Optical spectroscopic investigation on the coupling of electronic and magnetic structure in multiferroic hexagonal RMnO3 (R = Gd, Tb, Dy, and Ho) thin films
Woo Seok Choi, Soon Jae Moon, Sung Seok A. Seo, Daesu Lee, Jung Hyuk Lee, Pattukkannu Murugavel, Tae Won Noh, Yun Sang Lee
We investigated the effects of temperature and magnetic field on the electronic structure of hexagonal RMnO3 (R = Gd, Tb, Dy, and Ho) thin films using optical spectroscopy. As the magnetic ordering of the system was disturbed, a systematic change in the electronic structure was commonly identified in this series. The optical absorption peak near 1.7 eV showed an unexpectedly large shift of more than 150 meV from 300 K to 15 K, accompanied by an anomaly of the shift at the Neel temperature. The magnetic field dependent measurement clearly revealed a sizable shift of the corresponding peak when a high magnetic field was applied. Our findings indicated strong coupling between the magnetic ordering and the electronic structure in the multiferroic hexagonal RMnO3 compounds.
Magnetic order of the manganese and rare-earth lattices according to different symmetry representations is observed in multiferroic hexagonal (h-) DyMnO$_3$ by optical second harmonic generation and neutron diffraction. The incompatibility reveals that the 3d-4f coupling in the h-$R$MnO$_3$ system ($R$ = Sc, Y, In, Dy - Lu) is substantially less developed than commonly expected. As a consequence, magnetoelectric coupling effects in this type of split-order parameter multiferroic that were previously assigned to a pronounced 3d-4f coupling have now to be scrutinized with respect to their origin…
We report single-crystal neutron diffraction study of the magnetic structure of the multiferroic compound YbMnO$_3$, a member of the hexagonal manganite family, in zero-field and under a magnetic field applied along the $c$-axis. We propose a scenario for the zero-field magnetic ordering and for the field-induced magnetic reorientation of the Mn and of the two Yb on distinct crystallographic sites, compatible with the macroscopic measurements, as well as with previous powder neutron diffraction experiment and results from other techniques (optical second harmonic generation, Mössbauer spectros…
Hexagonal manganites are multiferroic materials with two highly-dissimilar phase transitions: a ferroelectric transition (from P63/mmc to P63cm) at a temperature higher than 1000 K and an antiferromagnetic transition at TN=65 - 130 K. Despite its critical relevance to the intriguing ferroelectric domain physics, the details of the ferroelectric transition are yet not well known to date primarily because of the ultra-high transition temperature. Using high-temperature X-ray diffraction experiments, we show that the ferroelectric transition is a single transition of abrupt order and R-Op displac…
We performed magnetic and ferroelectric measurements, associated with Landau theory and symmetry analysis, in order to clarify the situation of the YMnO3 system, a classical example of type I multiferroics. We found that the only magnetic group compatible with all experimental data (neutrons scattering, magnetization,polarization, dielectric constant, second harmonic generation) is the P6'3 group. In this group a small ferromagnetic component along c is induced by the Dzyaloshinskii-Moriya interaction, and observed here in SQUID magnetization measurements. We found that the ferromagnetic and a…
The symmetric splitting of two spin-wave branches in an antiferromagnetic resonance (AFR) experiment has been an essential measurement of antiferromagnets for over half a century. In this work, circularly polarized time-domain THz spectroscopy experiments performed on the low symmetry multiferroic h-HoMnO$_3$ reveal an AFR of the Mn sublattice to split asymmetrically in applied magnetic field, with an $\approx$ 50\% difference in $g$-factors between the high and low energy branches of this excitation. The temperature dependence of the $g$-factors, including a drastic renormalization at the Ho …
