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Abstract: The phase-space path-integral approach to the damped harmonic oscillator is analyzed beyond the Markovian approximation. It is found that pairs of nonclassical trajectories contribute to the path-integral representation of the Wigner propagating function. Due to the linearity of the problem, the sum coordinate of a pair still satisfies the classical equation of motion. Furthermore, it is shown that the broadening of the Wigner propagating function of the damped oscillator arises due to the time-nonlocal interaction mediated by the heat bath. [ABSTRACT FROM AUTHOR]

The dynamics of the surface plasmon in laser-driven metallic nanoparticles is described by means of a master-equation formalism. Within the Markov approximation, the dynamics is studied for different regimes ranging from weak excitation in photoabsorption experiments to strong excitation in pump-probe spectroscopy. It is shown that two collective levels are sufficient to describe the dynamics of the surface plasmon. On this basis, we predict the appearance of sidebands in the absorption spectrum of the probe laser field in pump-probe experiments. [ABSTRACT FROM AUTHOR]

FEMTO, a femtosecond (fs) X-ray source based on laser interaction with a relativistic electron beam, began operation in the fall of 2006. It is installed at the μXAS beamline of the Swiss Light Source (SLS) at the Paul Scherrer Institut, Villigen. “Laser slicing” of an electron beam has first been proposed and demonstrated at the ALS [1] and has recently been implemented at BESSY [2] to generate fs soft X-rays (1-2 keV) with variable polarization. FEMTO is the first undulator source providing tunable, fs hard X-rays in the range 4.5-12 keV for laser/X-ray pump-probe absorption and diffraction experiments. [ABSTRACT FROM AUTHOR]

The dynamics of the surface plasmon in laser-driven metallic nanoparticles is described by means of a master-equation formalism. Within the Markov approximation, the dynamics is studied for different regimes ranging from weak excitation in photoabsorption experiments to strong excitation in pump-probe spectroscopy. It is shown that two collective levels are sufficient to describe the dynamics of the surface plasmon. On this basis, we predict the appearance of sidebands in the absorption spectrum of the probe laser field in pump-probe experiments. [ABSTRACT FROM AUTHOR]

The Swiss Light Source (SLS) at the Paul Scherrer Institut (PSI) started user operation in 2001. It has been the first medium energy light source to rely on undulators for the production of X-rays up to 20 keV. For soft X-rays, APPLE II-type undulators, providing full polarization control and quasiperiodic electromagnetic undulators, have been installed. The hard X-ray range has been accessed by the newly developed small-gap, short-period, in-vacuum undulators operated on high harmonics. Based on this, FEMTO, the first hard X-ray undulator source for femtosecond (fs) experiments, started operation in 2006. [ABSTRACT FROM PUBLISHER]

Abstract: We use X-ray diffraction to confirm that the 5M phase of the stoichiometric Heusler alloy Ni2MnGa has an incommensurate modulation with wavevector . We find the crystal to be macroscopically twinned with a structure well described by the theory of martensitic phase transitions, though theoretical calculations of the X-ray diffraction rule out the existence of an adaptive phase. The premartensite phase is found to be slightly incommensurate with . [Copyright &y& Elsevier]

We use time-resolved x-ray diffraction and magneto-optical Kerr effect to study the laser-induced antiferromagnetic to ferromagnetic phase transition in FeRh. The structural response is given by the nucleation of independent ferromagnetic domains (&tgr;1 ∼ 30 ps). This is significantly faster than the magnetic response (&tgr;2 ∼ 60 ps) given by the subsequent domain realignment. X-ray diffraction shows that the two phases coexist on short time scales and that the phase transition is limited by the speed of sound. A nucleation model describing both the structural and magnetic dynamics is presented. [ABSTRACT FROM AUTHOR]

Transition metal oxides are among the most promising solar materials, whose properties rely on the generation, transport and trapping of charge carriers (electrons and holes). Identifying the latter's dynamics at room temperature requires tools that combine elemental and structural sensitivity, with the atomic scale resolution of time (femtoseconds, fs). Here, we use fs Ti K-edge X-ray absorption spectroscopy (XAS) upon 3.49 eV (355 nm) excitation of aqueous colloidal anatase titanium dioxide nanoparticles to probe the trapping dynamics of photogenerated electrons. We find that their localization at Titanium atoms occurs in <300 fs, forming Ti3+ centres, in or near the unit cell where the electron is created. We conclude that electron localization is due to its trapping at pentacoordinated sites, mostly present in the surface shell region. The present demonstration of fs hard X-ray absorption capabilities opens the way to a detailed description of the charge carrier dynamics in transition metal oxides. [ABSTRACT FROM AUTHOR]

