Finite-Time Thermodynamics and Complex Energy Landscapes: A Perspective.

Finite-time thermodynamics (FTT) describes the study of thermodynamic processes that take place in finite time. Due to the finite-time requirement, in general the system cannot move from equilibrium state to equilibrium state. As a consequence, excess entropy is generated, available work is reduced, and/or the maximally achievable efficiency is not achieved; minimizing these negative side-effects constitutes an optimal control problem.

Hierarchical access to encoded data on DNA nanostructures using administrator and user keys.

DNA nanotechnology has shown great potential for molecular information encoding and controlled access. With the remarkable progress of DNA data storage systems, it is imperative to develop DNA-based hierarchical access techniques to manage user data. However, to our knowledge, this aspect has yet to be fully explored.

Revisiting the Hydration and Dehydration Behavior of and : Crystal Structure Determination of an Intermediate Hydrated Phase.

Lithium indium chloride, LiInCl, is a promising solid-state electrolyte for all-solid-state batteries (ASSBs) due to its high room-temperature ionic conductivity and electrochemical stability. However, its sensitivity to atmospheric moisture leads to the formation of stable crystalline hydrates, which significantly affect both its electrochemical performance and crystal chemistry. In this study, temperature- and time-dependent X-ray diffraction was employed to investigate the underlying mechanisms governing the hydration and dehydration processes of LiInCl and its hydrated counterpart, LiInClHO ( > 2), by monitoring the associated structural transformations.

Deterministic optimization of Jastrow factors.

Highly flexible Jastrow factors have found significant use in stochastic electronic structure methods such as variational Monte Carlo (VMC) and diffusion Monte Carlo, as well as in quantum chemical transcorrelated (TC) approaches, which have recently seen great success in generating highly accurate electronic energies using moderately sized basis sets. In particular, for the latter, the intrinsic noise in the Jastrow factor due to its optimization by VMC can pose a problem, especially when targeting weak (non-covalent) interactions. In this paper, we propose a deterministic alternative to VMC Jastrow optimization, based on minimizing the "variance of the TC reference energy" in a standard basis set.

Aperiodic defects in periodic solids.

To date, computational methods for modeling defects (vacancies, adsorbates, etc.) have relied on periodic supercells in which the defect is far enough from its repeated image that they can be assumed non-interacting. Yet, the relative proximity and periodic repetition of the defect's images may lead to spurious, unphysical artifacts, especially if the defect is charged and/or open-shell, causing a very slow convergence to the thermodynamic limit (TDL).

Nonlinear Optical Response in Layer-Stacked Gallenene with Ferroelectric Polarization.

Polar metals are very rare and challenging to realize due to the incompatibility of ferroelectricity and metallicity. Mobile electrons in polar metals effectively screen the static electric field and dipoles. Recent studies show that 2D van der Waals metals without an inversion center can have polar order due to specific layer stacking.

Substrate-Controlled Response Coefficients in Thin Films.

To obtain materials with desired properties, material compositions are primarily altered, whereas thin films offer additional unique avenues. By combining state-of-the-art first-principles calculations and experimental investigations of thin films of strontium titanate as an exemplary representative of a broad class of perovskite oxides and the extensive family of ferroelectrics, a novel approach is presented to achieving superior material responses to external stimuli. The findings reveal that substrate-imposed deformations, or strains, significantly alter the frequencies and magnitudes of atomic vibrations in thin films.

Long Used but Hardly Known: Synthesis and Crystal Structure of Tritium Breeding LiBeO.

A main challenge for the operation of a nuclear fusion reactor is the consumption of tritium during the fusion process and the limited availability of tritium in natural resources or its production in nuclear power plants. The most promising approach is breeding of new tritium within the operating fusion reactor. For this purpose, suitable breeding materials are needed.

Tensor decomposed distinguishable cluster. I. Triples decomposition.

We present a cost-reduced approach for the distinguishable cluster approximation to coupled cluster with singles, doubles, and iterative triples (DC-CCSDT) based on a tensor decomposition of the triples amplitudes. The triples amplitudes and residuals are processed in the singular-value-decomposition (SVD) basis. Truncation of the SVD basis according to the values of the singular values together with the density fitting (or Cholesky) factorization of the electron repulsion integrals reduces the scaling of the method to N6, and the DC approximation removes the most expensive terms of the SVD triples residuals and at the same time improves the accuracy of the method.

Non-equilibrium anti-Stokes Raman spectroscopy for investigating Higgs modes in superconductors.

Even before its role in electroweak symmetry breaking, the Anderson-Higgs mechanism was introduced to explain the Meissner effect in superconductors. Spontaneous symmetry-breaking yields massless phase modes representing the low-energy excitations of the Mexican-Hat potential. Only in superconductors the phase mode is shifted towards higher energies owing to the gauge field of the charged condensate.

A Dynamically Induced Phase Transition in NaPS─Ultrafast Na Mobility Triggering Rotor Phase Formation.

The physical properties of any crystalline solid, such as the irregular movement of ions or atoms, are closely linked to its structure. Changes in local structure or local defect chemistry are typically attributed to changes in ion hopping. Conversely, one might also ask whether fast ionic diffusion can cause structural changes, finally initiating an overall phase transition.

Stabilization of the garnet lattice by silicon incorporation in polycrystalline katoite.

