High-quality Pr0.7Ca0.3MnO3/SrRuO3 superlattices with ultrathin layers were fabricated by pulsed laser deposition on SrTiO3 substrates. The superlattices were studied by atomically resolved scanning transmission electron microscopy, high-resolution transmission electron microscopy, resistivity and magnetoresistance measurements. The superlattices grew coherently without growth defects. Viewed along the growth direction, SrRuO3 and Pr0.7Ca0.3MnO3 layers were terminated by RuO2 and MnO2, respectively, which imposes a unique structure to their interfaces. Superlattices with a constant thickness of the SrRuO3 layers, but varying thickness of the Pr0.7Ca0.3MnO3 layers showed a change of crystalline symmetry of the SrRuO3 layers. At a low Pr0.7Ca0.3MnO3 layer thickness of 1.5 nm transmission electron microscopy proved the SrRuO3 layers to be orthorhombic, whereas these were non-orthorhombic for a Pr0.7Ca0.3MnO3 layer thickness of 4.0 nm. Angular magnetoresistance measurements showed orthorhombic (with small monoclinic distortion) symmetry in the first case and tetragonal symmetry of the SrRuO3 layers in the second case. Mechanisms driving this orthorhombic to tetragonal transition are briefly discussed.
A-122 pnictides (A an alkaline earth element) possess striped antiferromagnetic states of orthorhombic (OR) symmetry and nonmagnetic states of tetragonal (T) symmetry. Based on total energy calculations, we show that the T = 0K pressure-driven transition from OR to T states occurs at a pressure, $P_H$, where the tetragonal enthalpy drops below the orthorhombic. The OR state remains metastable up to a higher pressure, $P_M$ > $P_H$. We find anomalies in magnetism and orthorhombicity as $P \rightarrow P_M$, and a trend towards elastic instability.
EuAl4 possesses the BaAl4 crystal structure type with tetragonal symmetry I4/mmm. It undergoes a charge-density-wave (CDW) transition at TCDW = 145 K and it features four consecutive antiferromagnetic phase transitions below 16 K. Here, we use single-crystal x-ray diffraction to determine incommensurately modulated crystal structure of EuAl4 in its CDW state. The CDW is shown to be incommensurate with modulation wave vector q = (0, 0, 0.1781(3)) at 70 K. The symmetry of the incommensurately modulated crystal structure is orthorhombic with superspace group Fmmm(00σ)s00, where Fmmm is a subgroup…
High-quality Pr0.7Ca0.3MnO3/SrRuO3 superlattices were fabricated by pulsed laser deposition and were investigated by high-resolution transmission electron microscopy and SQUID magnetometry. Superlattices with orthorhombic and tetragonal SrRuO3 layers were investigated. The superlattices grew coherently; in the growth direction Pr0.7Ca0.3MnO3 layers were terminated by MnO2- and SrRuO3 layers by RuO2-planes. All superlattices showed antiferromagnetic interlayer coupling in low magnetic fields. The coupling strength was significantly higher for orthorhombic than for tetragonal symmetry of the SrR…
Using high resolution X-Ray diffraction (XRD) on high purity powders, we resolved the structure and $ab$ symmetry of the intriguing compound \svo$ $ from room temperature down to 20 K to an unprecedented level of accuracy. Upon cooling, this new set of data unambiguously reveals a second order phase transition lowering the symmetry from tetragonal to orthorhombic at a temperature $T_{c2}=136$ K. The observation of an orthorhombic distortion of the $ab$-plane is attributed to nematic phase formation supported by local Jahn-Teller (JT) dynamical instability. At $T_{N}=105$ K, spins order and at …
It is shown that a quasi two dimensional (layered) Heisenberg antiferromagnet with fully frustrated interplane couplings ({\it e.g.} on a body-centered tetragonal lattice) generically exhibits two thermal phase transitions with lowering temperature -- an upper transition at $T_{TO}$ (``order from disorder without order'') in which the lattice point-group symmetry is spontaneously broken, and a lower Néel transition at $T_{N}$ at which spin-rotation symmetry is broken. Although this is the same sequence of transitions observed in La$_2$CuO$_4$, in the Heisenberg model (without additional lattic…
Synchrotron x-ray diffraction experiments were performed on BaFe$_2$As$_2$ and Sr(Fe$_{1-x}$Co$_{x}$)$_2$As$_2$ single crystals as a function of temperature and applied magnetic field along the tetragonal $[1 \bar{1} 0]$ direction, complemented by electrical resistivity and specific heat experiments. For a BaFe$_2$As$_2$ crystal with spin-density-wave antiferromagnetic ordering temperature $T_{AF}=132.5$ K and onset of the orthorhombic phase at $T_{o}=137$ K, the magnetic field favors the growth of tetragonal domains that compete with orthorhombic ones for $T \gtrsim T_{AF}$. For a Sr(Fe$_{1-x…
