AIMD/DFT-MD for electrochemistry at aqueous interfaces and coupling to spectroscopies in operando conditions

• Auteur / Autrice : Yijing Yang
• Direction : Marie-Pierre Gaigeot
• Type : Projet de thèse
• Discipline(s) : Chimie
• Date : Inscription en doctorat le 10/01/2022
• Etablissement(s) : université Paris-Saclay
• Ecole(s) doctorale(s) : École doctorale Sciences chimiques : molécules, matériaux, instrumentation et biosystèmes
• Partenaire(s) de recherche : Laboratoire : Laboratoire analyse et modélisation pour la biologie et l'environnement (Evry, Essonne ; 1998-)
• Partenaire(s) de recherche : référent : Université d'Évry Val d'Essonne

Mots clés

Mots clés libres

Dynamique moléculaire ab initio

Chimie théorique et computationnelle

Spectroscopies

Matériaux

Électrochimie

Dft-md/aimd

Ab initio molecular dynamics

Theoretical and computational chemistry

Materials

Dft-md/aimd

Electrochemistry

Spectroscopies

Résumé

The PhD work will consist in applying ab initio molecular dynamics simulations AIMD/DFT-MD to simulate electrochemical aqueous interfaces in order to extract structural, dynamical and vibrational spectroscopic properties of the interfaces in operando conditions. The central issues in the AIMD simulations are the electrochemical conditions that are non trivial to set-up in the quantum representation, and for which some of the developed theoretical methods will be tested, and the calculation and interpretation of spectroscopic signals such as SFG (Sum Frequency Generation) and THz-IR for which our group is expert. Our simulations will be coupled to spectroscopic experiments performed by some of our collaborators: Prof P. Petersen at the University of Bochum-Germany, Prof M. Havenith at the University of Bochum-Germany, Prof W. Liu and Prof Y.R. Shen at the Fudan University in Shanghai-China and UC Berkeley-USA, and with the electrochemistry group of Prof K. Tschulik at the University of Bochum-Germany. The electrochemical systems of interest are typically related to the CO2 reduction for improving this electrocatalysis process. Codes developed in our group are used for the analyses and the extraction of structural/dynamical/spectroscopic/reactivity properties from the trajectories. For those interested, theoretical developments can be considered and/or development of codes for trajectory analyses. Our group is internationally recognized in AIMD/DFT-MD simulations of solid/liquid interfaces. The following references illustrate some of our recent original works and innovative developments in the field of interfaces and in the field of theoretical SFG spectroscopy [J. Am. Chem. Soc. 142:6991-7000 (2020), PNAS 116:1520(2019), Phys. Chem. Chem. Phys. 21:22188-22202 (2019), J.Chem.Phys. 150:041721(2019), Phys.Chem.Chem.Phys. 20:5190(2018), Minerals 8:305(2018), J.Phys.Chem.Letters 8:3133(2017), J.Phys.Chem.C. 120:14034(2016)]. Our group is composed of 5 permanent academic researchers, 1 Engineer in informatics, 4 PhDs (Chinese, Italians, French), 1 Post-Doc, 2-3 foreign visitors/year. Our group is internationally recognized and funded by several French national ANR and LABEX research schemes, e.g. bilateral ANR-NSF/USA, ANR-DFG/Germany & LABEX CHARM3AT. Our University is a member of the larger University Paris-Saclay. The city of Evry is located 45' from the center of Paris via RER D train line or 30' from Paris-Saclay via bus. The University is 2' walk from the RER station Evry-Courcouronnes. See https://www.univ-evry.fr/accueil.html for more practical details.