Combined theoretical and experimental study of band-edge control of Si through surface functionalization

Yan Li, Leslie E. O'Leary, Nathan S Lewis, Giulia Galli

Research output: Contribution to journalArticle

38 Citations (Scopus)

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)-IPH-Si(111), computed using DFT were in good agreement with spectroscopic and electrical measurements.

Original languageEnglish
Pages (from-to)5188-5194
Number of pages7
JournalJournal of Physical Chemistry C
Volume117
Issue number10
DOIs
Publication statusPublished - Mar 14 2013

Fingerprint

Ionization potential
ionization potentials
Density functional theory
Adsorbates
density functional theory
perturbation theory
Electronegativity
Dipole moment
Surface potential
elementary excitations
Photoelectron spectroscopy
particle energy
electrical measurement
dipole moments
photoelectron spectroscopy
trends
shift
Experiments

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Electronic, Optical and Magnetic Materials
  • Surfaces, Coatings and Films
  • Energy(all)

Cite this

Combined theoretical and experimental study of band-edge control of Si through surface functionalization. / Li, Yan; O'Leary, Leslie E.; Lewis, Nathan S; Galli, Giulia.

In: Journal of Physical Chemistry C, Vol. 117, No. 10, 14.03.2013, p. 5188-5194.

Research output: Contribution to journalArticle

@article{e7eb3be1b0564b0fba1f20cdff31d624,
title = "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)-IPH-Si(111), computed using DFT were in good agreement with spectroscopic and electrical measurements.",
author = "Yan Li and O'Leary, {Leslie E.} and Lewis, {Nathan S} and Giulia Galli",
year = "2013",
month = "3",
day = "14",
doi = "10.1021/jp3124583",
language = "English",
volume = "117",
pages = "5188--5194",
journal = "Journal of Physical Chemistry C",
issn = "1932-7447",
publisher = "American Chemical Society",
number = "10",

}

TY - JOUR

T1 - Combined theoretical and experimental study of band-edge control of Si through surface functionalization

AU - Li, Yan

AU - O'Leary, Leslie E.

AU - Lewis, Nathan S

AU - Galli, Giulia

PY - 2013/3/14

Y1 - 2013/3/14

N2 - 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)-IPH-Si(111), computed using DFT were in good agreement with spectroscopic and electrical measurements.

AB - 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)-IPH-Si(111), computed using DFT were in good agreement with spectroscopic and electrical measurements.

UR - http://www.scopus.com/inward/record.url?scp=84874492315&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84874492315&partnerID=8YFLogxK

U2 - 10.1021/jp3124583

DO - 10.1021/jp3124583

M3 - Article

AN - SCOPUS:84874492315

VL - 117

SP - 5188

EP - 5194

JO - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

SN - 1932-7447

IS - 10

ER -