Using a combination of first-principles and magnetization-dynamics calculations, we study the effect of the intense optical excitation of phonons on the magnetic behavior in insulating magnetic materials. Taking the prototypical magnetoelectric \CrO\ as our model system, we show that excitation of a polar mode at 17 THz causes a pronounced modification of the magnetic exchange interactions through a change in the average Cr-Cr distance. In particular, the quasi-static deformation induced by nonlinear phononic coupling yields a structure with a modified magnetic state, which persists for the duration of the phonon excitation. In addition, our time-dependent magnetization dynamics computations show that systematic modulation of the magnetic exchange interaction by the phonon excitation modifies the magnetization dynamics. This temporal modulation of the magnetic exchange interaction strengths using phonons provides a new route to creating non-equilibrium magnetic states and suggests new avenues for fast manipulation of spin arrangements and dynamics.
PSI Center for Scientific Computing, Theory and Data（瑞士保罗谢勒研究所科学计算、理论与数据中心）；Institute of Physics, Ecole Polytechnique Fédérale de Lausanne (EPFL)（洛桑联邦理工学院物理系）；Condensed Matter Theory, Department of Physics, TU Dortmund University（多特蒙德大学物理系凝聚态理论）
We study the non-equilibrium structural dynamics of the incommensurate and nearly-commensurate charge-density wave phases in 1T-TaS$_2$. Employing ultrafast low-energy electron diffraction (ULEED) with 1 ps temporal resolution, we investigate the ultrafast quench and recovery of the CDW-coupled periodic lattice distortion. Sequential structural relaxation processes are observed by tracking the intensities of main lattice as well as satellite diffraction peaks as well as the diffuse scattering background. Comparing distinct groups of diffraction peaks, we disentangle the ultrafast quench of the…
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…
In solids, the response of the lattice to photo-excitation is often described by the inertial evolution on an impulsively modified potential energy surface which leads to coherent motion. However, it remains unknown if vibrational coherence is sustained through a phase transition, during which coupling between modes can be strong and may lead to rapid loss of coherence. Here we use coherent phonon spectroscopy to track lattice coherence in the structural phase transition of V$_2$O$_3$. In both the low and high symmetry phases unique coherent phonon modes are generated at low fluence. However, …
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…
Ultrafast Stiffening of the Lattice Potential and Metastable State Formation in 1$T$-TiSe$_2$
Central South University（中南大学）；Hunan University of Science and Technology（湖南科技大学）；Beijing Academy of Quantum Information Sciences（北京量子信息科学研究院）；Uppsala University（乌普萨拉大学）
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 …
Ultrafast optical pump - optical probe and optical pump - terahertz probe spectroscopy were performed on vanadium dioxide (VO2) and vanadium sesquioxide (V2O3) thin films over a wide temperature range. A comparison of the experimental data from these two different techniques and two different vanadium oxides, in particular a comparison of the electronic oscillations generated by the photoinduced longitudinal acoustic modulation, reveals the strong electron-phonon coupling that exists in the metallic state of both materials. The low energy Drude response of V2O3 appears more susceptible than VO…
Finite lattice models are a prototype for strongly correlated quantum systems and capture essential properties of condensed matter systems. With the dramatic progress in ultracold atoms in optical lattices, finite fermionic Hubbard systems have become directly accessible in experiments, including their ultrafast dynamics far from equilibrium. Here, we present a theoretical approach that is able to treat these dynamics in any dimension and fully includes inhomogeneity effects. The method consists in stochastic sampling of mean-field trajectories and is found to be more accurate and efficient th…
