arXiv subjects

Andreas Kreyssig

Publications and source records attributed to Andreas Kreyssig.

At least 19 recordsLinked to original sources

arXiv2026

Synthetic control over marcasite-pyrite polymorph formation in the Fe1-xCoxSe2 series

Transition-metal dichalcogenides of the pyrite-marcasite family are model systems of crystal chemistry. A few of these show polymorphism. The theoretical ground state of CoSe2 is marcasite, but the material is typically synthesized in the pyrite structure. Polymorphism has been observed in nanoparticles and synthetic control of the polymorphs of CoSe2 has not been achieved. We have synthesized material libraries of the Fe1-xCoxSe2 series by combining combinatorial deposition and ex-situ selenization. The approach allows to efficiently explore substitution ranges and crystal structures that form for different synthesis conditions. We find that higher levels of Co content x within the marcasite structure are possible when synthesizing at low temperatures. At a synthesis temperature of only 250° C, we have successfully synthesized marcasite CoSe2 as the majority phase. Density functional theory simulations reveal that the two isomorphs of CoSe2 are extremely close in energy and that the orthorhombic phase is the energetic ground state. Our experimental and theoretical data show that the marcasite structure is the equilibrium phase of Fe1-xCoxSe2 in the entire composition range.

cond-mat.mtrl-sci↗

arXiv2025

Magnetism and Peierls distortion in Dirac semimetal CaMnBi$_2$

Dirac semimetals of the form $A$Mn$X_2$ ($A =$ alkaline-earth or divalent rare earth; $X =$ Bi, Sb) host conducting square-net Dirac-electron layers of $X$ atoms interleaved with antiferromagnetic Mn$X$ layers. In these materials, canted antiferromagnetism can break time-reversal symmetry (TRS) and produce a Weyl semimetallic state. CaMnBi$_2$ was proposed to realize this behavior below $T^{*}\sim 50$ K, where anomalies in resistivity and optical conductivity were reported. We investigate single-crystal CaMnBi$_{2}$ using polarized and unpolarized neutron diffraction, x-ray diffraction, and density functional theory (DFT) calculations to elucidate the underlying crystal and magnetic structures. The results show that the observed anomalies do not originate from spin canting or weak ferromagnetism; no measurable uniform Mn spin canting is detected. Instead, CaMnBi$_2$ undergoes a coupled structural and magnetic symmetry-lowering transition at $T^{*} = 46(2)$ K, from a tetragonal lattice with C-type antiferromagnetism to an orthorhombic phase with unit-cell doubling along the $c$ axis and minimal impact on magnetism. Analysis of superlattice peak intensities and lattice distortion reveals a continuous second-order transition governed by a single order parameter. The refined atomic displacements correspond to a zigzag bond-order-wave (BOW) modulation of Bi-Bi bonds, consistent with an electronically driven Peierls-type instability in the Dirac-electron Bi layer, long anticipated by Hoffmann and co-workers [W.~Tremel and R.~Hoffmann, \textit{J. Am. Chem. Soc.} \textbf{109}, 124 (1987); G.~A.~Papoian and R.~Hoffmann, \textit{Angew. Chem. Int. Ed.} \textbf{39}, 2408 (2000)]. %\textcite{TremelHoffman_JACS1987} [JACS {\bf 109}, 124 (1987)].

cond-mat.mtrl-sci↗

arXiv2022

Weak itinerant magnetic phases of La2Ni7

La2Ni7 is an intermetallic compound that is thought to have itinerant magnetism with a small moment ordering below 65 K. A recent study of single crystal samples by Ribeiro et. al. [Phys. Rev. B 105, 014412 (2022)] determined detailed anisotropic H-T phase diagrams and revealed three zero-field magnetic phase transitions at T1 ~ 61.0 K, T2 ~ 56.5K, and T3 ~ 42 K. In that study only the highest temperature phase is shown to have a clear ferromagnetic component. Here we present a single crystal neutron diffraction study determining the propagation vector and magnetic moment direction of the three magnetically ordered phases, two incommensurate and one commensurate, as a function of temperature. The higher temperature phases have similar, incommensurate propagation vectors, but with different ordered moment directions. At lower temperatures the magnetic order becomes commensurate with magnetic moments along the c direction as part of a first-order magnetic phase transition. We find that the low-temperature commensurate magnetic order is consistent with a proposal from earlier DFT calculations.

