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Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)

Laser-related spectroscopic parameters of NV colour centres in diamond

Vasili G. Savitski, Elisabeth Fraczek, Matthew W. Dale, Ben G. Breeze, Łukasz Dziechciarczyk, Phil Diggle, Matthew Markham, A. Bennett, Harpreet K. Dhillon, Mark E. Newton, Alan J. Kemp

Published Jun 1, 2017• 2 citations
Publisher

Abstract

One of the most common impurities in synthetic diamond is single substitutional nitrogen, which is incorporated in the diamond lattice substituting a carbon atom. If the nitrogen is adjacent to a vacancy in the diamond lattice, it forms the nitrogen-vacancy (NV) colour centre (CC). The negatively charged state of this CC, NV-, is particularly well studied since its quantum properties are suitable for applications such as quantum information processing, single-photon sources and optical magnetometry. NV CCs in the neutral state (NV0) are less widely studied. This CC exhibits broadband luminescence at slightly shorter wavelengths than NV-, and hence is also potentially of interest for tuneable and ultrafast visible laser applications. In this report, we present a detailed study of the laser-related spectroscopic properties of a diamond containing NV0 and NV-CCs.

DOI
10.1109/cleoe-eqec.2017.8086316

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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.

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One of the most common impurities in synthetic diamond is single substitutional nitrogen, which is incorporated in the diamond lattice substituting a carbon atom. If the nitrogen is adjacent to a vacancy in the diamond lattice, it forms the nitrogen-vacancy (NV) colour centre (CC). The negatively charged state of this CC, NV-, is particularly well studied since its quantum properties are suitable for applications such as quantum information processing, single-photon sources and optical magnetometry. NV CCs in the neutral state (NV0) are less widely studied. This CC exhibits broadband luminescence at slightly shorter wavelengths than NV-, and hence is also potentially of interest for tuneable and ultrafast visible laser applications. In this report, we present a detailed study of the laser-related spectroscopic properties of a diamond containing NV0 and NV-CCs.
In this paper, we analyse the prospects for using nitrogen-vacancy centre (NV) containing diamond as a laser gain material by measuring its key laser related parameters. Synthetic chemical vapour deposition grown diamond samples with an NV concentration of ~1 ppm have been selected because of their relatively high NV concentration and low background absorption in comparison to other samples available to us. For the samples measured, the luminescence lifetimes of the NV- and NV0 centres were measured to be 8±1 ns and 20±1 ns respectively. The respective peak stimulated emission cross-sections were (3.6±0.1)×10-17 cm2 and (1.7±0.1)×10-17 cm2. These measurements were combined with absorption measurements to calculate the gain spectra for NV- and NV0 for differing inversion levels. Such calculations indicate that gains approaching those required for laser operation may be possible with one of the samples tested and for the NV- centre.
The Nitrogen Vacancy (NV) centre is a point defect consisting of a nitrogen-vacancy lattice pair embedded in diamond. The NV centre has two stable charge states, the neutral charge state and the (NV0) and the negatively charged state (NV-) with photo induced interconversion between these two states [1]. The NV centre is an intensively studied material that has shown a wide range of applications in both Physics and Biology due to its high stability and interesting optical properties. Applications ranging from imaging and tracking biological structures, to nanoscale sensing, to applications in highly controlled quantum experiments have all been realised using these centres [2, 3]. However, these applications rely only on the NV-charge stage and often neglect the effects of the neutral charge state. As a result the NV0charge state has not received the same level of study as the NV-state and the effects of the interconversion between the two states are poorly understood, even though it can have a significant effect on the emitted fluorescence.
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.
Nitrogen-vacancy (NV) complex in diamond is one of the most prominent solid state defects as the negatively charged NV defect (NV−) is a leading contender for quantum technologies. In quantum information processing applications, NV− is photoexcited that often leads to photoionization to neutral NV defect, NV0, and re-ionization back to NV− should occur to control the S=1 spin of NV−. As a consequence, understanding the photophysics of NV0 is crucial for controlling NV−. Furthermore, recent studies have shown that the S=1/2 electron spin of NV0 can also be initialized and read out at certain conditions that turns single NV0 a potential quantum bit. Quantum optics protocols rest on detailed knowledge on the electronic structure of the given system, which is obviously missing for NV0 in diamond. In this study, we combine the group theory and density functional theory calculations toward exploring the nature of the ground and excited states of NV0. We show that the effective three-electron system of NV0 leads to high correlation effects that make this system very challenging for ab initio simulations.
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.
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.