We show the ferro-rotational nature of the commensurate charge density wave (CCDW) in $1T$-$\mathrm{TaS}_2$ and track its dynamic modulations by temperature-dependent and time-resolved electric quadrupole rotation anisotropy-second harmonic generation (EQ RA-SHG), respectively. The ultrafast modulations manifest as the breathing and the rotation of the EQ RA-SHG patterns at three frequencies around the reported single CCDW amplitude mode frequency. A sudden shift of the triplet frequencies and a dramatic increase in the breathing and rotation magnitude further reveal a photo-induced transient CDW phase across a critical pump fluence of ~ 0.5 mJ/cm$^2$.
We use an x-ray free-electron laser to study the ultrafast lattice dynamics following above band-gap photoexcitation of the incipient ferroelectric potassium-tantalate, \kto. % We use ultrafast near-UV (central wavelength 266\,nm and 50 fs pulse duration) laser light to photoexcite charge carriers across the gap and probe the ultrafast lattice dynamics by recording the x-ray diffuse intensity throughout multiple Brillouin zones using pulses from the Linac Coherent Light Source (LCLS) (central wavelength 1.3\,Å\, and $< 10$~fs pulse duration). We observe changes in the diffuse intensity that we…
Rashba materials have appeared as an ideal playground for spin-to-charge conversion in prototype spintronics devices. Among them, $α$-GeTe(111) is a non-centrosymmetric ferroelectric (FE) semiconductor for which a strong spin-orbit interaction gives rise to giant Rashba coupling. Its room temperature ferroelectricity was recently demonstrated as a route towards a new type of highly energy-efficient non-volatile memory device based on switchable polarization. Currently based on the application of an electric field, the writing and reading processes could be outperformed by the use of femtosecon…
We analyze theoretically the demagnetization dynamics in a ferromagnetic model system due to the interplay of spin-orbit coupling and electron-electron Coulomb scattering. We compute the $k$-resolved electronic reduced spin-density matrix including precessional dynamics around internal spin-orbit and exchange fields as well as the electron-electron Coulomb scattering for densities and spin coherences. Based on a comparison with numerical solutions of the full Boltzmann scattering integrals, we establish that the $k$-resolved reduced spin-density matrix dynamics are well described using a simpl…
Weakly coupled ferroelectric/dielectric superlattice thin film heterostructures exhibit complex nanoscale polarization configurations that arise from a balance of competing electrostatic, elastic, and domain-wall contributions to the free energy. A key feature of these configurations is that the polarization can locally have a significant component that is not along the thin-film surface normal direction, while maintaining zero net in-plane polarization. PbTiO3/SrTiO3 thin-film superlattice heterostructures on a conducting SrRuO3 bottom electrode on SrTiO3 have a room-temperature stripe nanodo…
Ultrafast optical control of ferroelectricity using intense terahertz fields has attracted significant interest. Here we show that the nonlinear interactions between two optical phonons in SnTe, a two-dimensional in-plane ferroelectric material, enables a dynamical amplification of the electric polarization within subpicoseconds time domain. Our first principles time dependent simulations show that the infrared-active out-of-plane phonon mode, pumped to nonlinear regimes, spontaneously generates in-plane motions, leading to rectified oscillations in the in-plane electric polarization. We sugge…
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…
Following the demonstration of laser-induced ultrafast demagnetization in ferromagnetic nickel, several theoretical and phenomenological propositions have sought to uncover its underlying physics. In this work we revisit the three temperature model (3TM) and the microscopic three temperature model (M3TM) to perform a comparative analysis of ultrafast demagnetization in 20-nm-thick cobalt, nickel and permalloy thin films measured using an all-optical pump-probe technique. In addition to the ultrafast dynamics at the femtosecond timescales, the nanosecond magnetization precession and damping are…
We report on an element- and time-resolved investigation of femtosecond laser induced ultrafast dynamics of 3d and 4f spins in a ferrimagnetic Co80Dy20 alloy as a function of temperature. We observe an increase of the Co3d characteristic demagnetization time and a decrease of the Dy4f demagnetization time when the temperature is approaching the Curie temperature. It suggests that the critical slowing down regime, which affects the laser induced ultrafast dynamics in pure 3d transition metals and 4f rare-earth ferromagnetic layers, vanishes for the Dy sublattice in the CoDy alloy, in line with …
Spin-to-charge conversion (SCC) involving topological surface states (TSS) is one of the most promising routes for highly efficient spintronic devices for terahertz (THz) emission. Here, the THz generation generally occurs mainly via SCC consisting in efficient dynamical spin injection into spin-locked TSS. In this work, we demonstrate sizable THz emission from a nanometric thick topological insultator (TI)/ferromagnetic junction - SnBi$_2$Te$_4$/Co - specifically designed to avoid bulk band crossing with the TSS at the Fermi level, unlike its parent material Bi$_2$Te$_3$. THz emission time do…
Damping effects form the core of many emerging concepts for high-speed spintronic applications. Important characteristics such as device switching times and magnetic domain-wall velocities depend critically on the damping rate. While the implications of spin damping for relaxation processes are intensively studied, damping effects during impulsive spin excitations are assumed to be negligible because of the shortness of the excitation process. Herein, we show that, unlike in ferromagnets, ultrafast damping plays a crucial role in antiferromagnets because of their strongly elliptical spin prece…
Spintronic structures are extensively investigated for their spin orbit torque properties, required for magnetic commutation functionalities. Current progress in these materials is dependent on the interface engineering for the optimization of spin transmission. Here, we advance the analysis of ultrafast spin-charge conversion phenomena at ferromagnetic-transition metal interfaces due to their inverse spin-Hall effect properties. In particular the intrinsic inverse spin Hall effect of Pt-based systems and extrinsic inverse spin-Hall effect of Au:W and Au:Ta in NiFe/Au:(W,Ta) bilayers are inves…