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Water (H2O) ice is ubiquitous component of the universe, having been detected in a variety of interstellar and Solar System environments where radiation plays an important role in its physico-chemical transformations. Although the radiation chemistry of H2O astrophysical ice analogues has been well studied, direct and systematic comparisons of different solid phases are scarce and are typically limited to just two phases. In this article, we describe the results of an in-depth study of the 2 keV electron irradiation of amorphous solid water (ASW), restrained amorphous ice (RAI) and the cubic (Ic) and hexagonal (Ih) crystalline phases at 20 K so as to further uncover any potential dependence of the radiation physics and chemistry on the solid phase of the ice. Mid-infrared spectroscopic analysis of the four investigated H2O ice phases revealed that electron irradiation of the RAI, Ic, and Ih phases resulted in their amorphization (with the latter undergoing the process more slowly) while ASW underwent compaction. The abundance of hydrogen peroxide (H2O2) produced as a result of the irradiation was also found to vary between phases, with yields being highest in irradiated ASW. This observation is the cumulative result of several factors including the increased porosity and quantity of lattice defects in ASW, as well as its less extensive hydrogen-bonding network. Our results have astrophysical implications, particularly with regards to H2O-rich icy interstellar and Solar System bodies exposed to both radiation fields and temperature gradients., Published in the European Physical Journal D: Atomic, Molecular, Optical, and Plasma Physics

Lithium-ion batteries, comprising nanoparticulate Ni–Mn–Co (NMC) cathodes that have been used to power electric vehicles, can be improved by blending NMC with Li–Mn–O (LMO). However, LMO undergoes a cubic to tetragonal phase change during charge cycling, which cracks and pulverizes the material, resulting in capacity fading. Structural characterization during the phase transition is the first step in mitigating capacity fading and can be challenging experimentally and computationally. Here, we use simulated amorphization and crystallization to generate atom-level models of the LMO nanoparticles. This simulation strategy does not require any structural information to be predetermined. Instead, the structures evolve “naturally” from amorphous precursors. Analysis of the model Li–Mn–O nanoparticles reveals that they comprise domains of defect-rich spinel, Mn\(_3\)O\(_4\), layered Li\(_2\)MnO\(_3\), and lithium-rich spinel Li\(_{1+x}\)Mn\(_{2–x}\)O\(_4\) phases together with complex microstructural features. The discharge process was modeled by inserting surplus lithium atoms into the nanoparticles, resulting in structural changes, accompanied by a variety of constituent polymorphs. A transitional multigrained structure, between the cubic (Li\(_1\)Mn\(_2\)O\(_4\)) and tetragonal (Li\(_2\)Mn\(_2\)O\(_4\)) phases, is observed at Li\(_{1.75}\)Mn\(_2\)O\(_4\). We also find that microstructural features, such as microtwinning and intrinsic dopants, vacancies, etc., result in a network of Li transport pathways, enabling Li mobility in all three spatial directions.

Recent μSR measurements revealed remarkable signatures of spontaneous magnetism coexisting with superconductivity in elemental rhenium. Thus, pure rhenium could be the first elemental crystal where unconventional superconductivity is realized in nature. Here we provide a quantitative theory that uncovers the nature of the superconducting instability by incorporating every details of the electronic structure together with spin-orbit coupling and multiorbital physics. We show that conventional s-wave superconductivity combined with strong spin-orbit coupling is inducing even-parity odd-orbital spin triplet Cooper pairs, and in presence of a screw-axis Cooper pairs' migration between the induced equal-spin triplet component leads to an exotic magnetic state with atomic-scale texture. Our first-principles-based model contains two phenomenological parameters that characterizes the pairing interaction fixed by the experimental value of the superconducting transition temperature and the slope of the specific heat, and allows quantitative prediction of the magnetic structure., G.Cs. acknowledges support from the European Union’s Horizon 2020 research and innovation program under the Marie Sklodowska-Curie Grant Agreement No. 754510 and thanks Aline Ramires for fruitful discussions. B.U. acknowledges for the support of NKFIH K131938 and BME Nanotechnology FIKP grants. This research was supported by EPSRC through the project “Unconventional Superconductors: New paradigms for new materials” (Grants No. EP/P00749X/1 and No. EP/P007392/1).

When the transition temperature of a continuous phase transition is tuned to absolute zero, new ordered phases and physical behaviour emerge in the vicinity of the resulting quantum critical point. Sr3Ru2O7 can be tuned through quantum criticality with magnetic field at low temperature. Near its critical field Bc it displays the hallmark T-linear resistivity and a \documentclass[12pt]{minimal} \usepackage{amsmath} \usepackage{wasysym} \usepackage{amsfonts} \usepackage{amssymb} \usepackage{amsbsy} \usepackage{mathrsfs} \usepackage{upgreek} \setlength{\oddsidemargin}{-69pt} \begin{document}$$T\,{{{{{{\mathrm{log}}}}}}}\,(1/T)$$\end{document}Tlog(1/T) electronic heat capacity behaviour of strange metals. However, these behaviours have not been related to any critical fluctuations. Here we use inelastic neutron scattering to reveal the presence of collective spin fluctuations whose relaxation time and strength show a nearly singular variation with magnetic field as Bc is approached. The large increase in the electronic heat capacity and entropy near Bc can be understood quantitatively in terms of the scattering of conduction electrons by these spin-fluctuations. On entering the spin-density-wave ordered phase present near Bc, the fluctuations become stronger suggesting that the order is stabilised through an “order-by-disorder” mechanism., Sr3Ru2O7 exhibits a quantum critical point tunable by magnetic field and has been widely used in the study of criticality. Here, by using inelastic neutron scattering, the authors measure collective magnetic excitations near the quantum critical point and relate them to thermodynamic properties and spin density wave order.