Hexagonal LuFeO$_3$ has drawn a lot of research attention due to its contentious room-temperature multiferroicity. Due to the unstability of hexagonal phase in the bulk form, most experimental studies focused on LuFeO$_3$ thin films which can be stabilized by strain using proper substrates. Here we report on the hexagonal phase stabilization, magnetism, and magnetoelectric coupling of bulk LuFeO$_3$ by partial Sc-substitution of Lu. First, our first-principles calculations show that the hexagonal structure can be stabilized by partial Sc substitution, while the multiferroic properties includin…
We have investigated the effects of substituting In for Mn on the antiferromagnetic phase transition in YMnO3 using magnetic, dielectric, and specific heat measurements. We prepared a set of isostructural phase pure hexagonal YMn$_{1-x}$In$_{x}$O$_{3}$ samples having x=0 to x=0.9, which exhibit a systematic decrease of the antiferromagnetic ordering temperature with increasing In content. The multiferroic phase, which develops below TN, appears to be completely suppressed for x$\geq$0.5 in the temperature range investigated, which can be attributed solely to the dilution of magnetic interactio…
We present data on the magnetic and magneto-elastic coupling in the hexagonal multiferroic manganite LuMnO3 from inelastic neutron scattering, magnetization and thermal expansion measurements. We measured the magnon dispersion along the main symmetry directions and used this data to determine the principal exchange parameters from a spin-wave model. An analysis of the magnetic anisotropy in terms of the crystal field acting on the Mn is presented. We compare the results for LuMnO3 with data on other hexagonal RMnO3 compounds.
The magnetic phase diagrams of RMnO3 (R = Er, Yb, Tm, Ho) are investigated up to 14 Tesla via magnetic and dielectric measurements. The stability range of the AFM order below the Neel temperature of the studied RMnO3 extends to far higher magnetic fields than previously assumed. Magnetic irreversibility indicating the presence of a spontaneous magnetic moment is found near 50 K for R=Er, Yb, and Tm. At very low temperatures and low magnetic fields the phase boundary defined by the ordering of the rare earth moments is resolved. The sizable dielectric anomalies observed along all phase boundari…
The rare earth nickelates RNiO3 are metallic at high temperatures and insulating and magnetically ordered at low temperatures. The low temperature phase has been predicted to be type II multiferroic, i.e. ferroelectric and magnetic order are coupled and occur simultaneously. Confirmation of those ideas has been inhibited by the absence of experimental data on single crystals. Here we report on Raman spectroscopic data of RNiO3 single crystals (R = Y, Er, Ho, Dy, Sm, Nd) for temperatures between 10 K and 1000 K. Entering the magnetically ordered phase we observe the appearance of a large number…
Hexagonal YMnO_3 with space group P63cm is one of the rare examples of multiferroic materials that exhibit co-dependence of a robust ferroelectric phase along with antiferromagnetic ordering. This is primarily ascribed to tilting of the MnO_5 polyhedra driven by magnetoelectric coupling. We report on the effect of magnetic field at the atomic level in YMnO_3 by utilizing magnetic field and temperature dependent neutron diffraction measurements. We show that near the Néel temperature the lattice parameters, effective magnetic moment per site, Mn-O bond lengths and O-Mn-O bond angles show large …
We report on the magnetic structure and ordering of hexagonal LuFeO3 films grown by molecular-beam epitaxy (MBE) on YSZ (111) and Al2O3 (0001) substrates. Using a set of complementary probes including neutron diffraction, we find that the system magnetically orders into a ferromagnetically-canted antiferromagnetic state via a single transition between 138-155 K, while a paraelectric to ferroelectric transition occurs above 1000 K. The symmetry of the magnetic structure in the ferroelectric state implies that this material is a strong candidate for linear magnetoelectric coupling and control of…
Magnetic and dielectric properties of the hexagonal triangular lattice antiferromagnet 2H-AgFeO2 have been studied by neutron diffraction, magnetic susceptibility, specific heat, pyroelectric current, and dielectric constant measurements. The ferroelectric polarization, P ~ 5 μC/m2, has been found to appear below 11 K due to a polar nature of the magnetic ground state of the system. In the temperature range of 11 K < T < 18 K, an incommensurate spin density wave (ICM1) with the nonpolar magnetic point group mmm1' and the k1 = (0,q1_b,0; q1_b = 0.390-0.405)propagation vector takes place. Below …
