In recent years, the optical control of exchange interactions has emerged as an exciting new direction in the study of the ultrafast optical control of magnetic order. Here we review recent theoretical works on antiferromagnetic systems, devoted to i) simulating the ultrafast control of exchange interactions, ii) modeling the strongly nonequilibrium response of the magnetic order and iii) the relation with relevant experimental works developed in parallel. In addition to the excitation of spin precession, we discuss examples of rapid cooling and the control of ultrafast coherent longitudinal spin dynamics in response to femtosecond optically induced perturbations of exchange interactions. These elucidate the potential for exploiting the control of exchange interactions to find new scenarios for both faster and more energy-efficient manipulation of magnetism.
Photo-excitation in complex oxides1 transfers charge across semicovalent bonds, drastically perturbing spin and orbital orders2. Light may then be used in compounds like magnetoresistive manganites to control magnetism on nanometre lengthscales and ultrafast timescales. Here, we show how ultrafast resonant soft x-ray diffraction can separately probe the photo-induced dynamics of spin and orbital orders in La0.5Sr1.5MnO4. Ultrafast melting of CE antiferromagnetic spin order is evidenced by the disappearance of a (1/4,1/4,1/2) diffraction peak. On the other hand the (1/4,1/4,0) peak, reflecting …
We investigate the efficiency of the recently proposed Restricted Boltzmann Machine (RBM) representation of quantum many-body states to study both the static properties and quantum spin dynamics in the two-dimensional Heisenberg model on a square lattice. For static properties we find close agreement with numerically exact Quantum Monte Carlo results in the thermodynamical limit. For dynamics and small systems, we find excellent agreement with exact diagonalization, while for systems up to N=256 spins close consistency with interacting spin-wave theory is obtained. In all cases the accuracy co…
Photoirradiation effects in correlated electrons coupled with localized spins are studied based on the extended double-exchange model. In particular, we examine melting of an antiferromagnetic (AFM) charge order insulating state by varying the light intensity. When intense light is irradiated, the AFM insulating characteristics are strengthened, rather than change into the ferromagnetic metallic characteristic, which are expected from the conventional double exchange interaction when carriers are introduced by weak light irradiation or chemical doping. This provides a new principle for optical…
Optical control of magnetism, of interest for high-speed data processing and storage, has only been demonstrated with near-infrared excitation to date. However, in absorbing materials, such high photon energies can lead to significant dissipation, making switch back times long and miniaturization challenging. In manganites, magnetism is directly coupled to the lattice, as evidenced by the response to external and chemical pressure, or to ferroelectric polarization. Here, femtosecond mid-infrared pulses are used to excite the lattice in La0.5Sr1.5MnO4 and the dynamics of electronic order are me…
Although ultrafast manipulation of magnetism holds great promise for new physical phenomena and applications, targeting specific states is held back by our limited understanding of how magnetic correlations evolve on ultrafast timescales. Using ultrafast resonant inelastic x-ray scattering we demonstrate that femtosecond laser pulses can excite transient magnons at large wavevectors in gapped antiferromagnets, and that they persist for several picoseconds which is opposite to what is observed in nearly gapless magnets. Our work suggests that materials with isotropic magnetic interactions are p…
The strongest interaction between microscopic spins in magnetic materials is the exchange interaction $J_\text{ex}$. Therefore, ultrafast control of $J_\text{ex}$ holds the promise to control spins on ultimately fast timescales. We demonstrate that time-periodic modulation of the electronic structure by electric fields can be used to reversibly control $J_\text{ex}$ on ultrafast timescales in extended antiferromagnetic Mott insulators. In the regime of weak driving strength, we find that $J_\text{ex}$ can be enhanced and reduced for frequencies below and above the Mott gap, respectively. Moreo…
The multiferroic compound CuO exhibits low temperature magnetic properties similar to antiferromagnetic iron oxides, while the electronic properties have much more in common with the high $T_c$ cuprate superconductors. This suggests novel possibilities for the ultrafast optical excitation of magnetism. On the basis on atomistic spin dynamics simulations, we study the effect of phonon-assisted multimagnon absorption and photodoping on the spin dynamics in the vicinity of the first-order phase transition from collinear to spin-spiral magnetic order. Similar as in recent experiments, we find that…
The original observation of the Einstein-de Haas effect was a landmark experiment in the early history of modern physics that illustrates the relationship between magnetism and angular momentum. Today the effect is still discussed in elementary physics courses to demonstrate that the angular momentum associated with the aligned electron spins in a ferromagnet can be converted to mechanical angular momentum by reversing the direction of magnetisation using an external magnetic field. In recent times, a related problem in magnetism concerns the time-scale over which this angular momentum transfe…
We study the photoinduced ultrafast dynamics in relativistic Mott insulators, i.e., Mott insulators with strong spin-orbit coupling. For this purpose, we consider a minimal one-band Hubbard model on lattices with square and triangular symmetries, as relevant for layered transition metal compounds such as Sr$_2$IrO$_4$. Depending on the lattice and the spin-orbit coupling, the systems have canted antiferromagnetic or $120^\circ$ order. They are excited by simulating a short laser pulse, and the dynamics is solved using nonequilibrium dynamical mean-field theory. The pulse generates hot carriers…
