Material Physics Center

Wannier90 is an open-source computer program for calculating maximally-localised Wannier functions (MLWFs) from a set of Bloch states. It is interfaced to many widely used electronic-structure codes thanks to its independence from the basis sets representing these Bloch states. In the past few years the development of Wannier90 has transitioned to a community-driven model; this has resulted in a number of new developments that have been recently released in Wannier90 v3.0. In this article we describe these new functionalities, that include the implementation of new features for wannierisation and disentanglement (symmetry-adapted Wannier functions, selectively-localised Wannier functions, selected columns of the density matrix) and the ability to calculate new properties (shift currents and Berry-curvature dipole, and a new interface to many-body perturbation theory); performance improvements, including parallelisation of the core code; enhancements in functionality (support for spinor-valued Wannier functions, more accurate methods to interpolate quantities in the Brillouin zone); improved usability (improved plotting routines, integration with high-throughput automation frameworks), as well as the implementation of modern software engineering practices (unit testing, continuous integration, and automatic source-code documentation). These new features, capabilities, and code development model aim to further sustain and expand the community uptake and range of applicability, that nowadays spans complex and accurate dielectric, electronic, magnetic, optical, topological and transport properties of materials.

This critical review presents the state of the art research progress, proposes strategies to improve the conductivity of solid electrolytes, discusses the chemical and electrochemical stabilities, and uncovers future perspectives for solid state batteries.

The physics of one-dimensional interacting bosonic systems is reviewed. Beginning with results from exactly solvable models and computational approaches, the concept of bosonic Tomonaga-Luttinger liquids relevant for one-dimensional Bose fluids is introduced, and compared with Bose-Einstein condensates existing in dimensions higher than one. The effects of various perturbations on the Tomonaga-Luttinger liquid state are discussed as well as extensions to multicomponent and out of equilibrium situations. Finally, the experimental systems that can be described in terms of models of interacting bosons in one dimension are discussed.

Here, we report advanced materials and devices that enable high-efficiency mechanical-to-electrical energy conversion from the natural contractile and relaxation motions of the heart, lung, and diaphragm, demonstrated in several different animal models, each of which has organs with sizes that approach human scales. A cointegrated collection of such energy-harvesting elements with rectifiers and microbatteries provides an entire flexible system, capable of viable integration with the beating heart via medical sutures and operation with efficiencies of ∼2%. Additional experiments, computational models, and results in multilayer configurations capture the key behaviors, illuminate essential design aspects, and offer sufficient power outputs for operation of pacemakers, with or without battery assist.

Research efforts in the past two decades have resulted in thousands of potential application areas for nanoparticles - which materials have become industrially relevant? Where are sustainable applications of nanoparticles replacing traditional processing and materials? This tutorial review starts with a brief analysis on what makes nanoparticles attractive to chemical product design. The article highlights established industrial applications of nanoparticles and then moves to rapidly emerging applications in the chemical industry and discusses future research directions. Contributions from large companies, academia and high-tech start-ups are used to elucidate where academic nanoparticle research has revolutionized industry practice. A nanomaterial-focused analysis discusses new trends, such as particles with an identity, and the influence of modern instrument advances in the development of novel industrial products.

Nanoshell arrays have recently been found to possess ideal properties as a substrate for combining surface enhanced raman scattering (SERS) and surface enhanced infrared absorption (SEIRA) spectroscopies, with large field enhancements at the same spatial locations on the structure. For small interparticle distances, the multipolar plasmon resonances of individual nanoshells hybridize and form red-shifted bands, a relatively narrow band in the near-infrared (NIR) originating from quadrupolar nanoshell resonances enhancing SERS, and a very broadband in the mid-infrared (MIR) arising from dipolar resonances enhancing SEIRA. The large field enhancements in the MIR and at longer wavelengths are due to the lightning-rod effect and are well described with an electrostatic model.

A novel Zn/Co zeolitic imidazolate framework (ZIF) has been constructed which demonstrates better gas adsorption (CO₂, CH₄ and N₂) and catalytic (CO₂ conversion) properties compared with ZIF-8 and ZIF-67.

On-surface synthesis is appearing as an extremely promising research field aimed at creating new organic materials. A large number of chemical reactions have been successfully demonstrated to take place directly on surfaces through unusual reaction mechanisms. In some cases the reaction conditions can be properly tuned to steer the formation of the reaction products. It is thus possible to control the initiation step of the reaction and its degree of advancement (the kinetics, the reaction yield); the nature of the reaction products (selectivity control, particularly in the case of competing processes); as well as the structure, position, and orientation of the covalent compounds, or the quality of the as-formed networks in terms of order and extension. The aim of our review is thus to provide an extensive description of all tools and strategies reported to date and to put them into perspective. We specifically define the different approaches available and group them into a few general categories. In the last part, we demonstrate the effective maturation of the on-surface synthesis field by reporting systems that are getting closer to application-relevant levels thanks to the use of advanced control strategies.