We investigated the electronic structure of multiferroic hexagonal RMnO3 (R = Gd, Tb, Dy, and Ho) thin films using both optical spectroscopy and first-principles calculations. Using artificially stabilized hexagonal RMnO3, we extended the optical spectroscopic studies on the hexagonal multiferroic manganite system. We observed two optical transitions located near 1.7 eV and 2.3 eV, in addition to the predominant absorption above 5 eV. With the help of first-principles calculations, we attribute the low-lying optical absorption peaks to inter-site transitions from the oxygen states hybridized s…
The complex interplay between the 3d and 4f moments in hexagonal ErMnO3 is investigated by magnetization, optical second harmonic generation, and neutron-diffraction measurements. We revise the phase diagram and provide a microscopic model for the emergent spin structures with a special focus on the intermediary phase transitions. Our measurements reveal that the 3d exchange between Mn^{3+} ions dominates the magnetic symmetry at 10 K < T < T_N with Mn^3+ order according to the Gamma_4 representation triggering 4f ordering according to the same representation on the Er^{3+}(4b) site. Below 10 …
We deduce the intrinsic conductivity properties of the ferroelectric domain walls around the topologically protected domain vortex cores in multiferroic YMnO3. This is achieved by performing a careful equivalent-circuit analysis of dielectric spectra measured in single-crystalline samples with different vortex densities. The conductivity contrast between the bulk domains and the less conducting domain boundaries is revealed to reach up to a factor 500 at room temperature, depending on sample preparation. Tunneling of localized defect charge carriers is the dominant charge-transport process in …
We investigated the electronic structure and lattice dynamics of multiferroic MnWO4 by optical spectroscopy. With variation of polarization, temperature, and magnetic field, we obtained optical responses over a wide range of photon energies. The electronic structure of MnWO4 near to the Fermi level was examined, with inter-band transitions identified in optical conductivity spectra above a band-gap of 2.5 eV. As for the lattice dynamics, we identified all the infrared transverse optical phonon modes available according to the group-theory analysis. Although we did not observe much change in gl…
Simultaneous co-existence of room-temperature(T) ferromagnetism and ferroelectricity in Fe doped BaTiO$_3$ (BTO) is intriguing, as such Fe doping into tetragonal BTO, a room-T ferroelectric (FE), results in the stabilization of its hexagonal polymorph which is FE only below $\sim$80K. Here, we investigate its origin and show that Fe-doped BTO has a mixed-phase room-temperature multiferroicity, where the ferromagnetism comes from the majority hexagonal phase and a minority tetragonal phase gives rise to the observed weak ferroelectricity. In order to achieve majority tetragonal phase (responsib…
Inelastic neutron scattering has been used to study the magneto-elastic excitations in the multiferroic manganite hexagonal YMnO$_3$. An avoided crossing is found between magnon and phonon modes close to the Brillouin zone boundary in the $(a,b)$-plane. Neutron polarization analysis reveals that this mode has mixed magnon-phonon character. An external magnetic field along the $c$-axis is observed to cause a linear field-induced splitting of one of the spin wave branches. A theoretical description is performed, using a Heisenberg model of localized spins, acoustic phonon modes and a magneto-ela…
Local structural measurements have been performed on hexagonal HoMnO3 in order to ascertain the specific changes in bond distances which accompany magnetic ordering transitions. The transition from paramagnetic to the antiferromagetic (noncollinear) phase near ~70 K is dominated by changes in the a-b plane Mn-Mn bond distances. The spin rotation transition near ~40 K involves both Mn-Mn and nearest neighbor Ho-Mn interactions while the low temperature transition below 10 K involves all interactions, Mn-Mn, Ho-Mn (nearest and next nearest) and Ho-Ho correlations. These changes in bond distances…
