We report high-resolution dilatometry on high-quality single crystals of NiTiO3 grown by means of the optical floating-zone technique. The anisotropic magnetic phase diagram is constructed from thermal expansion and magnetostriction studies up to B=15T and magnetization studies in static (15T) and pulsed (60T) magnetic fields. Our data allow to quantitatively study magneto-elastic coupling and to determine uniaxial pressure dependencies. While the entropy changes are found to be of magnetic nature, Grüneisen analysis implies only one relevant energy scale in the whole low-temperature regime. Thereby, our data suggest that the observed structural changes due to magneto-elastic coupling and previously reported magnetodielectric coupling[1] are driven by the same $magnetic$ degrees of freedom that lead to long-range magnetic order in NiTiO3, which in turn, establishes a linear magnetodielectric coupling in this compound.
We report on structural, magnetic and magnetocaloric properties of MnxFe1.95-xP0.50Si0.50 (x > 1.10) compounds. With increasing the Mn:Fe ratio, a first-order magneto-elastic transition gradually changes into a first-order magneto-structural transition via a second-order magnetic transition. The study also shows that thermal hysteresis can be tuned by varying the Mn:Fe ratio. Small thermal hysteresis (less than 1 K) can be obtained while maintaining a giant magnetocaloric effect. This achievement paves the way for real refrigeration applications using magnetic refrigerants.
Structural, magnetic and magnetocaloric properties of Fe2P-based Mn-Fe-P-Si compounds were investigated. The study reveals a large magneto-elastic coupling that starts to develop in the paramagnetic state and grows when the ferromagnetic transition temperature is approached. Based on the behavior of the magneto-elastic coupling, we show the thermal evolution of the magnetic moments. On cooling, magnetic moments on the tetrahedral site form and gradually increase in the paramagnetic state. At the magnetic ordering temperature the moments attain a much larger value in a discontinuous step. We al…
We have studied the magneto-elastic coupling in the double layered Mn perovskite La$_{1.2}$Sr$_{1.8}$Mn$_2$O$_7$ with an ultrasonic velocity technique. The temperature profile of both the in-plane and out-of-plane longitudinal velocities showed a large stiffening anomaly below the insulating paramagnetic to metallic ferromagnetic transition. Magnetic fluctuations effects consistent with the layered structure are evidenced as a frequency dependent velocity softening above the transition. The magneto-elastic coupling has been studied in magnetic field values up to 8 Tesla: the observations are c…
We have used in-field neutron and X-ray single crystal diffraction to measure the incommensurability δ of the crystal and magnetic structure of multiferroic TbMnO3 . We show that the flop in the electric polarization at the critical field HC, for field H along the a− and b−axis coincides with a 1st order transition to a commensurate phase with propagation vector κ = (0, 1/4, 0). In-field X-ray diffraction measurements show that the quadratic magneto-elastic coupling breaks down with applied field as shown by the observation of the 1st harmonic lattice reflections above an…
Using high resolution neutron diffraction and capacitance dilatometry we show that the thermal evolution of the helimagnetic state in CoMnSi is accompanied by a change in inter-atomic distances of up to 2%, the largest ever found in a metallic magnet. Our results and the picture of competing exchange and strongly anisotropic thermal expansion that we use to understand them sheds light on a new mechanism for large magnetoelastic effects that does not require large spin-orbit coupling.
