Various near-atom-thickness two-dimensional (2D) van der Waals (vdW) crystals with unparalleled electromechanical properties have been explored for transformative devices. Currently, the availability of 2D vdW crystals is rather limited in nature as they are only obtained from certain mother crystals with intrinsically possessed layered crystallinity and anisotropic molecular bonding. Recent efforts to transform conventionally non-vdW three-dimensional (3D) crystals into ultrathin 2D-like structures have seen rapid developments to explore device building blocks of unique form factors. Herein, we explore a “peel-and-stick” approach, where a nonlayered 3D platinum sulfide (PtS) crystal, traditionally known as a cooperate mineral material, is transformed into a freestanding 2D-like membrane for electromechanical applications. The ultrathin (∼10 nm) 3D PtS films grown on large-area (>cm2) silicon dioxide/silicon (SiO2/Si) wafers are precisely “peeled” inside water retaining desired geometries via a capillary-force-driven surface wettability control. Subsequently, they are “sticked” on strain-engineered patterned substrates presenting prominent semiconducting properties, i.e., p-type transport with an optical band gap of ∼1.24 eV. A variety of mechanically deformable strain-invariant electronic devices have been demonstrated by this peel-and-stick method, including biaxially stretchable photodetectors and respiratory sensing face masks. This study offers new opportunities of 2D-like nonlayered semiconducting crystals for emerging mechanically reconfigurable and stretchable device technologies.

The possibility to achieve charge-to-spin conversion via Rashba spin–orbit effects provides stimulating opportunities toward the development of nanoscale spintronics. Here, we use first-principles calculations to study the electronic and spintronic properties of Tl₂O/PtS₂ heterostructure, for which we have confirmed the dynamical stability by its positive phonon frequencies. An unexpectedly high binding energy of −0.38 eV per unit cell depicts strong interlayer interactions between Tl₂O and PtS₂. Interestingly, we discover Rashba spin-splittings (with a large α_R value) in the valence band of Tl₂O stemming from interfacial spin–orbit effects caused by PtS₂. The role of van der Waals binding on the orbital rearrangements has been studied using the electron localization function and atomic orbital projections, which explains in detail the electronic dispersion near the Fermi level. Moreover, we explain the distinct band structure alignment in momentum space but separation in real space of Tl₂O/PtS₂ heterostructure. Since two-dimensional (2D) Tl₂O still awaits experimental confirmation, we calculate, for the first time, the Raman spectra of pristine Tl₂O and the Tl₂O/PtS₂ heterostructure and discuss peak positions corresponding to vibrational modes of the atoms. These findings offer a promising avenue to explore spin physics for potential spintronics applications via 2D heterostructures.

Artificial heterojunctions formed by vertical stacking of dissimilar two-dimensional (2D) transition metal dichalcogenide (TMD) monolayer materials in a chosen sequence hold tantalizing prospects for futuristic atomically thin circuits. The emergence of 2D topological insulators (TI), including Bi2Te3, Bi2Se3, and Sb2Te3, represents a new class of 2D building blocks and can complement the existing artificial heterojunctions as a result of their intriguing surface states protected by the time-reversal symmetry. However, the determination of band alignments of such 2D TI/TMD vertical heterojunctions, the key parameter for designing HJ-based electronic/photonic devices, which lies in the development of epitaxy growth, remains in its infancy. Here, we demonstrate the epitaxy growth of 2D TI/TMD vertical heterojunctions comprised of Bi2Te3/WSe2 with atomically clean interfaces that are spectroscopically accessible, and theoretically tractable. Cross-sectional scanning transmission electron microscopy (STEM) images and the presence of interlayer-coupled characteristics from Raman spectroscopy collectively confirm the neat stacking of Bi2Te3/WSe2 with the absence of unwanted containments. Microbeam X-ray photoelectron spectroscopy (ΌXPS) measurement coupled with the density functional theory (DFT) calculations and electrical characteristics of field effect transistors quantitatively reveals the type-II alignment of vertically stacked of quintuple layers (QL) Bi2Te3/WSe2. Meanwhile, the type-III band emerges when transitioning to multi-quintuple layer (MQL) Bi2Te3/WSe2. The finding here provides a well-defined example of the epitaxy growth paradigm, the interlayer coupling-electronic properties relationship, for these emerging 2D TI/TMDs vertical heterojunctions. © 2020 American Chemical Society.

2D PtTe₂ layers, a relatively new class of 2D crystals, have unique band structure and remarkably high electrical conductivity promising for emergent opto-electronics. This intrinsic superiority can be further leveraged toward practical device applications by merging them with mature 3D semiconductors, which has remained largely unexplored. Herein, we explored 2D/3D heterojunction devices by directly growing large-area (>cm²) 2D PtTe₂ layers on Si wafers using a low-temperature CVD method and unveiled their superior opto-electrical characteristics. The devices exhibited excellent Schottky transport characteristics essential for high-performance photovoltaics and photodetection, i.e., well-balanced combination of high photodetectivity (>10¹³ Jones), small photo-responsiveness time (∼1 μs), high current rectification ratio (>10⁵), and water super-hydrophobicity driven photovoltaic improvement (>300%). These performances were identified to be superior to those of previously explored 2D/3D or 2D layer-based devices with much smaller junction areas, and their underlying principles were confirmed by DFT calculations.

We use first-principles calculations to show that van der Waals (vdW) heterostructures consisting of few-layer Bi₂Se₃ and PtSe₂ exhibit electronic and spintronics properties that can be tuned by varying the constituent layers. Type-II band alignment with layer-tunable band gaps and type-III band alignment with spin-splittings have been found. Most notably, we reveal the coexistence of Rashba-type spin-splittings (with large α_R parameters) in both the conduction and valence band stemming from few-layer Bi₂Se₃ and PtSe₂, respectively, which has been confirmed by spin-texture plots. We discuss the role of inversion symmetry breaking, changes in orbital hybridization, and spin–orbit coupling in altering electronic dispersion near the Fermi level. Since low-temperature growth mechanisms are available for both materials, we believe that few-layer Bi₂Se₃/PtSe₂ vdW heterostructures are feasible to realize experimentally, offering great potential for electronic and spintronics applications.