Hexagonal LuFe2O4 is a promising charge-order (CO) driven multiferroic material with high charge and spin ordering temperatures. The coexisting charge and spin orders on Fe3+/Fe2+ sites result in novel magnetoelectric behaviors, but the coupling mechanism between the charge and spin orders remains elusive. Here, by tuning external pressure, we reveal three correlated spin-charge ordered phases in LuFe2O4: i) a centrosymmetric incommensurate three-dimensional CO with ferrimagnetism, ii) a non-centrosymmetric incommensurate quasi-two-dimensional CO with ferrimagnetism, and iii) a centrosymmetric…
We provide a theoretical description of frustrated multiferroic $\rm MnI_2$ with a spiral magnetic ordering in magnetic field $\bf h$. We demonstrate that subtle interplay of exchange coupling, dipolar forces, hexagonal anisotropy, and the Zeeman energy account for the main experimental findings observed recently in this material (Kurumaji, et al., Phys.\ Rev.\ Lett.\ {\bf 106}, 167206 (2011)). We describe qualitatively the non-trivial evolution of electric polarization $\bf P$ upon $\bf h$ rotation, changing $\bf P$ direction upon $h$ increasing, and disappearance of ferroelectricity at $h>h_…
The magnetic exchange bias between epitaxial thin films of the multiferroic (antiferromagnetic and ferroelectric) hexagonal YMnO3 oxide and a soft ferromagnetic (FM) layer is used to couple the magnetic response of the ferromagnetic layer to the magnetic state of the antiferromagnetic one. We will show that biasing the ferroelectric YMnO3 layer by an appropriate electric field allows modifying and controlling the magnetic exchange bias and subsequently the magnetotransport properties of the FM layer. This finding may contribute to pave the way towards a new generation of electric-field control…
Epitaxial thin films of hexagonal ErMnO3 fabricated on Pt(111)/Al2O3(0001) and YSZ(111) substrates exhibited both ferroelectric character and magnetic ordering at low temperatures. As the temperature was reduced, the ErMnO3 films first showed antiferromagnetism. At lower temperatures, the films deposited at lower oxygen partial pressures exhibited spin glass behavior. This re-entrant spin glass behavior was attributed to competition between an antiferromagnetic interaction in the hexagonal geometry and a ferromagnetic interaction caused by a change in Mn valence induced by excess electrons fro…
Strong spin-lattice coupling and prominent frustration effects observed in the 50$\%$ Fe-doped frustrated hexagonal ($h$)LuMnO$_3$ are reported. A Néel transition at $T_{\mathrm N} \approx$ 112~K and a possible spin re-orientation transition at $T_{\mathrm {SR}} \approx$ 55~K are observed in the magnetization data. From neutron powder diffraction data, the nuclear structure at and below 300~K was refined in polar $P6_3cm$ space group. While the magnetic structure of LuMnO$_3$ belongs to the $Γ_4$ ($P6'_3c'm$) representation, that of LuFe$_{0.5}$Mn$_{0.5}$O$_3$ belongs to $Γ_1$ ($P6_3cm$) which…
Non-collinear two-dimensional triangular lattice antiferromagnets (2D TLAF) are currently an area of very active research due to their unique magnetic properties, which lead to non-trivial quantum effects that experimentally manifest themselves in the spin excitation spectra. Recent examples of such insulating 2D TLAF include (Y,Lu)MnO$_3$, LiCrO$_2$, and CuCrO$_2$. Hexagonal LuFeO3 is a recently synthesized 2D TLAF which exhibits properties of an ideal multiferroic material, partially because of the high spin ($S=5/2$) and strong magnetic super-exchange interactions. We report the full range …
Hexagonal RMnO3 is a multiferroic compound with a giant spin-lattice coupling at an antiferromagnetic transition temperature [1]. Despite extensive studies over the past two decades, however, the origin and underlying microscopic mechanism of the strong spin-lattice coupling remain still very much elusive. In this study, we have tried to address this problem by measuring the thermal expansion and dielectric constant of doped single crystals Y1-xLuxMnO3 with x = 0, 0.25, 0.5, 0.75, and 1.0. From these measurements, we confirm that there is a progressive change in the physical properties with do…