$^{75}$As and $^{139}$La NMR results of LaFeAs(O$_{1-x}$F$_x$) ($x$=0, 0.025, and 0.04) were reported. Upon F-doping, the tetragonal-to-orthorhombic structural phase transition temperature $T_S$, antiferromagnetic transition temperature $T_N$ and internal magnetic field $μ_0H_{\rm int}$ are gradually reduced for $x<0.04$. However, at $x=0.04$, $T_N$ is abruptly suppressed to be 30 K along with a tiny $μ_0H_{\rm int}$, which is distinct from the continuous disappearance of the ordered phases in the Ba122 systems of Ba(Fe,Co)$_2$As$_2$ and BaFe$_2$(As,P)$_2$. The anisotropy of the spin-lattice r…
Understanding the interplay between nematicity, magnetism and superconductivity is pivotal for elucidating the physics of iron-based superconductors. Here we use neutron scattering to probe magnetic and nematic orders throughout the phase diagram of NaFe$_{1-x}$Ni$_x$As, finding that while both static antiferromagnetic and nematic orders compete with superconductivity, the onset temperatures for these two orders remain well-separated approaching the putative quantum critical points. We uncover local orthorhombic distortions that persist well above the tetragonal-to-orthorhombic structural tran…
We present uniaxial pressure structural relaxations for CaFe2As2 and BaFe2Ase2 within density functional theory and compare them with calculations under hydrostatic pressure conditions as well as available experimental results. We find that CaFe2As2 shows a unique phase transition from a magnetic orthorhombic phase to a nonmagnetic collapsed tetragonal phase for both pressure conditions and no indication of a tetragonal phase is observed at intermediate uniaxial pressures. In contrast, BaFe2As2 shows for both pressure conditions two phase transitions from a magnetic orthorhombic to a collapsed…
Results of in situ high pressure x-ray powder diffraction on the mixed valence compound Cs2Au(I)Au(III)I6 (CsAuI3) are reported, for pressures up to 21 GPa in a diamond anvil cell under hydrostatic conditions. We find a reversible pressure-induced tetragonal to orthorhombic structural transition at 5.5-6 GPa, and reversible amorphization at 12-14 GPa. Two alternative structures are proposed for the high-pressure orthorhombic phase, and are discussed in the context of a possible Au valence transition.
We report detailed thermal expansion and magnetostriction experiments on GdCoIn$_5$ and GdRhIn$_5$ single crystal samples that show a sudden change in the dilation at a field B$^\ast$ for temperatures below the Néel transition temperature TN. We present a first-principles model including crystal-field effects, dipolar and exchange interactions, and the dependence of the exchange couplings with lattice distortions in order to fully account for the magnetostriction and magnetic susceptibility data. The mean-field solution of the model shows that a transition between metastable states occurs at t…
We use neutron polarization analysis to study temperature dependence of the spin excitation anisotropy in BaFe$_2$As$_2$, which has a tetragonal-to-orthorhombic structural distortion at $T_s$ and antiferromagnetic (AF) phase transition at $T_N$ with ordered moments along the orthorhombic $a$-axis below $T_s\approx T_N\approx 136$ K. In the paramagnetic tetragonal state at 160 K, spin excitations are isotropic in spin space with $M_a=M_b=M_c$, where $M_a$, $M_b$, and $M_c$ are spin excitations polarized along the $a$, $b$, and $c$-axis directions of the orthorhombic lattice, respectively. On co…
We use polarized neutron scattering to demonstrate that in-plane spin excitations in electron doped superconducting BaFe1.904Ni0.096As2 (Tc=19.8 K) change from isotropic to anisotropic in the tetragonal phase well above the antiferromagnetic (AF) ordering and tetragonal-to-orthorhombic lattice distortion temperatures (Tn=Ts=33 K) without an uniaxial pressure. While the anisotropic spin excitations are not sensitive to the AF order and tetragonal-to-orthorhombic lattice distortion, superconductivity induces further anisotropy for spin excitations along the [1,1,0] and [1,-1,0] directions. These…
We use inelastic light scattering to study Sr$_{1-x}$Na$_x$Fe$_2$As$_2$ ($x\approx0.34$), which exhibits a robust tetragonal magnetic phase that restores the four-fold rotation symmetry inside the orthorhombic magnetic phase. With cooling, we observe splitting and recombination of an $E_g$ phonon peak upon entering the orthorhombic and tetragonal magnetic phases, respectively, consistent with the reentrant phase behavior. Our electronic Raman data reveal a pronounced feature that is clearly associated with the tetragonal magnetic phase, suggesting the opening of an electronic gap. No phonon ba…
