arXiv subjects

S. J. L. Billinge

Publications and source records attributed to S. J. L. Billinge.

At least 19 recordsLinked to original sources

arXiv2025

scikit-package -- software packaging standards and roadmap for sharing reproducible scientific software

Scientific advancement relies on the ability to share and reproduce results. When data analysis or calculations are carried out using software written by scientists there are special challenges around code versions, quality and code sharing. scikit-package provides a roadmap to facilitate code reuse and sharing with minimal effort through tutorials coupled with automated and centralized reusable workflows. The goal of the project is to provide pedagogical and practical tools for scientists who are not professionally trained software engineers to write more reusable and maintainable software code. Code reuse can occur at multiple levels of complexity-from turning a code block into a function within a single script, to publishing a publicly installable, fully tested, and documented software package scikit-package provides a community maintained set of tools, and a roadmap, to help scientists bring their software higher levels of reproducibility and shareability.

cs.SE↗

arXiv2023

Nanoscale Sn off-centering behind low thermal conductivity in SnSe thermoelectric

The local atomic structure of SnSe was characterized across its orthorhmbic-to-orthorhombic structural phase transition using x-ray pair distribution function analysis. Substantial Sn off-centering distortions persist in the high symmetry high temperature phase, with symmetry different from that of ordered distortions below the transition. The analysis implies that the transition is neither order-disorder nor displacive, but rather a complex crossover where the character of coupling changes from 3D-like at low temperature to 2D-like at high temperature. Robust ferro-coupled SnSe intra-layer distortions suggest a ferroelectric-like instability as the driving force. Complex local Sn off-centering is integral to the ultra-low lattice thermal conductivity mechanism in SnSe.

cond-mat.mtrl-sci↗

arXiv2020

Dual Orbital Degeneracy Lifting in a Strongly Correlated Electron System

The local structure of NaTiSi$_{2}$O$_{6}$ is examined across its Ti-dimerization orbital-assisted Peierls transition at 210 K. An atomic pair distribution function approach evidences local symmetry breaking preexisting far above the transition. The analysis unravels that on warming the dimers evolve into a short range orbital degeneracy lifted (ODL) state of dual orbital character, persisting up to at least 490 K. The ODL state is correlated over the length scale spanning $\sim$6 sites of the Ti zigzag chains. Results imply that the ODL phenomenology extends to strongly correlated electron systems.

cond-mat.str-el↗

arXiv2019

Room temperature local nematicity in FeSe superconductor

We report pair distribution function measurements of the iron-based superconductor FeSe above and below the structural transition temperature. Structural analysis reveals a local orthorhombic distortion with a correlation length of about 4 nm at temperatures where an average tetragonal symmetry is observed. The analysis further demonstrates that the local distortion is larger than the distortion at temperatures where the average observed symmetry is orthorhombic. Our results suggest that the low-temperature macroscopic nematic state in FeSe forms from an imperfect ordering of orbital-degeneracy-lifted nematic fluctuations which persist up to at least 300 K.

cond-mat.supr-con↗

arXiv2019

Local orbital degeneracy lifting as a precursor to an orbital-selective Peierls transition

Fundamental electronic principles underlying all transition metal compounds are the symmetry and filling of the $d$-electron orbitals and the influence of this filling on structural configurations and responses. Here we use a sensitive local structural technique, x-ray atomic pair distribution function analysis, to reveal the presence of fluctuating local-structural distortions at high temperature of one such compound, \cis . We show that this hitherto overlooked fluctuating symmetry lowering is electronic in origin and will significantly modify the energy-level spectrum and electronic and magnetic properties. The explanation is a local, fluctuating, orbital-degeneracy-lifted state. The natural extension of our result would be that this phenomenon is likely to be widespread amongst diverse classes of partially filled nominally degenerate d-electron systems, with potentially broad implications for our understanding of their properties.

cond-mat.mtrl-sci↗

arXiv2019

Photoinduced ultrafast dynamics of local nematicity and lattice distortions in FeSe crystals

Formation of electronic nematicity is a common thread of unconventional superconductors. In iron-based materials, the long-range nematic order is revealed by the orthorhombic lattice distortion, which importance is a highly controversial topic due the small magnitude of the distortion. Here, we study the local crystal structure of FeSe and its interaction with electronic degrees of freedom using ultrafast electron diffraction, x-ray pair distribution function analysis, and transmission electron microscopy and find a significant lattice response to local nematicity. The study demonstrates how local lattice distortions, which exist even at temperatures above the nematic phase transition, can be released by photoexcitation, leading to an enhancement of the crystalline order. The observed local atomic structures and their out-of-equilibrium behavior unravel a sophisticated coupling between the lattice and nematic order parameter in FeSe.