We study the relaxation mechanism of a highly excited carrier propagating in the antiferromagnetic background modeled by the $t$-$J$ Hamiltonian on a square lattice. We show that the relaxation consists of two distinct stages. The initial ultrafast stage with the relaxation time $τ\sim (\hbar/t_0)(J/t_0)^{-2/3}$ (where $t_0$ is the hopping integral and $J$ is the exchange interaction) is based on generation of string states in the close proximity of the carrier. This unusual scaling of $τ$ is obtained by means of comparison of numerical results with a simplified $t$-$J_z$ model on a Bethe latt…
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 use femtosecond electron diffraction to study ultrafast lattice dynamics in the highly correlated antiferromagnetic (AF) semiconductor NiO. Using the scattering vector (Q) dependence of Bragg diffraction, we introduce a Q-resolved effective lattice temperature, and identify a nonthermal lattice state with preferential displacement of O compared to Ni ions, which occurs within ~0.3 ps and persists for 25 ps. We associate this with transient changes to the AF exchange striction-induced lattice distortion, supported by the observation of a transient Q-asymmetry of Friedel pairs. Our observatio…
The emergent properties of quantum materials, such as symmetry-broken phases and associated spectral gaps, can be effectively manipulated by ultrashort photon pulses. Impulsive optical excitation generally results in a complex non-equilibrium electron and lattice dynamics that involves multiple processes on distinct timescales, and a common conception is that for times shorter than about 100 fs the gap in the electronic spectrum is not seriously affected by lattice vibrations. Here, we directly monitor the photo-induced collapse of the spectral gap in a canonical charge-density-wave material, …
Orbital-lattice coupling and polaronic dressing of electronic states in Pr$_{0.5}$Ca$_{1.5}$MnO$_4$ revealed by ultrafast broadband spectroscopy
ICFO - Institut de Ciències Fotòniques, The Barcelona Institute of Science and Technology（巴塞罗那科学技术学院光子科学研究所（ICFO））；Aarhus University（奥胡斯大学）；ALBA Synchrotron Light Source（ALBA同步辐射光源）；Univ Rennes（雷恩大学）；CNRS（法国国家科学研究中心）；IMDEA Nanoscience（IMDEA纳米科学研究所）
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…
The study of photoexcited strongly correlated materials is attracting growing interest since their rich phase diagram often translates into an equally rich out-of-equilibrium behavior, including non-thermal phases and photoinduced phase transitions. With femtosecond optical pulses, electronic and lattice degrees of freedom can be transiently decoupled, giving the opportunity of stabilizing new states of matter inaccessible by quasi-adiabatic pathways. Here we present a study of the ultrafast non-equilibrium evolution of the prototype Mott-Hubbard material V2O3, which presents a transient non-t…
Femtosecond time-resolved core-level photoemission spectroscopy with a free-electron laser is used to measure the atomic-site specific charge-order dynamics in the charge-density-wave/Mott insulator 1T-TaS2. After strong photoexcitation, a prompt loss of charge order and subsequent fast equilibration dynamics of the electron-lattice system are observed. On the time scale of electron-phonon thermalization, about 1 ps, the system is driven across a phase transition from a long-range charge ordered state to a quasi-equilibrium state with domain-like short-range charge and lattice order. The exper…
The electronic nematic phase is an unconventional state of matter that spontaneously breaks the rotational symmetry of electrons. In iron-pnictides/chalcogenides and cuprates, the nematic ordering and fluctuations have been suggested to have as-yet-unconfirmed roles in superconductivity. However, most studies have been conducted in thermal equilibrium, where the dynamical property and excitation can be masked by the coupling with the lattice. Here we use femtosecond optical pulse to perturb the electronic nematic order in FeSe. Through time-, energy-, momentum- and orbital-resolved photo-emiss…
We report on ultrafast optical experiments in which femtosecond mid-infrared radiation is used to excite the lattice of complex oxide heterostructures. By tuning the excitation energy to a vibrational mode of the substrate, a long-lived five-order-of-magnitude increase of the electrical conductivity of NdNiO3 epitaxial thin films is observed as a structural distortion propagates across the interface. Vibrational excitation, extended here to a wide class of heterostructures and interfaces, may be conducive to new strategies for electronic phase control at THz repetition rates.
