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  Charge Transfer-Mediated Dramatic Enhancement of Raman Scattering upon Molecular Point Contact Formation

Cirera, B., Litman, Y., Lin, C., Akkoush, A., Hammud, A., Wolf, M., et al. (2022). Charge Transfer-Mediated Dramatic Enhancement of Raman Scattering upon Molecular Point Contact Formation. Nano Letters, 22(6), 2170-2176. doi:10.1021/acs.nanolett.1c02626.

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nl1c02626_si_001.pdf (Supplementary material), 2MB
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Supporting Information: Materials and methods, incident laser power dependence of the TERS intensity in the tunneling regime, tip condition dependence of TERS for a C60 molecule on Ag(111), models used in the DFT calculations, projected electronic density of states, detailed analysis of the Raman active modes of C60 on Ag(111) and C60-tip, Δz-dependent TERS of a C60-tip on Ag(111) at small Vbias, enlarged Δz-dependent TERS of a C60-tip on Ag(111) highlighting the shifting of the vibrational modes, simulations of the static Raman polarizability of C60, wavelength dependence of MPC-TERS (PDF)
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© The Authors. Published by American Chemical Society

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https://doi.org/10.1021/acs.nanolett.1c02626 (Publisher version)
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 Creators:
Cirera, B.1, Author
Litman, Y.2, Author              
Lin, C.1, Author
Akkoush, A.2, Author              
Hammud, A.3, Author
Wolf, M.1, Author
Rossi, M.2, Author              
Kumagai, T.1, 4, Author
Affiliations:
1Department of Physical Chemistry, Fritz-Haber Institute of the Max-Planck Society, ou_persistent22              
2Simulations from Ab Initio Approaches, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_3185035              
3Department of Inorganic Chemistry, Fritz-Haber Institute of the Max-Planck Society, ou_persistent22              
4Center for Mesoscopic Sciences, Institute for Molecular Science, ou_persistent22              

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 Abstract: Charge-transfer enhancement of Raman scattering plays a crucial role in current-carrying molecular junctions. However, the microscopic mechanism of light scattering in such nonequilibrium systems is still imperfectly understood. Here, using low-temperature tip-enhanced Raman spectroscopy (TERS), we investigate how Raman scattering evolves as a function of the gap distance in the single C60-molecule junction consisting of an Ag tip and various metal surfaces. Precise gap-distance control allows the examination of two distinct transport regimes, namely tunneling regime and molecular point contact (MPC). Simultaneous measurement of TERS and the electric current in scanning tunneling microscopy shows that the MPC formation results in dramatic Raman enhancement that enables one to observe the vibrations undetectable in the tunneling regime. This enhancement is found to commonly occur not only for coinage but also transition metal substrates. We suggest that the characteristic enhancement upon the MPC formation is rationalized by charge-transfer excitation.

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Language(s): eng - English
 Dates: 2022-02-112021-07-052022-02-212022-03-23
 Publication Status: Published in print
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acs.nanolett.1c02626
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Title: Nano Letters
  Abbreviation : Nano Lett.
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 22 (6) Sequence Number: - Start / End Page: 2170 - 2176 Identifier: ISSN: 1530-6984
CoNE: https://pure.mpg.de/cone/journals/resource/110978984570403