cond-mat.supr-con↗

arXiv2017

Magnetism in Semiconducting Molybdenum Dichalcogenides

Transition metal dichalcogenides (TMDs) are interesting for understanding fundamental physics of two-dimensional materials (2D) as well as for many emerging technologies, including spin electronics. Here, we report the discovery of long-range magnetic order below TM = 40 K and 100 K in bulk semiconducting TMDs 2H-MoTe2 and 2H-MoSe2, respectively, by means of muon spin-rotation (muSR), scanning tunneling microscopy (STM), as well as density functional theory (DFT) calculations. The muon spin rotation measurements show the presence of a large and homogeneous internal magnetic fields at low temperatures in both compounds indicative of long-range magnetic order. DFT calculations show that this magnetism is promoted by the presence of defects in the crystal. The STM measurements show that the vast majority of defects in these materials are metal vacancies and chalcogen-metal antisites which are randomly distributed in the lattice at the sub-percent level. DFT indicates that the antisite defects are magnetic with a magnetic moment in the range of 0.9-2.8 mu_B. Further, we find that the magnetic order stabilized in 2H-MoTe2 and 2H-MoSe2 is highly sensitive to hydrostatic pressure. These observations establish 2H-MoTe2 and 2H-MoSe2 as a new class of magnetic semiconductors and opens a path to studying the interplay of 2D physics and magnetism in these interesting semiconductors.

cond-mat.mtrl-sci↗

arXiv2017

Pressure tuning of structure, superconductivity and novel magnetic order in the Ce-underdoped electron-doped cuprate T'-Pr_1.3-xLa_0.7Ce_xCuO_4 (x = 0.1)

High-pressure neutron powder diffraction, muon-spin rotation and magnetization studies of the structural, magnetic and the superconducting properties of the Ce-underdoped superconducting (SC) electron-doped cuprate system T'-Pr_1.3-xLa_0.7Ce_xCuO_4 with x = 0.1 are reported. A strong reduction of the lattice constants a and c is observed under pressure. However, no indication of any pressure induced phase transition from T' to T structure is observed up to the maximum applied pressure of p = 11 GPa. Large and non-linear increase of the short-range magnetic order temperature T_so in T'-Pr_1.3-xLa_0.7Ce_xCuO_4 (x = 0.1) was observed under pressure. Simultaneously pressure causes a non-linear decrease of the SC transition temperature T_c. All these experiments establish the short-range magnetic order as an intrinsic and a new competing phase in SC T'-Pr_1.2La_0.7Ce_0.1CuO_4. The observed pressure effects may be interpreted in terms of the improved nesting conditions through the reduction of the in-plane and out-of-plane lattice constants upon hydrostatic pressure.

cond-mat.supr-con↗

arXiv2017

Possible topologically non-trivial superconducting order parameter in type-II Weyl semimetal T_d-MoTe_2

MoTe_2, with the orthorhombic T_d phase, is a new type (type-II) of Weyl semimetal, where the Weyl Fermions emerge at the boundary between electron and hole pockets. Non-saturating magnetoresistance (MR), and superconductivity were also observed in T_d-MoTe_2. Understanding the superconductivity in T_d-MoTe_2, which was proposed to be topologically non-trivial, is of eminent interest. Here, we report high-pressure (p_max = 1.3 GPa) muon spin rotation experiments on the temperature-dependent magnetic penetration depth in T_d-MoTe_2. A substantial increase of the superfluid density n_s/m^* and a linear scaling with T_c is observed under pressure. Moreover, the superconducting order parameter in T_d-MoTe_2 is determined to be two gap (s+s)-wave symmetric. We also excluded time reversal symmetry breaking in the SC state with sensitive zero-field $μ$SR experiments. Considering the previous report \cite{Balicas1} on the strong suppression of T_c in T_d-MoTe_2 by disorder, we suggest that s^{+-} (topological order parameter) state is more likely to be realized in MoTe_2 than the s^{++} (trivial) state. Should s^{+-} be the SC gap symmetry, the T_d-MoTe_2 is, to our knowledge, the first known example of a time reversal invariant topological (Weyl) superconductor.

cond-mat.supr-con↗

arXiv2017

Cooperative coupling of static magnetism and bulk superconductivity in the stripe phase of La_2-xBa_xCuO_4: Pressure- and doping-dependent studies