Superlattices consist of two ferromagnets La0.7Sr0.3MnO3(LSMO)and SrRuO3(SRO) were grown in (110)-orientation on SrTiO3(STO) substrates. The x-ray diffraction and Raman spectra of these superlattices show the presence of in-plane compressive strain and orthorhombic structure of less than 4 u.c. thick LSMO spacer,respectively. Magnetic measurements reveal several features including reduced magnetization, enhanced coercivity, antiferromagnetic coupling, and switching from antiferromagnetic to ferromagnetic coupling with magnetic field orientations. These magnetic properties are explained by the …
We undertake a detailed high-resolution diffraction study of a novel plain band insulator, La$_2$MgO$_4$, which may be viewed as a structural surrogate system of the undoped end-member of the high-T$_c$ superconductors, La$_{2-x-y}$A$^{2+}_x$RE$^{3+}_y$CuO$_{4}$ (A = Ba, Sr, RE= Rare Earth). We find that La$_2$MgO$_4$ exhibits the infamous low-temperature orthorhombic (LTO) to low-temperature tetragonal (LTT) phase transition that has been linked to the suppression of superconductivity in a variety of underdoped cuprates, including the well known La$_{2-x}$Ba$_{x}$CuO$_4$ ($x=0.125$). Furtherm…
Magnetic interactions are generally believed to play a key role in mediating electron pairing for superconductivity in iron arsenides; yet their character is only partially understood. Experimentally, the antiferromagnetic (AF) transition is always preceded by or coincident with a tetragonal to orthorhombic structural distortion. Although it has been suggested that this lattice distortion is driven by an electronic nematic phase, where a spontaneously generated electronic liquid crystal state breaks the C4 rotational symmetry of the paramagnetic state, experimental evidence for electronic anis…
Measurements of the resistive properties and the lattice parameters of a (LaVO3)[6 unit cells]/(SrVO3)[1 unit cell] superlattice between 10K and room temperature are presented. A low temperature metallic phase compatible with a Fermi liquid behavior is evidenced. It disappears in the vicinity of a structural transition from a monoclinic to tetragonal phase, in which disorder seems to strongly influence the transport. Our results will enrich the understanding of the electronic properties of complex heterostructures.
We present an elaborate electron-spin resonance study of the low-energy dynamics and magnetization in the ordered phase of the magnetically frustrated spinel ZnCr$_2$O$_4$. We observe several resonance modes corresponding to different structural domains and found that the number of domains can be easily reduced by field-cooling the sample through the transition point. To describe the observed antiferromagnetic resonance spectra it is necessary to take into account an orthorhombic lattice distortion in addition to the earlier reported tetragonal distortion which both appear at the antiferromagn…
We report on the different roles of two orbital-active Fe$^{2+}$ at the A site and V$^{3+}$ at the B site in the magnetic excitations and on the anomalous spin wave broadening in FeV$_{2}$O$_{4}$. FeV$_{2}$O$_{4}$ exhibits three structural transitions and successive paramagnetic (PM)-collinear ferrimagnetic (CFI)-noncollinear ferrimagnetic (NCFI) transitions. The high-temperature tetragonal/PM -orthorhombic/CFI transition is accompanied by the appearance of an energy gap with a high magnitude in the magnetic excitations due to strong spin-orbit coupling induced anisotropy at the Fe$^{2+}$ site…
We study the order parameter for mixed-symmetry states involving a major $d_{x^2-y^2}$ state and various minor s-wave states ($s$, $s_{xy}$, and $s_{x^2+y^2}$) for different filling and temperature for mixing angles 0 and $π/2$. We employ a two-dimensional tight-binding model incorporating second-neighbor hopping for tetragonal and orthorhombic lattice. There is mixing for the symmetric $s$ state both on tetragonal and orthorhombic lattice. The $s_{xy}$ state mixes with the $d_{x^2-y^2}$ state only on orthorhombic lattice. The $s_{x^2+y^2}$ state never mixes with the $d_{x^2-y^2}$ state. The t…
The symmetry of the Bloch functions in the conduction band of tetragonal and orthorhombic La_2CuO_4 is examined for the existence of symmetry-adapted and optimally localizable (usual or spin-dependent) Wannier functions. It turns out that such Wannier functions do not exist in the tetragonal phase. In the orthorhombic phase, on the other hand, the Bloch functions can be unitarily transformed in three different ways into optimally localizable Wannier functions: they can be chosen to be adapted to each of the three phases observed in the pure or doped material, that is, to the antiferromagnetic …
