Origin of the Nonmonotonic Pressure Dependence of the Band Gap in the Orthorhombic Perovskite CsPbBr.

The perovskite CsPbBr exhibits an unusual nonmonotonic dependence of the band gap on increasing pressure to about 2.0 GPa as compared to conventional semiconductors. Using the first-principles calculation method, we show that under pressure, isotropic volume deformation induces considerable compression of the Pb-Br bond length and thus an enhanced interaction between atomic orbitals of the antibonding valence band maximum states and the mostly nonbonding conduction band minimum states, resulting in a monotonic decrease in the band gap.

Interface-confined intermediate phase in TiO enables efficient photocatalysis.

As a prototypical photocatalyst, TiO[Formula: see text] has been extensively studied. An interesting yet puzzling experimental fact was that P25-a mixture of anatase and rutile TiO[Formula: see text]-outperforms the individual phases; the origin of this mysterious fact, however, remains elusive. Employing rigorous first-principles calculations, here we uncover a metastable intermediate structure (MIS), which is formed due to confinement at the anatase/rutile interface.

Understanding the glassy dynamics from melting temperatures in binary glass-forming liquids.

It is natural to expect that small particles in binary mixtures move faster than large ones. However, in binary glass-forming liquids with soft-core particle interactions, we observe the counterintuitive dynamic reversal between large and small particles along with the increase of pressure by performing molecular dynamics simulations. The structural relaxation (dynamic heterogeneity) of small particles is faster (weaker) than large ones at low pressures, but becomes slower (stronger) above a crossover pressure.

Distinguishing the Geometric and Electronic Structures of Actinide Carbides AnC (An = Th, U; = 2, 3) through Exchange Interactions.

Global-minimum optimizations combined with relativistic quantum chemistry calculations have been performed to characterize the ground-state stable structures of four titled compounds and to analyze the bonding properties. ThC was identified as being a ThC-Th(C) structure, UC has been found to favor the U-U(C) structure, and both ThC and UC adopt the (AnC)-(AnC) structure. Then, the wave function analyses reveal that the interactions between the Th 7-based orbital and the σ molecular orbital of the C unit compensate for the excitation energy of 76 → 6 and lead to the stabilization of two Th(IV)s in the ThC-Th(C) structure.

Interface thermal conductivities induced by van der Waals interactions.

The interface heat transfer of two layers induced by van der Waals (vdW) contacts is theoretically investigated, based on first-principles calculations at low temperatures. The results suggest that out-of-plane acoustic phonons with low frequencies dominate the interface thermal transport due to the vdW interaction. The interface thermal conductivity is proportional to the cubic of temperature at very low temperatures, but becomes linearly proportional to temperature as temperature increases.

Discovery of novel inhibitors of histone deacetylase 6: Structure-based virtual screening, molecular dynamics simulation, enzyme inhibition and cell viability assays.

Histone deacetylase 6 (HDAC6) contributes to cancer metastasis in several cancers, including triple-negative breast cancer (TNBC)-the most lethal form that lacks effective therapy. Although several efforts have been invested to develop selective HDAC6 inhibitors, none have been approved by the FDA. Toward this goal, existing computational studies used smaller compound libraries and shorter MD simulations.

Charging Quantum Batteries via Indefinite Causal Order: Theory and Experiment.

In the standard quantum theory, the causal order of occurrence between events is prescribed, and must be definite. This has been maintained in all conventional scenarios of operation for quantum batteries. In this study we take a step further to allow the charging of quantum batteries in an indefinite causal order (ICO).

Tunneling Valley Hall Effect Driven by Tilted Dirac Fermions.

Valleytronics is a research field utilizing a valley degree of freedom of electrons for information processing and storage. A strong valley polarization is critical for realistic valleytronic applications. Here, we predict a tunneling valley Hall effect (TVHE) driven by tilted Dirac fermions in all-in-one tunnel junctions based on a two-dimensional (2D) valley material.

Moiré magnetic exchange interactions in twisted magnets.

In addition to moiré superlattices, twisting can also generate moiré magnetic exchange interactions (MMEIs) in van der Waals magnets. However, owing to the extreme complexity and twist-angle-dependent sensitivity, all existing models fail to fully capture MMEIs and thus cannot provide an understanding of MMEI-induced physics. Here, we develop a microscopic moiré spin Hamiltonian that enables the effective description of MMEIs via a sliding-mapping approach in twisted magnets, as demonstrated in twisted bilayer CrI.

Defect modeling and control in structurally and compositionally complex materials.

Conventional computational approaches for modeling defects face difficulties when applied to complex materials, mainly due to the vast configurational space of defects. In this Perspective, we discuss the challenges in calculating defect properties in complex materials, review recent advances in computational techniques and showcase new mechanistic insights developed from these methods. We further discuss the remaining challenges in improving the accuracy and efficiency of defect modeling in complex materials, and provide an outlook on potential research directions.

Controlling Charge Carrier Dynamics in Porphyrin Nanorings by Optically Active Templates.

Understanding the dynamics of photogenerated charge carriers is essential for enhancing the performance of solar and optoelectronic devices. Using atomistic quantum dynamics simulations, we demonstrate that a short π-conjugated optically active template can be used to control hot carrier relaxation, charge carrier separation, and carrier recombination in light-harvesting porphyrin nanorings. Relaxation of hot holes is slowed by 60% with an optically active template compared to that with an analogous optically inactive template.

Oxidation-induced superelasticity in metallic glass nanotubes.