cond-mat.str-el↗

arXiv2021

A Low Temperature Structural Transition in Canfieldite, Ag$_8$SnS$_6$, Single Crystals

Canfieldite, Ag$_8$SnS$_6$, is a semiconducting mineral notable for its high ionic conductivity, photosensitivity, and low thermal conductivity. We report the solution growth of large single crystals of Ag$_8$SnS$_6$ of mass up to 1 g from a ternary Ag-Sn-S melt. On cooling from high temperature, Ag$_8$SnS$_6$ undergoes a known cubic (F-43m) to orthorhombic (Pna2$_1$) phase transition at $\approx$ 460 K. By studying the magnetization and thermal expansion between 5-300 K, we discover a second structural transition at $\approx$ 120 K. Single crystal X-ray diffraction reveals the low temperature phase adopts a different orthorhombic structure with space group Pmn2$_1$ (a = 7.6629(5) Å, b = 7.5396(5) Å, c = 10.6300(5) Å, Z = 2 at 90 K) that is isostructural to the room temperature forms of the related Se-based compounds Ag$_8$SnSe$_6$ and Ag$_8$GeSe$_6$. The 120 K transition is first-order and has a large thermal hysteresis. Based on magnetization and thermal expansion data, the room temperature polymorph can be kinetically arrested into a metastable state by rapidly cooling to temperatures below 40 K. We lastly compare the room and low temperature forms of Ag$_8$SnS$_6$ with its argyrodite analogues, Ag$_8$TQ$_6$ (T = Si, Ge, Sn; Q = S, Se), and identify a trend relating the preferred structures to the unit cell volume, suggesting smaller phase volume favors the Pna2$_1$ arrangement. We support this picture by showing that the transition to the Pmn2$_1$ phase is avoided in Ge alloyed Ag$_8$Sn$_{1-x}$Ge$_x$S$_6$ samples as well as pure Ag$_8$GeS$_6$.

cond-mat.mtrl-sci↗

arXiv2020

Formation of short-range magnetic order and avoided ferromagnetic quantum criticality in pressurized LaCrGe$_3$

LaCrGe$_3$ has attracted attention as a paradigm example of the avoidance of ferromagnetic (FM) quantum criticality in an itinerant magnet. By combining thermodynamic, transport, x-ray and neutron scattering as well as $μ$SR measurements, we refined the temperature-pressure phase diagram of LaCrGe$_3$. We provide thermodynamic evidence (i) for the first-order character of the FM transition when it is suppressed to low temperatures and (ii) for the formation of new phases at high pressures. From our microscopic data, we infer that short-range FM ordered clusters exist in these high-pressure phases. These results suggest that LaCrGe$_3$ is a rare example, which fills the gap between the two extreme limits of avoided FM quantum criticality in clean and strongly disordered metals.

cond-mat.str-el↗

arXiv2020

Evidence for large Rashba splitting in PtPb4 from Angle-Resolved Photoemission Spectroscopy

We studied the electronic structure of PtPb$_{4}$ using laser angle-resolved photoemission spectroscopy(ARPES) and density functional theory(DFT) calculations. This material is closely related to PtSn$_{4}$, which exhibits exotic topological properties such as Dirac node arcs. Fermi surface(FS) of PtPb$_{4}$ consists of two electron pockets at the center of the Brillouin zone(BZ) and several hole pockets around the zone boundaries. Our ARPES data reveals significant Rashba splitting at the $Γ$ point in agreement with DFT calculations. The presence of Rashba splitting may render this material of potential interest for spintronic applications.

cond-mat.mtrl-sci↗

arXiv2019

Superelasticity and Cryogenic Linear Shape Memory Effects of CaFe2As2

Shape memory materials have the ability to recover their original shape after a significant amount of deformation when they are subjected to certain stimuli, for instance, heat or magnetic fields. However, their performance is often limited by the energetics and geometry of the martensitic-austenitic phase transformation. Here, we report a unique shape memory behavior in CaFe2As2, which exhibits superelasticity with over 13% recoverable strain, over 3 GPa yield strength, repeatable stress-strain response even at the micrometer scale, and cryogenic linear shape memory effects near 50 K. These properties are acheived through a reversible uni-axial phase transformation mechanism, the tetragonal/orthorhombic-to-collapsed-tetragonal phase transformation. Our results offer the possibility of developing cryogenic linear technologies with a high precision and high actuation power per-unit-volume for deep space exploration, and more broadly, suggest a mechanistic path to a class of shape memory materials, ThCr2Si2-structured intermetallic compounds.

