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Physical review. B./Physical review. B

Spectroscopy of photoionization from the E 1 singlet state in nitrogen-vacancy centers in diamond

Sean M. Blakley, Thuc T. Mai, Stephen J. Moxim, Jason Thomas Ryan, Adam J. Biacchi, Angela R. Hight Walker, R. D. McMichael

Published Oct 17, 2024• 2 citations
Publisher

Abstract

The $^{1}E$--$^{1}A_{1}$ singlet manifold of the negatively charged nitrogen vacancy ($\mathrm{N}{V}^{\ensuremath{-}}$) center in diamond plays a central role in its quantum-information and quantum-sensing applications. However, the energy gap between the $^{1}E$ singlet state and diamond band edges or the $^{3}A_{2}$--$^{3}E$ triplet manifold has not been measured directly. Using the magnetic-field quenching effect on the $\mathrm{N}{V}^{\ensuremath{-}}$ photoluminescence (PL) spectra, we measure these energy gaps as a function of temperature, applied magnetic field, excitation wavelength, and excitation power in a heavily nitrogen-doped sample. Increased PL and decreased zero-phonon line width from the $\mathrm{N}{V}^{0}$ center were observed in the presence of an applied magnetic field, indicating ionization from the long-lived $^{1}E$ singlet state. A temperature-dependent ionization threshold between 532 and 550 nm was found, locating the singlet states within the diamond band gap.

DOI
10.1103/physrevb.110.134109

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The negatively charged diamond nitrogen‐vacancy () center plays a central role in many quantum sensing applications, though much is still unknown about the energy levels in this system. The ionization energy of the singlet state in the center has only recently been measured to be between 2.25 and 2.33 eV. In this work, we reduce this uncertainty by measuring the ionization energy as a function of excitation laser wavelength and diamond temperature via magnetically mediated spin‐selective photoluminescence (PL) quenching that transfers population from the in the into the neutral charge configuration. Measurements are performed for excitation wavelengths between 450 and 470 nm, and between 540 and 566 nm in increments of 2 nm, and for temperatures ranging from about 50 to 150 K in 5 K increments. We determine the ionization energy to be between 2.29 and 2.33 eV, which provides about a twofold reduction in uncertainty of this quantity. Distribution level: A. Approved for public release; distribution unlimited.
The singlet states of the negatively charged nitrogen-vacancy centers in diamond play a key role in its optical spin control and readout. In this work, the hitherto unknown ionization energy of the singlet is measured experimentally and found to be in the range 1.91--2.25 eV. This is obtained by analyzing photoluminescence measurements incorporating spin control and nitrogen-vacancy charge state differentiation, along with simulations based on the nitrogen-vacancy's master equation. This work establishes a protocol for a more accurate estimate of this ionization energy, which can possibly lead to improved readout methods.
We report on the spectroscopic and laser characterization of negatively charged nitrogen-vacancy (NV−) centers in diamond. Spectroscopic properties such as absorption and emission spectra as well as kinetics were studied, and parameters such as cross-sections and lifetimes were estimated. A vibronic band of NV0 with zero phonon line (ZPL) at 575 nm was detected under 532 nm pulsed excitation due to the photoionization of NV−. Transmission of 532 nm pump pulses saturate around ∼10%, which is much smaller than the theoretical level. Δk/k0 kinetics revealed slow recovery of NV− centers after photoionization under 532 nm pumping, which involved different relaxation channels depending on the probe beam wavelengths. Localization of the electrons in the metastable state of NV0 centers resulted in higher saturated transmission of 632 nm pump.