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arXiv:1301.6197 · Physical Review B

Infrared absorption band and vibronic structure of the nitrogen-vacancy center in diamond

Pauli Kehayias, Marcus W. Doherty, D. English, Ran Fischer, Andrey Jarmola, Kasper Jensen, N. Leefer, Philip Hemmer, Neil B. Manson, Dmitry Budker

Published Oct 16, 2013• 92 citations
arXivHTMLPDF

Abstract

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 ${}^{1}{A}_{1}$ 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 ${}^{1}{A}_{1}$ level.

DOI
10.1103/physrevb.88.165202

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Negatively charged nitrogen-vacancy (NV\ensuremath−{}^{\ensuremath{-}}\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−{}^{\ensuremath{-}}\ensuremath− centers remain unresolved. Understanding these properties can validate theoretical models of NV\ensuremath−{}^{\ensuremath{-}}\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 1E\ensuremath→1A1{}^{1}E\ensuremath{\rightarrow}{}^{1}{A}_{1}1E\ensuremath→1A1​ electronic transition in the NV\ensuremath−{}^{\ensuremath{-}}\ensuremath− center. From this we calculated the 1E\ensuremath→1A1{}^{1}E\ensuremath{\rightarrow}{}^{1}{A}_{1}1E\ensuremath→1A1​ one-phonon absorption spectrum and found it to differ from that of the 3E\ensuremath→3A2{}^{3}E\ensuremath{\rightarrow}{}^{3}{A}_{2}3E\ensuremath→3A2​ transition, a result which is not anticipated by previous group-theoretical models of the NV\ensuremath−{}^{\ensuremath{-}}\ensuremath− electronic states. We identified a high-energy 169-meV localized phonon mode of the 1A1{}^{1}{A}_{1}1A1​ level.
The negatively charged nitrogen-vacancy (NV) defect (NV center) in diamond is a leading candidate to realize solid-state qubits and ultrasensitive magnetometers in ambient conditions. A new interpretation of some of the properties of the center is presented. We show that the double peak in the absorption phonon sidebands may correspond to the local a 1 and e vibration modes of the defect that have very similar energies, and that tunneling of nitrogen atoms in the vacancy does not occur as had been previously suggested.
Abstract Nitrogen-vacancy (NV) defect centers in diamond are key to applications in quantum sensing and quantum computing. They create localized electronic states in the diamond lattice with distinct population relaxation pathways following photoexcitation that ultimately enable its unique properties. The defect is known to exist in two charge states: neutral and negative, with respectively one and two known optically-active electronic transitions. Here, we report on the observation of a large number of hitherto undiscovered excited electronic states in both charge states as evidenced by distinct optical transitions in the infrared to ultraviolet part of the spectrum. These transitions are observed by monitoring the electronic relaxation of NV centers after photoexcitation using transient absorption spectroscopy, directly probing transient phenomena occurring on timescales from femtoseconds to microseconds. We also for the first time probed the electron transfer dynamics from the 3 E state of NV− to nearby single-substitutional nitrogen defects (N s ) that leads to the well-known effect of NV photoluminescence quenching.
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.
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 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 3E^{3}E3E 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 A1{A}_{1}A1​ and EEE character. The results shed light on the NV level structure and optical pumping mechanism.
Nitrogen-vacancy (NV) defect centers in diamond have generated much interest for their uses in quantum information and sensing. Despite the ongoing improvements in sensitivity and the range of new applications, much about the NV basic physics remains unresolved, which is important to understand in order to fully exploit potential uses. In this work I describe a series of experiments on NV basic properties, applications, and projects in between. First, I describe an NV singlet absorption spectroscopy experiment, which searched for additional NV electronic states and studied the 1A1 phonon modes. Next, I discuss an NV microwave saturation spectroscopy experiment, which is useful for NV thermometry, removes inhomogeneous broadening, and can yield information about diamond magnetic spin bath dynamics. I then describe an NV relaxation experiment that senses GHz-frequency magnetic noise, which we demonstrated using paramagnetic substitutional nitrogen (P1) centers. Finally, I describe open questions on the NV singlet states, saturation spectroscopy, and relaxation (and how to address them), and report on my ongoing work on using NVs for nuclear polarization and rotation sensing.