cond-mat.mtrl-sci↗

arXiv2019

Crystal growth, microstructure and physical properties of SrMnSb$_2$

We report on the crystal and magnetic structures, magnetic, and transport properties of SrMnSb$_2$ single crystals grown by the self-flux method. Magnetic susceptibility measurements reveal an antiferromagnetic (AFM) transition at $T_{\rm N} = 295(3)$ K. Above $T_{\rm N}$, the susceptibility slightly increases and forms a broad peak at $T \sim 420$ K, which is a typical feature of two-dimensional magnetic systems. Neutron diffraction measurements on single crystals confirm the previously reported C-type AFM structure below $T_{\rm N}$. Both de Haas-van Alphen (dHvA) and Shubnikov-de Haas (SdH) effects are observed in SrMnSb$_2$ single crystals. Analysis of the oscillatory component by a Fourier transform shows that the prominent frequencies obtained by the two different techniques are practically the same within error regardless of sample size or saturated magnetic moment. Transmission electron microscopy (TEM) reveals the existence of stacking faults in the crystals, which result from a horizontal shift of Sb atomic layers suggesting possible ordering of Sb vacancies in the crystals. Increase of temperature in susceptibility measurements leads to the formation of a strong peak at $T \sim {570}$ K that upon cooling under magnetic field the susceptibility shows a ferromagnetic transition at $T_{\rm C} \sim 580$ K. Neutron powder diffraction on crushed single-crystals does not support an FM phase above $T_{\rm N}$. Furthermore, X-ray magnetic circular dichroism (XMCD) measurements of a single crystal at the $L_{2,3}$ edge of Mn shows a signal due to induced canting of AFM moments by the applied magnetic field. All evidence strongly suggests that a chemical transformation at the surface of single crystals occurs above 500 K concurrently producing a minute amount of ferromagnetic impurity phase.

cond-mat.mtrl-sci↗

arXiv2018

Distinct pressure evolution of coupled nematic and magnetic order in FeSe

FeSe, despite being the structurally simplest compound in the family of iron-based superconductors, shows an astoundingly rich interplay of physical phenomena including nematicity and pressure-induced magnetism. Here, we present a microscopic study of these two phenomena by high-energy x-ray diffraction and time-domain Mössbauer spectroscopy on FeSe single crystals over a wide temperature and pressure range. The topology of the pressure-temperature phase diagram is a surprisingly close parallel to the well-known doping-temperature phase diagram of BaFe2As2 generated through partial Fe/Co and Ba/Na substitution. In FeSe with pressure p as a control parameter, the magneto-structural ground state can be tuned from "pure" nematic - paramagnetic with an orthorhombic lattice distortion - through a strongly coupled magnetically ordered and orthorhombic state to a magnetically ordered state without an orthorhombic lattice distortion. The magnetic hyperfine field increases monotonically over a wide pressure range. However, the orthorhombic distortion initially decreases under increasing pressure, but is stabilized by cooperative coupling to the pressure-induced magnetic order. Close to the reported maximum of the superconducting critical temperature Tc (occuring at p = 6.8 GPa), the orthorhombic distortion suddenly disappears and FeSe remains tetragonal down to the lowest temperature measured. Analysis of the structural and magnetic order parameters suggests an independent origin of the structural and magnetic ordering phenomena, and their cooperative coupling leads to the similarity with the canonical phase diagram of iron pnictides.

cond-mat.supr-con↗

arXiv2017

Collapsed Tetragonal Phase Transition in LaRu$_2$P$_2$

The structural properties of LaRu$_2$P$_2$ under external pressure have been studied up to 14 GPa, employing high-energy x-ray diffraction in a diamond-anvil pressure cell. At ambient conditions, LaRu$_2$P$_2$ (I4/mmm) has a tetragonal structure with a bulk modulus of $B=105(2)$ GPa and exhibits superconductivity at $T_c= 4.1$ K. With the application of pressure, LaRu$_2$P$_2$ undergoes a phase transition to a collapsed tetragonal (cT) state with a bulk modulus of $B=175(5)$ GPa. At the transition, the c-lattice parameter exhibits a sharp decrease with a concurrent increase of the a-lattice parameter. The cT phase transition in LaRu$_2$P$_2$ is consistent with a second order transition, and was found to be temperature dependent, increasing from $P=3.9(3)$ GPa at 160 K to $P=4.6(3)$ GPa at 300 K. In total, our data are consistent with the cT transition being near, but slightly above 2 GPa at 5 K. Finally, we compare the effect of physical and chemical pressure in the RRu$_2$P$_2$ (R = Y, La-Er, Yb) isostructural series of compounds and find them to be analogous.

