Moiré effects in vertical stacks of two-dimensional crystals give rise to new quantum materials with rich transport and optical phenomena that originate from modulations of atomic registries within moiré supercells. Due to finite elasticity, however, the superlattices can transform from moiré-type to periodically reconstructed patterns. Here we expand the notion of such nanoscale lattice reconstruction to the mesoscopic scale of laterally extended samples and demonstrate rich consequences in optical studies of excitons in MoSe2–WSe2 heterostructures with parallel and antiparallel alignments. Our results provide a unified perspective on moiré excitons in near-commensurate semiconductor heterostructures with small twist angles by identifying domains with exciton properties of distinct effective dimensionality, and establish mesoscopic reconstruction as a compelling feature of real samples and devices with inherent finite size effects and disorder. Generalized to stacks of other two-dimensional materials, this notion of mesoscale domain formation with emergent topological defects and percolation networks will instructively expand the understanding of fundamental electronic, optical and magnetic properties of van der Waals heterostructures.
Layered two-dimensional materials exhibit rich transport and optical phenomena in twisted or lattice-incommensurate heterostructures with spatial variations of interlayer hybridization arising from moiré interference effects. Here, we report experimental and theoretical studies of excitons in twisted heterobilayers and heterotrilayers of transition metal dichalcogenides. Using MoSe2-WSe2 stacks as representative realizations of twisted van der Waals bilayer and trilayer heterostructures, we observe contrasting optical signatures and interpret them in the theoretical framework of interlayer moiré excitons in different spin and valley configurations. We conclude that the photoluminescence of MoSe2-WSe2 heterobilayer is consistent with joint contributions from radiatively decaying valley-direct interlayer excitons and phonon-assisted emission from momentum-indirect reservoirs that reside in spatially distinct regions of moiré supercells, whereas the heterotrilayer emission is entirely due to momentum-dark interlayer excitons of hybrid-layer valleys. Our results highlight the profound role of interlayer hybridization for transition metal dichalcogenide heterostacks and other realizations of multi-layered semiconductor van der Waals heterostructures.
The studying of how twisted light interacts with chiral matter on the nanoscale is paramount for tackling the challenging task of optomechanical separation of nanoparticle enantiomers, whose solution can revolutionize the entire pharmaceutical industry. Here we calculate optical forces and torques exerted on chiral nanoparticles by Laguerre–Gaussian beams carrying a topological charge. We show that regardless of the beam polarization, the nanoparticles are exposed to both chiral and achiral forces with nonzero reactive and dissipative components. Longitudinally polarized beams are found to produce chirality densities that can be 109times higher than those of transversely polarized beams and that are comparable to the chirality densities of beams polarized circularly. Our results and analytical expressions prove useful in designing new strategies for mechanical separation of chiral nanoobjects with the help of highly focussed beams.
17 September 2018 in Physical Chemistry Chemical Physics