Phonon-assisted emission and absorption of individual color centers in hexagonal boron nitride (original) (raw)
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Theory of phonon-assisted luminescence in solids: Application to hexagonal boron nitride
Physical Review B, 2019
We study luminescence of hexagonal boron nitride (h-BN) by means of non-equilibrium Green's functions plus finite-difference electron-phonon coupling. We derive a formula for light emission in solids in the limit of a weak excitation that includes perturbatively the contribution of electronphonon coupling at the first order. This formula is applied to study luminescence in bulk h-BN. This material has attracted interest due to its strong luminescence in the ultraviolet region of the electromagnetic spectrum [Watanabe et al., Nature Mat. 3, 404(2004)]. The origin of this intense luminescence signal has been widely discussed, but only recently a clear signature of phonon mediated light emission started emerging from the experiments [Cassabois et al., Nature Phot. 10, 262(2016)]. By means of our new theoretical framework we provide a clear and full explanation of light emission in h-BN.
Nano Letters, 2016
We investigate the distribution and temperature-dependent optical properties of sharp, zero-phonon emission from defect-based single photon sources in multilayer hexagonal boron nitride (h-BN) flakes. We observe sharp emission lines from optically active defects distributed across an energy range that exceeds 500 meV. Spectrally-resolved photon-correlation measurements verify single photon emission, even when multiple emission lines are simultaneously excited within the same h-BN flake. We also present a detailed study of the temperature-dependent linewidth, spectral energy shift, and intensity for two different zero-phonon lines centered at 575 nm and 682 nm, which reveals a nearly identical temperature dependence despite a large difference in transition energy. Our temperature-dependent results are best described by a lattice vibration model that considers piezoelectric coupling to in-plane phonons. Finally, polarization spectroscopy measurements suggest that whereas the 575 !!! nm emission line is directly excited by 532 nm excitation, the 682 nm line is excited indirectly.
Exciton and Phonon Radiative Linewidths in Monolayer Boron Nitride
Physical Review X, 2022
The light-matter interaction in bulk semiconductors is in the strong-coupling regime with hybrid eigenstates, the so-called exciton polaritons and phonon polaritons. In two-dimensional (2D) systems, the translational invariance is broken in the direction perpendicular to the plane of the 2D system. The lightmatter interaction switches to the weak-coupling regime with a finite radiative lifetime of the matter excitations in 2D. Radiative phenomena have been extensively studied for 2D excitons in quantum wells and 2D crystals, but their counterpart has never been addressed for optical phonons in 2D. Here we present a parallel study of the exciton and phonon radiative linewidths in atomically thin layers of hexagonal boron nitride (h-BN), epitaxially grown on graphite. Reflectivity experiments are performed either in the deep ultraviolet for the excitonic resonance or in the midinfrared for the phononic one. A quantitative interpretation is implemented in the framework of a transfer matrix approach generalized to the case of monolayers with the inclusion of Breit-Wigner resonances of either excitonic or phononic nature. For the exciton we find a giant radiative broadening in comparison to other 2D crystals, with a value of ∼25 meV related to the strong excitonic effects in h-BN. For the phonon we provide the first estimation of the radiative linewidth of a 2D phonon, with a value of ∼0.2 meV in monolayer h-BN. Our results are found to be in good agreement with first-principles calculations. Our study unravels the existence of radiative states for optical phonons in 2D, with numerous perspectives for fundamental physics, optoelectronic applications in the midinfrared spectral range, and advanced thermal management, and h-BN is emerging as a model system in this novel topic.
Quantum Emission from Defects in Single-Crystalline Hexagonal Boron Nitride
Physical Review Applied, 2016
Bulk hexagonal boron nitride (hBN) is a highly nonlinear natural hyperbolic material that attracts major attention in modern nanophotonics applications. However, studies of its optical properties in the visible part of the spectrum and quantum emitters hosted by bulk hBN have not been reported to date. In this work we study the emission properties of hBN crystals in the red spectral range using sub-bandgap optical excitation. Quantum emission from defects is observed at room temperature and characterized in detail. Our results advance the use of hBN in quantum nanophotonics technologies and enhance our fundamental understanding of its optical properties.
Tunable Phonon Polaritons in Atomically Thin van der Waals Crystals of Boron Nitride
van der Waals heterostructures assembled from atomically thin crystalline layers of diverse two-dimensional solids are emerging as a new paradigm in the physics of materials. We used infrared anoimaging to study the properties of surface phonon polaritons in a representative van der Waals crystal, hexagonal boron nitride. We launched, detected, and imaged the polaritonic waves in real space and altered their wavelength by varying the number of crystal layers in our specimens. The measured dispersion of polaritonic waves was shown to be governed by the crystal thickness according to a scaling law that persists down to a few atomic layers. Our results are likely to hold true in other polar van der Waals crystals and may lead to new functionalities.
Excitons in van der Waals materials: From monolayer to bulk hexagonal boron nitride
Physical Review B, 2017
We present a general picture of the exciton properties of layered materials in terms of the excitations of their single-layer building blocks. To this end, we derive a model excitonic Hamiltonian by drawing an analogy with molecular crystals, which are other prototypical van der Waals materials. We employ this simplified model to analyze in detail the excitation spectrum of hexagonal boron nitride (hBN) that we have obtained from the ab initio solution of the many-body Bethe-Salpeter equation as a function of momentum. In this way, we identify the character of the lowest-energy excitons in hBN, discuss the effects of the interlayer hopping and the electron-hole exchange interaction on the exciton dispersion, and illustrate the relation between exciton and plasmon excitations in layered materials.
Quantum Emission from Defects in Single Crystal Hexagonal Boron Nitride
2016
Bulk hexagonal boron nitride (hBN) is a highly nonlinear natural hyperbolic material that attracts major attention in modern nanophotonics applications. However, studies of its optical properties in the visible part of the spectrum and quantum emitters hosted by bulk hBN have not been reported to date. In this work we study the emission properties of hBN crystals in the red spectral range using sub-bandgap optical excitation. Quantum emission from defects is observed at room temperature and characterized in detail. Our results advance the use of hBN in quantum nanophotonics technologies and enhance our fundamental understanding of its optical properties.
Hexagonal boron nitride (hBN) is a wide-band gap van der Waals material able to host light-emitting centers behaving as single photon sources. Here, we report the generation of color defects in hBN nanosheets dispersed on different kinds of substrates by thermal treatment processes. The optical properties of these defects have been studied using microspectroscopy techniques and far-field simulations of their light emission. Using these techniques, we have found that subsequent ozone treatments of the deposited hBN nanosheets improve the optical emission properties of created defects, as revealed by their zero-phonon linewidth narrowing and reduction of background emission. Microlocalized color defects deposited on dielectric substrates show bright (≈1 MHz) and stable room-temperature light emission with zero-phonon line peak energy varying from 1.56 to 2.27 eV, being the most probable value 2.16 eV. In addition to this, we have observed a substrate dependence of the optical performance of the generated color defects. The energy range of the emitters prepared on gold substrates is strongly reduced, as compared to that observed in dielectric substrates or even alumina. We attribute this effect to the quenching of low-energy color defects (these of energies lower than 1.9 eV) when gold substrates are used, which reveals the surface nature of the defects created in hBN nanosheets. Results described here are important for future quantum light experiments and their integration in photonic chips.