cond-mat.supr-con↗

arXiv2017

Direct visualization of phase separation between superconducting and nematic domains in Co-doped CaFe2As2 close to a first order phase transition

We show that biaxial strain induces alternating tetragonal superconducting and orthorhombic nematic domains in Co substituted CaFe2As2. We use Atomic Force, Magnetic Force and Scanning Tunneling Microscopy (AFM, MFM and STM) to identify the domains and characterize their properties, finding in particular that tetragonal superconducting domains are very elongated, more than several tens of micron long and about 30 nm wide, have the same Tc than unstrained samples and hold vortices in a magnetic field. Thus, biaxial strain produces a phase separated state, where each phase is equivalent to what is found at either side of the first order phase transition between antiferromagnetic orthorhombic and superconducting tetragonal phases found in unstrained samples when changing Co concentration. Having such alternating superconducting domains separated by normal conducting domains with sizes of order of the coherence length opens opportunities to build Josephson junction networks or vortex pinning arrays and suggests that first order quantum phase transitions lead to nanometric size phase separation under the influence of strain.

cond-mat.supr-con↗

arXiv2017

Dynamic Elastoresistivity Evidence for Slow Nematic Fluctuations in BaFe$_2$As$_2$

An instrumentation problem with the signal acquisition at high frequencies was discovered and we no longer believe that the experimental data presented in the manuscript, showing a frequency enhancement of the elastoresistivity, are correct. After correcting the problem, the elastoresistivity data is frequency independent in the range investigated. Therefore, the authors have withdrawn this submission. We would like to thank Alex Hristov, Johanna Palmstrom, Josh Straquadine and Ian Fisher (Stanford) for the kind discussions and assistance we received which helped us identify these problems.

cond-mat.str-el↗

arXiv2017

Pressure induced half-collapsed-tetragonal phase in CaKFe$_4$As$_4$

We report the temperature-pressure phase diagram of CaKFe$_4$As$_4$ established using high pressure electrical resistivity, magnetization and high energy x-ray diffraction measurements up to 6 GPa. With increasing pressure, both resistivity and magnetization data show that the bulk superconducting transition of CaKFe$_4$As$_4$ is suppressed and then disappears at $p$ $\gtrsim$ 4 GPa. High pressure x-ray data clearly indicate a phase transition to a collapsed tetragonal phase in CaKFe$_4$As$_4$ under pressure that coincides with the abrupt loss of bulk superconductivity near 4 GPa. The x-ray data, combined with resistivity data, indicate that the collapsed tetragonal transition line is essentially vertical, occuring at 4.0(5) GPa for temperatures below 150 K. Band structure calculations also find a sudden transition to a collapsed tetragonal state near 4 GPa, as As-As bonding takes place across the Ca-layer. Bonding across the K-layer only occurs for $p$ $\geq$ 12 GPa. These findings demonstrate a new type of collapsed tetragonal phase in CaKFe$_4$As$_4$: a half-collapsed-tetragonal phase.

cond-mat.supr-con↗

arXiv2016

Unconventional superconductors: Iron-based diversity

Nine years ago, superconductors based on the magnetic element iron were discovered. A flurry of research activity has revealed an unprecedented diversity of chemical structures and physical properties. Similarly to other unconventional superconductors, stripe-type antiferromagnetism seems to play an important role. Particularly interesting is its strong coupling to the crystal lattice. The systematic comparison of different compounds may allow to identify key elements in the mechanism of superconductivity and provide guidelines for the search for new and better superconductors.

cond-mat.supr-con↗

arXiv2014

Magnetic and transport properties of i-$R$-Cd icosahedral quasicrystals ($R$ = Y, Gd-Tm)

