The recently discovered negatively charged tin-vacancy centre in diamond is a promising candidate for applications in quantum information processing (QIP). We here present a detailed spectroscopic study encompassing single photon emission and polarisation properties, the temperature dependence of emission spectra as well as a detailed analysis of the phonon sideband and Debye-Waller factor. Using photoluminescence excitation spectroscopy (PLE) we probe an energetically higher lying excited state and prove fully lifetime limited linewidths of single emitters at cryogenic temperatures. For these emitters we also investigate the stability of the charge state under resonant excitation. These results provide a detailed insight into the spectroscopic properties of the $text{SnV}^-$ centre and lay the foundation for further studies regarding its suitability in QIP.
Negatively charged nitrogen-vacancy centres in diamond are promising quantum magnetic field sensors. Laser threshold magnetometry has been a theoretical approach for the improvement of NV-centre ensemble sensitivity via increased signal strength and magnetic field contrast. In this work we experimentally demonstrate laser threshold magnetometry. We use a macroscopic high-finesse laser cavity containing a highly NV-doped and low absorbing diamond gain medium that is pumped at 532nm and resonantly seeded at 710nm. This enables amplification of the signal power by stimulated emission of 64%. We show the magnetic-field dependency of the amplification and thus, demonstrate magnetic-field dependent stimulated emission from an NV-centre ensemble. This emission shows a record contrast of 33% and a maximum output power in the mW regime. These advantages of coherent read-out of NV-centres pave the way for novel cavity and laser applications of quantum defects as well as diamond NV magnetic field sensors with significantly improved sensitivity for the health, research and mining sectors.
Stimulated emission is the process fundamental to laser operation, thereby producing coherent photon output. Despite negatively-charged nitrogen-vacancy (NV$^-$) centres being discussed as a potential laser medium since the 1980s, there have been no definitive observations of stimulated emission from ensembles of NV$^-$ to date. Reasons for this lack of demonstration include the short excited state lifetime and the occurrence of photo-ionisation to the neutral charge state by light around the zero-phonon line. Here we show both theoretical and experimental evidence for stimulated emission from NV$^-$ states using light in the phonon-sidebands. Our system uses a continuous wave pump laser at 532 nm and a pulsed stimulating laser that is swept across the phononic sidebands of the NV$^-$. Optimal stimulated emission is demonstrated in the vicinity of the three-phonon line at 700 nm. Furthermore, we show the transition from stimulated emission to photoionisation as the stimulating laser wavelength is reduced from 700nm to 620 nm. While lasing at the zero-phonon line is suppressed by ionisation, our results open the possibility of diamond lasers based on NV centres, tuneable over the phonon-sideband. This broadens the applications of NV magnetometers from single centre nanoscale sensors to a new generation of ultra-precise ensemble laser sensors, which exploit the contrast and signal amplification of a lasing system.
We study single silicon vacancy (SiV) centres in chemical vapour deposition (CVD) nanodiamonds on iridium as well as an ensemble of SiV centres in a high quality, low stress CVD diamond film by using temperature dependent luminescence spectroscopy in the temperature range 5-295 K. We investigate in detail the temperature dependent fine structure of the zero-phonon-line (ZPL) of the SiV centres. The ZPL transition is affected by inhomogeneous as well as temperature dependent homogeneous broadening and blue shifts by about 20 cm-1 upon cooling from room temperature to 5 K. We employ excitation power dependent g(2) measurements to explore the temperature dependent internal population dynamics of single SiV centres and infer almost temperature independent dynamics.
Group-IV color centers in diamond are a promising light-matter interface for quantum networking devices. The negatively charged tin-vacancy center (SnV) is particularly interesting, as its large spin-orbit coupling offers strong protection against phonon dephasing and robust cyclicity of its optical transitions towards spin-photon entanglement schemes. Here, we demonstrate multi-axis coherent control of the SnV spin qubit via an all-optical stimulated Raman drive between the ground and excited states. We use coherent population trapping and optically driven electronic spin resonance to confirm coherent access to the qubit at 1.7 K, and obtain spin Rabi oscillations at a rate of $Omega/2pi$=3.6(1) MHz. All-optical Ramsey interferometry reveals a spin dephasing time of $T_2^*$=1.3(3)$mu$s and two-pulse dynamical decoupling already extends the spin coherence time to $T_2$=0.33(14) ms. Combined with transform-limited photons and integration into photonic nanostructures, our results make the SnV a competitive spin-photon building block for quantum networks.
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.