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arXiv:2106.02380 · New Journal of Physics

Revealing superradiant emission in the single-to-bulk transition of quantum emitters in nanodiamond agglomerates

Jonas Gutsche, Ashkan Zand, Marek Bültel, Artur Widera

Published Apr 29, 2022• 5 citations
arXivHTMLPDF

Abstract

Abstract Individual quantum emitters form a fundamental building block for emerging quantum technologies. Collective effects of emitters, such as superradiance, might improve the performance of applications even further. When scaling materials to larger sizes, however, the optical density of states is modified by the surrounding material, and the collective coupling in small domains might be covered by transitions to bulk properties due to the presence of multiple collectively emitting domains, which inhomogeneously add. Here, we probe the optical properties of nitrogen vacancy centers in agglomerates of nanodiamonds. We quantify the transition from individual emitters to bulk emission by fluorescence lifetime measurements, and find a transition to occur on a length scale of ∼ 3 wavelengths around the emitter. While our lifetime measurements are consistent with superradiant decay, the second-order correlation function, which is a standard measure to reveal collective properties, fails to probe collective effects for our case of an ensemble of collectively contributing domains to the emission. Therefore, we propose and apply a new measure to trace collective effects based on the intensity fluctuations of the emitted light. Our work points toward systematically studying collective effects in a scalable solid-state quantum system, and using them for quantum optical applications in agglomerates of highly-doped nanodiamonds.

