Diamond surface functionalization via visible light-driven C-H activation for nanoscale quantum sensing

Rodgers, L.V.H. and Nguyen, S.T. and Cox, J.H. and Zervas, K. and Yuan, Z. and Sangtawesin, S. and Stacey, A. and Jaye, C. and Weiland, C. and Pershin, Anton and Gali, Ádám and Thomsen, L. and Meynell, S.A. and Hughes, L.B. and Jayich, A.C.B. and Gui, X. and Cava, R.J. and Knowles, R.R. and de, Leon N.P. (2024) Diamond surface functionalization via visible light-driven C-H activation for nanoscale quantum sensing. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 121 (11). -e2316032121. ISSN 0027-8424

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Abstract

Nitrogen- vacancy (NV) centers in diamond are a promising platform for nanoscale NMR sensing. Despite significant progress toward using NV centers to detect and localize nuclear spins down to the single spin level, NV- based spectroscopy of individual, intact, arbitrary target molecules remains elusive. Such sensing requires that target molecules are immobilized within nanometers of NV centers with long spin coherence. The inert nature of diamond typically requires harsh functionalization techniques such as thermal annealing or plasma processing, limiting the scope of functional groups that can be attached to the surface. Solution- phase chemical methods can be readily generalized to install diverse functional groups, but they have not been widely explored for single- crystal diamond surfaces. Moreover, realizing shallow NV centers with long spin coherence times requires highly ordered single- crystal surfaces, and solution- phase functionalization has not yet been shown with such demanding conditions. In this work, we report a versatile strategy to directly functionalize C–H bonds on single- crystal diamond surfaces under ambient conditions using visible light, forming C–F, C–Cl, C–S, and C–N bonds at the surface. This method is compatible with NV centers within 10 nm of the surface with spin coherence times comparable to Downloaded from https://www.pnas.org by 62.201.67.88 on September 20, 2026 from IP address 62.201.67.88. the state of the art. As a proof- of- principle demonstration, we use shallow ensembles of NV centers to detect nuclear spins from surface- bound functional groups. Our approach to surface functionalization opens the door to deploying NV centers as a tool for chemical sensing and single- molecule spectroscopy.

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