Symmetry-mode analysis for local structure investigations using pair distribution function data

Symmetry-adapted distortion modes provide a natural way to describe distorted structures derived from higher-symmetry parent phases. Structural refinements using symmetry-mode amplitudes as fit variables have been used for at least 10 years in Rietveld refinements of the average crystal structure from diffraction data; more recently, this approach has also been used for investigations of the local structure using real-space pair distribution function (PDF) data. Here, we further demonstrate the value of performing symmetry-mode fits to PDF data through the successful application of this method to two topical materials: TiSe$_2$, where we detect the subtle but long-range structural distortion driven by the formation of a charge density wave, and MnTe, where we characterize a large but highly localized structural distortion in terms of symmetry-lowering displacements of the Te atoms. The analysis is performed using fully open-source code within the DiffPy framework using two packages we developed for this work: isopydistort, which provides a scriptable interface to the ISODISTORT web application for group theoretical calculations, and isopytools, which converts the ISODISTORT output into a DiffPy-compatible format for subsequent fitting and analysis. These developments expand the potential impact of symmetry-adapted PDF analysis by enabling high throughput analysis and removing the need for any commercial software

Discovery of Superconductivity and Electron-Phonon Drag in the Non-Centrosymmetric Semimetal LaRhGe3_3

We present a comprehensive study of the non-centrosymmetric semimetal LaRhGe$_3$. Our transport measurements reveal evidence for electron-hole compensation at low temperatures, resulting in a large magnetoresistance of 3000% at 1.8 K and 14 T. The carrier concentration is on the order of $10^{21}\rm{/cm}^3$, higher than typical semimetals. We predict theoretically the existence of $\textit{almost movable}$ Weyl nodal lines that are protected by the tetragonal space group. We discover superconductivity for the first time in this compound with a $T_{\text c}$ of 0.39(1) K and $B_{\rm{c}}(0)$ of 2.1(1) mT, with evidence from specific heat and transverse-field muon spin relaxation ($\mu \rm{SR}$). LaRhGe$_3$ is a weakly-coupled type-I superconductor, and we find no evidence for time-reversal symmetry breaking in our zero-field $\mu \rm{SR}$. We study the electrical transport in the normal state and find an unusual $\sim T^{3}$ dependence at low temperature while Seebeck coefficient and thermal conductivity measurements reveal a peak in the same temperature range. We conclude that the transport properties of LaRhGe$_3$ in its normal state are strongly influenced by electron-phonon interactions. Furthermore, we examine the temperature dependent Raman spectra of LaRhGe$_3$ and find that the lifetime of the lowest energy $A_1$ phonon is dominated by phonon-electron scattering instead of anharmonic decay

Disentangling superconducting and magnetic orders in NaFe_1-xNi_xAs using muon spin rotation

Muon spin rotation and relaxation studies have been performed on a "111" family of iron-based superconductors NaFe_1-xNi_xAs. Static magnetic order was characterized by obtaining the temperature and doping dependences of the local ordered magnetic moment size and the volume fraction of the magnetically ordered regions. For x = 0 and 0.4 %, a transition to a nearly-homogeneous long range magnetically ordered state is observed, while for higher x than 0.4 % magnetic order becomes more disordered and is completely suppressed for x = 1.5 %. The magnetic volume fraction continuously decreases with increasing x. The combination of magnetic and superconducting volumes implies that a spatially-overlapping coexistence of magnetism and superconductivity spans a large region of the T-x phase diagram for NaFe_1-xNi_xAs . A strong reduction of both the ordered moment size and the volume fraction is observed below the superconducting T_C for x = 0.6, 1.0, and 1.3 %, in contrast to other iron pnictides in which one of these two parameters exhibits a reduction below TC, but not both. The suppression of magnetic order is further enhanced with increased Ni doping, leading to a reentrant non-magnetic state below T_C for x = 1.3 %. The reentrant behavior indicates an interplay between antiferromagnetism and superconductivity involving competition for the same electrons. These observations are consistent with the sign-changing s-wave superconducting state, which is expected to appear on the verge of microscopic coexistence and phase separation with magnetism. We also present a universal linear relationship between the local ordered moment size and the antiferromagnetic ordering temperature TN across a variety of iron-based superconductors. We argue that this linear relationship is consistent with an itinerant-electron approach, in which Fermi surface nesting drives antiferromagnetic ordering.Comment: 20 pages, 14 figures, Correspondence should be addressed to Prof. Yasutomo Uemura: [email protected]

Field-induced quantum critical point in the new itinerant antiferromagnet Ti3_3Cu4_4

New phases of matter emerge at the edge of magnetic instabilities. In local moment systems, such as heavy fermions, the magnetism can be destabilized by pressure, chemical doping, and, rarely, by magnetic field, towards a zero-temperature transition at a quantum critical point (QCP). Even more rare are instances of QCPs induced by pressure or doping in itinerant moment systems, with no known examples of analogous field-induced \textit{T} = 0 transitions. Here we report the discovery of a new itinerant antiferromagnet with no magnetic constituents, in single crystals of Ti$_3$Cu$_4$ with $T_N$ = 11.3 K. Band structure calculations point to an orbital-selective, spin density wave ground state, a consequence of the square net structural motif in Ti$_3$Cu$_4$. A small magnetic field, $H_C$ = 4.87 T, suppresses the long-range order via a continuous second-order transition, resulting in a field-induced QCP. The magnetic Gr\"uneisen ratio diverges as $H \rightarrow H_C$ and $T\rightarrow0$, with a sign change at $H_C$ and $T^{-1}$ scaling at $H~=~H_C$, providing evidence from thermodynamic measurements for quantum criticality for $H \parallel c$. Non-Fermi liquid (NFL) to Fermi liquid (FL) crossover is observed close to the QCP, as revealed by the power law behavior of the electrical resistivity

The Future of the Correlated Electron Problem

The understanding of material systems with strong electron-electron interactions is the central problem in modern condensed matter physics. Despite this, the essential physics of many of these materials is still not understood and we have no overall perspective on their properties. Moreover, we have very little ability to make predictions in this class of systems. In this manuscript we share our personal views of what the major open problems are in correlated electron systems and we discuss some possible routes to make progress in this rich and fascinating field. This manuscript is the result of the vigorous discussions and deliberations that took place at Johns Hopkins University during a three-day workshop January 27, 28, and 29, 2020 that brought together six senior scientists and 46 more junior scientists. Our hope, is that the topics we have presented will provide inspiration for others working in this field and motivation for the idea that significant progress can be made on very hard problems if we focus our collective energies.Comment: 55 pages, 19 figure

Understanding the role of entropy in high entropy oxides

The field of high entropy oxides (HEOs) flips traditional materials science paradigms on their head by seeking to understand what properties arise in the presence of profound configurational disorder. This disorder, which originates from multiple elements sharing a single lattice site, can take on a kaleidoscopic character due to the vast numbers of possible elemental combinations. High configurational disorder appears to imbue some HEOs with functional properties that far surpass their non-disordered analogs. While experimental discoveries abound, efforts to characterize the true magnitude of the configurational entropy and understand its role in stabilizing new phases and generating superior functional properties have lagged behind. Understanding the role of configurational disorder in existing HEOs is the crucial link to unlocking the rational design of new HEOs with targeted properties. In this Perspective, we attempt to establish a framework for articulating and beginning to address these questions in pursuit of a deeper understanding of the true role of entropy in HEOs.Comment: 18 pages, 7 figure