For atomic thin layer insulating materials we provide an exact analytic form of the two-dimensional (2D) screened potential. In contrast to three-dimensional systems where the macroscopic screening can be described by a static dielectric constant, in 2D systems the macroscopic screening is nonlocal ($q$ dependent) showing a logarithmic divergence for small distances and reaching the unscreened Coulomb potential for large distances. The crossover of these two regimes is dictated by 2D layer polarizability that can be easily computed by standard first-principles techniques. The present results have strong implications for describing gap-impurity levels and also exciton binding energies. The simple model derived here captures the main physical effects and reproduces well, for the case of graphane, the full many-body $\mathrm{GW}$ plus Bethe-Salpeter calculations. As an additional outcome we show that the impurity hole-doping in graphane leads to strongly localized states, which hampers applications in electronic devices. In spite of the inefficient and nonlocal two-dimensional macroscopic screening we demonstrate that a simple $\mathbf{k}\ifmmode\cdot\else\textperiodcentered\fi{}\mathbf{p}$ approach is capable to describe the electronic and transport properties of confined 2D systems.

Observing the intricate chemical transformation of an individual molecule as it undergoes a complex reaction is a long-standing challenge in molecular imaging. Advances in scanning probe microscopy now provide the tools to visualize not only the frontier orbitals of chemical reaction partners and products, but their internal covalent bond configurations as well. We used noncontact atomic force microscopy to investigate reaction-induced changes in the detailed internal bond structure of individual oligo-(phenylene-1,2-ethynylenes) on a (100) oriented silver surface as they underwent a series of cyclization processes. Our images reveal the complex surface reaction mechanisms underlying thermally induced cyclization cascades of enediynes. Calculations using ab initio density functional theory provide additional support for the proposed reaction pathways.

Using density functional theory and Monte Carlo calculations, we study the thickness dependence of the magnetic and electronic properties of a van der Waals interlayer antiferromagnet in the two-dimensional limit. Considering MnBi_{2}Te_{4} as a model material, we find it to demonstrate a remarkable set of thickness-dependent magnetic and topological transitions. While a single septuple layer block of MnBi_{2}Te_{4} is a topologically trivial ferromagnet, the thicker films made of an odd (even) number of blocks are uncompensated (compensated) interlayer antiferromagnets, which show wide band gap quantum anomalous Hall (zero plateau quantum anomalous Hall) states. Thus, MnBi_{2}Te_{4} is the first stoichiometric material predicted to realize the zero plateau quantum anomalous Hall state intrinsically. This state has been theoretically shown to host the exotic axion insulator phase.

Water oxidation activity of nickel–iron layered double hydroxide ([NiFe]-LDH) nanosheet electrocatalysts is a function of interlayer anion basicity.

A prerequisite for future graphene nanoribbon (GNR) applications is the ability to fine-tune the electronic band gap of GNRs. Such control requires the development of fabrication tools capable of precisely controlling width and edge geometry of GNRs at the atomic scale. Here we report a technique for modifying GNR band gaps via covalent self-assembly of a new species of molecular precursors that yields n = 13 armchair GNRs, a wider GNR than those previously synthesized using bottom-up molecular techniques. Scanning tunneling microscopy and spectroscopy reveal that these n = 13 armchair GNRs have a band gap of 1.4 eV, 1.2 eV smaller than the gap determined previously for n = 7 armchair GNRs. Furthermore, we observe a localized electronic state near the end of n = 13 armchair GNRs that is associated with hydrogen-terminated sp(2)-hybridized carbon atoms at the zigzag termini.

This review focuses on state-of-the-art solutions and strategies for MOF/polymer interface issues in mixed matrix membranes.

