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Accurate characterization of charge-transfer excited states

Periodic Reporting for period 1 - AccuCT (Accurate characterization of charge-transfer excited states)

Reporting period: 2016-01-04 to 2018-01-03

Electronic charge transfer (CT) processes play an important role in photoactive molecules that have found great potential in solar energy conversion and environmental remediation. A correct computational description of the electronic structure of CT excitations is essential for the bottom-up rational design of new photoactive molecules and materials. These materials are of paramount importance for the 'development of a secure, clean and more efficient energy', one of the main focuses of the Horizon 2020 program. The ideal computational method to study this kind of excitations should provide a quantitative description of state properties at low computational lost, making time-dependent density functional theory (TDDFT) the method of choice. However, current TDDFT approximations fail to describe processes such as double excitations, Rydberg states, and particularly CT excitations. The goal of this project is developing a new family electronic structure methods for the quantitative description of CT excited states.
The main results achieved during the reporting period are the development and implementation of three new electronic structure methods, namely, Time-dependent Orbital-optimized second-order perturbation theory (TD-OOMP2),
Spin-flip Orbital-Optimized Orbital-optimized second-order perturbation theory (SF-OOMP2), and Time-dependent Orbital-Optimized Double Hybrids (TD-OODH). These methods are able to describe properly excited states with strong
charge-transfer character.
A correct computational description of the electronic structure of CT excitations, such as the one provided by using the methods developed in this project, is essential for the bottom-up rational design of new photoactive molecules and materials. These materials are of paramount importance for the 'development of a secure, clean and more efficient energy', one of the main focuses of the Horizon 2020 program
Real-space descriptors of dynamic and nondynamic electron correlation.