Static spin-stripe order and superconductivity were systematically studied in La_2-xBa_xCuO_4 (0.11 - 0.17) at ambient pressure by means of magnetization and muSR experiments. We find that all the investigated La_2-xBa_xCuO_4 samples exhibit static spin-stripe order and that the quasi two-dimensional superconducting (SC) transition temperature T_c1 and the static spin-stripe order temperature T_so have very similar values throughout the phase diagram. Moreover, the magnetic and the SC properties of the x = 0.155 (LBCO-0.155) and x = 0.17 (LBCO-0.17) samples were studied under hydrostatic pressure. As a remarkable result, in these bulk cuprate superconductors the three-dimensional SC transition temperature T_c and T_so nearly coincide at all pressure investigated (0 - 2.3 GPa). We also observed a pressure induced transition from long-range spin stripe order to a disordered magnetic state at 1.6 GPa in LBCO-0.155, coexisting with a SC state with substantial superfluid density. In LBCO-0.17 a disordered magnetic state is present at all p. The present results indicate that static magnetic order and SC pairing correlations develop in a cooperative fashion in La_2-xBa_xCuO_4, and provide a new route of understanding the complex interplay between static magnetism and superconductivity in the stripe phase of cuprates.

cond-mat.supr-con↗

arXiv2016

Enhanced Thermoelectric Power and Electronic Correlations in RuSe$_2$

We report the electronic structure, electric and thermal transport properties of Ru$_{1-x}$Ir$_{x}$Se$_2$ ($x \leq 0.2$). RuSe$_2$ is a semiconductor that crystallizes in a cubic pyrite unit cell. The Seebeck coefficient of RuSe$_2$ exceeds -200 $μ$V/K around 730 K. Ir substitution results in the suppression of the resistivity and the Seebeck coefficient, suggesting the removal of the peaks in density of states near the Fermi level. Ru$_{0.8}$Ir$_{0.2}$Se$_{2}$ shows a semiconductor-metal crossover at about 30 K. The magnetic field restores the semiconducting behavior. Our results indicate the importance of the electronic correlations in enhanced thermoelectricity of RuSb$_{2}$.

cond-mat.str-el↗

arXiv2014

Imaging Dirac-Mass Disorder from Magnetic Dopant-Atoms in the Ferromagnetic Topological Insulator Cr$_x$(Bi$_{0.1}$Sb$_{0.9}$)$_{2-x}$Te$_3$

To achieve and utilize the most exotic electronic phenomena predicted for the surface states of 3D topological insulators (TI),it is necessary to open a "Dirac-mass gap" in their spectrum by breaking time-reversal symmetry. Use of magnetic dopant atoms to generate a ferromagnetic state is the most widely used approach. But it is unknown how the spatial arrangements of the magnetic dopant atoms influence the Dirac-mass gap at the atomic scale or, conversely, whether the ferromagnetic interactions between dopant atoms are influenced by the topological surface states. Here we image the locations of the magnetic (Cr) dopant atoms in the ferromagnetic TI Cr$_{0.08}$(Bi$_{0.1}$Sb$_{0.9}$)$_{1.92}$Te$_3$. Simultaneous visualization of the Dirac-mass gap $Δ(r)$ reveals its intense disorder, which we demonstrate directly is related to fluctuations in $n(r)$, the Cr atom areal density in the termination layer. We find the relationship of surface-state Fermi wavevectors to the anisotropic structure of $Δ(r)$ consistent with predictions for surface ferromagnetism mediated by those states. Moreover, despite the intense Dirac-mass disorder, the anticipated relationship $Δ(r)\propto n(r)$ is confirmed throughout, and exhibits an electron-dopant interaction energy $J^*$=145$meV\cdot nm^2$. These observations reveal how magnetic dopant atoms actually generate the TI mass gap locally and that, to achieve the novel physics expected of time-reversal-symmetry breaking TI materials, control of the resulting Dirac-mass gap disorder will be essential.

cond-mat.mtrl-sci↗

arXiv2014

Resonant Spin Tunneling in Randomly Oriented Nanospheres of Mn$_{12}$ Acetate

We report measurements and theoretical analysis of resonant spin tunneling in randomly oriented nanospheres of a molecular magnet. Amorphous nanospheres of Mn$_{12}$ acetate have been fabricated and characterized by chemical, infrared, TEM, X-ray, and magnetic methods. Magnetic measurements have revealed sharp tunneling peaks in the field derivative of the magnetization that occur at the typical resonant field values for Mn$_{12}$ acetate. Theoretical analysis is provided that explains these observations. We argue that resonant spin tunneling in a molecular magnet can be established in a powder sample, without the need for a single crystal and without aligning the easy magnetization axes of the molecules. This is confirmed by re-analyzing the old data on a powdered sample of non-oriented micron-size crystals of Mn$_{12}$ acetate. Our findings can greatly simplify the selection of candidates for quantum spin tunneling among newly synthesized molecular magnets.