We present a detailed characterization of the recently discovered i-$R$-Cd ($R$ = Y, Gd-Tm) binary quasicrystals by means of x-ray diffraction, temperature-dependent dc and ac magnetization, temperature-dependent resistance and temperature-dependent specific heat measurements. Structurally, the broadening of x-ray diffraction peaks found for i-$R$-Cd is dominated by frozen-in phason strain, which is essentially independent of $R$. i-Y-Cd is weakly diamagnetic and manifests a temperature-independent susceptibility. i-Gd-Cd can be characterized as a spin-glass below 4.6 K via dc magnetization cusp, a third order non-linear magnetic susceptibility peak, a frequency-dependent freezing temperature and a broad maximum in the specific heat. i-$R$-Cd ($R$ = Ho-Tm) is similar to i-Gd-Cd in terms of features observed in thermodynamic measurements. i-Tb-Cd and i-Dy-Cd do not show a clear cusp in their zero-field-cooled dc magnetization data, but instead show a more rounded, broad local maximum. The resistivity for i-$R$-Cd is of order 300 $μΩ$ cm and weakly temperature-dependent. The characteristic freezing temperatures for i-$R$-Cd ($R$ = Gd-Tm) deviate from the de Gennes scaling, in a manner consistent with crystal electric field splitting induced local moment anisotropy.

cond-mat.mtrl-sci↗

arXiv2013

i-R-Cd (R = Gd - Tm, Y): A new family of binary magnetic icosahedral quasicrystals

"Seek and ye shall find, the unsought shall go undetected." This adage, attributed to Aristophanes' can be considered one of the defining mantras of new materials research; if you don't look, you certainly will not discover. As a result of our recent discovery of the binary quasicrystalline phase i-Sc12Zn88 we proposed that there may well be other binary quasicrystalline phases lurking nearby known crystalline approximants, perhaps as peritectally forming compounds with very limited liquidus surfaces, offering greatly reduced ranges of composition/temperature for primary solidification. Here we report that, as the adage goes, we have found. Indeed, adjacent to the RCd6, cubic approximate structure, we have discovered the long sought after model system for magnetic quasicrystals: a new family of at least seven rare earth icosahedral quasicrystals: i-R-Cd for R = Gd - Tm, Y, six of which now form the known set of moment bearing, binary quasicrystals.

cond-mat.mtrl-sci↗

arXiv2009

Similarities between structural distortions under pressure and chemical doping in superconducting BaFe2As2

The discovery of a new family of high Tc materials, the iron arsenides (FeAs), has led to a resurgence of interest in superconductivity. Several important traits of these materials are now apparent, for example, layers of iron tetrahedrally coordinated by arsenic are crucial structural ingredients. It is also now well established that the parent non-superconducting phases are itinerant magnets, and that superconductivity can be induced by either chemical substitution or application of pressure, in sharp contrast to the cuprate family of materials. The structure and properties of chemically substituted samples are known to be intimately linked, however, remarkably little is known about this relationship when high pressure is used to induce superconductivity in undoped compounds. Here we show that the key structural features in BaFe2As2, namely suppression of the tetragonal to orthorhombic phase transition and reduction in the As-Fe-As bond angle and Fe-Fe distance, show the same behavior under pressure as found in chemically substituted samples. Using experimentally derived structural data, we show that the electronic structure evolves similarly in both cases. These results suggest that modification of the Fermi surface by structural distortions is more important than charge doping for inducing superconductivity in BaFe2As2.

cond-mat.supr-con↗

arXiv2009

Magnetic and lattice coupling in single-crystal SrFe$_2$As$_2$: A neutron scattering study

A detailed elastic neutron scattering study of the structural and magnetic phase transitions in single-crystal SrFe$_2$As$_2$ reveals that the orthorhombic (O)-tetragonal (T) and the antiferromagnetic transitions coincide at $T_\texttt{O}$ = $T_\texttt{N}$ = (201.5 $\pm$ 0.25) K. The observation of coexisting O-T phases over a finite temperature range at the transition and the sudden onset of the O distortion provide strong evidences that the structural transition is first order. The simultaneous appearance and disappearance within 0.5 K upon cooling and within 0.25 K upon warming, respectively, indicate that the magnetic and structural transitions are intimately coupled. We find that the hysteresis in the transition temperature extends over a 1-2 K range. Based on the observation of a remnant orthorhombic phase at temperatures higher than \emph{T}$_\texttt{O}$, we suggest that the T-O transition may be an order-disorder transition.

cond-mat.str-el↗