We propose a superconducting instability where microscopic supercurrent loops form spontaneously within a unit cell at the superconducting transition temperature with only uniform, onsite and intra-orbital singlet pairing. As a result of the circulating currents time-reversal symmetry is spontaneously broken in the superconducting state. Using Ginzburg-Landau theory, we describe in detail how these currents emerge in a toy model. We discuss the crystallographic symmetry requirements to realize such a state and show that they are met by the Re6X (X=Zr, Hf, Ti) family of time-reversal symmetry breaking, but otherwise seemingly conventional, superconductors. We estimate an upper bound for the resulting internal fields and find it to be consistent with recent muon-spin relaxation experiments., Comment: 10 pages, 3 figures (More references added)

The Hofstadter model is a popular choice for theorists investigating the fractional quantum Hall effect on lattices, due to its simplicity, infinite selection of topological flat bands, and increasing applicability to real materials. In particular, fractional Chern insulators in bands with Chern number $|C|>1$ can demonstrate richer physical properties than continuum Landau level states and have recently been detected in experiments. Motivated by this, we examine the stability of fractional Chern insulators with higher Chern number in the Hofstadter model, using large-scale infinite density matrix renormalization group simulations on a thin cylinder. We confirm the existence of fractional states in bands with Chern numbers $C=1,2,3,4,5$ at the filling fractions predicted by the generalized Jain series [Phys. Rev. Lett. 115, 126401 (2015)]. Moreover, we discuss their metal-to-insulator phase transitions, as well as the subtleties in distinguishing between physical and numerical stability. Finally, we comment on the relative suitability of fractional Chern insulators in higher Chern number bands for proposed modern applications., 16 pages, 13 figures

We present a theoretical study of the potential of Principal Component Analysis to analyse magnetic diffuse neutron scattering data on quantum materials. To address this question, we simulate the scattering function $S\left(\mathbf{q}\right)$ for a model describing a cluster magnet with anisotropic spin-spin interactions under different conditions of applied field and temperature. We find high dimensionality reduction and that the algorithm can be trained with surprisingly small numbers of simulated observations. Subsequently, observations can be projected onto the reduced-dimensionality space defined by the learnt principal components. Constant-field temperature scans corresponds to trajectories in this space which show characteristic bifurcations at the critical fields corresponding to ground-state phase boundaries. Such plots allow the ground-state phase diagram to be accurately determined from finite-temperature measurements., 12 pages, 9 figures; author's accepted version with improved discussions and additional appendices

Increased demand for lithium products for use in lithium-ion batteries has led to a search for new lithium resources in recent years to meet projected future consumption. One potential lithium resource is low lithium bearing brines that are discharged from hydraulically fractured oil and gas wells as flowback and produced water (FPW). In this way, hydraulic fracturing presents an opportunity to turn what is normally considered wastewater into a lithium resource. In this research, two manganese-based lithium-selective adsorbents were prepared using a co-precipitation method and were employed for lithium recovery from FPW. At optimized conditions, lithium uptake reached 18 mg g−1, with a > 80% lithium recovery within 30 min. The recovered lithium was isolated and concentrated to 15 mM in an acidic final product. The degree of sorbent loss during acid desorption of lithium was significantly higher for sorbents used in the FPW as compared to recovery from a synthetic lithium-bearing brine (4.5% versus 0.8%). Thus, we propose that organic molecules present in the FPW reduce manganese in the sorbent structure during lithium sorption, leading to increased sorbent loss through reductive dissolution. Systematic characterization including wet chemical manganese valence measurements, along with EXAFS, XPS, and TEM-EELS show that exposure to FPW causes tetravalent manganese in the bulk sorbent structure to be reduced during lithium sorption, which subsequently dissolves during acid desorption. Partial removal of these organic molecules by nanofiltration leads to decreased sorbent dissolution in acid. In this way, we show that dissolved organic molecules represent a critical control on the reductive dissolution of manganese-based lithium ion exchange sorbents. This research provides promising results on the use of manganese-based lithium sorbents in FPW.

Platinum functions exceptionally well as a nanoparticulate catalyst in many important fields, such as in the removal of atmospheric pollutants, but it is scarce, expensive and not always sufficiently durable. Here, we report a perovskite system in which 0.5 wt% Pt is integrated into the support and its subsequent conversion through exsolution to achieve a resilient catalyst. Owing to the instability of most Pt oxides at high temperatures, a thermally stable platinum oxide precursor, barium platinate, was used to preserve the platinum as an oxide during the solid-state synthesis in an approach akin to the Trojan horse legend. By tailoring the procedure, it is possible to produce a uniform equilibrated structure with active emergent Pt nanoparticles strongly embedded in the perovskite surface that display better CO oxidation activity and stability than those of conventionally prepared Pt catalysts. This catalyst was further evaluated for a variety of reactions under realistic test environments—CO and NO oxidation, diesel oxidation catalysis and ammonia slip reactions were investigated. Nanoparticulate platinum is a highly active catalyst, but it is scarce, expensive and not always sufficiently durable. Now, barium platinate has been used as a vehicle to preserve platinum as an oxide during the solid-state synthesis of a Pt-doped titanate perovskite; this enables the production of a structure with active and stable Pt nanoparticles on the perovskite surface that catalyses CO oxidation.

In recent years, Artificial Intelligence techniques have proved to be very successful when applied to problems in physical sciences. Here we apply an unsupervised Machine Learning (ML) algorithm called Principal Component Analysis (PCA) as a tool to analyse the data from muon spectroscopy experiments. Specifically, we apply the ML technique to detect phase transitions in various materials. The measured quantity in muon spectroscopy is an asymmetry function, which may hold information about the distribution of the intrinsic magnetic field in combination with the dynamics of the sample. Sharp changes of shape of asymmetry functions - measured at different temperatures - might indicate a phase transition. Existing methods of processing the muon spectroscopy data are based on regression analysis, but choosing the right fitting function requires knowledge about the underlying physics of the probed material. Conversely, Principal Component Analysis focuses on small differences in the asymmetry curves and works without any prior assumptions about the studied samples. We discovered that the PCA method works well in detecting phase transitions in muon spectroscopy experiments and can serve as an alternative to current analysis, especially if the physics of the studied material are not entirely known. Additionally, we found out that our ML technique seems to work best with large numbers of measurements, regardless of whether the algorithm takes data only for a single material or whether the analysis is performed simultaneously for many materials with different physical properties., Comment: 11 pages, 7 figures, to be submitted to the Journal of Physics: Condensed Matter special issue on "Machine Learning in Condensed Matter Physics"

