Generation and Detection of Strain-Localized Excitons in WS Monolayer by Plasmonic Metal Nanocrystals.

Excitons in a transition-metal dichalcogenide (TMDC) monolayer can be modulated through strain with spatial and spectral control, which offers opportunities for constructing quantum emitters for applications in on-chip quantum communication and information processing. Strain-localized excitons in TMDC monolayers have so far mainly been observed under cryogenic conditions because of their subwavelength emission area, low quantum yield, and thermal-fluctuation-induced delocalization. Herein, we demonstrate both generation and detection of strain-localized excitons in WS monolayer through a simple plasmonic structure design, where WS monolayer covers individual Au nanodisks or nanorods.

Light-Controlled Ultrafast Magnetic State Transition in Antiferromagnetic-Ferromagnetic van der Waals Heterostructures.

Manipulating spin in antiferromagnetic (AFM) materials has great potential in AFM opto-spintronics. Laser pulses can induce a transient ferromagnetic (FM) state in AFM metallic systems but have never been proven in two-dimensional (2D) AFM semiconductors and related van der Waals (vdW) heterostructures. Herein, using 2D vdW heterostructures of FM MnS and AFM MXenes as prototypes, we investigated optically induced interlayer spin transfer dynamics based on real-time time-dependent density functional theory.

Anisotropic Phononic and Electronic Thermal Transport in BeN.

Beryllium polynitride (BeN) has been recently synthesized under high-pressure conditions [Bykov . 2021, 126, 175501]. Its anisotropic lattice structure dependent on the applied pressure motivates exploration of its thermal transport properties with a theoretical framework that combines the Boltzmann transport equation with calculations.

Anomalously Isotropic Electron Transport and Weak Electron-Phonon Interactions in Hexagonal Noble Metals.

The electrical transport properties of typical hexagonal metals are anisotropic because of their anisotropic lattice structures. Unexpectedly, we show that the electron transport properties in hexagonal close-packed () noble metals are almost isotropic. Although the electron transport properties of an individual electronic band are highly anisotropic, the total contributions are almost equal in different crystalline orientations because of the complementary contributions of different bands.

Effect of interfacial defects on the electronic properties of MoS based lateral T-H heterophase junctions.

The coexistence of semiconducting (2H) and metallic (1T) phases of MoS monolayers has further pushed their strong potential for applications in the next generation of electronic devices based on two-dimensional lateral heterojunctions. Structural defects have considerable effects on the properties of these 2D devices. In particular, the interfaces of two phases are often imperfect and may contain numerous vacancies created by phase engineering techniques, under an electron beam.

Assembly of gold nanorods functionalized by zirconium-based metal-organic frameworks for surface enhanced Raman scattering.

Surface-enhanced Raman scattering (SERS) is a promising detection technique providing outstanding molecular fingerprint identification and high sensitivity of analytes. Developing sensitive and stable SERS substrates is highly desirable but remains a challenge. We herein report a wet-chemistry approach for the preparation of (Au nanorod core)@(Zr-based metal-organic framework shell) (Au nanorod@Zr-MOF) nanostructures with the Zr-MOF shell thickness ranging from 3 nm to 90 nm.

Ultrafast Light-Induced Ferromagnetic State in Transition Metal Dichalcogenides Monolayers.

Ultrafast optical control of magnetism had great potential to revolutionize magnetic storage technology and spintronics, but for now, its potential remains mostly untapped in two-dimensional (2D) magnets. Here, using the state-of-the-art real-time time-dependent density functional theory (rt-TDDFT), we demonstrate that an ultrafast laser pulse can induce a ferromagnetic state in nonmagnetic MoSe monolayers interfaced with van der Waals (vdW) ferromagnetic MnSe. Our results show that the transient ferromagnetism in MoSe derives from photoinduced direct ultrafast interlayer spin transfer from Mn to Mo via a vdW-coupled interface, albeit with a delay of approximately a few femtoseconds.

Structure-Based Simulation and Sampling of Transcription Factor Protein Movements along DNA from Atomic-Scale Stepping to Coarse-Grained Diffusion.

One-dimensional (1-D) sliding of transcription factor (TF) protein along DNA is essential for facilitated diffusion of the TF to locate target DNA site for genetic regulation. Detecting base-pair (bp) resolution of the TF sliding or stepping on the DNA is still experimentally challenging. We have recently performed all-atom molecular dynamics (MD) simulations capturing spontaneous 1-bp stepping of a small WRKY domain TF protein along DNA.

