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Theoretical Chemistry of Unbound Electrons

Project description

Novel theoretical models could point to quantum catalysis without bounds

From petroleum refining to food processing to DNA sequencing, catalysts assist reactions to get larger product yields in less time. They alter the rate of a reaction without being altered by it, moving around binding and unbinding, lowering the energy required for a reaction to occur and then moving on. Unbound electrons can act as simple and versatile catalysts. However, theoretical descriptions of unbound electron behaviours in complex systems do not exist and thus pathways and products are poorly understood. T-CUBE is changing all that. Molecular dynamics simulations and integration of individual quantum simulations (quantum embedding) to describe systems of more than 100 atoms with unbound electrons will significantly advance theoretical modelling of chemistry involving the continuum.

Objective

T-CUBE aims at the theoretical modeling of chemistry involving the continuum. Traditionally, chemistry has been concerned with electrons that remain bound to the nuclei during a reaction. However, in many settings that deal with X rays or plasma, electrons can enter and leave the system; they are unbound.

Most theoretical approaches for unbound electrons are not applicable to extended systems in complex environments. As a consequence, pathways and product distributions of processes such as dissociative electron attachment and Coulomb explosion are poorly understood. This hinders progress in laboratory and technology: The electron is a simple and versatile catalyst, but corresponding applications are
still in an infant stadium.

T-CUBE seeks to overcome these limitations. Often, unbound electrons can be described by resonances, electronic states with complex-valued energy. In recent years, I contributed to advancing this approach significantly. Small molecules in gas phase can now be described with an accuracy that allows for quantitative comparison to experiment.

Here, I propose to investigate the chemistry of unbound electrons in larger molecules and condensed phase, for example, in solutions, polymeric networks, and biomolecules. Aspects that we will address include: energetics and character of resonances in different environments, resulting changes in chemical reactivity, and the interplay of nuclear motion and electron loss.

To achieve these goals, quantum chemistry for electronic resonances needs to be advanced substantially. We will develop electronic-structure methods suitable for over a hundred of atoms, a quantum embedding scheme for describing different environments, and molecular dynamics simulations that take into account electron loss. In addition, we will advance the theory of electronic resonances itself. In exemplary applications, we will investigate phenomena involving dissociative electron attachment, electron transfer, and Coulomb explosion.

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Keywords

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Topic(s)

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Funding Scheme

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ERC-STG - Starting Grant

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Call for proposal

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(opens in new window) ERC-2019-STG

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Host institution

KATHOLIEKE UNIVERSITEIT LEUVEN
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.

€ 1 495 205,00
Address
OUDE MARKT 13
3000 LEUVEN
Belgium

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Region
Vlaams Gewest Prov. Vlaams-Brabant Arr. Leuven
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.

€ 1 495 205,00

Beneficiaries (2)

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