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arXiv:2205.04780 · Optica

Resonant and phonon-assisted ultrafast coherent control of a single hBN color center

Johann A. Preuß, Daniel Groll, Robert Schmidt, Thilo Hahn, Paweł Machnikowski, Rudolf Bratschitsch, T. Kühn, Steffen Michaelis de Vasconcellos, Daniel Wigger

Published Mar 14, 2022• 28 citations
arXivHTMLPDF

Abstract

Single-photon emitters in solid-state systems are important building blocks for scalable quantum technologies. Recently, quantum light emitters have been discovered in the wide-gap van der Waals insulator hexagonal boron nitride (hBN). These color centers have attracted considerable attention due to their quantum performance at elevated temperatures and wide range of transition energies. Here, we demonstrate coherent state manipulation of a single hBN color center with ultrafast laser pulses and investigate in our joint experiment–theory study the coupling between the electronic system and phonons. We demonstrate that coherent control can be performed not only resonantly on the optical transition giving access to the decoherence but also phonon-assisted, which reveals the internal phonon quantum dynamics. In the case of optical phonons, we measure their decoherence, stemming in part from their anharmonic decay. Dephasing induced by the creation of acoustic phonons manifests as a rapid decrease in the coherent control signal when traveling phonon wave packets are emitted. Furthermore, we demonstrate that the quantum superposition between a phonon-assisted process and resonant excitation causes ultrafast oscillations of the coherent control signal. Our results pave the way for ultrafast phonon quantum state control on the nanoscale and open up a new promising perspective for hybrid quantum technologies.

