Efficient single photon emission from a high-purity hexagonal boron nitride crystal

Martínez, Luis; Pelini, Thomas; Waselowski, Victor; Maze, J. R.; Gil, Bernard; Cassabois, Guillaume; Jacques, Vincent

doi:10.1103/physrevb.94.121405

Cited by 186 publications

(245 citation statements)

References 52 publications

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“…2) exhibit striking differences both in shape and spectral weight, with features extending between 550-700 nm (1.77-2.25 eV). Some spectra, such as for SE1 and SE2, include a clear zero-phonon line (ZPL) and phonon sideband (PSB) and are similar in shape to those reported from experiments with supported h-BN samples [19][20][21][22][23]. Other spectra, such as for SE3 and SE4, display spectral features distinct from what has been thus far reported.…”

supporting

confidence: 68%

“…Carbon impurities have also been implicated in ultraviolet photoluminescence [16] and cathodoluminescence [17] from h-BN, even at the single-defect level [18]. Recently, single-photon sources at visible wavelengths have been reported from supported monolayer, multilayer, and bulk h-BN [19][20][21][22][23], but existing observations and interpretations vary widely in terms of basic emitter properties (e.g., optical lifetime, spectral line shape, brightness) and proposed physical models. By focusing on regions of suspended h-BN, we eliminate substrate interactions that are observed to play an important role in the material's visible emission characteristics.…”

mentioning

confidence: 99%

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Optical Signatures of Quantum Emitters in Suspended Hexagonal Boron Nitride

Exarhos¹,

Hopper²,

Grote³

et al. 2017

ACS Nano

190

267

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Hexagonal boron nitride (h-BN) is a tantalizing material for solid-state quantum engineering. Analogously to three-dimensional wide-bandgap semiconductors like diamond, h-BN hosts isolated defects exhibiting visible fluorescence, and the ability to position such quantum emitters within a two-dimensional material promises breakthrough advances in quantum sensing, photonics, and other quantum technologies. Critical to such applications, however, is an understanding of the physics underlying h-BN's quantum emission. We report the creation and characterization of visible single-photon sources in suspended, single-crystal, h-BN films. The emitters are bright and stable over timescales of several months in ambient conditions. With substrate interactions eliminated, we study the spectral, temporal, and spatial characteristics of the defects' optical emission, which offer several clues about their electronic and chemical structure. Analysis of the defects' spectra reveals similarities in vibronic coupling despite widely-varying fluorescence wavelengths, and a statistical analysis of their polarized emission patterns indicates a correlation between the optical dipole orientations of some defects and the primitive crystallographic axes of the single-crystal h-BN film. These measurements constrain possible defect models, and, moreover, suggest that several classes of emitters can exist simultaneously in free-standing h-BN, whether they be different defects, different charge states of the same defect, or the result of strong local perturbations.Defect engineering in solid-state materials is a rapidly progressing field with applications in quantum information science [1, 2], nanophotonics [3], and nanoscale sensing in biology and chemistry [4]. Inspired by the success of the archetypal nitrogen-vacancy center in diamond [5], recent efforts have uncovered analogous systems in other wide-bandgap semiconductors such as silicon carbide [6, 7] which offer exciting new opportunities for defect engineering in three-dimensional materials. However, optically active impurities in low-dimensional materials and thin films can provide unique functionalities due to intrinsic spatial confinement and the ability to create multi-functional layered materials [8, 9]. Within the class of van der Waals materials, hexagonal boron nitride (h-BN) is an ideal candidate for exploring new defect physics due to its large (∼6 eV) bandgap [10] and its unique optical [11], electrical [12, 13], and vibronic properties [14] that may influence the underlying physics of its defects. At present, however, progress is impeded by an incomplete understanding of the electronic and chemical structure of defects responsible for h-BN's visible fluorescence.