We have studied the ultrafast changes of electronic states in bulk ZnO upon intense hard x-ray excitation from a free electron laser. By monitoring the transient anisotropy induced in an optical probe beam, we observe a delayed breaking of the initial c-plane symmetry of the crystal that lasts for several picoseconds. Interaction with the intense x-ray pulses modifies the electronic state filling in a manner inconsistent with a simple increase in electronic temperature. These results may indicate a way to use intense ultrashort x-ray pulses to investigate high-energy carrier dynamics and to control certain properties of solid-state materials. [ABSTRACT FROM AUTHOR]

1T-TaS 2 is a 2D metallic compound which undergoes a series of electronically driven phase transitions toward charge density wave and Mott phases. Its intricate electron–phonon interactions and electron–electron correlations have been promising peculiar out-of-equilibrium dynamics. In this paper, we provide the first direct information on the atomic structure response to an ultra-fast infrared laser pulse in the commensurate phase of 1T-TaS 2 , by using femtosecond time-resolved X-ray diffraction. We show that ultra-fast excitation with near-infrared photons drives a displacive excitation of the amplitude mode of the commensurate charge density wave. About 3 ps after laser excitation, the system reaches a new, photo-induced state that is maintained for at least 10 ps. We give evidence that this long-lived state exhibits the same structural modulation as in the thermodynamically stable commensurate phase, with a large correlation length. Only the average amplitude of the modulation is found to decrease. We propose that the long-lived state is formed from the commensurate phase by reducing the modulation amplitude on few superlattice nodes. The underlying mechanism proposed is the annihilation of self-trapped polarons. [ABSTRACT FROM AUTHOR]

Using femtosecond time-resolved x-ray diffraction we investigate the structural dynamics of the coherently excited A1g phonon mode in the Fe-pnictide parent compound BaFe2As2. The fluence dependent intensity oscillations of two specific Bragg reflections with distinctly different sensitivity to the pnictogen height in the compound allow us to quantify the coherent modifications of the Fe-As tetrahedra, indicating a transient increase of the Fe magnetic moments. By a comparison with time-resolved photoemission data, we derive the electron-phonon deformation potential for this particular mode. The value of Δμ/Δz = -(1.0-1.5) eV/Å is comparable with theoretical predictions and demonstrates the importance of this degree of freedom for the electron-phonon coupling in the Fe pnictides. [ABSTRACT FROM AUTHOR]

Magnetic shape-memory Heusler alloys are multiferroics stabilized by the correlations between electronic, magnetic, and structural order. To study these correlations we use time-resolved x-ray diffraction and magnetooptical Kerr effect experiments to measure the laser induced dynamics in a Heusler alloy Ni2MnGa him and reveal a set of time scales intrinsic to the system. We observe a coherent phonon which we identify as the amplitudon of the modulated structure and an ultrafast phase transition leading to a quenching of the incommensurate modulation within 300 fs with a recovery time of a few ps. The thermally driven martensitic transition to the high temperature cubic phase proceeds via nucleation within a few ps and domain growth limited by the speed of sound. The demagnetization time is 320 fs, which is comparable to the quenching of the structural modulation. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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 K0.3MoO3 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. [ABSTRACT FROM AUTHOR]

We use ultrafast resonant x-ray diffraction to study the magnetic order in CuO under conditions of high electronic excitation. By measuring changes in the spectral shape of the Cu2+ magnetic (1/20 – 1/2) reflection we investigate how an intense optical pump pulse perturbs the electronic and magnetic states. We observe an energy shift in the magnetic resonance at short times after the pump pulse. This shift is compared with expectations from band structure calculations at different electronic temperatures. This spectral line shift indicates that although the electrons are heated to effective electron temperatures far above TN on a time scale faster than the experimental resolution, magnetic order persists in this highly excited state for several hundred femtoseconds. [ABSTRACT FROM AUTHOR]

The strength of the electron-phonon coupling parameter and its evolution throughout a solid's phase diagram often determines phenomena such as superconductivity, charge- and spin-density waves. Its experimental determination relies on the ability to distinguish thermally activated phonons from those emitted by conduction band electrons, which can be achieved in an elegant way by ultrafast techniques. Separating the electronic from the out-of-equilibrium lattice subsystems, we probed their reequilibration by monitoring the transient lattice temperature through femtosecond x-ray diffraction in La2-xSrxCuO4 single crystals with x=0.1 and 0.21. The temperature dependence of the electron-phonon coupling is obtained experimentally and shows similar trends to what is expected from the ab initio calculated shape of the electronic density of states near the Fermi energy. This study evidences the important role of band effects in the electron-lattice interaction in solids, in particular, in superconductors. [ABSTRACT FROM AUTHOR]