The electronic and structural properties of a material are strongly determined by its symmetry. Changing the symmetry via a photoinduced phase transition offers new ways to manipulate material properties on ultrafast timescales. However, in order to identify when and how fast these phase transitions occur, methods that can probe the symmetry change in the time domain are required. We show that a time-dependent change in the coherent phonon spectrum can probe a change in symmetry of the lattice potential, thus providing an all-optical probe of structural transitions. We examine the photoinduced…
Femtosecond time-resolved x-ray diffraction is employed to study the dynamics of the periodic lattice distortion (PLD) associated with the charge-density-wave (CDW) in K0.3MoO3. Using a multi-pulse scheme we show the ability to extend the lifetime of coherent oscillations of the PLD about the undistorted structure through re-excitation of the electronic states. This suggests that it is possible to enter a regime where the symmetry of the potential energy landscape corresponds to the high symmetry phase but the scattering pathways that lead to the damping of coherent dynamics are still controll…
We report on a transient optical reflectivity study of the charge density wave (CDW) in CuxTiSe2 single crystals. Our measurements reveal that the system undergoes a quantum phase transition at x=0.04 from a strong commensurate CDW (x<0.04) to a soft incommensurate CDW (x>0.04). We find that the cooperative driving mechanisms for the commensurate CDW, the excitonic insulator mechanism and the soft L$_1$$^-$ phonon mode, decouple at x=0.04 with the observed fluctuations in the folded Se-4p band dominating the transition. We also demonstrate a loss of coherence in the A$_{1g}$ phonon with increa…
Experimental observations of the ultrafast (less than 50 fs) demagnetization of Ni have so far defied theoretical explanations particularly since its spin-flipping time is much less than that resulting from spin-orbit and electron-lattice interactions. Through the application of an approach that benefits from spin-flip time-dependent density-functional theory and dynamical mean-field theory, we show that proper inclusion of electron correlations and memory (time-dependence of electron-electron interaction) effects leads to demagnetization at the femtosecond scale, in good agreement with experi…
Ultrafast recovery dynamics of dimer stripes in IrTe2
University of Fribourg（弗里堡大学）；Fribourg Centre for Nanomaterials（弗里堡纳米材料中心）；Université de Lorraine（洛林大学）；CNRS（法国国家科学研究中心）；IJL（约尔研究所）；Deutsches Elektronen-Synchrotron DESY（德国电子同步辐射研究所）；European XFEL（欧洲XFEL）；Institut für Experimentelle und Angewandte Physik, Christian-Albrechts-Universität zu Kiel（基尔大学实验与应用物理研究所）；Max Planck Institute for Chemical Physics of Solids（马克斯·普朗克固体化学物理研究所）；Ruprecht Haensel Laboratory（鲁普雷希特·亨塞尔实验室）；Department of Quantum Matter Physics, University of Geneva（日内瓦大学量子物质物理系）
We apply ultrafast X-ray diffraction with femtosecond temporal resolution to monitor the lattice dynamics in a thin film of multiferroic BiFeO$_3$ after above-bandgap photoexcitation. The sound-velocity limited evolution of the observed lattice strains indicates a quasi-instantaneous photoinduced stress which decays on a nanosecond time scale. This stress exhibits an inhomogeneous spatial profile evidenced by the broadening of the Bragg peak. These new data require substantial modification of existing models of photogenerated stresses in BiFeO$_3$: the relevant excited charge carriers must rem…
The interplay among charge, spin and lattice degrees of freedom in solids gives rise to intriguing macroscopic quantum phenomena such as colossal magnetoresistance, multiferroicity and high-temperature superconductivity. Strong coupling or competition between various orders in these systems presents the key to manipulate their functional properties by means of external perturbations such as electric and magnetic fields or pressure. Ultrashort and intense optical pulses have emerged as an interesting tool to investigate elementary dynamics and control material properties by melting an existing …
To date, two types of coupling between electromagnetic radiation and a crystal lattice have been identified experimentally. One is direct, for infrared (IR)-active vibrations that carry an electric dipole. The second is indirect, it occurs through intermediate excitation of the electronic system via electron-phonon coupling, as in stimulated Raman scattering. Nearly 40 years ago, proposals were made of a third path, referred to as ionic Raman scattering (IRS). It was posited that excitation of an IR-active phonon could serve as the intermediate state for a Raman scattering process relying on l…
Ultrafast light pulses can modify the electronic properties of quantum materials by perturbing the underlying, intertwined degrees of freedom. In particular, iron-based superconductors exhibit a strong coupling among electronic nematic fluctuations, spins, and the lattice, serving as a playground for ultrafast manipulation. Here we use time-resolved x-ray scattering to measure the lattice dynamics of photo-excited BaFe2As2. Upon optical excitation, no signature of an ultrafast change of the crystal symmetry is observed, but the lattice oscillates rapidly in time due to the coherent excitation …
Light enables ultrafast, direct and nonthermal control of the exchange and Dzyaloshinskii-Moriya interactions. We consider two-dimensional honeycomb lattices described by the Kane-Mele-Hubbard model at half filling and in the strongly correlated limit, i.e., the Mott insulator phase of a canted antiferromagnet. Based on Floquet theory, we demonstrate that by changing the amplitude and frequency of polarized laser pulses, one can tune the amplitudes and signs of and even the ratio between the exchange and Dzyaloshinskii-Moriya spin interactions. Furthermore, the renormalizations of the spin int…
