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Strain broadening of the 1042-nm zero phonon line of the NV- center in diamond: A promising spectroscopic tool for defect tomography

Alexander N. Smirnov, Audrius Alkauskas, Marcus W. Doherty, Timur Biktagirov, V. A. Soltamov, Валерий Александрович Давыдов, Brant C. Gibson

Published Jan 1, 2017• 2 citations
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Strain broadening of the 1042-nm zero phonon line of the NV− center in diamond: A promising spectroscopic tool for defect tomography

Timur Biktagirov, Alexander N. Smirnov, Валерий Александрович Давыдов +4 more

The negatively charged nitrogen-vacancy $({\mathrm{NV}}^{\ensuremath{-}})$ center in diamond is a promising candidate for many quantum applications. Here, we examine the splitting and broadening of the center's infrared (IR) zero-phonon line (ZPL). We develop a model for these effects that accounts for the strain induced by photodependent microscopic distributions of defects. We apply this model to interpret observed variations of the IR ZPL shape with temperature and photoexcitation conditions. We identify an anomalous temperature-dependent broadening mechanism and that defects other than the substitutional nitrogen center significantly contribute to strain broadening. The former conclusion suggests the presence of a strong Jahn-Teller effect in the center's singlet levels and the latter indicates that major sources of broadening are yet to be identified. These conclusions have important implications for the understanding of the center and the engineering of diamond quantum devices. Finally, we propose that, once the major sources of broadening are identified, the IR ZPL has the potential to be a sensitive spectroscopic tool for probing microscopic strain fields and performing defect tomography.

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Optical Spectroscopy of Xenon-Related Defects in Diamond

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The work presents the results of optical studies of Xe-related defect in diamond. This defect is one of a few having narrow zero-phonon line in the near-infrared part of the photo-luminescence spectra. It appears in diamond after Xe+ ion implantation followed by thermal annealing. Given unique physical properties of diamond (hardness, optical transparency in wide spectral range, chemical inertness, high thermal conductivity, low thermal expansion coefficient) and stability of Xe-related center it can be viewed as an potential candidate for the source of single-photons, or as optically manipulated qubit, not unlike nitrogen-vacancy center. However, compared to the latter Xe-related center is not as well understood and it is necessary to gain thorough understanding of its spatial structure, symmetry, electronic states and mechanisms of interaction with the host diamond lattice. This thesis addresses several questions, in regard to Xe-related center: 1) How efficiently this center is formed in the implantation/annealing process; 2) How does it interact with the host lattice to produce both homogeneous and inhomogeneous shape of the 811.7 nm zero-phonon line; and 3) What is the type and nature of transitions responsible for the 811.7 nm zero-phonon line. In answering the first question two methods for measuring the conversion efficiency of any kind of optically active defect have been developed and applied to Xe-related center in diamond. The study of line-broadening mechanisms showed how this center interacts with the strain produced by other neighboring Xe-centers, distributed in a plane-like geometry. Also, interaction with vibrational motions of the diamond lattice localized in the vicinity of the Xe-centers is analyzed and the parameters of this pseudo-local mode are found. Finally, using the effects of optical saturation in photo-luminescence under excitation with Gaussian laser beams it has been shown that 811.7 nm zero-phonon line is due to absorption and emission by circular magnetic dipole. Also, the site symmetry of Xe-related center has been confirmed as trigonal with the threefold axis oriented alongdirection in the diamond crystal.

•Jan 1, 2014•2 citations

Spectroscopy on single N–V defect centers in diamond: tunneling of nitrogen atoms into vacancies and fluorescence spectra

S. Ya. Kilin, Alexander P. Nizovtsev, Tatiana M. Maevskaya +2 more

Journal of Luminescence•Apr 1, 2000•29 citations
The negatively charged nitrogen-vacancy $({\mathrm{NV}}^{\ensuremath{-}})$ center in diamond is a promising candidate for many quantum applications. Here, we examine the splitting and broadening of the center's infrared (IR) zero-phonon line (ZPL). We develop a model for these effects that accounts for the strain induced by photodependent microscopic distributions of defects. We apply this model to interpret observed variations of the IR ZPL shape with temperature and photoexcitation conditions. We identify an anomalous temperature-dependent broadening mechanism and that defects other than the substitutional nitrogen center significantly contribute to strain broadening. The former conclusion suggests the presence of a strong Jahn-Teller effect in the center's singlet levels and the latter indicates that major sources of broadening are yet to be identified. These conclusions have important implications for the understanding of the center and the engineering of diamond quantum devices. Finally, we propose that, once the major sources of broadening are identified, the IR ZPL has the potential to be a sensitive spectroscopic tool for probing microscopic strain fields and performing defect tomography.
The time-averaged emission spectrum of single nitrogen-vacancy defects in diamond gives zero-phonon lines of both the negative charge state at 637 nm (1.945 eV) and the neutral charge state at 575 nm (2.156 eV). This occurs through photoconversion cycling between the two charge states. Due to strain in the diamond the zero-phonon lines of both charge states are split and it is found that the splitting and polarization of the two zero-phonon lines are the same. From this observation and consideration of the electronic structure of the nitrogen-vacancy center it is concluded that the excited state of the neutral center has A2{A}_{2}A2​ orbital symmetry. The assignment of the 575-nm transition to a 2E{}^{2}E2E-2A2{}^{2}{A}_{2}2A2​ transition has not been established previously.
The work presents the results of optical studies of Xe-related defect in diamond. This defect is one of a few having narrow zero-phonon line in the near-infrared part of the photo-luminescence spectra. It appears in diamond after Xe+ ion implantation followed by thermal annealing. Given unique physical properties of diamond (hardness, optical transparency in wide spectral range, chemical inertness, high thermal conductivity, low thermal expansion coefficient) and stability of Xe-related center it can be viewed as an potential candidate for the source of single-photons, or as optically manipulated qubit, not unlike nitrogen-vacancy center. However, compared to the latter Xe-related center is not as well understood and it is necessary to gain thorough understanding of its spatial structure, symmetry, electronic states and mechanisms of interaction with the host diamond lattice. This thesis addresses several questions, in regard to Xe-related center: 1) How efficiently this center is formed in the implantation/annealing process; 2) How does it interact with the host lattice to produce both homogeneous and inhomogeneous shape of the 811.7 nm zero-phonon line; and 3) What is the type and nature of transitions responsible for the 811.7 nm zero-phonon line. In answering the first question two methods for measuring the conversion efficiency of any kind of optically active defect have been developed and applied to Xe-related center in diamond. The study of line-broadening mechanisms showed how this center interacts with the strain produced by other neighboring Xe-centers, distributed in a plane-like geometry. Also, interaction with vibrational motions of the diamond lattice localized in the vicinity of the Xe-centers is analyzed and the parameters of this pseudo-local mode are found. Finally, using the effects of optical saturation in photo-luminescence under excitation with Gaussian laser beams it has been shown that 811.7 nm zero-phonon line is due to absorption and emission by circular magnetic dipole. Also, the site symmetry of Xe-related center has been confirmed as trigonal with the threefold axis oriented alongdirection in the diamond crystal.