X-Ray sum frequency generation; direct imaging of ultrafast electron dynamics

X-ray diffraction from molecules in the ground state produces an image of their charge density, and time-resolved X-ray diffraction can thus monitor the motion of the nuclei. However, the density change of excited valence electrons upon optical excitation can barely be monitored with regular diffraction techniques due to the overwhelming background contribution of the core electrons. We present a nonlinear X-ray technique made possible by novel free electron laser sources, which provides a spatial electron density image of valence electron excitations. The technique, sum frequency generation carried out with a visible pump and a broadband X-ray diffraction pulse, yields snapshots of the transition charge densities, which represent the electron density variations upon optical excitation. The technique is illustrated by ab initio simulations of transition charge density imaging for the optically induced electronic dynamics in a donor/acceptor substituted stilbene

Monitoring Nonadiabatic Electron-Nuclear Dynamics in Molecules by Attosecond Streaking of Photoelectrons

Streaking of photoelectrons has long been used for the temporal characterization of attosecond extreme ultraviolet pulses. When the time-resolved photoelectrons originate from a coherent superposition of electronic states, they carry an additional phase information, which can be retrieved by the streaking technique. In this contribution we extend the streaking formalism to include coupled electron and nuclear dynamics in molecules as well as initial coherences and demonstrate how it offers a novel tool to monitor non-adiabatic dynamics as it occurs in the vicinity of conical intersections and avoided crossings. Streaking can enhance the time resolution and provide direct signatures of electronic coherences, which affect many primary photochemical and biological events

Cooperation, collective action, and the archeology of large-scale societies

Archeologists investigating the emergence of large-scale societies in the past have renewed interest in examining the dynamics of cooperation as a means of understanding societal change and organizational variability within human groups over time. Unlike earlier approaches to these issues, which used models designated voluntaristic or managerial, contemporary research articulates more explicitly with frameworks for cooperation and collective action used in other fields, thereby facilitating empirical testing through better definition of the costs, benefits, and social mechanisms associated with success or failure in coordinated group action. Current scholarship is nevertheless bifurcated along lines of epistemology and scale, which is understandable but problematic for forging a broader, more transdisciplinary field of cooperation studies. Here, we point to some areas of potential overlap by reviewing archeological research that places the dynamics of social cooperation and competition in the foreground of the emergence of large-scale societies, which we define as those having larger populations, greater concentrations of political power, and higher degrees of social inequality. We focus on key issues involving the communal-resource management of subsistence and other economic goods, as well as the revenue flows that undergird political institutions. Drawing on archeological cases from across the globe, with greater detail from our area of expertise in Mesoamerica, we offer suggestions for strengthening analytical methods and generating more transdisciplinary research programs that address human societies across scalar and temporal spectra

Optical pulse-shaping for internal cooling of molecules

We consider the use of pulse-shaped broadband femtosecond lasers to optically cool rotational and vibrational degrees of freedom of molecules. Since this approach relies on cooling rotational and vibrational quanta by exciting an electronic transition, it is most easily applicable to molecules with similar ground and excited potential energy surfaces, such that the vibrational state is usually unchanged during electronic relaxation. Compared with schemes that cool rotations by exciting vibrations, this approach achieves internal cooling on the orders-of- magnitude faster electronic decay timescale and is potentially applicable to apolar molecules. For AlH+, a candidate species, a rate-equation simulation indicates that rovibrational equilibrium should be achievable in 8 \mu s. In addition, we report laboratory demonstration of optical pulse shaping with sufficient resolution and power for rotational cooling of AlH+

Averages of b-hadron Properties at the End of 2005

This article reports world averages for measurements on b-hadron properties obtained by the Heavy Flavor Averaging Group (HFAG) using the available results as of at the end of 2005. In the averaging, the input parameters used in the various analyses are adjusted (rescaled) to common values, and all known correlations are taken into account. The averages include lifetimes, neutral meson mixing parameters, parameters of semileptonic decays, branching fractions of B meson decays to final states with open charm, charmonium and no charm, and measurements related to CP asymmetries

Antarctic climate and ice-sheet configuration during the early Pliocene interglacial at 4.23Ma

The geometry of Antarctic ice sheets during warm periods of the geological past is difficult to determine from geological evidence, but is important to know because such reconstructions enable a more complete understanding of how the ice-sheet system responds to changes in climate. Here we investigate how Antarctica evolved under orbital and greenhouse gas conditions representative of an interglacial in the early Pliocene at 4.23Ma, when Southern Hemisphere insolation reached a maximum. Using offline-coupled climate and ice-sheet models, together with a new synthesis of high-latitude palaeoenvironmental proxy data to define a likely climate envelope, we simulate a range of ice-sheet geometries and calculate their likely contribution to sea level. In addition, we use these simulations to investigate the processes by which the West and East Antarctic ice sheets respond to environmental forcings and the timescales over which these behaviours manifest. We conclude that the Antarctic ice sheet contributed 8.6±2.8m to global sea level at this time, under an atmospheric CO2 concentration identical to present (400ppm). Warmer-than-present ocean temperatures led to the collapse of West Antarctica over centuries, whereas higher air temperatures initiated surface melting in parts of East Antarctica that over one to two millennia led to lowering of the ice-sheet surface, flotation of grounded margins in some areas, and retreat of the ice sheet into the Wilkes Subglacial Basin. The results show that regional variations in climate, ice-sheet geometry, and topography produce long-term sea-level contributions that are non-linear with respect to the applied forcings, and which under certain conditions exhibit threshold behaviour associated with behavioural tipping points