We apply grazing-incidence femtosecond x-ray diffraction to investigate the details of the atomic motion connected with a displacively excited coherent optical phonon. We concentrate on the low frequency phonon associated with the charge and orbital order in the mixed valence manganite La0.25Pr0.375Ca0.375MnO3 for T≲210 K. We measure the response of three superlattice reflections that feature different sensitivities to the motion of the unit cell constituents. The results support the assignment to a translational mode of the Mn4+ atoms together with the oxygen atoms connecting adjacent Mn4+ sites. [ABSTRACT FROM AUTHOR]

The Swiss Light Source (SLS) is a synchrotron radiation user facility (2000 users/year, 18 beamlines, 5000 hrs/year) in operation at Paul Scherrer Institut (PSI) since 2001. Figure 1 presents a schematic view. [ABSTRACT FROM AUTHOR]

We directly measure by femtosecond time-resolved x-ray diffraction the Eg symmetry coherent phonon excited in bismuth by a strong optical pulse. The magnitude of the Eg mode observed is 0.2 pm peak-to-peak, compared against the 2.7-pm initial displacement of the fully symmetric AIg mode. The much smaller motion of the Eg mode is a consequence of the short lifetime of the electronic states that drive the atomic motion. The experimentally measured magnitude of the Eg motion allows us to rule out a previously suggested scenario for explaining the dynamics in bismuth that relies on strong coupling between these modes. [ABSTRACT FROM AUTHOR]

We investigate the structural response of charge and orbitally ordered (CO/OO) manganites to ultrafast optical excitation using optical reflectivity and x-ray diffraction as a probe. We study a La0.42Ca0.58MnO3 (LCMO) thin film and a La0.25Pr0.375Ca0.375MnO3 (LPCMO) single crystal. For both materials we observe oscillations in the optical responses that are assigned to a coherent optical phonon generated via displacive excitation. The coherent phonon disappears either when increasing the temperature above TCo/oo or when raising the excitation fluence above a certain threshold. At low excitation fluences the amplitude and lifetime of this phonon behave similarly to the order parameter of the structural phase transition. [ABSTRACT FROM AUTHOR]

We use time-resolved optical reflectivity to study the laser stimulated dynamics in the magnetic shape memory alloy Ni2MnGa. We observe two coherent optical phonons, at 1.2 THz in the martensite phase and at 0.7 THz in the pre-martensite phase, which we interpret as a zone-folded acoustic phonon and a heavily damped amplitudon, respectively. In the martensite phase the martensitic phase transition can be induced by a fs laser pulse on a timescale of a few ps. [ABSTRACT FROM AUTHOR]

The article focuses on an experiment which investigated the ultrafast dynamics of magnetic order in a single crystal of CuO in response to strong optical excitation, using femtosecond resonant x-ray diffraction. It was found that a femtosecond laser pulse induces sudden, nonequilibfium increase in magnetic disorder. The experiment showed that long-wavelength magnetic excitation connecting the two phases limits the ultimate speed for antiferromagnetic reorientation transition in CuO.

We report on the use of grazing-incidence time-resolved x-ray diffraction to investigate the evolution of strain in natural graphite excited by femtosecond-laser pulses in the fluence range of 6-35 mJ/cm2. Strains corresponding to up to ~2.8% c-axis expansion were observed. We show that the experimental data is in good agreement with calculations based on the Thomsen strain model in conjunction with dynamical diffraction theory. Furthermore we find no evidence of nonthermal lattice expansion as reported in recent ultrafast electron-diffraction studies of laser-excited graphite conducted under comparable excitation conditions. [ABSTRACT FROM AUTHOR]

We investigate the relationship between persistent currents in multi-channel rings containing an embedded scatterer and the conductance through the same scatterer attached to leads. The case of two uncoupled channels corresponds to a Hubbard chain, for which the one-dimensional embedding method is readily generalized. Various tests are carried out to validate this new procedure, and the conductance of short one-dimensional Hubbard chains attached to perfect leads is computed for different system sizes and interaction strengths. In the case of two coupled channels the conductance can be obtained from a statistical analysis of the persistent current or by reducing the multi-channel scattering problem to several single-channel setups. [ABSTRACT FROM AUTHOR]