Chiral superconductors are novel topological materials with finite angular momentum Cooper pairs circulating around a unique chiral axis, thereby spontaneously breaking time-reversal symmetry. They are rather scarce and usually feature triplet pairing: a canonical example is the chiral p-wave state realized in the A-phase of superfluid He3. Chiral triplet superconductors are, however, topologically fragile with the corresponding gapless boundary modes only weakly protected against symmetry-preserving perturbations in contrast to their singlet counterparts. Using muon spin relaxation measurements, here we report that the weakly correlated pnictide compound LaPt3P has the two key features of a chiral superconductor: spontaneous magnetic fields inside the superconducting state indicating broken time-reversal symmetry and low temperature linear behaviour in the superfluid density indicating line nodes in the order parameter. Using symmetry analysis, first principles band structure calculation and mean-field theory, we unambiguously establish that the superconducting ground state of LaPt3P is a chiral d-wave singlet., Nature Communications, 12 (1), ISSN:2041-1723

Recent nuclear magnetic resonance experiments measuring the Knight shift in Sr2RuO4 have challenged the widely accepted picture of chiral pairing in this superconductor. Here we study the implications of helical pairing on the superconducting state while comparing our results with the available experimental data on the upper critical field and Knight shift. We solve the Bogoliubov–de Gennes equation employing a realistic three-dimensional tight-binding model that captures the experimental Fermi surface very well. In agreement with experiments we find a Pauli limiting to the upper critical field and, at low temperatures and high fields, a second superconducting transition. These transitions, which form a superconducting subphase in the H-T phase diagram are first-order in nature and merge into a single second-order transition at a bicritical point (T∗,H∗),for which we find (0.8 K, 2.4 T) with experiment reporting (0.8 K,∼1.2 T) [Phys. Rev. B93, 184513 (2016)]. Furthermore, we find a substantial drop in the Knight shift in agreement with recent experiments.

Superconductivity and magnetism are antagonistic states of matter. The presence of spontaneous magnetic fields inside the superconducting state is, therefore, an intriguing phenomenon prompting extensive experimental and theoretical research. In this review, we discuss recent experimental discoveries of unconventional superconductors which spontaneously break time-reversal symmetry and theoretical efforts in understanding their properties. We discuss the main experimental probes and give an extensive account of theoretical approaches to understand the order parameter symmetries and the corresponding pairing mechanisms including the importance of multiple bands., 29 pages, 10 figures

We report the discovery of Zr$_3$Ir as a new type of unconventional noncentrosymmetric superconductor (with $T_c = 2.3$ K), here investigated mostly via muon-spin rotation/relaxation ($\mu$SR) techniques. Its superconductivity was characterized using magnetic susceptibility, electrical resistivity, and heat capacity measurements. The low-temperature superfluid density, determined via transverse-field $\mu$SR and electronic specific heat, suggests a fully-gapped superconducting state. The spontaneous magnetic fields, revealed by zero-field $\mu$SR below $T_c$, indicate the breaking of time-reversal symmetry in Zr$_3$Ir and, hence, the unconventional nature of its superconductivity. By using symmetry arguments and electronic-structure calculations we obtain a superconducting order parameter that is fully compatible with the experimental observations. Hence, our results clearly suggest that Zr$_3$Ir represents a new member of noncentrosymmetric superconductors with broken time-reversal symmetry., Comment: 6 pages, 4 figuress; supplementary materials can be accessed from corresponding authors

Ginzburg-Landau vortices in superconductors attract or repel depending on whether the value of the coupling constant is less than 1 or larger than 1. At critical coupling it was previously observed that a strongly localised magnetic impurity behaves very similarly to a vortex. This remains true for axially symmetric configurations away from critical coupling. In particular, a delta function impurity of a suitable strength is related to a vortex configuration without impurity by singular gauge transformation. However, the interaction of vortices and impurities is more subtle and depends not only on the coupling constant and the impurity strength, but also on how broad the impurity is. Furthermore, the interaction typically depends on the distance and may be attractive at short distances and repulsive at long distances. Numerical simulations confirm moduli space approximation results for the scattering of one and two vortices with an impurity. However, a double vortex will split up when scattering with an impurity, and the direction of the split depends on the sign of the impurity. Head-on collisions of a single vortex with different impurities away from critical coupling is also briefly discussed., 39 pages, 18 figures, this version is accepted for publication in PRD

The exceptionally low-symmetry crystal structures of the time-reversal symmetry breaking superconductors LaNiC$_2$ and LaNiGa$_2$ lead to an internally-antisymmetric non-unitary triplet (INT) state as the only possibility compatible with experiments. We argue that this state has a distinct signature: a double-peak structure in the Density of States (DOS) which resolves in the spin channel in a particular way. We construct a detailed model of LaNiGa$_2$ capturing its electronic band structure and magnetic properties ab initio. The pairing mechanism is described via a single adjustable parameter. The latter is fixed by the critical temperature $T_c$ allowing parameter-free predictions. We compute the electronic specific heat and find excellent agreement with experiment. The size of the ordered moment in the superconducting state is compatible with zero-field muon spin relaxation experiments and the predicted spin-resolved DOS suggests the spin-splitting is within the reach of present experimental technology., Comment: Accepted in PRB as a rapid communication

The dynamics and behavior of ferromagnets have a great relevance even beyond the domain of statistical physics. In this work, we propose a Monte Carlo method, based on random graphs, for modeling their dilution. In particular, we focus on ferromagnets with dimension $D \ge 4$, which can be approximated by the Curie-Weiss model. Since the latter has as graphic counterpart a complete graph, a dilution can be in this case viewed as a pruning process. Hence, in order to exploit this mapping, the proposed strategy uses a modified version of the Erd\H{o}s-Renyi graph model. In doing so, we are able both to simulate a continuous dilution, and to realize diluted ferromagnets in one step. The proposed strategy is studied by means of numerical simulations, aimed to analyze main properties and equilibria of the resulting diluted ferromagnets. To conclude, we also provide a brief description of further applications of our strategy in the field of complex networks., Comment: 23 pages, 7 figures; accepted for publication in Complexity

Topological states of matter exhibit many novel properties due to the presence of robust topological invariants such as the Chern index. These global characteristics pertain to the system as a whole and are not locally defined. However, local topological markers can distinguish between topological phases, and they can vary in space. In equilibrium, we show that the topological marker can be used to extract the critical behaviour of topological phase transitions. Out of equilibrium, we show that the topological marker spreads via a flow of currents emanating from the sample boundaries, and with a bounded maximum propagation speed. We discuss the possibilities for measuring the topological marker and its flow in experiment.

