Toward an optimal use of mechanical forces and electric fields for the catalysis of chemical reactions

Prof. Josep Maria Bofill and Dr. Jordi Ribas
jmbofill@ub.edu, j.ribas@ub.edu
http://www.ub.edu/gem2/welcome.html

Details

The use of external mechanical forces and external oriented electric fields (OEEFs) to catalyze chemical reactions is an emerging research field at the frontier of knowledge between physics and chemistry that has attracted a great deal of interest because these techniques hold great promise as new tools for the synthesis of molecules. Different types of single-molecule experiments have demonstrated that mechanical stress and electric fields can accelerate reactions. Yet, the coupling between mechanical stress/electric fields with chemical reactivity is far from being completely understood. One of the main issues that has not yet been addressed is the following one: given a reaction that can be activated by mechanical means and/or by OEEFs, how should the external perturbation be applied to the system in order to induce the reaction in the most efficient way (i.e, using a mechanical force or an OEEF with the minimal magnitude)? This project will be based on theoretical/computational work aimed at developing and using algorithms for the optimal control of reactions by means of mechanical forces and OEEFs. The results that will obtained in the project will be important for single-molecule experiments, mechanoresponsive polymers (given the importance of mechanophores in the design of self-healing polymers) and for enzymatic catalysis (in view of most recent experiments that have demonstrated the key role of electric fields developed in the active site of enzymes in catalyzing reactions).
The two principal investigators of this project have a strong background in theoretical/computational work applied to the field of mechanochemistry [1-4] and in devising algorithms and computational protocols to explore potential energy surfaces of reactive molecular systems [5,6].

[1] Chem. Rev. 2012, 112, 5412
[2] Phys. Rev. Lett. 2015, 114, 075501
[3] J. Phys. Chem. A 2017, 121, 2820
[4] Nat. Chem. 2017, 9, 164
[5] J. Chem. Phys. 2017, 147, 152710
[6] J. Chem. Theory Comput. 2019, 15, 5426

Job position description

For this thesis, we seek a motivated student with interests in theoretical/computational chemistry and in interdisciplinary research that involves both chemistry and physics. The applicant should hold, or be close to completing, a degree or master degree in fields related to physics or chemistry. Previous experience in electronic structure calculations, coding, and/or algorithm development would be highly beneficial for the project.

The student is expected to perform the following tasks:

i) to carry out electronic structure calculations using standard quantum chemistry packages (like GAMESS-US and/or TURBOMOLE) to explore how mechanical forces and OEEFs modify the potential energy surfaces of several reactive molecular systems;

ii) to write codes that can be interfaced with these packages in order to efficiently explore the potential energy surfaces under the effects of external mechanical forces and/or OEEFs (including the location of critical points, transition states and minimum energy paths):

iii) if time allows, to devise new algorithms to ensure an optimal control of mechanical forces and OEEFs in the catalysis of reactions;

iv) to write scientific articles and prepare talks and posters related to the obtained results.

Summary of conditions

The project proposal is included in the DOCTORAL INPhINIT FELLOWSHIPS PROGRAMME – INCOMING FRAME, more information at: https://obrasociallacaixa.org/en/investigacion-y-becas/becas-de-la-caixa/doctorado-inphinit/incoming

Contract Length: 3 years

Estimated Incorporation date: From July to September 2020