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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
HISTORY
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