Combined Theoretical and Experimental Study of Band-Edge Control of Si through Surface Functionalization
Abstract
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.
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.Attached Files
Published - jp3124583.pdf
Supplemental Material - jp3124583_si_001.pdf
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Additional details
- Eprint ID
- 37888
- Resolver ID
- CaltechAUTHORS:20130411-103710875
- Department of Energy (DOE)
- DE-AC02-98CH10886
- Link Foundation Energy fellowship
- NSF
- CHE-0802907
- Created
-
2013-04-11Created from EPrint's datestamp field
- Updated
-
2021-11-09Created from EPrint's last_modified field
- Caltech groups
- CCI Solar Fuels