We have performed Raman scattering investigations on the high energy magnetic excitations in a BiFeO$_3$ single crystal as a function of both temperature and laser excitation energy. A strong feature observed at 1250 cm$^{-1}$ in the Raman spectra has been previously assigned to two phonon overtone. We show here that its unusual frequency shift with the excitation energy and its asymmetric temperature dependent Fano lineshape reveal a strong coupling to magnetic excitations. In the same energy range, we have also identified the two-magnon excitation with a temperature dependence very similar to $α$-Fe$_2$O$_3$ hematite.
Low-energy magnon excitations in multiferroic BiFeO$_3$ were measured in detail as a function of temperature around several Brillouin zone centers by inelastic neutron scattering experiments on single crystals. Unique features around 1 meV are directly associated with the interplay of the Dzyaloshinskii-Moriya interaction and a small single-ion anisotropy. The temperature dependence of these and the exchange interactions were determined by fitting the measured magnon dispersion with spin-wave calculations. The spectra best fits an easy-axis type magnetic anisotropy and the deduced exchange and…
Raman scattering measurements on BiFeO3 single crystals show an important coupling between the magnetic order and lattice vibrations. The temperature evolution of phonons shows that the lowest energy E and A1 phonon modes are coupled to the spin order up to the Neel temperature. Furthermore, low temperature anomalies associated with the spin re-orientation are observed simultaneously in both the E phonon and the magnon. These results suggest that magnetostriction plays an important role in BiFeO3.
We have performed Raman scattering measurements on BiFeO3 nanoparticles and studied both magnetic and lattice modes. We reveal strong anomalies between 140 K and 200 K in the frequency of magnon and E(LO1), E(TO1) and A1(LO1) phonon modes. These anomalies are related to a surface expansion and are enhanced for nanoparticle sizes approaching the spin cycloidal length. These observations point out the strong interplay between the surface, the lattice, and the magnetism for sizes of BiFeO3 nanoparticles close to the cycloid periodicity.
The idea of embedding and transmitting information within the fluctuations of the magnetic moments of spins (spin waves) has been recently proposed and experimentally tested. The coherence of spin waves, which describes how well defined these excitations are, is of course vital to this process, and themost significant factor that affects the spin-wave coherence is temperature. Here we present neutron inelastic scattering measurements of the full threedimensional spin-wave dispersion in BiFeO3, which is one of the most promising functional multiferroic material, for temperatures from 5K to 700K…
Multiferroic materials have attracted much interest due to the unusual coexistence of ferroelectric and (anti-)ferromagnetic ground states in a single compound. They offer an exciting platform for new physics and potentially novel devices. BiFeO$_3$ is one of the most celebrated of multiferroic materials with highly desirable properties. It is the only known room-temperature multiferroic with $T_\mathrm{C}\approx 1100~ \mathrm{K}$ and $T_\mathrm{N}\approx 650~\mathrm{K}$, and exhibits one of the largest spontaneous electric polarisation, $P\approx 80~μ\mathrm{C/cm}^2$. At the same time, it has…
The phonon density of states (DOS) and magnetic excitation spectrum of polycrystalline BiFeO$_3$ were measured for temperatures $200 \leq T \leq 750\,$K, using inelastic neutron scattering (INS). Our results indicate that the magnetic spectrum of BiFeO$_3$ closely resembles that of similar Fe perovskites, such as LaFeO$_3$, despite the cycloid modulation in BiFeO$_3$. We do not find any evidence for a spin gap. A strong $T$-dependence of the phonon DOS was found, with a marked broadening of the whole spectrum, providing evidence of strong anharmonicity. This anharmonicity is corroborated by la…
Magnetic dc susceptibility between 1.5 and 800 K, ac susceptibility and magnetization, thermodynamic properties, temperature dependence of radio and audio-wave dielectric constants and conductivity, contact-free dielectric constants at mm-wavelengths, as well as ferroelectric polarization are reported for single crystalline BiFeO3. A well developed anomaly in the magnetic susceptibility signals the onset of antiferromagnetic order close to 635 K. Beside this anomaly no further indications of phase or glass transitions are indicated in the magnetic dc and ac susceptibilities down to the lowest …
