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Reactive Intermediates in Condensed Phase:
Radiation and Photochemistry

The fundamental mechanisms of internal energy conversion following excitation are studied by probing the dynamics and structural changes that unravel electronic structure and mechanisms of relaxation of transient species in the condensed phase. In order to control chemical reactions, it is necessary to understand the mechanisms of formation and relaxation of chemically active species. Knowledge of the initial events in condensed phase well before the transient species have relaxed is necessary because the fate of transient species, such as electron-hole pairs, and the subsequent chemistries are determined by the history. As a consequence, the early stages determine chemical reactions and reveal the necessary steps for the design and optimization of reactions involving the transfer of an electron from a donor site to acceptor sites within the condensed phase. These reactions are among the most fundamental transformations that occur in condensed phase chemistry and the related sciences of physics and biology, and are the key steps for efficient energy conversion, catalysis, and energy storage.

The research outlined in the first subtask addresses the dynamics of localization and thermalization of primary charge carriers obtained by radiolysis and photolysis of molecular glasses, crystals, fluids, and semiconductor nanomaterials. These initial rapid processes are coupled to the consequent chemistry of thermalized species. Additionally, real-time monitoring of the transformation of the highly reactive, energetic intermediates is studied in order to improve the performance of photocatalysts and photovoltaic devices. The second subtask outlines the development of ultrafast methods of radiation chemistry that promise to open up new windows for observing these important electron driven processes. The development of a terawatt table-top laser system allows, for the first time, a suitable means to test and measure many ultrafast phenomena involving electrons, X-rays, and plasmas. Additionally, the existing T3 system developed in our laboratory produces a multi-terawatt laser field intensity in an ultrashort super-intense pulse, which can result in fundamentally new interactions of atoms and molecules with light.

STAFF

SUBTASK 1.  Reactive Intermediates in High-Energy Chemistry

SUBTASK 2.  Radiation Chemistry of Nonaqueous Systems

FACILITIES

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Glassblowing

Interfacial Processes

Radiation and Photochemistry

Photosynthesis
Biological Materials Growth Facility

Cluster Studies

Chemical Dynamics

Atomic Physics

Nanophotonics

Heavy Elements

Coordination Chemistry

f-Electron Interactions

Actinide Facility

Computational Materials and Electrochemical Processes

   
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