Efficient Optical Quantification of Heterogeneous Emitter Ensembles

Breitweiser, S. Alex; Exarhos, Annemarie L.; Patel, Raj N.; Saouaf, Jennifer; Porat, Benjamin; Hopper, David A.; Bassett, Lee C.

doi:10.1021/acsphotonics.9b01707

Cited by 16 publications

(28 citation statements)

References 46 publications

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“…properties: a strong response to applied strain and electric fields (Stark shifts), 9,10,11 stability under high pressure and elevated temperatures, 12,13 potential for resonant excitation above 70 cryogenic temperatures, 14,15,16 and addressability via spin-selective optical transitions. 17,18 Yet, despite the numerous experimental characterizations and in-depth theoretical attempts to model their possible crystalline structure, 6,19,20,21,22,23,24,25 the nature of these defects remains 73 unknown. 74…”

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confidence: 99%

Identifying carbon as the source of visible single-photon emission from hexagonal boron nitride

et al. 2020

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Single photon emitters (SPEs) in hexagonal boron nitride (hBN) have garnered significant attention over the last few years due to their superior optical properties. However, despite the vast range of experimental results and theoretical calculations, the defect structure responsible for the observed emission has remained elusive. Here, by controlling the incorporation of impurities into hBN via various bottom-up synthesis methods and directly through ion implantation we provide direct evidence that the visible SPEs are carbon related. Room temperature optically detected magnetic resonance (ODMR) is demonstrated on ensembles of these defects. We perform ion implantation experiments and confirm that only carbon implantation creates SPEs in the visible spectral range. Computational analysis of the simplest 12 carbon-containing defect species suggest the negatively charged V B C N − defect as a viable 53 candidate and predict that out-of-plane deformations make the defect environmentally sensitive. 54Our results resolve a long-standing debate about the origin of single emitters at the visible range 55 grown epitaxially. 28, 29 The energy detuning between the ZPL of the ensemble and phonon sideband (PSB) peak is ~176 meV on average (Extended Data Fig. 1). 30, 31 X-ray photoelectron spectroscopy (XPS) was used to quantify the incorporation of carbon (Extended Data Fig. 2). Figure 1b(c) demonstrate a near linear correlation between C-B (C-N) bonding and increasing TEB flux, with C-B bonding being roughly an order of magnitude more prevalent than C-N bonding. Preferential formation of C-B bonds follows logically from noting the B species are introduced with three pre-existing bonds to C. PL intensity of the resulting ensemble emission likewise displays a linear correlation with carbon concentration (Extended Data Fig. 3). Based on these results, we advance that the SPE emission at ~580 nm in hBN is likely to originate from a carbon-related defect complex. Figure 1-Photoluminescence from MOVPE hBN Samples. a. MOVPE hBN grown with increasing flow rates of triethyl borane (TEB). As TEB flow increases, the fluorescence of SPE ensembles increases. b. Percentage of B-C bonding with increasing TEB flow evaluated by XPS. c. Percentage of N-C bonding with increasing TEB flow evaluated by XPS. d. Room temperature ODMR displayed as relative contrast, spin-dependent variation in photoluminescence (∆PL/PL), observed from the ~585 nm ensemble emission of MOPVE hBN (TEB 60) at applied fields of 19, 24, and 29 mT respectively. e.

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confidence: 99%

Identifying carbon as the source of visible single-photon emission from hexagonal boron nitride

et al. 2020

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“…Fluorescence measurements from traditional ensemble emitters were limited due to heterogeneity of emitters and individual defect-by defect studies are impractical. New techniques were proposed to quickly and accurately characterize the emission from ensemble emitters as experimented in ref 107 .…”

Section: Photophysics Of Hbn Quantum Emittersmentioning

confidence: 99%

Optical quantum technologies with hexagonal boron nitride single photon sources

Shaik

2021

Sci Rep

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Single photon quantum emitters are important building blocks of optical quantum technologies. Hexagonal boron nitride (hBN), an atomically thin wide band gap two dimensional material, hosts robust, optically active luminescent point defects, which are known to reduce phonon lifetimes, promises as a stable single-photon source at room temperature. In this Review, we present the recent advances in hBN quantum light emission, comparisons with other 2D material based quantum sources and analyze the performance of hBN quantum emitters. We also discuss state-of-the-art stable single photon emitter’s fabrication in UV, visible and near IR regions, their activation, characterization techniques, photostability towards a wide range of operating temperatures and harsh environments, Density-functional theory predictions of possible hBN defect structures for single photon emission in UV to IR regions and applications of single photon sources in quantum communication and quantum photonic circuits with associated potential obstacles.

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“…The samples were then annealed in a tube furnace at 850 °C in low flow Ar atmosphere for 2 hours. Annealing h-BN has been found to brighten the emitters [35]. While not the focus of study here, annealing for longer time (2 hours vs commonly used 30 minutes) appears to improve emitter stability.…”

Section: A Sample Preparationmentioning

confidence: 84%

“…Prior to the optical studies, the samples were annealed in a tube furnace at 850 °C in Ar atmosphere for 2 hours. This annealing process has been shown to brighten the emitters [35]. The QEs are illuminated with either of two continuous-wave lasers operating at 532 nm and 592 nm wavelengths, where excitation power and polarization are controlled.…”

Section: A Photoluminescence Characterizationmentioning

confidence: 99%

“…Ultraviolet emission around 4.1 eV has been attributed to the carbon dimer C B C N [20], whereas near-infrared emission around 1.7 eV and an associated optically detected magnetic resonance signal is attributed to the negatively-charged boron vacancy, V − B [12]. For QEs in the visible spectrum, experiments utilizing various forms of electron and optical microscopy, spectroscopy, and materials growth and treatments have generated a detailed, yet complicated, empirical understanding of the QEs' creation, stabilization, and principal optical signatures [3,[21][22][23][24][25][26][27][28][29][30][31][32][33][34][35][36][37][38][39]. Theoretical work suggests that vacancies and their complexes, along with substitutional carbon atoms and dangling bonds, are likely candidates, although consensus is still lacking [40][41][42][43][44][45].…”

Section: Introductionmentioning

confidence: 99%

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Probing the Optical Dynamics of Quantum Emitters in Hexagonal Boron Nitride

Patel¹,

Hopper²,

Gusdorff³

et al. 2022

Preprint

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Hexagonal boron nitride is a van der Waals material that hosts visible-wavelength quantum emitters at room temperature. However, experimental identification of the quantum emitters' electronic structure is lacking, and key details of their charge and spin properties remain unknown. Here, we probe the optical dynamics of quantum emitters in hexagonal boron nitride using photon emission correlation spectroscopy. Several quantum emitters exhibit ideal single-photon emission with noise-limited photon antibunching, g (2) (0) = 0. The photoluminescence emission lineshapes are consistent with individual vibronic transitions. However, polarization-resolved excitation and emission suggests the role of multiple optical transitions, and photon emission correlation spectroscopy reveals complicated optical dynamics associated with excitation and relaxation through multiple electronic excited states. We compare the experimental results to quantitative optical dynamics simulations, develop electronic structure models that are consistent with the observations, and discuss the results in the context of ab initio theoretical calculations.

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Efficient Optical Quantification of Heterogeneous Emitter Ensembles

Cited by 16 publications

References 46 publications

Identifying carbon as the source of visible single-photon emission from hexagonal boron nitride

Identifying carbon as the source of visible single-photon emission from hexagonal boron nitride

Optical quantum technologies with hexagonal boron nitride single photon sources

Probing the Optical Dynamics of Quantum Emitters in Hexagonal Boron Nitride

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