Strongly correlated electron systems often exhibit very strong interactions between structural and electronic degrees of freedom that lead to complex and interesting phase diagrams. For technological applications of these materials it is important to learn how to drive transitions from one phase to another. A key question here is the ultimate speed of such phase transitions, and to understand how a phase transition evolves in the time domain. Here we apply time-resolved X-ray diffraction to directly measure the changes in long-range order during ultrafast melting of the charge and orbitally ordered phase in a perovskite manganite. We find that although the actual change in crystal symmetry associated with this transition occurs over different timescales characteristic of the many electronic and vibrational coordinates of the system, the dynamics of the phase transformation can be well described using a single time-dependent 'order parameter' that depends exclusively on the electronic excitation.

The original observation of the Einstein-de Haas effect was a landmark experiment in the early history of modern physics that illustrates the relationship between magnetism and angular momentum 1, 2 . Today the effect is still discussed in elementary physics courses to demonstrate that the angular momentum associated with the aligned electron spins in a ferromagnet can be converted to mechanical angular momentum by reversing the direction of magnetisation using an external magnetic field. In recent times, a related problem in magnetism concerns the time-scale over which this angular momentum transfer can occur. It is known experimentally for several metallic ferromagnets that intense photoexcitation leads to a drop in the magnetisation on a time scale shorter than 100 fs, a phenomenon called ultrafast demagnetisation 3-5 . The microscopic mechanism for this process has been hotly debated, with one key question still unanswered: where does the angular momentum go on these femtosecond time scales? Here we show using femtosecond time-resolved x-ray diffraction that a majority of the angular momentum lost from the spin system on the laser-induced demagnetisation of ferromagnetic iron is transferred to the lattice on sub-picosecond timescales, manifesting as 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 occurs on a time scale of 200 fs and corresponds to 80% of the angular momentum lost from the spin system. Our results show that interaction with the lattice plays an essential role in the process of ultrafast demagnetisation in this system. 2Broadly speaking, proposed mechanisms for ultrafast demagnetisation fall into two categories: spin-flip scattering mechanisms and spin transport mechanisms. The first category explains the demagnetisation process as a sudden increase in scattering processes that ultimately result in a decrease of spin order. These scattering processes can include electron-electron, electron-phonon, electron-magnon and even direct spin-light interactions. On average, such scattering must necessarily involve a transfer of angular momentum from the electronic spins to some other subsystem(s). Candidates include the lattice, the electromagnetic field, and the orbital angular momentum of the electrons. Numerical estimates and experiments using circularly polarised light strongly suggest that the amount of angular momentum given to the electromagnetic field interaction is negligible 6 , and experiments using femtosecond x-ray magnetic dichroism (XMCD) indicate that the angular momentum of both electronic spins and orbitals decrease in magnitude nearly simultaneously 7-9 . The only remaining possibility for a spin-flip induced change in angular momentum therefore appears to be a transfer to the lattice via spin-orbit coupling, but this remains to be experimentally verified.The second category of proposed mechanisms relies on the idea that laser excitation causes a ...

Using femtosecond time-resolved x-ray diffraction, we directly monitor the coherent lattice dynamics through an ultrafast charge-density-wave-to-metal transition in the prototypical Peierls system K(0.3)MoO(3) over a wide range of relevant excitation fluences. While in the low fluence regime we directly follow the structural dynamics associated with the collective amplitude mode; for fluences above the melting threshold of the electronic density modulation we observe a transient recovery of the periodic lattice distortion. We can describe these structural dynamics as a motion along the coordinate of the Peierls distortion triggered by the prompt collapse of electronic order after photoexcitation. The results indicate that the dynamics of a structural symmetry-breaking transition are determined by a high-symmetry excited state potential energy surface distinct from that of the initial low-temperature state.

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 (E1, 2p → 5d) or quadrupole (E2, 2p → 4f) transition allows us to selectively and independently study the spin dynamics of the itinerant 5d and localized 4f electronic subsystems via the suppression of the magnetic (2 1 3-τ) satellite peak. We find demagnetization time scales very similar to ferromagnetic 4f 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 4f-5d 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. DOI: 10.1103/PhysRevLett.116.257202 The manipulation of magnetic order by ultrashort light pulses is of fundamental interest in solid state research and promises high technological relevance. Since the discovery of the demagnetization of Ni in <1 ps almost two decades ago [1], the ultrafast magnetization dynamics of ferromagnetic systems has been intensely studied both experimentally and theoretically [2-6]; for a review see Refs. [7,8]. In particular, the phenomenon of ultrafast magnetization reversal recently observed in ferrimagnetic lanthanide transition metal intermetallics [8][9][10][11][12][13] has attracted much attention. In these materials a complex interaction between localized f moments in the rare-earth ions and the itinerant transition metal d electrons is thought to enable the reversal of the magnetic moment on subpicosecond time scales. The interaction leads to several unexpected phenomena such as a transient ferromagnetic state in FeCoGd [10] and ultrafast angular momentum transfer between different volumes within an inhomogeneous ferrimagnetic alloy [12].In the rare-earth metals, the magnetic exchange interaction between the large localized moments of the open 4f shells is mediated by the indirect Ruderman-Kittel-KasuyaYosida (RKKY) interaction via the itinerant 5d6s electrons, leading to a parallel alignment of the two subsystems. Depending on the details of the band structure, this interaction results in a variety of magnetically ordered ground states, ranging from ferromagnetic alignment in Gd and Tb to complex antiferromagnetic (AFM) structures in the heavier rare earths. As optical excitation directly interacts with the valence electrons and not with the localized 4f states, these systems present an ideal case to study the 4f-5d interaction directly in the time domain by separately investigating the dynamics of these two subsystems. While early experiments using x-ray magnetic circular dichroism (XMCD) and the magneto-optical Kerr effect (MOKE) on the ferromagnetic lanthanides Gd and Tb found similar demagnetization time scales of 4f and 5d electrons [14], more...

Material properties can be controlled via strain, pressure, chemical composition, or dimensionality. Nickelates are particularly susceptible due to their strong variations of the electronic and magnetic properties on such external stimuli. Here, we analyze the photoinduced dynamics in a single crystalline NdNiO 3 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 with 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 electronic ordering phase transitions.