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Title: Hole doping and pressure effects on the II-II-V-based diluted magnetic semiconductor ( B a 1 - x K x ) ( Z n 1 - y M n y ) 2 A s 2

Abstract

We investigate doping- and pressure-induced changes in the electronic state of Mn 3d and As 4p orbitals in II-II-V based diluted magnetic semiconductor (Ba 1-x,K x)(Zn 1-y,Mn y) 2As 2 to shed light into the mechanism of indirect exchange interactions leading to high ferromagnetic ordering temperature (T c = 230 K in optimally doped samples). A suite of x-ray spectroscopy experiments (emission, absorption and dichroism) show that the emergence, and further enhancement of ferromagnetic interactions with increased hole doping into the As 4p band is accompanied by a decrease in local 3d spin density at Mn sites. This is a result of increasing Mn 3d - As 4p hybridization with hole doping which enhances indirect exchange interactions between Mn dopants and gives rise to induced magnetic polarization in As 4p states. On the contrary, application of pressure suppresses exchange interactions. While Mn Kβ emission spectra show a weak response of 3d state to pressure, clear As 4p band broadening (hole delocalization) is observed under pressure ultimately leading to loss of ferromagnetism concomitant with a semiconductor to metal transition. The pressure response of As 4p and Mn 3d states is intimately connected with the evolution of the As-As interlayer distance andmore » the geometry of the MnAs 4 tetrahedral units, which we probed with X-ray diffraction. Our results indicate that hole doping increases the degree of covalency between the anion (As) p states and cation (Mn) d states in the MnA s4 tetrahedron, a crucial ingredient to promote indirect exchange interactions between Mn dopants and high T c ferromagnetism. As a result, the instability of ferromagnetism and semiconducting state against pressure is mainly dictated by delocalization of anion p states.« less