Although metallic nanostructures have been attracting tremendous research interest in nanoscience and nanotechnologies, it is known that environmental attacks, such as surface oxidation, can easily initiate cracking on the surface of metals, thus deteriorating their overall functional/structural properties. In sharp contrast, here we report that severely oxidized metallic glass nanotubes can attain an ultrahigh recoverable elastic strain of up to ~14% at room temperature, which outperform bulk metallic glasses, metallic glass nanowires and many other superelastic metals hitherto reported. Through in situ experiments and atomistic simulations, we reveal that the physical mechanisms underpinning the observed superelasticity can be attributed to the formation of a percolating oxide network in metallic glass nanotubes, which not only restricts atomic-scale plastic events during loading but also leads to the recovery of elastic rigidity on unloading.

Unusual Band Gap Bowing in CsCdPbBr Alloys Due to a Chemical Mismatch.

In this work, the band structure of CsCdPbBr alloys is investigated through first-principles calculations. An unusual upward band gap bowing is revealed, which is consistent with the experimental observations of the blue-shifted gap in Cd doped CsPbBr. The gap bowing is found to be mainly contributed to by the conduction band minimum.

Poisson representation: a bridge between discrete and continuous models of stochastic gene regulatory networks.

Stochastic gene expression dynamics can be modelled either discretely or continuously. Previous studies have shown that the mRNA or protein number distributions of some simple discrete and continuous gene expression models are related by Gardiner's Poisson representation. Here, we systematically investigate the Poisson representation in complex stochastic gene regulatory networks.

Critical Phase Dualities in 1D Exactly Solvable Quasiperiodic Models.

We propose a solvable class of 1D quasiperiodic tight-binding models encompassing extended, localized, and critical phases, separated by nontrivial mobility edges. Limiting cases include the Aubry-André model and the models of Sriram Ganeshan, J. H.

Quantum Reliability.

Quantum technology has led to increasingly sophisticated and complex quantum devices. Assessing their reliability (quantum reliability) is an important issue. Although reliability theory for classical devices has been well developed in industry and technology, a suitable metric on quantum reliability and its loss has not been systematically investigated.

Dual-Level Enhanced Nonradiative Carrier Recombination in Wide-Gap Semiconductors: The Case of Oxygen Vacancy in SiO.

The conventional single-defect-mediated Shockley-Read-Hall model suggests that the nonradiative carrier recombination rate in wide-band gap (WBG) semiconductors would be negligible because the single-defect level is expected to be either far from valence-band-maximum (VBM) or conduction-band-minimum (CBM), or both. However, this model falls short of elucidating the substantial nonradiative recombination phenomena often observed experimentally across various WBG semiconductors. Owing to more localized nature of defect states inherent to WBG semiconductors, when the defect charge state changes, there is a pronounced structural relaxation around the local defect site.

Generalized Quantum Measurements on a Higher-Dimensional System via Quantum Walks.

Quantum measurements play a fundamental role in quantum mechanics. Especially, generalized quantum measurements provide a powerful and versatile tool to extract information from quantum systems. However, how to realize them on an arbitrary higher-dimensional quantum system remains a challenging task.

A machine learning approach for computation of cardiovascular intrinsic frequencies.

Analysis of cardiovascular waveforms provides valuable clinical information about the state of health and disease. The intrinsic frequency (IF) method is a recently introduced framework that uses a single arterial pressure waveform to extract physiologically relevant information about the cardiovascular system. The clinical usefulness and physiological accuracy of the IF method have been well-established via several preclinical and clinical studies.

Quantum Phase Transition in Magnetic Nanographenes on a Lead Superconductor.

Quantum spins, also known as spin operators that preserve SU(2) symmetry, lack a specific orientation in space and are hypothesized to display unique interactions with superconductivity. However, spin-orbit coupling and crystal field typically cause a significant magnetic anisotropy in d/f shell spins on surfaces. Here, we fabricate atomically precise = 1/2 magnetic nanographenes on Pb(111) through engineering sublattice imbalance in the graphene honeycomb lattice.

Wavy Two-Dimensional Conjugated Metal-Organic Framework with Metallic Charge Transport.

Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) have emerged as a new class of crystalline layered conducting materials that hold significant promise for applications in electronics and spintronics. However, current 2D c-MOFs are mainly made from organic planar ligands, whereas layered 2D c-MOFs constructed by curved or twisted ligands featuring novel orbital structures and electronic states remain less developed. Herein, we report a Cu-catecholate wavy 2D c-MOF (Cu(HFcHBC)) based on a fluorinated core-twisted contorted hexahydroxy-hexa-cata-hexabenzocoronene (HFcHBC) ligand.

Glass-like Transport Dominates Ultralow Lattice Thermal Conductivity in Modular Crystalline BiOSeCl.

Crystalline BiOSeCl exhibits record-low 0.1 W/mK lattice thermal conductivity (κ), but the underlying transport mechanism is not yet understood. Using a theoretical framework which incorporates first-principles anharmonic lattice dynamics into a unified heat transport theory, we compute both the particle-like and glass-like components of κ in crystalline and pellet BiOSeCl forms.

Non-homogeneous pairing in disordered two-orbital s-wave superconductors.

We investigate the effects of non-magnetic disorder in a hybridized two-dimensional two-orbital s-wave superconductor (SC) model. The situation in which electronic orbitals overlap such that the hybridizationVi,jamong them is antisymmetric, under inversion symmetry, was taken into account. The on-site disorder is given by a random impurity potential.