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Register a new userElectronic structure of the negatively-charged silicon-vacancy center in diamond
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The negatively-charged silicon-vacancy (SiV$^-$) center in diamond is a promising single photon source for quantum communications and information processing. However, the centers implementation in such quantum technologies is hindered by contention surrounding its fundamental properties. Here we present optical polarization measurements of single centers in bulk diamond that resolve this state of contention and establish that the center has a $langle111rangle$ aligned split-vacancy structure with $D_{3d}$ symmetry. Furthermore, we identify an additional electronic level and evidence for the presence of dynamic Jahn-Teller effects in the centers 738 nm optical resonance.
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The neutrally-charged silicon vacancy in diamond is a promising system for quantum technologies that combines high-efficiency, broadband optical spin polarization with long spin lifetimes (T2 ~ 1 ms at 4 K) and up to 90% of optical emission into its 946 nm zero-phonon line. However, the electronic structure of SiV0 is poorly understood, making further exploitation difficult. Performing photoluminescence spectroscopy of SiV0 under uniaxial stress, we find the previous excited electronic structure of a single 3A1u state is incorrect, and identify instead a coupled 3Eu - 3A2u system, the lower state of which has forbidden optical emission at zero stress and so efficiently decreases the total emission of the defect: we propose a solution employing finite strain to form the basis of a spin-photon interface. Isotopic enrichment definitively assigns the 976 nm transition associated with the defect to a local mode of the silicon atom.
Deep defects in wide band gap semiconductors have emerged as leading qubit candidates for realizing quantum sensing and information applications. Due to the spatial localization of the defect states, these deep defects can be considered as artificial atoms/molecules in a solid state matrix. Here we show that unlike single-particle treatments, the multiconfigurational quantum chemistry methods, traditionally reserved for atoms/molecules, accurately describe the many-body characteristics of the electronic states of these defect centers and correctly predict properties that single-particle treatments fail to obtain. We choose the negatively charged nitrogen-vacancy (NV$^-$) center in diamond as the prototype defect to study with these techniques due to its importance for quantum information applications and because its properties are well-known, which makes it an ideal benchmark system. By properly accounting for electron correlations and including spin-orbit coupling and dipolar spin-spin coupling in the quantum chemistry calculations, for the NV$^-$ center in diamond clusters, we are able to: (i) show the correct splitting of the ground (first-excited) triplet state into two levels (four levels), (ii) calculate zero-field splitting values of the ground and excited triplet states, in good agreement with experiment, and (iii) calculate the energy differences between ground and exited spin-triplet and spin-singlet states, as well as their ordering, which are also found to be in good agreement with recent experimental data. The numerical procedure we have developed is general and it can screen other color centers whose properties are not well known but promising for applications.
The nitrogen-vacancy (NV) center is a well utilized system for quantum technology, in particular quantum sensing and microscopy. Fully employing the NV centers capabilities for metrology requires a strong understanding of the behavior of the NV center with respect to changing temperature. Here, we probe the NV electronic spin density as the surrounding crystal temperature changes from 10 K to 700 K by examining its $^{13}$C hyperfine interactions. These results are corroborated with textit{ab initio} calculations and demonstrate that the change in hyperfine interaction is small and dominated by a change in the hybridization of the orbitals constituting the spin density. Thus indicating that the defect and local crystal geometry is returning towards an undistorted structure at higher temperature.
We performed high-temperature luminescence studies of silicon-vacancy color centers obtained by ion implantation in single crystal diamond. We observed reduction of the integrated fluorescence upon increasing temperature, ascribable to a transition channel with an activation energy of 180 meV that populates a shelving state. Nonetheless, the signal decreased only 50% and 75% with respect to room temperature at 500 K and 700 K, respectively. In addition, the color center is found highly photostable at temperatures exceeding 800 K. The luminescence of this color center is thus extremely robust even at large temperatures and it holds promise for novel diamond-based light-emitting devices.
Optical and microwave double resonance techniques are used to obtain the excited state structure of single nitrogen-vacancy centers in diamond. The excited state is an orbital doublet and it is shown that it can be split and associated transition strengths varied by external electric fields and by strain. A group theoretical model is developed. It gives a good account of the observations and contributes to an improved understanding of the electronic structure of the center. The findings are important for quantum information processing and other applications of the center.
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