First-principles approach to calculating energy level alignment at aqueous semiconductor interfaces

Neerav Kharche, James Muckerman, Mark S. Hybertsen

Research output: Contribution to journalArticle

49 Citations (Scopus)

Abstract

A first-principles approach is demonstrated for calculating the relationship between an aqueous semiconductor interface structure and energy level alignment. The physical interface structure is sampled using density functional theory based molecular dynamics, yielding the interface electrostatic dipole. The GW approach from many-body perturbation theory is used to place the electronic band edge energies of the semiconductor relative to the occupied 1b1 energy level in water. The application to the specific cases of nonpolar (101¯0) facets of GaN and ZnO reveals a significant role for the structural motifs at the interface, including the degree of interface water dissociation and the dynamical fluctuations in the interface Zn-O and O-H bond orientations. These effects contribute up to 0.5 eV.

Original languageEnglish
Article number176802
JournalPhysical Review Letters
Volume113
Issue number17
DOIs
Publication statusPublished - Oct 21 2014

Fingerprint

energy levels
alignment
water
flat surfaces
perturbation theory
dissociation
electrostatics
dipoles
molecular dynamics
density functional theory
electronics
energy

ASJC Scopus subject areas

  • Physics and Astronomy(all)

Cite this

First-principles approach to calculating energy level alignment at aqueous semiconductor interfaces. / Kharche, Neerav; Muckerman, James; Hybertsen, Mark S.

In: Physical Review Letters, Vol. 113, No. 17, 176802, 21.10.2014.

Research output: Contribution to journalArticle

@article{f1f8f509ccca46f78526aea7214db9be,
title = "First-principles approach to calculating energy level alignment at aqueous semiconductor interfaces",
abstract = "A first-principles approach is demonstrated for calculating the relationship between an aqueous semiconductor interface structure and energy level alignment. The physical interface structure is sampled using density functional theory based molecular dynamics, yielding the interface electrostatic dipole. The GW approach from many-body perturbation theory is used to place the electronic band edge energies of the semiconductor relative to the occupied 1b1 energy level in water. The application to the specific cases of nonpolar (101¯0) facets of GaN and ZnO reveals a significant role for the structural motifs at the interface, including the degree of interface water dissociation and the dynamical fluctuations in the interface Zn-O and O-H bond orientations. These effects contribute up to 0.5 eV.",
author = "Neerav Kharche and James Muckerman and Hybertsen, {Mark S.}",
year = "2014",
month = "10",
day = "21",
doi = "10.1103/PhysRevLett.113.176802",
language = "English",
volume = "113",
journal = "Physical Review Letters",
issn = "0031-9007",
publisher = "American Physical Society",
number = "17",

}

TY - JOUR

T1 - First-principles approach to calculating energy level alignment at aqueous semiconductor interfaces

AU - Kharche, Neerav

AU - Muckerman, James

AU - Hybertsen, Mark S.

PY - 2014/10/21

Y1 - 2014/10/21

N2 - A first-principles approach is demonstrated for calculating the relationship between an aqueous semiconductor interface structure and energy level alignment. The physical interface structure is sampled using density functional theory based molecular dynamics, yielding the interface electrostatic dipole. The GW approach from many-body perturbation theory is used to place the electronic band edge energies of the semiconductor relative to the occupied 1b1 energy level in water. The application to the specific cases of nonpolar (101¯0) facets of GaN and ZnO reveals a significant role for the structural motifs at the interface, including the degree of interface water dissociation and the dynamical fluctuations in the interface Zn-O and O-H bond orientations. These effects contribute up to 0.5 eV.

AB - A first-principles approach is demonstrated for calculating the relationship between an aqueous semiconductor interface structure and energy level alignment. The physical interface structure is sampled using density functional theory based molecular dynamics, yielding the interface electrostatic dipole. The GW approach from many-body perturbation theory is used to place the electronic band edge energies of the semiconductor relative to the occupied 1b1 energy level in water. The application to the specific cases of nonpolar (101¯0) facets of GaN and ZnO reveals a significant role for the structural motifs at the interface, including the degree of interface water dissociation and the dynamical fluctuations in the interface Zn-O and O-H bond orientations. These effects contribute up to 0.5 eV.

UR - http://www.scopus.com/inward/record.url?scp=84908148537&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84908148537&partnerID=8YFLogxK

U2 - 10.1103/PhysRevLett.113.176802

DO - 10.1103/PhysRevLett.113.176802

M3 - Article

AN - SCOPUS:84908148537

VL - 113

JO - Physical Review Letters

JF - Physical Review Letters

SN - 0031-9007

IS - 17

M1 - 176802

ER -