No Arabic abstract
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.
The thermal conductivity of suspended few-layer hexagonal boron nitride (h-BN) was measured using a micro-bridge device with built-in resistance thermometers. Based on the measured thermal resistance values of 11-12 atomic layer h-BN samples with suspended length ranging between 3 and 7.5 um, the room-temperature thermal conductivity of a 11-layer sample was found to be about 360 Wm-1K-1, approaching the basal plane value reported for bulk h-BN. The presence of a polymer residue layer on the sample surface was found to decrease the thermal conductivity of a 5-layer h-BN sample to be about 250 Wm-1K-1 at 300 K. Thermal conductivities for both the 5 layer and the 11 layer samples are suppressed at low temperatures, suggesting increasing scattering of low frequency phonons in thin h-BN samples by polymer residue.
The relative orientation of successive sheets, i.e. the stacking sequence, in layered two-dimensional materials is central to the electronic, thermal, and mechanical properties of the material. Often different stacking sequences have comparable cohesive energy, leading to alternative stable crystal structures. Here we theoretically and experimentally explore different stacking sequences in the van der Waals bonded material hexagonal boron nitride (h-BN). We examine the total energy, electronic bandgap, and dielectric response tensor for five distinct high symmetry stacking sequences for both bulk and bilayer forms of h-BN. Two sequences, the generally assumed AA sequence and the relatively unknown (for h-BN) AB (Bernal) sequence, are predicted to have comparably low energy. We present a scalable modified chemical vapor deposition method that produces large flakes of virtually pure AB stacked h-BN; this new material complements the generally available AA stacked h-BN.
The relative twist angle in heterostructures of two-dimensional (2D) materials with similar lattice constants result in a dramatic alteration of the electronic properties. Here, we investigate the electrical and magnetotransport properties in bilayer graphene (BLG) encapsulated between two hexagonal boron nitride (hBN) crystals, where the top and bottom hBN are rotationally aligned with bilayer graphene with a twist angle $theta_tsim 0^{circ} text{and}~ theta_b < 1^{circ}$, respectively. This results in the formation of two moire superlattices, with the appearance of satellite resistivity peaks at carrier densities $n_{s1}$ and $n_{s2}$, in both hole and electron doped regions, together with the resistivity peak at zero carrier density. Furthermore, we measure the temperature(T) dependence of the resistivity ($rho$). The resistivity shows a linear increment with temperature within the range 10K to 50K for the density regime $n_{s1} <n<n_{s2}$ with a large slope d$rho$/dT $sim$ 8.5~$Omega$/K. The large slope of d$rho$/dT is attributed to the enhanced electron-phonon coupling arising due to the suppression of Fermi velocity in the reconstructed minibands, which was theoretically predicted, recently in doubly aligned graphene with top and bottom hBN. Our result establishes the uniqueness of doubly aligned moire system to tune the strength of electron-phonon coupling and to modify the electronic properties of multilayered heterostructures.
The stacking orders in layered hexagonal boron nitride bulk and bilayers are studied using high-level ab initio theory (local second-order Moller-Plesset perturbation theory, LMP2). Our results show that both electrostatic and London dispersion interactions are responsible for interlayer distance and stacking order, with AA being the most stable one. The minimum energy sliding path includes only the AA high-symmetry stacking, and the energy barrier is 3.4 meV per atom for the bilayer. State-of-the-art Density-functionals with and without London dispersion correction fail to correctly describe the interlayer energies with the exception of PBEsol that agrees very well with our LMP2 results and experiment.