Computational infrared and Raman spectra by hybrid QM/MM techniques: a study on molecular and catalytic material systems

Guan, J. et al. (2023) Computational infrared and Raman spectra by hybrid QM/MM techniques: a study on molecular and catalytic material systems. Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, 381(2250), 20220234. (doi: 10.1098/rsta.2022.0234) (PMID:37211033) (PMCID:PMC10200352)

Abstract

Vibrational spectroscopy is one of the most well-established and important techniques for characterizing chemical systems. To aid the interpretation of experimental infrared and Raman spectra, we report on recent theoretical developments in the ChemShell computational chemistry environment for modelling vibrational signatures. The hybrid quantum mechanical and molecular mechanical approach is employed, using density functional theory for the electronic structure calculations and classical forcefields for the environment. Computational vibrational intensities at chemical active sites are reported using electrostatic and fully polarizable embedding environments to achieve more realistic vibrational signatures for materials and molecular systems, including solvated molecules, proteins, zeolites and metal oxide surfaces, providing useful insight into the effect of the chemical environment on the signatures obtained from experiment. This work has been enabled by the efficient task-farming parallelism implemented in ChemShell for high-performance computing platforms. This article is part of a discussion meeting issue ‘Supercomputing simulations of advanced materials’.

• Item Type: Articles
• Additional Information: The authors acknowledge funding for this work from EPSRC grant no. EP/R001847/1. ChemShell development additionally benefits from support provided by CoSeC, the Computational Science Centre for Research Communities, through the UK’s HEC Materials Chemistry Consortium (MCC). Via our membership of the MCC, which is funded by EPSRC (EP/R029431), this work used the ARCHER2 UK National Supercomputing Service (www.archer2.ac.uk) and the UK Materials and Molecular Modelling Hub for computational resources, MMM Hub, which is partially funded by EPSRC (EP/T022213). Additional computing resources were provided by STFC Scientific Computing Department’s SCARF cluster and local resources at UCL. A.J.L. acknowledges funding by the UKRI Future Leaders Fellowship programme (MR/T018372/1).
• Keywords: Embedded cluster, infrared, Raman, QM/MM, vibrational spectroscopy, ChemShell.
• Status: Published
• Refereed: Yes
• Glasgow Author(s) Enlighten ID: Senn, Dr Hans

Creator Roles

Senn, H. M.: Conceptualization, Funding acquisition, Investigation, Methodology, Validation, Writing – review and editing

• Authors: Guan, J., Lu, Y., Sen, K., Abdul Nasir, J., Desmoutier, A. W., Hou, Q., Zhang, X., Logsdail, A. J., Dutta, G., Beale, A. M., Strange, R. W., Yong, C., Sherwood, P., Senn, H. M., Catlow, C. R. A., Keal, T. W., and Sokol, A. A.
• College/School: College of Science and Engineering > School of Chemistry
• Journal Name: Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences
• Publisher: Royal Society
• ISSN: 1364-503X
• ISSN (Online): 1471-2962
• Published Online: 22 May 2023
• Copyright Holders: Copyright © 2023 The Authors
• First Published: First published in Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences 381(2250): 20220234
• Publisher Policy: Reproduced under a Creative Commons License
• Data DOI: 10.6084/m9.figshare.c.6607478

Project Code	Award No	Project Name	Principal Investigator	Funder's Name	Funder Ref	Lead Dept
303293		Transition metal controlled nitrogen chemistry in zeolite and protein environments using a unified quantum embedding	Hans Senn	Engineering and Physical Sciences Research Council (EPSRC)	EP/R001847/1	Chemistry