Ultrafast characterization and control of many-body interactions and elementary excitations are critical to understanding and manipulating emergent phenomena in strongly correlated systems. In particular, spin interaction plays an important role in unconventional superconductivity, but efficient tools for probing spin dynamics especially out of equilibrium, are still lacking. To address this question, we develop a theory for nonresonant time-resolved Raman scattering, which can be a generic and powerful tool for nonequilibrium studies. We also use exact diagonalization to simulate the pump-probe dynamics of correlated electrons in the square-lattice single-band Hubbard model. Different ultrafast processes are shown to exist in the time-resolved Raman spectra and dominate under different pump conditions. For high-frequency and off-resonance pumps, we show that the Floquet theory works well in capturing the softening of bimagnon excitation. By comparing the Stokes/anti-Stokes spectra, we also show that effective heating dominates at small pump fluences, while a coherent many-body effect starts to take over at larger pump amplitudes and frequencies on resonance to the Mott gap. Time-resolved Raman scattering thereby provides the platform to explore different ultrafast processes and design material properties out of equilibrium.
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 …
Measurement and control of magnetic order and correlations in real time is a rapidly developing scientific area relevant for magnetic memory and spintronics [1,15]. In these experiments an ultra-short laser pulse (pump) is first absorbed by excitations carrying electric dipole moment. These then give their energy to the magnetic subsystem monitored by a time-resolved probe. A lot of progress has been made in investigations of ferromagnets but antiferromagnets are more challenging. Here we introduce time-resolved two-magnon Raman scattering as a novel real time probe of magnetic correlations es…
A grand challenge underlies the entire field of topology-enabled quantum logic and information science: how to establish topological control principles driven by quantum coherence and understand the time-dependence of such periodic driving? Here we demonstrate a THz pulse-induced phase transition in Dirac materials that is periodically driven by vibrational coherence due to excitation of the lowest Raman-active mode. Above a critical field threshold, there emerges a long-lived metastable phase with unique Raman coherent phonon-assisted switching dynamics, absent for optical pumping. The switch…
One of the goals of pump/probe spectroscopies is to determine how electrons relax after they have been driven out of equilibrium. It is challenging to determine how close electrons are to a thermal state solely by fitting their distribution to a Fermi-Dirac distribution. Instead, we propose that one compare the effective temperatures of both fermions and collective bosonic modes (derived from the fermions) to determine the distance from a thermal state. Measurements of effective fermionic and bosonic temperatures can be achieved directly via photoemission and nonresonant Raman scattering. Thei…
Strongly correlated systems exhibit intriguing properties caused by intertwined microscopic in- teractions that are hard to disentangle in equilibrium. Employing non-equilibrium time-resolved photoemission spectroscopy on the quasi-two-dimensional transition-metal dichalcogenide 1T-TaS$_2$, we identify a spectroscopic signature of double occupied sites (doublons) that are reflects fundamental Mott physics. Doublon-hole recombination is estimated to occur on time scales of one electronic hopping cycle $\hbar/J\approx$ 14 fs. Despite strong electron-phonon coupling the dynamics can be explained …
We investigate the hot carrier dynamics of ZrTe$_5$ by ultrafast time-resolved optical reflectivity. Our results reveal a phonon-mediated across-gap recombination, consistent with its temperature-dependent gap nature as observed previously by photoemission. In addition, two distinct relaxations with a kink feature right after initial photoexcitation are well resolved, suggesting the complexity of electron thermalization process. Our findings indicate that correlated many-body effects play important role for the transient dynamics of ZrTe$_5$.
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…
The correlated polar semimetal Ca$_3$Ru$_2$O$_7$ exhibits a rich phase diagram including two magnetic transitions ($T_N$=56 K and $T_C$=48 K) with the appearance of an insulating-like pseudogap (at $T_C$). In addition, there is a crossover back to metallic behavior at $T^*$=30 K, the origin of which is still under debate. We utilized ultrafast optical pump optical probe spectroscopy to investigate quasiparticle dynamics as a function of temperature in this enigmatic quantum material. We identify two dynamical processes, both of which are influenced by the onset of the pseudogap. This includes …
We analyze the thermalization of a photoexcited charge carrier coupled to a single branch of quantum phonons within the Holstein model. To this end, we calculate the far-from-equilibrium time evolution of a pure many-body state and compare it with predictions of the thermal Gibbs ensemble. We show that at strong enough carrier excitation, the nonequilibrium system evolves towards a thermal steady state. Our analysis is based on two classes of observables. First, the occupations of fermionic momenta, which are the eigenvalues of the one-particle density matrix, match in the steady state the val…
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…
Ultrafast optical pump-probe spectroscopy is used to track carrier dynamics in the large magnetoresistance material WTe$_{2}$. Our experiments reveal a fast relaxation process occurring on a sub-picosecond time scale that is caused by electron-phonon thermalization, allowing us to extract the electron-phonon coupling constant. An additional slower relaxation process, occurring on a time scale of $\sim$5-15 picoseconds, is attributed to phonon-assisted electron-hole recombination. As the temperature decreases from 300 K, the timescale governing this process increases due to the reduction of the…
Momentum-Selective Electron and Spin Dynamics under Ultrafast Photoexcitation
CPHT, CNRS, École polytechnique, Institut Polytechnique de Paris（法国高等理工学院）；Institut für Theoretische Physik, Universität Hamburg（汉堡大学理论物理研究所）；European X-Ray Free-Electron Laser Facility（欧洲X射线自由电子激光设施）；The Hamburg Centre for Ultrafast Imaging（汉堡超快成像中心）；Collège de France（法兰西学院）
The possibility of investigating the dynamics of solids on timescales faster than the thermalization of the internal degrees of freedom has disclosed novel non-equilibrium phenomena that have no counterpart at equilibrium. Transition metal oxides (TMOs) provide an interesting playground in which the correlations among the charges in the metal $d$-orbitals give rise to a wealth of intriguing electronic and thermodynamic properties involving the spin, charge, lattice and orbital orders. Furthermore, the physical properties of TMOs can be engineered at the atomic level, thus providing the platfor…
We investigate the excited state electronic structure of the model phase transition system In/Si(111) using femtosecond time- and angle-resolved photoemission spectroscopy (trARPES) with an XUV laser source at 500 kHz . Excited state band mapping is used to characterize the normally unoccupied electronic structure above the Fermi level in both structural phases of indium nanowires on Si(111): the metallic (4x1) and the gapped (8x2) phases. The extracted band positions are compared with the band structure calculated using density functional theory (DFT) within both the LDA and GW approximations…