The timescales for structural changes in a single crystal of bismuth after excitation with an intense near-infrared laser pulse are studied with femtosecond pump-probe X-ray diffraction. Changes in the intensity and reciprocal-lattice vector of several reflections give quantitative information on the structure factor and lattice strain as a function of time, with a resolution of 200 fs. The results indicate that the majority of excess carrier energy that remains near the surface is transferred to vibrational modes on a timescale of about 10 ps, and that the resultant increase in the variance of the atomic positions at these times is consistent with the overall magnitude of lattice strain that develops. [ABSTRACT FROM AUTHOR]

X-ray absorption spectroscopy is a powerful probe of molecular structure, but it has previously been too slow to track the earliest dynamics after photoexcitation. We investigated the ultrafast formation of the lowest quintet state of aqueous iron(II) tris(bipyridine) upon excitation of the singlet metal-to-ligand-charge-transfer (¹MLCT) state by femtosecond optical pump/x-ray probe techniques based on x-ray absorption near-edge structure (XANES). By recording the intensity of a characteristic XANES feature as a function of laser pump/x-ray probe time delay, we find that the quintet state is populated in about 150 femtoseconds. The quintet state is further evidenced by its full XANES spectrum recorded at a 300-femtosecond time delay. These results resolve a long-standing issue about the population mechanism of quintet states in iron(II)-based complexes, which we identify as a simple ¹MLCT→³MLCT→5ST cascade from the initially excited state. The time scare of the ³MLCT→5ST relaxation corresponds to the period of the iron-nitrogen stretch vibration. [ABSTRACT FROM AUTHOR]

We consider one-dimensional transport through an interacting region in series with a point-like one-body scatterer. When the conductance of the interacting region is perfect, independently of the interaction strength, a nonlocal interaction effect yields a total conductance of the composed system that depends on the interaction strength and is lower than the transmission of the one-body scatterer. This qualitative nonlocal effect allows to probe the dressing cloud of an interacting system in ideal noninteracting leads. The conductance correction increases with the strength of the interaction and the reflection of the one-body scatterer (attaining relative changes >50%), and decreases with the distance between the interacting region and the one-body scatterer. Scaling laws are obtained and possible experimental realizations are suggested. [ABSTRACT FROM AUTHOR]

Abstract: The Materials Science Beamline at the Swiss Light Source (SLS) has been designed to produce hard X-rays in the photon-energy range 5–40keV, at an intermediate energy (2.4GeV) synchrotron. To this end, it employs a novel “minigap wiggler”. Important issues in the design and realization of the beamline are the high heat load, robust system design, flexibility of operation and user-friendliness. A conventional collimating-mirror/sagittally focusing double-crystal monochromator/focusing mirror optics has been chosen with approximately 1:1 symmetry. Established component designs have been used wherever possible. Three serial end-stations are served with X-rays. Besides the minigap wiggler, other novel or unusual features are: continuous “top-up” injection in the SLS storage-ring, a rotating carbon “cup” filter in the beamline front-end, angles and bending radii of the optics mirrors which are adjusted at each change in photon-energy and special experimental-station equipment including high-speed one- and two-dimensional semiconductor detectors for powder and surface diffraction and a two-dimensional “Bragg magnifier” for tomography. In this work, a comparison is made between predicted and measured beamline properties, and Appendices with useful formulae and algorithms are provided. [Copyright &y& Elsevier]

We study a method to determine the residual conductance of a correlated system by means of the ground-state properties of a large ring composed of the system itself and a long non-interacting lead. The transmission probability through the interacting region, and thus its residual conductance, is deduced from the persistent current induced by a flux threading the ring. Density Matrix Renormalization Group techniques are employed to obtain numerical results for one-dimensional systems of interacting spinless fermions. As the flux dependence of the persistent current for such a system demonstrates, the interacting system coupled to an infinite non-interacting lead behaves as a non-interacting scatterer, but with an interaction dependent elastic transmission coefficient. The scaling to large lead sizes is discussed in detail as it constitutes a crucial step in determining the conductance. Furthermore, the method, which so far had been used at half filling, is extended to arbitrary filling and also applied to disordered interacting systems, where it is found that repulsive interaction can favor transport. [ABSTRACT FROM AUTHOR]

Understanding the initial steps during ultrafast molecular reactions involving large spin state changes is a vital goal in structural dynamics research. These involve knowledge of the geometric structure of the system. Ultrafast X-ray absorption spectroscopy with 50-100 picosecond time resolution establishes the geometric structure of the short-lived (τ = 0:6 ns) high spin state. Here we focus on time-resolved X-ray absorption studies with 160-200 fs temporal resolution to monitor the structural evolution in this spin-conversion process. [ABSTRACT FROM AUTHOR]

