116 research outputs found
Coherent Acoustic Perturbation of Second-Harmonic-Generation in NiO
We investigate the structural and magnetic origins of the unusual ultrafast
second-harmonicgeneration (SHG) response of femtosecond-laser-excited nickel
oxide (NiO) previously attributed to oscillatory reorientation dynamics of the
magnetic structure induced by d-d excitations. Using time-resolved x-ray
diffraction from the (3/2 3/2 3/2) magnetic planes, we show that changes in the
magnitude of the magnetic structure factor following ultrafast optical
excitation are limited to = 1.5% in the first 30 ps. An
extended investigation of the ultrafast SHG response reveals a strong
dependence on wavelength as well as characteristic echoes, both of which give
evidence for an acoustic origin of the dynamics. We therefore propose an
alternative mechanism for the SHG response based on perturbations of the
nonlinear susceptibility via optically induced strain in a spatially confined
medium. In this model, the two observed oscillation periods can be understood
as the times required for an acoustic strain wave to traverse one coherence
length of the SHG process in either the collinear or anti-collinear geometries.Comment: 26 pages, 7 figure
Dynamic pathway of the photoinduced phase transition of TbMnO
We investigate the demagnetization dynamics of the cycloidal and sinusoidal
phases of multiferroic TbMnO by means of time-resolved resonant soft x-ray
diffraction following excitation by an optical pump. Using orthogonal linear
x-ray polarizations, we suceeded in disentangling the response of the
multiferroic cycloidal spin order from the sinusoidal antiferromagnetic order
in the time domain. This enables us to identify the transient magnetic phase
created by intense photoexcitation of the electrons and subsequent heating of
the spin system on a picosecond timescale. The transient phase is shown to be a
spin density wave, as in the adiabatic case, which nevertheless retains the
wave vector of the cycloidal long range order. Two different pump photon
energies, 1.55 eV and 3.1 eV, lead to population of the conduction band
predominantly via intersite - transitions or intrasite -
transitions, respectively. We find that the nature of the optical excitation
does not play an important role in determining the dynamics of magnetic order
melting. Further, we observe that the orbital reconstruction, which is induced
by the spin ordering, disappears on a timescale comparable to that of the
cycloidal order, attesting to a direct coupling between magnetic and orbital
orders. Our observations are discussed in the context of recent theoretical
models of demagnetization dynamics in strongly correlated systems, revealing
the potential of this type of measurement as a benchmark for such complex
theoretical studies
Dynamics of the photoinduced insulator-to-metal transition in a nickelate film
The control of materials properties with light is a promising approach
towards the realization of faster and smaller electronic devices. With phases
that can be controlled via strain, pressure, chemical composition or
dimensionality, nickelates are good candidates for the development of a new
generation of high performance and low consumption devices. Here we analyze the
photoinduced dynamics in a single crystalline NdNiO film upon excitation
across the electronic gap. Using time-resolved reflectivity and resonant x-ray
diffraction, we show that the pump pulse induces an insulator-to-metal
transition, accompanied by the melting of the charge order. Finally we compare
our results to similar studies in manganites and show that the same model can
be used to describe the dynamics in nickelates, hinting towards a unified
description of these photoinduced phase transitions.Comment: 17 pages, 6 figure
The ultrafast Einstein–de Haas effect
The Einstein-de Haas effect was originally observed in a landmark experiment1 demonstrating that the angular momentum associated with aligned electron spins in a ferromagnet can be converted to mechanical angular momentum by reversing the direction of magnetization using an external magnetic field. A related problem concerns the timescale of this angular momentum transfer. Experiments have established that intense photoexcitation in several metallic ferromagnets leads to a drop in magnetization on a timescale shorter than 100 femtoseconds—a phenomenon called ultrafast demagnetization2,3,4. Although the microscopic mechanism for this process has been hotly debated, the key question of where the angular momentum goes on these femtosecond timescales remains unanswered. Here we use femtosecond time-resolved X-ray diffraction to show that most of the angular momentum lost from the spin system upon laser-induced demagnetization of ferromagnetic iron is transferred to the lattice on sub-picosecond timescales, launching a transverse strain wave that propagates from the surface into the bulk. By fitting a simple model of the X-ray data to simulations and optical data, we estimate that the angular momentum transfer occurs on a timescale of 200 femtoseconds and corresponds to 80 per cent of the angular momentum that is lost from the spin system. Our results show that interaction with the lattice has an essential role in the process of ultrafast demagnetization in this system
Itinerant and Localized Magnetization Dynamics in Antiferromagnetic Ho
Using femtosecond time-resolved resonant magnetic x-ray diffraction at the Ho L 3 absorption edge, we investigate the demagnetization dynamics in antiferromagnetically ordered metallic Ho after femtosecond optical excitation. Tuning the x-ray energy to the electric dipole ( E 1 , 2 p → 5 d ) or quadrupole ( E 2 , 2 p → 4 f ) transition allows us to selectively and independently study the spin dynamics of the itinerant 5 d and localized 4 f electronic subsystems via the suppression of the magnetic (2 1 3 − τ ) satellite peak. We find demagnetization time scales very similar to ferromagnetic 4 f systems, suggesting that the loss of magnetic order occurs via a similar spin-flip process in both cases. The simultaneous demagnetization of both subsystems demonstrates strong intra-atomic 4 f − 5 d exchange coupling. In addition, an ultrafast lattice contraction due to the release of magneto-striction leads to a transient shift of the magnetic satellite peak
Disentangling charge and structural contributions during coherent atomic motions studied by ultrafast resonant x-ray diffraction
We report on the ultrafast dynamics of charge order and structural response
during the photoinduced suppression of charge and orbital order in a
mixed-valence manganite. Employing femtosecond time-resolved resonant x-ray
diffraction below and at the Mn K absorption edge, we present a method to
disentangle the transient charge order and structural dynamics in thin films of
Pr0.5Ca0.5MnO3. Based on the static resonant scattering spectra, we extract the
dispersion correction of charge ordered Mn3+ and Mn4+ ions, allowing us to
separate the transient contributions of purely charge order from structural
contributions to the scattering amplitude after optical excitation. Our finding
of a coherent structural mode at around 2.3 THz, which primarily modulates the
lattice, but does not strongly affect the charge order, confirms the picture of
the charge order being the driving force of the combined charge, orbital and
structural transition
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