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

Rodgers, Lila V. H.; Nguyen, Suong T.; Cox, James H.; Zervas, Kalliope; Yuan, Zhiyang; Sangtawesin, Sorawis; Stacey, Alastair; Jaye, Cherno; Weiland, Conan; Pershin, Anton; Gali, Adam; Thomsen, Lars; Meynell, Simon A.; Hughes, Lillian B.; Jayich, Ania C. Bleszynski; Gui, Xin; Cava, Robert J.; Knowles, Robert R.; de Leon, Nathalie P.

doi:10.1073/pnas.2316032121

Title: Diamond surface functionalization via visible light–driven C–H activation for nanoscale quantum sensing

Journal Article · 06 March 2024 · Proceedings of the National Academy of Sciences of the United States of America

DOI: https://doi.org/10.1073/pnas.2316032121 · OSTI ID:2320316

^[1]; Nguyen, Suong T. ^[1]; Cox, James H. ^[1];

^[1];

^[1]; Sangtawesin, Sorawis ^[2]; Stacey, Alastair ^[3]; Jaye, Cherno ^[4]; Weiland, Conan ^[4];

^[5]; Gali, Adam ^[6]; Thomsen, Lars ^[7]; Meynell, Simon A. ^[8];

^[8]; Jayich, Ania C. Bleszynski ^[8]; Gui, Xin ^[1]; Cava, Robert J. ^[1];

^[1];

^[1]

Princeton Univ., NJ (United States)
Suranaree Univ. of Technology (Thailand)
School of Science, RMIT University, Melbourne, VIC 3000, Australia; Univ. of Melbourne, VIC (Australia); Royal Melbourne Inst. of Technology, VIC (Australia)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Wigner Research Center for Physics, Budapest (Hungary)
Wigner Research Center for Physics, Budapest (Hungary); Budapest Univ. of Technology and Economic (Hungary)
Australian Nuclear Science and Technology Organisation (ANSTO), Clayton, VIC (Australia). Australian Synchrotron
Univ. of California, Santa Barbara, CA (United States)

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 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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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Northwestern Univ., Evanston, IL (United States); Princeton Univ., NJ (United States); Univ. of California, Santa Barbara, CA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704; SC0018978; SC0019241; SC0021314

OSTI ID:: 2320316

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 11 Vol. 121; ISSN 1091-6490; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Diamond surface functionalization via visible light–driven C–H activation for nanoscale quantum sensing

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