STIR Proposal: Radiationless Transitions Induced by Natural Incoherent Light
Abstract
Very little is known about the highly significant, and ubiquitous, radiationless transition processes as they occur in nature, i.e., under steady state conditions resulting from excitation with incoherent radiation (e.g. sunlight). Rather, much of the published research focus has been on time-dependent dynamics in pulsed laser domain. As a consequence, both our understanding and our ability to utilize natural incoherent light to drive physical processes is severely hampered. Examples include isomerization, internal conversion, and energy and charge transfer. This STIR proposal aims to test and substantiate a new fully quantum theoretical and computational approach to addressing, and gaining physical insight into, a wide variety of radiationless processes in nature. Specifically we propose to reach the overall objective by developing theoretical and computational tools to address radiationless transition processes induced by natural incoherent light (see figure), via a 1. New proposed methodology to compute the steady state under incoherent illumination 2. Enhanced projection operator methodology to partition the steady state into "reactants" and "products" 3. Highly efficient methodology to compute rates of radiationless transitions in the steady state The goal of this STIR proposal is develop and apply this three step approach to the linear vibrionic coupling model system and obtain quantitatively accurate results when compared to exact quantum calculations. The successful application of this approach to this system, which introduces new physically motivated approximations, is the STIR proposal milestone, and will serve as a gateway to applications to polyatomic systems where the approach is expected to solve the problem of exponentially growing computational cost scaling with increasing molecule size. That is, by achieving this milestone within the term of the STIR grant, we will be able to proceed to applying the developed methodologies to explore steady state internal conversion in realistic molecular systems such as pyrazine and donor-acceptor energy transfer compounds like 9-((1-naphthyl)-methyl)-anthracene, as well as to investigate charge and energy transport in open systems.
Document Details
- Document Type
- DoD Grant Award
- Publication Date
- Aug 06, 2019
- Source ID
- W911NF1910433
Entities
People
- Paul Brumer
Organizations
- Army Contracting Command
- United States Army
- University of Toronto