X-ray and optical wave mixing.

Light-matter interactions are ubiquitous, and underpin a wide range of basic research fields and applied technologies. Although optical interactions have been intensively studied, their microscopic details are often poorly understood and have so far not been directly measurable. X-ray and optical wave mixing was proposed nearly half a century ago as an atomic-scale probe of optical interactions but has not yet been observed owing to a lack of sufficiently intense X-ray sources. Here we use an X-ray laser to demonstrate X-ray and optical sum-frequency generation. The underlying nonlinearity is a reciprocal-space probe of the optically induced charges and associated microscopic fields that arise in an illuminated material. To within the experimental errors, the measured efficiency is consistent with first-principles calculations of microscopic optical polarization in diamond. The ability to probe optical interactions on the atomic scale offers new opportunities in both basic and applied areas of science.

X-rays only when you want them: optimized pump-probe experiments using pseudo-single-bunch operation.

Laser pump-X-ray probe experiments require control over the X-ray pulse pattern and timing. Here, the first use of pseudo-single-bunch mode at the Advanced Light Source in picosecond time-resolved X-ray absorption experiments on solutions and solids is reported. In this mode the X-ray repetition rate is fully adjustable from single shot to 500 kHz, allowing it to be matched to typical laser excitation pulse rates. Suppressing undesired X-ray pulses considerably reduces detector noise and improves signal to noise in time-resolved experiments. In addition, dose-induced sample damage is considerably reduced, easing experimental setup and allowing the investigation of less robust samples. Single-shot X-ray exposures of a streak camera detector using a conventional non-gated charge-coupled device (CCD) camera are also demonstrated.

Thin water film formation on metal oxide crystal surfaces.

Reactions taking place at hydrated metal oxide surfaces are of considerable environmental and technological importance. Surface-sensitive X-ray methods can provide structural and chemical information on stable interfacial species, but it is challenging to perform in situ studies of reaction kinetics in the presence of water. We have implemented a new approach to creating a micrometer-scale water film on a metal oxide surface by combining liquid and gas jets on a spinning crystal. The water films are stable indefinitely and sufficiently thin to allow grazing incidence X-ray reflectivity and spectroscopy measurements. The approach will enable studies of a wide range of surface reactions and is compatible with interfacial optical-pump/X-ray-probe studies.

Ultrafast evolution and transient phases of a prototype out-of-equilibrium Mott-Hubbard material.

The study of photoexcited strongly correlated materials is attracting growing interest since their rich phase diagram often translates into an equally rich out-of-equilibrium behaviour. With femtosecond optical pulses, electronic and lattice degrees of freedom can be transiently decoupled, giving the opportunity of stabilizing new states inaccessible by quasi-adiabatic pathways. Here we show that the prototype Mott-Hubbard material V2O3 presents a transient non-thermal phase developing immediately after ultrafast photoexcitation and lasting few picoseconds. For both the insulating and the metallic phase, the formation of the transient configuration is triggered by the excitation of electrons into the bonding a1g orbital, and is then stabilized by a lattice distortion characterized by a hardening of the A1g coherent phonon, in stark contrast with the softening observed upon heating. Our results show the importance of selective electron-lattice interplay for the ultrafast control of material parameters, and are relevant for the optical manipulation of strongly correlated systems.

The effect of buffer osmolality on the survival of cat (Felis catus ) spermatozoa at 5 degrees C.

Cat semen was diluted at 37 degrees C in Tes-Tris buffer (TesT), pH 7.5, at osmolalities ranging from 195 to 390 m0sm/kg, cooled to 5 degrees C over 90 minutes and stored for 24 hours at that temperature. Motility and percentage of spermatozoa staining with a supravital stain were estimated before cooling, after cooling and after storage for 24 hours. The osmolality of undiluted pooled ejaculates from five animals was measured, and also that of different diluents (citrate with phosphate buffer, lactose and TesT-egg yolk) used for cat semen. The osmolality measurements of cat semen suggested an osmolality of less than 320 m0sm/kg at ejaculation, increasing with time after ejaculation. Varying the egg yolk concentrations (2% to 20%) did not affect the osmolality of TesT diluent. Diluent osmolalities of less than 292 m0sm/kg were found to reduce sperm motility significantly (P <0.001 ) although there was no significant increase in the percentage of cells staining with a supravital stain, while those greater than 325 m0sm/kg increased the variation of response among animals. Cooling and storage significantly reduced motility (P <0.01 to P <0.001 ) and increased the number of stained cells (P <0.001 ). There were significant differences between ejaculates (P <0.01 ) and significant interactions between osmolality and cooling/storage (P <0.05 to P <0.001 ). The best overall results were seen with a TesT diluent of 292 to 325 m0sm/kg which supported good motility for at least 24 hours.

Glass-like recovery of antiferromagnetic spin ordering in a photo-excited manganite Pr0.7Ca0.3MnO3.

