- Open Access
Spectral-focusing coherent anti-Stokes Raman scattering driven by bright correlated twin beams
Phys. Rev. Applied 23, 064015 – Published 6 June, 2025
DOI: https://doi.org/10.1103/7pvj-3dqt
Abstract
An understanding of the interaction between bright correlated twin beams and matter is important for expanding the applications of optical quantum technology. In particular, it is worthwhile to clarify the advantages of twin-beam correlation in spectroscopic applications, since twin-beam sources that use parametric down-conversion have a wide range of wavelength tunability. Here, we theoretically and experimentally demonstrate that the spectral-focusing technique used in coherent anti-Stokes Raman scattering (CARS) can be implemented by twin beams without the use of ultrashort-pulse lasers. In typical spectral focusing using ultrashort pulses, spectral resolution is improved by narrowing the instantaneous frequency width due to frequency chirping. Similarly, we show theoretically that the formation of a chirp structure within the temporal correlation of twin beams produces an effect similar to typical spectral focusing. To experimentally demonstrate twin-beam spectral focusing, CARS spectroscopy of polyethylene is performed when the time delay between the chirped twin beams is set within the correlation width or it is set outside the correlation width. We observe that the spectral resolution is improved when the correlation is effective. By comparing with theoretical simulations, we confirm that the improvement is caused by frequency chirping.
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References (18)
- F. Boitier, A. Godard, N. Dubreuil, P. Delaye, C. Fabre, and E. Rosencher, Photon extrabunching in ultrabright twin beams measured by two-photon counting in a semiconductor, Nat. Commun. 2, 425 (2011).
- O. Jedrkiewicz, J.-L. Blanchet, E. Brambilla, P. Di Trapani, and A. Gatti, Detection of the ultranarrow temporal correlation of twin beams via sum-frequency generation, Phys. Rev. Lett. 108, 253904 (2012).
- M. V. Chekhova, S. Germanskiy, D. B. Horoshko, G. K. Kitaeva, M. I. Kolobov, G. Leuchs, C. R. Phillips, and P. A. Prudkovskii, Broadband bright twin beams and their upconversion, Opt. Lett. 43, 375 (2018).
- Y. Eto, Enhancement of cascaded frequency upconversion by ultrafast temporal correlation of twin beams, Opt. Lett. 49, 3344 (2024).
- T. Hellerer, A. M. Enejder, and A. Zumbusch, Spectral focusing: High spectral resolution spectroscopy with broad-bandwidth laser pulses, Appl. Phys. Lett. 85, 25 (2004).
- D. Oron, E. Tal, and Y. Silberberg, Scanningless depth-resolved microscopy, Opt. Express 13, 1468 (2005).
- G. Zhu, J. van Howe, M. Durst, W. Zipfel, and C. Xu, Simultaneous spatial and temporal focusing of femtosecond pulses, Opt. Express 13, 2153 (2005).
- K. Goda, A. Ayazi, D. R. Gossett, J. Sadasivam, C. K. Lonappan, E. Sollier, A. M. Fard, S. C. Hur, J. Adam, C. Murray, C. Wang, N. Brackbill, D. D. Carlo, and B. Jalali, High-throughput single-microparticle imaging flow analyzer, Proc. Natl. Acad. Sci. 109, 11630 (2012).
- U. Bäder, J.-P. Meyn, J. Bartschke, T. Weber, A. Borsutzky, R. Wallenstein, R. G. Batchko, M. M. Fejer, and R. L. Byer, Nanosecond periodically poled lithium niobate optical parametric generator pumped at 532 nm by a single-frequency passively -switched :YAG laser, Opt. Lett. 24, 1608 (1999).
- R. C. Prince, R. R. Frontiera, and E. O. Potma, Stimulated Raman scattering: From bulk to nano, Chem. Rev. 117, 5070 (2017).
- C. L. Evans and X. S. Xie, Coherent anti-Stokes Raman scattering microscopy: Chemical imaging for biology and medicine, Annu. Rev. Anal. Chem. 1, 883 (2008).
- A. Dementjev, V. Gulbinas, A. Serbenta, M. Kaucikas, and G. Niaura, Coherent anti-Stokes Raman scattering spectroscope/microscope based on a widely tunable laser source, J. Mod. Opt. 57, 503 (2010).
- Y. Eto, M. Nuriya, and H. Kano, Quantum frequency-resolved optical gating measurement for ultranarrow temporal correlation of twin beams, Optica Quantum 2, 468 (2024).
- F. Boitier, A. Godard, N. Dubreuil, P. Delaye, C. Fabre, and E. Rosencher, Two-photon-counting interferometry, Phys. Rev. A 87, 013844 (2013).
- F. Boitier, A. Godard, A. Ryasnyanskiy, N. Dubreuil, P. Delaye, C. Fabre, and E. Rosencher, Second order coherence of broadband down-converted light on ultrashort time scale determined by two photon absorption in semiconductor, Opt. Express 18, 20401 (2010).
- G. Bjorklund, Effects of focusing on third-order nonlinear processes in isotropic media, IEEE J. Quantum. Electron. 11, 287 (1975).
- C. Otto, A. Voroshilov, S. G. Kruglik, and J. Greve, Vibrational bands of luminescent zinc(II)-octaethylporphyrin using a polarization-sensitive “microscopic” multiplex CARS technique, J. Raman. Spectrosc. 32, 495 (2001).
- W. M. Tolles, J. W. Nibler, J. R. McDonald, and A. B. Harvey, A review of the theory and application of coherent anti-Stokes Raman spectroscopy (cars), Appl. Spectrosc. 31, 253 (1977).
