.
- G. Reinaudi, T. Lahaye, Z. Wang, and D. Guéry-Odelin, Strong saturation absorption imaging of dense clouds of ultracold atoms, Opt. Lett. 32, 3143 (2007).
- K. Hueck, N. Luick, L. Sobirey, J. Siegl, T. Lompe, H. Moritz, L. W. Clark, and C. Chin, Calibrating high intensity absorption imaging of ultracold atoms, Opt. Express 25, 8670 (2017).
- E. L. Raab, M. Prentiss, A. Cable, S. Chu, and D. E. Pritchard, Trapping of neutral sodium atoms with radiation pressure, Phys. Rev. Lett. 59, 2631 (1987).
- A. J. Olson, E. J. Carlson, and S. K. Mayer, Two-photon spectroscopy of rubidium using a grating-feedback diode laser, Am. J. Phys. 74, 218 (2006).
- C. L. A. Collins, K. D. Bonin, and M. A. Kadar-Kallen, Absolute two-photon cross section of Rb measured by differential absorption, Opt. Lett. 18, 1754 (1993).
- K. Hassanin, P. Federsel, F. Karlewski, and C. Zimmermann, 5 S-5D two-photon transition in rubidium vapor at high densities, Phys. Rev. A 107, 043104 (2023).
- K. M. Parzuchowski, M. D. Mazurek, C. H. Camp Jr., M. J. Stevens, and R. Jimenez, A liquid-core fiber platform for classical and entangled two-photon absorption measurements, ACS Photonics 12, 1470 (2025).
- J. A. Rushton, M. Aldous, and M. D. Himsworth, The feasibility of a fully miniaturized magneto-optical trap for portable ultracold quantum technology, Rev. Sci. Instrum. 85, 121501 (2014).
- D. Pizzey, J. D. Briscoe, F. D. Logue, F. S. Ponciano-Ojeda, S. A. Wrathmall, and I. G. Hughes, Laser spectroscopy of hot atomic vapours: From ’scope to theoretical fit, New J. Phys. 24, 125001 (2022).
- O. Terra and H. Hussein, An ultra-stable optical frequency standard for telecommunication purposes based upon the two-photon transition in rubidium, Appl. Phys. B 122, 27 (2016).
- R. E. Ryan, L. A. Westling, and H. J. Metcalf, Two-photon spectroscopy in rubidium with a diode laser, J. Opt. Soc. Am. B 10, 1643 (1993).
- SABIC Innovative Plastics, ULTEM® 1000 Polyetherimide (PEI) Resin Datasheet (2024).
- U. Schünemann, H. Engler, R. Grimm, M. Weidemüller, and M. Zielonkowski, Simple scheme for tunable frequency offset locking of two lasers, Rev. Sci. Instrum. 70, 242 (1999).
- K. Luksch. Measurement of the number of atoms in a magneto-optical trap using absorption imaging, Diss. Diploma thesis, National University of Singapore, 2012.
- W. DeGraffenreid and C. J. Sansonetti, transition of atomic lithium by Doppler-free two-photon spectroscopy, Phys. Rev. A 67, 012509 (2003).
- W. DeGraffenreid, S. C. Campbell, and C. J. Sansonetti, Foreign gas pressure broadening and shifts of the 2s–4s two-photon transition of atomic lithium, J. Phys. B 36, 2099 (2003).
- G. C. Tisone and P. J. Hargis Jr., Laser absorption and fluorescence studies of the lithium 2s–3d transition, AIP Conf. Proc. 160, 404 (1987).
- I. Labazan and S. Milošević, Lithium vapour excitation at two-photon resonance, Eur. Phys. J. D 8, 41 (2000).
- M. D. Levenson and N. Bloembergen, Observation of two-photon absorption without Doppler Broadening on the transition in sodium vapor, Phys. Rev. Lett. 32, 645 (1974).
- T. W. Hänsch, K. C. Harvey, G. Meisel, and A. L. Schawlow, Two-photon spectroscopy of Na without Doppler Broadening using a CW dye laser, Opt. Commun. 11, 50 (1974).
- Y.-W. Liu and P. E. G. Baird, Two-photon spectroscopy in potassium, Meas. Sci. Technol. 12, 740 (2001).
- M.-S. Ko and Y.-W. Liu, Observation of rubidium two-photon transitions with a diode laser, Opt. Lett. 29, 1799 (2004).
- P. Morzyński, P. Wcisłó, P. Ablewski, R. Gartman, W. Gawlik, P. Masłowski, B. Nagórny, F. Ozimek, C. Radzewicz, M. Witkowski, R. Ciuryło, and M. Zawada, Absolute frequency measurement of rubidium two-photon transitions, Opt. Lett. 38, 4581 (2013).
- S. Wang, J. Yuan, L. Wang, L. Xiao, and S. Jia, A stable frequency standard based on the one-color two-photon transition in rubidium vapor, Opt. Express 16, 125204 (2019).
- V. A. Sautenkov, S. A. Saakyan, E. V. Vilshanskaya, B. B. Zelener, and B. V. Zelener, Power broadening of two-photon coherent resonances on Rydberg atomic transitions in a magneto-optical trap, J. Russ. Laser Res. 38, 91 (2017).
- V. A. Sautenkov, S. A. Saakyan, A. A. Bobrov, E. V. Vilshanskaya, B. B. Zelener, and B. V. Zelener, Differential two-photon spectroscopy for nondestructive temperature measurements of cold light atoms in a magneto-optical trap, J. Opt. Soc. Am. B 35, 1546 (2018).
- D. W. Allan, Statistics of atomic frequency standards, Proc. IEEE 54, 221 (1966).
- Zemax OpticStudio User Manual (Zemax LLC, 2022).
- D. A. Steck, Rubidium 85 D Line Data (2003–2026).
- D. A. Steck, Rubidium 87 D Line Data (2003–2026).
- A. Sargsyan, T. A. Vartanyan, and D. Sarkisyan, Broadening and shift of the D1 and D2 lines of Rb atoms by neon: Resolving hyperfine components in a half-wave cell using double differentiation with respect to frequency, Opt. Spectrosc. 129, 1173 (2021).
- H. Eicher, Third-order susceptibility of alkali metal vapors, IEEE J. Quantum Electron. 11, 121 (1975).
- G.-W. Truong, D. A. Long, A. Cygan, D. Lisak, R. D. van Zee, and J. T. Hodges, Comb-linked, cavity ring-down spectroscopy for measurements of molecular transition frequencies at the kHz-level, J. Chem. Phys. 138, 094201 (2013).