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Title: Revisiting Photoemission and Inverse Photoemission Spectra of Nickel Oxide from First Principles: Implications for Solar Energy Conversion

Abstract

We use two different ab initio quantum mechanics methods, complete active space self-consistent field theory applied to electrostatically embedded clusters and periodic many-body G₀W₀ calculations, to reanalyze the states formed in nickel(II) oxide upon electron addition and ionization. In agreement with interpretations of earlier measurements, we find that the valence and conduction band edges consist of oxygen and nickel states, respectively. However, contrary to conventional wisdom, we find that the oxygen states of the valence band edge are localized whereas the nickel states at the conduction band edge are delocalized. We argue that these characteristics may lead to low electron-hole recombination and relatively efficient electron transport, which, coupled with band gap engineering, could produce higher solar energy conversion efficiency compared to that of other transition-metal oxides. Both methods find a photoemission/inverse-photoemission gap of 3.6-3.9 eV, in good agreement with the experimental range, lending credence to our analysis of the electronic structure of NiO.

Authors:
; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1222109
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Physical Chemistry B, 118(28):7963–7971
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Alidoust, Nima, Toroker, Maytal, and Carter, Emily A. Revisiting Photoemission and Inverse Photoemission Spectra of Nickel Oxide from First Principles: Implications for Solar Energy Conversion. United States: N. p., 2014. Web. doi:10.1021/jp500878s.
Alidoust, Nima, Toroker, Maytal, & Carter, Emily A. Revisiting Photoemission and Inverse Photoemission Spectra of Nickel Oxide from First Principles: Implications for Solar Energy Conversion. United States. doi:10.1021/jp500878s.
Alidoust, Nima, Toroker, Maytal, and Carter, Emily A. Thu . "Revisiting Photoemission and Inverse Photoemission Spectra of Nickel Oxide from First Principles: Implications for Solar Energy Conversion". United States. doi:10.1021/jp500878s.
@article{osti_1222109,
title = {Revisiting Photoemission and Inverse Photoemission Spectra of Nickel Oxide from First Principles: Implications for Solar Energy Conversion},
author = {Alidoust, Nima and Toroker, Maytal and Carter, Emily A.},
abstractNote = {We use two different ab initio quantum mechanics methods, complete active space self-consistent field theory applied to electrostatically embedded clusters and periodic many-body G₀W₀ calculations, to reanalyze the states formed in nickel(II) oxide upon electron addition and ionization. In agreement with interpretations of earlier measurements, we find that the valence and conduction band edges consist of oxygen and nickel states, respectively. However, contrary to conventional wisdom, we find that the oxygen states of the valence band edge are localized whereas the nickel states at the conduction band edge are delocalized. We argue that these characteristics may lead to low electron-hole recombination and relatively efficient electron transport, which, coupled with band gap engineering, could produce higher solar energy conversion efficiency compared to that of other transition-metal oxides. Both methods find a photoemission/inverse-photoemission gap of 3.6-3.9 eV, in good agreement with the experimental range, lending credence to our analysis of the electronic structure of NiO.},
doi = {10.1021/jp500878s},
journal = {Journal of Physical Chemistry B, 118(28):7963–7971},
number = ,
volume = ,
place = {United States},
year = {Thu Jul 17 00:00:00 EDT 2014},
month = {Thu Jul 17 00:00:00 EDT 2014}
}