Polycrystalline single-phase bulk hydrogrossulars (CaAl(SiO)(OH) (0 ≤ ≤ 3)) of various compositions were synthesized for the first time utilizing hydrothermal treatment at 200 °C of the phyllosilicate strätlingite (CaAlSiO(OH)·2.25HO) in its mother liquor. The reproducibility of previously reported synthetic methods for both Si-free katoite and hydrogrossulars was evaluated.

DNA moiré superlattices.

Moiré superlattices have been extensively designed and implemented in atomic-scale van der Waals systems and submicrometre-scale photonic systems. However, bridging the structural gap between these scales has remained a substantial challenge. Here we demonstrate engineered DNA moiré superlattices with sublattice constants as small as ~2 nm and moiré periodicities spanning tens of nanometres.

Enhanced Photothermal Conversion through 2D/0D Nano-Heterojunction Engineering for Highly Efficient Solar Desalination.

Two-dimensional (2D) materials are promising candidates for solar-driven desalination. However, conventional photothermal 2D materials like transition metal carbides and nitrides (MXenes) as well as transition metal dichalcogenides (TMDs) suffer from major limitations such as their complex synthesis and low photothermal conversion efficiency. In contrast, metal phosphorus trichalcogenides (MPCh) do not display the same drawbacks and possess widely tunable bandgaps (1.

Coulomb blockade thermometry based nanocalorimetry.

Specific heat is a powerful probe offering insights into the entropy and excitation spectrum of the studied material. While it is well established, a key challenge remains the measurement of microcrystals or thin films, especially in the sub-Kelvin, high magnetic field regime. Here, we present a setup combining the high sensitivity of SiNx membrane based calorimetry with the absolute accuracy of Coulomb blockade thermometry to realize a nanocalorimeter for such tasks.

CO and HO Sorption Induced Bulk-Phase Changes of CALF-20 Captured Using Laboratory X-ray Powder Diffraction.

The zinc oxalate (ox) triazolate (trz)-based MOF, Calgary Framework 20 (CALF-20), exhibits remarkable cycling stability for carbon dioxide and water adsorption and desorption and is therefore a promising candidate material for CO sequestration on an industrial scale. Upon gas and vapor loading and unloading, the MOF shows pronounced structural dynamics leading to a variety of potential CALF-20 polymorphs. A systematic study on CO and HO ad- and desorption using high-resolution, laboratory X-ray powder diffraction (XRPD) shows that the CO-breathing behavior changes upon gas loading.

Dynamic breathing behaviour of the titanium-based metal-organic framework NTU-9 upon adsorption of water and organic solvents.

Understanding the structural response of framework materials to external stimuli has been of great interest. However, little is known about the stimuli responsiveness of titanium-based metal-organic frameworks. We investigate the reproducibility of the synthesis of the two-dimensional metal-organic framework NTU-9 (NTU = Nanyang Technological University) composed of Ti cations and 2,5-dihydroxyterephtalate as the organic linker and the flexible response of the framework structure to external stimuli.

Isotopologue-induced structural dynamics of a triazolate metal-organic framework for efficient hydrogen isotope separation.

Efficient hydrogen isotope separation remains the biggest challenge due to the nearly identical physicochemical properties of H and D. Through in situ neutron powder diffraction and gas adsorption experiments, we investigate the hydrogen isotopologue-induced structural dynamics of the triazole-based metal-organic framework [Mn(ta)]. Gas loading induces a measurable lattice expansion, more pronounced for H than D, and two distinct adsorption sites are identified with a subtle but significant difference in the occupancy of H and D at 60 K.

Identifying Bottlenecks in the Photocatalytic Oxygen Evolution Reaction with Covalent Organic Frameworks.

Covalent organic frameworks (COFs) have emerged as promising semiconducting materials for photocatalytic applications due to their large surface area, high crystallinity, and vast synthetic tunability. This is especially noticeable in the context of photocatalytic water splitting, where many COFs have been employed for the hydrogen evolution half-reaction. There, sacrificial reagents typically replace the kinetically demanding oxygen evolution half-reaction.

The influence of public policy and administration expertise on policy: an empirical study.

Academic expertise is a key pillar of governance processes around the world. A goal of policy and public sector actors is to draw on research to improve decision making, and correspondingly, a goal of public policy and public administration researchers is to provide relevant expertise. It is not clear, however, to what extent these goals are achieved.

Localized Spin Textures Stabilized by Geometry-Induced Strain in 2D Magnet FeGeTe.

Strain engineering promises to enable manipulation and control of the properties of exfoliated flakes of 2D van der Waals (vdW) ferromagnets for spintronic applications. However, while previous studies of strain effects have focused on global properties, the impact on local magnetic spin textures remains unexplored. Here, manipulation of magnetism in the 2D ferromagnet FeGeTe (FGT) is demonstrated using geometry-induced strain.

Deformed One-Dimensional Covalent Organic Polymers for Enhanced CO Electroreduction to Methanol.

Spatially arranged molecular catalysts in polymeric frameworks, typically in a layered structure, are emerging strategies to mitigate the molecular aggregation and improve the catalytic performance. However, the effect of local coordination induced by polymerization remains underexplored. Here, we develop one-dimensional cobalt-tetra-amino-phthalocyanine-based covalent organic polymers (1D-COP) for the electrochemical CO reduction reaction (CORR).

Combining Fast Exploration with Accurate Reweighting in the OPES-eABF Hybrid Sampling Method.

On-the-fly probability enhanced sampling (OPES) has recently been introduced [Invernizzi, M.; Parrinello, M. 2022, 18, 3988-3996], with important improvements over the highly popular metadynamics methods.