Irreversible organic crystalline chemistry monitored in real time
- PMID: 16946037
- DOI: 10.1126/science.1127826
Irreversible organic crystalline chemistry monitored in real time
Abstract
Because multiple laser shots are typically required to monitor ultrafast photochemical reaction dynamics, sample depletion and product accumulation have greatly restricted the range of substrates and structural environments amenable to study. By implementing a two-dimensional spatial delay gradient across the profile of a femtosecond probe pulse, we can monitor in a single laser shot organic crystalline reaction dynamics despite the formation of permanent photoproducts that cannot be conveniently removed. We monitored the photolysis of the triiodide anion, I3-, and subsequent recombination or relaxation of its reaction products, in three very different pure organic molecular crystals. The experimental results and associated molecular dynamics simulations illustrate the intimate connection between lattice structure and reaction dynamics, highlighting the role of lattice constraints in directing phase-coherent geminate recombination of photofragments within a crystalline reaction cage.
Comment in
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Chemistry. A pixellated window on chemistry in solids.Science. 2006 Sep 22;313(5794):1747-8. doi: 10.1126/science.1133024. Epub 2006 Aug 31. Science. 2006. PMID: 16946034 No abstract available.
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