Depending on the crystal growth conditions, an orthorhombic (O-type) or a tetragonal (T-type) structure can be found in the solid solution Cs2CuCl4-xBrx (0 < x < 4). Here we present measurements of the temperature-dependent magnetic susceptibility and isothermal magnetization on the T-type compounds x = 1.6 and 1.8 and compare these results with the magnetic properties recently derived for the O-type variant by Cong et al., Phys. Rev. B 83, 064425 (2011). The systems were found to exhibit quite dissimilar magnetic properties which can be assigned to differences in the Cu coordination in these …
An interface modification of LCMO-BTO superlattices was found to massively influence magnetic and magnetotransport properties. Moreover it determines the crystal structure of the manganite layers, changing it from orthorhombic (Pnma) for the conventional superlattice (cSL), to rhombohedral (R-3c) for the modified one (mSL). While the cSL shows extremely nonlinear ac transport, the mSL is an electrically homogeneous material. The observations go beyond an oversimplified picture of dead interface layers and evidence the importance of electronic correlations at perovskite interfaces.
We show that the introduction of frustration into the spin-1/2 two-dimensional (2D) antiferromagnetic Heisenberg model on a square lattice via a next-nearest neighbor exchange interaction can lead to a Peierls-like transition, from a tetragonal to an orthorhombic phase, when the spins are coupled to adiabatic phonons. The two different orthorhombic ground states define an Ising order parameter, which is expected to lead to a finite temperature transition. Implications for ${\rm Li_2VOSiO_4}$, the first realization of that model, will be discussed.
With decreasing temperature Sr$_2$VO$_4$ undergoes two structural phase transitions, tetragonal-to-orthorhombic-to-tetragonal, without long-range magnetic order. Recent experiments suggest, that only at very low temperature Sr$_{2}$VO$_{4}$ might enter some, yet unknown, phase with long-range magnetic order, but without orthorhombic distortion. By combining relativistic density functional theory with an extended spin-1/2 compass-Heisenberg model we find an antiferromagnetic single-stripe ground state with highly competing exchange interactions, involving a non negligible inter-layer coupling, …
The Sr concentration dependence of the structural transition from the orthorhombic into the tetragonal low-temperature phase in rare-earth-doped (R = Nd, Eu) La_{2-x-y}Sr_xR_yCuO_4 has been studied in detail. Independently of the rare earth concentration the transition temperature is strongly reduced at x ~ 0.05. We give a qualitative argument that the effect can be attributed to the Coulomb repulsion between doped carriers. We find the enthalpy jump at the low-temperature transition to scale transition temperature between the high-temperature tetragonal and the orthorhombic phase. This effect…
Iron-based superconductors are well-known for their intriguing phase diagrams, which manifest a complex interplay of electronic, magnetic and structural degrees of freedom. Among the phase transitions observed are superconducting, magnetic, and several types of structural transitions, including a tetragonal-to-orthorhombic and a collapsed-tetragonal transition. In particular, the widely-observed tetragonal-to-orthorhombic transition is believed to be a result of an electronic order that is coupled to the crystalline lattice and is, thus, referred to as nematic transition. Nematicity is therefo…
We found, using density-functional theory calculations within the generalized gradient approximation, that Cs$_2$AgF$_4$ is stabilized in the insulating orthorhombic phase rather than in the metallic tetragonal phase. The lattice distortion present in the orthorhombic phase corresponds to the $x^2-z^2$/$y^2-z^2$ hole-orbital ordering of the Ag$^{2+}$ $4d^9$ ions, and this orbital ordering leads to the observed ferromagnetism, as confirmed by the present total-energy calculations. This picture holds in the presence of moderate 4d-electron correlation. The results are compared with the picture o…
The interplay between magnetism and crystal structures in three CaFe$_{2}$As$_{2}$ samples is studied. For the nonmagnetic quenched crystals, different crystalline domains with varying lattice parameters are found, and three phases (orthorhombic, tetragonal, and collapsed tetragonal) coexist between T$_{S}$ = 95 K and 45 K. Annealing of the quenched crystals at 350°C leads to a strain relief through a large (~1.3 %) expansion of the c-parameter and a small (~0.2 %) contraction of the a-parameter, and to local ~0.2 Å displacements at the atomic-level. This annealing procedure results in the mos…
