Photodynamics of quantum emitters in hexagonal boron nitride revealed by low-temperature spectroscopy

Sontheimer, Bernd; Braun, Merle; Nikolay, Niko; Sadzak, Nikola; Aharonovich, Igor; Benson, Oliver

doi:10.1103/physrevb.96.121202

Cited by 77 publications

(118 citation statements)

References 42 publications

(64 reference statements)

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“…Single photon sources in this 2D, van der Waals material have emerged as promising candidates for quantum applications, thanks to their robustness, and their highly polarized and ultra-bright emission at room-temperature. [26][27][28][29][30][31][32][33] As they often suffer from spectral diffusion, 16,[34][35][36] they are an excellent test case for understanding the fundamental mechanism, as well as demonstrating the effectiveness of the approach we hereby propose.…”

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confidence: 99%

Suppression of spectral diffusion by anti-Stokes excitation of quantum emitters in hexagonal boron nitride

Tran

Bradac

Solntsev

et al. 2019

Applied Physics Letters

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Solid-state quantum emitters are garnering a lot of attention due to their role in scalable quantum photonics. A notable majority of these emitters, however, exhibit spectral diffusion due to local, fluctuating electromagnetic fields. In this work, we demonstrate efficient Anti-Stokes (AS) excitation of quantum emitters in hexagonal boron nitride (hBN), and show that the process results in the suppression of a specific mechanism responsible for spectral diffusion of the emitters. We also demonstrate an all-optical gating scheme that exploits Stokes and Anti-Stokes excitation to manipulate spectral diffusion so as to switch and lock the emission energy of the photon source. In this scheme, reversible spectral jumps are deliberately enabled by pumping the emitter with high energy (Stokes) excitation; AS excitation is then used to lock the system into a fixed state characterized by a fixed emission energy. Our results provide important insights into the photophysical properties of quantum emitters in hBN, and introduce a new strategy for controlling the emission wavelength of quantum emitters.

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Section: Textmentioning

confidence: 99%

Suppression of spectral diffusion by anti-Stokes excitation of quantum emitters in hexagonal boron nitride

Tran

Bradac

Solntsev

et al. 2019

Applied Physics Letters

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“…Defects in hexagonal boron nitride (hBN) exhibit promising quantum-optical properties including narrow linewidth, 9 high brightness, 8 high photostability, 11,12 and high emission into the zero phonon line (ZPL). 13 However, both intrinsic and engineered defects in mono-and multi-layer films exhibit large spectral variability.…”

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Revealing multiple classes of stable quantum emitters in hexagonal boron nitride with correlated optical and electron microscopy

et al. 2020

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Single photon emitters (SPEs) in solids have emerged as promising candidates for quantum photonic sensing, 1-3 communications, 4, 5 and computing. 6, 7 Defects in hexagonal boron nitride (hBN) exhibit high-brightness, room-temperature quantum emission, 8-10 but their large spectral variability and unknown local structure significantly challenge their technological utility. Here, we directly correlate hBN quantum emission with the material's local strain using a combination of photoluminescence (PL), cathodoluminescence (CL) and nanobeam electron diffraction. Across 40 emitters and 15 samples, we observe zero phonon lines (ZPLs) in PL and CL ranging from 540-720 nm. CL mapping reveals that multiple defects and distinct defect species located within an optically-diffraction-limited region can each contribute to the observed PL spectra. Local strain maps indicate that strain is not required to activate the emitters and is not solely responsible for the observed ZPL spectral range. Instead, four distinct defect classes are responsible for the observed emission range. One defect class has ZPLs near 615 nm with predominantly matched CL-PL responses; it is not a straintuned version of another defect class with ZPL emission centered at 580 nm. A third defect class at 650 nm has low visible-frequency CL emission; and a fourth defect species centered at 705 nm has a small, ∼10 nm shift between its CL and PL peaks. All studied defects are stable upon both electron and optical irradiation. Our results provide an important foundation for atomic-scale optical characterization of color centers, as well as a foundation for engineering defects with precise emission properties. 1 arXiv:1901.05952v2 [cond-mat.mtrl-sci]

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“…Room temperature SPE from a zero-dimensional boron nitride allotrope (the boron nitride nano-cocoon) has also been demonstrated with ZPL energy centred around 2.14 eV 110 .The lineshape of the ZPL is usually Lorentzian in basic shape, but this can undergo significant distortions and variation, especially for Group 1 SPEs. Complex lineshapes can be indicative of: more than one process controlling the excited-state lifetime, inhomogeneous broadening associated with ultra-fast spectral diffusion present in these emitters113 , hot-band anti-Stokes 1-0 transitions enabled by thermal phonon population in the initial state before emission61 , or interference from other emitters at slightly different frequencies. Whereas anti-Stokes transitions usually just broaden the low wavelength side of the ZPL in accordance with the appropriate Boltzmann factor, emission at energies of 160 meV higher than excitation can also be observed by this process, with the expected extremely low quantum yield61 .Such effects may become important technologically as quantum emitters in h-BN havebeen shown to be stable and operate at elevated temperatures55 .…”

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Single-photon emitters in hexagonal boron nitride: a review of progress

2020

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This report summarizes progress made in understanding properties such as zerophonon-line energies, emission and absorption polarizations, electron-phonon couplings, strain tuning and hyperfine coupling of single photon emitters in hexagonal boron nitride. The primary aims of this research are to discover the chemical nature of the emitting centres and to facilitate deployment in device applications. Critical analyses of the experimental literature and data interpretation, as well as theoretical approaches used to predict properties, are made. In particular, computational and theoretical limitations and challenges are discussed, with a range of suggestions made to overcome these limitations, striving to achieve realistic predictions concerning the nature of emitting centers. A symbiotic relationship is required in which calculations focus on properties that can easily be measured, whilst experiments deliver results in a form facilitating mass-produced calculations.

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Photodynamics of quantum emitters in hexagonal boron nitride revealed by low-temperature spectroscopy

Cited by 77 publications

References 42 publications

Suppression of spectral diffusion by anti-Stokes excitation of quantum emitters in hexagonal boron nitride

Suppression of spectral diffusion by anti-Stokes excitation of quantum emitters in hexagonal boron nitride

Revealing multiple classes of stable quantum emitters in hexagonal boron nitride with correlated optical and electron microscopy

Single-photon emitters in hexagonal boron nitride: a review of progress

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