Bulk studies have revealed a first-order valence phase transition in Ba$_2$PrRu$_{1-x}$Ir$_x$O$_6$ ($0.10 \le x \le 0.25$), which is absent in the parent compounds with $x = 0$ (Pr$^{3+}$) and $x =1$ (Pr$^{4+}$), which exhibit antiferromagnetic order with transition temperatures $T_{\rm N} = 120$ and 72 K, respectively. In the present study, we have used magnetization, heat capacity, neutron diffraction, inelastic neutron scattering and x-ray absorption measurements to investigate the nature of the Pr ion in $x =0.1$. The magnetic susceptibility and heat capacity of $x =0.1$ show a clear sign of the first order valence phase transition below 175 K, where the Pr valence changes from 3+ to 4+. Neutron diffraction analysis reveals that $x =0.1$ crystallizes in a monoclinic structure with space group $P2_1/n$ at 300 K, but below 175 K two phases coexist, the monoclinic having the Pr ion in a 3+ valence state and a cubic one ($Fm\overline{3}m$) having the Pr ion in a 4+ valence state. Clear evidence of an antiferromagnetic ordering of the Pr and Ru moments is found in the monoclinic phase of the $x = 0.1$ compound below 110 K in the neutron diffraction measurements. Meanwhile the cubic phase remains paramagnetic down to 2 K, a temperature below which heat capacity and susceptibility measurements reveal a ferromagnetic ordering. High energy inelastic neutron scattering data reveal well-defined high-energy magnetic excitations near 264 meV at temperatures below the valence transition. The high energy excitations are assigned to the Pr$^{4+}$ ions in the cubic phase and the low energy excitations to the Pr$^{3+}$ ions in the monoclinic phase. Further direct evidence of the Pr valence transition has been obtained from the x-ray absorption spectroscopy., Comment: 10 pages and 10 figures

The spin ice materials Ho$_{2}$Ti$_{2}$O$_{7}$ and Dy$_{2}$Ti$_{2}$O$_{7}$ are by now perhaps the best-studied classical frustrated magnets. A crucial step towards the understanding of their low temperature behaviour -- both regarding their unusual dynamical properties and the possibility of observing their quantum coherent time evolution -- is a quantitative understanding of the spin-flip processes which underpin the hopping of magnetic monopoles. We attack this problem in the framework of a quantum treatment of a single-ion subject to the crystal, exchange and dipolar fields from neighbouring ions. By studying the fundamental quantum mechanical mechanisms, we discover a bimodal distribution of hopping rates which depends on the local spin configuration, in broad agreement with rates extracted from experiment. Applying the same analysis to Pr$_{2}$Sn$_{2}$O$_{7}$ and Pr$_{2}$Zr$_{2}$O$_{7}$, we find an even more pronounced separation of timescales signalling the likelihood of coherent many-body dynamics., 5 pages, 2 figures, 1 table; supplemental material attached

An analytical model of electric field assisted diffusion of ions into glass is extended to include two indigenous mobile ion species that are initially uniformly distributed within the glass. A quasi-stationary state solution that includes diffusion effects and is applicable when the invasive ions have a lower mobility than the two indigenous species is presented. It is relevant to the electrical poling of soda-lime and borosilicate glasses with concentrations of mobile ions (Na+, K+) that are processed with a non-blocking anode where hydrogen ion injection occurs. The model is compared with numerical solutions based on the drift-diffusion equations and Poisson's equation and shows good agreement. The increase in the concentration of the indigenous species with the lower mobility (K+) below the poled layer within a pile-up region is accurately modelled.

Innovation and evolution are two processes of paramount relevance for social and biological systems. In general, the former allows the introduction of elements of novelty, while the latter is responsible for the motion of a system in its phase space. Often, these processes are strongly related, since an innovation can trigger the evolution, and the latter can provide the optimal conditions for the emergence of innovations. Both processes can be studied by using the framework of evolutionary game theory, where evolution constitutes an intrinsic mechanism. At the same time, the concept of innovation requires an opportune mathematical representation. Notably, innovation can be modeled as a strategy, or it can constitute the underlying mechanism that allows agents to change strategy. Here, we analyze the second case, investigating the behavior of a heterogeneous population, composed of imitative and innovative agents. Imitative agents change strategy only by imitating that of their neighbors, whereas innovative ones change strategy without the need for a copying source. The proposed model is analyzed by means of analytical calculations and numerical simulations in different topologies. Remarkably, results indicate that the mixing of mechanisms can be detrimental to cooperation near phase transitions. In those regions, the spatial reciprocity from imitative mechanisms is destroyed by innovative agents, leading to the downfall of cooperation. Our investigation sheds some light on the complex dynamics emerging from the heterogeneity of strategy revision methods, highlighting the role of innovation in evolutionary games.

