Probing nucleobase photoprotection with soft x-rays

Nucleobases absorb strongly in the ultraviolet region, leading to molecular excitation into reactive states. The molecules avoid the photoreactions by funnelling the electronic energy into less reactive states on an ultrafast timescale via non-Born-Oppenheimer dynamics. Current theory on the nucleobase thymine discusses two conflicting pathways for the photoprotective dynamics. We present our first results of our free electron laser based UV-pump soft x-ray-probe study of the photoprotection mechanism of thymine. We use the high spatial sensitivity of the Auger electrons emitted after the soft x-ray pulse induced core ionization. Our transient spetra show two timescales on the order of 200 fs and 5 ps, in agreement with previous (all UV) ultrafast experiments. The timescales appear at different Auger kinetic energies which will help us to decipher the molecular dynamics

Strongly Dispersive Transient Bragg Grating for High Harmonics

We create a transient Bragg grating in a high harmonic generation medium using two counterpropagating pulses. The Bragg grating disperses the harmonics in angle and can diffract a large bandwidth with temporal resolution limited only by the source size

Using behavior-analytic implicit tests to assess sexual interests among normal and sex-offender populations

The development of implicit tests for measuring biases and behavioral predispositions is a recent development within psychology. While such tests are usually researched within a social-cognitive paradigm, behavioral researchers have also begun to view these tests as potential tests of conditioning histories, including in the sexual domain. The objective of this paper is to illustrate the utility of a behavioral approach to implicit testing and means by which implicit tests can be built to the standards of behavioral psychologists. Research findings illustrating the short history of implicit testing within the experimental analysis of behavior are reviewed. Relevant parallel and overlapping research findings from the field of social cognition and on the Implicit Association Test are also outlined. New preliminary data obtained with both normal and sex offender populations are described in order to illustrate how behavior-analytically conceived implicit tests may have potential as investigative tools for assessing histories of sexual arousal conditioning and derived stimulus associations. It is concluded that popular implicit tests are likely sensitive to conditioned and derived stimulus associations in the history of the test-taker rather than 'unconscious cognitions', per se

Femtosecond X-ray-induced explosion of C60 at extreme intensity

Understanding molecular femtosecond dynamics under intense X-ray exposure is critical to progress in biomolecular imaging and matter under extreme conditions. Imaging viruses and proteins at an atomic spatial scale and on the time scale of atomic motion requires rigorous, quantitative understanding of dynamical effects of intense X-ray exposure. Here we present an experimental and theoretical study of C60 molecules interacting with intense X-ray pulses from a free-electron laser, revealing the influence of processes not previously reported. Our work illustrates the successful use of classical mechanics to describe all moving particles in C60, an approach that scales well to larger systems, for example, biomolecules. Comparisons of the model with experimental data on C60 ion fragmentation show excellent agreement under a variety of laser conditions. The results indicate that this modelling is applicable for X-ray interactions with any extended system, even at higher X-ray dose rates expected with future light sources

Experimental strategies for optical pump - Soft x-ray probe experiments at the LCLS

Free electron laser (FEL) based x-ray sources show great promise for use in ultrafast molecular studies due to the short pulse durations and site/element sensitivity in this spectral range. However, the self amplified spontaneous emission (SASE) process mostly used in FELs is intrinsically noisy resulting in highly fluctuating beam parameters. Additionally timing synchronization of optical and FEL sources adds delay jitter in pump-probe experiments. We show how we mitigate the effects of source noise for the case of ultrafast molecular spectroscopy of the nucleobase thymine. Using binning and resorting techniques allows us to increase time and spectral resolution. In addition, choosing observables independent of noisy beam parameters enhances the signal fidelity

Attosecond Molecular Spectroscopies with XUV Harmonic Radiation

When irradiated by an intense pulse of an infrared (IR) laser, molecules emit a coherent radiation composed of a frequency comb of harmonics of the pump laser frequency, ranging from ultraviolet (UV) up to soft X-rays. These harmonics are emitted during extremely short time windows, within the attosecond range. The properties of harmonic emission are of much interest when applied to issues of relevance to AMOP (Atomic, Molecular and Optical Physics) and they have opened a new domain of investigation in the emerging field of attophysics. In the spectral domain, analyzing high harmonic spectra provides original information on the electronic structure of the outer orbitals that are active in the generation process. In the time domain, the use of attosecond pulses of Extreme Ultra-Violet (XUV) harmonics within a pump-probe scheme opens unique opportunities to develop a new time-resolved spectroscopy of transient excited molecular states. In this review, we shall report on recent advances in the field and we shall address several issues of interest with the objective to go beyond the "proof-of-principle" demonstrations that have been reported so far. © Springer-Verlag Berlin Heidelberg 2013