We use neutron diffraction, magnetometry and low temperature heat capacity to probe giant magneto-elastic coupling in CoMnSi-based antiferromagnets and to establish the origin of the entropy change that occurs at the metamagnetic transition in such compounds. We find a large difference between the electronic density of states of the antiferromagnetic and high magnetisation states. The magnetic field-induced entropy change is composed of this contribution and a significant counteracting lattice component, deduced from the presence of negative magnetostriction. In calculating the electronic entr…
We present results of ultrasonic measurements on a single crystal of the distorted diamond-chain compound azurite Cu$_3$(CO$_3$)$_2$(OH)$_2$. Pronounced elastic anomalies are observed in the temperature dependence of the longitudinal elastic mode $c_{22}$ which can be assigned to the relevant magnetic interactions in the system and their couplings to the lattice degrees of freedom. From a quantitative analysis of the magnetic contribution to $c_{22}$ the magneto-elastic coupling $G$ = $\partial J_2$/$\partial ε_b$ can be determined, where $J_2$ is the intra-dimer coupling constant and $ε_b$ th…
The Landau theory was applied to treat the phase diagrams for a multiferroic with two second order phase transitions taking into account the coupling of the primary order parameters with strain. Two order parameters are coupled biquadratically which corresponds to the magnetoelectric materials. The coupling with strain is assumed to be linear in strain and quadratic in order parameters. Three ordered phases are discussed. Analytic relationships were obtained for the phase transition temperatures and for elastic modulus changes through the phase transitions. Strong influence of the coupling wit…
The antiferromagnet Mn$_5$Si$_3$ has recently attracted attention because a noncollinear spin arrangement has been shown to produce a topological anomalous Hall effect and an inverse magnetocaloric effect. Here we synthesize single crystals of Mn$_5$Si$_3$ using flux growth. We determine the phase diagram through magnetization and measure the magnetoresistance and the Hall effect. We find the collinear and noncollinear antiferromagnetic phases at low temperatures and, in addition, a third magnetic phase, in between the two antiferromagnetic phases which has ferromagnetic character. The latter …
Within the random phase approximation to the spin-Peierls transition two parameter regimes of phonon softening and hardening are present. Magneto-elastic excitations are discussed in detail for phonons coupled to the exactly solvable model of XY spin chains for both regimes, leading to a modified interpretation of the 30 cm$^{-1}$ mode in CuGeO$_3$. Frustrated Heisenberg chains coupled to phonons satisfactory describe the pre-transitional quasi-elastic scattering in CuGeO$_3$. A real space interpretation of the quasi-elastic scattering is given justifying effective Ising model approaches.
The magneto-elastic interaction in cubic helimagnets with B20 symmetry is considered. It is shown that this interaction is responsible for negative contribution to the square of the spin-wave gap $Δ$ which is alone has to disrupt assumed helical structure. It is suggested that competition between positive part of $Δ^2_I$ which stems from magnon-magnon interaction and its negative magneto-elastic part leads to the quantum phase transition observed at high pressure in $Mn Si$ and $Fe Ge$. This transition has to occur when $Δ^2=0$. For $Mn Si$ from rough estimations at ambient pressure both parts…
We propose the phase diagram of a new pseudo-ternary compound, CoMnGe_{1-x}Sn_{x}, in the range x less than or equal to 0.1. Our phase diagram is a result of magnetic and calometric measurements. We demonstrate the appearance of a hysteretic magnetostructural phase transition in the range x=0.04 to x=0.055, similar to that observed in CoMnGe under hydrostatic pressure. From magnetisation measurements, we show that the isothermal entropy change associated with the magnetostructural transition can be as high as 4.5 J/(K kg) in a field of 1 Tesla. However, the large thermal hysteresis in this tra…
We use neutron powder diffraction to investigate the magnetic and crystalline structure of Cr$_2$GaN. A magnetic phase transition is identified at $T \approx 170$ K, whereas no trace of structural transition is observed down to 6 K. Combining Rietveld refinement with irreducible representations, the spin configuration of Cr ions in Cr$_2$GaN is depicted as an incommensurate sinusoidal modulated structure characterized by a propagating vector ${k}$=(0.365, 0.365, 0). Upon warming up to the paramagnetic state, the magnetic order parameter closely resembles to the temperature dependence of $c$-ax…
