The efficiency of ultrafast excitation of spins in antiferromagnetic $\mathrm{α-Fe_{2}O_{3}}$ using nearly single-cycle THz pulse is studied as a function of the polarization of the THz pulse and the sample temperature. Above the Morin point the most efficient excitation is achieved when the magnetic field of the THz pulse is perpendicular to the antiferromagnetically coupled spins. Using the experimental results and equations of motion for spins, we show that the mechanism of the spin excitation above and below the Morin point relies on magnetic-dipole interaction of the THz magnetic field with spins and the efficiency of the coupling is proportional to the time derivative of the magnetic field.
Excitation, detection and control of coherent THz magnetic excitation in antiferromagnets are challenging problems that can be addressed using ever shorter laser pulses. We study experimentally excitation of magnetic dynamics at THz frequencies in an antiferromagnetic insulator CoF$_2$ by sub-10 fs laser pulses. Time-resolved pump-probe polarimetric measurements at different temperatures and probe polarizations reveal laser-induced transient circular birefringence oscillating at the frequency of 7.45 THz and present below the Néel temperature. The THz oscillations of circular birefringence are…
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…
Understanding spin-lattice coupling represents a key challenge in modern condensed matter physics, with crucial importance and implications for ultrafast and 2D-magnetism. The efficiency of angular momentum and energy transfer between spins and the lattice imposes fundamental speed limits on the ability to control spins in spintronics, magnonics and magnetic data storage. We report on an efficient nonlinear mechanism of spin-lattice coupling driven by THz light pulses. A nearly single-cycle THz pulse resonantly interacts with a coherent magnonic state in the antiferromagnet CoF2 and excites th…
We report on THz time-domain spectroscopy on multiferroic GeV4S8, which undergoes orbital ordering at a Jahn-Teller transition at 30.5 K and exhibits antiferromagnetic order below 14.6 K. The THz experiments are complemented by dielectric experiments at audio and radio frequencies. We identify a low-lying excitation close to 15 cm-1, which is only weakly temperature dependent and probably corresponds to a molecular excitation within the electronic level scheme of the V4 clusters. In addition, we detect complex temperature-dependent behavior of a low-lying phononic excitation, closely linked to…
THz magnetization dynamics is excited in ferrimagnetic thulium iron garnet with a picosecond, single-cycle magnetic field pulse and seen as a high-frequency modulation of the magneto-optical Faraday effect. Data analysis combined with numerical modelling and evaluation of the effective Lagrangian allow us to conclude that the dynamics corresponds to the exchange mode excited by Zeeman interaction of the THz field with the antiferromagnetically coupled spins. We argue that THz-pump IR-probe experiments on ferrimagnets offer a unique tool for quantitative studies of dynamics and mechanisms to co…
The $\mathrm{Co_2}$ family of ferromagnetic Heusler alloys have attracted interest due to their fully spin-polarized nature, making them ideal for applications in spintronic devices. More recently, the existence of room temperature time-reversal-breaking Weyl nodes near the Fermi level was predicted and confirmed in these systems. As a result of the presence of these Weyl nodes, these systems possess a non-zero momentum space Berry curvature that can dramatically influence transport properties such as the anomalous Hall effect. One of these candidate compounds is $\mathrm{Co_2 Ti Ge}$. Recentl…
Evidence for a Dual-Source Mechanism of THz Radiation from Rectangular Mesas of Single Crystalline \bm{$\mathrm{Bi_2Sr_2CaCu_2O_{8+δ}}$} Intrinsic Josephson Junctions
Graduate School of Pure & Applied Sciences, University of Tsukuba（筑波大学理工学群）；Department of Physics, University of Central Florida（中佛罗里达大学物理系）