A review of the present status, recent enhancements, and applicability of the Siesta program is presented. Since its debut in the mid-1990s, Siesta's flexibility, efficiency, and free distribution have given advanced materials simulation capabilities to many groups worldwide. The core methodological scheme of Siesta combines finite-support pseudo-atomic orbitals as basis sets, norm-conserving pseudopotentials, and a real-space grid for the representation of charge density and potentials and the computation of their associated matrix elements. Here, we describe the more recent implementations on top of that core scheme, which include full spin-orbit interaction, non-repeated and multiple-contact ballistic electron transport, density functional theory (DFT)+U and hybrid functionals, time-dependent DFT, novel reduced-scaling solvers, density-functional perturbation theory, efficient van der Waals non-local density functionals, and enhanced molecular-dynamics options. In addition, a substantial effort has been made in enhancing interoperability and interfacing with other codes and utilities, such as wannier90 and the second-principles modeling it can be used for, an AiiDA plugin for workflow automatization, interface to Lua for steering Siesta runs, and various post-processing utilities. Siesta has also been engaged in the Electronic Structure Library effort from its inception, which has allowed the sharing of various low-level libraries, as well as data standards and support for them, particularly the PSeudopotential Markup Language definition and library for transferable pseudopotentials, and the interface to the ELectronic Structure Infrastructure library of solvers. Code sharing is made easier by the new open-source licensing model of the program. This review also presents examples of application of the capabilities of the code, as well as a view of on-going and future developments.

Plasmonic nanoparticle pairs known as "dimers" embody a simple system for generating intense nanoscale fields for surface enhanced spectroscopies and for developing an understanding of coupled plasmons. Individual nanoshell dimers in directly adjacent pairs and touching geometries show dramatically different plasmonic properties. At close distances, hybridized plasmon modes appear whose energies depend extremely sensitively on the presence of a small number of molecules in the interparticle junction. When touching, a new plasmon mode arising from charge transfer oscillations emerges. The extreme modification of the overall optical response due to minute changes in very reduced volumes opens up new approaches for ultrasensitive molecular sensing and spectroscopy.

Wannier90 is an open-source computer program for calculating maximally-localised Wannier functions (MLWFs) from a set of Bloch states. It is interfaced to many widely used electronic-structure codes thanks to its independence from the basis sets representing these Bloch states. In the past few years the development of Wannier90 has transitioned to a community-driven model; this has resulted in a number of new developments that have been recently released in Wannier90 v3.0. In this article we describe these new functionalities, that include the implementation of new features for wannierisation and disentanglement (symmetry-adapted Wannier functions, selectively-localised Wannier functions, selected columns of the density matrix) and the ability to calculate new properties (shift currents and Berry-curvature dipole, and a new interface to many-body perturbation theory); performance improvements, including parallelisation of the core code; enhancements in functionality (support for spinor-valued Wannier functions, more accurate methods to interpolate quantities in the Brillouin zone); improved usability (improved plotting routines, integration with high-throughput automation frameworks), as well as the implementation of modern software engineering practices (unit testing, continuous integration, and automatic source-code documentation). These new features, capabilities, and code development model aim to further sustain and expand the community uptake and range of applicability, that nowadays spans complex and accurate dielectric, electronic, magnetic, optical, topological and transport properties of materials.

In this review, we have portrayed the structure, synthesis and applications of a variety of biomimetic MOFs from an unprecedented angle. Synthetic MOF analogues of five distinct enzymes: phosphotriesterase, hydrogenase, cytochrome P450, chymotrypsin and carbonic anhydrase, have been discussed with their skeletal comparison to actual enzymatic active sites as reference, and an explanation of catalytic pathways from the mechanistic cycle of the corresponding enzymes is depicted. We demonstrated critically each of the five discrete situations by assimilating available benchmark researches in an attempt to provide a concise literature source on the ingenious design strategies and versatile biomimetic applications of this domain of materials.

This review of design and operating conditions of electrochemical CO₂reduction covers electrolytes, electrodes, reactors, temperature, pressure, and pH effects.

A covalently-bonded atom typically has a region of lower electronic density, a "σ-hole," on the side of the atom opposite to the bond, along its extension. There is frequently a positive electrostatic potential associated with this region, through which the atom can interact attractively but noncovalently with negative sites. This positive potential reflects not only the lower electronic density of the σ-hole but also contributions from other portions of the molecule. These can significantly influence both the value and also the angular position of the positive potential, causing it to deviate from the extension of the covalent bond. We have surveyed these effects, and their consequences for the directionalities of subsequent noncovalent intermolecular interactions, for atoms of Groups IV-VII. The overall trends are that larger deviations of the positive potential result in less linear intermolecular interactions, while smaller deviations lead to more linear interactions. We find that the deviations of the positive potentials and the nonlinearities of the noncovalent interactions tend to be greatest for atoms of Groups V and VI. We also present arguments supporting the use of the 0.001 a.u. contour of the electronic density as the molecular surface on which to compute the electrostatic potential.