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Register a new userOrientation dependence of high-harmonic generation in monolayer transition metal dichalcogenides
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We theoretically investigate the orientation dependence of high-harmonic generation (HHG) in monolayer transition metal dichalcogenides (TMDCs). We find that, unlike conventional solid-state and atomic layered materials such as graphene, both parallel and perpendicular emissions with respect to the incident electric field exist in TMDCs. Interestingly, the parallel (perpendicular) emissions principally contain only odd-(even-) order harmonics. Both harmonics show the same periodicity in the crystallographic orientations but opposite phases. These peculiar behaviors can be understood on the basis of the dipole moments in TMDCs, which reflect the symmetries of both atomic orbitals and lattice structures. Our findings are qualitatively consistent with recent experi- mental results and provide a possibility for high-harmonic spectroscopy of solid-state materials.
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We theoretically investigate detuning-dependent properties of high-order harmonic generation (HHG) in monolayer transition metal dichalcogenides (TMDCs). In contrast to HHG in conventional materials, TMDCs show both parallel and perpendicular emissions with respect to the incident electric field. We find that such an anomalous emission can be artificially controlled by the frequency detuning of the incident electric fields, i.e., the parallel and perpendicular HHG can be strongly enhanced by multiphoton resonances. This peculiar phenomenon would provide a way for controlling HHG in TMDCs and stimulate the realization of novel optical devices.
Monolayer transition metal dichalcogenides (TMDs) exhibit high nonlinear optical (NLO) susceptibilities. Experiments on MoS$_2$ have indeed revealed very large second-order ($chi^{(2)}$) and third-order ($chi^{(3)}$) optical susceptibilities. However, third harmonic generation results of other layered TMDs has not been reported. Furthermore, the reported $chi^{(2)}$ and $chi^{(3)}$ of MoS$_2$ vary by several orders of magnitude, and a reliable quantitative comparison of optical nonlinearities across different TMDs has remained elusive. Here, we investigate second- and third-harmonic generation, and three-photon photoluminescence in TMDs. Specifically, we present an experimental study of $chi^{(2)}$, and $chi^{(3)}$ of four common TMD materials (ce{MoS2}, ce{MoSe2}, ce{WS2} and ce{WSe2}) by placing different TMD flakes in close proximity to each other on a common substrate, allowing their NLO properties to be accurately obtained from a single measurement. $chi^{(2)}$ and $chi^{(3)}$ of the four monolayer TMDs have been compared, indicating that they exhibit distinct NLO responses. We further present theoretical simulations of these susceptibilities in qualitative agreement with the measurements. Our comparative studies of the NLO responses of different two-dimensional layered materials allow us to select the best candidates for atomic-scale nonlinear photonic applications, such as frequency conversion and all-optical signal processing.
The optical properties of atomically thin transition metal dichalcogenide (TMDC) semiconductors are shaped by the emergence of correlated many-body complexes due to strong Coulomb interaction. Exceptional electron-hole exchange predestines TMDCs to study fundamental and applied properties of Coulomb complexes such as valley depolarization of excitons and fine-structure splitting of trions. Biexcitons in these materials are less understood and it has been established only recently that they are spectrally located between exciton and trion. Here we show that biexcitons in monolayer TMDCs exhibit a distinct fine structure on the order of meV due to electron-hole exchange. Ultrafast pump-probe experiments on monolayer WSe$_2$ reveal decisive biexciton signatures and a fine structure in excellent agreement with a microscopic theory. We provide a pathway to access biexciton spectra with unprecedented accuracy, which is valuable beyond the class of TMDCs, and to understand even higher Coulomb complexes under the influence of electron-hole exchange.
Recently, the celebrated Keldysh potential has been widely used to describe the Coulomb interaction of few-body complexes in monolayer transition-metal dichalcogenides. Using this potential to model charged excitons (trions), one finds a strong dependence of the binding energy on whether the monolayer is suspended in air, supported on SiO$_2$, or encapsulated in hexagonal boron-nitride. However, empirical values of the trion binding energies show weak dependence on the monolayer configuration. This deficiency indicates that the description of the Coulomb potential is still lacking in this important class of materials. We address this problem and derive a new potential form, which takes into account the three atomic sheets that compose a monolayer of transition-metal dichalcogenides. The new potential self-consistently supports (i) the non-hydrogenic Rydberg series of neutral excitons, and (ii) the weak dependence of the trion binding energy on the environment. Furthermore, we identify an important trion-lattice coupling due to the phonon cloud in the vicinity of charged complexes. Neutral excitons, on the other hand, have weaker coupling to the lattice due to the confluence of their charge neutrality and small Bohr radius.
To advance fundamental understanding, and ultimate application, of transition-metal dichalcogenide (TMD) monolayers, it is essential to develop capabilities for the synthesis of high-quality single-layer samples. Molecular beam epitaxy (MBE), a leading technique for the fabrication of the highest-quality epitaxial films of conventional semiconductors has, however, typically yielded only small grain sizes and sub-optimal morphologies when applied to the van der Waals growth of monolayer TMDs. Here, we present a systematic study on the influence of adatom mobility, growth rate, and metal:chalcogen flux on the growth of NbSe2, VSe2 and TiSe2 using MBE. Through this, we identify the key drivers and influence of the adatom kinetics that control the epitaxial growth of TMDs, realising four distinct morphologies of the as-grown compounds. We use this to determine optimised growth conditions for the fabrication of high-quality monolayers, ultimately realising the largest grain sizes of monolayer TMDs that have been achieved to date via MBE growth.
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