Pulse-Bandwidth Dependence of Coherent Phase Control of Resonance-Mediated (2+1) Three-Photon Absorption

We study in detail coherent phase control of femtosecond resonance-mediated (2+1) three-photon absorption and its dependence on the spectral bandwidth of the excitation pulse. The regime is the weak-field regime of third perturbative order. The corresponding interference mechanism involves a group of three-photon excitation pathways that are on resonance with the intermediate state and a group of three-photon excitation pathways that are near resonant with it. The model system of the study is atomic sodium (Na), for which experimental and numerical-theoretical results are obtained. Prominent among the results is our finding that with simple proper pulse shaping an increase in the excitation bandwidth leads to a corresponding increase in the enhancement of the three-photon absorption over the absorption induced by the (unshaped) transform-limited pulse. For example, here, a 40-nm bandwidth leads to an order-of-magnitude enhancement over the transform-limited absorption.Comment: 23 pages, 5 figure

Coherent ultrafast lattice-directed reaction dynamics of triiodide anion photodissociation

Solid-state reactions are influenced by the spatial arrangement of the reactants and the electrostatic environment of the lattice, which may enable lattice-directed chemical dynamics. Unlike the caging imposed by an inert matrix, an active lattice participates in the reaction, however, little evidence of such lattice participation has been gathered on ultrafast timescales due to the irreversibility of solid-state chemical systems. Here, by lowering the temperature to 80 K, we have been able to study the dissociative photochemistry of the triiodide anion (I₃−) in single-crystal tetra-n-butylammonium triiodide using broadband transient absorption spectroscopy. We identified the coherently formed tetraiodide radical anion (I₄•−) as a reaction intermediate. Its delayed appearance after that of the primary photoproduct, diiodide radical I₂•−, indicates that I₄•− was formed via a secondary reaction between a dissociated iodine radical (I^•) and an adjacent I₃−. This chemistry occurs as a result of the intermolecular interaction determined by the crystalline arrangement and is in stark contrast with previous solution studies

Team Dynamics Theory: Nomological network among cohesion, team mental models, coordination, and collective efficacy

I put forth a theoretical framework, namely Team Dynamics Theory (TDT), to address the need for a parsimonious yet integrated, explanatory and systemic view of team dynamics. In TDT, I integrate team processes and outputs and explain their relationships within a systemic view of team dynamics. Specifically, I propose a generative nomological network linking cohesion, team mental models, coordination, collective efficacy, and team outcomes. From this nomological conceptualization, I illustrate how myriad alternative models can be derived to account for variance in different working teams, each comprised of unique members, and embedded in singular contexts. I outline TDT’s applied implications for team development, the enhancement of team functioning, and the profiling of team resilience. I conclude by discussing how TDT’s ontological and nomological propositions can be tested through various theoretical inquiries, methodological approaches, and intervention-based studies

Dependency network and node influence : application to the study of financial markets

Much effort has been devoted to assess the importance of nodes in complex networks. Examples of commonly used measures of node importance include node degree, node centrality and node vulnerability score (the effect of the node deletion on the network efficiency). Here we present a new approach to compute and investigate the mutual dependencies between network nodes from the matrices of node–node correlations. The dependency network approach provides a new system level analysis of the activity and topology of directed networks. The approach extracts topological relations between the networks nodes (when the network structure is analyzed), and provides an important step towards inference of causal activity relations between the network nodes (when analyzing the network activity). The resulting dependency networks are a new class of correlation-based networks, and are capable of uncovering hidden information on the structure of the network. Here, we present a review of the new approach, and an example of its application to financial markets. We apply the methodology to the daily closing prices of all Dow Jones Industrial Average (DJIA) index components for the period 1939–2010. Investigating the structure and dynamics of the dependency network across time, we find fingerprints of past financial crises, illustrating the importance of this methodology

Simplified setup for high-resolution spectroscopy that uses ultrashort pulses

Includes bibliographical references (page 363).Using a broadband femtosecond laser and a simple optical setup, we demonstrate narrow-bandwidth tunable excitation of vibrational modes in CCl4 and CHBr3 liquids. The resolution obtained is 80 times higher than the laser bandwidth. A pair of time-shifted, linearly chirped pulses is created by use of a high-order dispersion-compensated prism-interferometer setup. We use this pulse pair to selectively excite Raman active transitions. Our setup represents a significant simplification with improved resolution, of previous approaches to the use of ultrashort pulses for chemically selective spectroscopy

Photochemistry: Caught in the act

Femtochemistry, the real-time study of reactions on a timescale that captures the molecular and atomic activity involved, has traditionally been performed in the gas or liquid phase. It has now been extended to the solid state in a study that highlights how a controlled reaction environment can place steric constraints on the motions of photoproducts