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Mankowsky, R.

Publications and source records attributed to Mankowsky, R..

Strain wave pathway to semiconductor-to-metal transition revealed by time-resolved X-ray powder diffraction

One of the main challenges in ultrafast material science is to trigger phase transitions with short pulses of light. Here we show how strain waves, launched by electronic and structural precursor phenomena, determine a coherent macroscopic transformation pathway for the semiconducting-to-metal transition in bistable Ti 3 O 5 nanocrystals. Employing femtosecond powder X-ray diffraction, we measure the lattice deformation in the phase transition as a function of time. We monitor the early intra-cell distortion around the light absorbing metal dimer and the long range deformations governed by acoustic waves propagating from the laser-exposed Ti 3 O 5 surface. We developed a simplified elastic model demonstrating that picosecond switching in nanocrystals happens concomitantly with the propagating acoustic wavefront, several decades faster than thermal processes governed by heat diffusion.

36 MATERIALS SCIENCE↗

Nonlinear electron-phonon coupling in doped manganites

Here, we employ time-resolved resonant x-ray diffraction to study the melting of charge order and the associated insulator-to-metal transition in the doped manganite Pr 0.5 Ca 0.5 MnO 3 after resonant excitation of a high-frequency infrared-active lattice mode. We find that the charge order reduces promptly and highly nonlinearly as function of excitation fluence. Density-functional theory calculations suggest that direct anharmonic coupling between the excited lattice mode and the electronic structure drives these dynamics, highlighting a new avenue of nonlinear phonon control.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Optically induced lattice deformations, electronic structure changes, and enhanced superconductivity in YBa 2 Cu 3 O 6.48

Resonant optical excitation of apical oxygen vibrational modes in the normal state of underdoped YBa 2 Cu 3 O 6+x induces a transient state with optical properties similar to those of the equilibrium superconducting state. Amongst these, a divergent imaginary conductivity and a plasma edge are transiently observed in the photo-stimulated state. Femtosecond hard x-ray diffraction experiments have been used in the past to identify the transient crystal structure in this non-equilibrium state. Here, we start from these crystallographic features and theoretically predict the corresponding electronic rearrangements that accompany these structural deformations. Using density functional theory, we predict enhanced hole-doping of the CuO 2 planes. The empty chain Cu dy 2 -z 2 orbital is calculated to strongly reduce in energy, which would increase c-axis transport and potentially enhance the interlayer Josephson coupling as observed in the THz-frequency response. From these results, we calculate changes in the soft x-ray absorption spectra at the Cu L -edge. As a result, femtosecond x-ray pulses from a free electron laser are used to probe changes in absorption at two photon energies along this spectrum and provide data consistent with these predictions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Multiple Supersonic Phase Fronts Launched at a Complex-Oxide Heterointerface

Selective optical excitation of a substrate lattice can drive phase changes across heterointerfaces. This phenomenon is a nonequilibrium analogue of static strain control in heterostructures and may lead to new applications in optically controlled phase change devices. Here, we make use of time-resolved nonresonant and resonant x-ray diffraction to clarify the underlying physics and to separate different microscopic degrees of freedom in space and time. We also measure the dynamics of the lattice and that of the charge disproportionation in NdNiO 3 , when an insulator-metal transition is driven by coherent lattice distortions in the LaAlO 3 substrate. We find that charge redistribution propagates at supersonic speeds from the interface into the NdNiO 3 film, followed by a sonic lattice wave. Our results establish a hierarchy of events for ultrafast control at complex-oxide heterointerfaces, when combined with measurements of magnetic disordering and of the metal-insulator transition.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Restoring interlayer Josephson coupling in La 1.885 Ba 0.115 CuO 4 by charge transfer melting of stripe order

Here, we show that disruption of charge-density-wave (stripe) order by charge transfer excitation, enhances the superconducting phase rigidity in La 1.885 Ba 0.115 CuO 4 . Time-resolved resonant soft x-ray diffraction demonstrates that charge order melting is prompt following near-infrared photoexcitation whereas the crystal structure remains intact for moderate fluences. THz time-domain spectroscopy reveals that, for the first 2 ps following photoexcitation, a new Josephson plasma resonance edge, at higher frequency with respect to the equilibrium edge, is induced indicating enhanced superconducting interlayer coupling. Furthermore, the fluence dependence of the charge-order melting and the enhanced superconducting interlayer coupling are correlated with a saturation limit of ~0.5mJ/cm 2 . When using a combination of x-ray and optical spectroscopies we establish a hierarchy of timescales between enhanced superconductivity, melting of charge order, and rearrangement of the crystal structure.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ultrafast energy- and momentum-resolved dynamics of magnetic correlations in the photo-doped Mott insulator Sr 2 IrO 4

Measuring how the magnetic correlations evolve in doped Mott insulators has greatly improved our understanding of the pseudogap, non-Fermi liquids and high-temperature superconductivity 1, 2, 3, 4 . Recently, photo-excitation has been used to induce similarly exotic states transiently 5, 6, 7 . However, the lack of available probes of magnetic correlations in the time domain hinders our understanding of these photo-induced states and how they could be controlled. Here, we implement magnetic resonant inelastic X-ray scattering at a free-electron laser to directly determine the magnetic dynamics after photo-doping the Mott insulator Sr 2 IrO 4 . We find that the non-equilibrium state, 2 ps after the excitation, exhibits strongly suppressed long-range magnetic order, but hosts photo-carriers that induce strong, non-thermal magnetic correlations. These two-dimensional (2D) in-plane Néel correlations recover within a few picoseconds, whereas the three-dimensional (3D) long-range magnetic order restores on a fluence-dependent timescale of a few hundred picoseconds. In conclusion, the marked difference in these two timescales implies that the dimensionality of magnetic correlations is vital for our understanding of ultrafast magnetic dynamics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Spatially resolved ultrafast magnetic dynamics initiated at a complex oxide heterointerface

Static strain in complex oxide heterostructures 1,2 has been extensively used to engineer electronic and magnetic properties at equilibrium 3 . In the same spirit, deformations of the crystal lattice with light may be used to achieve functional control across heterointerfaces dynamically 4 . Here, by exciting large-amplitude infrared-active vibrations in a LaAlO 3 substrate we induce magnetic order melting in a NdNiO 3 film across a heterointerface. Femtosecond resonant soft X-ray diffraction is used to determine the spatiotemporal evolution of the magnetic disordering. We observe a magnetic melt front that propagates from the substrate interface into the film, at a speed that suggests electronically driven motion. Lastly, light control and ultrafast phase front propagation at heterointerfaces may lead to new opportunities in optomagnetism, for example by driving domain wall motion to transport information across suitably designed devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Femtosecond x rays link melting of charge-density wave correlations and light-enhanced coherent transport in YB a 2 C u 3 O 6.6

In this study, we use femtosecond resonant soft x-ray diffraction to measure the optically stimulated ultrafast changes of charge density wave correlations in underdoped YBa₂Cu₃O₆.₆. We find that when coherent interlayer transport is enhanced by optical excitation of the apical oxygen distortions, at least 50% of the in-plane charge density wave order is melted. These results indicate that charge ordering and superconductivity may be competing up to the charge ordering transition temperature, with the latter becoming a hidden phase that is accessible only by nonlinear phonon excitation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