cond-mat.mes-hall↗

arXiv2013

Cu(Ir$_{1-x}$Cr$_x$)$_2$S$_4$: a model system for studying nanoscale phase coexistence at the metal-insulator transition

Increasingly, nanoscale phase coexistence and hidden broken symmetry states are being found in the vicinity of metal-insulator transitions (MIT), for example, in high temperature superconductors, heavy fermion and colossal magnetoresistive materials, but their importance and possible role in the MIT and related emergent behaviors is not understood. Despite their ubiquity, they are hard to study because they produce weak diffuse signals in most measurements. Here we propose Cu(Ir$_{1-x}$Cr$_x$)$_2$S$_4$ as a model system, where robust local structural signals lead to key new insights. We demonstrate a hitherto unobserved coexistence of a Ir$^{4+}$ charge-localized dimer phase and Cr-ferromagnetism. The resulting phase diagram that takes into account the short range dimer order, is highly reminiscent of a generic MIT phase diagram similar to the cuprates. We suggest that the presence of quenched strain from dopant ions acts as an arbiter deciding between the competing ground states.

cond-mat.mtrl-sci↗

arXiv2013

Local Structural Evidence for Strong Electronic Correlations in LiRh$_2$O$_4$ Spinel

The local structure of the spinel LiRh$_2$O$_4$ has been studied using atomic pair distribution function (PDF) analysis of powder x-ray diffraction data. This measurement is sensitive to the presence of short Rh-Rh bonds that form due to dimerization of Rh$^{4+}$ ions on the pyrochlore sublattice, independent of the existence of long range order. We show that structural dimers exist in the low-temperature phase, as previously supposed, with a bond shortening of $Δr \sim 0.15$ Å. The dimers persist up to 350 K, well above the insulator-metal transition, with $Δr$ decreasing in magnitude on warming. Such behavior is inconsistent with the Fermi surface nesting-driven Peierls transition model. Instead, we argue that LiRh$_2$O$_4$ should properly be described as a strongly correlated system.

cond-mat.mtrl-sci↗

arXiv2010

Magnetic phase transition in V2O3 nanocrystals

V2O3 nanocrystals can be synthesized through hydrothermal reduction of VO(OH)2 using hydrazine as a reducing agent. Addition of different ligands to the reaction produces nanoparticles, nanorods and nanoplatelets of different sizes. Small nanoparticles synthesized in this manner show suppression of the magnetic phase transition to lower temperatures. Using muon spin relaxation spectroscopy and synchrotron x-ray diffraction, it is determined that the volume fraction of the high-temperature phase, characterized by a rhombohedral structure and paramagnetism, gradually declines with decreasing temperature, in contrast to the sharp transition observed in bulk V2O3.

cond-mat.str-el↗

arXiv2010

SrRietveld: A program for automating Rietveld refinements for high throughput powder diffraction studies

SrRietveld is a highly automated software toolkit for Rietveld refinement. Compared to traditional refinement programs, it is more efficient to use and easier to learn. It is designed for modern high throughput diffractometers and capable of processing large numbers of data-sets with minimal effort. The new software currently uses conventional Rietveld refinement engines, automating GSAS and FullProf refinements. However, as well as automating and extending many tasks associated with these programs, it is designed in a flexible and extensible way so that in the future these engines can be replaced with new refinement engines as they become available. SrRietveld is an open source software package developed in Python.

cond-mat.mtrl-sci↗

arXiv2009

Neutron powder diffraction atomic pair distribution function analysis using the ARCS chopper spectrometer at the Spallation Neutron Source

The frst neutron powder diffraction based atomic pair distribution functions (PDFs) are reported from the new wide angular-range chopper spectrometer ARCS at the Spallation Neutron Source at Oak Ridge National Laboratory. The spectrometer was run in white-beam mode, with no Fermi chopper. The PDF patterns of Si, Ni, and Al2O3 were refined using the PDFfit method and the results compared to data collected at the NPDF diffractometer at Los Alamos National Laboratory. The resulting fits are of high quality demonstrating that quantitatively reliable powder diffraction data can be obtained from ARCS when operated in this configuration.

cond-mat.mtrl-sci↗