DOI
10.1364/optica.448124

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Single-photon emitters in solid-state systems are important building blocks for scalable quantum technologies. Recently, quantum light emitters have been discovered in the wide-gap van der Waals insulator hexagonal boron nitride (hBN). These color centers have attracted considerable attention due to their quantum performance at elevated temperatures and wide range of transition energies. Here, we demonstrate coherent state manipulation of a single hBN color center with ultrafast laser pulses and investigate in our joint experiment–theory study the coupling between the electronic system and phonons. We demonstrate that coherent control can be performed not only resonantly on the optical transition giving access to the decoherence but also phonon-assisted, which reveals the internal phonon quantum dynamics. In the case of optical phonons, we measure their decoherence, stemming in part from their anharmonic decay. Dephasing induced by the creation of acoustic phonons manifests as a rapid decrease in the coherent control signal when traveling phonon wave packets are emitted. Furthermore, we demonstrate that the quantum superposition between a phonon-assisted process and resonant excitation causes ultrafast oscillations of the coherent control signal. Our results pave the way for ultrafast phonon quantum state control on the nanoscale and open up a new promising perspective for hybrid quantum technologies.
Single-photon sources are crucial components for building quantum networks and communications, but their optical coherent control remains a significant challenge in the development of quantum technologies. Recently, single-photon sources in atomically thin 2D materials such as transition metal dichalcogenides and van der Waals materials have emerged as promising solid-state quantum light emitters [1]. Hexagonal boron nitride (hBN) is a 2D insulator, which hosts optically active states in its band gap that efficiently emit single photons even at room temperature. The wide range of emission wavelengths, narrow emission lines, and convenient tunability of these hBN emitters make them particularly interesting for quantum sensing and wavelength division multiplexed quantum communications. They can also be found in commercially available nanocrystals, making them ideal for creating large arrays of single-photon emitters [2] and efficient coupling to photonic structures, such as 3D-printed microlenses [3].
Defects in solid-state systems constitute a promising platform for the realization of deterministic quantum emitters. Among many candidate materials and emitters, point defects in hexagonal Boron Nitride (hBN) have recently emerged as particularly promising. In this work, we probe the coherence of an individual B center with a zero phonon line at 436 nm, under pulsed resonant excitation. We observe power-dependent Rabi oscillations up to 5π, demonstrating optical coherent control of the transition. We achieve an excellent single photon purity of 93% at π-pulse. Furthermore, we probe the coherence of the two-level system using Ramsey interferometry, revealing an inhomogeneous coherence time of T_2*=0.60 ns. These results establish B centers in hBN as viable candidates for triggered, coherent quantum emitters and represent an important step towards their integration into quantum photonic platforms.
Hyperbolic phonon polaritons (HPPs) in hexagonal boron nitride (hBN) confine mid-infrared light to deep-subwavelength scales and may offer a powerful route to strong light-matter interactions. Generation and control of HPPs are typically accessed using classical near-field probes, which limits experiments at the quantum level.A complementary frontier in hBN research focuses on color centers: bright, stable, atomically localized emitters that have rapidly emerged as a promising platform for solid-state quantum optics. Here we establish a key connection between these two directions by developing a cavity-QED framework in which a single hBN color center serves as a quantum source of HPPs. We quantify the emitter-HPP interaction and analyze two generation schemes. The first is spontaneous emission into the phonon sideband, which can produce single-HPP events and, in ultrathin slabs, becomes single-mode with an enhanced decay rate. The second is a stimulated Raman process that provides frequency selectivity, tunable conversion rate, and narrowband excitation. This drive launches spatially confined, ray-like HPPs that propagate over micrometer distances. We also outline a two-emitter correlation measurement that can directly test the single-polariton character of these emissions. By connecting color-center quantum optics with hyperbolic polaritonics, our approach enables quantum emitters to act as on-chip quantum sources and controls for HPPs, while HPPs provide long-range channels that couple spatially separated emitters. Together, these capabilities point to a new direction for mid-infrared photonic experiments that unite strong coupling, spectral selectivity, and spatial reach within a single material system.
Color centers hosted in hexagonal boron nitride have emerged as a highly promising platform for single-photon emission and spin-photon technologies relevant to quantum communication and quantum networking. As a wide-bandgap van der Waals material, hBN can host optically active quantum defects across a broad spectral range. Here, we demonstrate a simple and scalable oxygen-plasma process that reproducibly creates single quantum emitters in hBN with blinking-free zero-phonon lines spanning the near-infrared from 700 up to 971 nm. These emitters combine MHz-level brightness, single-photon purity up to 99.9\%, and ultranarrow cryogenic linewidths down to 2.7~GHz under quasi-resonant excitation, placing them in a particularly attractive regime for quantum photonics. Photostability measurements further reveal resistance to photobleaching, sub-nm spectral stability over long timescales, and near-shot-noise-limited intensity fluctuations. Analysis of the phonon sidebands shows weak vibronic coupling and ZPL-dominated emission, with Debye--Waller factors approaching 50\%. Control experiments together with EDS elemental mapping support oxygen incorporation as a necessary ingredient in activating the NIR emitter population, while first-principles calculations identify ON_NN​VN_NN​ and ON_NN​VN_NN​H as the leading defect candidates. These results establish a high-performance NIR quantum-emitter platform in hBN for free-space quantum networking and future integrated quantum-photonic architectures.
The potential of solid-state quantum emitters for applications critically depends on several key figures of merit. One of the most important is the quantum coherence of the emitted single photons, which can be compromised by fast dephasing and spectral diffusion. In hexagonal boron nitride (hBN), blue-emitting color centers (or B centers) are seen as favorable in this regard, in the light of prior studies mainly based on resonant excitation. Yet, their coherence properties in the more accessible regime of non-resonant excitation (or photoluminescence) has not been extensively characterized. Here, we investigate the coherence and spectral diffusion of the photoluminescence from a B center in the continuous wave regime using photon correlation Fourier spectroscopy. We determine that the emission lineshape consists in a homogeneous contribution, whose linewidth increases with the laser power, and which is broadened by spectral diffusion at a timescale of 10 to 100 microseconds. At low power and short time, the emission line is only a factor ~2 above the Fourier limit, while at long times, the inhomogeneous linewidth increases up to more than a gigahertz. Our work deepens the understanding of decoherence processes of this preeminent family of quantum emitters in hBN.
Quantum emitters in hexagonal boron nitride (hBN) are promising building blocks for solid-state quantum photonics because of their bright room-temperature emission. These emitters strongly interact with lattice vibrations, which partially underpins their excitation efficiency. Here, using complementary cathodoluminescence (CL) and photoluminescence (PL) spectroscopy, we demonstrate cavity-mediated interactions between hBN quantum emitters coupled to the same plasmonic Au void cavity at the room temperature. Cathodoluminescence measurements reveal that a vibronic transition of the 443 nm emitter hybridizes with the cavity mode, giving rise to a spectrally resolved splitting, while the neighboring 537 nm emitter remains in the weak-coupling regime despite spectral overlap. The energy split of the CL peak is at the order of 36.2 meV, whereas the PL-resolved peak is approximately 24.1 meV, which is due to the collective excitations of multiple emitters per electron excitation and their mutual interactions. Maxwell-Bloch simulations reproduce the experimental spectra and identify the observed splitting as the result of cavity-induced hybridization. Excitation-dependent PL further shows that the hybridized state can be accessed through phonon-assisted excitations below the zero-phonon transition. These results demonstrate that vibronic transitions provide an effective pathway for controlling interactions between multiple quantum emitters in hybrid plasmonic nanophotonic systems.