We report the magnetic field dependence of the THz absorption and non-reciprocal directional dichroism spectra of BiFeO$_3$ measured on the three principal crystal cuts for fields applied along the three principal directions of each cut. From the systematic study of the light polarization dependence we deduced the optical selection rules of the spin-wave excitations. Our THz data, combined with small-angle neutron scattering results showed that i) an in-plane magnetic field rotates the $\mathbf{q}$ vectors of the cycloids perpendicular to the magnetic field, and ii) the selection rules are mos…
A sharp feature in the charge-density excitation spectra of single-crystal MgB$_{2}$, displaying a remarkable cosine-like, periodic energy dispersion with momentum transfer ($q$) along the $c^{*}$-axis, has been observed for the first time by high-resolution non-resonant inelastic x-ray scattering (NIXS). Time-dependent density-functional theory calculations show that the physics underlying the NIXS data is strong coupling between single-particle and collective degrees of freedom, mediated by large crystal local-field effects. As a result, the small-$q$ collective mode residing in the single-p…
We study the elementary excitations in 5d transition metal oxideSr$_2$IrO$_4$ by calculating the particle-hole Green's function within the random phase approximation on an antiferromagnetic ground state in the two-dimensional multi-orbital Hubbard model. The obtained magnetic excitations of bound states show a characteristic dispersion in consistent with the experiments. In addition, two new types of excitations are found due to the interplay between spin-orbit interaction and Hund's coupling: a magnetic excitation as a bound state, which has energy gap at the $Γ$ point, and an exciton as a re…
Recently, oxide multiferroics have attracted much attention due to their large magnetoelectric effect which allows the tuning of magnetic properties with electric field and vice versa and open new venues for future spintronic applications such as multiple-state memory devices with dual magnetic and electric control. BiFeO$_3$ (BFO) belongs to this new class of materials and shows both ferroelectric and antiferromagnetic orders at room temperature with a large electric polarizationassociated with a cycloidal spiral magnetic ordering. The incommensurate magnetic order induces magnon zone folding…
The microscopic theory of interaction between the heavy fermions and the crystal field excitations in Kondo lattices is presented. It is shown that the heavy-fermion spectrum scaled by the Kondo temperature $T_K$ can be modified by the crystal field excitations with the energy $Δ_{CF}$ provided the inequality $Δ_{CF}<T_K$ is realized. On the base of general description of excitation spectrum the detailed qualitative and quantitative explanation of anisotropic inelastic neutron scattering spectra and low-temperature specific heat of orthorhombic CeNiSn is given. The theory resolves the apparent…
We report an infrared spectroscopy study of the axion topological insulator candidate EuIn$_2$As$_2$ for which the Eu moments exhibit an A-type antiferromagnetic (AFM) order below $T_N \simeq 18 \mathrm{K}$. The low energy response is composed of a weak Drude peak at the origin, a pronounced infrared-active phonon mode at 185 cm$^{-1}$ and a free carrier plasma edge around 600 cm$^{-1}$. The interband transitions start above 800 cm$^{-1}$ and give rise to a series of weak absorption bands at 5\,000 and 12\,000 cm$^{-1}$ and strong ones at 20\,000, 27\,500 and 32\,000 cm$^{-1}$. The AFM transit…
On the basis of Quantum Monte Carlo simulations of the two-dimensional Hubbard model which cover the doping range from the under- to the over-doped regime, we find that the single-particle spectral weight $A (\vec k,ω)$ qualitatively reproduces both the momentum ($d_{x^2-y^2}$--symmetry) and doping dependence of the pseudogap as found in photoemission experiments. The drastic doping dependence of the spin response $χ_{s} (\vec q,ω)$ which is sharp in both $\vec q (\approx(π,π))$ and $ω$ in the under-doped regime but broad and structureless otherwise, identifies remnants of the antiferromagneti…
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 present a powder inelastic neutron scattering study of magnetic excitations in Ba$_2$FeReO$_6$, a member of the double perovskite family of materials which exhibit half-metallic behavior and high Curie temperatures. We find clear evidence of two well-defined dispersing magnetic modes in its low temperature ferrimagnetic state. We develop a local moment model, which incorporates the interaction of Fe spins with spin-orbit locked magnetic moments on Re, and show that this captures our experimental observations. Our study further opens up double perovskites as model systems to explore the inte…