We investigate whether by synthesising superconductors that are tuned to a topological, node-reconstruction transition point we could create superconducting wires that are intrinsically resilient to quenches. Recent work shows that the exponent characterising the temperature dependence of the specific heat of a nodal superconductor is lowered over a region of the phase diagram near topological transitions where nodal lines form or reconnect. Our idea is that the resulting enhancement of the low-temperature specific heat could have potential application in the prevention of superconductor quenches. We perform numerical simulations of a simplified superconductor quench model. Results show that decreasing the specific heat exponent can prevent a quench from occurring and improve quench resilience, though in our simple model the effects are small. Further work will be necessary to establish the practical feasibility of this approach., Comment: Accepted version for IEEE-TAS (Proceedings of EUCAS 2017)

We study theoretically the transport of the one-dimensional single-channel interacting electron gas through a strong potential barrier in the parameter regime where the spin sector of the low-energy Luttinger liquid theory is gapped by interaction. This phase is of particular interest since it exhibits non-trivial interaction-induced topological properties. Using bosonization and an expansion in the tunneling strength, we calculate the conductance through the barrier as a function of the temperature as well as the local density of states (LDOS) at the barrier. Our main result concerns the mechanism of bound-state mediated tunneling. The characteristic feature of the topological phase is the emergence of protected zero-energy bound states with fractional spin located at the impurity position. By flipping the fractional spin the edge states can absorb or emit spinons and thus enable single electron tunneling across the impurity even though the bulk spectrum for these excitations is gapped. This results in a finite LDOS below the bulk gap and in a non-monotonic behavior of the conductance. The system represents an important physical example of an interacting symmetry-protected topological phase---which combines features of a topological spin insulator and a topological charge metal---in which the topology can be probed by measuring transport properties., Comment: 14 pages, 6 figures

We study the stability of composite fermion fractional quantum Hall states in Harper-Hofstadter bands with Chern number $|C|>1$. We analyze the states of the composite fermion series for bosons with contact interactions and (spinless) fermions with nearest-neighbor interactions. We examine the scaling of the many-body gap as the bands are tuned to the effective continuum limit $n_\phi\to 1/|C|$. Near these points, the Hofstadter model realises large magnetic unit cells that yield bands with perfectly flat dispersion and Berry curvature. We exploit the known scaling of energies in the effective continuum limit in order to maintain a fixed square aspect ratio in finite-size calculations. Based on exact diagonalization calculations of the band-projected Hamiltonian, we show that almost all finite-size spectra yield the ground-state degeneracy predicted by composite fermion theory. We confirm that states at low ranks in the composite fermion hierarchy are the most robust and yield a clear gap in the thermodynamic limit. For bosons in $|C|=2$ and $|C|=3$ bands, our data for the composite fermion states are compatible with a finite gap in the thermodynamic limit. We also report new evidence for gapped incompressible states of fermions in $|C|>1$ bands, which have large entanglement gaps. For cases with a clear spectral gap, we confirm that the thermodynamic limit commutes with the effective continuum limit. We analyze the nature of the correlation functions for the Abelian composite fermion states and find that they feature $|C|^2$ smooth sheets. We examine two cases associated with a bosonic integer quantum Hall effect (BIQHE): For $\nu=2$ in $|C|=1$ bands, we find a strong competing state with a higher ground-state degeneracy, so no clear BIQHE is found in the band-projected Hofstadter model; for $\nu=1$ in $|C|=2$ bands, we present additional data confirming the existence of a BIQHE state., Comment: 25 pages, 24 figures

A diverse range of materials and properties are exhibited by layered perovskites. We report on the synthesis, characterization, and computational investigation of a new ferroelectric?CsBi2Ti2NbO10, an n = 3 member of the Dion?Jacobson (DJ) family. Structural studies using variable temperature neutron powder diffraction indicate that a combination of octahedral rotations and polar displacements result in the polar structure. Density functional theory calculations reveal that the wider perovskite blocks in CsBi2Ti2NbO0 stabilize proper ferroelectricity, in contrast to the hybrid-improper ferroelectricity reported for all other DJ phases. Our results raise the possibility of a new class of proper ferroelectric materials analogous to the well-known Aurivillius phases.

Clustered quantum materials provide a new platform for the experimental study of many-body entanglement. Here we address a simple model of a single-molecule nano-magnet featuring N interacting spins in a transverse field. The field can induce an entanglement transition (ET). We calculate the magnetisation, low-energy gap and neutron-scattering cross-section and find that the ET has distinct signatures, detectable at temperatures as high as 5% of the interaction strength. The signatures are stronger for smaller clusters., 14 pages, 11 Figures; minor changes; Phys. Rev. B (accepted)

We study zigzag interfaces between insulating compounds that are isostructural to graphene, specifically II-VI, III-V and IV-IV two-dimensional (2D) honeycomb insulators. We show that these one-dimensional interfaces are polar, with a net density of excess charge that can be simply determined by using the ideal (integer) formal valence charges, regardless of the predominant covalent character of the bonding in these materials. We justify this finding on fundamental physical grounds, by analyzing the topology of the formal polarization lattice in the parent bulk materials. First principles calculations elucidate an electronic compensation mechanism not dissimilar to oxide interfaces, which is triggered by a Zener-like charge transfer between interfaces of opposite polarity. In particular, we predict the emergence of one dimensional electron and hole gases (1DEG), which in some cases are ferromagnetic half-metallic., Comment: 5 pages, 3 figures

The formation of a two-dimensional electron gas at oxide interfaces as a consequence of polar discontinuities has generated an enormous amount of activity due to the variety of interesting effects it gives rise to. Here we study under what circumstances similar processes can also take place underneath ferroelectric thin films. We use a simple Landau model to demonstrate that in the absence of extrinsic screening mechanisms a monodomain phase can be stabilized in ferroelectric films by means of an electronic reconstruction. Unlike in the LaAlO$_3$/SrTiO$_3$ heterostructure, the emergence with thickness of the free charge at the interface is discontinuous. This prediction is confirmed by performing first principles simulations of free standing slabs of PbTiO$_3$. The model is also used to predict the response of the system to an applied electric field, demonstrating that the two-dimensional electron gas can be switched on and off discontinuously and in a non-volatile fashion. Furthermore, the reversal of the polarization can be used to switch between a two-dimensional electron gas and a two-dimensional hole gas, which should, in principle, have very different transport properties. We discuss the possible formation of polarization domains and how such configuration competes with the spontaneous accumulation of free charge at the interfaces., Comment: 19 pages, 10 figures