The impulsive generation of two-magnon modes in antiferromagnets by femtosecond optical pulses, so-called femto-nanomagnons, leads to coherent longitudinal oscillations of the antiferromagnetic order parameter that cannot be described by a thermodynamic Landau-Lifshitz approach. We argue that this dynamics is triggered as a result of a laser-induced modification of the exchange interaction. In order to describe the oscillations we have formulated a quantum mechanical description in terms of magnon pair operators and coherent states. Such an approach allowed us to} derive an effective macroscop…
We report on optical excitations in the magnetically ordered phases of multiferroic Fe$_{1.86}$Zn$_{0.14}$Mo$_3$O$_8$ in the frequency range from 10-130 cm$^{-1}$ (0.3-3.9 THz). In the collinear easy-axis antiferromagnetic phase below $T_N=50$~K eleven optically active modes have been observed in finite magnetic fields, assuming that the lowest-lying mode is doubly degenerate. The large number of modes reflects either a more complex magnetic structure than in pure Fe$_{2}$Mo$_3$O$_8$ or that spin stretching modes become active in addition to the usual spin precessional modes. Their magnetic fi…
Thermal expansion, magnetostriction and magnetization measurements under magnetic field and hydrostatic pressure were performed on a $\mathrm{UAu_{2}Si_{2}}$ single crystal. They revealed a large anisotropy of magnetoelastic properties manifested by prominent length changes leading to a collapse of the unit-cell volume accompanied by breaking the fourfold symmetry (similar to that in $\mathrm{URu_{2}Si_{2}}$ in the hidden-order state) in the antiferromagnetic state as consequences of strong magnetoelastic coupling. The magnetostriction curves measured at higher temperatures confirm a bulk char…
We investigate spin dynamics in the antiferromagnetic (AFM) multiferroic TbMnO3 using optical- pump, terahertz (THz)-probe spectroscopy. Photoexcitation results in a broadband THz transmission change, with an onset time of 25 ps at 6 K that becomes faster at higher temperatures. We attribute this time constant to spin-lattice thermalization. The excellent agreement between our measurements and previous ultrafast resonant x-ray diffraction measurements on the same material confirms that our THz pulse directly probes spin order. We suggest that this could be the case in general for insulating AF…
Non-reciprocal directional dichroism, also called the optical-diode effect, is an appealing functional property inherent to the large class of non-centrosymmetric magnets. However, the in-situ electric control of this phenomenon is challenging as it requires a set of conditions to be fulfilled: Special symmetries of the magnetic ground state, spin-excitations with comparable magnetic- and electric-dipole activity and switchable electric polarization. We demonstrate the isothermal electric switch between domains of Ba$_2$CoGe$_2$O$_7$ possessing opposite magnetoelectric susceptibilities. Combin…
Coherent spin oscillations were non-thermally induced by circularly polarized pulses in fully compensated antiferromagnetic NiO. This effect is attributed to an entirely new mechanism of the action, on the spins, of the effective magnetic field generated by an inverse Faraday effect. The novelty of this mechanism is that spin oscillations are driven by the time derivative of the effective magnetic field acting even on "pure" antiferromagnets with zero net magnetic moment in the ground state. The measured frequencies (1.07 THz and 140 GHz) of the spin oscillations correspond to the out-of-plane…
The Kondo semiconductor CeOs$_{2}$Al$_{10}$ exhibits an antiferromagnetic (AFM) order at $T_\mathrm{N}= 28.5$ K, whose temperature is unexpectedly high for the small ordered moment of $0.3$ $μ_\mathrm{B}/$Ce. We have studied the effects of electron- and hole-doping on the hybridization gap and AFM order by measuring the magnetization $M$, magnetic susceptibility $χ$, electrical resistivity $ρ$, and specific heat $C$ on single crystals of Ce(Os$_{1-x}$Ir$_{x}$)$_{2}$Al$_{10}$($x \le 0.15$) and Ce(Os$_{1-y}$Re$_{y}$)$_{2}$Al$_{10}$($y \le 0.1$). The results of $M (B)$ indicates that the AFM orde…