Unveiling the Interplay of Charge and Magnetic Excitations in HgBa$_2$Ca$_2$Cu$_3$O$_{8+δ}$
Chalmers University of Technology（查尔姆斯理工大学）；Politecnico di Milano（米兰理工大学）；ESRF, The European Synchrotron（欧洲同步辐射装置）；CEA Saclay（法国原子能和替代能源委员会萨克雷中心）；Université Paris Cité（巴黎西岱大学）；BTU Cottbus-Senftenberg（科特布斯-森夫滕贝格勃兰登堡工业大学）
Motivated by the iron-based superconductors, we develop a self-consistent electronic theory for the itinerant spin excitations in the regime of coexistence of the antiferromagnetic stripe order with wavevector ${\bf Q}_{1} = (π,0)$ and $s^{+-}$ superconductivity. The onset of superconductivity leads to the appearance of a {\em magnetic} resonance near the wavevector ${\bf Q}_{2} = (0,π)$ where magnetic order is absent. This resonance is isotropic in spin space, unlike the excitations near ${\bf Q}_{1}$ where the magnetic Goldstone mode resides. We discuss several features which can be observed…
Our inelastic neutron scattering experiments of the spin excitations in the slightly overdoped La{1.83}Sr{0.17}CuO{4} compound show that, under the application of a magnetic field of 5 Tesla, the low-temperature susceptibility undergoes a weight redistribution centered at the spin-gap energy. Furthermore, by comparing the temperature dependence of the neutron data with ac-susceptibility and magnetization measurements, we conclude that the filling in of the spin gap tracks the irreversibility/melting temperature rather than Tc2, which indicates an unusual interplay between the magnetic vortices…
This work is devoted to the study of how spin texture excitations are affected by the presence of a static nonmagnetic impurity whenever they lie on a conical support. We realize a number of novelties as compared to the flat plane case. Indeed, by virtue of the conical shape, the interaction potential between a soliton and an impurity appears to become stronger as long as the cone is tighten. As a consequence, a new kind of solitonic excitation shows up exhibiting lower energy than in the absence of such impurity. In addition, we conclude that such an energy is also dependent upon conical aper…
Metal organic magnets have enormous potential to host a variety of electronic and magnetic phases that originate from a strong interplay between the spin, orbital and lattice degrees of freedom. We control this interplay in the quantum magnet CuF$_2$(D$_2$O)$_2$pyz by using high pressure to drive the system through a structural and magnetic phase transition. Using neutron scattering, we show that the low pressure state, which hosts a two-dimensional square lattice with spin-wave excitations and a dominant exchange coupling of 0.89 meV, transforms at high pressure into a one-dimensional spin-ch…
Strongly coupled conformal field theory appears to describe universal scaling around quantum criticality, where critical exponents reflect the nature of emergent excitations. In particular, novel symmetries can emerge from strong interactions, expected to be responsible for quantum number fractionalization. The underlying mechanism has been proposed that an emergent enhanced symmetry allows a topological term associated with anomaly, which assigns a fermion's quantum number to a topological excitation, referred as the Goldstone-Wilczek current. Although this mechanism has been verified in one …
We present a comprehensive theoretical study of the physical phenomena that determine the relative energies of the three of the lowest electronic states of each of the square-planar copper complexes $\cucl$, $\cunh$ and $\cuwater$, and present a detailed analysis of the extent to which truncated configuration interaction (CI) and coupled cluster (CC) theories succeed in predicing the excitation energies. We find that ligand-metal charge transfer (CT) single excitations play a crucial role in the correct determination of the properties of these systems, even though the CT processes first occur …
We study the uniform time reversal invariant $U(1)$ quantum spin liquid (QSL) with low energy fermionic quasi-particles for rare earth pyrochlore magnets and explore its magnetic instability employing an augmented fermionic parton mean field theory approach. Self consistent calculations stabilise an uniform $U(1)$ QSL with both gapped and gapless parton excitations as well as fractionalised magnetically ordered phases in an experimentally relevant part of the phase diagram near the classical phase boundaries of the magnetically ordered phases. The gapped QSL has a band-structure with a non-zer…