We report about the existence of magneto-acoustic pulses propagating in a 200-nm-thick ferromagnetic nickel film excited with 120 fs laser pulses. They result from the coupling between the magnetization of the ferromagnetic film and the longitudinal acoustic waves associated to the propagation of the lattice deformation induced by the femtosecond laser pulses. The magneto-acoustic pulses are detected from both the front and back sides of the film, using the time-resolved magneto-optical Kerr technique, measuring both the time dependent rotation and ellipticity. We show that the propagating aco…
VO$_{2}$ is a model material system which exhibits a metal to insulator transition at 67$^\circ$C. This holds potential for future ultrafast switching in memory devices, but typically requires a purely electronic process to avoid the slow lattice response. The role of lattice vibrations is thus important, but it is not well understood and it has been a long-standing source of controversy. We use a combination of ultrafast spectroscopy and ab initio quantum calculations to unveil the mechanism responsible for the transition. We identify an atypical Peierls vibrational mode which acts as a trigg…
Exciting atomic oscillations with light is a powerful technique to control the electronic properties of materials, leading to remarkable phenomena such as light-induced superconductivity and ultrafast insulator to metal transitions. Here we show that light-driven lattice vibrations can be utilised to encode efficiently spin information in a magnetic medium. Intense mid-infrared electric field pulses, tuned to resonance with a vibrational normal mode of antiferromagnetic DyFeO3, drive the emergence of long-living weak ferromagnetic order. Light-driven phonon displacements promptly lower the ene…
The transition between different states in manganites can be driven by various external stimuli. Controlling these transitions with light opens the possibility to investigate the microscopic path through which they evolve. We performed femtosecond (fs) transmission electron microscopy on a bi-layered manganite to study its response to ultrafast photoexcitation. We show that a photoinduced temperature jump launches a pressure wave that provokes coherent oscillations of the lattice parameters, detected via ultrafast electron diffraction. Their impact on the electronic structure are monitored via…
Hidden phonon-assisted charge density wave transition in BaFe2Al9 revealed by ultrafast optical spectroscopy
Beijing Normal University（北京师范大学）；Institute of Physics, Chinese Academy of Sciences（中国科学院物理研究所）；University of Chinese Academy of Sciences（中国科学院大学）；Institute of Metal Research, Chinese Academy of Sciences（中国科学院金属研究所）
Strongly correlated systems of fermions have an interesting phase diagram arising from the Hubbard gap. Excitation across the gap leads to the formation of doubly occupied lattice sites (doublons). This state offers interesting electronic and optical properties. Moreover, when the system is driven out of equilibrium interesting collective dynamics may arise that are related to the spatial propagation of doublons. Here, a novel mechanism that was recently proposed by us [Balzer \textit{et al.}, submitted for publication] is verified by exact diagonalization and nonequilibrium Green functions (N…
Fast and dynamical control of quantum phases is highly desired in the application of quantum phenomena in devices. On the experimental side, ultrafast laser pulses provide an ideal platform to induce femtosecond dynamics in a variety of materials. Here, we show that a laser pulse driven heavy fermion system, can be tuned to dynamically evolve into a phase, which is not present in equilibrium. Using the state-of-the-art time-dependent variational Monte Carlo method, we perform numerical simulations of realistic laser pulses applied to the Kondo Lattice model. By tracking spin and charge degrees…
We study the relaxation dynamics and intersystem-crossing to the metastable state in laser-pumped tetra and hexa-coordinated nickel porphyrins. We use a ligand-field model which takes into account the crystal field created by the porphyrin ring and axial ligands. By accounting for the energy redistribution of the lattice vibrations of the metal-ligand stretch mode we get an irreversible decay within the order of the hundreds of femtoseconds timescale. We show how non-equilibrium time-dependent x-ray absorption atthe Ni K-edge measurements can elucidate the nature of the intermediate states inv…
Disentangling the primary order parameter from secondary order parameters in phase transitions is critical to the interpretation of the transition mechanisms in strongly correlated systems and quantum materials. Here we present a study of structural phase transition pathways in superionic Cu2S nanocrystals that exhibit intriguing properties. Utilizing ultrafast electron diffraction techniques sensitive in both momentum-space and the time-domain, we distinguish the dynamics of crystal symmetry breaking and lattice expansion in this system. We are able to follow the transient states along the tr…
We review recent progress in utilizing ultrafast light-matter interaction to control the macroscopic properties of quantum materials. Particular emphasis is placed on photoinduced phenomena that do not result from ultrafast heating effects but rather emerge from microscopic processes that are inherently nonthermal in nature. Many of these processes can be described as transient modifications to the free-energy landscape resulting from the redistribution of quasiparticle populations, the dynamical modification of coupling strengths and the resonant driving of the crystal lattice. Other pathways…
