High oscillator strength interlayer excitons in two-dimensional heterostructures for mid-infrared photodetection.

The development of infrared photodetectors is mainly limited by the choice of available materials and the intricate crystal growth process. Moreover, thermally activated carriers in traditional III-V and II-VI semiconductors enforce low operating temperatures in the infrared photodetectors. Here we demonstrate infrared photodetection enabled by interlayer excitons (ILEs) generated between tungsten and hafnium disulfide, WS2/HfS2. The photodetector operates at room temperature and shows an even higher performance at higher temperatures owing to the large exciton binding energy and phonon-assisted optical transition. The unique band alignment in the WS2/HfS2 heterostructure allows interlayer bandgap tuning from the mid- to long-wave infrared spectrum. We postulate that the sizeable charge delocalization and ILE accumulation at the interface result in a greatly enhanced oscillator strength of the ILEs and a high responsivity of the photodetector. The sensitivity of ILEs to the thickness of two-dimensional materials and the external field provides an excellent platform to realize robust tunable room temperature infrared photodetectors.

Engineering covalently bonded 2D layered materials by self-intercalation.

Two-dimensional (2D) materials1-5 offer a unique platform from which to explore the physics of topology and many-body phenomena. New properties can be generated by filling the van der Waals gap of 2D materials with intercalants6,7; however, post-growth intercalation has usually been limited to alkali metals8-10. Here we show that the self-intercalation of native atoms11,12 into bilayer transition metal dichalcogenides during growth generates a class of ultrathin, covalently bonded materials, which we name ic-2D. The stoichiometry of these materials is defined by periodic occupancy patterns of the octahedral vacancy sites in the van der Waals gap, and their properties can be tuned by varying the coverage and the spatial arrangement of the filled sites7,13. By performing growth under high metal chemical potential14,15 we can access a range of tantalum-intercalated TaS(Se)y, including 25% Ta-intercalated Ta9S16, 33.3% Ta-intercalated Ta7S12, 50% Ta-intercalated Ta10S16, 66.7% Ta-intercalated Ta8Se12 (which forms a Kagome lattice) and 100% Ta-intercalated Ta9Se12. Ferromagnetic order was detected in some of these intercalated phases. We also demonstrate that self-intercalated V11S16, In11Se16 and FexTey can be grown under metal-rich conditions. Our work establishes self-intercalation as an approach through which to grow a new class of 2D materials with stoichiometry- or composition-dependent properties.

Classifying the Electronic and Optical Properties of Janus Monolayers.

Inspired by the recent synthesis of monolayer MoSSe, we conduct a first-principles high-throughput investigation of 216 MXY Janus monolayers consisting of a middle layer of metal atoms (M) sandwiched between different types of chalcogen, halogen, or pnictogen atoms (X,Y). Using density functional theory and many-body perturbation theory, we perform an exhaustive computational characterization of the 70 most stable semiconducting monolayers. These are found to exhibit diverse and fascinating properties including finite out-of-plane dipoles, giant Rashba-splittings, direct and indirect band gaps ranging from 0.7 to 3.0 eV, large exciton binding energies, and very strong light-matter interactions. The data have been generated using the workflow behind the Computational 2D Materials Database and are freely available online. Our work expands the class of known Janus monolayers and points to several potentially synthesizable structures, which could be interesting candidates for valley- or optoelectronic applications or for generating out-of-plane electric fields to control charge transfer, charge separation, or band alignments in van der Waals heterostructures.