Rapid discrimination of chemically distinctive surface terminations in 2D material based heterostructures by direct van der Waals identification.

We demonstrate that surfaces presenting heterogeneous and atomically flat domains can be directly and rapidly discriminated via robust intensive quantifiables by exploiting one-pass noninvasive methods in standard atomic force microscopy (AFM), single ∼2 min passes, or direct force reconstruction, i.e., ∼103 force profiles (∼10 min collection time), allowing data collection, interpretation, and presentation in under 20 min, including experimental AFM preparation and excluding only sample fabrication, in situ and without extra experimental or time load. We employ a misfit SnTiS3 compound as a model system. Such heterostructures can be exploited as multifunctional surface systems and provide multiple support sites with distinguishable chemical, mechanical, or opto-electronic distinct properties. In short, they provide an ideal model system to exemplify how current AFM methods can significantly support material discovery across fields.

Insights into graphene wettability transparency by locally probing its surface free energy.

In this work, we study the surface energy of monolayer, bilayer and multilayer graphene coatings, produced through exfoliation of natural graphite flakes and chemical vapor deposition. We employ bimodal atomic force microscopy and micro-Raman spectroscopy for high spatial resolution and large area scanning of force of adhesion on the regions of the graphene/SiO2 surface with different graphene layers. Our measurements show that the interface conditions between graphene and SiO2 dominate the experimentally observed graphene surface energy. This finding sheds new light on the controversy surrounding graphene transparency studies. By separating the surface energy into polar and non-polar interactions, our findings suggest that monolayer graphene is nearly van der Waals opaque but partially transparent (near 60%) to polar interactions, which is further supported by characterizing graphene on the copper surface and two levels of density functional theory simulation. In addition to providing quantitative insight into the surface interactions of complicated graphene coatings, this work demonstrates a new route to nondestructively monitor the interface between graphene and coated substrates.

Multi-Valley Superconductivity in Ion-Gated MoS2 Layers.

Layers of transition metal dichalcogenides (TMDs) combine the enhanced effects of correlations associated with the two-dimensional limit with electrostatic control over their phase transitions by means of an electric field. Several semiconducting TMDs, such as MoS2, develop superconductivity (SC) at their surface when doped with an electrostatic field, but the mechanism is still debated. It is often assumed that Cooper pairs reside only in the two electron pockets at the K/K' points of the Brillouin Zone. However, experimental and theoretical results suggest that a multivalley Fermi surface (FS) is associated with the SC state, involving six electron pockets at Q/Q'. Here, we perform low-temperature transport measurements in ion-gated MoS2 flakes. We show that a fully multivalley FS is associated with the SC onset. The Q/Q' valleys fill for doping ≳ 2 × 1013 cm-2, and the SC transition does not appear until the Fermi level crosses both spin-orbit split sub-bands Q 1 and Q 2. The SC state is associated with the FS connectivity and promoted by a Lifshitz transition due to the simultaneous population of multiple electron pockets. This FS topology will serve as a guideline in the quest for new superconductors.

High photosensitivity and broad spectral response of multi-layered germanium sulfide transistors.

In this paper, we report the optoelectronic properties of multi-layered GeS nanosheet (∼28 nm thick)-based field-effect transistors (called GeS-FETs). The multi-layered GeS-FETs exhibit remarkably high photoresponsivity of Rλ ∼ 206 A W(-1) under 1.5 µW cm(-2) illumination at λ = 633 nm, Vg = 0 V, and Vds = 10 V. The obtained Rλ ∼ 206 A W(-1) is excellent as compared with a GeS nanoribbon-based and the other family members of group IV-VI-based photodetectors in the layered-materials realm, such as GeSe and SnS2. The gate-dependent photoresponsivity of GeS-FETs was further measured to be able to reach Rλ ∼ 655 A W(-1) operated at Vg = -80 V. Moreover, the multi-layered GeS photodetector holds high external quantum efficiency (EQE ∼ 4.0 × 10(4)%) and specific detectivity (D* ∼ 2.35 × 10(13) Jones). The measured D* is comparable to those of the advanced commercial Si- and InGaAs-based photodiodes. The GeS photodetector also shows an excellent long-term photoswitching stability over a long period of operation (>1 h). These extraordinary properties of high photocurrent generation, broad spectral range, and long-term stability make the GeS-FET photodetector a highly qualified candidate for future optoelectronic applications.

High performance and bendable few-layered InSe photodetectors with broad spectral response.

Two-dimensional crystals with a wealth of exotic dimensional-dependent properties are promising candidates for next-generation ultrathin and flexible optoelectronic devices. For the first time, we demonstrate that few-layered InSe photodetectors, fabricated on both a rigid SiO2/Si substrate and a flexible polyethylene terephthalate (PET) film, are capable of conducting broadband photodetection from the visible to near-infrared region (450-785 nm) with high photoresponsivities of up to 12.3 AW(-1) at 450 nm (on SiO2/Si) and 3.9 AW(-1) at 633 nm (on PET). These photoresponsivities are superior to those of other recently reported two-dimensional (2D) crystal-based (graphene, MoS2, GaS, and GaSe) photodetectors. The InSe devices fabricated on rigid SiO2/Si substrates possess a response time of ∼50 ms and exhibit long-term stability in photoswitching. These InSe devices can also operate on a flexible substrate with or without bending and reveal comparable performance to those devices on SiO2/Si. With these excellent optoelectronic merits, we envision that the nanoscale InSe layers will not only find applications in flexible optoelectronics but also act as an active component to configure versatile 2D heterostructure devices.

Chemical vapor deposition synthesis and Raman spectroscopic characterization of large-area graphene sheets.

We present a chemical vapor deposition (CVD) method to catalytically synthesize large-area, transferless, single- to few-layer graphene sheets using hexamethyldisilazane (HMDS) on a SiO2/Si substrate as a carbon source and thermally evaporated alternating Ni/Cu/Ni layers as a catalyst. The as-synthesized graphene films were characterized by Raman spectroscopic imaging to identify single- to few-layer sheets. This HMDS-derived graphene layer is continuous over the entire growth substrate, and single- to trilayer mixed sheets can be up to 30 µm in the lateral dimension. With the synthetic CVD method proposed here, graphene can be grown into tailored shapes directly on a SiO2/Si surface through vapor priming of HMDS onto predefined photolithographic patterns. The transparent and conductive HMDS-derived graphene exhibits its potential for widespread electronic and opto-electronic applications.