We make use of the strong spin-charge coupling in the electron-doped cuprate $\mathrm{Nd}_{2-x}\mathrm{Ce}_x\mathrm{CuO}_4$ to probe changes in its spin system via magnetotransport measurements. We present a detailed study of the out-of-plane magnetoresistance in underdoped single crystals of this compound, including the nonsuperconducting, $0.05\,\leq x\,\leq 0.115$, and superconducting, $0.12\,\leq x\,\leq 0.13$, compositions. Special focus is put on the dependence of the magnetoresistance on the field orientation in the plane of the CuO$_2$ layers. In addition to the kink at the field-induc…
With extensive variational Monte Carlo simulation, we show that the uniform resonating valence bond state(U-RVB) on square lattice is actually antiferromagnetic long range ordered. The ordered moment is estimated to be $m\approx 0.17$. Finite size scaling analysis on lattice up to lattice size of $50\times 50$ shows that the spin structure factor at the antiferromagnetic ordering wave vector follows perfectly the $\mathrm{S}_{\mathrm{q}=(π,π)} \simeq S_{0}+α(1/L)^{5/4}$ behavior, where $L$ is linear scale of the lattice. Such a behavior is quite unexpected from the slave Boson mean field treat…
We report a neutron diffraction study of single-crystal CePtAl$_3$ complemented by measurements of the specific heat under applied magnetic field. Below $T_\mathrm{N}$=3 K CePtAl$_3$ develops incommensurate antiferromagnetic order with a single modulation vector $\vec{k}$=$(0.676 \, 0 \, 0)$. Residual magnetic scattering intensity above $T_\mathrm{N}$ and a broadening of the specific heat anomaly at $T_\mathrm{N}$ may be consistently described in terms of a Gaussian distribution of transition temperatures with a standard deviation $σ\approx0.5\,{\rm K}$. The distribution of $T_\mathrm{N}$ may …
Charge excitations across an electronic band gap play an important role in opto-electronics and light harvesting. In contrast to conventional semiconductors, studies of above-band-gap photoexcitations in strongly correlated materials are still in their infancy. Here we reveal the ultrafast dynamics controlled by Hund's physics in strongly correlated photo-excited NiO. By combining time-resolved two-photon photoemission experiments with state-of-the-art numerical calculations, an ultrafast ($\lesssim$ 10\,fs) relaxation due to Hund excitations and related photo-induced in-gap states are identif…
We report the magnetocaloric effect (MCE) in a polycrystalline plumbide sample of $\mathrm{Ho_2Pd_2Pb}$. Arc-melted $\mathrm{Ho_2Pd_2Pb}$ crystallizes in $\mathrm{Mo_2B_2Fe}$ type of tetragonal crystal structure and shows an antiferromagnetic behavior with Néel temperature of 4.5 K. The Arrott plots indicate that $\mathrm{Ho_2Pd_2Pb}$ undergoes a second-order antiferromagnetic phase transition. The calculated isothermal magnetic entropy change ($ΔS_m$), and relative power cooling (refrigeration capacity) for a change of field 0-8 T are 17.8 J.kg$^{-1}$.K$^{-1}$, and 680(497)~J.kg$^{-1}$ respec…
We report on magnetization, specific heat and resistivity experiments on single crystals of the novel heavy Fermion compound Ce$_3$PdIn$_{11}$. At ambient pressure the compound exhibits two successive transitions at T$_{1}$ = 1.63 K and T$_{\mathrm {N}}$ = 1.49 K into incommensurate and commensurate local moment antiferromagnetic states, respectively, before becoming superconducting below T$_{\mathrm {c}}$ = 0.42 K. The large values of dB$_{\mathrm {c2}}$/dT and B$_{\mathrm {c2}}$ = 2.8 T imply that heavy quasiparticles form the Cooper pairs. Thus, Ce$_{3}$PdIn$_{11}$ is the first ambient pres…
Coherent control of individual molecular spins in nano-devices is a pivotal prerequisite for fulfilling the potential promised by molecular spintronics. By applying electric field pulses during time-resolved electron spin resonance measurements, we measure the sensitivity of the spin in several antiferromagnetic molecular nanomagnets to external electric fields. We find a linear electric field dependence of the spin states in Cr$_7$Mn, an antiferromagnetic ring with a ground-state spin of $S=1$, and in a frustrated Cu$_3$ triangle, both with coefficients of about $2~\mathrm{rad}\, \mathrm{s}^{…
