Photocatalysis is an emerging technology with great potential for addressing energy shortage and environmental pollution. Among the various types of photocatalysts, single-atom photocatalysts (SAPCs) have demonstrated high effeciency and remarkable activity owing to their unique spatial separation state, tunable coordination structure, and distinct local electronic properties. Gaining a comprehensive understanding of the ultrafast catalytic processes induced by light is essential for the rational design of photocatalysts, enabling enhanced photocatalytic performance and improved utilization of solar energy. In situ/operando characterization techniques, such as synchronous illumination X-ray photoelectron spectroscopy (XPS), provide valuable insights into the dynamic changes in the location, geometry, and electronic structures of single atoms and their interactions with the catalyst support during photocatalytic reactions. Additionally, these techniques offer crucial information for the development of highly efficient photocatalysts and the investigation of their underlying mechanisms.

Despite the progress made through experimental studies, the interpretation of these phenomena remains contentious. This is primarily attributed to the lack of ab initio understanding regarding the dynamics of light-induced ultrafast excited carriers and structural changes occurring at the single active site of photocatalysts. Bridging this gap between experimental observations and theoretical insights is crucial to advance our understanding and enable the rational design of high performance SAPCs. On the other hand, ab initio investigating light-driven ultrafast catalytic processes in photocalytic materials is still challenging due to the presence of phenomena such as ultrafast charge transfer, nonadiabatic electron-nuclei couplings, and the high computational cost.

This project aims to investigate the laser pulse induced ultrafast electronic and structural dynamics of SAPCs based on nanomaterials (such as 2D materials, oxides, or zeolites) for applications in water splitting and CO2 reduction at the microscopic scale. The research will employ state-of-the-art real-time time-dependent density functional theory (rt-TDDFT) and ab initio non-adiabatic molecular dynamics (NAMD) theory (surface hopping and Ehrenfest dynamics), to explore the ultrafast catalytic processes occurring in these SAPCs. Specifically, the project tasks will encompass:

(i) Mechanism elucidation of photoexcited carrier separation and recombination at active sites in SAPCs. (ii) Investigation of vibrational model excitation and bond dynamics for adsorbed molecules (such as CO2 or H2O). (iii) Examination of the dynamic evolution of the valence state and coordination environment during the photocatalytic reaction process. (iv) Analysis of the solid-liquid interaction of nanomaterials (with active sites) under photoexcitation. (v) Study of the effects of defects and catalyst supports on the ultrafast catalytic processes.

Publications of research group related to this topic:

1. J. He, S. Li, A. Bandyopadhyay, T. Frauenheim, Unravelling Photoinduced Interlayer Spin Transfer Dynamics in 2D Nonmagnetic-Ferromagnetic van der Waals Heterostructures, Nano Lett., 2021, 21, 3237-3244.

2. J. He, S. Li, L. Zhou, T. Frauenheim, Ultrafast Light-Induced Ferromagnetic State in Transition Metal Dichalcogenides Monolayers. J. Phys. Chem. Lett., 2022, 13, 2765-2771.

3. Z. Zhou, J. He, T. Frauenheim, O. V. Prezhdo, J. Wang, Control of Hot Carrier Cooling in Lead Halide Perovskites by Point Defects. J. Am. Chem. Soc., 2022, 144, 18126–18134.

4. S. Li, L. Zhou, T. Frauenheim, J. He, Light-Controlled Ultrafast Magnetic State Transition in Antiferromagnetic-ferromagnetic van der Waals Heterostructures. J. Phys. Chem. Lett., 2022, 13, 6223-6229.

5. J. He, T. Frauenheim, Optically driven ultrafast magnetic order transitions in two-dimensional ferrimagnetic MXenes. J. Phys. Chem. Lett., 2020, 11, 15, 6219–6226.

Qualifications:
A PhD degree in Computational Chemistry/Physics, Computational Materials Science or a related discipline is required, with experience in atomistic modelling of materials or first principles. Experience with programming is highly desired.

Salary: co-founding 1000 EUR/month is ensured
Co-founding resources: Department of physical and macromolecular chemistry budget
Department: Department of physical and macromolecular chemistry
Supervisor: Junjie He, Ph.D.
E-mail: junjie.he@natur.cuni.cz
Position available from: January 1, 2024
Deadline date for applications: 27th July, 2023

Applicants must submit required documents to: junjie.he@natur.cuni.cz (project supervisor) and in a copy to pavla.pouskova@natur.cuni.cz (International Department)