Productivity of Concentration-Dependent Conversion of Substitutional Nitrogen Atoms into Nitrogen-Vacancy Quantum Emitters in Synthetic-Diamond by Ultrashort Laser Pulses

Abstract

Tightly focused 515-nm, 0.3-ps laser pulses modify in a laser filamentation regime the crystalline structure of an Ib-type high-pressure, high-temperature (HPHT) synthesized diamond in a thin-plate form. The modified microregions (micromarks) in the yellow and colorless crystal zones, possessing different concentrations of elementary substitutional nitrogen (N) impurity atoms (C-centers), exhibit their strongly diminished local IR absorption (upon correction to the thickness scaling factor). Simultaneously, local visible-range (400–550 nm) absorption coefficients were increased, and photoluminescence (PL) yield was strongly enhanced in the broad range of 450–800 nm. The strong yellow-red PL enhancement saturates with laser exposure, implying the complete conversion of C-centers into nitrogen-vacancy (NV0,−) ones due to the laser-induced generation of Frenkel “interstitial-vacancy” I–V carbon pairs. The other emerging blue-green (>470 nm) and green-yellow (>500 nm) PL bands were also simultaneously saturated versus the laser exposure. The observed IR/optical absorption and PL spectral changes enlighten the ultrashort pulse laser inscription of NV0−-based quantum-emitter centers in synthetic diamonds and enable the evaluation of the productivity of their inscription along with the corresponding I–V generation rates.

Keywords

• HPHT diamond
• substitutional nitrogen atoms
• femtosecond laser
• filaments
• 3D-scanning Raman and photoluminescence micro-spectroscopy
• optically active radiation defects