Ultrafast Laser-induced Dynamics Research Articles

Ultrafast Laser-Induced Dynamics of Non-Equilibrium Electron Spill-Out in Nanoplasmonic Bilayers.

Contemporary quantum plasmonics capture subtle corrections to the properties of plasmonic nano-objects in equilibrium. Here, we demonstrate non-equilibrium spill-out redistribution of the electronic density at the ultrafast time scale. As revealed by time-resolved 2D spectroscopy of nanoplasmonic Fe/Au bilayers, an injection of the laser-excited non-thermal electrons induces transient electron spill-out thus changing the plasma frequency. The response of the local electronic density switches the electronic density behavior from spill-in to strong (an order of magnitude larger) spill-out at the femtosecond time scale. The superdiffusive transport of hot electrons and the lack of a direct laser heating indicate significantly non-thermal origin of the underlying physics. Our results demonstrate an ultrafast and non-thermal way to control surface plasmon dispersion through transient variations of the spatial electron distribution at the nanoscale. These findings expand quantum plasmonics into previously unexplored directions by introducing ultrashort time scales in the non-equilibrium electronic systems.

Ultrafast Spin Dynamics and Photoinduced Insulator-to-Metal Transition in α-RuCl3.

Laser-induced ultrafast demagnetization is a phenomenon of utmost interest and attracts significant attention because it enables potential applications in ultrafast optoelectronics and spintronics. As a spin-orbit coupling assisted magnetic insulator, α-RuCl3 provides an attractive platform to explore the physics of electronic correlations and unconventional magnetism. Using time-dependent density functional theory, we explore the ultrafast laser-induced dynamics of the electronic and magnetic structures in α-RuCl3. Our study unveils that laser pulses can introduce ultrafast demagnetizations, accompanied by an out-of-equilibrium insulator-to-metal transition in a few tens of femtoseconds. The spin response significantly depends on the laser wavelength and polarization on account of the electron correlations, band renormalizations, and charge redistributions. These findings provide physical insights into the coupling between the electronic and magnetic degrees of freedom in α-RuCl3 and shed light on suppressing the long-range magnetic orders and reaching a proximate spin liquid phase for two-dimensional magnets on an ultrafast time scale.

Ultrafast laser-induced spin–lattice dynamics in the van der Waals antiferromagnet CoPS3

CoPS3 stands out in the family of the van der Waals antiferromagnets XPS3 (X = Mn, Ni, Fe, and Co) due to the unquenched orbital momentum of the magnetic Co2+ ions, which is known to facilitate the coupling of spins to both electromagnetic waves and lattice vibrations. Here, using a time-resolved magneto-optical pump–probe technique, we experimentally study the ultrafast laser-induced dynamics of mutually correlated spins and lattice. It is shown that a femtosecond laser pulse acts as an ultrafast heater and, thus, results in the melting of the antiferromagnetic order. At the same time, the resonant pumping of the 4T1g → 4T2g electronic transition in Co2+ ions effectively changes their orbital momentum, giving rise to a mechanical force that moves the ions in the direction parallel to the orientation of their spins, thus generating a coherent Bg phonon mode at the frequency of about 4.7 THz.

Understanding real-time time-dependent density-functional theory simulations of ultrafast laser-induced dynamics in organic molecules.

Real-time time-dependent density functional theory, in conjunction with the Ehrenfest molecular dynamics scheme, is becoming a popular methodology to investigate ultrafast phenomena on the nanoscale. Thanks to recent developments, it is also possible to explicitly include in the simulations a time-dependent laser pulse, thereby accessing the transient excitation regime. However, the complexity entailed in these calculations calls for in-depth analysis of the accessible and yet approximate (either "dressed" or "bare") quantities in order to evaluate their ability to provide us with a realistic picture of the simulated processes. In this work, we analyze the ultrafast dynamics of three small molecules (ethylene, benzene, and thiophene) excited by a resonant laser pulse in the framework of the adiabatic local-density approximation. The electronic response to the laser perturbation in terms of induced dipole moment and excited-state population is compared to the results given by an exactly solvable two-level model. In this way, we can interpret the charge-carrier dynamics in terms of simple estimators, such as the number of excited electrons. From the computed transient absorption spectra, we unravel the appearance of nonlinear effects such as excited-state absorption and vibronic coupling. In this way, we observe that the laser excitation affects the vibrational spectrum by enhancing the anharmonicities therein, while the coherent vibrational motion contributes to stabilizing the electronic excitation already within a few tens of femtoseconds.