Formation of magnetically ordered state in the Kondo lattices is treated within the degenerate $s-f$ exchange and Coqblin-Schrieffer models. The Kondo renormalizations of the effective coupling parameter, magnetic moment and spin excitation frequencies are calculated within perturbation theory. The results of one-loop scaling consideration of the magnetic state in Kondo lattices are analyzed. The dependence of the critical values of the bare model parameters on the type of the magnetic phase and space dimensionality is investigated. Renormalization of the effective Kondo temperature by the int…
In this review, we present a summary of the results on single crystal growth of two types of iron-chalcogenide superconductors, Fe(1+y)Te(1-x)Se(x) (11), and A(x)Fe(2-y)Se(2) (A= K, Rb, Cs, Tl, Tl/K, Tl/Rb), using Bridgman, zone-melting, vapor self-transport, and flux techniques. The superconducting and magnetic properties (the latter gained mainly from neutron scattering measurements) of these materials are reviewed to demonstrate the connection between magnetism and superconductivity. It will be shown that for the 11 system, while static magnetic order around the reciprocal lattice position …
We review a recently proposed mechanism for superconductivity in hole-doped cuprates exhibiting a strong interplay between pairing and antiferromagnetism. Starting from the t-t'-J model for the CuO planes, we show that this interplay can explain in a unified framework the pseudogap phenomenology of the spectral weight of the hole, the hourglass-like structure of the magnetic excitation, the critical exponent of the superfluid density, the relation between the scale of the magnetic resonance and Tc.
We present a Raman spectroscopic investigation of the Herbertsmithite ZnCu3(OH)6Cl2, the first realization of a Heisenberg s=1/2 antiferromagnet on a perfect kagome lattice. The magnetic excitation spectrum of this compound is dominated by two components, a high temperature quasi elastic signal and a low temperature, broad maximum. The latter has a linear low energy slope and extends to high energy. We have investigated the temperature dependence and symmetry properties of both signals. Our data agree with previous calculations and point to a spin liquid ground state.
The Berezinskii-Kosterlitz-Thouless (BKT) mechanism describes universal vortex unbinding in many two-dimensional systems, including the paradigmatic XY model. However, most of these systems present a complex interplay between excitations at different length scales that complicates theoretical calculations of nonuniversal thermodynamic quantities. These difficulties may be overcome by suitably modifying the initial conditions of the BKT flow equations to account for noncritical fluctuations at small length scales. In this work, we perform a systematic study of the validity and limits of this tw…
We have computed the quasiparticle wave function corresponding to a hole injected in a triangular antiferromagnet. We have taken into account multi-magnon contributions within the self consistent Born approximation. We have found qualitative differences, under sign reversal of the integral transfer t, regarding the multi-magnon components and the own existence of the quasiparticle excitations. Such differences are due to the subtle interplay between magnon-assisted and free hopping mechanisms. We conclude that the conventional quasiparticle picture can be broken by geometrical frustration with…
Magnetic order and excitations in multiferroic DyMnO3 were studied by neutron scattering experiments using a single crystal prepared with enriched 162Dy isotope. The ordering of Mn moments exhibits pronounced hysteresis arising from the interplay between Mn and Dy magnetism which possesses a strong impact on the ferroelectric polarization. The magnon dispersion resembles that reported for TbMnO3. We identify the excitations at the magnetic zone center and near the zone boundary in the b direction, which can possess electromagnon character. The lowest frequency of the zone-center magnons is in …
Ultrafast spectroscopies constitute a fundamental tool to investigate the dynamics of non-equilibrium many-body states in correlated materials. Two-pulses (pump-probe) experiments have shed new light on the interplay between high-energy electronic excitations and the emerging low-energy properties, such as superconductivity and charge-order, in many interesting materials. Here we will review some recent results on copper oxides and we will propose the use of high-resolution multi-dimensional techniques to investigate the decoherence processes of optical excitations in these systems. This novel…