Authors:
 [1];  [2];  [3];  [2];  [4];  [5];  [5];  [5];  [6];  [4];  [6];  [7]
  1. Chinese Academy of Sciences (CAS), Beijing (China); Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Chinese Academy of Sciences (CAS), Beijing (China)
  3. Argonne National Lab. (ANL), Argonne, IL (United States); Brazilian Synchrotron Light Lab. (LNLS), Campinas, SP (Brazil)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Carnegie Inst. of Washington, Argonne, IL (United States)
  6. Carnegie Inst. of Washington, Argonne, IL (United States); Center for High Pressure Science and Technology Advanced Research (HPSTAR), Shanghai (China)
  7. Chinese Academy of Sciences (CAS), Beijing (China); Collaborative Innovation Center of Quantum Matter, Beijing (China); Univ. of Chinese Academy of Sciences, Beijing (China)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1373594
Alternate Identifier(s):
OSTI ID: 1346761
Grant/Contract Number:  
AC02-06CH11357; FG02-99ER45775; NA0001974
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 95; Journal Issue: 9; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Sun, F., Zhao, G. Q., Escanhoela, Jr., C. A., Chen, B. J., Kou, R. H., Wang, Y. G., Xiao, Y. M., Chow, P., Mao, H. K., Haskel, D., Yang, W. G., and Jin, C. Q. Hole doping and pressure effects on the II-II-V-based diluted magnetic semiconductor (Ba1-xKx)(Zn1-yMny)2As2. United States: N. p., 2017. Web. doi:10.1103/PhysRevB.95.094412.
Sun, F., Zhao, G. Q., Escanhoela, Jr., C. A., Chen, B. J., Kou, R. H., Wang, Y. G., Xiao, Y. M., Chow, P., Mao, H. K., Haskel, D., Yang, W. G., & Jin, C. Q. Hole doping and pressure effects on the II-II-V-based diluted magnetic semiconductor (Ba1-xKx)(Zn1-yMny)2As2. United States. doi:10.1103/PhysRevB.95.094412.
Sun, F., Zhao, G. Q., Escanhoela, Jr., C. A., Chen, B. J., Kou, R. H., Wang, Y. G., Xiao, Y. M., Chow, P., Mao, H. K., Haskel, D., Yang, W. G., and Jin, C. Q. Mon . "Hole doping and pressure effects on the II-II-V-based diluted magnetic semiconductor (Ba1-xKx)(Zn1-yMny)2As2". United States. doi:10.1103/PhysRevB.95.094412. https://www.osti.gov/servlets/purl/1373594.
@article{osti_1373594,
title = {Hole doping and pressure effects on the II-II-V-based diluted magnetic semiconductor (Ba1-xKx)(Zn1-yMny)2As2},
author = {Sun, F. and Zhao, G. Q. and Escanhoela, Jr., C. A. and Chen, B. J. and Kou, R. H. and Wang, Y. G. and Xiao, Y. M. and Chow, P. and Mao, H. K. and Haskel, D. and Yang, W. G. and Jin, C. Q.},
abstractNote = {We investigate doping- and pressure-induced changes in the electronic state of Mn 3d and As 4p orbitals in II-II-V based diluted magnetic semiconductor (Ba1-x,Kx)(Zn1-y,Mny)2As2 to shed light into the mechanism of indirect exchange interactions leading to high ferromagnetic ordering temperature (Tc = 230 K in optimally doped samples). A suite of x-ray spectroscopy experiments (emission, absorption and dichroism) show that the emergence, and further enhancement of ferromagnetic interactions with increased hole doping into the As 4p band is accompanied by a decrease in local 3d spin density at Mn sites. This is a result of increasing Mn 3d - As 4p hybridization with hole doping which enhances indirect exchange interactions between Mn dopants and gives rise to induced magnetic polarization in As 4p states. On the contrary, application of pressure suppresses exchange interactions. While Mn Kβ emission spectra show a weak response of 3d state to pressure, clear As 4p band broadening (hole delocalization) is observed under pressure ultimately leading to loss of ferromagnetism concomitant with a semiconductor to metal transition. The pressure response of As 4p and Mn 3d states is intimately connected with the evolution of the As-As interlayer distance and the geometry of the MnAs4 tetrahedral units, which we probed with X-ray diffraction. Our results indicate that hole doping increases the degree of covalency between the anion (As) p states and cation (Mn) d states in the MnAs4 tetrahedron, a crucial ingredient to promote indirect exchange interactions between Mn dopants and high Tc ferromagnetism. As a result, the instability of ferromagnetism and semiconducting state against pressure is mainly dictated by delocalization of anion p states.},
doi = {10.1103/PhysRevB.95.094412},
journal = {Physical Review B},
issn = {2469-9950},
number = 9,
volume = 95,
place = {United States},
year = {2017},
month = {3}
}

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Works referenced in this record:

ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
journal, June 2005


Narrow Bandgap in β-BaZn 2 As 2 and Its Chemical Origins
journal, October 2014

  • Xiao, Zewen; Hiramatsu, Hidenori; Ueda, Shigenori
  • Journal of the American Chemical Society, Vol. 136, Issue 42
  • DOI: 10.1021/ja507890u

Spintronics: Fundamentals and applications
journal, April 2004


Probing the 3d Spin Momentum with X-ray Emission Spectroscopy:  The Case of Molecular-Spin Transitions
journal, June 2006

  • Vankó, György; Neisius, Thomas; Molnár, Gábor
  • The Journal of Physical Chemistry B, Vol. 110, Issue 24
  • DOI: 10.1021/jp0615961

What does the K-edge x-ray magnetic circular dichroism spectrum tell us?
journal, December 1996


The forbidden gap and insulator-metal transition under pressure
journal, July 2002

  • Zarochentsev, E. V.; Troitskaya, E. P.
  • Physics of the Solid State, Vol. 44, Issue 7
  • DOI: 10.1134/1.1494638

Ferromagnetism at 230 K in (Ba0.7K0.3)(Zn0.85Mn0.15)2As2 diluted magnetic semiconductor
journal, May 2014


X-ray Mn K β emission spectra of manganese oxides and manganates
journal, January 1976

  • Tsutsumi, Kenjiro; Nakamori, Hiroo; Ichikawa, Kouichi
  • Physical Review B, Vol. 13, Issue 2
  • DOI: 10.1103/PhysRevB.13.929

Hole-mediated ferromagnetism in tetrahedrally coordinated semiconductors
journal, April 2001


