M. Trigo

Time-resolved pump-probe experiments at the LCLS

The first time-resolved x-ray/optical pump-probe experiments at the SLAC Linac Coherent Light Source (LCLS) used a combination of feedback methods and post-analysis binning techniques to synchronize an ultrafast optical laser to the linac-based x-ray laser. Transient molecular nitrogen alignment revival features were resolved in time-dependent x-ray-induced fragmentation spectra. These alignment features were used to find the temporal overlap of the pump and probe pulses. The strong-field dissociation of x-ray generated quasi-bound molecular dications was used to establish the residual timing jitter. This analysis shows that the relative arrival time of the Ti:Sapphire laser and the x-ray pulses had a distribution with a standard deviation of approximately 120 fs. The largest contribution to the jitter noise spectrum was the locking of the laser oscillator to the reference RF of the accelerator, which suggests that simple technical improvements could reduce the jitter to better than 50 fs.

Driving magnetic order in a manganite by ultrafast lattice excitation

Femtosecond midinfrared pulses are used to directly excite the lattice of the single-layer manganite La0.5Sr1.5MnO4. Magnetic and orbital orders, as measured by femtosecond resonant soft x-ray diffraction with an x-ray free-electron laser, are reduced within a few picoseconds. This effect is interpreted as a displacive exchange quench, a prompt shift in the equilibrium value of the magnetic- and orbital-order parameters after the lattice has been distorted. Control of magnetism through ultrafast lattice excitation may be of use for high-speed optomagnetism.

Femtosecond Dynamics of the Collinear-to-Spiral Antiferromagnetic Phase Transition in CuO

We report on the ultrafast dynamics of magnetic order in a single crystal of CuO at a temperature of 207 K in response to strong optical excitation using femtosecond resonant x-ray diffraction. In the experiment, a femtosecond laser pulse induces a sudden, nonequilibrium increase in magnetic disorder. After a short delay ranging from 400 fs to 2 ps, we observe changes in the relative intensity of the magnetic ordering diffraction peaks that indicate a shift from a collinear commensurate phase to a spiral incommensurate phase. These results indicate that the ultimate speed for this antiferromagnetic reorientation transition in CuO is limited by the long-wavelength magnetic excitation connecting the two phases.

Speed limit of the insulator–metal transition in magnetite

As the oldest known magnetic material, magnetite (Fe3O4) has fascinated mankind for millennia. As the first oxide in which a relationship between electrical conductivity and fluctuating/localized electronic order was shown, magnetite represents a model system for understanding correlated oxides in general. Nevertheless, the exact mechanism of the insulator-metal, or Verwey, transition has long remained inaccessible. Recently, three-Fe-site lattice distortions called trimerons were identified as the characteristic building blocks of the low-temperature insulating electronically ordered phase. Here we investigate the Verwey transition with pump-probe X-ray diffraction and optical reflectivity techniques, and show how trimerons become mobile across the insulator-metal transition. We find this to be a two-step process. After an initial 300 fs destruction of individual trimerons, phase separation occurs on a 1.5±0.2 ps timescale to yield residual insulating and metallic regions. This work establishes the speed limit for switching in future oxide electronics.

Temporal cross-correlation of x-ray free electron and optical lasers using soft x-ray pulse induced transient reflectivity.

The recent development of x-ray free electron lasers providing coherent, femtosecond-long pulses of high brilliance and variable energy opens new areas of scientific research in a variety of disciplines such as physics, chemistry, and biology. Pump-probe experimental techniques which observe the temporal evolution of systems after optical or x-ray pulse excitation are one of the main experimental schemes currently in use for ultrafast studies. The key challenge in these experiments is to reliably achieve temporal and spatial overlap of the x-ray and optical pulses. Here we present measurements of the x-ray pulse induced transient change of optical reflectivity from a variety of materials covering the soft x-ray photon energy range from 500eV to 2000eV and outline the use of this technique to establish and characterize temporal synchronization of the optical-laser and FEL x-ray pulses.