We have investigated magnetoelastic effects in multiferroic HoMnO$_3$ below the antiferromagnetic phase transition $T_N \approx 75$ K by neutron powder diffraction. The lattice parameter $a$ of the hexagonal unit cell of HoMnO$_3$ decrease in the usual way at lower temperatures and then shows abrupt contraction below $T_N$ whereas the lattice parameter $c$ increases continuously with decreasing temperature and shows an anomalous increase below $T_N$. The unit cell volume decreases continuously with decreasing temperature and undergoes abrupt contraction below $T_N$. By fitting the background t…
Lattice and spin excitations have been studied by Raman scattering in hexagonal YbMnO3 single crystals. The temperature dependences of the phonon modes show that the E2 mode at 256 cm-1 related to the displacement of Mn and O ions in a-b plane is coupled to the spin order. The A1 phonon mode at 678 cm-1 presents a soft mode behavior at the Neel temperature. Connected to the motion of the apical oxygen ions along the c direction, this mode controls directly the Mn-Mn interactions between adjacent Mn planes and the superexchange path. Crystal field and magnon mode excitations have been identifie…
We have performed high resolution neutron diffraction and inelastic neutron scattering experiments in the frustrated multiferroic hexagonal compounds RMnO3 (R=Ho, Yb, Sc, Y), which provide evidence of a strong magneto-elastic coupling in the the whole family. We can correlate the atomic positions, the type of magnetic structure and the nature of the spin waves whatever the R ion and temperature. The key parameter is the position of the Mn ions in the unit cell with respect to a critical threshold of 1/3, which determines the sign of the coupling between Mn triangular planes.
Hexagonal Dy(0.5)Y(0.5)MnO3, a multiferroic rare-earth manganite with geometrically frustrated antiferromagnetism, has been investigated with single-crystal neutron diffraction measurements. Below 3.4 K magnetic order is observed on both the Mn (antiferromagnetic) and Dy (ferrimagnetic) sublattices that is identical to that of undiluted hexagonal DyMnO3 at low temperature. The Mn moments undergo a spin reorientation transition between 3.4 K and 10 K, with antiferromagnetic order of the Mn sublattice persisting up to 70 K; the antiferromagnetic order in this phase is distinct from that observed…
Optical control of the spin degree of freedom is often desired in application of the spin technology. Here we report spin-rotational excitations observed through inelastic light scattering of the hexagonal LuMnO3 in the antiferromagnetically (AFM) ordered state. We propose a model based on the spin-spin interaction Hamiltonian associated with the spin rotation of the Mn ions, and find that the spin rotations are angularly quantized by 60, 120, and 180 degrees. Angular quantization is considered to be a consequence of the symmetry of the triangular lattice of the Mn-ion plane in the hexagonal L…
Spectroscopic modes provide the most sensitive probe of the very weak interactions responsible for the properties of the long-wavelength cycloid in the multiferroic phase of \BF below $\TN \approx 640$ K. Three of the four modes measured by THz and Raman spectroscopies were recently identified using a simple microscopic model. While a Dzyaloshinskii-Moriya (DM) interaction $D$ along $[-1,2,-1]$ induces the cycloid with wavevector $(2π/a)(0.5+δ, 0.5, 0.5-δ)$ ($δ\approx 0.0045$), easy-axis anisotropy $K$ along the $[1,1,1]$ direction of the electric polarization ${\bf P}$ induces higher harmonic…
We used Raman and terahertz spectroscopies to investigate lattice and magnetic excitations and their cross-coupling in the hexagonal YMnO3 multiferroic. Two phonon modes are strongly affected by the magnetic order. Magnon excitations have been identified thanks to comparison with neutron measurements and spin wave calculations but no electromagnon has been observed. In addition, we evidenced two additional Raman active peaks. We have compared this observation with the anti-crossing between magnon and acoustic phonon branches measured by neutron. These optical measurements underly the unusual s…
