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

Journal Article · · Proceedings of the National Academy of Sciences of the United States of America
ORCiD logo [1];  [2];  [2]; ORCiD logo [1]; ORCiD logo [1];  [3];  [4];  [5];  [5]; ORCiD logo [6];  [7];  [8];  [9]; ORCiD logo [10];  [9];  [2];  [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Department of Electrical and Computer Engineering, Princeton University, Princeton, NJ 08540
  2. Department of Chemistry, Princeton University, Princeton, NJ 08540
  3. School of Physics, Suranaree University of Technology, Nakhon Ratchasima 30000, Thailand, Center of Excellence in Advanced Functional Materials, Suranaree University of Technology, Nakhon Ratchasima 30000, Thailand
  4. School of Physics, University of Melbourne, Parkville, VIC 3010, Australia, School of Science, RMIT University, Melbourne, VIC 3000, Australia
  5. Materials Measurement Science Division, Material Measurement Laboratory, National Institute of Standards and Technology, Gaithersburg, MD 20899
  6. HUN-REN Wigner Research Centre for Physics, Institute for Solid State Physics and Optics, Budapest H-1525, Hungary, MTA-WFK Lendület “Momentum” Semiconductor Nanostructures Research Group, Budapest H-1525, Hungary
  7. HUN-REN Wigner Research Centre for Physics, Institute for Solid State Physics and Optics, Budapest H-1525, Hungary, MTA-WFK Lendület “Momentum” Semiconductor Nanostructures Research Group, Budapest H-1525, Hungary, Department of Atomic Physics, Institute of Physics, Budapest University of Technology and Economics, Budapest H-1111, Hungary
  8. Australian Synchrotron, Australian Nuclear Science and Technology Organisation, Clayton, VIC 3168, Australia
  9. Physics Department, University of California, Santa Barbara, CA 93106
  10. Materials Department, University of California, Santa Barbara, CA 93106

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.

Sponsoring Organization:
USDOE
Grant/Contract Number:
SC0018978; SC0019241
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 0027-8424
Publisher:
Proceedings of the National Academy of SciencesCopyright Statement
Country of Publication:
United States
Language:
English

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