The effect of inertial spin dynamics is compared between ferromagnetic, antiferromagnetic and ferrimagnetic systems. The linear response to an oscillating external magnetic field is calculated within the framework of the inertial Landau--Lifshitz--Gilbert equation using analytical theory and computer simulations. Precession and nutation resonance peaks are identified, and it is demonstrated that the precession frequencies are reduced by the spin inertia, while the lifetime of the excitations is enhanced. The interplay between precession and nutation is found to be the most prominent in antiferromagnets, where the timescale of the exchange-driven sublattice dynamics is comparable to inertial relaxation times. Consequently, antiferromagnetic resonance techniques should be better suited for the search for intrinsical inertial spin dynamics on ultrafast timescales than ferromagnetic resonance.
Spin nutation resonance has been well-explored in one-sublattice ferromagnets. Here, we investigate the spin nutation in two-sublattice antiferromagnets as well as, for comparison, ferrimagnets with inter-and intra-sublattice nutation coupling. In particular, we derive the susceptibility of the two-sublattice magnetic system in response to an applied external magnetic field. To this end, the antiferromagnetic and ferrimagnetic (sub-THz) precession and THz nutation resonance frequencies are calculated. Our results show that the precession resonance frequencies and effective damping decrease wit…
The dynamics of a two-level spin system dressed by bichromatic radiation is studied under the conditions of double resonance when the frequency of one (microwave) field is equal to the Larmor frequency of the spin system and the frequency of the other (radio-frequency) field ω_{rf} is close to the Rabi frequency ω_{1} in a micro-wave field. It is shown theoretically that Rabi oscillations between dressed-spin states with the frequency εare accompanied by higher-frequency oscillations at frequencies nω_{rf} and nω_{rf}\pm ε, where n = 1, 2, .... The most intense among these are the signals corr…
We investigate in details the inertial dynamics of a uniform magnetization in the ferromagnetic resonance (FMR) context. Analytical predictions and numerical simulations of the complete equations within the Inertial Landau-Lifshitz-Gilbert (ILLG) model are presented. In addition to the usual precession resonance, the inertial model gives a second resonance peak associated to the nutation dynamics provided that the damping is not too large. The analytical resolution of the equations of motion yields both the precession and nutation angular frequencies. They are function of the inertial dynamics…
The effect of dipolar and exchange interactions within pairs of paramagnetic electronic states on Pauli-blockade-controlled spin-dependent transport and recombination rates during magnetic resonant spin excitation is studied numerically using the superoperator Liouville-space formalism. The simulations reveal that spin-Rabi nutation induced by magnetic resonance can control transition rates which can be observed experimentally by pulsed electrically (pEDMR) and pulsed optically (pODMR) detected magnetic resonance spectroscopies. When the dipolar coupling exceeds the difference of the pair part…
The dynamics of multiphoton transitions in a two-level spin system excited by transverse microwave and longitudinal RF fields with the frequencies w_{mw} and w_{rf}, respectively, is analyzed. The effective time-independent Hamiltonian describing the "dressed" spin states of the "spin + bichromatic field" system is obtained by using the Krylov-Bogoliubov-Mitropolsky averaging method. The direct detection of the time behavior of the spin system by the method of nonstationary nutations makes it possible to identify the multiphoton transitions for resonances w_{0} = w_{mw} + rw_{rf} (w_{0} is the…
Hematite ($α$-Fe$_2$O$_3$) is an antiferromagnetic material with a very low spin damping and high Néel temperature. The temperature dependence of the antiferromagnetic resonance in a bulk single crystal of hematite was characterized from room temperature up to the Néel temperature in the frequency range of 0.19-0.5 THz. From these data, the Néel temperature was estimated as 966 K.
