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Register a new userExciton spectroscopy of hexagonal boron nitride using non-resonant x-ray Raman scattering
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We report non-resonant x-ray Raman scattering (XRS) measurements from hexagonal boron nitride for transferred momentum from 2 to 9 $mathrm{AA}^{-1}$ along directions both in and out of the basal plane. A symmetry-based argument, together with real-space full multiple scattering calculations of the projected density of states in the spherical harmonics basis, reveals that a strong pre-edge feature is a dominantly $Y_{10}$-type Frenkel exciton with no other textit{s}-, textit{p}-, or textit{d}- components. This conclusion is supported by a second, independent calculation of the textbf{q}-dependent XRS cross-section based on the Bethe-Salpeter equation.
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High pressure Raman experiments on Boron Nitride multi-walled nanotubes show that the intensity of the vibrational mode at ~ 1367 cm-1 vanishes at ~ 12 GPa and it does not recover under decompression. In comparison, the high pressure Raman experiments on hexagonal Boron Nitride show a clear signature of a phase transition from hexagonal to wurtzite at ~ 13 GPa which is reversible on decompression. These results are contrasted with the pressure behavior of carbon nanotubes and graphite.
Quantum emitters in layered hexagonal boron nitride (hBN) have recently attracted a great attention as promising single photon sources. In this work, we demonstrate resonant excitation of a single defect center in hBN, one of the most important prerequisites for employment of optical sources in quantum information application. We observe spectral linewidths of hBN emitter narrower than 1 GHz while the emitter experiences spectral diffusion. Temporal photoluminescence measurements reveals an average spectral diffusion time of around 100 ms. On-resonance photon antibunching measurement is also realized. Our results shed light on the potential use of quantum emitters from hBN in nanophotonics and quantum information.
Graphene has demonstrated great promise for future electronics technology as well as fundamental physics applications because of its linear energy-momentum dispersion relations which cross at the Dirac point. However, accessing the physics of the low density region at the Dirac point has been difficult because of the presence of disorder which leaves the graphene with local microscopic electron and hole puddles, resulting in a finite density of carriers even at the charge neutrality point. Efforts have been made to reduce the disorder by suspending graphene, leading to fabrication challenges and delicate devices which make local spectroscopic measurements difficult. Recently, it has been shown that placing graphene on hexagonal boron nitride (hBN) yields improved device performance. In this letter, we use scanning tunneling microscopy to show that graphene conforms to hBN, as evidenced by the presence of Moire patterns in the topographic images. However, contrary to recent predictions, this conformation does not lead to a sizable band gap due to the misalignment of the lattices. Moreover, local spectroscopy measurements demonstrate that the electron-hole charge fluctuations are reduced by two orders of magnitude as compared to those on silicon oxide. This leads to charge fluctuations which are as small as in suspended graphene, opening up Dirac point physics to more diverse experiments than are possible on freestanding devices.
The temperature-dependent optical response of excitons in semiconductors is controlled by the exciton-phonon interaction. When the exciton-lattice coupling is weak, the excitonic line has a Lorentzian profile resulting from motional narrowing, with a width increasing linearly with the lattice temperature $T$. In contrast, when the exciton-lattice coupling is strong, the lineshape is Gaussian with a width increasing sublinearly with the lattice temperature, proportional to $sqrt{T}$. While the former case is commonly reported in the literature, here the latter is reported for the first time, for hexagonal boron nitride. Thus the theoretical predictions of Toyozawa [Progr. Theor. Phys. 20, 53 (1958)] are supported by demonstrating that the exciton-phonon interaction is in the strong coupling regime in this Van der Waals crystal.
Despite the recognition of two-dimensional (2D) systems as emerging and scalable host materials of single photon emitters or spin qubits, uncontrolled and undetermined chemical nature of these quantum defects has been a roadblock to further development. Leveraging the design of extrinsic defects can circumvent these persistent issues and provide an ultimate solution. Here we established a complete theoretical framework to accurately and systematically design quantum defects in wide-bandgap 2D systems. With this approach, essential static and dynamical properties are equally considered for spin qubit discovery. In particular, many-body interactions such as defect-exciton couplings are vital for describing excited state properties of defects in ultrathin 2D systems. Meanwhile, nonradiative processes such as phonon-assisted decay and intersystem crossing rates require careful evaluation, which compete together with radiative processes. From a thorough screening of defects based on first-principles calculations, we identify promising single photon emitters such as SiVV and spin qubits such as TiVV and MoVV in hexagonal boron nitride. This work provided a complete first-principles theoretical framework for defect design in 2D materials.
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