The ultrafast dynamics of the octahedral rotation in Ca:SrTiO3 is studied by time-resolved x-ray diffraction after photoexcitation over the band gap. By monitoring the diffraction intensity of a superlattice reflection that is directly related to the structural order parameter of the soft-mode driven antiferrodistortive phase in Ca:SrTiO3, we observe an ultrafast relaxation on a 0.2 ps timescale of the rotation of the oxygen octahedron, which is found to be independent of the initial temperature despite large changes in the corresponding soft-mode frequency. A further, much smaller reduction on a slower picosecond timescale is attributed to thermal effects. Time-dependent density-functional-theory calculations show that the fast response can be ascribed to an ultrafast displacive modification of the soft-mode potential towards the normal state induced by holes created in the oxygen 2p states. [ABSTRACT FROM AUTHOR]

We use femtosecond x-ray diffraction to study the structural response of charge and orbitally ordered Pr 1−xCax MnO3 thin films across a phase transition induced by 800 nm laser pulses. By investigating the dynamics of both superlattice reflections and regular Bragg peaks, we disentangle the different structural contributions and analyze their relevant timescales. The dynamics of the structural and charge order response are qualitatively different when excited above and below a critical fluence fc . For excitations below f c the charge order and the superlattice is only partially suppressed and the ground state recovers within a few tens of nanosecond via diffusive cooling. When exciting above the critical fluence the superlattice vanishes within approximately half a picosecond followed by a change of the unit cell parameters on a 10 picoseconds timescale. At this point all memory from the symmetry breaking is lost and the recovery time increases by many order of magnitudes due to the first order character of the structural phase transition. [ABSTRACT FROM AUTHOR]

The prototypical magnetic memory shape alloy Ni2MnGa undergoes various phase transitions as a function of the temperature, pressure, and doping. In the low-temperature phases below 260 K, an incommensurate structural modulation occurs along the [110] direction which is thought to arise from the softening of a phonon mode. It is not at present clear how this phenomenon is related, if at all, to the magnetic memory effect. Here we report time-resolved measurements which track both the structural and magnetic components of the phase transition from the modulated cubic phase as it is brought into the high-symmetry phase. The results suggest that the photoinduced demagnetization modifies the Fermi surface in regions that couple strongly to the periodicity of the structural modulation through the nesting vector. The amplitude of the periodic lattice distortion, however, appears to be less affected by the demagnetization. [ABSTRACT FROM AUTHOR]

Femtosecond time-resolved x-ray diffraction is used to study a photoinduced phase transition between two charge density wave (CDW) states in 1T-TaS2, namely the nearly commensurate (NC) and the incommensurate (I) CDW states. Structural modulations associated with the NC-CDW order are found to disappear within 400 fs. The photoinduced I-CDW phase then develops through a nucleation and growth process which ends 100 ps after laser excitation. We demonstrate that the newly formed I-CDW phase is fragmented into several nanometric domains that are growing through a coarsening process. The coarsening dynamics is found to follow the universal Lifshitz-Allen-Cahn growth law, which describes the ordering kinetics in systems exhibiting a nonconservative order parameter. [ABSTRACT FROM AUTHOR]

We use resonant elastic and inelastic x-ray scattering at the Ir-L3 edge to study the doping-dependent magnetic order, magnetic excitations, and spin-orbit excitons in the electron-doped bilayer iridate (Sr1-xLax)3Ir2O7 (0≤x≤0.065). With increasing doping x, the three-dimensional long range antiferromagnetic order is gradually suppressed and evolves into a three-dimensional short range order across the insulator-to-metal transition from x=0 to 0.05, followed by a transition to two-dimensional short range order between x=0.05 and 0.065. Because of the interactions between the Jeff=½ pseudospins and the emergent itinerant electrons, magnetic excitations undergo damping, anisotropic softening, and gap collapse, accompanied by weakly doping-dependent spin-orbit excitons. Therefore, we conclude that electron doping suppresses the magnetic anisotropy and interlayer couplings and drives (Sr1-xLax)3Ir2O7 into a correlated metallic state with two-dimensional short range antiferromagnetic order. Strong antiferromagnetic fluctuations of the Jeff=½ moments persist deep in this correlated metallic state, with the magnon gap strongly suppressed. [ABSTRACT FROM AUTHOR]