Ultrafast X-ray Pump–Probe Investigation of the Formation Dynamics of SiV Centers in Diamond
Color centers in diamond are promising single-photon sources for quantum technologies and biomedical applications. We studied the formation dynamics of negatively charged silicon-vacancy (SiV) centers during diamond nucleation using time-resolved X-ray pump–probe experiments at the European X-ray Free-Electron Laser Facility. A silicon-containing adamantane precursor was flash-heated within diamond anvil cells using ultrashort femtosecond X-ray pulses at a 2.2-MHz repetition rate. We captured the structural evolution of diamond with X-ray diffraction patterns separated by 443 ns. Correlating these dynamics with postexperiment SiV photoluminescence reveals, for the first time, a link between ultrafast diamond nucleation and color-center inclusion. SiV formation is contingent on diamond formation and occurs only above pressure-dependent energy-delivery-rate thresholds: 34.3 J·s –1 at 17.8 GPa and 178.4 J·s –1 at 14.4 GPa. Our findings define synthesis windows for generating SiV and reveal a kinetic regime in which diamond nucleates without optically active SiV, informing rate- and pressure-aware strategies for producing various color centers.
Authors
- Minxue Tang (ORCID: https://orcid.org/0000-0002-3923-0677)
- Zuzana Konôpková
- Vitali B. Prakapenka (ORCID: https://orcid.org/0000-0001-9270-2330)
- Torsten Laurus (ORCID: https://orcid.org/0000-0002-2258-2123)
- Khachiwan Buakor (ORCID: https://orcid.org/0000-0003-0257-2822)
- Yanyao Zhang (ORCID: https://orcid.org/0000-0002-3846-1131)
- C. Strohm (ORCID: https://orcid.org/0000-0001-6384-0259)
- Yu Lin (ORCID: https://orcid.org/0000-0001-5174-9546)
- Karen Appel (ORCID: https://orcid.org/0000-0002-2902-2102)
- Stella Chariton (ORCID: https://orcid.org/0000-0001-5522-0498)
- Yan‐Kai Tzeng (ORCID: https://orcid.org/0000-0003-3603-1661)
- Sulgiye Park (ORCID: https://orcid.org/0000-0001-5875-4727)
- Sebastian Goede
- Mungo Frost (ORCID: https://orcid.org/0000-0001-6879-0422)
- Carsten Baehtz (ORCID: https://orcid.org/0000-0003-1480-511X)
- Anna Celeste (ORCID: https://orcid.org/0000-0001-6728-8449)
- Bora Kalkan (ORCID: https://orcid.org/0000-0002-2824-4598)
- R. S. McWilliams (ORCID: https://orcid.org/0000-0002-3730-8661)
- Heinz Graafsma
- J. Sztuk-Dambietz
- Minkyung Han
- Wendy L. Mao
- Rachel Husband
- Martin Kunz
Institutions
- Lawrence Berkeley National Laboratory (US)
- University of California, Santa Cruz (US)
- Helmholtz-Zentrum Dresden-Rossendorf (DE)
- Deutsches Elektronen-Synchrotron DESY (DE)
- SLAC National Accelerator Laboratory (US)
- University of Chicago (US)
- Joint Laboratory for Extreme Conditions Matter Properties (CN)
- Digital Heritage Netherlands (NL)
- Advanced Light Source
- European X-Ray Free-Electron Laser (DE)
- Stanford University (US)
- University of Edinburgh (GB)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2026-06-18
- DOI
- https://doi.org/10.1021/jacs.6c05691
- Primary Topic
- Diamond and Carbon-based Materials Research
- Type
- article
- Field-Weighted Citation Impact
- 0.00