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arXiv:0902.2256 · New Journal of Physics

Time-averaging within the excited state of the nitrogen-vacancy centre in diamond

Lachlan J. Rogers, R L McMurtrie, Matthew J. Sellars, N B Manson

Published Jun 3, 2009• 113 citations
arXivHTMLPDF

Abstract

The emission intensity of diamond samples containing negatively charged nitrogen-vacancy centres are measured as a function of magnetic field along the ⟨111⟩ direction for various temperatures. At low temperatures the responses are sample and stress dependent and can be modelled in terms of the previous understanding of the 3 E excited state fine structure which is strain dependent. At room temperature the responses are largely sample and stress independent, and modelling involves invoking a strain independent excited state with a single zero field spin-level splitting of 1.42 GHz. The change in behaviour is attributed to a temperature dependent averaging process over the components of the excited state orbital doublet. It decouples orbit and spin and at high temperature the spin levels become independent of any orbit splitting. One significant implication of this averaging is that it simplifies the development of room temperature applications.

DOI
10.1088/1367-2630/11/6/063007

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The emission intensity of diamond samples containing negatively charged nitrogen-vacancy centres are measured as a function of magnetic field along the ⟨111⟩ direction for various temperatures. At low temperatures the responses are sample and stress dependent and can be modelled in terms of the previous understanding of the 3 E excited state fine structure which is strain dependent. At room temperature the responses are largely sample and stress independent, and modelling involves invoking a strain independent excited state with a single zero field spin-level splitting of 1.42 GHz. The change in behaviour is attributed to a temperature dependent averaging process over the components of the excited state orbital doublet. It decouples orbit and spin and at high temperature the spin levels become independent of any orbit splitting. One significant implication of this averaging is that it simplifies the development of room temperature applications.
Under optical illumination in the blue or green, negatively charged nitrogen vacancy centres in diamond emit in the red. The intensity of this emission varies slightly depending on spin state occupation. Optical transitions occur predominantly without change of spin projection. However, excited ms=±1 states can decay non-radiatively to the ground ms=0 state via intermediary singlet states. With continuous excitation, this effect transfers most of the population to the ms=0 state resulting in decay becoming almost entirely radiative so that optical emission is stronger than when all spin states are occupied equally. However, under optical illumination the ms=0 polarization is reduced when an applied magnetic field induces avoided crossings between energy levels. The spin states are mixed and some population is diverted into the ms=±1 states with consequent reduction in optical emission. The change of emission can be calculated from a rate equation model involving the spin states of the ground and excited levels plus one singlet level [5]. The spin states of the excited levels are also affected by strain and in this work we calculate the variation in optical emission with changing magnetic field for various fixed values of strain.
The negative Nitrogen-Vacancy (NV) colour centre in diamond is an atomic-level impurity that is remarkably well suited for quantum information processing and quantum metrology applications. Underlying these properties is the fact that optical illumination causes the NV centre to preferentially populate one of its three spin levels. The mechanism that gives rise to this spin polarisation has not been well understood, despite intense research interest in the NV centre and its applications. This thesis arrives at an account of the spin polarisation mechanism, although a detailed theoretical treatment remains outstanding. The energy level structure of the NV centre is investigated using techniques of solid state spectroscopy. These include absorption and photoluminescence measurements made on diamonds at cryogenic and room temperatures in the presence of uniaxial stress, magnetic fields, and microwaves. Pulsed light experiments allow the dynamic processes within the NV centre to be measured. It is shown that at room temperature the orbital doublet excited state behaves like an orbital singlet, and this description is elegantly confirmed by single-site observations. This picture of the excited state is inconsistent with cryogenic measurements, and its behaviour is examined across a range of temperatures in order to resolve this tension. It is shown that electron-vibration interaction accounts for the quenching of orbital properties in the excited state with temperature. A new optical transition within the NV centre is reported at a wavelength of 1042 nm. It is established that this transition occurs between the intermediate singlet levels which are thought to provide the decay pathway that produces spin polarisation. The results are consistent with this understanding, and the order and properties of these singlet levels are established. Electron-vibration interaction is observed to be important within the singlet system. It is shown that electron-vibration interaction is an important detail in the NV optical pumping cycle. Taking it into consideration leads to the first plausible physical description of the spin polarisation mechanism. -- provided by Candidate.
We present a comprehensive study of the temperature- and magnetic-field-dependent photoluminescence (PL) of individual NV centers in diamond, spanning the temperature-range from cryogenic to ambient conditions. We directly observe the emergence of the NV's room-temperature effective excited-state structure and provide a clear explanation for a previously poorly understood broad quenching of NV PL at intermediate temperatures around 50 K, as well as the subsequent revival of NV PL. We develop a model based on two-phonon orbital averaging that quantitatively explains all of our findings, including the strong impact that strain has on the temperature dependence of the NV's PL. These results complete our understanding of orbital averaging in the NV excited state and have significant implications for the fundamental understanding of the NV center and its applications in quantum sensing.
We investigate the magnetic field dependent photophysics of individual nitrogen-vacancy (NV) color centers in diamond under cryogenic conditions. At distinct magnetic fields, we observe significant reductions in the NV photoluminescence rate, which indicate a marked decrease in the optical readout efficiency of the NV's ground state spin. We assign these dips to excited state level anticrossings, which occur at magnetic fields that strongly depend on the effective, local strain environment of the NV center. Our results offer new insights into the structure of the NVs' excited states and a new tool for their effective characterization. Using this tool, we observe strong indications for strain-dependent variations of the NV's orbital g factor, obtain new insights into NV charge state dynamics, and draw important conclusions regarding the applicability of NV centers for low-temperature quantum sensing.
We report on measurements of the photoluminescence properties of single nitrogen-vacancy centers in diamond at temperatures between 4 K and 300 K. We observe a strong reduction of the PL intensity and spin contrast between ca. 10 K and 100 K that recovers to high levels below and above. Further, we find a rich dependence on magnetic bias field and crystal strain. We develop a comprehensive model based on spin mixing and orbital hopping in the electronic excited state that quantitatively explains the observations. Beyond a more complete understanding of the excited-state dynamics, our work provides a novel approach for probing electron-phonon interactions and a predictive tool for optimizing experimental conditions for quantum applications.
We report a study of the 3E excited-state structure of single negatively charged nitrogen-vacancy (NV) defects in diamond, combining resonant excitation at cryogenic temperatures and optically detected magnetic resonance. A theoretical model is developed and shows excellent agreement with experimental observations. In addition, we show that the two orbital branches associated with the 3E excited state are averaged when operating at room temperature. This study leads to an improved physical understanding of the NV defect electronic structure, which is invaluable for the development of diamond-based quantum information processing.