The magnetic, thermal and transport properties as well as electronic band structure of MnPtSi are reported. MnPtSi is a metal that undergoes a ferromagnetic transition at $T_{\mathrm{C}}=340$(1) K and a spin-reorientation transition at $T_{\mathrm{N}}=326$(1) K to an antiferromagnetic phase. First-principles electronic structure calculations indicate a not-fully polarized spin state of Mn in a $d^5$ electron configuration with $J=S=3$/2, in agreement with the saturation magnetization of 3~$μ_{\mathrm{B}}$ in the ordered state and the observed paramagnetic effective moment. A sizeable anomalous…
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 …
We present results of single crystal neutron diffraction experiments on the rare-earth, half-Heusler antiferromagnet (AFM) NdBiPt. This compound exhibits an AFM phase transition at $T_{\mathrm N}=2.18$~K with an ordered moment of $1.78(9)$~$μ_{\mathrm B}$ per Nd atom. The magnetic moments are aligned along the $[001]$-direction, arranged in a type-I AFM structure with ferromagnetic planes, alternating antiferromagnetically along a propagation vector $τ$ of $(100)$. The $R$BiPt ($R$= Ce-Lu) family of materials has been proposed as candidates of a new family of antiferromagnetic topological insu…
Motivated by the experimentally observed $\sqrt{5} \times \sqrt{5}$ iron vacancy order and a block spin antiferromagnetic phase with large magnetic moment in $\mathrm{K}_{0.8}\mathrm{Fe}_{1.6}\mathrm{Se}_2$, we study the magnetic phase diagram of an extended $J_1-J_2$ model on a 1/5-depleted square lattice with $\sqrt{5} \times \sqrt{5}$ vacancy order, using a classical Monte Carlo analysis. The magnetic phase diagram involves various antiferromagnetically ordered phases, and most of them have higher order commensuration. We find that the experimentally relevant block-spin state occupies a sig…
We demonstrate a new approach for directly measuring the ultrafast energy transfer between elec- trons and magnons, enabling us to track spin dynamics in an antiferromagnet (AFM). In multiferroic HoMnO3, optical photoexcitation creates hot electrons, after which changes in the spin order are probed with a THz pulse tuned to a magnon resonance. This reveals a photoinduced transparency, which builds up over several picoseconds as the spins heat up due to energy transfer from hot elec- trons via phonons. This spin-lattice thermalization time is ?10 times faster than that of typical ferromagnetic …
Nonclassical dynamics of Néel vector and magnetization accompanied by THz and high-harmonic radiation from ultrafast-light-driven NiO antiferromagnet insulator
CeIrSn with a quasikagome Ce lattice in the hexagonal basal plane is a strongly valence fluctuating compound, as we confirm by hard x-ray photoelectron spectroscopy and inelastic neutron scattering, with a high Kondo temperature of $T_{\mathrm{K}}\sim 480$\,K. We report a negative in-plane thermal expansion $α/T$ below 2\,K, which passes through a broad minimum near 0.75\,K. Volume and $a$-axis magnetostriction for $B \parallel a$ are markedly negative at low fields and change sign before a sharp metamagnetic anomaly at 6\,T. These behaviors are unexpected for Ce-based intermediate valence sys…
We report a variation with temperature ($T$) of the effective interdimeric interaction $J^\prime_{\mathrm{eff}}$ in the antiferromagnetic (AFM) copper dimeric organic compound Cu$_2$[TzTs]$_4$ [N-thiazol-2-yl-toluenesulfonamidate Cu$^\mathrm{II}$]. This $T$ dependence was obtained from measurements of the effects in the electron paramagnetic resonance (EPR) spectra of the proposed quantum phase transition associated to the exchange narrowing processes. Cu$_2$[TzTs]$_4$ contains exchange coupled pairs of Cu$^\mathrm{II}$ spins $\mathbf{S_\mathrm{A}}$ and $\mathbf{S_\mathrm{B}}$ ($S$ = 1/2), wit…
Using THz spectroscopy, we show that the spin-wave spectrum of multiferroic BiFeO$_3$ in its high-field canted antiferromagnetic state is well described by a spin model that violates rhombohedral symmetry. We demonstrate that the monoclinic distortion of the canted antiferromagnetic state is induced by the single-ion magnetoelastic coupling between the lattice and the two nearly anti-parallel spins. The revised spin model for BiFeO$_3$ contains two new single-ion anisotropy terms that violate rhombohedral symmetry and depend on the direction of the magnetic field.
