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Register a new userPhonon-assisted emission and absorption of individual color centers in hexagonal boron nitride
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Defect centers in hexagonal boron nitride represent room-temperature single-photon sources in a layered van der Waals material. These light emitters appear with a wide range of transition energies ranging over the entire visible spectrum, which renders the identification of the underlying atomic structure challenging. In addition to their eminent properties as quantum light emitters, the coupling to phonons is remarkable. Their photoluminescence exhibits significant side band emission well separated from the zero phonon line (ZPL) and an asymmetric broadening of the ZPL itself. In this combined theoretical and experimental study we show that the phonon side bands can be well described in terms of the coupling to bulk longitudinal optical (LO) phonons. To describe the ZPL asymmetry we show that in addition to the coupling to longitudinal acoustic (LA) phonons also the coupling to local mode oscillations of the defect center with respect to the entire host crystal has to be considered. By studying the influence of the emitters wave function dimensions on the phonon side bands we find reasonable values for size of the wave function and the deformation potentials. We perform photoluminescence excitation measurements to demonstrate that the excitation of the emitters is most efficient by LO-phonon assisted absorption.
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We theoretically study physical properties of the most promising color center candidates for the recently observed single-photon emissions in hexagonal boron nitride (h-BN) monolayers. Through our group theory analysis combined with density functional theory (DFT) calculations we provide several pieces of evidence that the electronic properties of the color centers match the characters of the experimentally observed emitters. We calculate the symmetry-adapted multi-electron wavefunctions of the defects using group theory methods and analyze the spin-orbit and spin-spin interactions in detail. We also identify the radiative and non-radiative transition channels for each color center. An advanced ab-initio DFT method is then used to compute energy levels of the color centers and their zero-phonon-line (ZPL) emissions. The computed ZPLs, the profile of excitation and emission dipole polarizations, and the competing relaxation processes are discussed and matched with the observed emission lines. By providing evidence for the relation between single-photon emitters and local defects in h-BN, this work provides the first steps towards harnessing quantum dynamics of these color centers.
Electron tunneling spectroscopy measurements on van der Waals heterostructures consisting of metal and graphene (or graphite) electrodes separated by atomically thin hexagonal boron nitride tunnel barriers are reported. The tunneling conductance dI/dV at low voltages is relatively weak, with a strong enhancement reproducibly observed to occur at around |V| ~ 50 mV. While the weak tunneling at low energies is attributed to the absence of substantial overlap, in momentum space, of the metal and graphene Fermi surfaces, the enhancement at higher energies signals the onset of inelastic processes in which phonons in the heterostructure provide the momentum necessary to link the Fermi surfaces. Pronounced peaks in the second derivative of the tunnel current, are observed at voltages where known phonon modes in the tunnel junction have a high density of states. In addition, features in the tunneling conductance attributed to single electron charging of nanometer-scale defects in the boron nitride are also observed in these devices. The small electronic density of states of graphene allows the charging spectra of these defect states to be electrostatically tuned, leading to Coulomb diamonds in the tunneling conductance.
Atomically thin van der Waals crystals have recently enabled new scientific and technological breakthroughs across a variety of disciplines in materials science, nanophotonics and physics. However, non-classical photon emission from these materials has not been achieved to date. Here we report room temperature quantum emission from hexagonal boron nitride nanoflakes. The single photon emitter exhibits a combination of superb quantum optical properties at room temperature that include the highest brightness reported in the visible part of the spectrum, narrow line width, absolute photo-stability, a short excited state lifetime and a high quantum efficiency. Density functional theory modeling suggests that the emitter is the antisite nitrogen vacancy defect that is present in single and multi-layer hexagonal boron nitride. Our results constitute the unprecedented potential of van der Waals crystals for nanophotonics, optoelectronics and quantum information processing.
Quantum emitters in hexagonal boron nitride (hBN) are emerging as bright and robust sources of single photons for applications in quantum optics. In this work we present detailed studies on the limiting factors to achieve Fourier Transform limited spectral lines. Specifically, we study phonon dephasing and spectral diffusion of quantum emitters in hBN via resonant excitation spectroscopy at cryogenic temperatures. We show that the linewidths of hBN quantum emitters are phonon broadened, even at 5K, with typical values of the order of one GHz. While spectral diffusion dominates at increasing pump powers, it can be minimized by working well below saturation excitation power. Our results are important for future utilization of quantum emitters in hBN for quantum interference experiments.
We investigate the effect of surface acoustic waves on the atomic-like optical emission from defect centers in hexagonal boron nitride layers deposited on the surface of a LiNbO$_3$ substrate. The dynamic strain field of the surface acoustic waves modulates the emission lines resulting in intensity variations as large as 50% and oscillations of the emission energy with an amplitude of almost 1 meV. From a systematic study of the dependence of the modulation on the acoustic wave power, we determine a hydrostatic deformation potential for defect centers in this two-dimensional material of about 40 meV/%. Furthermore, we show that the dynamic piezoelectric field of the acoustic wave could contribute to the stabilization of the optical properties of these centers. Our results show that surface acoustic waves are a powerful tool to modulate and control the electronic states of two-dimensional materials.
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