Raman laser from an optical resonator with a grafted single-molecule monolayer

Abstract

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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Fig. 1: Excitation of SSRS using an integrated optical microcavity.
Fig. 2: Surface chemistry on silica resonator devices.
Fig. 3: Device characterization method and optical device performance.
Fig. 4: Characterization of Raman emission.
Fig. 5: Raman lasing behaviours.
Fig. 6: Comparison of Raman lasing performance from OH, MS and DMS devices with two different diameters (~53 μm and ~83 μm) excited at two different polarizations.

Data availability

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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Acknowledgements

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).

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Contributions

X.S. and H.C. conceived the project. X.S., H.C. and A.M.A. designed the experiments. H.C. fabricated the devices. X.S. functionalized the devices. X.S. and H.C. conducted testing and data analysis. W.Z. conducted DFT simulations of the model molecules. D.C. performed the finite-element method simulations. X.S., H.C. and A.M.A. wrote the manuscript. All authors revised and commented on the manuscript. All authors have given approval to the final version of the manuscript and Supplementary Information.

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Correspondence to Xiaoqin Shen or Andrea M. Armani.

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Supplementary Information

Supplementary details, Figs. 1–6, refs. 1–10 and Tables 1–3.

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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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