Phonon Thermal Transport in Silicene/Graphene Heterobilayer Nanostructures: Effect of Interlayer Interactions.

Heterostructuring, as a promising route to optimize the physical properties of 2D materials, has attracted great attention from the academic community. In this paper, we investigated the room-temperature in-plane and cross-plane phonon thermal transport in silicene/graphene van der Waals (vdW) heterostructures using molecular dynamics simulations. Our simulation results demonstrated that heat current along the graphene layer is remarkably larger than that along the silicene layer, which suggests that graphene dominates the thermal transport in silicene/graphene heterostructures.

DNA sequencing based on electronic tunneling in a gold nanogap: a first-principles study.

Deoxyribonucleic acid (DNA) sequencing has found wide applications in medicine including treatment of diseases, diagnosis and genetics studies. Rapid and cost-effective DNA sequencing has been achieved by measuring the transverse electronic conductance as a single-stranded DNA is driven through a nanojunction. With the aim of improving the accuracy and sensitivity of DNA sequencing, we investigate the electron transport properties of DNA nucleobases within gold nanogaps based on first-principles quantum transport simulations.

Carrier doping-induced strong magnetoelastic coupling in 2D lattice.

The realization of intertwined ferroelasticity and ferromagnetism in two-dimensional (2D) lattices is of great interest for broad nanoscale applications but still remains a remarkable challenge. Here, we propose an alternative approach to realize the strongly coupled ferromagnetism and ferroelasticity by carrier doping. We demonstrate that prototypical 2D β-PbO is dynamically, thermally and mechanically stable.

Density functional tight binding approach utilized to study X-ray-induced transitions in solid materials.

Intense X-ray pulses from free-electron lasers can trigger ultrafast electronic, structural and magnetic transitions in solid materials, within a material volume which can be precisely shaped through adjustment of X-ray beam parameters. This opens unique prospects for material processing with X rays. However, any fundamental and applicational studies are in need of computational tools, able to predict material response to X-ray radiation.

Switching promotor recognition of phage RNA polymerase in silico along lab-directed evolution path.

In this work, we computationally investigated how a viral RNA polymerase (RNAP) from bacteriophage T7 evolves into RNAP variants under lab-directed evolution to switch recognition from T7 promoter to T3 promoter in transcription initiation. We first constructed a closed initiation complex for the wild-type T7 RNAP and then for six mutant RNAPs discovered from phage-assisted continuous evolution experiments. All-atom molecular dynamics simulations up to 1 μs each were conducted on these RNAPs in a complex with the T7 and T3 promoters.

Localized Orbital Excitation Drives Bond Formation in Plasmonic Catalysis.

Localized surface plasmons generated on metallic nanostructures can be used to accelerate molecular transformations; however, the efficiency is limited by the challenge to control the energy/charge transfer at the interfaces. Here, we combine density functional theory (DFT) calculations and experiments to reveal the mechanism of nitrophenol reduction on Au nanoparticles under visible-light irradiation and propose a strategy to further enhance the reaction rates. DFT calculations show a reduced activation barrier under electronic excitation on Au(111), thus explaining the measured higher rates under visible-light irradiation.

Ferromagnetic barrier induced large enhancement of tunneling magnetoresistance in van der Waals perpendicular magnetic tunnel junctions.

van der Waals (vdW) intrinsic magnets are promising for miniaturization of devices beyond Moore's law for future energy efficient nanoelectronic devices and have been successfully used for constructing high performance vdW magnetic tunnel junctions (vdW MTJs). Here, using first principles calculations, we investigate the magnetic anisotropy, spin-dependent transport and tunneling magnetoresistance (TMR) effect of vdW MTJs formed by sandwiching a ferromagnetic (FM) monolayer CrI or non-magnetic monolayer ScI barrier between two vdW FM FeGeTe electrodes, respectively. It is found that two vdW MTJs possess strong perpendicular magnetic anisotropy.

Stacking Engineering: A Boosting Strategy for 2D Photocatalysts.

