eprintid: 1395992
rev_number: 28
eprint_status: archive
userid: 608
dir: disk0/01/39/59/92
datestamp: 2013-06-11 19:37:44
lastmod: 2021-09-19 23:43:23
status_changed: 2013-06-11 19:37:44
type: article
metadata_visibility: show
item_issues_count: 0
creators_name: Scanlon, DO
creators_name: Kehoe, AB
creators_name: Watson, GW
creators_name: Jones, MO
creators_name: David, WI
creators_name: Payne, DJ
creators_name: Egdell, RG
creators_name: Edwards, PP
creators_name: Walsh, A
title: Nature of the band gap and origin of the conductivity of PbO2 revealed by theory and experiment.
ispublished: pub
divisions: UCL
divisions: B04
divisions: C06
divisions: F56
note: © 2011 American Physical Society
abstract: Lead dioxide has been used for over a century in the lead-acid battery. Many fundamental questions concerning PbO2 remain unanswered, principally: (i) is the bulk material a metal or a semiconductor, and (ii) what is the source of the high levels of conductivity? We calculate the electronic structure and defect physics of PbO2, using a hybrid density functional, and show that it is an n-type semiconductor with a small indirect band gap of ∼0.2  eV. The origin of electron carriers in the undoped material is found to be oxygen vacancies, which forms a donor state resonant in the conduction band. A dipole-forbidden band gap combined with a large carrier induced Moss-Burstein shift results in a large effective optical band gap. The model is supported by neutron diffraction, which reveals that the oxygen sublattice is only 98.4% occupied, thus confirming oxygen substoichiometry as the electron source.
date: 2011-12-09
official_url: http://dx.doi.org/10.1103/PhysRevLett.107.246402
vfaculties: VMPS
oa_status: green
language: eng
primo: open
primo_central: open_green
article_type_text: Journal Article
verified: verified_manual
elements_source: PubMed
elements_id: 875729
doi: 10.1103/PhysRevLett.107.246402
lyricists_name: Scanlon, David
lyricists_id: DSCAN57
full_text_status: public
publication: Physical Review Letters
volume: 107
number: 24
article_number: 246402
event_location: US
issn: 0031-9007
citation:        Scanlon, DO;    Kehoe, AB;    Watson, GW;    Jones, MO;    David, WI;    Payne, DJ;    Egdell, RG;         ... Walsh, A; + view all <#>        Scanlon, DO;  Kehoe, AB;  Watson, GW;  Jones, MO;  David, WI;  Payne, DJ;  Egdell, RG;  Edwards, PP;  Walsh, A;   - view fewer <#>    (2011)    Nature of the band gap and origin of the conductivity of PbO2 revealed by theory and experiment.                   Physical Review Letters , 107  (24)    , Article 246402.  10.1103/PhysRevLett.107.246402 <https://doi.org/10.1103/PhysRevLett.107.246402>.       Green open access   
 
document_url: https://discovery.ucl.ac.uk/id/eprint/1395992/1/1395992.pdf