DOI
10.1088/1367-2630/ac6bb8

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Abstract Individual quantum emitters form a fundamental building block for emerging quantum technologies. Collective effects of emitters, such as superradiance, might improve the performance of applications even further. When scaling materials to larger sizes, however, the optical density of states is modified by the surrounding material, and the collective coupling in small domains might be covered by transitions to bulk properties due to the presence of multiple collectively emitting domains, which inhomogeneously add. Here, we probe the optical properties of nitrogen vacancy centers in agglomerates of nanodiamonds. We quantify the transition from individual emitters to bulk emission by fluorescence lifetime measurements, and find a transition to occur on a length scale of ∼ 3 wavelengths around the emitter. While our lifetime measurements are consistent with superradiant decay, the second-order correlation function, which is a standard measure to reveal collective properties, fails to probe collective effects for our case of an ensemble of collectively contributing domains to the emission. Therefore, we propose and apply a new measure to trace collective effects based on the intensity fluctuations of the emitted light. Our work points toward systematically studying collective effects in a scalable solid-state quantum system, and using them for quantum optical applications in agglomerates of highly-doped nanodiamonds.
The nitrogen vacancy (NV) center is the most widely studied single optical defect in diamond with great potential for applications in quantum technologies. Development of practical single-photon devices requires an understanding of the emission under a range of conditions and environments. In this work, we study the properties of a single NV center in nanodiamonds embedded in an air-like silica aerogel environment which provides a new domain for probing the emission behavior of NV centers in nanoscale environments. In this arrangement, the emission rate is governed primarily by the diamond crystal lattice with negligible contribution from the surrounding environment. This is in contrast to the conventional approach of studying nanodiamonds on a glass coverslip. We observe an increase in the mean lifetime due to the absence of a dielectric interface near the emitting dipoles and a distribution arising from the irregularities in the nanodiamond geometry. Our approach results in the estimation of the mean quantum efficiency (~0.7) of the nanodiamond NV emitters.
When an ensemble of quantum emitters couples to a common radiation field, their polarizations can synchronize and a collective emission termed superfluorescence can occur. Entering this regime in a free-space setting requires a large number of emitters with a high spatial density as well as coherent optical transitions with small inhomogeneity. Here, we show that, by coupling nitrogen-vacancy centers in a diamond membrane to a high-finesse microcavity, also few, incoherent, inhomogeneous, and spatially separated emitters—as are typical for solid state systems—can enter the regime of collective emission. We observe a superlinear power dependence of the emission rate as a hallmark of collective emission. Furthermore, we find simultaneous photon bunching and antibunching on different timescales in the second-order autocorrelation function, revealing cavity-induced interference in the quantized emission from about 15 emitters. We develop theoretical models for mesoscopic emitter numbers to analyze the behavior in the Dicke state basis and find that the population of collective states together with cavity enhancement and filtering can explain the observations. Such a system has prospects for the generation of multiphoton quantum states, the preparation of entanglement in few-emitter systems, and enhancement of signals in quantum sensing. Published by the American Physical Society 2024
We perform intensity correlation (g(2)(τ)g^{(2)}(τ)g(2)(τ)) measurements on nitrogen-vacancy (NV) emitters embedded in diamond nanopillars. We observe an increase in transition rates from both the singlet and triplet states by a factor of ≈6\approx 6≈6, indicating cooperative effects between the multiple emitters in the pillar, at room temperature. We simultaneously observe a g(2)(0)>0.5(→1g^{(2)}(0) > 0.5 (\to 1g(2)(0)>0.5(→1) as opposed to g(2)(0)<0.5g^{(2)}(0) < 0.5g(2)(0)<0.5 for others (and as expected for single emitters), indicating the presence of at least two emitters. Furthermore, we observe a triple exponential behaviour for the g(2)g^{(2)}g(2) in contrast to the standard double exponential behaviour seen for single NV emitters. To understand our experimental observations, we developed a theoretical model. We solve the Lindblad master equation, tailored for single and two NV centers, to study their dissipative dynamics when coupled to a common electromagnetic field, at a finite temperature. Through this, we identify superradiant emission from a two-emitter system as the most likely explanation for our observed data. We also find that random number generation using the coupled emitter system performs better under the NIST test suite and explain it in terms of an entropy-driven model for a coupled emitter system. Our results provide a new signature for multiphotonic states, such as superradiant states, using intensity correlation measurements, that will become important for quantum photonic technologies progress.
Collective light emission from many-body quantum systems is a cornerstone of quantum optics, yet its implementation in solid-state platforms operating under ambient conditions remains highly challenging. Large-bandgap van der Waals materials such as hexagonal boron nitride (hBN) host stable room-temperature single-photon emitters with narrow linewidths across a broad spectral range. However, cooperative radiative effects in this system have not been previously explored. Here we demonstrate collective emission from quantum-emitter ensembles in hBN layers when the emitters are nearly indistinguishable and positioned within a sub-wavelength proximity. Using confocal microscopy and a Hanbury Brown-Twiss (HBT) configuration, we identify both isolated emitters and ensembles activated by localized electron-beam irradiation. Time-resolved photoluminescence measurements reveal a superlinear intensity enhancement and a pronounced acceleration of the radiative decay in tightly confined ensembles, with lifetimes approaching the temporal resolution of our experimental system (about 500 ps), compared to approximately 1.85 ns for single emitters or large, spatially extended ensembles. Complementary second-order photon-correlation measurements exhibit sub-Poissonian antidip consistent with emission from a few indistinguishable emitters. The simultaneous observation of lifetime shortening and enhanced emission provides direct evidence of cooperative emission at room temperature, achieved without optical cavities or cryogenic cooling. These results establish optically active defect ensembles in hBN as a scalable solid-state platform for engineered collective quantum optics in two-dimensional materials, opening avenues toward ultrabright superradiant light sources and nonclassical photonic states for quantum technologies.
Their intrinsic properties render single quantum systems as ideal tools for quantum enhanced sensing and microscopy. As an additional benefit, their size is typically on an atomic scale that enables sensing with very high spatial resolution. Here, we report on utilizing a single nitrogen vacancy center in nanodiamond for performing three-dimensional scanning-probe fluorescence lifetime imaging microscopy. By measuring changes of the single emitter's lifetime, information on the local density of optical states is acquired at the nanoscale. Three-dimensional ab initio discontinuous Galerkin time-domain simulations are used in order to verify the results and to obtain additional insights. This combination of experiment and simulations to gather quantitative information on the local density of optical states is of direct relevance for the understanding of fundamental quantum optical processes as well as for the engineering of novel photonic and plasmonic devices.
The nitrogen vacancy center in diamond in its negative charge state is a promising candidate for quantum optic experiments that require single photon emitters. Important benefits of the NV center are its high brightness and photo-stability, even at room temperature. Engineering the emission properties of NV centers with optical resonators is a widely followed approach to meet the requirements for quantum technological applications, but the effect on non-radiative decay paths is yet to be understood. Here we report on modifying the internal quantum efficiency of a single NV center in a nanodiamond coupled to a 1D photonic crystal cavity. We assess the Purcell enhancement via three independent measurement techniques and perform autocorrelation measurements at elevated excitation powers in confocal microscopy. Employing a three-level model allows us to extract the setup efficiency, individual transition rates and thus the internal quantum efficiency of our system. Combining our results, we find that the enhancement of the radiative decay rate via the Purcell effect results in an internal quantum efficiency of 90 % for cavity-coupled NV centers. Our findings will facilitate the realization of nano-scale single photon sources with near-unity internal quantum efficiencies operating at high repetition rates.