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Homogeneous broadening of the zero-phonon line in the nitrogen-vacancy centre in diamond for all strain regimes

Thom Fronik

Published Jan 1, 2018• 0 citations
OpenAlex

Abstract

The nitrogen-vacancy centre in diamond has shown to be a promising solid-state spin-qubit for applications in quantum information processing. NV centres can be used as nodes in quantum communication networks by remote controlled entanglement. The success of such entanglement schemes depends on the probability of photons being emitted in the zero-phonon line. To increase this probability, NV centres in thin diamond membranes are placed in optical cavities. However, NV centres in thin diamond membranes often show much larger strain splitting. In this thesis, the effect of such strain interactions on the population dynamics and homogeneous broadening of the zero-phonon line of the excited state is determined.

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The Nitrogen-Vacancy (NV) centre in diamond possesses an optical read out of its spin state and shows great promise for applications in solid state quantum technologies. Its broad phonon assisted emission spectrum, with only 4% of emission from the zero-phonon line, is a major drawback to this. The optical microcavity will be essential in efficiently interfacing these centres with photonic networks. Here we present investigations into the coupling of NV centres in nanodiamond to tunable open-microcavities, both at room temperature and at cryogenic temperatures. These structures will be shown to achieve good photon confinement, with mode volumes down to 5λ3. Room temperature studies on ensembles of NVs will illustrate the tunable spectral and spatial overlap between the emitter and the cavity mode. It will be shown that small enhancements are possible in this regime. After the preparation and characterisation of single emitters, low temperature coupling to the narrowed zero-phonon line will be the central theme of this thesis. Single photon emission into the cavity mode is verified. We observe the enhancement of the light-matter interaction in this regime, by a 39% increase in the emission rate when cavity-coupled, with the dependence on mode volume also demonstrated. These results are important for the realisation of a spin-photon interface in scalable quantum networks.

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The realisation of an efficient spin-photon interface using the negatively charged nitrogen-vacancy centre (NV-) in diamond requires the resonant coupling of the zero phonon line (ZPL) of the centre to an optical microcavity [1]. The cavity serves to encourage emission into the ZPL in preference to the phonon sidebands, and potentially also to increase the homogeneous linewidth via a reduction of the lifetime (the Purcell effect) thus assisting in the generation of indistinguishable photons. Cavity coupling thus has potential to improve by orders of magnitude the speed with which entanglement can be created between spatially remote NV- centres [2], and to enable other mechanisms for realising spin-photon interfaces via non-demolition measurements [3].