The hexagonal RMnO$_3$ (h-RMnO$_3$) are multiferroic materials, which exhibit the coexistence of a magnetic order and ferroelectricity. Their distinction is in their geometry that both results in an unusual mechanism to break inversion symmetry, and also produces a 2D triangular lattice of Mn spins, which is subject to geometrical magnetic frustration due to the antiferromagnetic interactions between nearest neighbour Mn ions. This unique combination makes the h-RMnO$_3$ a model system to test ideas of spin-lattice coupling, particularly when the both the improper ferroelectricity and the Mn t…
We have studied the crystal and magnetic structures of Fe-doped hexagonal manganites LuMn1-xFexO3 (x = 0, 0.1, 0.2, and 0.3) by using bulk magnetization and neutron powder diffraction methods. The samples crystalize consistently in a hexagonal structure and maintain the space group P63cm from 2 to 300 K. The Néel temperature TN increases continuously with increasing Fe-doping. In contrast to a single Γ4 representation in LuMnO3, the magnetic ground state of the Fe-doped samples can only be described with a spin configuration described by a mixture of Γ3 (P63'cm') and Γ4 (P63'c'm) representatio…
Multiferroic rare earth manganites attracted recent attention because of the coexistence of different types of magnetic and ferroelectric orders resulting in complex phase diagrams and a wealth of physical phenomena. The coupling and mutual interference of the different orders and the large magnetoelectric effect observed in several compounds are of fundamental interest and bear the potential for future applications in which the dielectric (magnetic) properties can be modified by the onset of a magnetic (dielectric) transition or the application of a magnetic (electric) field. The physical mec…
We report on the exchange bias between antiferromagnetic and ferroelectric hexagonal YMnO3 epitaxial thin films sandwiched between a metallic electrode (Pt) and a soft ferromagnetic layer (Py). Anisotropic magnetoresistance measurements are performed to monitor the presence of an exchange bias field. When the heteroestructure is biased by an electric field, it turns out that the exchange bias field is suppressed. We discuss the dependence of the observed effect on the amplitude and polarity of the electric field. Particular attention is devoted to the role of current leakage across the ferroel…
We present a detailed temperature-dependent spectroscopic study of DyMnO3 single crystals with distorted perovskite structure. Energies of 36 crystal-field levels of Dy3+ in paramagnetic DyMnO3 were determined. The Dy3+ ground Kramers doublet does not split at T_N^Mn = 39 K and splits below Tlock = 18 K. The splitting grows fast at temperatures near T_N^Dy = 6.5 K and reaches Δ0 = 11 cm-1 at 4 K. Using the experimental temperature dependence Δ0(T), we calculate the dysprosium magnetic moment mDy(T) and the dysprosium contribution into specific heat and magnetic susceptibility. Analysing all th…
We investigate partially disordered antiferromagnetism in CoCl$_2$-2SC(NH$_2$)$_2$, in which a-b plane hexagonal layers are staggered along the c-axis, rather than stacked. A robust 1/3 state forms in applied magnetic fields which the spins are locked, varying neither as a function of temperature nor field. By contrast, in zero field, partial antiferromagnetic order occurs, in which free spins are available to create a Curie-like magnetic susceptibility. We report measurements of the crystallographic structure, and the specific heat, magnetization, and electric polarization down to $T$ = 50 mK…
Magnetic monopoles and toroidal order are compelling features that have long been theorized but remain elusive in real materials. Multiferroic hexagonal ferrites are an interesting realization of frustrated triangular lattice, where magnetic order is coupled to ferroelectricity and trimerization. Here we propose a mechanism, through which magnetic monopolar and toroidal orders emerge from the combination of 120$^\circ$ antiferromagnetism and trimerization, present in hexagonal manganites and ferrites. The experimentally observable signatures of magnetic monopolar and toroidal orders are identi…