Two-dimensional (2D) photocatalytic material is a vital project for modern solar energy conversion and storage. Despite a vast family of potential 2D photocatalysts that is demonstrated, their commercial applications are severely limited because of fast photogenerated electron-hole recombination. Here, based on first-principles, we propose a general paradigm to boost the separation of photoexcited charge carriers in 2D photocatalysts by stacking engineering.

Site-Selective Deposition of Metal-Organic Frameworks on Gold Nanobipyramids for Surface-Enhanced Raman Scattering.

Site-selective deposition of metal-organic frameworks (MOFs) on metal nanocrystals has remained challenging because of the difficult control of the nucleation and growth of MOFs. Herein we report on a facile wet-chemistry approach for the selective deposition of zeolitic imidazolate framework-8 (ZIF-8) on anisotropic Au nanobipyramids (NBPs) and nanorods. ZIF-8 is selectively deposited at the ends and waist and around the entire surface of the elongated Au nanocrystals.

First-principles prediction of infrared phonon and dielectric function in biaxial hyperbolic van der Waals crystal α-MoO.

Layered biaxial hyperbolic molybdenum trioxide (α-MoO) with weak van der Waals (vdW) interlayer bonding recently received extensive attention due to its anisotropic dielectric response to infrared (IR) radiation, which couples to the lattice vibrations and allows for manipulating the radiative energy transport. However, the understanding of IR-active phonon modes and dielectric function of it has not yet been fully achieved. Here, by utilizing mode-level first-principles analysis based on density functional theory (DFT), the phonon modes contributing to the IR dielectric response of α-MoO are fully determined.

Advances in Electrochemical Ammonia Synthesis Beyond the Use of Nitrogen Gas as a Source.

Electrocatalytic reduction of dinitrogen has emerged as a new strategy for ammonia synthesis. Despite being environmentally benign and energy-saving, it suffers from low conversion efficiency and short yield of ammonia because of the challenges of activating the inert N≡N bond at room temperature and atmospheric pressure. As a result of this, researchers proposed to reduce the nitrogenous species, one category of air and water pollutants, into valuable ammonia.

Ion exchange in atomically thin clays and micas.

The physical properties of clays and micas can be controlled by exchanging ions in the crystal lattice. Atomically thin materials can have superior properties in a range of membrane applications, yet the ion-exchange process itself remains largely unexplored in few-layer crystals. Here we use atomic-resolution scanning transmission electron microscopy to study the dynamics of ion exchange and reveal individual ion binding sites in atomically thin and artificially restacked clays and micas.

Phononic Thermal Transport along Graphene Grain Boundaries: A Hidden Vulnerability.

While graphene grain boundaries (GBs) are well characterized experimentally, their influence on transport properties is less understood. As revealed here, phononic thermal transport is vulnerable to GBs even when they are ultra-narrow and aligned along the temperature gradient direction. Non-equilibrium molecular dynamics simulations uncover large reductions in the phononic thermal conductivity (κ ) along linear GBs comprising periodically repeating pentagon-heptagon dislocations.

Tracking Electron Dynamics of Single Molecules in Scanning Tunneling Microscopy Junctions with Laser Pulses.

On the basis of real-time simulations, we devise a method to extend the capability of scanning tunneling microscopy (STM) to track the electronic dynamics of molecules on a material's surface with the ultrafast temporal resolution of laser pulses. The intrinsic mechanism of visualization of electronic dynamics by measuring tunneling charge is attributed to the interference between the electronic oscillations stimulated by pump and probe pulses. The charge-transfer rate from molecule to the surrounding environment can be estimated with the decay time of electronic dynamics, which can also be detected by measuring the tunneling charge across the STM junction.

Allosteric regulation in CRISPR/Cas1-Cas2 protospacer acquisition mediated by DNA and Cas2.

Cas1 and Cas2 are highly conserved proteins across clustered-regularly-interspaced-short-palindromic-repeat-Cas systems and play a significant role in protospacer acquisition. Based on crystal structure of twofold symmetric Cas1-Cas2 in complex with dual-forked protospacer DNA (psDNA), we conducted all-atom molecular dynamics simulations to study the psDNA binding, recognition, and response to cleavage on the protospacer-adjacent-motif complementary sequence, or PAMc, of Cas1-Cas2. In the simulation, we noticed that two active sites of Cas1 and Cas1' bind asymmetrically to two identical PAMc on the psDNA captured from the crystal structure.