Energy Pooling Upconversion in Organic Molecular Systems

TL;DR

This paper develops a computational method to estimate energy pooling rates in organic molecules, demonstrating high efficiency in specific configurations and providing design rules for optimizing upconversion processes.

Contribution

A new computational approach combining quantum electrodynamics, perturbation theory, and ab initio calculations for estimating 3-body singlet upconversion rates in organic systems.

Findings

Energy pooling efficiency can reach at least 90% in certain configurations.

The methodology aligns with previous experimental data for stilbene-fluorescein.

Design rules for optimizing energy pooling were established.

Abstract

A combination of molecular quantum electrodynamics, perturbation theory, and ab initio calculations was used to create a computational methodology capable of estimating the rate of 3-body singlet upconversion in organic molecular assemblies. The approach was applied to quantify the conditions under which such relaxation rates, known as energy pooling, become meaningful for two test systems: stilbene-fluorescein and hexabenzocoronene-oligothiophene. Both exhibit low intra-molecular conversion but inter-molecular configurations exist in which pooling efficiency is at least 90\% when placed in competition with more conventional relaxation pathways. For stilbene-fluorescein, the results are consistent with data generated in an earlier experimental investigation. Exercising these model systems facilitated the development of a set of design rules for the optimization of energy pooling.