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arXiv:1009.0032 · Physical Review B

Optical properties of the nitrogen-vacancy singlet levels in diamond

Víctor M. Acosta, Andrey Jarmola, Erik Bauch, Dmitry Budker

Published Nov 17, 2010• 228 citations
arXivHTMLPDF

Abstract

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 ${m}_{s}=\ifmmode\pm\else\textpm\fi{}1$ sublevels of the $^{3}E$ excited state and is short lived with a lifetime of $\ensuremath{\lesssim}1\text{ }\text{ns}$. 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 light on the NV level structure and optical pumping mechanism.

DOI
10.1103/physrevb.82.201202

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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 ms=\ifmmode±\else\textpm\fi1{m}_{s}=\ifmmode\pm\else\textpm\fi{}1ms​=\ifmmode±\else\textpm\fi1 sublevels of the 3E^{3}E3E excited state and is short lived with a lifetime of \ensuremath≲1 ns\ensuremath{\lesssim}1\text{ }\text{ns}\ensuremath≲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 A1{A}_{1}A1​ and EEE character. The results shed light on the NV level structure and optical pumping mechanism.
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.
The negatively charged nitrogen vacancy ($\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$) defect in diamond serves as a popular platform for manipulating and exploiting long-lived coherent spin dynamics at room temperature combined with optical readout. The required spin polarization of the spin triplet 3A2^{3}A_{2}3A2​ electronic ground state occurs through a cycle of repetitious optical photoexcitation events to the 3E^{3}E3E electronic excited state that is accompanied by a series of electronic transitions to a 1A1^{1}A_{1}1A1​ and a 1E^{1}E1E electronic state, and back to the 3A2^{3}A_{2}3A2​ state. The timescales of these transitions are largely known, yet for the relaxation time of the $^{1}A_{1}\ensuremath{\rightarrow}^{1}E$ infrared transition, which predominantly occurs via nonradiative recombination, only an upper limit of 1 ns could be determined so far. Here, we employ ultrafast transient absorption spectroscopy to probe the dynamics of the nonradiative relaxation from the 1A1^{1}A_{1}1A1​ to the 1E^{1}E1E state after photoexcitation of the 3E^{3}E3E state and find a relaxation time of 100 ps at a temperature of 78 K.
Negatively charged nitrogen-vacancy (NV${}^{\ensuremath{-}}$) color centers in diamond have generated much interest for use in quantum technology. Despite the progress made in developing their applications, many questions about the basic properties of NV${}^{\ensuremath{-}}$ centers remain unresolved. Understanding these properties can validate theoretical models of NV${}^{\ensuremath{-}}$, improve their use in applications, and support their development into competitive quantum devices. In particular, knowledge of the phonon modes of the 1A1{}^{1}{A}_{1}1A1​ electronic state is key for understanding the optical pumping process. Using pump-probe spectroscopy, we measured the phonon sideband of the ${}^{1}E\ensuremath{\rightarrow}{}^{1}{A}_{1}$ electronic transition in the NV${}^{\ensuremath{-}}$ center. From this we calculated the ${}^{1}E\ensuremath{\rightarrow}{}^{1}{A}_{1}$ one-phonon absorption spectrum and found it to differ from that of the ${}^{3}E\ensuremath{\rightarrow}{}^{3}{A}_{2}$ transition, a result which is not anticipated by previous group-theoretical models of the NV${}^{\ensuremath{-}}$ electronic states. We identified a high-energy 169-meV localized phonon mode of the 1A1{}^{1}{A}_{1}1A1​ level.
We report on the spectroscopic and laser characterization of negatively charged nitrogen-vacancy (NV−) centers in diamond. Spectroscopic properties such as absorption and emission spectra as well as kinetics were studied, and parameters such as cross-sections and lifetimes were estimated. A vibronic band of NV0 with zero phonon line (ZPL) at 575 nm was detected under 532 nm pulsed excitation due to the photoionization of NV−. Transmission of 532 nm pump pulses saturate around ∼10%, which is much smaller than the theoretical level. Δk/k0 kinetics revealed slow recovery of NV− centers after photoionization under 532 nm pumping, which involved different relaxation channels depending on the probe beam wavelengths. Localization of the electrons in the metastable state of NV0 centers resulted in higher saturated transmission of 632 nm pump.
Optical illumination on negatively charged nitrogen-vacancy $(\mathrm{N}{\mathrm{V}}^{\ensuremath{-}})$ centers inevitably causes stochastic charge-state transitions between the $\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$ and the neutral charge state of the NV center. It limits the steady-state population of $\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$ to 5% at minimum (\ensuremath{\sim}610 nm) and 80% (\ensuremath{\sim}532 nm) at maximum in intrinsic diamond depending on the wavelength. Here, we show Fermi-level control by phosphorus doping generates 99.4 \ifmmode\pm\else\textpm\fi{} 0.1% $\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$ under 1-\ensuremath{\mu}W and 593-nm excitation which is close to maximum absorption of $\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$. The pure $\mathrm{N}{\mathrm{V}}^{\ensuremath{-}}$ shows a fivefold increase in luminescence and a fourfold enhancement of an optically detected magnetic resonance under 593-nm excitation compared with those in intrinsic diamond.
We investigate spin-dependent decay and intersystem crossing (ISC) in the optical cycle of single negatively charged nitrogen-vacancy (NV) centres in diamond. We use spin control and pulsed optical excitation to extract both the spin-resolved lifetimes of the excited states and the degree of optically induced spin polarization. By optically exciting the centre with a series of picosecond pulses, we determine the spin-flip probabilities per optical cycle, as well as the spin-dependent probability for ISC. This information, together with the independently measured decay rate of singlet population, provides a full description of spin dynamics in the optical cycle of NV centres. The temperature dependence of the singlet population decay rate provides information about the number of singlet states involved in the optical cycle.