The time resolved Magnetooptical Kerr effect in the substrate-strain-induced insulating ferromagnetic phase in (Pr$_{0.6}$Ca$_{0.4}$)MnO$_3$ thin films on two different substrates was measured in a magnetic field up to 1.1T. The photoinduced Kerr rotation and ellipticity show remarkably different magnetic-field dependence. From the comparison of the magnetic field dependencies of the photoinduced and static Kerr rotation and ellipticity we conclude that a transient ferromagnetic metallic phase, embedded within the insulating ferromagnetic phase, is created upon the photoexcitation at low temperatures. A comparison of temporal dependence of the photoinduced Kerr signals with the photoinduced reflectivity indicates the change of the fractions of the phases takes place on a timescale of ten picoseconds independent of the substrate.
Ultrafast dynamics across the photoinduced three-dimensional Peierls-like insulator-metal (IM) transition in CuIr$_{2}$S$_{4}$ was investigated by means of the all-optical ultrafast multi-pulse time-resolved spectroscopy. The structural coherence of the low-$T$ broken symmetry state is strongly suppressed on a sub-picosecond timescale above a threshold excitation fluence of $F_{\mathrm{c}}\approx3$ mJ/cm$^{2}$ (at 1.55-eV photon energy) resulting in a structurally inhomogeneous transient state which persists for several-tens of picoseconds before reverting to the original low-$T$ state. The el…
In this work we have studied the effect of light and electric field on the electrical properties of La0.7Sr0.3MnO3 (LSMO) film at 300 K. Taking advantage of it's charge, spin, orbital and lattice degrees of freedom, we have successfully shown that light and electric field together can be used to tune the resistance states of the manganite system. Using applied gate voltage (Vg) and light we were able to obtain a change in resistance of about +/-7.5%. Furthermore, incorporating an ultra thin interfacial LaTiO3 (LTO) layer provides valuable insight on the origin of the photoinduced effect. The o…
Observation of photoinduced phase transition in phase-separated Pr$_{0.55}$(Ca$_{1-y}$Sr$_{y}$)$_{0.45}$MnO$_3$ thin films via x-ray photoemission spectroscopy
The spinel-structure CuIr$_{2}$S$_{4}$ compound displays a rather unusual orbitally-driven three-dimensional Peierls-like insulator-metal transition. The low-T symmetry-broken insulating state is especially interesting due to the existence of a metastable irradiation-induced disordered weakly conducting state. Here we study intense femtosecond optical pulse irradiation effects by means of the all-optical ultrafast multi-pulse time-resolved spectroscopy. We show that the structural coherence of the low-T broken symmetry state is strongly suppressed on a sub-picosecond timescale above a threshol…
We studied the ultrafast third-order optical nonlinearity in a single crystal of multiferroic bismuth ferrite (BiFeO3) in the near-infrared range of 0.5-1.0 eV, where the material is fundamentally transparent,at room temperature. With pump pulses at 1.55 eV, which is off-resonant to the strong inter-band charge transfer (CT) transition, we observed instantaneous transient absorption with pencil-like temporal profile originating from the two-photon CT transition from the oxygen 2p to the iron 3p levels. In contrast, under pumping with 3.10-eV photons, the pencil-like absorption change was not o…
We report on systematic investigation of hot carrier dynamics in Ti4O7 by ultrafast time-resolved optical reflectivity. We find the transient indication for its two-step insulator-metal (I-M) transition, in which two phase transitions occur from long-range order bipolaron low-temperature insulating (LI) phase to disordered bipolaron high-temperature insulating (HI) phase at Tc1 and to free carrier metallic (M) phase at Tc2. Our results reveal that photoexcitation can effectively lower down both Tc1 and Tc2 with pump fluence increasing, allowing a light-control of I-M transition. We address a p…
Manipulating crystal structure and the corresponding electronic properties in quantum materials provides opportunities for the exploration of exotic physics and practical applications. Here, by ultrafast electron diffraction, structure factor calculation and TDDFT-MD simulations, we report the photoinduced concurrent intralayer and interlayer structural transitions in the Td and 1T' phase of XTe2 (X=Mo, W). Concomitant with the interlayer structural transition by shear displacement, the ultrafast suppression of the intralayer Peierls distortion within 0.3 ps is demonstrated and attributed to M…
Photoinduced hidden phases are often observed in materials with intertwined orders. Understanding the formation of these non-thermal phases is challenging and requires a resolution of the cooperative interplay between different orders on the ultrashort timescale. In this work, we demonstrate that non-equilibrium photo-excitations can induce a state with spin-orbital orders entirely different from the equilibrium state in the three-quarter-filled two-band Hubbard model. We identify a general mechanism governing the transition to the hidden state, which relies on a non-thermal partial melting of…