We investigate extrinsic wormholelike twist defects that effectively increase the genus of space in lattice versions of multicomponent fractional quantum Hall systems. Although the original band structure is distorted by these defects, leading to localized midgap states, we find that a new lowest flat band representing a higher genus system can be engineered by tuning local single-particle potentials. Remarkably, once local many-body interactions in this new band are switched on, we identify various Abelian and non-Abelian fractional quantum Hall states, whose ground-state degeneracy increases with the number of defects, i.e, with the genus of space. This sensitivity of topological degeneracy to defects provides a "proof of concept" demonstration that genons, predicted by topological field theory as exotic non-Abelian defects tied to a varying topology of space, do exist in realistic microscopic models. Specifically, our results indicate that genons could be created in the laboratory by combining the physics of artificial gauge fields in cold atom systems with already existing holographic beam shaping methods for creating twist defects., 10 pages, 11 figures, including a Supplementary Material. Published version

NXFitis a program for obtaining optimized structural parameters from amorphous materials by simultaneously fitting X-ray and neutron pair-distribution functions. Partial correlation functions are generated inQspace, summed and Fourier transformed for comparison with the experimental data inrspace.NXFituses the Nelder–Mead method to vary a set of `best guess' parameters to achieve a fit to experimentally derived data. The output parameters fromNXFitare coordination number, atomic separation and disorder parameter for each atomic correlation used in the fitting process. The use ofNXFithas been demonstrated by fitting both X-ray and neutron diffraction data from two quite different amorphous materials: a melt-quenched (Na2O)0.5(P2O5)0.5glass and a (TiO2)0.18(SiO2)0.82sol–gel.

Conventional intercalation cathodes for lithium batteries store charge in redox reactions associated with the transition metal cations, e.g., Mn3+/4+ in LiMn2O4, and this limits the energy storage of Li-ion batteries. Compounds such as Li[Li0.2Ni0.2Mn0.6]O-2 exhibit a capacity to store charge in excess of the transition metal redox reactions. The additional capacity occurs at and above 4.5 V versus Li+/Li. The capacity at 4.5 V is dominated by oxidation of the O-2(-) anions accounting for similar to 0.43 e(-)/formula unit, with an additional 0.06 e(-)/formula unit being associated with O loss from the lattice. In contrast, the capacity above 4.5 V is mainly O loss, similar to 0.08 e(-)/formula. The O redox reaction involves the formation of localized hole states on O during charge, which are located on O coordinated by (Mn4+/Li+). The results have been obtained by combining operando electrochemical mass spec on 180 labeled Li[Li0.2Ni0.2Mn0.6]O-2 with XANES, soft X-ray spectroscopy, resonant inelastic X-ray spectroscopy, and Raman spectroscopy. Finally the general features of O redox are described with discussion about the role of comparatively ionic (less covalent) 3d metal oxygen interaction on anion redox in lithium rich cathode materials.

The layered perovskite Ca3-xSrxMn2O7 is shown to exhibit a switching from a material exhibiting uniaxial negative to positive thermal expansion as a function of x. The switching is shown to be related to two closely competing phases with different symmetries. The negative thermal expansion (NTE) effect is maximized when the solid solution is tuned closest to this region of phase space but is switched off suddenly on passing though the transition. Our results show for the first time that, by understanding the symmetry of the competing phases alone, one may achieve unprecedented chemical control of this unusual property.

The nature of the pairing states of superconducting LaNiC\(_2\) and LaNiGa\(_2\) has to date remained a puzzling question. Broken time reversal symmetry has been observed in both compounds and a group theoretical analysis implies a non-unitary triplet pairing state. However all the allowed non-unitary triplet states have nodal gap functions but most thermodynamic and NMR measurements indicate fully gapped superconductivity in LaNiC\(_2\). Here we probe the gap symmetry of LaNiGa\(_2\) by measuring the London penetration depth, specific heat and upper critical field. These measurements demonstrate two-gap nodeless superconductivity in LaNiGa\(_2\), suggesting that this is a common feature of both compounds. These results allow us to propose a novel triplet superconducting state, where the pairing occurs between electrons of the same spin, but on different orbitals. In this case the superconducting wavefunction has a triplet spin component but isotropic even parity gap symmetry, yet the overall wavefunction remains antisymmetric under particle exchange. This model leads to a nodeless two-gap superconducting state which breaks time reversal symmetry, and therefore accounts well for the seemingly contradictory experimental results.

The study of magnetic correlations in dipolar-coupled nanomagnet systems with synchrotron x-ray scattering provides a means to uncover emergent phenomena and exotic phases, in particular in systems with thermally active magnetic moments. From the diffuse signal of soft x-ray resonant magnetic scattering, we have measured magnetic correlations in a highly dynamic artificial kagome spin ice with sub-70-nm Permalloy nanomagnets. On comparing experimental scattering patterns with Monte Carlo simulations based on a needle-dipole model, we conclude that kagome ice I phase correlations exist in our experimental system even in the presence of moment fluctuations, which is analogous to bulk spin ice and spin liquid behavior. In addition, we describe the emergence of quasi-pinch-points in the magnetic diffuse scattering in the kagome ice I phase. These quasi-pinch-points bear similarities to the fully developed pinch points with singularities of a magnetic Coulomb phase, and continually evolve into the latter on lowering the temperature. The possibility to measure magnetic diffuse scattering with soft x rays opens the way to study magnetic correlations in a variety of nanomagnetic systems., 8 pages, 5 figures; http://journals.aps.org/prb/abstract/10.1103/PhysRevB.93.224413

© 2016 American Chemical Society.Hybrid perovskites are currently the fastest growing photovoltaic technology, having reached a solar cell efficiency of over 20%. One possible strategy to further improve the efficiency of perovskite solar cells is to tune the degree of octahedral tilting of the halide frame, since this in turn affects the optical band gap and carrier effective masses. It is commonly accepted that the ion sizes are the main control parameter influencing the degree of tilting in perovskites. Here we re-examine the origin of octahedral tilts in halide perovskites from systematic first-principles calculations. We find that while steric effects dominate the tilt magnitude in inorganic halides, hydrogen bonding between an organic A-cation and the halide frame plays a significant role in hybrids. For example, in the case of MAPbI3, our calculations suggest that, without the contribution from hydrogen bonding, the octahedra would not tilt at all. These results demonstrate that tuning the degree of hydrogen bonding can be used as an additional control parameter to optimize the photovoltaic properties of perovskites.