We report the synthesis and characterization of a new quantum magnet [2-[Bis(2-hydroxybenzyl)aminomethyl]pyridine]Ni(II)-trimer (BHAP-Ni3) in single-crystalline form. Our combined experimental and theoretical investigations reveal an exotic spin state that stabilizes a robust 2/3 magnetization plateau between 7 and 20 T in an external magnetic field. AC-susceptibility measurements show the absence of any magnetic order/glassy state down to 60 mK. The magnetic ground state is disordered and specific-heat measurements reveal the gapped nature of the spin excitations. Most interestingly, our theo…
We investigate the temperature dependent optical properties of NaV2O5, in the energy range 4meV-4eV. The symmetry of the system is discussed on the basis of infrared phonon spectra. By analyzing the optically allowed phonons at temperatures below and above the phase transition, we conclude that a second-order change to a larger unit cell takes place below 34 K, with a fluctuation regime extending over a broad temperature range. In the high temperature undistorted phase, we find good agreement with the recently proposed centrosymmetric space group Pmmn. On the other hand, the detailed analysis …
A synchrotron x-ray diffraction study of the crystallographic structure of PrO2 in the Jahn-Teller distorted phase is reported. The distortion of the oxygen sublattice, which was previously ambiguous, is shown to be a chiral structure in which neighbouring oxygen chains have opposite chiralities. A temperature dependent study of the magnetic excitation spectrum, probed by neutron inelastic scattering, is also reported. Changes in the energies and relative intensities of the crystal field transitions provide an insight into the interplay between the static and dynamic Jahn-Teller effects.
Nonequilibrium dynamics in correlated materials has attracted attention due to the possibility of characterizing, tuning, and creating complex ordered states. To understand the photoinduced microscopic dynamics, especially the linkage under realistic pump conditions between transient states and remnant elementary excitations, we performed nonperturbative simulations of various time-resolved spectroscopies. We used the Mott antiferromagnetic insulator as a model platform. The transient dynamics of multi-particle excitations can be attributed to the interplay between Floquet virtual states and a…
Using dynamic cluster quantum Monte Carlo simulations, we study the superconducting behavior of a 1/8 doped two-dimensional Hubbard model with imposed uni-directional stripe-like charge density wave modulation. We find a significant increase of the pairing correlations and critical temperature relative to the homogeneous system when the modulation length-scale is sufficiently large. With a separable form of the irreducible particle-particle vertex, we show that optimized superconductivity is obtained for moderate modulation strength due to a delicate balance between the modulation enhanced pai…
The ability to electrically-drive spin excitations in molecules with magnetic anisotropy is key for high-density storage and quantum-information technology. Electrons, however, also tunnel via the vibrational excitations unique to a molecule. The interplay of spin and vibrational excitations offers novel routes to study and, ultimately, electrically manipulate molecular magnetism. Here we use a scanning tunneling microscope to electrically induce spin and vibrational excitations in a single molecule consisting of a nickelocene magnetically coupled to a Ni atom. We evidence a vibron-assisted sp…
The infra-red properties of three-dimensional abelian lattice gauge theory are known to be governed by a neutral plasma of magnetic monopole excitations. We address the fate of these monopoles in the presence of light dynamical fermions, using a lattice formulation of compact QED_3 with N_f=4 fermion flavors supplemented by a four-fermi contact term permitting numerical Monte Carlo simulations in the chiral limit. Our data hint at a restoration of chiral symmetry above a critical value of the (inverse) coupling beta. By performing simulations in a sector of non-vanishing magnetic charge, we ar…
It is a widely accepted view that the interplay of spin- and charge-degrees of freedom in doped antiferromagnets (AFMs) gives rise to the rich physics of high-temperature superconductors. Nevertheless, it remains unclear how effective low-energy degrees of freedom and the corresponding field theories emerge from microscopic models, including the $t-J$ and Hubbard Hamiltonians. A promising view comprises that the charge carriers have a rich internal parton structure on intermediate scales, but the interplay of the emergent partons with collective magnon excitations of the surrounding AFM remain…
