Ultrafast spectroscopy of the uranium(IV) and thorium(IV) bis(ketimide) complexes (C5Me5)2An[-N=C(Ph)(CH2Ph)]2 (An = Th, U)

Ultrafast pump-probe spectroscopic studies have been performed on (C 5Me 5) 2U[- N=C(Ph)(CH 2Ph)] 2 and (C 5Me 5) 2Th[- N=C(Ph)(CH 2Ph)] 2 including, for the uranium complex, the first direct measurement of dynamics of electronic deactivation within a 5f-electron manifold. Evidence has been found for strong coupling between the electronic ground state and the f-electron manifold which dominates the dynamics of the excited states of the bis(ketimide) uranium complex. These also demonstrate strong singlet-f manifold coupling, which assists in the deactivation of the photoexcited state of the uranium complex, and provide information on intersystem crossing and internal conversion processes in both complexes.     

Coupled charge-spin dynamics of the magnetoresistive pyrochlore TI2Mn2O7 probed using ultrafast midinfrared spectroscopy

Optical-pump midinfrared probe spectroscopy is used to investigate coupled charge-spin dynamics in the magnetoresistive pyrochlore TI(2)Mn(2)O(7). We find that the temporal persistence of the photoexcited carrier density is strongly influenced by spin disorder above and below the ferromagnetic Curie temperature. Our results are consistent with a picture whereby spin disorder leads to spatial segregation of the initially excited Tl 6s-O 2p electron-hole pairs, effectively reducing the probability for recombination. This further implies that colossal magnetoresistance in these materials may be driven primarily by Mn t(2g) spin disorder.     

Self-starting mode locking in a Cr:forsterite laser by use of non-epitaxially-grown semiconductor-doped silica films

We demonstrate RF sputtered, non-epitaxially-grown semiconductor nanocrystallite-doped silica films for mode locking a Cr:forsterite laser. We controlled the size and the optical properties of the nanocrystallites by varying the ratio of InAs to SiO(2) during fabrication. Femtosecond pump-probe measurements were performed to characterize the nonlinear optical properties of these films, revealing their lower saturation fluences. Using the InAs-doped silica films as saturable absorbers permitted self-starting Kerr-lens mode locking (KLM), generating pulses of 25-fs duration with 91-nm spectral bandwidth at 1.3 microm . We also describe saturable-absorber mode-locked operation without KLM and investigate its dependence on intracavity dispersion.     

Magnetoelectric effect in cobalt ferrite-barium titanate composites and their electrical properties

CoFe₂O₄-BaTiO₃ composites were prepared using conventional ceramic double sintering process with various compositions. Presence of two phases in the composites was confirmed using X-ray diffraction. The dc resistivity and thermoemf as a function of temperature in the temperature range 300 K to 600 K were measured. Variation of dielectric constant (ɛ′) with frequency in the range 100 Hz to 1 MHz and also with temperature at a fixed frequency of 1 kHz was studied. The ac conductivity was derived from dielectric constant (ɛ′) and loss tangent (tan δ). The nature of conduction is discussed on the basis of small polaron hopping model. The static value of magnetoelectric conversion factor has been studied as a function of magnetic field.     

Enhanced photosusceptibility near Tc for the light-induced insulator-to-metal phase transition in vanadium dioxide

We use optical-pump terahertz-probe spectroscopy to investigate the near-threshold behavior of the photoinduced insulator-to-metal (IM) transition in vanadium dioxide thin films. Upon approaching Tc a reduction in the fluence required to drive the IM transition is observed, consistent with a softening of the insulating state due to an increasing metallic volume fraction (below the percolation limit). This phase coexistence facilitates the growth of a homogeneous metallic conducting phase following superheating via photoexcitation. A simple dynamic model using Bruggeman effective medium theory describes the observed initial condition sensitivity.     

The onset of coulomb explosions in polyatomic molecules

With the development of high intensity femtosecond lasers, the ionisation and dissociation dynamics of molecules has become an area of considerable interest. Using the technique of femtosecond laser mass spectrometry (FLMS), the molecules carbon disulphide, pyrimidine, toluene, cyclohexanone and benzaldehyde are studied with pulse widths of 50 fs in the near infrared (IR) wavelength region (790 nm). Results are presented and contrasted for laser beam intensities around 10(15) and 10(16) W cm(-2). For the lower intensities, the mass spectra yield dominant singly charged parent ions. Additionally, the appearance of doubly charged parent ions is evident for carbon disulphide, toluene and benzaldehyde with envelopes of doubly charged satellite species existing in these local regions. Carbon disulphide also reveals a small triply charged component. Such atomic-like features are thought to be a strong fingerprint of FLMS at these intensities. However, upon increasing the laser intensity to approximately 10(16) W cm(-2), parent ion dominance decreases and the appearance of multiply charged atomic species occurs, particularly carbon. This phenomenon has been attributed to Coulomb explosions in which the fast absorption of many photons may produce transient highly ionised parent species which can subsequently blow apart. Copyright 1999 John Wiley & Sons, Ltd.