BaMn$_{2}$As$_{2}$ is an antiferromagnetic insulator where a metal-insulator transition occurs with hole doping via the substitution of Ba with K. The metal-insulator transition causes only a small suppression of the Néel temperature ($T_\mathrm{N}$) and the ordered moment, suggesting that doped holes interact weakly with the Mn spin system. Powder inelastic neutron scattering measurements were performed on three different powder samples of Ba$_{1-x}$K$_{x}$Mn$_{2}$As$_{2}$ with $x=$0, 0.125 and 0.25 to study the effect of hole doping and metallization on the spin dynamics of these compounds. …
Multimodal Terahertz Spectroscopy of the Pairing Symmetry and Normal-State Pseudogap in (La,Pr)$_3$Ni$_2$O$_7$ Films
Center for High Pressure Science and Technology Advanced Research（高压科学实验中心）；International Center for Quantum Materials, School of Physics, Peking University（北京大学物理学院量子材料国际中心）；Quantum Science Center of Guangdong-Hong Kong-Macao Greater Bay Area（粤港澳大湾区量子科学中心）；Department of Physics and Guangdong Basic Research Center of Excellence for Quantum Science, Southern University of Science and Technology（南方科技大学物理系及广东省量子科学基础研究中心）；Beijing Academy of Quantum Information Sciences（北京量子信息科学研究院）；Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所凝聚态物理国家实验室）；Tsung-Dao Lee Institute, Department of Physics and Astronomy, Shanghai Jiao Tong University（上海交通大学物理与天文学院李政道研究所）；Department of Physics, Tsinghua University（清华大学物理系）
We report on THz absorption spectroscopy combined with high magnetic fields of polycrystalline RCrO3 (R= Pr, Sm, Er) aiming understanding spin wave resonances at their low temperature magnetic phases. Our measurements show that the temperature, and the implicit anisotropies at which the Cr3+ spin reorientation at TSR takes place, are determinant on the ferromagnetic-like (FM) and the antiferromagnetic-like (AFM) spin modes being optically active. It is found that they are dependent on Rare Earth 4f moment and ion size. We also studied temperature and field dependence of crystal field levels in…
We report $^{31}$P NMR studies of an oriented polycrystalline superconductor of Ba$_{0.5}$Sr$_{0.5}$Fe$_{2}$(As$_{1-x}$P$_{x}$)$_{2}$ with $x\sim$ 0.4 ($T_\mathrm{c}$ = 29 K) at $T$ = 14$-$325 K and $B_{0}$ = 1 and 5 T. The $^{31}$P Knight shift $K_{ab}$ at $B_{0}\perp c$ shows a nearly $T$-independent uniform spin susceptibility above $T_\mathrm{c}$ and a spin singlet decrease below $T_\mathrm{c}$. The $^{31}$P nuclear spin-lattice relaxation rate 1/$T_{1}$ shows an asymptotic behavior of $a+bT$ ($a$ and $b$ are constants) at $T >$ 100 K and the minimum at 40 K with an upturn toward $T_\mathr…
The coherence of collective modes, such as phonons, and their modulation of the electronic states are long sought in complex systems, which is a cross-cutting issue in photovoltaics and quantum electronics. In photovoltaic cells and lasers based on metal halide perovskites, the presence of polaronic coupling, i.e., photocarriers dressed by the macroscopic motion of charged lattice, assisted by terahertz (THz) longitudinal optical (LO) phonons, has been intensely studied yet still debated. This may be key for explaining the remarkable properties of the perovskite materials, e.g., defect toleran…
We report the low-temperature properties of phase-pure single crystals of the half-Heusler compound CuMnSb grown by means of optical float-zoning. The magnetization, specific heat, electrical resistivity, and Hall effect of our single crystals exhibit an antiferromagnetic transition at $T_{\mathrm{N}} = 55~\mathrm{K}$ and a second anomaly at a temperature $T^{*} \approx 34~\mathrm{K}$. Powder and single-crystal neutron diffraction establish an ordered magnetic moment of $(3.9\pm0.1)~μ_{\mathrm{B}}/\mathrm{f.u.}$, consistent with the effective moment inferred from the Curie-Weiss dependence of …
We report both experimental and theoretical investigations of the physical properties of Ba$_\mathrm{2}$Mn$_\mathrm{2}$Sb$_\mathrm{2}$O single crystals. This material exhibits a hexagonal structure with lattice constants: a = 4.7029(15) Å and c = 19.9401(27) Å, as obtained from powder X-ray diffraction measurements, and in agreement with structural optimization through density functional theory (DFT) calculations. The magnetic susceptibility and specific heat show anomalies at T$_\mathrm{N}$ = 60 K, consistent with antiferromagnetic ordering. However, the magnitude of T$_\mathrm{N}$ is signifi…
Inelastic neutron scattering measurements of paramagnetic SrCo$_{2}$As$_{2}$ at T=5 K reveal antiferromagnetic (AFM) spin fluctuations that are peaked at a wavevector of $\textbf{Q}_{\mathrm{AFM}}=(1/2,1/2,1)$ and possess a large energy scale. These stripe spin fluctuations are similar to those found in $A$Fe$_{2}$As$_{2}$ compounds, where spin-density wave AFM is driven by Fermi surface nesting between electron and hole pockets separated by $\textbf{Q}_{\mathrm{AFM}}$. SrCo$_{2}$As$_{2}$ has a more complex Fermi surface and band structure calculations indicate a potential instability towards …
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…