Experimental probing of the interplay between ferromagnetism and localization in (Ga, Mn)As
journal, November 2009

  • Sawicki, Maciej; Chiba, Daichi; Korbecka, Anna
  • Nature Physics, Vol. 6, Issue 1
  • DOI: 10.1038/nphys1455

High resolution 1s core hole X-ray spectroscopy in 3d transition metal complexes—electronic and structural information
journal, January 2005


X-ray circular dichroism and local magnetic fields
journal, February 1993


Pressure-induced ferromagnetism in (In,Mn)Sb dilute magnetic semiconductor
journal, May 2005

  • Csontos, M.; Mihály, G.; Jankó, B.
  • Nature Materials, Vol. 4, Issue 6
  • DOI: 10.1038/nmat1388

Transformation of GaAs into an indirect L -band-gap semiconductor under uniaxial strain
journal, August 2009


(Ga,Mn)As under pressure: A first-principles investigation
journal, May 2015


Insulating Nickel at a Pressure of 34 TPa
journal, October 1982


A ten-year perspective on dilute magnetic semiconductors and oxides
journal, November 2010


Superconductivity at 38 K in the Iron Arsenide ( Ba 1 x K x ) Fe 2 As 2
journal, September 2008


High resolution study of Kβ′ and Kβ1,3 X-ray emission lines from Mn-compounds
journal, February 2010


Theory of Mn-doped II-II-V semiconductors
journal, October 2014


Making Nonmagnetic Semiconductors Ferromagnetic
journal, August 1998


Li(Zn,Mn)As as a new generation ferromagnet based on a I–II–V semiconductor
journal, August 2011

  • Deng, Z.; Jin, C. Q.; Liu, Q. Q.
  • Nature Communications, Vol. 2, Issue 1
  • DOI: 10.1038/ncomms1425

X-ray magnetic circular dichroism—a high energy probe of magnetic properties
journal, January 2005

  • Funk, Tobias; Deb, Aniruddha; George, Simon J.
  • Coordination Chemistry Reviews, Vol. 249, Issue 1-2
  • DOI: 10.1016/j.ccr.2004.05.017

Metal Kβ X-ray emission spectra of first row transition metal compounds
journal, February 2001

  • Gamblin, Stuart D.; Urch, David S.
  • Journal of Electron Spectroscopy and Related Phenomena, Vol. 113, Issue 2-3
  • DOI: 10.1016/S0368-2048(00)00416-3

Effect of hydrostatic pressure on the transport properties in magnetic semiconductors
journal, December 2004


Roadmap for Emerging Materials for Spintronic Device Applications
journal, October 2015

  • Hirohata, Atsufumi; Sukegawa, Hiroaki; Yanagihara, Hideto
  • IEEE Transactions on Magnetics, Vol. 51, Issue 10
  • DOI: 10.1109/TMAG.2015.2457393

Chemical dependence of interatomic X-ray transition energies and intensities – a study of Mn Kβ″ and Kβ2,5 spectra
journal, March 1999


X-ray circular dichroism as a probe of orbital magnetization
journal, March 1992


A XANES study of mixed-valence transition-metal oxides and rare-earth alloys
journal, May 1983


High-resolution manganese x-ray fluorescence spectroscopy. Oxidation-state and spin-state sensitivity
journal, April 1994

  • Peng, G.; deGroot, F. M. F.; Haemaelaeinen, K.
  • Journal of the American Chemical Society, Vol. 116, Issue 7
  • DOI: 10.1021/ja00086a024

(Ga,Mn)As: A new diluted magnetic semiconductor based on GaAs
journal, July 1996

  • Ohno, H.; Shen, A.; Matsukura, F.
  • Applied Physics Letters, Vol. 69, Issue 3
  • DOI: 10.1063/1.118061

Dilute ferromagnetic semiconductors: Physics and spintronic structures
journal, March 2014


Controlling the Curie temperature in (Ga,Mn)As through location of the Fermi level within the impurity band
journal, February 2012

  • Dobrowolska, M.; Tivakornsasithorn, K.; Liu, X.
  • Nature Materials, Vol. 11, Issue 5
  • DOI: 10.1038/nmat3250