RelPro · Relativistic non-linear optical property calculations with density functional theory
Horizon 2020 — Marie Skłodowska-Curie Actions
- Duration
- 2017-04-18 → 2019-04-17
- EU contribution
- €159,461
- Participants
- 1
- Scheme
- MSCA-IF
Lines connect the coordinator with its partners.
Results in brief
Relativistic non-linear optical property calculations with density functional theory
The RelPro project had the aim of implementing a computational technique for calculating non-linear optical molecular properties with a relativistic quantum chemistry method. Non-linear optical properties are spectroscopical properties which depend on the intensity of the incident radiation. They are relevant for a large amount of technical applications such as for photochromic materials, frequency conversion of lasers or photodynamic canter therapy. Structure-property relations for these properties are very complex and design of new materials in this field often needs support from computational chemistry. Relativistic effects are effects originating from the theory of relativity. Most quantum chemical approaches neglect these effects as they render the working equations extremely complex while and their impact on the result is normally very small as long as only lighter element atoms are considered. As heavier atoms come into play, relativistic effects become more and more important it can no longer be neglected. The overall objective of the RelPro project was to provide a fast and reliable computational method which is able to calculate non-linear optical properties for molecular systems including heavy atoms using time-dependent density functional theory (TD-DFT). During the RelPro project, the fundamental equations for these properties have been derived and a program has been written that is able to calculate first-order hyperpolarizabilities of heavy atom compounds in combination with other quantum chemistry programs.
Data: CORDIS, © European Union
Project objective
Non-linear optical properties of molecules with strong relativistic effects play an important role in current research e.g. for photochromic materials and bioimaging. Up to now, there is no computational treatment of these molecular properties such as two-photon absorption (TPA) and first hyperpolarizabilities using density functional theory (DFT). Such a computational technique will, however, be very benefitial for research in this field as by result prediction and computational assistance for the interpretation of results, it will allow for a much more efficient use of synthesis ressources both regarding manpower and chemicals. The molecular properties will be treated in terms of energy derivatives w.r.t. the electric field using response theory. Relativistic effects will be taken into account as part of the zeroth-order Hamiltonian. Namely, the four-component Hamiltonian will be used. As the first main task of the project, the so-called second exchange-correlation kernel, the third derivative of the exchange-correlation energy with respect to the variational parameters, will be formulated and implemented. Due to the innovativeness of the response theory approach to be used, TPA, first hyperpolarizabilities and excited state dipole moments will be available at the same time allowing for a large variety of applications right from the start. This project is a big challenge for quantum chemical method development as taking into account relativistic effects using the four-component Hamiltonian operator renders the fundamental expressions very complex. However, the risk behind this project will be minimized by the organization in terms of work packages which ensure that the implementation will be performed in different steps with increasing complexity.
Original text from CORDIS.
Participants
- HEINRICH-HEINE-UNIVERSITAET DUESSELDORF · DusseldorfCoordinatorGermany
Links
Data: CORDIS, © European Union