Quantum cutting using organic molecules
文献信息
Michael D. LaCount, Mark T. Lusk
A methodology is presented in which a combination of quantum electrodynamics, time-dependent perturbation theory, and computational electronic structure analysis allow the prospect for organic quantum cutting to be quantitatively examined from first principles. The internal quantum yield of quantum cutting is ultimately expressed in terms of rate equations that account for all relevant processes. These are populated with excited state properties found using time-dependent density functional theory and configuration interaction methods. The rate equations are incorporated into an optimization routine in which the quantum yield is maximized by changing the spacing and orientation of the molecules. Adapting design criteria first developed for energy pooling, a system of squarylium dye III and fluorene was identified as being capable of carrying out meaningful quantum cutting. With relative position and orientation optimized, the internal quantum yield of this test system is predicted to be 1.2. In the absence of non-radiative decay, the internal yield is predicted to be 1.9.
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来源期刊
Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.












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