Non-equilibrium phenomena and molecular reaction dynamics: mode space, energy space and conformer space
| Autor: | Robert Lightfoot, Jeremy N. Harvey, David R. Glowacki |
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| Rok vydání: | 2013 |
| Předmět: |
CHEMICAL-REACTIONS
NONSTATISTICAL DYNAMICS Biophysics TRANSITION-STATE THEORY theoretical chemistry CN RADICAL REACTIONS Molecular dynamics Transition state theory PHASE BIMOLECULAR REACTIONS Quantum mechanics Master equation Vibrational energy relaxation ALKENE HYDROBORATION Statistical physics Physical and Theoretical Chemistry COMPUTER-SIMULATIONS Molecular Biology Conformational isomerism ENZYME CATALYSIS Chemistry VIBRATIONAL-RELAXATION Condensed Matter Physics molecular dynamics MASTER EQUATION non-equilibrium Reaction dynamics Phase space reaction kinetics |
| Zdroj: | Glowacki, D R, Lightfoot, R & Harvey, J N 2013, ' Non-equilibrium phenomena and molecular reaction dynamics: mode space, energy space and conformer space ', Molecular Physics, vol. 111, no. 5, pp. 631-640 . https://doi.org/10.1080/00268976.2013.780100 |
| ISSN: | 1362-3028 0026-8976 |
| DOI: | 10.1080/00268976.2013.780100 |
| Popis: | The ability to characterise and control matter far away from equilibrium is a frontier challenge facing modern science. In this article, we sketch out a heuristic structure for thinking about the different ways in which non-equilibrium phenomena can impact molecular reaction dynamics. Our analytical schema includes three different regimes, organised according to increasing dynamical resolution: at the lowest resolution, we have conformer phase space, at an intermediate resolution, we have energy space; and at the highest resolution, we have mode space. Within each regime, we discuss practical definitions of non-equilibrium phenomena, mostly in terms of the corresponding relaxation timescales. Using this analytical framework, we discuss some recent non-equilibrium reaction dynamics studies spanning isolated small-molecule ensembles, gas-phase ensembles and solution-phase ensembles. This includes new results that provide insight into how non-equilibrium phenomena impact the solution-phase alkenehydroboration reaction. We emphasise that interesting non-equilibrium dynamical phenomena often occur when the relaxation timescales characterising each regime are similar. In closing, we reflect on outstanding challenges and future research directions to guide our understanding of how non-equilibrium phenomena impact reaction dynamics. |
| Databáze: | OpenAIRE |
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