We report measurements of antiferromagnetic resonances in the van der Waals easy-axis antiferromagnet CrSBr. The interlayer exchange field and magnetocrystalline anisotropy fields are comparable to laboratory magnetic fields, allowing a rich variety of gigahertz-frequency dynamical modes to be accessed. By mapping the resonance frequencies as a function of the magnitude and angle of applied magnetic field we identify the different regimes of antiferromagnetic dynamics. The spectra show good agreement with a Landau-Lifshitz model for two antiferromagnetically-coupled sublattices, accounting for…
The magnetization dynamics for ferrimagnets at the angular momentum compensation temperature T_A is believed to be analogous to that for antiferromagnets. We investigated the pulsed-laser-induced magnetization dynamics in amorphous rare-earth transition-metal ferrimagnet films with a T_A just above room temperature. For a low pulse fluence, the magnetization precession frequency decreases as the applied magnetic field increases, whereas for a higher pulse fluence, it increases as the applied field increases. The result was well explained by the left-handed and right-handed precession modes of …
We report on measurements of magnetic field and temperature dependence of antiferromagnetic resonances in the prototypical antiferromagnet NiO. The frequencies of the magnetic resonances in the vicinity of 1 THz have been determined in the time-domain via time-resolved Faraday measurements after selective excitation by narrow-band superradiant terahertz (THz) pulses at temperatures down to 3K and in magnetic fields up to 10 T. The measurements reveal two antiferromagnetic resonance modes, which can be distinguished by their characteristic magnetic field dependencies. The nature of the two mode…
Room-temperature antiferromagnetic resonance in NaMnAs
Charles University(查理大学);Laboratoire National des Champs Magnétiques Intenses, LNCMI-EMFL, CNRS UPR3228, Univ. Grenoble Alpes, Univ. Toulouse, Univ. Toulouse 3, INSA-T(强磁场国家实验室,LNCMI-EMFL,法国国家科学研究中心UPR3228,格勒诺布尔阿尔卑斯大学,图卢兹大学,图卢兹第三大学,国立应用科学学院图卢兹分校);Institute of Physics, Academy of Science of the Czech Republic(捷克科学院物理研究所);Department of Physics, University of Fribourg(弗里堡大学物理系)
The AFMR spectra of the NdFe$_3$(BO$_3$)$_4$ crystal are measured in a wide range of frequencies and temperatures. It is found that by the type of magnetic anisotropy the compound is an "easy-plane" antiferromagnet with a weak anisotropy in the basal plane. The effective magnetic parameters are determined: anisotropy fields $H_{a1}$=1.14 kOe and $H_{a2}$=60 kOe and magnetic excitation gaps $Δν_1$=101.9 GHz and $Δν_2$=23.8 GHz. It is shown that commensurate-incommensurate phase transition causes a shift in resonance field and a considerable change in absorption line width. At temperatures below…
The antiferromagnet is a closed Hermitian system, we find that its excitations, even in the absence of dissipation, can be viewed as a non-Hermitian system with dissipative coupling. Consequently, the antiferromagnetic resonance spectrum does not show the typical level repulsion, but shows the level attraction -- a characteristic behavior often observed in non-Hermitian systems. Such behavior is because the antiferromagnetic ground state is $\mathcal{PT}$-symmetric. This new understanding on antiferromagnetic resonance also explains the mysterious enhancement of antiferromagnetic damping rate.…
We report broadband microwave absorption spectroscopy of the layered antiferromagnet CrCl3. We observe a rich structure of resonances arising from quasi-two-dimensional antiferromagnetic dynamics. Due to the weak interlayer magnetic coupling in this material, we are able to observe both optical and acoustic branches of antiferromagnetic resonance in the GHz frequency range and a symmetry-protected crossing between them. By breaking rotational symmetry, we further show that strong magnon-magnon coupling with large tunable gaps can be induced between the two resonant modes.
In this work, we report ferromagnetic resonance spectroscopy of EuFe2As2 single crystals. We observe ferromagnetic resonance responses, which are attributed to antiferromagnetic resonances of Eu sub-lattice with orthorhombic crystal structure and with different orientations of twin domains relative to the external field. We confirm validity of the recently-proposed spin Hamiltonian with anisotropic Eu-Eu exchange interaction and biquadratic Eu-Fe exchange interaction.
