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arXiv:2407.09755 · Physical Review A

Superradiance from nitrogen-vacancy centers coupled to an ultranarrow optical cavity

Yidan Qu, Yuan Zhang, Peinan Ni, Chongxin Shan, David Hunger, Klaus Mølmer

Published Mar 18, 2025• 6 citations
arXivHTMLPDF

Abstract

Nitrogen-vacancy (NV) centers in diamond have been successfully coupled to various optical structures to enhance their radiation by the Purcell effect. The participation of many NV centers in these studies may naturally lead to cooperative emission and superradiance, and our recent experimental study with a diamond membrane in a fiber-based ultranarrow optical cavity demonstrated nonlinear radiation and fast photon bunching as signatures of the collective effects. In this theoretical article, we go beyond the simple model used in the previous study to address more phenomena, such as the appearance of bunching shoulders in second-order correlation function, Rabi splitting in steady-state spectrum, and population dynamics on excited Dicke states, which for moderate pumping explains the observed collective effects. Overall, our results can guide further experiments with NV centers, and they are also relevant for other solid-state color centers, such as silicon-vacancy centers in diamond and silicon carbide, boron-vacancy centers, and carbon-related centers in hexagonal boron nitride.

DOI
10.1103/physreva.111.033711

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Nitrogen-vacancy (NV) centers in diamond have been successfully coupled to various optical structures to enhance their radiation by the Purcell effect. The participation of many NV centers in these studies may naturally lead to cooperative emission and superradiance, and our recent experimental study with a diamond membrane in a fiber-based ultranarrow optical cavity demonstrated nonlinear radiation and fast photon bunching as signatures of the collective effects. In this theoretical article, we go beyond the simple model used in the previous study to address more phenomena, such as the appearance of bunching shoulders in second-order correlation function, Rabi splitting in steady-state spectrum, and population dynamics on excited Dicke states, which for moderate pumping explains the observed collective effects. Overall, our results can guide further experiments with NV centers, and they are also relevant for other solid-state color centers, such as silicon-vacancy centers in diamond and silicon carbide, boron-vacancy centers, and carbon-related centers in hexagonal boron nitride.
This thesis investigates the coupling of the fluorescence of nitrogen-vacancy (NV) centers in diamond to tunable optical microresonators at ambient conditions, in particular in the regime of Purcell enhancement. We use fiber-based, open-access Fabry-Pérot cavities optimized for high finesse and ultra-small mode volume. Different regimes of cavity enhancement are studied that are complementary to each other: A first experiment relies on a high-finesse cavity with dielectric mirrors. The scaling laws of Purcell enhancement are explicitly demonstrated by a large-range variation of both the cavity mode volume (V = 16 − 600 µm^3 ) and the quality factor (Q = 6 · 10^3 − 2 · 10^6). We detect an enhancement of the emission spectral density by up to a factor of 300. The full potential of this resonator can be exploited with emitters having a linewidth which is narrower than the resonance linewidth of the cavity. This concept holds promise for the implementation of wavelength-tunable, narrow-band single-photon sources as well as the generation of indistinguishable single-photons at ambient conditions. However, for broad-band emitters like the NV center at room temperature, the emission lifetime is not affected noticeably in this configuration. In order to directly observe lifetime changes and Purcell-enhanced single-photon emission, we manufacture fiber-based cavities with silver-coated mirrors having ultra-small mode volumes, as small as V = 1.0 λ^3 = 0.34 µm^3. We demonstrate cavity-enhanced fluorescence imaging, which allows to locate and analyze several single NV centers with one cavity. The Purcell effect is evidenced by an enhanced fluorescence collection of up to 1.6 · 10^6 photons per second from single-NV centers and a tunable variation of the emission lifetime corresponding to an effective Purcell factor of up to 2. We furthermore investigate a benefcial regime of optical confinement where the Fabry-Pérot cavity mode is combined with additional mode confinement by the diamond nanocrystal itself, enabling sub-λ^3 mode volumes. We perform simulations that predict effective Purcell factors of up to 11 for NV centers and of up to 63 for silicon-vacancy centers, revealing a great potential for bright single-photon sources and effcient spin readout at ambient conditions.
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
A key requirement for many applications in solid-state quantum sciences is a high fluence of indistinguishable photons. The spontaneous emission of these photons is governed by the coupling of an excited quantum system to electromagnetic vacuum fluctuations. In our experiment, we enhance this coupling by engineering a tunable Fabry-Perot microcavity. The quantum system we study is the nitrogen-vacancy (NV) center in diamond, a workhorse for quantum science and engineering, due to its optical transitions and the coherent electron spin system it hosts. Our device consists of a high-quality, nano-fabricated, single-crystalline diamond membrane bonded to a planar mirror; the cavity is completed by a second, concave mirror. Using piezo positioners, we achieve full spectral and spatial tunability and freedom in selecting NVs with favorable emission properties in our low-temperature (4 Kelvin) experiments. Upon tuning of the cavity into resonance, we find significant enhancement of the 637 nm zero phonon line for several individual NVs which is accompanied by a strong reduction of the overall photoluminescence (PL) lifetime. We infer a 30-fold enhancement of the zero-phonon transition rate at best. The fraction of the PL emission associated to this resonant transition is thereby increased from 3% to 46%. Our results constitute a significant leap on the route towards the implementation of fast long-distance quantum networks, which are currently limited by the photon emission rate in their nodes. Furthermore, our versatile design is readily applicable to other solid-state quantum emitters like color centers in silicon carbide.
Nitrogen-vacancy (NV) color centers in diamond have emerged as promising quantum solid-state systems, with applications ranging from quantum information processing to magnetic sensing. One of the most useful properties of NVs is the ability to read their ground-state spin projection optically at room temperature. Using theoretical analysis of Purcell-enhanced NV optical coupling, we identify parameters for a significantly enhanced single-to-noise ratio (SNR) of the optical spin-state readout. We then demonstrate that a combined increase in spontaneous emission (through Purcell enhancement) and in optical excitation could significantly increase the readout SNR. Our combined analytical and numerical analysis, which is relevant for various optically active solid-state systems, differentiates between state-mixing processes and provides insights into the optimal light-matter coupling design.
A study of the photophysical properties of nitrogen-vacancy (NV) color centers in diamond nanocrystals of size 50 nm or below is carried out by means of second-order time-intensity photon correlation and cross-correlation measurements as a function of the excitation power for both pure charge states, neutral and negatively charged, as well as for the photochromic state, where the center switches between both states at any power. A dedicated three-level model implying a shelving level is developed to extract the relevant photophysical parameters coupling all three levels. Our analysis confirms the very existence of the shelving level for the neutral NV center. It is found that it plays a negligible role on the photophysics of this center, whereas it is responsible for an increasing photon bunching behavior of the negative NV center with increasing power. From the photophysical parameters, we infer a quantum efficiency for both centers, showing that it remains close to unity for the neutral center over the entire power range, whereas it drops with increasing power from near unity to approximately 0.5 for the negative center. The photophysics of the photochromic center reveals a rich phenomenology that is to a large extent dominated by that of the negative state, in agreement with the excess charge release of the negative center being much slower than the photon emission process.