We discuss a model scenario for multiferroic systems of type II (collinear spins) where the electric dipolar order competes with a frustrated magnetic order in determining the elastic distortions of the lattice ion positions. High magnetic frustration due to second neighbors exchange and small spin easy-axis anisotropy lead to the appearance of the so called quantum magnetic plateau states. Increasing the magnetic field above the plateau border produces composite excitations, where fractionalized spin tertions arise together with spontaneous dipolar flips (in the form of domain walls) and enha…
The magnetoelastic coupling in multiferroic $DyMn_2O_5$ is investigated by magnetostriction measurements along the three crystallographic orientations. Strong lattice anomalies as a function of the magnetic field are detected at the low temperature magnetic and ferroelectric phase transitions. The sign and magnitude of the magnetostrictive coefficient as well as the lattice anomalies at the transitions are correlated with the Dy moment order and with the sharp changes of the dielectric constant and the ferroelectric polarization. With the magnetic field applied along the c-axis a new high-fiel…
Within the BaFe2As2 crystal lattice, we partially substitute thallium for barium and report the effects of interlayer coupling in Ba1-xTlxFe2As2 crystals. We demonstrate the unusual effects of magneto-elastic coupling and charge doping in this iron-arsenide material, whereby Neel temperature rises with small x, and then falls with additional x. Specifically, we find that Neel and structural transitions in BaFe2As2 (TN =Ts= 133 K) increase for x=0.05 (TN = 138 K, Ts = 140 K) from magnetization, heat capacity, resistivity, and neutron diffraction measurements. Evidence from single crystal X-ray …
We present a combined neutron and synchrotron powder diffraction study of the crystal and magnetic structure of VOCl. The occurrence of antiferromagnetic order in VOCl is accompanied by a monoclinic distortion. The high sensitivity of the magnetic interaction parameters on V-O-V bond angles and V-V distances yields strong magnetoelastic coupling which implies the structural distortion below T$_N$ as well as anomalous structural effects in the paramagnetic phase.
We examine the relevance of magneto-elastic coupling to describe the complex magnetic and structural behaviour of the different classes of the iron superconductors. We model the system as a two-dimensional metal whose magnetic excitations interact with the distortions of the underlying square lattice. Going beyond mean field we find that quantum fluctuation effects can explain two unusual features of these materials that have attracted considerable attention. First, why iron telluride orders magnetically at a non-nesting wave-vector $(π/2, π/2)$ and not at the nesting wave-vector $(π, 0)$ as i…
Cerium diantimonide (CeSb$_2$) is one of a family of rare earth based magnetic materials that exhibit metamagnetism, enabling control of the magnetic ground state through an applied magnetic field. At low temperatures, CeSb$_2$ hosts a rich phase diagram with multiple magnetically ordered phases for many of which the order parameter is only poorly understood. In this paper, we report a study of its metamagnetic properties by Scanning Tunneling Microscopy (STM) and magnetization measurements. We use STM measurements to characterize the sample magnetostriction with sub-picometer resolution from …
Extensive magnetization and magnetostriction measurements were carried out on a single crystal of GdNi2B2C along the main tetragonal axes. Within the paramagnetic phase, the magnetic and strain susceptibilities revealed a weak anisotropy in the exchange couplings and two-ion tetragonal-preserving alpha-strain modes. Within the ordered phase, magnetization and magnetostriction revealed a relatively strong orthorhombic distortion mode and rich field-temperature phase diagrams. For H//(100) phase diagram, three field-induced transformations were observed, namely, at: Hd(T), related to the domain …