We have performed high resolution x-ray scattering measurements on single crystal samples of Ba(Fe(1-x)Cr(x))2As2 (x = 0 to 0.335). These measurements examine the effect of Cr-doping on the high temperature tetragonal (I4/mmm) to low temperature orthorhombic (Fmmm) structural phase transition of the parent compound BaFe2As2. Increasing Cr concentration is found to suppress the structural transition temperature (Ts), and reduce the magnitude of the orthorhombic strain (delta). The doping dependence of the orthorhombic strain, combined with complementary measurements of the high temperature magn…
FeSe undergoes a transition from a tetragonal to a slightly orthorhombic phase at 90\,K, and becomes a superconductor below 8\,K. The orthorhombic phase is sometimes called a nematic phase because quantum oscillation, neutron, and other measurements detect a significant asymmetry in $x$ and $y$. How nematicity affects superconductivity has recently become a matter of intense speculation. Here we employ an advanced \emph{ab-initio} Green's function description of superconductivity and show that bulk tetragonal FeSe would, in principle, superconduct with almost the same T$_{c}$ as the nematic ph…
We study the crystal structure of the tetragonal iron selenide FeSe and its nematic phase transition to the low-temperature orthorhombic structure using synchrotron x-ray and neutron scattering analyzed in both real and reciprocal space. We show that in the local structure the orthorhombic distortion associated with the electronically driven nematic order is more pronounced at short length scales. It also survives up to temperatures above 90 K where reciprocal-space analysis suggests tetragonal symmetry. Additionally, the real-space pair distribution function analysis of the synchrotron x-ray …
Room temperature charge density wave in a tetragonal polymorph of Gd2Os3Si5 and study of its origin in the RE2T3X5 (RE = Rare earth, T = transition metal, X = Si, Ge) series
TThe parent compounds of iron-arsenide superconductors, $A$Fe$_{2}$As$_{2}$ ($A$=Ca, Sr, Ba), undergo a tetragonal to orthorhombic structural transition at a temperature $T_{\mathrm{TO}}$ in the range 135 to 205K depending on the alkaline earth element. Below $T_{\mathrm{TO}}$ the free standing crystals split into equally populated structural domains, which mask intrinsic, in-plane, anisotropic properties of the materials. Here we demonstrate a way of mechanically detwinning CaFe$_{2}$As$_{2}$ and BaFe$_{2}$As$_{2}$. The detwinning is nearly complete, as demonstrated by polarized light imaging…
The structure and interface characteristics of (LaVO3)6m(SrVO3)m superlattices deposited on (100)-SrTiO3 (STO) substrate were studied using Transmission Electron Microscopy (TEM). Cross-section TEM studies revealed that both LaVO3 (LVO) and SrVO3 (SVO) layers are good single crystal quality and epitaxially grown with respect to the substrate. It is evidenced that LVO layers are made of two orientational variants of a distorted perovskite compatible with bulk LaVO3 while SVO layers suffers from a tetragonal distortion due to the substrate induced stain. Electron Energy Loss Spectroscopy (EELS) …
Magneto-structural phase transitions in Ba1-xAxFe2As2 (A = K, Na) materials are discussed for both magnetically and orbitally driven mechanisms, using a symmetry analysis formulated within the Landau theory of phase transitions. Both mechanisms predict identical orthorhombic space-group symmetries for the nematic and magnetic phases observed over much of the phase diagram, but they predict different tetragonal space-group symmetries for the newly discovered re-entrant tetragonal phase in Ba1-xNaxFe2As2 (x ~ 0.24-0.28). In a magnetic scenario, magnetic order with moments along the c-axis, as fo…
Single crystals of Ca(Fe1-xRux)2As2 (0<x<0.065) and Ca1-yLay(Fe0.973Ru0.027)2As2 (0<y<0.2) have been synthesized and studied with respect to their structural, electronic and magnetic properties. The partial substitution of Fe by Ru induces a decrease of the c-axis constant leading for x<0.023 to a suppression of the coupled magnetic and structural (tetragonal to orthorhombic) transitions. At x_cr=0.023 a first order transition to a collapsed tetragonal (CT) phase is found, which behaves like a Fermi liquid and which is stabilized by further increase of x. The absence of superconductivity near …
