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  First-Principles Simulations of Tip Enhanced Raman Scattering Reveal Active Role of Substrate on High-Resolution Images

Litman, Y., Bonafé, F., Akkoush, A., Appel, H., & Rossi, M. (2023). First-Principles Simulations of Tip Enhanced Raman Scattering Reveal Active Role of Substrate on High-Resolution Images. The Journal of Physical Chemistry Letters, 14(30), 6850-6859. doi:10.1021/acs.jpclett.3c01216.

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Supporting Information: Detailed derivation of eq 3, further computational details, and validation tests
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https://arxiv.org/abs/2211.09475 (Preprint)
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https://doi.org/10.1021/acs.jpclett.3c01216 (Publisher version)
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 Creators:
Litman, Y.1, 2, Author           
Bonafé, F.3, Author           
Akkoush, A.2, 4, Author           
Appel, H.3, Author           
Rossi, M.2, 4, Author           
Affiliations:
1Yusuf Hamied Department of Chemistry, University of Cambridge, ou_persistent22              
2Simulations from Ab Initio Approaches, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_3185035              
3Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
4Fritz Haber Institute of the Max Planck Society, ou_persistent22              

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 Abstract: Tip-enhanced Raman scattering (TERS) has emerged as a powerful tool to obtain subnanometer spatial resolution fingerprints of atomic motion. Theoretical calculations that can simulate the Raman scattering process and provide an unambiguous interpretation of TERS images often rely on crude approximations of the local electric field. In this work, we present a novel and first-principles-based method to compute TERS images by combining Time Dependent Density Functional Theory (TD-DFT) and Density Functional Perturbation Theory (DFPT) to calculate Raman cross sections with realistic local fields. We present TERS results on free-standing benzene and C60 molecules, and on the TCNE molecule adsorbed on Ag(100). We demonstrate that chemical effects on chemisorbed molecules, often ignored in TERS simulations of larger systems, dramatically change the TERS images. This observation calls for the inclusion of chemical effects for predictive theory-experiment comparisons and an understanding of molecular motion at the nanoscale.

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Language(s): eng - English
 Dates: 2023-05-052023-07-142023-07-242023-08-03
 Publication Status: Issued
 Pages: 10
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: arXiv: 2211.09475
DOI: 10.1021/acs.jpclett.3c01216
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Grant ID : 895747
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)
Project name : The authors wish to acknowledge the support of the Max Planck Society. Y.L. has been partly funded by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) Project Number 467724959. F.P.B. acknowledges financial support from the European Union’s Horizon 2020 research and innovation programme under the Marie Sklodowska-Curie Grant Agreement no. 895747 (NanoLightQD). M.R. and A.A. acknowledge funding by the Deutsche Forschungsgemeinschaft (DFG), Projektnummer 182087777 – SFB 951. Y.L. would like to thank Oliver Hofmann for suggesting the investigation of the TCNE molecule in this project and Thomas Purcell for a critical reading of the manuscript.
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Source 1

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Title: The Journal of Physical Chemistry Letters
  Abbreviation : J. Phys. Chem. Lett.
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 14 (30) Sequence Number: - Start / End Page: 6850 - 6859 Identifier: ISSN: 1948-7185
CoNE: https://pure.mpg.de/cone/journals/resource/1948-7185