InMnO$_3$ is a peculiar member of the hexagonal manganites h-RMnO$_3$ (where R is a rare earth metal element), showing crystalline, electronic and magnetic properties at variance with the other compounds of the family. We have studied high quality samples synthesized at high pressure and temperature by powder neutron diffraction. The position of the Mn ions is found to be close to the threshold $\it{x}=1/3$ where superexchange Mn-Mn interactions along the $\it{c}$ axis compensate. Magnetic long range order occurs below $T_{\rm N}$= 120(2) K with a magnetic unit cell doubled along $\it{c}$, whe…
Spin-phonon coupling, the interaction of spins with surrounding lattice is a key parameter to understand the underlying physics of multiferroics and engineer their magnetization dynamics. Elementary excitations in multiferroic materials are strongly influenced by spin-phonon interaction, making Raman spectroscopy a unique tool to probe these coupling(s). Recently, it has been suggested that the dielectric and magnetic properties of 15R-type hexagonal BaMnO3 are correlated through the spin-lattice coupling. Here, we report the observation of an extensive renormalization of the Raman spectrum of…
The floating-zone method with different growth ambiances has been used to selectively obtain hexagonal or orthorhombic DyMnO$_{3}$ single crystals. The crystals were characterized by X-ray powder diffraction of ground specimen and a structure refinement as well as electron diffraction. We report magnetic susceptibility, magnetisation, and specific heat studies of this multiferroic compound in both the hexagonal and the orthorhombic structure. The hexagonal DyMnO$_{3}$ shows magnetic ordering of Mn$^{3+}$ (S =2) spins on a triangular Mn lattice at $T^{\mathrm {Mn}}_{N}$ = 57 K characterized by …
A microscopic model for the room-temperature multiferroic BiFeO$_3$ that includes two Dzyaloshinskii-Moriya interactions and single-ion anisotropy along the ferroelectric polarization predicts both the zero-field spectroscopic modes as well as their splitting and evolution in a magnetic field. Due to simultaneously broken time-reversal and spatial-inversion symmetries, the absorption of light changes as the magnetic field or the direction of light propagation is reversed. We discuss three physical mechanisms that may contribute to this absorption asymmetry known as non-reciprocal directional d…
We have investigated magnetoelastic effects in multiferroic YMnO$_3$ below the antiferromagnetic phase transition, $T_N \approx 70$ K, using neutron powder diffraction. The $a$ lattice parameter of the hexagonal unit cell of YMnO$_3$ decreases normally above $T_N$, but decreases anomalously below T$_N$, whereas the $c$ lattice parameter increases with decreasing temperature and then increases anomalously below T$_N$. The unit cell volume also undergoes an anomalous contraction below $T_N$. By fitting the background thermal expansion for a non-magnetic lattice with the Einstein-Grüneisen equati…
We used Raman scattering to study the lattice and magnetic excitations in the hexagonal HoMnO3 single crystals. The E2 phonon mode at 237 cm-1 is affected by the magnetic order. This mode is related to the displacement of Mn and O ions in a-b plane and modulates the Mn-O-Mn bond angles in a-b plane and the in-plane Mn-Mn superexchange interaction. The mode at 269 cm-1 associated to the displacement of the apical Ho3+ ions along the c direction presents an abrupt change of slope at TN showing that the role of the rare earth ions can not be neglected in the magnetic transition. We have identifie…
Interplay of Spin Waves, Crystal-Field Excitations, and Phonons in Multiferroic Ba3HoRu2O9 revealed by Inelastic Neutron Scattering, Crystal-Field Analysis, and Machine-Learned Phonon Calculations
Rajiv Gandhi Institute of Petroleum Technology（Rajiv Gandhi石油技术学院）；ISIS Neutron and Muon Source, STFC, Rutherford Appleton Laboratory（ISIS中子与缪子源，STFC，卢瑟福阿普顿实验室）；School of Physical Sciences, Indian Institute of Technology Goa（印度理工学院果阿分校物理科学学院）；UGC - DAE Consortium for Scientific Research Mumbai Centre, Bhabha Atomic Research Centre（UGC-DAE科学研究中心孟买中心，巴哈原子研究中心）；Highly Correlated Matter Research Group, Physics Department, University of Johannesburg（约翰内斯堡大学高度关联物质研究组物理系）