We report an ultrasonic study of the magneto-elastic coupling of the hydrogenated and deuterated (TMTTF)$_2$PF$_6$ organic salts. For both salts the temperature dependence of the longitudinal velocity along the c* axis displays a monotonic stiffening of the $C_{33}$ compressibility modulus upon cooling. Below the characteristic temperature scale 40 K the modulus stiffening becomes markedly enhanced, in concomitance with the reduction of spin degrees of freedom previously seen in magnetic measurements as low dimensional precursors of the spin-Peierls transition. The magneto-elastic coupling app…
Elastic constants, thermal expansion, magnetostriction and heat capacity measurements were performed with and without applied magnetic field on a single crystal of UIrSi$_3$. The elastic properties were interpreted within the theory of the strain-exchange effect. The exchange-striction model together with the Ising model for the behavior of magnetic localized 5$f$ electrons and itinerant electrons of uranium correctly reproduces the main features of our magneto-acoustic experiments in UIrSi$_3$. Data on thermal expansion and magnetostriction confirm the conclusion that the dominant contributio…
We present an X-ray diffuse scattering study of the pretransitional structural fluctuations of the magneto-elastic transition in alpha'-NaV2O5. This transition is characterized by the appearance below Tsp~35K of satellite reflections at the reduced wave vector (1/2,1/2,1/4). A large regime of structural fluctuations is measured up to 90 K. These fluctuations are three dimensional between Tsp and ~50K and quasi-one dimensional above ~60K. At 40 K the anisotropy ratio is found to be (xib :xia :xic)= (3.8 : 1.8 : 1), which reveals the importance of transverse interactions in the stabilization of …
Using Raman spectroscopy, we investigate the lattice phonons, magnetic excitations, and magneto-elastic coupling in the distorted triangular-lattice Heisenberg antiferromagnet alpha-SrCr2O4, which develops helical magnetic order below 43 K. Temperature dependent phonon spectra are compared to predictions from density functional theory calculations which allows us to assign the observed modes and identify weak effects arising from coupled lattice and magnetic degrees of freedom. Raman scattering associated with two-magnon excitations is observed at 20 meV and 40 meV. These energies are in gener…
The physical properties of epitaxial films can fundamentally differ from those of bulk single crystals even above the critical thickness. By a combination of non-resonant x-ray magnetic scattering, neutron diffraction and vector-mapped x-ray magnetic linear dichroism photoemission electron microscopy, we show that epitaxial (111)-BiFeO3 films support sub-micron antiferromagnetic domains, which are magneto-elastically coupled to a coherent crystallographic monoclinic twin structure. This unique texture, which is absent in bulk single crystals, should enable control of magnetism in BiFeO3 film d…
Quantum spin clusters with dominant antiferromagnetic Heisenberg exchange interactions typically exhibit a sequence of field-induced level crossings in the ground state as function of magnetic field. For fields near a level crossing, the cluster can be approximated by a two-level Hamiltonian at low temperatures. Perturbations, such as magnetic anisotropy or spin-phonon coupling, sensitively affect the behavior at the level-crossing points. The general two-level Hamiltonian of the spin system is derived in first-order perturbation theory, and the thermodynamic functions magnetization, magnetic …
We report a global structural distortion in Sr$_2$IrO$_4$ using spatially resolved optical second and third harmonic generation rotational anisotropy measurements. A symmetry lowering from an $I4_{1}/acd$ to $I4_{1}/a$ space group is observed both above and below the Néel temperature that arises from a staggered tetragonal distortion of the oxygen octahedra. By studying an effective super-exchange Hamiltonian that accounts for this lowered symmetry, we find that perfect locking between the octahedral rotation and magnetic moment canting angles can persist even in the presence of large non-cubi…
We report an ultrasonic investigation of the elastic moduli on a single crystal of hexagonal YMnO_3 as a function of temperature. Stiffening anomalies in the antiferromagnetic Néel state below T_N = 72.4 K are observed on all the four elastic moduli C_{ii}. The anomalies are the most important on C_{11} and C_{66} for in-plane elastic deformations; this is consistent with a strong coupling of the lattice with the in-plane exchange interactions. We use a Landau free energy model to account for these elastic anomalies. We derive an expression which relates the temperature profile of the anomaly …
