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arXiv:2402.18542 · Physical review. B./Physical review. B

Photon statistics of resonantly driven spectrally diffusive quantum emitters

Aymeric Delteil, Stéphanie Buil, Jean‐Pierre Hermier

Published Apr 26, 2024• 7 citations
arXivHTMLPDF

Abstract

Solid-state quantum emitters often suffer from temporal variations of their transition energies, inherited from fluctuations in the host crystal environment. This spectral diffusion (SD) is detrimental to the emitter linewidth but is often challenging to characterize experimentally. The authors show here that, under resonant laser excitation, the statistics of the scattered photons offer multiple signatures of the SD process, making it possible to discriminate between discrete jumps and continuous diffusion, as well as to access relevant parameters of the SD mechanisms.

DOI
10.1103/physrevb.109.155308

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Solid-state quantum emitters often suffer from temporal variations of their transition energies, inherited from fluctuations in the host crystal environment. This spectral diffusion (SD) is detrimental to the emitter linewidth but is often challenging to characterize experimentally. The authors show here that, under resonant laser excitation, the statistics of the scattered photons offer multiple signatures of the SD process, making it possible to discriminate between discrete jumps and continuous diffusion, as well as to access relevant parameters of the SD mechanisms.
Single-photon emitters in the solid state are subject to spectral broadening processes known as spectral diffusion and pure dephasing. Here, the authors show that a combination of quantum optics techniques, namely coherent laser drive and time-resolved photon correlations, can bring both processes to light in a single experimental protocol. This allows an extensive characterization of a large variety of solid-state quantum emitters. Their method is experimentally applied to a quantum emitter in the 2D material hexagonal boron nitride, further establishing this system as an appealing quantum photonics platform.
Solid-state quantum emitters are playing a crucial role in the development of photonic quantum technologies. However, several decoherence mechanisms are known to impact the device performances and scalability. In various quantum emitter materials the fluctuation of the two-level system has been investigated by different methods to capture the evolution of coherence reduction. However, resolving the dynamics of spectral diffusion in the fundamental framework of on-demand single-photon generation remained unsolved. Hereby, the challenge is to observe with high time and energy resolution the impact of fluctuations directly in the properties of the emitted photons. In this Rapid Communication, we demonstrate the use of dispersion in a slow-light medium to map the photons frequency domain into time domain, observed as frequency-dependent time-of-flight. This allows for the measurement of the emission spectrum and the quantification of the spectral diffusion dynamics in one intensity correlation measurement. On exemplary semiconductor quantum dots, the impact of charge and spin noise on the spectral diffusion are revealed to follow an Ornstein-Uhlenbeck process. By a single measurement, broadening from the excitation repetition up to the stationary limit is resolved. This enables one to extract time-dependent two-photon interference visibilities for various timescales, which is a key performance measure for quantum emitters.
The excited state population of single solid-state emitters is subjected to energy fluctuations around the equilibrium driven by the bath and relaxation through the emission of phonons or photons. Simultaneous measurement of the associated spectral dynamics requires a technique with a high spectral and temporal resolution with an additionally high temporal dynamic range. We propose a pulsed excitation-laser analog of photon-correlation Fourier spectroscopy (PCFS), which extracts the linewidth and spectral diffusion dynamics along the emission lifetime trajectory of the emitter, effectively discriminating spectral dynamics from relaxation and bath fluctuations. This lifetime-resolved PCFS correlates photon-pairs at the output arm of a Michelson interferometer in both their time-delay between laser-excitation and photon-detection T and the time-delay between two photons τ. We propose the utility of the technique for systems with changing relative contributions to the emission from multiple states, for example, quantum emitters exhibiting phonon-mediated exchange between different fine-structure states.
We experimentally investigate a solid-state quantum emitter---a B center in hexagonal boron nitride (hBN)---that has lifetime-limited coherence at short times, and experiences inhomogeneous broadening due to spectral diffusion at longer times. By making use of power broadening in resonant laser excitation, we explore the crossover between the inhomogeneous and the homogeneous broadening regimes. With the support of numerical simulations, we show that the line shape, count rate, second-order correlations, and long-time photon statistics evolve from a regime where they are dictated by spectral diffusion to a regime where they are simply given by the homogeneous response of the emitter, yielding restored Lorentzian shape and Poissonian photon statistics. Saturation of the count rate and line broadening occur not at the onset of the Rabi oscillations, but when the power-broadened homogeneous response becomes comparable with the inhomogeneous linewidth. Moreover, we identify specific signatures in both the second-order correlations and long-time photon statistics that are well explained by a microscopic spectral diffusion model based on discrete jumps at timescales of micro- to milliseconds. Our work provides an extensive description of the photophysics of B centers under resonant excitation, and can be readily extended to a wide variety of solid-state quantum emitters.
The optical spectrum of a quantum system is jointly determined by the properties of the emitter and the driving field. All-optical spectral control can hence be a promising method to engineer the properties of single photon emitters for quantum technological applications. It was proposed that driving a two-level system with a periodic sequence of optical pi-pulses during the excited state lifetime shifts the emission and absorption maximum to an arbitrarily detuned pulse carrier frequency, enabling the mitigation of spectral diffusion in noisy emitters. In this article, we report on the first experimental observation of this effect. We implement the protocol on a solid-state emitter and reduce its inhomogeneously broadened optical linewidth close to the lifetime limit. By detuning the excitation laser, we are able to concentrate approximately half of the absorption to a freely selectable target frequency. Our approach is solely based on properties of coherently evolving quantum systems, rendering it applicable to a wide range of individual and ensembles of quantum emitters.
Spectral diffusion is the phenomenon of random jumps in the emission wavelength of narrow lines. This phenomenon is a major hurdle for applications of solid state quantum emitters like quantum dots, molecules, or diamond defect centers in an integrated quantum optical technology. Here, we provide further insight into the underlying processes of spectral diffusion of the zero-phonon line of single nitrogen vacancy centers in nano-size diamond by using a novel method based on photon correlation interferometry. The method works although the spectral diffusion rate is several orders of magnitude higher than the photon detection rate and thereby improves the time resolution of previous experiments with nano-size diamond by 6 orders of magnitude. We study the dependency of the spectral diffusion rate on the excitation power, temperature, and excitation wavelength under off-resonant excitation. Our results bring insight into the mechanism of spectral diffusion and suggest a strategy to increase the number of spectrally indistinguishable photons emitted by diamond nanocrystals.