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Vibrational Sum Frequency Spectroscopic Investigation of the Azimuthal Anisotropy and Rotational Dynamics of Methyl-Terminated Silicon(111) Surfaces

Malyk, Sergey and Shalhout, Fadel Y. and O'Leary, Leslie E. and Lewis, Nathan S. and Benderskii, Alexander V. (2013) Vibrational Sum Frequency Spectroscopic Investigation of the Azimuthal Anisotropy and Rotational Dynamics of Methyl-Terminated Silicon(111) Surfaces. Journal of Physical Chemistry C, 117 (2). pp. 935-944. ISSN 1932-7447. doi:10.1021/jp3067298. https://resolver.caltech.edu/CaltechAUTHORS:20130225-163026469

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Abstract

Polarization-selected vibrational sum frequency generation spectroscopy (SFG) has been used to investigate the molecular orientation of methyl groups on CH_(3)-terminated Si(111) surfaces. The symmetric and asymmetric C–H stretch modes of the surface-bound methyl group were observed by SFG. Both methyl stretches showed a pronounced azimuthal anisotropy of the 3-fold symmetry in registry with the signal from the Si(111) substrate, indicating that the propeller-like rotation of the methyl groups was hindered at room temperature. The difference in the SFG line widths for the CH_3 asymmetric stretch that was observed for different polarization combinations (SPS and PPP for SFG, visible, and IR) indicated that the rotation proceeded on a 1–2 ps time scale, as compared to the 100 fs rotational dephasing of a free methyl rotor at room temperature.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/jp3067298DOIArticle
http://pubs.acs.org/doi/abs/10.1021/jp3067298PublisherArticle
ORCID:
AuthorORCID
Lewis, Nathan S.0000-0001-5245-0538
Benderskii, Alexander V.0000-0001-7031-2630
Additional Information:© 2012 American Chemical Society. Received: July 6, 2012; Revised: November 9, 2012; Published: December 14, 2012. This research was supported by the AFOSR, Grant No. FA9550-09-1-0547 (AVB), and by the NSF, CHE-0911682 (NSL). L.E.O. graciously thanks the financial support of the Link Foundation Energy Fellowship.
Funders:
Funding AgencyGrant Number
Air Force Office of Scientific Research (AFOSR)FA9550-09-1-0547
NSFCHE-0911682
Link FoundationUNSPECIFIED
Issue or Number:2
DOI:10.1021/jp3067298
Record Number:CaltechAUTHORS:20130225-163026469
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20130225-163026469
Official Citation:Vibrational Sum Frequency Spectroscopic Investigation of the Azimuthal Anisotropy and Rotational Dynamics of Methyl-Terminated Silicon(111) Surfaces Sergey Malyk, Fadel Y. Shalhout, Leslie E. O’Leary, Nathan S. Lewis, and Alexander V. Benderskii The Journal of Physical Chemistry C 2013 117 (2), 935-944
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:37124
Collection:CaltechAUTHORS
Deposited By: Jason Perez
Deposited On:26 Feb 2013 20:01
Last Modified:09 Nov 2021 23:26

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