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New excited state methods for overcoming challenges in sunlight conversion

Project description

Catching electrons in the act

Designing efficient solar energy conversion devices or understanding photosynthesis rests on knowing how electrons and atoms rearrange when molecules absorb light. The problem is that modelling such transient 'excited states' is still a major challenge in chemistry, especially for molecules in a condensed phase. The ERC-funded NEXUS project aims to develop computational methods for simulating light-triggered processes in realistic environments more efficiently and reliably than current approaches. The new methodologies will be used to interpret ultrafast X-ray experiments that catch electrons and atoms in motion after light excitation. Together, experiments and computer simulations will reveal how electronic and atomic structural changes unfold when organic molecules react with light, helping researchers design better solar energy conversion devices and other light-driven technologies.

Objective

The dynamics of charges and atoms when electrons are excited to energy levels above the ground state underpins energy conversion in photosynthesis, photocatalysis and solar cell technologies. Modelling excited electronic states remains however a major challenge. While density functional theory (DFT) has been hugely successful in predicting ground state properties of systems with several atoms and electrons, excited state extensions based on time-dependent formulations often lack the required accuracy. I have pioneered alternative approaches where the excited state orbitals are variationally optimized by converging on saddle points on the electronic energy surface. Preliminary studies show that such time-INdependent methods have similar efficiency and predictive power as ground state DFT. The central idea of NEXUS is to develop an innovative computational framework leveraging saddle point search strategies to significantly expand excited state simulations beyond their current scope.

Meanwhile, modern ultrafast X-ray techniques can achieve structural sensitivity for organic chromophores, offering a means to validate and complement the theoretical models for this important class of photoactive systems. By simulating the excited states in condensed phase rather than gas phase and directly visualizing atomic motion via ultrafast X-rays, NEXUS will provide unprecedented insights into the electronic and structural dynamics of organic molecules with application in photoswitching, singlet fission, and artificial photosynthesis. The goal is to unravel the elusive interplay between structure and function and pave the way to the rational design of photofunctional systems, enhancing the efficiency of solar energy conversion. An effective, low cost approach for modelling excited states of large systems is ground breaking and will have impact well beyond organic molecules, enabling the study of charge and atom dynamics in photochemical reactions for a wide range of applications.

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HORIZON-ERC - HORIZON ERC Grants

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(opens in new window) ERC-2024-STG

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Host institution

UNIVERSITA DEGLI STUDI DI TRIESTE
Net EU contribution

Net EU financial contribution. The sum of money that the participant receives, deducted by the EU contribution to its linked third party. It considers the distribution of the EU financial contribution between direct beneficiaries of the project and other types of participants, like third-party participants.

€ 1 262 011,50
Address
PIAZZALE EUROPA 1
34127 Trieste
Italy

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Region
Nord-Est Friuli-Venezia Giulia Trieste
Activity type
Higher or Secondary Education Establishments
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Total cost

The total costs incurred by this organisation to participate in the project, including direct and indirect costs. This amount is a subset of the overall project budget.

€ 1 262 011,50

Beneficiaries (2)

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