The Seebeck coefficient, thermoelectric power factor, electrical conductivity, and electronic thermal conductivity of the orthorhombic Pbnm phase of SrRuO3 are studied comprehensively by combining first-principles density functional calculations and Boltzmann transport theory. The influence of exchange-correlation functional on the Seebeck coefficient is carefully investigated. We show that the best agreement with experimental data is achieved when SrRuO3 is described as being at the limit of a half-metal. Furthermore, we analyze the role of individual symmetry-adapted atomic distortions on the Seebeck coefficient, highlighting a particularly strong sensitivity to R-4(+) oxygen rotational motions, which may shed light on how to manipulate the Seebeck coefficient. We confirm that the power factor of SrRuO3 can only be slightly improved by carrier doping. Our results provide a complete understanding of the thermoelectric properties of SrRuO3 and an interesting insight on the relationship between exchange-correlation functionals, atomic motions, and thermoelectric quantities.

Globally, more than 1000 tonnes of titanium (Ti) is implanted into patients in the form of biomedical devices on an annual basis. Ti is perceived to be ‘biocompatible’ owing to the presence of a robust passive oxide film (approx. 4 nm thick) at the metal surface. However, surface deterioration can lead to the release of Ti ions, and particles can arise as the result of wear and/or corrosion processes. This surface deterioration can result in peri-implant inflammation, leading to the premature loss of the implanted device or the requirement for surgical revision. Soft tissues surrounding commercially pure cranial anchorage devices (bone-anchored hearing aid) were investigated using synchrotron X-ray micro-fluorescence spectroscopy and X-ray absorption near edge structure. Here, we present the first experimental evidence that minimal load-bearing Ti implants, which are not subjected to macroscopic wear processes, can release Ti debris into the surrounding soft tissue. As such debris has been shown to be pro-inflammatory, we propose that such distributions of Ti are likely to effect to the service life of the device.

Bone is the second most widely transplanted tissue after blood. Synthetic alternatives are needed that can reduce the need for transplants and regenerate bone by acting as active temporary templates for bone growth. Bioactive glasses are one of the most promising bone replacement/regeneration materials because they bond to existing bone, are degradable and stimulate new bone growth by the action of their dissolution products on cells. Sol–gel-derived bioactive glasses can be foamed to produce interconnected macropores suitable for tissue ingrowth, particularly cell migration and vascularization and cell penetration. The scaffolds fulfil many of the criteria of an ideal synthetic bone graft, but are not suitable for all bone defect sites because they are brittle. One strategy for improving toughness of the scaffolds without losing their other beneficial properties is to synthesize inorganic/organic hybrids. These hybrids have polymers introduced into the sol–gel process so that the organic and inorganic components interact at the molecular level, providing control over mechanical properties and degradation rates. However, a full understanding of how each feature or property of the glass and hybrid scaffolds affects cellular response is needed to optimize the materials and ensure long-term success and clinical products. This review focuses on the techniques that have been developed for characterizing the hierarchical structures of sol–gel glasses and hybrids, from atomic-scale amorphous networks, through the covalent bonding between components in hybrids and nanoporosity, to quantifying open macroporous networks of the scaffolds. Methods for non-destructive in situ monitoring of degradation and bioactivity mechanisms of the materials are also included.

© 2018 IOP Publishing Ltd. Room temperature electron irradiation in aqueous environment is applied to CeO2 nanoparticles using a transmission electron microscope equipped with liquid environmental cell. Oxide dissolution kinetics become accessible at unprecedented scale of spatial and time resolution through irradiation activation of water within a sub-μm size volume, allowing direct measurements of transformation rate and morphologies. Successful live-observation of the formation of nano-needles provides essential inside in how 1D-nanostructures can form. Furthermore, formation of hydrogen bubbles is found and interpreted in relation to the dose needed for ceria dissolution. The results are of importance for many research applications of ceria in water, e.g. for catalysis, environmental remediation, biomedical radiation protection, anti-corrosion coatings, and ultimately via analogy to UO2 also for fission-power fuel engineering and waste disposal.

The Jahn-Teller distortion, by its very nature, is often at the heart of the various electronic properties displayed by perovskites and related materials. Despite the Jahn-Teller mode being non- polar in nature, we devise and demonstrate in the present letter an electric field control of Jahn-Teller distortions in bulk perovskites. The electric field control is enabled through an anharmonic lattice mode coupling between the Jahn-Teller distortion and a polar mode. We confirm this coupling, and explicitly an electric field effect, through first principles calculations. The coupling will always exist within the P b2 1 m space group, which is found to be the favoured ground state for various perovskites under sufficient tensile epitaxial strain. Intriguingly, the calculations reveal that this mechanism is not only restricted to Jahn-Teller active systems, promising a general route to tune or induce novel electronic functionality in perovskites as a whole.

The family of the superconducting quasiskutterudites (CaxSr1?x)3Rh4Sn13 features a structural quantum critical point at xc=0.9, around which a dome-shaped variation of the superconducting transition temperature Tc is found. Using specific heat, we probe the normal and the superconducting states of the entire series straddling the quantum critical point. Our analysis indicates a significant lowering of the effective Debye temperature on approaching xc, which we interpret as a result of phonon softening accompanying the structural instability. Furthermore, a remarkably large enhancement of 2?/kBTc and ?C/?Tc beyond the Bardeen-Cooper-Schrieffer values is found in the vicinity of the structural quantum critical point. The phase diagram of (CaxSr1?x)3Rh4Sn13 thus provides a model system to study the interplay between structural quantum criticality and strong electron-phonon coupling superconductivity.

