Tuning the magnetic properties of new layered iron chalcogenides (BaF)2Fe2- xQ3 (Q = S, Se) by changing the defect concentration on the iron sublattice

Mihai Sturza, Jared M. Allred, Christos D. Malliakas, Daniel E. Bugaris, Fei Han, Duck Young Chung, Mercouri G Kanatzidis

Research output: Contribution to journalArticle

14 Citations (Scopus)

Abstract

Effecting and controlling ferromagnetic-like properties in semiconductors has proven to be a complex problem, especially when approaching room temperature. Here, we demonstrate the important role of defects in the magnetic properties of semiconductors by reporting the structures and properties of the iron chalcogenides (BaF)2Fe2-xQ3 (Q = S, Se), which exhibit anomalous magnetic properties that are correlated with defects in the Fe-sublattice. The compounds form in both long-range ordered and disordered polytypes of a new structure typified by the alternate stacking of fluorite (BaF)22+ and (Fe2-xQ3)2- layers. The latter layers exhibit an ordered array of strong Fe-Fe dimers in edge-sharing tetrahedra. Given the strong Fe-Fe interaction, it is expected that the Fe-Fe dimer is antiferromagnetically coupled, yet crystals exhibit a weak ferromagnetic moment that orders at relatively high temperature: below 280-315 K and 240-275 K for the sulfide and selenide analogues, respectively. This transition temperature positively correlates with the concentration of defects in the Fe-sublattice, as determined by single-crystal X-ray diffraction. Our results indicate that internal defects in Fe2-xQ3 layers play an important role in dictating the magnetic properties of newly discovered (BaF)2Fe2-xQ3 (Q = S, Se), which can yield switchable ferromagnetically ordered moments at or above room temperature.

Original languageEnglish
Pages (from-to)3280-3290
Number of pages11
JournalChemistry of Materials
Volume27
Issue number9
DOIs
Publication statusPublished - May 12 2015

Fingerprint

Chalcogenides
Fluorspar
Magnetic properties
Iron
Tuning
Defects
Dimers
Semiconductor materials
Sulfides
Temperature
Superconducting transition temperature
Single crystals
X ray diffraction
Crystals

ASJC Scopus subject areas

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

Cite this

Tuning the magnetic properties of new layered iron chalcogenides (BaF)2Fe2- xQ3 (Q = S, Se) by changing the defect concentration on the iron sublattice. / Sturza, Mihai; Allred, Jared M.; Malliakas, Christos D.; Bugaris, Daniel E.; Han, Fei; Chung, Duck Young; Kanatzidis, Mercouri G.

In: Chemistry of Materials, Vol. 27, No. 9, 12.05.2015, p. 3280-3290.

Research output: Contribution to journalArticle

Sturza, Mihai ; Allred, Jared M. ; Malliakas, Christos D. ; Bugaris, Daniel E. ; Han, Fei ; Chung, Duck Young ; Kanatzidis, Mercouri G. / Tuning the magnetic properties of new layered iron chalcogenides (BaF)2Fe2- xQ3 (Q = S, Se) by changing the defect concentration on the iron sublattice. In: Chemistry of Materials. 2015 ; Vol. 27, No. 9. pp. 3280-3290.
@article{b26db539a296434e9db6652583b211cb,
title = "Tuning the magnetic properties of new layered iron chalcogenides (BaF)2Fe2- xQ3 (Q = S, Se) by changing the defect concentration on the iron sublattice",
abstract = "Effecting and controlling ferromagnetic-like properties in semiconductors has proven to be a complex problem, especially when approaching room temperature. Here, we demonstrate the important role of defects in the magnetic properties of semiconductors by reporting the structures and properties of the iron chalcogenides (BaF)2Fe2-xQ3 (Q = S, Se), which exhibit anomalous magnetic properties that are correlated with defects in the Fe-sublattice. The compounds form in both long-range ordered and disordered polytypes of a new structure typified by the alternate stacking of fluorite (BaF)22+ and (Fe2-xQ3)2- layers. The latter layers exhibit an ordered array of strong Fe-Fe dimers in edge-sharing tetrahedra. Given the strong Fe-Fe interaction, it is expected that the Fe-Fe dimer is antiferromagnetically coupled, yet crystals exhibit a weak ferromagnetic moment that orders at relatively high temperature: below 280-315 K and 240-275 K for the sulfide and selenide analogues, respectively. This transition temperature positively correlates with the concentration of defects in the Fe-sublattice, as determined by single-crystal X-ray diffraction. Our results indicate that internal defects in Fe2-xQ3 layers play an important role in dictating the magnetic properties of newly discovered (BaF)2Fe2-xQ3 (Q = S, Se), which can yield switchable ferromagnetically ordered moments at or above room temperature.",
author = "Mihai Sturza and Allred, {Jared M.} and Malliakas, {Christos D.} and Bugaris, {Daniel E.} and Fei Han and Chung, {Duck Young} and Kanatzidis, {Mercouri G}",
year = "2015",
month = "5",
day = "12",
doi = "10.1021/acs.chemmater.5b00287",
language = "English",
volume = "27",
pages = "3280--3290",
journal = "Chemistry of Materials",
issn = "0897-4756",
publisher = "American Chemical Society",
number = "9",