We have studied the magnetic field dependence of far-infrared active magnetic modes in a single ferroelectric domain \BFO/ crystal at low temperature. The modes soften close to the critical field of 18.8\,T along the [001] (pseudocubic) axis, where the cycloidal structure changes to the homogeneous canted antiferromagnetic state and a new strong mode with linear field dependence appears that persists at least up to 31\,T. A microscopic model that includes two \DM/ interactions and easy-axis anisotropy describes closely both the zero-field spectroscopic modes as well as their splitting and evol…
Ferroelectric materials possess a spontaneous electric polarization and may be utilized in various technological applications ranging from non-volatile memories to solar cells and light polarizers. Recently, hexagonal rare-earth manganites, h-RMnO$_3$ (R is a rare-earth ion) have attracted considerable interest due to their intricate multiferroic properties and improper ferroelectricity characterized by a sizable remnant polarization and high Curie temperature. Here, we demonstrate that these compounds can serve as very efficient photovoltaic materials and, in addition, possess remarkable opti…
The magnetic ordering of the hexagonal multiferroic compound YbMnO$_3$ has been studied between 100 K and 1.5 K by combining neutron powder diffraction, $^{170}$Yb Mössbauer spectroscopy and magnetization measurements. The Yb moments of the two crystallographic sites order at two different temperatures, the $4b$ site together with the Mn moments (at $T_N \simeq$85 K) and the $2a$ site well below (at 3.5 K). The temperature dependences of the Mn and Yb moments are explained within a molecular field model, showing that the $4b$ and $2a$ sites order via Yb-Mn and Yb-Yb interactions respectively. …
Thin films and heterostructures of hexagonal manganites as promising multiferroic materials have attracted a considerable interest recently. We report structural transformations of high quality epitaxial h-TMO/YSZ(111) films, analyzed by means of various characterization techniques. A phase transition from P63mc to P63mcm structure at TC~800 K was observed by temperature dependent Raman spectroscopy and optical ellipsometry. The latter probing directly electronic system, indicates its modification at the structural phase transition likely due to charge transfer from oxygen to Mn. In situ trans…
Magnetoelectric (ME) properties under rotating magnetic field H are comparatively investigated in two representative hexaferrites Y-type Ba0.5Sr1.5Zn2(Fe0.92Al0.08)12O22 and Z-type Ba0.52Sr2.48Co2Fe24O41, both of which have exhibited a similar transverse conical spin structure and giant ME coupling near room temperature. When the external H is rotated clockwise by 2pi, in-plane P vector is rotated clockwise by 2pi in the Y-type hexaferrite and counterclockwise by 4pi in the Z-type hexaferrite. A symmetry-based analysis reveals that the faster and opposite rotation of P vector in the Z-type hex…
Magnetic skyrmions, vortex-like swirling spin textures characterized by a quantized topological invariant, realized in chiral-lattice magnets are currently attracting intense research interest. In particular, their dynamics under external fields is an issue of vital importance both for fundamental science and for technical application. Whereas observations of magnetic skyrmions had been limited to metallic magnets so far, their realization was discovered also in a chiral-lattice insulating magnet Cu2OSeO3 in 2012. Skyrmions in the insulator turned out to exhibit multiferroic nature with spin-i…
Hexagonal YMnO$_{3}$ is a prototype antiferromagnet which exhibits multiferroic behavior with the ferroelectric and magnetic transitions occurring at different temperatures. We observe an out-of-plane canting of the Mn$^{3+}$ magnetic moments using resonant X-ray diffraction (RXD) in a single crystal of this material. These canted moments result in the symmetry-forbidden (0,0,1) magnetic Bragg reflection, which is observed at the Mn $L_{2,3}$ absorption edges. We also observe an unexpected difference in the RXD spectral shapes at different temperatures. Using ab initio calculations, we explore…
