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PreprintCC BY 4.0arXiv

Solution-phase fluorination of nanodiamond: near-surface NV- activation and spin relaxation

Abstract

Nanodiamonds hosting luminescent point defects, known as fluorescent nanodiamonds (FND), are a leading platform for quantum technology. The nitrogen-vacancy (NV) centre is the most intensively studied of these; its negatively charged state (NV-) can serve as a qubit at room temperature, and its stability is governed by surface functional groups. We present two solution-phase fluorination routes for stabilising NV-: direct C-F bond formation by decarboxylation with xenon difluoride via a radical mechanism, and the Balz-Schiemann reaction, which replaces surface amino groups with fluorine. The two routes were compared by infrared, X-ray photoelectron, energy-dispersive X-ray, Raman and photoluminescence spectroscopy. Both gave a high NV- fraction, up to ∼85% on average, which to our knowledge is among the highest reported for surface-terminated nanodiamonds of this size and, in particular, for fluorine termination. We attribute the stabilisation to the fluorination treatment, which removes acceptor-like carboxyl groups and forms C-F bonds that give the surface a positive electron affinity. Frequency-domain relaxometry shows that the fluorinated particles retain a long spin-lattice relaxation time, 733±56 and 712±20 μs for the XeF2 and Balz-Schiemann routes, several times the values reported for commercial HPHT nanodiamonds, although shorter than the 1173±123 μs of the as-received material. Fluorination thus activates near-surface NV- centres, which dominate relaxometric sensing, at the cost of a moderate shortening of T1.

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BibTeX
@misc{czene2026solutionphase,
  title = {{Solution-phase fluorination of nanodiamond: near-surface NV$^-$ activation and spin relaxation}},
  author = {Szabolcs Czene and Olga Krafcsik and Nikoletta Jegenyés and Dávid Beke and László Péter and Vladimir Verkhovlyuk and Adam Gali},
  howpublished = {arXiv},
  year = {2026},
  month = oct,
  doi = {10.48550/arxiv.2609.06605},
  eprint = {2609.06605},
  archivePrefix = {arXiv},
  url = {https://arxiv.org/abs/2609.06605},
  note = {CC BY 4.0},
}
RIS
TY  - UNPB
TI  - Solution-phase fluorination of nanodiamond: near-surface NV^- activation and spin relaxation
AU  - Szabolcs Czene
AU  - Olga Krafcsik
AU  - Nikoletta Jegenyés
AU  - Dávid Beke
AU  - László Péter
AU  - Vladimir Verkhovlyuk
AU  - Adam Gali
PY  - 2026
DA  - 2026/10/22
PB  - arXiv
DO  - 10.48550/arxiv.2609.06605
UR  - https://arxiv.org/abs/2609.06605
AB  - Nanodiamonds hosting luminescent point defects, known as fluorescent nanodiamonds (FND), are a leading platform for quantum technology. The nitrogen-vacancy (NV) centre is the most intensively studied of these; its negatively charged state (NV^-) can serve as a qubit at room temperature, and its stability is governed by surface functional groups. We present two solution-phase fluorination routes for stabilising NV^-: direct C-F bond formation by decarboxylation with xenon difluoride via a radical mechanism, and the Balz-Schiemann reaction, which replaces surface amino groups with fluorine. The two routes were compared by infrared, X-ray photoelectron, energy-dispersive X-ray, Raman and photoluminescence spectroscopy. Both gave a high NV^- fraction, up to ∼85% on average, which to our knowledge is among the highest reported for surface-terminated nanodiamonds of this size and, in particular, for fluorine termination. We attribute the stabilisation to the fluorination treatment, which removes acceptor-like carboxyl groups and forms C-F bonds that give the surface a positive electron affinity. Frequency-domain relaxometry shows that the fluorinated particles retain a long spin-lattice relaxation time, 733±56 and 712±20 μs for the XeF_2 and Balz-Schiemann routes, several times the values reported for commercial HPHT nanodiamonds, although shorter than the 1173±123 μs of the as-received material. Fluorination thus activates near-surface NV^- centres, which dominate relaxometric sensing, at the cost of a moderate shortening of T_1.
ER  -