Phase fluctuations and the absence of topological defects in a photo-excited charge-ordered nickelate

The dynamics of an order parameters amplitude and phase determines the collective behaviour of novel states emerging in complex materials. Time- and momentum-resolved pump-probe spectroscopy, by virtue of measuring material properties at atomic and electronic time scales out of equilibrium, can decouple entangled degrees of freedom by visualizing their corresponding dynamics in the time domain. Here we combine time-resolved femotosecond optical and resonant X-ray diffraction measurements on charge ordered La(1.75)Sr(0.25)NiO(4) to reveal unforeseen photoinduced phase fluctuations of the charge order parameter. Such fluctuations preserve long-range order without creating topological defects, distinct from thermal phase fluctuations near the critical temperature in equilibrium. Importantly, relaxation of the phase fluctuations is found to be an order of magnitude slower than that of the order parameters amplitude fluctuations, and thus limits charge order recovery. This new aspect of phase fluctuations provides a more holistic view of the phases importance in ordering phenomena of quantum matter.

Imaging nonequilibrium atomic vibrations with x-ray diffuse scattering.

We use picosecond x-ray diffuse scattering to image the nonequilibrium vibrations in the lattice following ultrafast laser excitation. We present images of nonequilibrium phonons in InP and InSb throughout the Brillouin zone which remain out of equilibrium up to nanoseconds. The results are analyzed using a Born model that helps identify the phonon branches contributing to the observed features in the time-resolved diffuse scattering. In InP this analysis shows a delayed increase in the transverse-acoustic (TA) phonon population along high-symmetry directions accompanied by a decrease in the longitudinal-acoustic phonons. In InSb the increase in TA phonon population is less directional.

Evidence for photo-induced monoclinic metallic VO2 under high pressure

We combine ultrafast pump-probe spectroscopy with a diamond-anvil cell to decouple the insulator-metal electronic transition from the lattice symmetry changing structural transition in the archetypal strongly correlated material vanadium dioxide. Coherent phonon spectroscopy enables tracking of the photo-excited phonon vibrational frequencies of the low temperature, monoclinic (M1)-insulating phase that transforms into the metallic, tetragonal rutile structured phase at high temperature or via non-thermal photo-excitations. We find that in contrast with ambient pressure experiments where strong photo-excitation promptly induces the electronic transition along with changes in the lattice symmetry, at high pressure, the coherent phonons of the monoclinic (M1) phase are still clearly observed upon the photo-driven phase transition to a metallic state. These results demonstrate the possibility of synthesizing and studying transient phases under extreme conditions.

Ultrafast electron diffraction from non-equilibrium phonons in femtosecond laser heated Au films

We use ultrafast electron diffraction to detect the temporal evolution of non-equilibrium phonons in femtosecond laser-excited ultrathin single-crystalline gold films. From the time-dependence of the Debye-Waller factor, we extract a 4.7 ps time-constant for the increase in mean-square atomic displacements. The observed increase in the diffuse scattering intensity demonstrates that the energy transfer from laser-heated electrons to phonon modes near the X and K points in the Au fcc Brillouin zone proceeds with timescales of 2.3 and 2.9 ps, respectively, faster than the Debye-Waller average mean-square displacement.

Generation mechanism of terahertz coherent acoustic phonons in Fe

T Henighan1,2,∗ M Trigo, S Bonetti, P Granitzka, D Higley, Z Chen, M P Jiang, R Kukreja, A Gray, A H Reid, E Jal, M C Hoffmann, M Kozina, S Song, M Chollet, D Zhu, P F Xu, J Jeong, K Carva, P Maldonado, P M Oppeneer, M G Samant, S S P. Parkin, D A Reis, and H A Dürr3† PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, California, USA Physics Department, Stanford University, Stanford, California, USA Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, CA 94025. Van der Waals-Zeeman Institute, University of Amsterdam, 1018XE Amsterdam, The Netherlands Department of Photon Science and Applied Physics, Stanford University, Stanford, California, USA Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, California, USA IBM Almaden Research Center, 650 Harry Road, San Jose, California 95120, USA Max-Planck Institute for Microstructure Physics, 06120 Halle (Saale), Germany Charles University, Faculty of Mathematics and Physics, Department of Condensed Matter Physics, Ke Karlovu 5, CZ-12116 Prague 2, Czech Republic and Department of Physics and Astronomy, Uppsala University, P. O. Box 516, S-75120 Uppsala, Sweden (Dated: September 14, 2015)