Atomic and molecular suite of R-matrix codes for ultrafast dynamics in strong laser fields and electron/positron scattering

SynopsisWe describe and illustrate a number of recent developments of the atomic and molecular ab initio R-matrix suites for both time-dependent calculations of ultrafast laser-induced dynamics and time-independent calculations of photoionization and electron scattering.

Ultrafast Spin Dynamics in Photodoped Spin-Orbit Mott Insulator Sr2IrO4

Ultrafast photodoping of the Mott insulators, possessing strong correlation between electronic and magnetic degrees of freedom, holds promise for launching an ultrafast dynamics of spins which cannot be described in terms of conventional models of ultrafast magnetism. Here we study the ultrafast laser-induced dynamics of the magnetic order in a novel spin-orbit Mott insulator Sr2IrO4 featuring an uncompensated pattern of antiferromagnetic spin ordering. Using the transient magneto-optical Kerr effect sensitive to the net magnetization, we reveal that photodoping by femtosecond laser pulses with photon energy above the Mott gap launches melting of the antiferromagnetic order seen as ultrafast demagnetization with a characteristic time of 300 fs followed by a sub-10-ps recovery. Nonequilibrium dynamical mean-field theory calculations based on the single-band Hubbard model confirm that ultrafast demagnetization is primarily governed by the laser-induced generation of electron-hole pairs, although the precise simulated time dependencies are rather different from the experimentally observed ones. To describe the experimental results, here we suggest a phenomenological model which is based on Onsager’s formalism and accounts for the photogenerated electron-hole pairs using the concepts of holons and doublons.

Exchange scattering as the driving force for ultrafast all-optical and bias-controlled reversal in ferrimagnetic metallic structures

Experimentally observed ultrafast all-optical magnetization reversal in ferrimagnetic metals and heterostructures based on antiferromagnetically coupled ferromagnetic $d-$ and $f-$metallic layers relies on intricate energy and angular momentum flow between electrons, phonons and spins. Here we treat the problem of angular momentum transfer in the course of ultrafast laser-induced dynamics in a ferrimagnetic metallic system using microscopical approach based on the system of rate equations. We show that the magnetization reversal is supported by a coupling of $d-$ and $f-$ subsystems to delocalized $s-$ or $p-$ electrons. The latter can transfer spin between the two subsystems in an incoherent way owing to the $(s;p)-(d;f)$ exchange scattering. Since the effect of the external excitation in this process is reduced to the transient heating of the mobile electron subsystem, we also discuss possibility to trigger the magnetization reversal by applying a voltage bias pulse to antiferromagnetically coupled metallic ferromagnetic layers embedded in point contact or tunneling structures. We argue that such devices allow controlling reversal with high accuracy. We also suggest to use the anomalous Hall effect to register the reversal, thus playing a role of reading probes.

Ultrafast laser-induced dynamics of noncollinear spin structures in amorphous NdFeCo and PrFeCo

The fanned out, noncollinear spin structure of the Fe(Co) sublattice in amorphous NdFeCo and PrFeCo alloys is shown to strongly affect its ultrafast laser-induced magnetization dynamics. An overshooting effect is discovered at low applied magnetic fields, where the magnetization temporarily increases above its equilibrium value. We explain this phenomenon by considering the dynamics of the noncollinear spin structure. After femtosecond laser excitation the system first reconstructs magnetic order on a time scale of 50--150 ps arriving at a state with a smaller opening angle of the fan. Subsequently, the original opening angle is restored on a time scale of nanoseconds. Increasing the field up to 0.6 T we can fully close the fan and therewith suppress the overshooting behavior.