Electronic orderings of charges, orbitals and spins are observed in many strongly correlated electron materials, and revealing their dynamics is a critical step toward undertsanding the underlying physics of important emergent phenomena. Here we use time-resolved resonant soft x-ray scattering spectroscopy to probe the dynamics of antiferromagnetic spin ordering in the manganite Pr0.7Ca0.3MnO3 following ultrafast photo-exitation. Our studies reveal a glass-like recovery of the spin ordering and a crossover in the dimensionality of the restoring interaction from quasi-1D at low pump fluence to 3D at high pump fluence. This behavior arises from the metastable state created by photo-excitation, a state characterized by spin disordered metallic droplets within the larger charge- and spin-ordered insulating domains. Comparison with time-resolved resistivity measurements suggests that the collapse of spin ordering is correlated with the insulator-to-metal transition, but the recovery of the insulating phase does not depend on the re-establishment of the spin ordering.

Band-selective measurements of electron dynamics in VO2 using femtosecond near-edge x-ray absorption.

We report on the first demonstration of femtosecond x-ray absorption spectroscopy, made uniquely possible by the use of broadly tunable bending-magnet radiation from "laser-sliced" electron bunches within a synchrotron storage ring. We measure the femtosecond electronic rearrangements that occur during the photoinduced insulator-metal phase transition in VO2. Symmetry- and element-specific x-ray absorption from V2p and O1s core levels (near 500 eV) separately measures the filling dynamics of differently hybridized V3d-O2p electronic bands near the Fermi level.

Vaginal anatomy of the domestic cat (Felis catus) in relation to copulation and artificial insemination.

In the course of an investigation of artificial insemination (AI) in the domestic cat, the site of deposition of the semen during vulval insemination was questioned. A limited study was carried out to ascertain both the anatomy and distensibility of the vagina and urogenital sinus, and the location of the cervix in relation to the vulva. In live restrained female cats a 4 mm diameter Teflon probe could not be inserted more than 20 mm, and elicited a cry similar to the copulatory vocalization when the resistance was encountered. However, a 1 mm diameter ball-tipped needle was passed to a depth of 40 mm. To confirm these observations, four adult female domestic cats were dissected. The cervix was located approximately 45 mm cranial to the vulva. The urogenital sinus narrowed approximately 17.5 mm from the vulva, preventing the passage of a 4 mm probe, and led to a constricted vagina, which permitted the passage of a 1 mm diameter probe to the depth of the cervix. A radiological investigation of a single anaesthetized cat supported these results. The erect penis of the adult male was measured during sexual arousal in five animals; the mean length and width (+/- SD) was 21.2 +/- 2.2 mm and 5.1 +/- 0.5 mm, respectively. These observations lead us to conclude that the stimulus for vocalization during natural mating is distention of the posterior vagina, where semen is probably deposited. The site of semen deposition is uncertain in several accounts of artificial insemination, as the passage of the insemination device depends on its diameter.

Observations on variability in LH release and fertility during oestrus in the domestic cat (Felis catus).

Hormonal changes, behaviour, ovulation and fertility were examined in response to coitus at two different times during oestrus in the female domestic cat housed in conditions of natural light (N = 13). On Day 2 or Day 4/5 of oestrus females were allowed 1 copulation in 15 min (single matings) or 2-3 copulations in 30 min (multiple matings). Plasma LH, oestradiol-17 beta and progesterone concentrations during the 24-h period after coitus were measured by radioimmunoassay; ovulation was assumed to have occurred if progesterone values were elevated 7-30 days after coitus. With the exception of 2 out of 3 animals receiving single matings on Day 2 of oestrus, all animals showed subsequent elevated progesterone values. Females receiving multiple matings had significantly greater releases of LH as measured by the area under the curve than those receiving single matings. There was significantly greater variability in the LH response of queens on Day 2 of oestrus compared to those on Day 4/5 for peak values and area under the curve; the only failure in release of LH was in queens on Day 2. Oestradiol levels did not differ significantly between Day 2 and Day 4/5 of oestrus. Progesterone values remained less than 1 ng/ml for 24 h after coitus. Both LH peak values and area under the curve were significantly greater for animals that became pregnant. There were also significant differences in coital behaviour between queens on Day 2 and those on Day 4/5 of oestrus.(ABSTRACT TRUNCATED AT 250 WORDS)

Metal-insulator transitions in an expanding metallic fluid: particle formation kinetics.

Core-level photoemission spectroscopy provides a local probe of expansion dynamics and associated transient chemical properties as a highly pressurized, metallic fluid expands into vacuum following impulsive heating of a semiconductor by an intense, ultrashort laser pulse. Transient photoemission peak shifts reveal that metal-insulator transitions occur rapidly following laser heating. These experiments probe constituents species and solidification kinetics occurring in the early moments of material ejection and provide insight into how particles arise in the current laser ablation regime.