Experimental characterization of a theoretically designed candidate p-type transparent conducting oxide

Li-doped Cr2MnO4

Arpun R. Nagaraja, Kevin H. Stone, Michael F. Toney, Haowei Peng, Stephan Lany, Thomas O Mason

Research output: Contribution to journalArticle

10 Citations (Scopus)

Abstract

The development of a p-type transparent conducting oxide (p-TCO) requires the deliberate design of a wide band gap and high hole conductivity. Using high-throughput theoretical screening, Cr2MnO4 was earlier predicted to be a p-TCO when doped with lithium. This constitutes a new class of p-TCO, one based on a tetrahedrally coordinated d5 cation. In this study, we examine and experimentally validate a few central properties of this system. Combined neutron diffraction and anomalous X-ray diffraction experiments give site occupancy that supports the theoretical prediction that lithium occupies the tetrahedral (Mn) site. The lattice parameter of the spinel decreases with lithium content to a solubility limit of [Li]/([Li] + [Mn]) ∼ 9.5%. Diffuse reflectance spectroscopy measurements show that at higher doping levels the transparency is diminished, which is attributed to both the presence of octahedral Mn and the increased hole content. Room-temperature electrical measurements of doped samples reveal an increase in conductivity of several orders of magnitude as compared to that of undoped samples, and high-temperature measurements show that Cr2MnO4 is a band conductor, as predicted by theory. The overall agreement between theory and experiment illustrates the advantages of a theory-driven approach to materials design.

Original languageEnglish
Pages (from-to)4598-4604
Number of pages7
JournalChemistry of Materials
Volume26
Issue number15
DOIs
Publication statusPublished - Aug 12 2014

Fingerprint

Lithium
Oxides
Neutron diffraction
Temperature measurement
Transparency
Lattice constants
Cations
Screening
Energy gap
Solubility
Positive ions
Experiments
Doping (additives)
Throughput
Spectroscopy
X ray diffraction
Temperature

ASJC Scopus subject areas

  • Materials Chemistry
  • Chemical Engineering(all)
  • Chemistry(all)

Cite this

Experimental characterization of a theoretically designed candidate p-type transparent conducting oxide : Li-doped Cr2MnO4. / Nagaraja, Arpun R.; Stone, Kevin H.; Toney, Michael F.; Peng, Haowei; Lany, Stephan; Mason, Thomas O.

In: Chemistry of Materials, Vol. 26, No. 15, 12.08.2014, p. 4598-4604.

Research output: Contribution to journalArticle

Nagaraja, Arpun R. ; Stone, Kevin H. ; Toney, Michael F. ; Peng, Haowei ; Lany, Stephan ; Mason, Thomas O. / Experimental characterization of a theoretically designed candidate p-type transparent conducting oxide : Li-doped Cr2MnO4. In: Chemistry of Materials. 2014 ; Vol. 26, No. 15. pp. 4598-4604.
@article{a7b690e5c399481f9a8f805675b4172f,
title = "Experimental characterization of a theoretically designed candidate p-type transparent conducting oxide: Li-doped Cr2MnO4",
abstract = "The development of a p-type transparent conducting oxide (p-TCO) requires the deliberate design of a wide band gap and high hole conductivity. Using high-throughput theoretical screening, Cr2MnO4 was earlier predicted to be a p-TCO when doped with lithium. This constitutes a new class of p-TCO, one based on a tetrahedrally coordinated d5 cation. In this study, we examine and experimentally validate a few central properties of this system. Combined neutron diffraction and anomalous X-ray diffraction experiments give site occupancy that supports the theoretical prediction that lithium occupies the tetrahedral (Mn) site. The lattice parameter of the spinel decreases with lithium content to a solubility limit of [Li]/([Li] + [Mn]) ∼ 9.5{\%}. Diffuse reflectance spectroscopy measurements show that at higher doping levels the transparency is diminished, which is attributed to both the presence of octahedral Mn and the increased hole content. Room-temperature electrical measurements of doped samples reveal an increase in conductivity of several orders of magnitude as compared to that of undoped samples, and high-temperature measurements show that Cr2MnO4 is a band conductor, as predicted by theory. The overall agreement between theory and experiment illustrates the advantages of a theory-driven approach to materials design.",
author = "Nagaraja, {Arpun R.} and Stone, {Kevin H.} and Toney, {Michael F.} and Haowei Peng and Stephan Lany and Mason, {Thomas O}",
year = "2014",
month = "8",
day = "12",
doi = "10.1021/cm501974t",
language = "English",
volume = "26",
pages = "4598--4604",
journal = "Chemistry of Materials",
issn = "0897-4756",
publisher = "American Chemical Society",
number = "15",