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The nitrogen-vacancy centre in diamond has shown to be a promising solid-state spin-qubit for applications in quantum information processing. NV centres can be used as nodes in quantum communication networks by remote controlled entanglement. The success of such entanglement schemes depends on the probability of photons being emitted in the zero-phonon line. To increase this probability, NV centres in thin diamond membranes are placed in optical cavities. However, NV centres in thin diamond membranes often show much larger strain splitting. In this thesis, the effect of such strain interactions on the population dynamics and homogeneous broadening of the zero-phonon line of the excited state is determined.
The Nitrogen-Vacancy (NV) centre in diamond possesses an optical read out of its spin state and shows great promise for applications in solid state quantum technologies. Its broad phonon assisted emission spectrum, with only 4% of emission from the zero-phonon line, is a major drawback to this. The optical microcavity will be essential in efficiently interfacing these centres with photonic networks. Here we present investigations into the coupling of NV centres in nanodiamond to tunable open-microcavities, both at room temperature and at cryogenic temperatures. These structures will be shown to achieve good photon confinement, with mode volumes down to 5λ3. Room temperature studies on ensembles of NVs will illustrate the tunable spectral and spatial overlap between the emitter and the cavity mode. It will be shown that small enhancements are possible in this regime. After the preparation and characterisation of single emitters, low temperature coupling to the narrowed zero-phonon line will be the central theme of this thesis. Single photon emission into the cavity mode is verified. We observe the enhancement of the light-matter interaction in this regime, by a 39% increase in the emission rate when cavity-coupled, with the dependence on mode volume also demonstrated. These results are important for the realisation of a spin-photon interface in scalable quantum networks.
The Nitrogen-Vacancy (NV) centre in diamond possesses an optical read out of its spin state and shows great promise for applications in solid state quantum technologies. Its broad phonon assisted emission spectrum, with only 4p of emission from the zero-phonon line, is a major drawback to this. The optical microcavity will be essential in efficiently interfacing these centres with photonic networks. Here we present investigations into the coupling of NV centres in nanodiamond to tunable open-microcavities, both at room temperature and at cryogenic temperatures. These structures will be shown to achieve good photon confinement, with mode volumes down to 5λ3. Room temperature studies on ensembles of NVs will illustrate the tunable spectral and spatial overlap between the emitter and the cavity mode. It will be shown that small enhancements are possible in this regime. After the preparation and characterisation of single emitters, low temperature coupling to the narrowed zero-phonon line will be the central theme of this thesis. Single photon emission into the cavity mode is verified. We observe the enhancement of the light-matter interaction in this regime, by a 39p increase in the emission rate when cavity-coupled, with the dependence on mode volume also demonstrated. These results are important for the realisation of a spin-photon interface in scalable quantum networks.
The realisation of an efficient spin-photon interface using the negatively charged nitrogen-vacancy centre (NV-) in diamond requires the resonant coupling of the zero phonon line (ZPL) of the centre to an optical microcavity [1]. The cavity serves to encourage emission into the ZPL in preference to the phonon sidebands, and potentially also to increase the homogeneous linewidth via a reduction of the lifetime (the Purcell effect) thus assisting in the generation of indistinguishable photons. Cavity coupling thus has potential to improve by orders of magnitude the speed with which entanglement can be created between spatially remote NV- centres [2], and to enable other mechanisms for realising spin-photon interfaces via non-demolition measurements [3].
Abstract Many applications of nitrogen-vacancy (NV) centers in diamond crucially rely on a spectrally narrow and stable optical zero-phonon line transition. Though many impressive proof-of-principle experiments have been demonstrated, much work remains in engineering NV centers with spectral properties that are sufficiently robust for practical implementation. To elucidate the mechanisms underlying their interactions with the environment, we apply multi-dimensional coherent spectroscopy to an NV center ensemble in bulk diamond at cryogenic temperatures. Our spectra reveal thermal dephasing due to quasi-localized vibrational modes as well as ultrafast spectral diffusion on the picosecond timescale. The intrinsic, ensemble-averaged homogeneous linewidth is found to be in the tens of GHz range by extrapolating to zero temperature. We also observe a temperature-dependent Stark splitting of the excited state manifold, relevant to NV sensing protocols.
The negatively charged nitrogen-vacancy $({\mathrm{NV}}^{\ensuremath{-}})$ center in diamond is a promising candidate for many quantum applications. Here, we examine the splitting and broadening of the center's infrared (IR) zero-phonon line (ZPL). We develop a model for these effects that accounts for the strain induced by photodependent microscopic distributions of defects. We apply this model to interpret observed variations of the IR ZPL shape with temperature and photoexcitation conditions. We identify an anomalous temperature-dependent broadening mechanism and that defects other than the substitutional nitrogen center significantly contribute to strain broadening. The former conclusion suggests the presence of a strong Jahn-Teller effect in the center's singlet levels and the latter indicates that major sources of broadening are yet to be identified. These conclusions have important implications for the understanding of the center and the engineering of diamond quantum devices. Finally, we propose that, once the major sources of broadening are identified, the IR ZPL has the potential to be a sensitive spectroscopic tool for probing microscopic strain fields and performing defect tomography.
The nitrogen-vacancy center in diamond is an attractive resource for the generation of remote entangled states owing to its optically addressable and long-lived electronic spin. However, its low native fraction of coherent photon emission, ~3%, undermines the achievable spin-photon entanglement rates. Here, we couple a nitrogen-vacancy center with a narrow extrinsically-broadened linewidth (159 MHz), hosted in a micron-thin membrane, to an open microcavity. The resulting Purcell factor of ~1.8 increases the zero-phonon line fraction to over 44%. Operation in the Purcell regime, together with an efficient collection of the zero-phonon-line photons, allows resonance fluorescence to be detected for the first time without any temporal filtering. We achieve a >10 signal-to-laser background ratio. This selective enhancement of the center's zero-phonon transitions could increase spin-spin entanglement success probabilities beyond an order of magnitude compared to state-of-the-art implementations, and enable powerful quantum optics techniques such as wave-packet shaping or all-optical spin manipulation.