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supporting

confidence: 68%

mentioning

confidence: 99%

Optical Signatures of Quantum Emitters in Suspended Hexagonal Boron Nitride

Exarhos¹,

Hopper²,

Grote³

et al. 2017

ACS Nano

190

267

View full text Add to dashboard Cite

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“…In h-BN, a narrow emission band has been observed with a zero phonon line (ZPL) transition at 1.95 eV [7,48,49] but the origin of this emission is unclear. Based on a broad examination of possible defect sites in h-BN using DFT with the PBE functional, we have reasoned that V N C B forms a likely candidate as its origin [33].…”

Section: Possible Photoluminescence Arising From Vncbmentioning

confidence: 99%

Defect states in hexagonal boron nitride: Assignments of observed properties and prediction of properties relevant to quantum computation

2018

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“…Some color centers, such as the nitrogen vacancy (NV) center in diamond [6][7][8][9][10][11], are bright enough to be investigated in the single defect limit using single-molecule microscopy techniques [12,13]. While diamond is the most celebrated host material, the last several years have witnessed the discovery of defect-based single photon sources in SiC [1,[14][15][16][17][18][19][20], ZnO [21][22][23][24][25][26], GaN [27], WSe2 [28][29][30], WS2 [31], and hexagonal boron nitride (h-BN) [32][33][34][35][36][37][38][39][40][41][42][43][44][45]. The latter three materials exist as two-dimensional monolayers and layered solids, thus offering the possibility of integrating single-photon sources with van der Waals heterostructure devices for tuning and other control.…”

mentioning

confidence: 99%

Optical Absorption and Emission Mechanisms of Single Defects in Hexagonal Boron Nitride

2017

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Abstract:We investigate the polarization selection rules of sharp zero-phonon lines (ZPLs) from isolated defects in hexagonal boron nitride (h-BN) and compare our findings with the predictions of a configuration coordinate model involving two electronic states. Our survey, which spans the spectral range ~550-740 nm, reveals that, in disagreement with a two-level model, the absorption and emission dipoles are often misaligned. We relate the dipole misalignment angle ( ) to the ZPL Stokes shift ( ) and find that ≈ 0° when corresponds to an allowed h-BN phonon frequency and that 0°≤ ≤ 90° when exceeds the maximum allowed h-BN phonon frequency. Consequently, a two-level configuration coordinate model succeeds at describing excitations mediated by the creation of one optical phonon but fails at describing excitations that require the creation of multiple phonons. We propose that direct excitations requiring the creation of multiple phonons are inefficient due to the low Huang-Rhys factors in In the Frank-Condon approximation, where the fast electronic rearrangement precedes the slower lattice relaxation, the transition rate from to ( * ,is proportional to where * − * are the associated Laguerre polynomials and is a measure of defect-lattice coupling called the Huang-Rhys factor. In natural units = To investigate the polarization properties of absorption, we rotate the polarization of the exciting light and monitor the total fluorescence intensity. The result of this absorption measurement is shown as the green triangles in Fig. 2b. Fixing the polarization of the exciting light to maximize the fluorescence, we determine the polarization of the emitted photons using a polarization analyzer placed in the collection path of the microscope. The result of this emission measurement is shown as the red circles in Fig. 2b. The solid lines are best fits to the data using the equationwhere 〈 〉 in each fit is the orientation of the absorption or emission dipole spectrally averaged over the collection window. As predicted by Equation 1, we find that the maxima of absorption and emission are aligned for this defect.Additionally, we have shown previously that the temperature dependence of the ZPL intensity in h-BN is well-modeled by the temperature-dependent DebyeWaller factor [33]. Thus, we conclude that the configuration coordinate model is a good description of the observed properties for the defect shown in Fig. 2.A survey of defect ZPLs that span an appreciable energy range reveals that, in contrast to the data shown in Fig. 2 For the emission measurement we fix the polarization angle of the exciting light to ( ) and record an emission spectrum for a series of positions of the polarization analyzer in the collection path. In an analogous fashion to the absorption case we obtain ( , ) and ( ) for the emitted light. For the case of emission we apply a calibration to ( ) to correct for wavelength-and polarization-dependent retardances (see Supporting Information) introduced by the collection path of the confocal microscope. To be...

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Efficient single photon emission from a high-purity hexagonal boron nitride crystal

Cited by 186 publications

References 52 publications

Optical Signatures of Quantum Emitters in Suspended Hexagonal Boron Nitride

Optical Signatures of Quantum Emitters in Suspended Hexagonal Boron Nitride

Defect states in hexagonal boron nitride: Assignments of observed properties and prediction of properties relevant to quantum computation

Optical Absorption and Emission Mechanisms of Single Defects in Hexagonal Boron Nitride

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