We report on the magnetic resonance of NH_3K_3C_60 powders in the frequency range of 9 to 225 GHz. The observation of an antiferromagnetic resonance below the phase transition at 40 K is evidence for an antiferromagnetically ordered ground state. In the normal state, above 40 K, the temperature dependence of the spin-susceptibilty measured by ESR agrees with previous static measurements and is too weak to be explained by interacting localized spins in an insulator. The magnetic resonance line width has an unusual magnetic-field dependence which is large and temperature independent in the magne…
Stability-threshold control of helicity-selective antiferromagnetic resonance
Institute for Solid State Physics, University of Tokyo(东京大学固体物理研究所);Department of Materials Physics, Nagoya University(名古屋大学物质物理学系);Institute of Industrial Science, The University of Tokyo(东京大学工业科学研究所)
Free electron laser-powered pulsed electron paramagnetic resonance (EPR) experiments performed at 240 GHz / 8.56 T on the crystalline organic radical BDPA reveal a tip-angle dependent resonant frequency. Frequency shifts as large as 11 MHz (45 ppm) are observed during a single Rabi oscillation. We attribute the frequency shifts to a "dressing" of the nutation by spin-spin interactions. A nonlinear semi-classical model which includes a temperature- and sample-geometry-dependent demagnetizing field reproduces experimental results. Because experiments are performed without a cavity, radiation dam…
We consider electron transport in ferromagnets or antiferromagnets sandwiched between metals. When spins in the magnetic materials precess, they emit currents into the surrounding conductors. Generally, adiabatic pumping in mesoscopic systems also enhances current fluctuations. We generalize the description of current fluctuations driven by spin dynamics in three ways using scattering theory. First, our theory describes a general junction with any given electron scattering properties. Second, we consider antiferromagnets as well as ferromagnets. Third, we treat multiterminal devices. Using sho…
Antiferromagnetic (AFM) materials recently have shown interest in the research in spintronics due to its zero stray magnetic field, high anisotropy, and spin orbit coupling. In this context, the bi-metallic AFM Mn2Au has drawn attention because it exhibits unique properties and its Neel temperature is very high. Here, we report spin pumping and inverse spin Hall effect investigations in Mn2Au and CoFeB bilayer system using ferromagnetic resonance. We found large spin Hall angle θ_SH = 0.22
We performed coplanar waveguide-based broadband ferromagnetic resonance experiments on the antiferromagnetic insulator MnF$_2$, while simultaneously recording the DC voltage arising in a thin platinum film deposited onto the MnF$_2$. The antiferromagnetic resonance is clearly reflected in both the transmission through the waveguide as well as the DC voltage in the Pt strip. The DC voltage remains largely unaffected by field reversal and thus presumably stems from microwave rectification and/or heating effects. However, we identify a small magnetic field orientation dependent contribution, comp…
We investigated a system based solely on a single molecular species, Cu(tmdt)$_{2}$, accommodating $d$ and $π$ orbitals within the molecule. $^{13}$C nuclear magnetic resonance measurements captured singlet-triplet excitations of $π$ spins indicating the existence of a $π$-electron-based spin-gapped Mott insulating subsystem, which has been hidden by the large magnetic susceptibility exhibited by the $d$ spins forming antiferromagnetic chains. The present results demonstrate a unique hybrid Mott insulator composed of antiferromagnetic and spin-singlet Mott subsystems with distinctive dimension…
We observe the excitation of collective modes in the THz range driven by the recently discovered Néel spin-orbit torques (NSOT) in the metallic antiferromagnet Mn$_{2}$Au. Temperature dependent THz spectroscopy reveals a strong absorption mode centered near 1 THz, which upon heating from 4 K to 450 K softens and looses intensity. Comparison with the estimated eigenmode frequencies implies that the observed mode is an in-plane antiferromagnetic resonance (AFMR) mode. The AFMR absorption strength exceeds those found in antiferromagnetic insulators, driven by the magnetic field of the THz radiati…
We propose a realization of the electric-field-induced antiferromagnetic resonance. We consider three-dimensional antiferromagnetic insulators with spin-orbit coupling characterized by the existence of a topological term called the $θ$ term. By solving the Landau-Lifshitz-Gilbert equation in the presence of the $θ$ term, we show that, in contrast to conventional methods using ac magnetic fields, the antiferromagnetic resonance state is realized by ac electric fields along with static magnetic fields. This mechanism can be understood as the inverse process of the dynamical chiral magnetic effec…
