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Register a new userOptical properties of the nitrogen-vacancy singlet levels in diamond
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We report measurements of the optical properties of the 1042 nm transition of negatively-charged Nitrogen-Vacancy (NV) centers in type 1b diamond. The results indicate that the upper level of this transition couples to the m_s=+/-1 sublevels of the {^3}E excited state and is short-lived, with a lifetime <~ 1 ns. The lower level is shown to have a temperature-dependent lifetime of 462(10) ns at 4.4 K and 219(3) ns at 295 K. The light-polarization dependence of 1042 nm absorption confirms that the transition is between orbitals of A_1 and E character. The results shed new light on the NV level structure and optical pumping mechanism.
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We report electrical tuning by the Stark effect of the excited-state structure of single nitrogen-vacancy (NV) centers located less than ~100 nm from the diamond surface. The zero-phonon line (ZPL) emission frequency is controllably varied over a range of 300 GHz. Using high-resolution emission spectroscopy, we observe electrical tuning of the strengths of both cycling and spin-altering transitions. Under resonant excitation, we apply dynamic feedback to stabilize the ZPL frequency. The transition is locked over several minutes and drifts of the peak position on timescales greater than ~100 ms are reduced to a fraction of the single-scan linewidth, with standard deviation as low as 16 MHz (obtained for an NV in bulk, ultra-pure diamond). These techniques should improve the entanglement success probability in quantum communications protocols.
We present a procedure that makes use of group theory to analyze and predict the main properties of the negatively charged nitrogen-vacancy (NV) center in diamond. We focus on the relatively low temperatures limit where both the spin-spin and spin-orbit effects are important to consider. We demonstrate that group theory may be used to clarify several aspects of the NV structure, such as ordering of the singlets in the ($e^2$) electronic configuration, the spin-spin and the spin-orbit interactions in the ($ae$) electronic configuration. We also discuss how the optical selection rules and the response of the center to electric field can be used for spin-photon entanglement schemes. Our general formalism is applicable to a broad class of local defects in solids. The present results have important implications for applications in quantum information science and nanomagnetometry.
We theoretically propose a method to realize optical nonreciprocity in rotating nano-diamond with a nitrogen-vacancy (NV) center. Because of the relative motion of the NV center with respect to the propagating fields, the frequencies of the fields are shifted due to the Doppler effect. When the control and probe fields are incident to the NV center from the same direction, the two-photon resonance still holds as the Doppler shifts of the two fields are the same. Thus, due to the electromagnetically-induced transparency (EIT), the probe light can pass through the NV center nearly without absorption. However, when the two fields propagate in opposite directions, the probe light can not effectively pass through the NV center as a result of the breakdown of two-photon resonance.
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.
A study of the photophysical properties of nitrogen-vacancy (NV) color centers in diamond nanocrystals of size of 50~nm or below is carried out by means of second-order time-intensity photon correlation and cross-correlation measurements as a function of the excitation power for both pure charge states, neutral and negatively charged, as well as for the photochromic state, where the center switches between both states at any power. A dedicated three-level model implying a shelving level is developed to extract the relevant photophysical parameters coupling all three levels. Our analysis confirms the very existence of the shelving level for the neutral NV center. It is found that it plays a negligible role on the photophysics of this center, whereas it is responsible for an increasing photon bunching behavior of the negative NV center with increasing power. From the photophysical parameters, we infer a quantum efficiency for both centers, showing that it remains close to unity for the neutral center over the entire power range, whereas it drops with increasing power from near unity to approximately 0.5 for the negative center. The photophysics of the photochromic center reveals a rich phenomenology that is to a large extent dominated by that of the negative state, in agreement with the excess charge release of the negative center being much slower than the photon emission process.
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