Raman-based technologies have enabled many ground-breaking scientific discoveries related to surface science, single-molecule chemistry and biology. For example, researchers have identified surface-bound molecules by their Raman vibrational modes and demonstrated polarization-dependent Raman gain. However, a surface-constrained Raman laser has yet to be demonstrated because of the challenges associated with achieving a sufficiently high photon population located at a surface to transition from spontaneous to stimulated Raman scattering. Here, advances in surface chemistry and in integrated photonics are combined to demonstrate lasing based on surface stimulated Raman scattering (SSRS). By creating an oriented, constrained Si–O–Si monolayer on the surface of integrated silica optical microresonators, the requisite conditions for SSRS are achieved with low threshold powers (200 μW). The expected polarization dependence of SSRS due to the orientation of the Si–O–Si bond is observed. Owing to the ordered monolayer, the Raman lasing efficiency is improved from ~5% to over 40%.
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The data that support the plots with this paper and other findings of this study are available from the corresponding authors upon reasonable request.
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We thank Y. Xiao and J. Chen for helpful discussions and M. Veksler for scientific visualization. We would like to acknowledge IARPA (2016-16070100002) and the Office of Naval Research (N00014-17-2270).
The authors declare no competing interests.
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Shen, X., Choi, H., Chen, D. et al. Raman laser from an optical resonator with a grafted single-molecule monolayer. Nat. Photonics 14, 95–101 (2020). https://doi.org/10.1038/s41566-019-0563-7
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