Dynamic Tilting of Ferroelectric Domain Walls Caused by Optically Induced Electronic Screening.

Optical excitation perturbs the balance of phenomena selecting the tilt orientation of domain walls within ferroelectric thin films. The high carrier density induced in a low-strain BaTiO_{3} thin film by an above-band-gap ultrafast optical pulse changes the tilt angle that 90° a/c domain walls form with respect to the substrate-film interface. The dynamics of the changes are apparent in time-resolved synchrotron x-ray scattering studies of the domain diffuse scattering.

Micro-focused MHz pink beam for time-resolved X-ray emission spectroscopy.

The full radiation from the first harmonic of a synchrotron undulator (between 5 and 12 keV) at the Advanced Photon Source is microfocused using a stack of beryllium compound refractive lenses onto a fast-moving liquid jet and overlapped with a high-repetition-rate optical laser. This micro-focused geometry is used to perform efficient nonresonant X-ray emission spectroscopy on transient species using a dispersive spectrometer geometry. The overall usable flux achieved on target is above 10 photons s at 8 keV, enabling photoexcited systems in the liquid phase to be tracked with time resolutions from tens of picoseconds to microseconds, and using the full emission spectrum, including the weak valence-to-core signal that is sensitive to chemically relevant electronic properties.

Nanosecond Optically Induced Phase Transformation in Compressively Strained BiFeO_{3} on LaAlO_{3}.

Above-band-gap optical illumination of compressively strained BiFeO_{3} induces a transient reversible transformation from a state of coexisting tilted tetragonal-like and rhombohedral-like phases to an untilted tetragonal-like phase. Time-resolved synchrotron x-ray diffraction reveals that the transformation is induced by an ultrafast optically induced lattice expansion that shifts the relative free energies of the tetragonal-like and rhombohedral-like phases. The transformation proceeds at interfaces between regions of the tetragonal-like phase and regions of a mixture of tilted phases, consistent with the motion of a phase boundary.

Simultaneous scanning near-field optical and X-ray diffraction microscopy for correlative nanoscale structure-property characterization.

A multimodal imaging instrument has been developed that integrates scanning near-field optical microscopy with nanofocused synchrotron X-ray diffraction imaging. The instrument allows for the simultaneous nanoscale characterization of electronic/near-field optical properties of materials together with their crystallographic structure, facilitating the investigation of local structure-property relationships. The design, implementation and operating procedures of this instrument are reported.

Tunable spin-state bistability in a spin crossover molecular complex.

The spin crossover (SCO) transitions at both the surface and over the entire volume of the [Fe{HB(pz)}(bipy)] polycrystalline films on AlO substrates have been studied, where pz  =  pyrazol-1-yl and bipy  =  2,2'-bipyridine. For [Fe{HB(pz)}(bipy)] films of hundreds of nm thick, magnetometry and x-ray absorption spectroscopy measurements show thermal hysteresis in the SCO transition with temperature, although the transition in bulk [Fe{HB(pz)}(bipy)] occurs in a non-hysteretic fashion at 157 K. While the size of the crystallites in those films are similar, the hysteresis becomes more prominent in thinner films, indicating a significant effect of the [Fe{HB(pz)}(bipy)]/AlO interface.

A color x-ray camera for 2-6 keV using a mass produced back illuminated complementary metal oxide semiconductor sensor.

There are several reports in the scientific literature of the use of mass-produced charge coupled device or complementary metal oxide semiconductor (CMOS) sensors as x-ray detectors that combine high spatial resolution with significant energy resolution. Exploiting a relatively new especially favorable ambient-temperature back-illuminated CMOS sensor, we report the development of a spectroscopic x-ray camera having particularly impressive performance for 2-6 keV photons. This instrument has several beneficial characteristics for advanced x-ray spectroscopy studies in the laboratory, at synchrotron light sources, at x-ray free electron lasers, or when using pulsed x-ray sources such as for laser plasma physics research.

X-ray and optical pulse interactions in GaAs.

Absorption of hard x-rays in GaAs creates excitations that can dramatically alter the propagation of optical laser pulses with photon energies near the bandgap. Measurements of optical transmission through a thin crystalline wafer of GaAs after absorption of an intense x-ray synchrotron pulse demonstrate how x-ray induced optical transparency depends on the recombination of excited conduction band electrons and valence band holes via Auger, spontaneous emission, and especially stimulated emission processes. The x-ray induced band fluorescence spectrum also reveals amplified spontaneous emission at the high x-ray fluences used, confirming the importance of stimulated emission.

Laser-induced electron diffraction for probing rare gas atoms.

Recently, using midinfrared laser-induced electron diffraction (LIED), snapshots of a vibrating diatomic molecule on a femtosecond time scale have been captured [C.I. Blaga et al.

Imaging ultrafast molecular dynamics with laser-induced electron diffraction.

Establishing the structure of molecules and solids has always had an essential role in physics, chemistry and biology. The methods of choice are X-ray and electron diffraction, which are routinely used to determine atomic positions with sub-ångström spatial resolution. Although both methods are currently limited to probing dynamics on timescales longer than a picosecond, the recent development of femtosecond sources of X-ray pulses and electron beams suggests that they might soon be capable of taking ultrafast snapshots of biological molecules and condensed-phase systems undergoing structural changes.

Redshift in the optical absorption of ZnO single crystals in the presence of an intense midinfrared laser field.

We report time-resolved electroabsorption of a weak probe in a 500 μm thick zinc-oxide crystal in the presence of a strong midinfrared pump in the tunneling limit. We observe a substantial redshift in the absorption edge that scales with the cube root of intensity up to 1 TW/cm(2) (0.38 eV cm(2/3) TW(-1/3)) after which it increases more slowly to 0.

An investigation of harmonic generation in liquid media with a mid-infrared laser.

We present a harmonic generation experiment using liquid H(2)O and D(2)O interrogated by a mid-infrared, 3.66 mum, laser at a maximum intensity of 8x10(13) W/cm(2). The unique aspects of the experiment include the long wavelength and short (9 cycle-110 fs) pulse duration of the laser as well as the near-resonant excitation of the H(2)O and D(2)O vibrational modes.