A detailed study of the angular, energy and polarization dependences of the electric dipolar (E1: 2p->5d) and quadrupolar (E2: 2p->4f) contributions to the x-ray scattering cross-section is presented for holmium in its basal plane spiral antiferromagnetic phase at the L3 edge. The corresponding E1 and E2 scattering factors have been extracted from fits to the experimental energy line shapes taking into account for the first time a split dipole resonance. Using the imaginary part of the resonant scattering factors to retrieve the XMCD spectrum, we find qualitative agreement with the dichroic sp…
Spin canting and complex spin textures in antiferromagnetic materials can often be described in terms of Dzyaloshinskii-Moriya interactions (DMI). Values for DMI parameters are not easily measurable directly, and often inferred from other quantities. In this work, we examine how domain wall dynamics in an antiferromagnetic optomagnonic system can display unique features directly related to the existence of DMI. Our results indicate that the presence of DMI enables spin interactions with cavity photons in a geometry which otherwise allows no magneto-optical coupling, and on the other hand modul…
We use \textit{ab-initio} calculations to investigate spin-orbit torques (SOTs) in FeRh(001) deposited on W(100). Since FeRh undergoes a ferromagnetic-antiferromagnetic phase transition close to room temperature, we consider both phases of FeRh. In the antiferromagnetic case we find that the effective magnetic field of the even torque is staggered and therefore ideal to induce magnetization dynamics or to switch the antiferromagnet (AFM). At the antiferromagnetic resonance the inverse SOT induces a current density, which can be determined from the SOT. In the ferromagnetic case our calculation…
Changes of the electronic structure accompanied by charge localization and a transition to an antiferromagnetic ground state were observed in the (DOEO)$_4$[HgBr$_4$]TCE organic semiconductor. Localization starts in the region of about 150 K and the antiferromagnetic state occurs below 60 K. The magnetic moment of the crystal contains contributions of antiferromagnetic inclusions (droplets), individual paramagnetic centers formed by localized holes and free charge carriers at 2 K. Two types of inclusions of 100-400 nm and 2-5 nm sizes were revealed by transmission electron microscopy. Studying…
Monolayer graphene grown by chemical vapor deposition and transferred to SiO_2 is used to introduce vacancies by Ar^+ ion bombardment at a kinetic energy of 50 eV. The density of defects visible in scanning tunneling microscopy (STM) is considerably lower than the ion fluence implying that most of the defects are single vacancies. The vacancies are characterized by scanning tunneling spectroscopy (STS) on graphene and HOPG exhibiting a peak close to the Fermi level. The peak persists after air exposure up to 180 min, albeit getting broader. After air exposure for less than 60 min, electron spi…
We observed surface acoustic wave (SAW) propagation on a multiferroic material CuB$_2$O$_4$ with use of two interdigital transducers (IDTs). The period of IDT fingers is as short as 1.6 $μ$m so that the frequency of SAW is 3 GHz, which is comparable with that of magnetic resonance. In antiferromagnetic phase, the SAW excitation intensity varied with the magnitude and direction of the magnetic field, owing to the dynamical coupling between SAWs and antiferromagnetic resonance of CuB$_2$O$_4$. The microscopic mechanism is discussed based on the symmetrically allowed magentoelastic coupling.
The CeIn3-xSnx cubic heavy fermion system presents an antiferromagnetic transition at T_N = 10 K, for x = 0, that decreases continuously down to 0 K upon Sn substitution at a critical concentration of x_c ~ 0.65. In the vicinity of T_N -> 0 the system shows non-Fermi liquid behavior due to antiferromagnetic critical fluctuations. For a high Sn content, x > 2.2, intermediate valence effects are present. In this work we show that Gd3+-doped electron spin resonance (ESR) probes a change in the character of the Ce 4f electron, as a function of Sn substitution. The Gd3+ ESR results indicate a trans…
We report the low-temperature multi-frequency ESR studies of copper pyrimidine dinitrate, a spin-1/2 antiferromagnetic chain with alternating $g$-tensor and the Dzyaloshinskii-Moriya interaction, allowing us to test a new theoretical concept proposed recently by Oshikawa and Affleck [Phys. Rev. Lett. 82, 5136 (1999)]. Their theory, based on bosonization and the self-energy formalism, can be applied for precise calculation of ESR parameters of $S=1/2$ antiferromagnetic chains in the perturbative spinon regime. Excellent quantitative agreement between the theoretical predictions and experiment i…
We have prepared crystalline nanowires (diameter ~ 50 nm, length ~ a few microns) of the charge ordering manganite Pr_0.5Ca_0.5Mn_O3 using a low reaction temperature hydrothermal method and characterized them using X-ray diffraction, transmission electron microscopy, SQUID magnetometry and electron magnetic resonance measurements. While the bulk sample shows a charge ordering transition at 245 K and an antiferromagnetic transition at 175 K, SQUID magnetometry and electron magnetic resonance experiments reveal that in the nanowires phase, a ferromagnetic transition occurs at ~ 105 K. Further, t…
