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Probing the limits for coherent optical control of a mechanically decoupled defect center in hexagonal boron nitride

M. Koch, Vibhav Bharadwaj, Alexander Kubanek

Published Nov 3, 2024• 5 citations
Publisher

Abstract

Abstract The coherent control of a two-level system is among the most essential challenges in modern quantum optics. Understanding its fundamental limitations is crucial, also for the realization of next generation quantum devices. The quantum coherence of a two-level system is fragile in particular, when the two levels are connected via an optical transition, which, at the same time, enables the manipulation of the system. When such quantum emitters are located in solids the coherence suffers from the interaction of the optical transition with the solid state environment, which requires the sample to be cooled to temperatures of a few Kelvin or below. Here, we use a mechanically isolated quantum emitter in hexagonal boron nitride to explore the individual mechanisms which affect the coherence of an optical transition under resonant drive. We operate the system at the threshold where the mechanical isolation collapses in order to study the onset and temperature-dependence of dephasing and independently of spectral diffusion. The insights on the underlying physical decoherence mechanisms reveal a limit in temperature until which coherent driving of the system is possible. This study enables to increase the operation temperature of hBN-based quantum devices, therefore reducing the need for cryogenic cooling.

DOI
10.1038/s43246-024-00686-y

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Abstract The coherent control of a two-level system is among the most essential challenges in modern quantum optics. Understanding its fundamental limitations is crucial, also for the realization of next generation quantum devices. The quantum coherence of a two-level system is fragile in particular, when the two levels are connected via an optical transition, which, at the same time, enables the manipulation of the system. When such quantum emitters are located in solids the coherence suffers from the interaction of the optical transition with the solid state environment, which requires the sample to be cooled to temperatures of a few Kelvin or below. Here, we use a mechanically isolated quantum emitter in hexagonal boron nitride to explore the individual mechanisms which affect the coherence of an optical transition under resonant drive. We operate the system at the threshold where the mechanical isolation collapses in order to study the onset and temperature-dependence of dephasing and independently of spectral diffusion. The insights on the underlying physical decoherence mechanisms reveal a limit in temperature until which coherent driving of the system is possible. This study enables to increase the operation temperature of hBN-based quantum devices, therefore reducing the need for cryogenic cooling.
The coherent control of a two-level system is among the most essential challenges in modern quantum optics. Understanding its fundamental limitations is crucial, also for the realization of next generation quantum devices. The quantum coherence of a two level system is fragile in particular, when the two levels are connected via an optical transition. When such quantum emitters are located in solids the coherence suffers from the interaction of the optical transition with the solid state environment, which requires the sample to be cooled to temperatures of a few Kelvin or below. Here, we use a mechanically isolated quantum emitter in hexagonal boron nitride to explore the individual mechanisms which affect the coherence of an optical transition under resonant drive. We operate the system at the threshold where the mechanical isolation collapses in order to study the onset and temperature-dependence of dephasing and independently of spectral diffusion. The new insights on the underlying physical decoherence mechanisms reveals a limit in temperature until which coherent driving of the system is possible. This study enables to increase the operation temperature of quantum devices, therefore reducing the need for cryogenic cooling.
Hexagonal boron nitride (hBN) has emerged as a promising two-dimensional host for stable single-photon emission owing to its wide bandgap, high photostability, and compatibility with nanophotonic integration. We present a simulation-based study of temperature-dependent spectral dynamics and optical coherence in a mechanically decoupled quantum emitter in hBN. Employing a hybrid stochastic framework that combines Ornstein--Uhlenbeck detuning fluctuations with temperature-dependent, Gaussian-distributed discrete frequency jumps, motivated by experimentally observed spectral diffusion and blinking, we reproduce the measured evolution of inhomogeneous linewidth broadening and the progressive degradation of photon coherence across the relevant cryogenic range (5-30K). The model captures phonon-related spectral diffusion with a cubic temperature dependence and the onset of jump-like spectral instabilities at higher temperatures. By calibrating the hybrid diffusion, jump parameters to the experimentally measured full width at half maximum (FWHM) of the emission line and analyzing the second-order correlation function g(2)(τ)g^{(2)}(τ)g(2)(τ) under resonant driving, we establish a unified phenomenological description that links stochastic detuning dynamics to the decay of optical coherence in a resonantly driven emitter. Analysis of g(2)(τ)g^{(2)}(τ)g(2)(τ) under resonant driving reveals an additional dephasing rate γsd+jγ_{\mathrm{sd+j}}γsd+j​ that rises monotonically with temperature and drive strength, leading to a predicted critical crossover to overdamped dynamics at Tcrit≈25.91T_{\mathrm{crit}} \approx 25.91Tcrit​≈25.91~K. This hybrid framework provides a quantitative connection between accessible spectroscopic observables and the dominant noise mechanisms limiting coherent optical control in mechanically decoupled quantum emitters, exemplified in hBN and generalizable to similar emitters in other materials.
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.
Mechanically isolated defect centers in hexagonal boron nitride are promising coherent quantum emitters, yet spectral instabilities persist, and their spin-related nature remains unclear. Here we investigate a single mechanically isolated quantum emitter in hBN integrated onto a coplanar waveguide. The emitter exhibits exceptionally bright resonant fluorescence with saturation count rates exceeding 10 Mc/s10\,\mathrm{Mc/s}10Mc/s. High-resolution spectroscopy reveals two closely spaced zero-phonon-line transitions originating from the same defect complex. Time-resolved spectroscopy shows that these transitions exhibit markedly different spectral diffusion dynamics, consistent with distinct donor-acceptor-pair-like recombination pathways with different sensitivities to local electrostatic fluctuations. Off-resonant blue illumination redistributes emission between the two transitions and increases the emission duty cycle without significantly modifying the dominant spectral diffusion rates at low temperature, indicating repumping from long-lived shelving states. Magnetic-field-dependent photoluminescence, optically detected magnetic resonance, and pump-probe measurements reveal millisecond-scale relaxation dynamics and magnetic-field-dependent fluorescence contrast, demonstrating spin-dependent population dynamics in the metastable shelving state. These results clarify how charge-driven spectral fluctuations and spin-dependent shelving jointly shape the optical cycling dynamics.
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.
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.