}

TY - JOUR

T1 - Experimental characterization of a theoretically designed candidate p-type transparent conducting oxide

T2 - Li-doped Cr2MnO4

AU - Nagaraja, Arpun R.

AU - Stone, Kevin H.

AU - Toney, Michael F.

AU - Peng, Haowei

AU - Lany, Stephan

AU - Mason, Thomas O

PY - 2014/8/12

Y1 - 2014/8/12

N2 - The development of a p-type transparent conducting oxide (p-TCO) requires the deliberate design of a wide band gap and high hole conductivity. Using high-throughput theoretical screening, Cr2MnO4 was earlier predicted to be a p-TCO when doped with lithium. This constitutes a new class of p-TCO, one based on a tetrahedrally coordinated d5 cation. In this study, we examine and experimentally validate a few central properties of this system. Combined neutron diffraction and anomalous X-ray diffraction experiments give site occupancy that supports the theoretical prediction that lithium occupies the tetrahedral (Mn) site. The lattice parameter of the spinel decreases with lithium content to a solubility limit of [Li]/([Li] + [Mn]) ∼ 9.5%. Diffuse reflectance spectroscopy measurements show that at higher doping levels the transparency is diminished, which is attributed to both the presence of octahedral Mn and the increased hole content. Room-temperature electrical measurements of doped samples reveal an increase in conductivity of several orders of magnitude as compared to that of undoped samples, and high-temperature measurements show that Cr2MnO4 is a band conductor, as predicted by theory. The overall agreement between theory and experiment illustrates the advantages of a theory-driven approach to materials design.

AB - The development of a p-type transparent conducting oxide (p-TCO) requires the deliberate design of a wide band gap and high hole conductivity. Using high-throughput theoretical screening, Cr2MnO4 was earlier predicted to be a p-TCO when doped with lithium. This constitutes a new class of p-TCO, one based on a tetrahedrally coordinated d5 cation. In this study, we examine and experimentally validate a few central properties of this system. Combined neutron diffraction and anomalous X-ray diffraction experiments give site occupancy that supports the theoretical prediction that lithium occupies the tetrahedral (Mn) site. The lattice parameter of the spinel decreases with lithium content to a solubility limit of [Li]/([Li] + [Mn]) ∼ 9.5%. Diffuse reflectance spectroscopy measurements show that at higher doping levels the transparency is diminished, which is attributed to both the presence of octahedral Mn and the increased hole content. Room-temperature electrical measurements of doped samples reveal an increase in conductivity of several orders of magnitude as compared to that of undoped samples, and high-temperature measurements show that Cr2MnO4 is a band conductor, as predicted by theory. The overall agreement between theory and experiment illustrates the advantages of a theory-driven approach to materials design.

UR - http://www.scopus.com/inward/record.url?scp=84905964476&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84905964476&partnerID=8YFLogxK

U2 - 10.1021/cm501974t

DO - 10.1021/cm501974t

M3 - Article

VL - 26

SP - 4598

EP - 4604

JO - Chemistry of Materials

JF - Chemistry of Materials

SN - 0897-4756

IS - 15

ER -