ReReDMFT · Development and implementation of reduced density matrix functionals for relativistic quantum chemistry.
Horizon 2020 — Marie Skłodowska-Curie Actions
- Duration
- 2021-02-01 → 2023-01-31
- EU contribution
- €175,572
- Participants
- 1
- Scheme
- MSCA-IF
Lines connect the coordinator with its partners.
Results in brief
Development and implementation of reduced density matrix functionals for relativistic quantum chemistry.
The aim of the Relativistic Reduced Density Matrix Functional Theory project (891647-ReReDMFT) was to propose a new methodology for studying (theoretically) compounds formed by heavy elements using quantum mechanics. The electronic structure of heavy elements is modified by relativistic effects as a consequence of the high speed (that approaches the speed of light) of the electrons; thus, relativistic quantum mechanics is the framework needed for studying these compounds. In principle, the exact method to account for relativistic and quantum effects is known. But, the computational cost of the exact method makes it impractical. Hence, numerical simulations to study the chemistry and physics of compounds formed by heavy elements require approximations. In this project, I proposed to extend the applicability of Reduced Density Matrix Functional Theory (RDMFT) to include relativistic effects (ReRDFMT). This new method should lead to an affordable computational cost and facilitate the study of compounds formed by heavy elements. The Chemistry of heavy elements plays a crucial role in several applications of modern societies, e.g.: a) medical treatments employ their radioactive properties, b) power plants involve nuclear fission, c) the development of new nanomaterials [e.g. molecular engines is based on Ln(II) and Ln(III) for the photoconversion], among others. Thence, with the new theory/method proposed in this project (i.e. ReRDMFT) we will be able, in the future, to improve several scientific disciplines and industrial applications, which will also have a deep impact in our societies. The main objective of this project was to propose the theoretical foundations of ReRDMFT and propose the approximations needed for numerical simulations. The second objective was to develop a computational program to be used in numerical simulations of compounds formed by heavy elements. Finally, I aimed to compute some systems of scientific and industrial interests to describe the quality of ReRDMFT and compare them with reference data. I would like to conclude this project by highlighting that thanks to the financial support of the Marie Skłodowska Curie Action, the major objective of this project is completed and a new theory/method has been proposed. Nevertheless, I would also like to comment that the remaining (secondary) objectives are not completed and it is work that is still in progress.
Data: CORDIS, © European Union
Project objective
Computational chemistry (CC) methods supply approximate solutions to the Schrödinger equation (SE) and make it possible to compute a wide range of chemical properties. A problem is, however, that the work horse method in CC, Kohn-Sham Density Functional Theory, cannot always describe the process of chemical bonds breaking or formation accurately (the errors produced in H2 dissociation are a simple example). Wave function-based methods are more reliable but their computational cost is prohibitive for large systems. Recent advances in reduced density matrix functional theory (RDMFT) have demonstrated the potential of this methodology to treat such non-dynamic electron correlation effects (near degeneracies occurring in bond dissociation) at reasonable computational cost.In this project I aim to explore RDMFT in an area in which a proper treatment of non-dynamic electron correlation effects is essential: the chemistry of heavy elements. For compounds of such elements, near-degeneracies of electronic energies is the rule rather than the exception, and RDFMT emerges as an excellent alternative in relativistic CC to wave function based and DFT methods . An important complication is the importance of relativistic effects requiring the use of the Dirac equation (DE) instead of the SE. In this project, I will work on transferring RDMFT to this domain by taking the following steps: a) set up the required theoretical background, b) analyze the performance of the currently available RDMFT approximations (for two-component Hamiltonians), c) develop a RDMFT approximation for the DE (four-component Hamiltonian), and d) make this methodology available to the scientific community by implementing it in the DIRAC code. I expect that RDMFT will predict energies accurately for the DE, and it can become a powerful method to predict properties of novel materials formed by heavy elements.
Original text from CORDIS.
Participants
- STICHTING VU · AmsterdamCoordinatorNetherlands
Links
Data: CORDIS, © European Union