}

TY - JOUR

T1 - Tuning the magnetic properties of new layered iron chalcogenides (BaF)2Fe2- xQ3 (Q = S, Se) by changing the defect concentration on the iron sublattice

AU - Sturza, Mihai

AU - Allred, Jared M.

AU - Malliakas, Christos D.

AU - Bugaris, Daniel E.

AU - Han, Fei

AU - Chung, Duck Young

AU - Kanatzidis, Mercouri G

PY - 2015/5/12

Y1 - 2015/5/12

N2 - Effecting and controlling ferromagnetic-like properties in semiconductors has proven to be a complex problem, especially when approaching room temperature. Here, we demonstrate the important role of defects in the magnetic properties of semiconductors by reporting the structures and properties of the iron chalcogenides (BaF)2Fe2-xQ3 (Q = S, Se), which exhibit anomalous magnetic properties that are correlated with defects in the Fe-sublattice. The compounds form in both long-range ordered and disordered polytypes of a new structure typified by the alternate stacking of fluorite (BaF)22+ and (Fe2-xQ3)2- layers. The latter layers exhibit an ordered array of strong Fe-Fe dimers in edge-sharing tetrahedra. Given the strong Fe-Fe interaction, it is expected that the Fe-Fe dimer is antiferromagnetically coupled, yet crystals exhibit a weak ferromagnetic moment that orders at relatively high temperature: below 280-315 K and 240-275 K for the sulfide and selenide analogues, respectively. This transition temperature positively correlates with the concentration of defects in the Fe-sublattice, as determined by single-crystal X-ray diffraction. Our results indicate that internal defects in Fe2-xQ3 layers play an important role in dictating the magnetic properties of newly discovered (BaF)2Fe2-xQ3 (Q = S, Se), which can yield switchable ferromagnetically ordered moments at or above room temperature.

AB - Effecting and controlling ferromagnetic-like properties in semiconductors has proven to be a complex problem, especially when approaching room temperature. Here, we demonstrate the important role of defects in the magnetic properties of semiconductors by reporting the structures and properties of the iron chalcogenides (BaF)2Fe2-xQ3 (Q = S, Se), which exhibit anomalous magnetic properties that are correlated with defects in the Fe-sublattice. The compounds form in both long-range ordered and disordered polytypes of a new structure typified by the alternate stacking of fluorite (BaF)22+ and (Fe2-xQ3)2- layers. The latter layers exhibit an ordered array of strong Fe-Fe dimers in edge-sharing tetrahedra. Given the strong Fe-Fe interaction, it is expected that the Fe-Fe dimer is antiferromagnetically coupled, yet crystals exhibit a weak ferromagnetic moment that orders at relatively high temperature: below 280-315 K and 240-275 K for the sulfide and selenide analogues, respectively. This transition temperature positively correlates with the concentration of defects in the Fe-sublattice, as determined by single-crystal X-ray diffraction. Our results indicate that internal defects in Fe2-xQ3 layers play an important role in dictating the magnetic properties of newly discovered (BaF)2Fe2-xQ3 (Q = S, Se), which can yield switchable ferromagnetically ordered moments at or above room temperature.

UR - http://www.scopus.com/inward/record.url?scp=84929179435&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84929179435&partnerID=8YFLogxK

U2 - 10.1021/acs.chemmater.5b00287

DO - 10.1021/acs.chemmater.5b00287

M3 - Article

AN - SCOPUS:84929179435

VL - 27

SP - 3280

EP - 3290

JO - Chemistry of Materials

JF - Chemistry of Materials

SN - 0897-4756

IS - 9

ER -