The Harper-Hofstadter model provides a fractal spectrum containing topological bands of any integer Chern number, $C$. We study the many-body physics that is realized by interacting particles occupying Harper-Hofstadter bands with $|C|>1$. We formulate the predictions of Chern-Simons or composite fermion theory in terms of the filling factor, $\nu$, defined as the ratio of particle density to the number of single-particle states per unit area. We show that this theory predicts a series of fractional quantum Hall states with filling factors $\nu = r/(r|C| +1)$ for bosons, or $\nu = r/(2r|C| +1)$ for fermions. This series includes a bosonic integer quantum Hall state (bIQHE) in $|C|=2$ bands. We construct specific cases where a single band of the Harper-Hofstadter model is occupied. For these cases, we provide numerical evidence that several states in this series are realized as incompressible quantum liquids for bosons with contact interactions., Comment: v1: 7 pages, 4 figures; v2: 5+5 pages, 2+4 figures (final author formatted version)

First principles calculations on the hybrid perovskite CH3NH3PbI3 predict strong hydrogen-bonding which influences the structure and dynamics of the methylammonium cation and reveal its interaction with the tilting of the PbI6 octahedra. The calculated atomic coordinates are in excellent agreement with neutron diffraction results.

In magnetic materials, the Pauli exclusion principle typically drives anti-alignment between electron spins on neighbouring species resulting in antiferromagnetic behaviour. Ferromagnetism exhibiting spontaneous spin alignment is a fairly rare behaviour, but once materialized is often associated with itinerant electrons in metals. Here we predict and rationalize robust ferromagnetism in an insulating oxide perovskite structure based on the popular titanate series. In half-doped layered titanates, the combination of Jahn–Teller and oxygen breathing motions opens a band gap and creates an unusual charge and orbital ordering of the Ti d electrons. It is argued that this intriguingly intricate electronic network favours the elusive inter-site ferromagnetic (FM) ordering, on the basis of intra-site Hund's rules. Finally, we find that the layered oxides are also ferroelectric with a spontaneous polarization approaching that of BaTiO3. The concepts are general and design principles of the technologically desirable FM ferroelectric multiferroics are presented., Magnetic insulators often display antiferromagnetic ordering owing to implications from the Pauli exclusion principle. Here, the authors predict ferromagnetism on the basis of intra-site Hund's rules in ferroelectric titanate superlattices showing charge and Jahn–Teller induced orbital orderings.

Motivated by its role as a central pillar of current theories of dynamics of spin ice in and out of equilibrium, we study the single-ion dynamics of the magnetic rare earth ions in their local environments, subject to the effective fields set up by the magnetic moments they interact with. This effective field has a transverse component with respect to the local easy-axis of the crystal electric field, which can induce quantum tunnelling. We go beyond the projective spin-1/2 picture and use instead the full crystal-field Hamiltonian. We find that the Kramers vs non-Kramers nature, as well as the symmetries of the crystal-field Hamiltonian, result in different perturbative behaviour at small fields ($\lesssim 1$ T), with transverse field effects being more pronounced in Ho$_{2}$Ti$_{2}$O$_{7}$ than in Dy$_{2}$Ti$_{2}$O$_{7}$. Remarkably, the energy splitting range we find is consistent with time scales extracted from experiments. We also present a study of the static magnetic response which highlights the anisotropy of the system in the form of an off-diagonal $g$ tensor and we investigate the effects of thermal fluctuations in the temperature regime of relevance to experiments. We show that there is a narrow yet accessible window of experimental parameters where the anisotropic response can be observed.

We study the Fermi surface topological transition of the pocket-opening type in a two dimensional Fermi liquid. We find that the paramagnetic fluctuations in an interacting Fermi liquid typically drive the transition first order at zero temperature. We first gain insight from a calculation using second order perturbation theory in the self-energy. This is valid for weak interaction and far from instabilities. We then extend the results to stronger interaction, using the self-consistent fluctuation approximation. Experimental signatures are given in the light of these results., Comment: 4.5 pages, 3 figures

The fractional quantum Hall (FQH) effect illustrates the range of novel phenomena which can arise in a topologically ordered state in the presence of strong interactions. The possibility of realizing FQH-like phases in models with strong lattice effects has attracted intense interest as a more experimentally accessible venue for FQH phenomena which calls for more theoretical attention. Here we investigate the physical relevance of previously derived geometric conditions which quantify deviations from the Landau level physics of the FQHE. We conduct extensive numerical many-body simulations on several lattice models, obtaining new theoretical results in the process, and find remarkable correlation between these conditions and the many-body gap. These results indicate which physical factors are most relevant for the stability of FQH-like phases, a paradigm we refer to as the geometric stability hypothesis, and provide easily implementable guidelines for obtaining robust FQH-like phases in numerical or real-world experiments., [v2]: substantial revision, addition of data for Moore-Read state; as submitted to Nature Communications

The quest for realizations of non-Abelian phases of matter, driven by their possible use in fault-tolerant topological quantum computing, has been spearheaded by recent developments in p-wave superconductors. The chiral p_x + i p_y-wave superconductor in two-dimensions exhibiting Majorana modes provides the simplest phase supporting non-Abelian quasiparticles and can be seen as the blueprint of fractional topological order. Alternatively, Kitaev's Majorana wire has emerged as an ideal toy model to understand Majorana modes. Here, we present a way to make the transition from Kitaev's Majorana wires to two-dimensional p-wave superconductors in a system with cold atomic gases in an optical lattice. The main idea is based on an approach to generate p-wave interactions by coupling orbital degrees of freedom with strong s-wave interactions. We demonstrate how this design can induce Majorana modes at edge dislocations in the optical lattice and we provide an experimentally feasible protocol for the observation of the non-Abelian statistics.

In this study, amorphous (Na2O)x(CaO)0.50−x(P2O5)0.50·yH2O (where x = ∼0.15 and y = ∼3) samples were prepared by a coacervate method. Thermal analysis showed that two types of water molecules were present in the coacervate structures: one type loosely bound and the other part of the phosphate structure. Structural studies using Fourier transform infrared spectroscopy (FTIR) and X-ray total diffraction revealed the samples to have very similar structures to melt-quenched glasses of comparable composition. Furthermore, no significant structural differences were observed between samples prepared using calcium nitrate as the calcium source or those prepared from calcium chloride. A sample containing ∼1 mol% Ag2O was prepared to test the hypothesis that calcium phosphate coacervate materials could be used as delivery agents for antibacterial ions. This sample exhibited significant antibacterial activity against the bacterium Psuedomonas aeruginosa. FTIR data revealed the silver-doped sample to be structurally akin to the analogous silver-free sample.