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Combined Theoretical and Experimental Study of Band-Edge Control of Si through Surface Functionalization

Li, Yan and O'Leary, Leslie E. and Lewis, Nathan S. and Galli, Giulia A. (2013) Combined Theoretical and Experimental Study of Band-Edge Control of Si through Surface Functionalization. Journal of Physical Chemistry C, 117 (10). pp. 5188-5194. ISSN 1932-7447. doi:10.1021/jp3124583.

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The band-edge positions of H-, Cl-, Br-, methyl-, and ethyl-terminated Si(111) surfaces were investigated through a combination of density functional theory (DFT) and many-body perturbation theory, as well as by photoelectron spectroscopy and electrical device measurements. The calculated trends in surface potential shifts as a function of the adsorbate type and coverage are consistent with the calculated strength and direction of the dipole moment of the adsorbate radicals in conjunction with simple electronegativity-based expectations. The quasi-particle energies, such as the ionization potential (IP), that were calculated by use of many-body perturbation theory were in good agreement with experiment. The IP values that were calculated by DFT exhibited substantial errors, but nevertheless, the IP differences, i.e., IP_(R–Si(111))–IP_(H–Si(111)), computed using DFT were in good agreement with spectroscopic and electrical measurements.

Item Type:Article
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Lewis, Nathan S.0000-0001-5245-0538
Additional Information:© 2013 American Chemical Society. Received: December 18, 2012; Revised: February 5, 2013; Published: February 13, 2013. Y.L. was supported by Brookhaven Science Associates, LLC under Contract No. DE-AC02-98CH10886, with the U.S. Department of Energy. L.E.O. was supported through a Link Foundation Energy fellowship. Part of the work was funded by NSF-CHE-0802907. The calculations were performed at the NERSC and TeraGrid facilities. We thank M. Hybertsen for useful discussions.
Group:CCI Solar Fuels
Funding AgencyGrant Number
Department of Energy (DOE)DE-AC02-98CH10886
Link Foundation Energy fellowshipUNSPECIFIED
Issue or Number:10
Record Number:CaltechAUTHORS:20130411-103710875
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Official Citation:Combined Theoretical and Experimental Study of Band-Edge Control of Si through Surface Functionalization Yan Li, Leslie E. O’Leary, Nathan S. Lewis, and Giulia Galli The Journal of Physical Chemistry C 2013 117 (10), 5188-5194
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:37888
Deposited On:11 Apr 2013 18:21
Last Modified:09 Nov 2021 23:32

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