Photo-induced stabilization and enhancement of the ferroelectric polarization in Ba$_{0.1}$Sr$_{0.9}$TiO$_{3}$/La$_{0.7}$Ca(Sr)$_{0.3}$MnO$_{3}$ thin film heterostructures
Novel phases of matter with unique properties that emerge from quantum and topological protection present an important thrust of modern research. Of particular interest is to engineer these phases on demand using ultrafast external stimuli, such as photoexcitation, which offers prospects of their integration into future devices compatible with optical communication and information technology. Here, we use MeV Ultrafast Electron Diffraction (UED) to show how a transient three-dimensional (3D) Dirac semimetal state can be induced by a femtosecond laser pulse in a topological insulator ZrTe$_5$. …
A major challenge in condensed matter physics is active control of quantum phases. Dynamic control with pulsed electromagnetic fields can overcome energetic barriers enabling access to transient or metastable states that are not thermally accessible. Here we demonstrate strain-engineered tuning of La2/3Ca1/3MnO3 into an emergent charge-ordered insulating phase with extreme photo-susceptibility where even a single optical pulse can initiate a transition to a long-lived metastable hidden metallic phase. Comprehensive single-shot pulsed excitation measurements demonstrate that the transition is c…
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）
We study periodically driven pure Kitaev model and ferromagnetic phase of the Kitaev-Heisenberg model on the honeycomb lattice by off-resonant linearly and circularly-polarized lights at zero magnetic field. Using a combination of linear spin wave and Floquet theories, we show that the effective time-independent Hamiltonians in the off-resonant regime map onto the corresponding anisotropic static spin model, plus a tunable photoinduced magnetic field along the $[111]$ direction, which precipitates Floquet topological magnons and chiral magnon edge modes. They are tunable by the light amplitude…
We use femtosecond x-ray diffraction to study the structural response of charge and orbitally ordered Pr$_{1-x}$Ca$_x$MnO$_3$ thin films across a phase transition induced by 800 nm laser pulses. By investigating the dynamics of both superlattice reflections and regular Bragg peaks, we disentangle the different structural contributions and analyze their relevant time-scales. The dynamics of the structural and charge order response are qualitatively different when excited above and below a critical fluence $f_c$. For excitations below $f_c$ the charge order and the superlattice is only partially…
The relationship between the magnetic interaction and photoinduced dynamics in antiferromagnetic perovskites is investigated in this study. In La${}_{1/3}$Sr${}_{2/3}$FeO${}_{3}$ thin films, commensurate spin ordering is accompanied by charge disproportionation, whereas SrFeO${}_{3}$ thin films show incommensurate helical antiferromagnetic spin ordering due to increased ferromagnetic coupling compared to La${}_{1/3}$Sr${}_{2/3}$FeO${}_{3}$. To understand the photoinduced spin dynamics in these materials, we investigate the spin ordering through time-resolved resonant soft X-ray scattering. In …
We combine ultrafast electron diffraction and time-resolved terahertz spectroscopy measurements to unravel the connection between structure and electronic transport properties during the photoinduced insulator-metal transitions in vanadium dioxide. We determine the structure of the metastable monoclinic metal phase, which exhibits anti-ferroelectric charge order arising from a thermally activated, orbital-selective phase transition in the electron system. The relative contribution of this photoinduced monoclinic metal (which has no equilibrium analog) and the photoinduced rutile metal (known f…
We use femtosecond resonant soft x-ray scattering to measure the ultrafast optical melting of charge-order correlations in La$_{1.875}$Ba$_{0.125}$CuO$_4$. By analyzing both the energy-resolved and energy-integrated order parameter dynamics, we find evidence of a short-lived nonequilibrium state, whose features are compatible with a sliding charge density wave coherently set in motion by the pump. This transient state exhibits shifts in both the quasielastic line energy and its wave vector, as expected from a classical Doppler effect. The wave vector change is indeed found to directly follow t…
The charge carrier dynamics of doped electronic correlated systems on ladders and chains, subject to ultrafast photoirradiation, is investigated using the time-dependent Lanczos method. The time-resolved optical conductivity and the temporal profiles of other relevant quantities, including the doublon number, the kinetic energy, and the interaction energy, are calculated. Two competitive factors that can influence the transient charge carrier dynamics are identified as the thermal effect and the charge effect. We demonstrate that the analysis of their interplay can provide an intuitive way to …
Clustering-Enhanced Time- and Angle-Resolved Photoemission Study of LaTe$_3$: Absence of a Photoinduced Secondary CDW in the Electronic Structure