This work reports an experimental investigation of the magneto-elastic coupling and polarization character of magnetic phases of the orthorhombic Eu1-xYxMnO3 system at low temperatures. The temperature dependence of the polarization reversal curves clearly reveals the existence of a reentrant improper ferroelectric phase for x = 0.2 and 0.3. Although a ferroelectric phase is also stable for x = 0.4, we have no experimental evidence that it vanishing at finite temperatures. From these results and those obtained from other experimental techniques, the corresponding (x,T) phase diagram was traced…
We reinterpret neutron scattering and Raman spectroscopy experiments in La(2-x)Sr(x)CuO(4), showing modulation of spin and lattice degrees of freedom both in the low-temperature orthorhombic and tetragonal phases, in terms of a magneto-elastic coupling between noncollinear configurations for the copper spins and the oxygen octahedra. The magneto-elastic coupling furthermore explains the recently discovered magnetic-field induced untwinning in La(2-x)Sr(x)CuO(4), for x<2%, and allows us to understand why in La(2-x-y)Sr(x)Nd(y)CuO(4) with y=0.4 and x=1/8, for example, when (1,0) and/or (0,1) sta…
The possibility for an appreciable many-body contribution to the electron-phonon interaction (EPI) in Fe-pnictides is discussed in the model where EPI is due to the electronic polarization of As- ions. The EPI-pol coupling ismuch larger than the one obtained in the LDA band structure calculations. It contributes significantly to the intra-band s-wave pairing and an appreciable positive As-isotope effect in the superconducting critical temperature is expected. In the Fe-breathing mode the linear (in the Fe-displacements) EPI-pol coupling vanishes, while the non-linear (quadratic) one is very st…
We show the importance of both strong frustration and spin-lattice coupling for the stabilization of magnetization plateaus in translationally invariant two-dimensional systems. We consider a frustrated spin-1/2 Heisenberg model coupled to adiabatic phonons under an external magnetic field. At zero magnetization, simple structures with two or at most four spins per unit cell are stabilized, forming dimers or $2 \times 2$ plaquettes, respectively. A much richer scenario is found in the case of magnetization $m=1/2$, where larger unit cells are formed with non-trivial spin textures and an analog…
The single ion physics of Ho$_2$Ti$_2$O$_7$ is well-understood to produce strong Ising anisotropy, which is an essential ingredient to its low-temperature spin ice state. We present inelastic neutron scattering measurements on Ho$_2$Ti$_2$O$_7$ that reveal a clear inconsistency with its established single ion Hamiltonian. Specifically, we show that a crystal field doublet near 60~meV is split by approximately 3~meV. Furthermore, this crystal field splitting is not isolated to Ho$_2$Ti$_2$O$_7$ but can also be found in its chemical pressure analogs, Ho$_2$Ge$_2$O$_7$ and Ho$_2$Sn$_2$O$_7$. We d…
We have investigated the elastic properties of the cubic dense Kondo compound Ce0.75La0.25B6 by means of ultrasonic measurements. We have obtained magnetic fields vs temperatures (H-T) phase diagrams under magnetic fields along the crystallographic [001], [110] and [111] axes. An ordered phase IV showing the elastic softening of c44 locates in low temperature region between 1.6 and 1.1 K below 0.7 T in all field directions. The phase IV shows an isotropic nature with regard to the field directions, while the antiferro-magnetic phase III shows an anisotropic character. A remarkable softening of…
In this work we investigate single crystal GdTiO$_{3}$, a promising candidate material for Floquet engineering and magnetic control, using ultrafast optical pump-probe reflectivity and magneto-optical Kerr spectroscopy. GdTiO${}_{3}$ is a Mott-Hubbard insulator with a ferrimagnetic and orbitally ordered ground state (\textit{T${}_{C}$} = 32 K). We observe multiple signatures of the magnetic phase transition in the photoinduced reflectivity signal, in response to above band-gap 660 nm excitation. Magnetic dynamics measured via Kerr spectroscopy reveal optical perturbation of the ferrimagnetic o…
We study the dc resistivity of UNi2Al3 thin films as a function of temperature and magnetic field. We focus on the temperature range around the antiferromagnetic transition (TN \approx 4 K in zero applied field). From a clear signature of TN in the dc resistance along the crystallographic a-direction, we extract the shape of the magnetic phase diagram. Here we find quantitative differences in comparison to previous studies on bulk crystals.