We have studied the ground state of a fullerene--based magnet, the $α'$--phase tetra--$kis$--(dimethylamino)--ethylene--C$_{60}$ ($α'$--TDAE--C$_{60}$), by electron spin resonance (ESR) and magnetic torque measurements. Below T$_N=7$ K, non--paramagnetic field dependent resonances with a finite excitation gap (1.7 GHz) are observed along the $a$--axis. Strong enhancement in their intensity as temperature is decreased is inconsistent with excitation from a singlet state, which had been proposed for the $α'$--phase ground state. Below T$_N$, non--quadratic field dependence of magnetic torque sig…
We measured two magnetic modes with finite and discrete energies in an antiferromagnetic ordered phase of a geometrically frustrated magnet MgCr2O4 by single-crystal inelastic neutron scattering, and clarified the spatial spin correlations of the two levels: one is an antiferromagnetic hexamer and the other is an antiferromagnetic heptamer. Since these correlation types are emblematic of quasielastic scattering with geometric frustration, our results indicate instantaneous suppression of lattice distortion in an ordered phase by spin-lattice coupling, probably also supported by orbital and cha…
We revisit the magnetic properties of the antiferromagnetic Kondo lattice CeNiAsO by $^{75}$As nuclear magnetic resonance measurements. Our results confirm two successive antiferromagnetic transitions of Ce moments at $T_{N1}=9.0(3)$ K and $T_{N2}=7.0(3)$ K. Incommensurate and commensurate antiferromagnetic orders are suggested for $T_{N2}<T<T_{N1}$ and $T<T_{N2}$ respectively, consistent with previous neutron and muon experiments. A Knight shift anomaly, characterized by the failure of $K(T)-χ(T)$ scaling, is observed below $T^*\sim15$ K, which gives a measure of the onset of coherent $c-f$ c…
We study the effects of 10% Cr substitution in Mn sites of Bi0.5Sr0.5MnO3 on the antiferromagnetic (AFM) (TN ~ 110 K) transition using structural, magnetic and electron paramagnetic resonance (EPR) techniques. Field cooled (FC) and zero field cooled (ZFC) magnetization measurements done from 400 K down to 4 K show that the compound is in the paramagnetic (PM) phase till 50 K where it undergoes a transition to a short range ferromagnetic phase (FM). Electron paramagnetic resonance measurements performed in the temperature range 300 K till 80 K conform with the magnetization measurements as symm…
We investigate the impact of pinned antiferromagnetic order on the decoherence of spin current in polycrystalline IrMn. In NiFe/Cu/IrMn/CoFe multilayers, we coherently pump an electronic spin current from NiFe into IrMn, whose antiferromagnetic order is globally pinned by static exchange-bias coupling with CoFe. We observe no anisotropic spin decoherence with respect to the orientation of the pinned antiferromagnetic order. We also observe no difference in spin decoherence for samples with and without pinned antiferromagnetic order. Moreover, although there is a pronounced resonance linewidth …
The heavy-fermion system $\mathrm{UTe_2}$ is a candidate for spin-triplet superconductivity, which is of considerable interest to quantum engineering. Among the outstanding issues is the nature of the pairing state. A recent surprising discovery is the observation of a resonance in the spin excitation spectrum at an antiferromagnetic wavevector [C. Duan {\it et al.}, Nature \textbf{600}, 636 (2021)], which stands in apparent contrast to the ferromagnetic nature of the interactions expected in this system. We show how the puzzle can be resolved by a multiorbital spin-triplet pairing constructed…
We search for dynamical magnetoelectric phenomena in three-dimensional correlated systems with spin-orbit coupling. We focus on the antiferromagnetic insulator phases where the dynamical axion field is realized by the fluctuation of the antiferromagnetic order parameter. It is shown that the dynamical chiral magnetic effect, an alternating current generation by magnetic fields, emerges due to the time dependences of the order parameter such as antiferromagnetic resonance. It is also shown that the anomalous Hall effect arises due to the spatial variations of the order parameter such as antifer…
Two-dimensional (2D) materials enable new types of magnetic and electronic phases mediated by their reduced dimensionality like magic-angle induced phase transitions, 2D Ising antiferromagnets and ferromagnetism in 2D atomic layers and heterostructures. However, only a few methods are available to study these phase transitions, which for example is particularly challenging for antiferromagnetic materials. Here, we demonstrate that these phases can be probed by the mechanical motion: the temperature dependent resonance frequency and quality factor of multilayer 2D material membranes show clear …