Aarhus University（奥胡斯大学）；CNR, Consiglio Nazionale delle Ricerche, Istituto officina dei materiali（意大利国家研究委员会材料研究所）；Central Laser Facility, STFC Rutherford Appleton Laboratory（STFC鲁瑟福阿普尔顿实验室中央激光设施）；SUPA, School of Physics and Astronomy, University of St Andrews（圣安德鲁斯大学物理与天文学学院）；Stanford University（斯坦福大学）；Diamond Light Source Ltd（钻石光源有限公司）；Princeton University（普林斯顿大学）；Department of Physics, Indian Institute of Technology Guwahati（印度理工学院古瓦哈提分校物理系）
Spontaneous C4-symmetry breaking phases are ubiquitous in layered quantum materials, and often compete with other phases such as superconductivity. Preferential suppression of the symmetry broken phases by light has been used to explain non-equilibrium light induced superconductivity, metallicity, and the creation of metastable states. Key to understanding how these phases emerge is understanding how C4 symmetry is restored. A leading approach is based on time-dependent Ginzburg-Landau theory, which explains the coherence response seen in many systems. However, we show that, for the case of th…
Optically-induced phase transitions of the manganite $\rm Pr_{1/3}Ca_{2/3}MnO_3$ have been simulated using a model Hamiltonian, that captures the dynamics of strongly correlated charge, orbital, lattice, and spin degrees of freedom. Its parameters have been extracted from first-principles calculations. Beyond a critical intensity of a femto-second light pulse, the material undergoes ultra-fast and non-thermal magnetic phase transition from a non-collinear to collinear antiferromagnetic phases. The light-pulse excites selectively either a spin-nematic or a ferroelectric phase depending on the l…
Evidence of a photoinduced non-thermal superconducting-to-normal-state phase transition in overdoped Bi$_{2}$Sr$_{2}$Ca$_{0.92}$Y$_{0.08}$Cu$_{2}$O$_{8+δ}$
在这里，我们报告了广泛的超快时间分辨反射率实验过掺杂的Bi $_{2}$ Sr $_{2}$ Ca $_{1-x}$ Y $_x$ Cu $_{2}$ O $_{8+δ}$单晶（T $_C$ =78 K），旨在澄清的性质的超导到正常状态的光致相变。实验数据表明，缺乏的准粒子衰变时间发散所需的能量密度诱导这种相变，在T $_C$观察到的热驱动的相变，并在最近报道的光致电荷密度波和自旋密度波到金属相变的差异。我们的实验结果证实了超导态到正常态光致相变的非热特性。数据已被分析，使用一个特设开发的时间依赖的Rothwarf-Taylor模型，打开这个非平衡相变的顺序上的问题。
We investigate the microscopic dynamics at the initial stage of photoinduced phase transitions in tetrathiafulvalene-$p$-chloranil by exact diagonalization. We first show that the one-dimensional extended Peierls-Hubbard model exhibits a neutral phase with small ionicity and negligible dimerization and an ionic phase with moderate ionicity and dimerization. Aside from these phases, we find a doubly ionized phase with strong dimerization that we call the "dipole" phase. These ground-state phases are characterized by various order parameters and the Zak phase, which is relevant to electronic pol…
The insulator-to-metal transition (IMT) of the simple binary compound of vanadium dioxide VO$_2$ at $\sim 340$ K has been puzzling since its discovery more than five decades ago. A wide variety of photon and electron probes have been applied in search of a satisfactory microscopic mechanistic explanation. However, many of the conclusions drawn have implicitly assumed a {\em homogeneous} material response. Here, we reveal inherently {\em inhomogeneous} behavior in the study of the dynamics of individual VO$_2$ micro-crystals using a combination of femtosecond pump-probe microscopy with nano-IR …
We investigate the nonequilibrium dynamics of the spinless Haldane model with nearest-neighbor interactions on the honeycomb lattice by employing an unbiased numerical method. In this system, a first-order transition from the Chern insulator (CI) at weak coupling to the charge-density-wave (CDW) phase at strong coupling can be characterized by a level crossing of the lowest energy levels. Here we show that adiabatically following the eigenstates across this level crossing, their Chern numbers are preserved, leading to the identification of a topologically-nontrivial low-energy excited state in…
Photoinduced non-thermal phase transitions are new paradigms of exotic non-equilibrium physics of strongly correlated materials. An ultrashort optical pulse can drive the system to a new order through complex microscopic interactions that do not occur in the equilibrium state. Ultrafast spectroscopies are unique tools to reveal the underlying mechanisms of such transitions which lead to transient phases of matter. Yet, their individual specificities often do not provide an exhaustive picture of the physical problem. One effective solution to enhance their performance is the integration of diff…
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 …
Nonlinear phononics holds the promise for controlling properties of quantum materials on the ultrashort timescale. Using nonequilibrium dynamical mean-field theory, we solve a model for the description of organic solids, where correlated electrons couple nonlinearly to a quantum phonon mode. Unlike previous works, we exactly diagonalize the local phonon mode within the noncrossing approximation to include the full phononic fluctuations. By exciting the local phonon in a broad range of frequencies near resonance with an ultrashort pulse, we show it is possible to induce a Mott insulator-to-meta…