Using SQUID magnetometry techniques, we have studied the change in magnetization versus applied ac electric field, i.e. the magnetoelectric (ME) susceptibility dM/dE, in the chiral-lattice ME insulator Cu2OSeO3. Measurements of the dM/dE response provide a sensitive and efficient probe of the magnetic phase diagram, and we observe clearly distinct responses for the different magnetic phases, including the skyrmion lattice phase. By combining our results with theoretical calculation, we estimate quantitatively the ME coupling strength as λ = 0.0146 meV/(V/nm) in the conical phase. Our study dem…
Precise thermal expansion and magnetostriction studies of the intermetallic compound Eu$_2$CuSi$_3$ in the temperature range between 5 and 300 K are presented. A clear sign of magnetic second order phase transition at the ferromagnetic Curie temperature $T_{\rm C}$ = 34 K indicates strong magneto-structural coupling. Uniaxial thermal expansion data show a large anisotropy between the magnetic easy $c$-axis and the hexagonal $ab$-plane, which is associated with a strongly anisotropic magnetic coupling. A spin-reorientation regime as well as a non-uniform energy scale are indicated by Grüneisen …
We calculate the effects of the spin-lattice coupling on the magnon spectrum of thin ferromagnetic films consisting of the magnetic insulator yttrium-iron garnet. The magnon-phonon hybridisation generates a characteristic minimum in the spin dynamic structure factor which quantitatively agrees with recent Brillouin light scattering experiments. We also show that at room temperature the phonon contribution to the magnon damping exhibits a rather complicated momentum dependence: In the exchange regime the magnon damping is dominated by Cherenkov type scattering processes, while in the long-wavel…
Biquadratic {\it antisymmetric} exchange terms of the form $ - [C_{ij} e^α_{ij}({\bf s}_i\times{\bf s}_j)_z]^2$, where ${\bf e}_{ij}$ is the unit vector connecting sites $i$ and $j$ and $α= x,y$, due partially to magnetoelectric coupling effects, are shown to be responsible for the spin-flop helical phase in CuFeO$_2$ at low magnetic field and temperature. Usual biquadratic {\it symmetric} exchange, likely due to magnetoelastic coupling, is found to support the stability of axial magnetic states at higher fields in this nearly-Heisenberg like stacked triangular antiferromagnet. A model Hamilto…
We have studied a one dimensional Hubbard superlattice with different Coulomb correlations at alternating sites for a half-filled band. Mean field calculations based on the Hartree-Fock approximation together with a real space renormalization group technique were used to study the ground state of the system. The phase diagrams obtained in these approaches agree with each other from the weak to the intermediate coupling regime. The mean field results show very quick convergence with system size. The renormalization group results indicate a spatial modulation of local moments that was identified…
The ferromagnetic and insulating state observed in La$_{1-x}$Ca$_{x}$MnO$_3$, 0.125$<$x$<$0.2, is characterized by structural and magnetic anomalies below T$_C$, similar to those observed in the x$_{Sr}$$\approx$1/8. A neutron scattering study of the superlattice {\bf Q$_0$}= (0,0,1+/4)$_{cub}$ peak, and of the magnetic excitations are reported in the x$_{Ca}$=0.2 sample. The occurrence of this superstructure is associated with the observation of a gap in the spin dynamics, at a {\bf q$_0$} wave-vector ({\bf q$_0$}={\bf Q$_0$}-$τ$) with the same modulus $|${\bf q$_0$}$|$ in all directions, whi…
A Ce-based metallic compound CeCoSi with a tetragonal structure exhibits successive phase transitions: the one whose order parameter is unidentified at T_0 = 12 K and the antiferromagnetic one at T_N = 9.4 K. We performed specific heat, magnetoresistivity (MR), and magnetization measurements for a single crystal CeCoSi at low temperatures in magnetic fields B of up to 14 T and constructed detailed magnetic field--temperature phase diagrams for both B || [100] and [001]. The longitudinal MR measured for B || [100] shows a sign change from negative to positive across T_0 = 13 K updated in the pr…