Understanding ultrafast magnetization dynamics on the microscopic level is of strong current interest due to the potential for applications in information storage. In recent years, the spin-lattice coupling has been recognized to be essential for ultrafast magnetization dynamics. Magnetoelectric multiferroics of type II possess intrinsic correlations among magnetic sublattices and electric polarization (P) through spin-lattice coupling, enabling fundamentally coupled dynamics between spins and lattice. Here we report on ultrafast magnetization dynamics in a room-temperature multiferroic hexafe…
We investigate entanglement dynamics in the antiferromagnetic Heisenberg model in two dimensions following a spatially anisotropic quench of the exchange interactions. Opposed to established results in one dimension, the magnon quasiparticles show an initial growth of entanglement dynamics that does not depend on the system size and is governed by the oscillation period of the exchange interaction. We ascribe this to the dominance of the intrinsic entanglement of short wavelength non-propagating magnon-pairs, which also leads to a competition between area-law and volume-law contribution in the…
Nonequilibrium many-body dynamics is becoming one of the central topics of modern condensed matter physics. Floquet topological states were suggested to emerge in photodressed band structures in the presence of periodic laser driving. Here we propose a viable nonequilibrium route without requiring coherent Floquet states to reach the elusive magnetic Weyl semimetallic phase in pyrochlore iridates by ultrafast modification of the effective electron-electron interaction with short laser pulses. Combining \textit{ab initio} calculations for a time-dependent self-consistent reduced Hubbard $U$ con…
Ultrafast giant enhancement of second harmonic generation in a strongly correlated cobaltite
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北京实验室）；University of Chinese Academy of Sciences（中国科学院大学）；International Center for Quantum Materials, School of Physics, Peking University（北京大学物理学院量子材料科学中心）；School of Electronic and Information Engineering, Beihang University（北京航空航天大学电子信息工程学院）；School of Physics and Center of Quantum Materials and Devices, Chongqing University（重庆大学物理学院量子材料与器件中心）；School of Materials Science and Engineering, Nankai University（南开大学材料科学与工程学院）
In the mixed-valence manganites, a near-infrared laser typically melts the orbital and spin order simultaneously, corresponding to the photoinduced $d^{1}d^{0}$ $\xrightarrow{}$ $d^{0}d^{1}$ excitations in the Mott-Hubbard bands of manganese. Here, we use ultrafast methods -- both femtosecond resonant x-ray diffraction and optical reflectivity -- to demonstrate that the orbital response in the layered manganite Nd$_{1-x}$Sr$_{1+x}$MnO$_{4}$ ($\it{x}$ = 2/3) does not follow this scheme. At the photoexcitation saturation fluence, the orbital order is only diminished by a few percent in the trans…
Ultrafast Terahertz and Optical Spectroscopy under Synergetic Extreme Conditions
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）；School of Physical Sciences, University of Chinese Academy of Sciences（中国科学院大学物理科学学院）；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紫江研究院）；International Center for Quantum Materials, School of Physics, Peking University（北京大学物理学院量子材料科学中心）
Wide-band-gap insulators such as NiO offer the exciting prospect of coherently manipulating electronic correlations with strong optical fields. Contrary to metals where rapid dephasing of optical excitation via electronic processes occurs, the sub-gap excitation in charge-transfer insulators has been shown to couple to low-energy bosonic excitations. However, it is currently unknown if the bosonic dressing field is composed of phonons or magnons. Here we use the prototypical charge-transfer insulator NiO to demonstrate that 1.5 eV sub-gap optical excitation leads to a renormalised NiO band-gap…
Ferroelectric and ferromagnetic materials possess spontaneous electric and magnetic order, respectively, which can be switched by the corresponding applied electric and magnetic fields. Multiferroics combine these properties in a single material, providing an avenue for controlling electric polarization with a magnetic field and magnetism with an electric field. These materials have been intensively studied in recent years, both for their fundamental scientific interest as well as their potential applications in a broad range of magnetoelectric devices [1, 2, 3, 4]. However, the microscopic or…
Using a time-resolved optically-pumped scanning optical microscopy technique we demonstrate the laser-driven excitation and propagation of spin waves in a 20-nm film of a ferromagnetic metallic alloy Galfenol epitaxially grown on a GaAs substrate. In contrast to previous all-optical studies of spin waves we employ laser-induced thermal changes of magnetocrystalline anisotropy as an excitation mechanism. A tightly focused 70-fs laser pulse excites packets of magnetostatic surface waves with a $e^{-1}$ propagation length of 3.4 $μ$m, which is comparable with that of permalloy. As a result, laser…
Strongly correlated Kagome magnets are promising candidates for achieving controllable topological devices owing to the rich interplay between inherent Dirac fermions and correlation-driven magnetism. Here we report tunable local magnetism and its intriguing control of topological electronic response near room temperature in the Kagome magnet Fe3Sn2 using small angle neutron scattering, muon spin rotation, and magnetoresistivity measurement techniques. The average bulk spin direction and magnetic domain texture can be tuned effectively by small magnetic fields. Magnetoresistivity, in response,…
Measuring how the magnetic correlations throughout the Brillouin zone evolve in a Mott insulator as charges are introduced dramatically improved our understanding of the pseudogap, non-Fermi liquids and high $T_C$ superconductivity. Recently, photoexcitation has been used to induce similarly exotic states transiently. However, understanding how these states emerge has been limited because of a lack of available probes of magnetic correlations in the time domain, which hinders further investigation of how light can be used to control the properties of solids. Here we implement magnetic resonant…
