We present a fully quantal version of the Langevin model for the total rate of exoergic ion-molecule reactions or inelastic processes. The model, which is derived from a rigorous multichannel quantum-defect formulation of bimolecular processes, agrees with the classical Langevin model at sufficiently high temperatures. It also gives an analytic description of ion-molecule reactions and inelasti...

What do we mean by a “supramolecular control” of a photochemical reaction? To answer this question, we will integrate the fundamental and familiar paradigm of molecular organic photochemistry (e.g., the R + hν → ∗R → I → P sequence) with the paradigm of supramolecular organic chemistry (guest@host chemistry). It will be convenient to consider supramolecular control of unimolecular and bimolecul...

We show that a DNA-based chemical system can be constructed such that it closely approximates the dynamic behavior of an arbitrary system of coupled chemical reactions. Using strand displacement reactions as a primitive we explicitly construct reaction cascades with effectively unimolecular and bimolecular kinetics. Our construction allows for individual reactions to be coupled in arbitrary way...

Ultrafast laser spectroscopy has extended reaction-dynamic studies into the dcosecond and femtosecond time domain. allowing for experimintal observations of transitory fragments that occur during collision or half-collision. This ability to observe molecular reactions allows real-time viewing of energy redistributions, measurements of state-to-state rates, and tests of microscopic statistical t...

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The results of two time-resolved experiments using femtosecond laser pulses are presented. In the first, molecular photoinduced detachment of I2 from methylene iodide is studied. The progress of the reaction is monitored by selective detection of fluorescence from the iodine product; molecular dynamics are probed by depletion of the fluorescent state. Pump-probe spectroscopy of the halogen moie...

A theoretical analysis of the recent femtosecond photoassociation spectroscopy ~FPAS! experiment on mercury @U. Marvet and M. Dantus, Chem. Phys. Lett. 245, 393 ~1995!# is presented. It is shown that when a thermal distribution of diatom collision pairs is excited from a free to a bound electronic state on a time scale shorter than molecular vibration, an ensemble of coherent wave packets is pr...