Two-dimensional (2D) ReSe2 has attracted considerable interest due to its unique anisotropic mechanical, optical, and exitonic characteristics. Recent transient absorption experiments demonstrated a prolonged lifetime of photoexcited charge carriers by stacking ReSe2 with MoS2, but the underlying mechanism remains elusive. Here, by combining time-domain density functional theory with nonadiabatic molecular dynamics, we investigate the electronic properties and charge carrier dynamics of 2D ReSe2/MoS2 van der Waals (vdW) heterostructure. ReSe2/MoS2 has a type II band alignment that exhibits spatially distinguished conduction and valence band edges, and a built-in electric field is formed due to interface charge transfer. Remarkably, in spite of the decreased band gap and increased decoherence time, we demonstrate that the photocarrier lifetime of ReSe2/MoS2 is ∼5 times longer than that of ReSe2, which originates from the greatly reduced nonadiabatic coupling that suppresses electron–hole recombination, perfectly explaining the experimental results. These findings not only provide physical insights into experiments but also shed light on future design and fabrication of functional optoelectronic devices based on 2D vdW heterostructures.

Point defects in semiconductors usually act as nonradiative charge carrier recombination centers, which severely limit the performance of optoelectronic devices. In this work, by combining time-domain density functional theory with nonadiabatic molecular dynamics simulations, we demonstrate suppressed nonradiative charge carrier recombination and prolonged carrier lifetime in two-dimensional (2D) ReX 2 (X = S, Se) with S/Se vacancies. In particular, a S vacancy introduces a shallow hole trap state in ReS 2 , while a Se vacancy introduces both hole and electron trap states in ReSe 2 . Photoexcited electrons and holes can be rapidly captured by these defect states, while the release process is slow, which contributes to an elongated photocarrier lifetime. The suppressed charge carrier recombination lies in the vacancy-induced lowfrequency phonon modes that weaken electron−phonon coupling, as well as the reduced overlap between electron and hole wave functions that decreases nonadiabatic coupling. This work provides physical insights into the charge carrier dynamics of 2D ReX 2 , which may stimulate considerable interest in using defect engineering for future optoelectronic nanodevices.

By combining tight-binding modelling with density functional theory based first-principles calculations, we investigate the band evolution of two-dimensional (2D) hexagonal lattices with (px, py) orbitals, focusing on the electronic structures and topological phase transitions. The (px, py)-orbital hexagonal lattice model possesses two flat bands encompassing two linearly dispersive Dirac bands. Breaking the A/B sublattice symmetry could transform the model into two triangular lattices, each featuring a flat band and a dispersive band. Inclusion of the spin-orbit coupling and magnetization may give rise to quantum spin Hall (QSH) and quantum anomalous Hall (QAH) states. As a proof of concept, we demonstrate that half-hydrogenated stanene is encoded by a triangular lattice with (px, py) orbitals, which exhibits ferromagnetism and QAH effect with a topological gap of ~0.15 eV, feasible for experimental observation. These results provide fundamental insights into the structure-property relationships involving the orbital degree of freedom, which may shed light on future design and preparation of 2D topological materials for novel electronic/spintronic and quantum computing devices.

The power of surface chemistry to create atomically precise nanoarchitectures offers intriguing opportunities to advance the field of quantum technology. Strategies for building artificial electronic lattices by individually positioning atoms or molecules result in precisely tailored structures but lack structural robustness. Here, taking the advantage of strong bonding of Br atoms on noble metal surfaces, we report the production of stable quantum corrals by dehalogenation of hexabromobenzene molecules on a preheated Au(111) surface. The byproducts, Br adatoms, are confined within a new surface reconstruction pattern and aggregate into nanopores with an average size of 3.7 ± 0.1 nm, which create atomic orbital-like quantum resonance states inside each corral due to the interference of scattered electron waves. Remarkably, the atomic orbitals can be hybridized into molecular-like orbitals with distinct bonding and antibonding states. Our study opens up an avenue to fabricate quantum structures with high yield and superior robustness.

Triangular lattice, with each site coordinating with six neighbors, is one most common network in two-dimensional (2D) limit. Manifestations of peculiar properties in the lattice, including magnetic frustration and quantum spin liquid, have been restricted to single-orbital tight-binding (TB) model so far, while the orbital degree of freedom is largely overlooked. Here, by combining TB modeling with first-principles calculations, we demonstrate the rich electronic structures of triangular lattice with multiple $(p_{x}, p_{y}, p_{z})$ ( p x , p y , p z ) orbitals. Type I/II Dirac point, quadratic nodal point and nodal-loops are observed, and the topological phase diagram is mapped out by manipulating the horizontal mirror symmetry, spin-orbit coupling and energy position of relevant orbitals. Remarkably, we show that large-gap quantum spin Hall phase (∼0.2 eV) can be realized in experimentally achievable systems by growing indium monolayer on a series of semiconducting substrates, such as C/Si/Ge(111) and SiC(0001) surfaces, and the proposed materials capture the TB parameter space well. Our work not only provides physical insights into the orbital physics in 2D lattices, but also sheds light on the integration of novel quantum states with conventional semiconductor technology for potential applications, such as dissipationless interconnects for electronic circuits.