DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Strong spin-lattice coupling in CrSiTe3

Abstract

CrSiTe3 has attracted recent interest as a candidate single-layer ferromagnetic semiconductor, but relatively little is known about the bulk properties of this material. Here, we report single-crystal X-ray diffraction, magnetic properties, thermal conductivity, vibrational, and optical spectroscopies and compare our findings with complementary electronic structure and lattice dynamics principles calculations. The high temperature paramagnetic phase is characterized by strong spin-lattice interactions that give rise to glassy behavior, negative thermal expansion, and an optical response that reveals that CrSiTe3 is an indirect gap semiconductor with indirect and direct band gaps at 0.4 and 1.2 eV, respectively. Measurements of the phonons across the 33 K ferromagnetic transition provide additional evidence for strong coupling between the magnetic and lattice degrees of freedom. In conclusion, the Si-Te stretching and Te displacement modes are sensitive to the magnetic ordering transition, a finding that we discuss in terms of the superexchange mechanism. Lastly, spin-lattice coupling constants are also extracted.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [2];  [3];  [3];  [3]; ORCiD logo [4];  [5];  [6];  [6]
  1. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Quantum Condensed Matter Division
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences
  4. Univ. of Florida, Gainesville, FL (United States). Dept. of Materials Science and Engineering
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
  6. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1265417
Grant/Contract Number:  
AC05-00OR22725; DMR 1410428; FG02-01ER-45885
Resource Type:
Accepted Manuscript
Journal Name:
APL Materials
Additional Journal Information:
Journal Volume: 3; Journal Issue: 4; Journal ID: ISSN 2166-532X
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Casto, L. D., Clune, A. J., Yokosuk, M. O., Musfeldt, J. L., Williams, T. J., Zhuang, H. L., Lin, M. -W., Xiao, K., Hennig, R. G., Sales, B. C., Yan, J. -Q., and Mandrus, D. Strong spin-lattice coupling in CrSiTe3. United States: N. p., 2015. Web. doi:10.1063/1.4914134.
Casto, L. D., Clune, A. J., Yokosuk, M. O., Musfeldt, J. L., Williams, T. J., Zhuang, H. L., Lin, M. -W., Xiao, K., Hennig, R. G., Sales, B. C., Yan, J. -Q., & Mandrus, D. Strong spin-lattice coupling in CrSiTe3. United States. https://doi.org/10.1063/1.4914134
Casto, L. D., Clune, A. J., Yokosuk, M. O., Musfeldt, J. L., Williams, T. J., Zhuang, H. L., Lin, M. -W., Xiao, K., Hennig, R. G., Sales, B. C., Yan, J. -Q., and Mandrus, D. Thu . "Strong spin-lattice coupling in CrSiTe3". United States. https://doi.org/10.1063/1.4914134. https://www.osti.gov/servlets/purl/1265417.
@article{osti_1265417,
title = {Strong spin-lattice coupling in CrSiTe3},
author = {Casto, L. D. and Clune, A. J. and Yokosuk, M. O. and Musfeldt, J. L. and Williams, T. J. and Zhuang, H. L. and Lin, M. -W. and Xiao, K. and Hennig, R. G. and Sales, B. C. and Yan, J. -Q. and Mandrus, D.},
abstractNote = {CrSiTe3 has attracted recent interest as a candidate single-layer ferromagnetic semiconductor, but relatively little is known about the bulk properties of this material. Here, we report single-crystal X-ray diffraction, magnetic properties, thermal conductivity, vibrational, and optical spectroscopies and compare our findings with complementary electronic structure and lattice dynamics principles calculations. The high temperature paramagnetic phase is characterized by strong spin-lattice interactions that give rise to glassy behavior, negative thermal expansion, and an optical response that reveals that CrSiTe3 is an indirect gap semiconductor with indirect and direct band gaps at 0.4 and 1.2 eV, respectively. Measurements of the phonons across the 33 K ferromagnetic transition provide additional evidence for strong coupling between the magnetic and lattice degrees of freedom. In conclusion, the Si-Te stretching and Te displacement modes are sensitive to the magnetic ordering transition, a finding that we discuss in terms of the superexchange mechanism. Lastly, spin-lattice coupling constants are also extracted.},
doi = {10.1063/1.4914134},
journal = {APL Materials},
number = 4,
volume = 3,
place = {United States},
year = {Thu Mar 19 00:00:00 EDT 2015},
month = {Thu Mar 19 00:00:00 EDT 2015}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 183 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

The time for CIGS
journal, August 2010

  • Tiwari, Ayodhya N.; Lincot, Daniel; Contreras, Miguel
  • Progress in Photovoltaics: Research and Applications, Vol. 18, Issue 6
  • DOI: 10.1002/pip.1010

Magnetic structure of the new layered ferromagnetic chromium hexatellurosilicate Cr2Si2Te6
journal, March 1991

  • Carteaux, V.; Ouvrard, G.; Grenier, J. C.
  • Journal of Magnetism and Magnetic Materials, Vol. 94, Issue 1-2
  • DOI: 10.1016/0304-8853(91)90121-P

Projector augmented-wave method
journal, December 1994


High-pressure synthesis and physical properties of perovskite and post-perovskite Ca 1 x Sr x Ir O 3
journal, February 2011


Special points for Brillouin-zone integrations
journal, June 1976

  • Monkhorst, Hendrik J.; Pack, James D.
  • Physical Review B, Vol. 13, Issue 12, p. 5188-5192
  • DOI: 10.1103/PhysRevB.13.5188

Magnetically Induced Phonon Anisotropy in ZnCr 2 O 4 from First Principles
journal, May 2006


Complex thermoelectric materials
journal, February 2008

  • Snyder, G. Jeffrey; Toberer, Eric S.
  • Nature Materials, Vol. 7, Issue 2, p. 105-114
  • DOI: 10.1038/nmat2090

Electronics and optoelectronics of two-dimensional transition metal dichalcogenides
journal, November 2012

  • Wang, Qing Hua; Kalantar-Zadeh, Kourosh; Kis, Andras
  • Nature Nanotechnology, Vol. 7, Issue 11, p. 699-712
  • DOI: 10.1038/nnano.2012.193

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


Superconductivity above 100 K in single-layer FeSe films on doped SrTiO3
journal, November 2014

  • Ge, Jian-Feng; Liu, Zhi-Long; Liu, Canhua
  • Nature Materials, Vol. 14, Issue 3
  • DOI: 10.1038/nmat4153

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Spin-glass behavior of the Cu2xCr2xSn2−2xS4 spinels: An antiferromagnetic frustrated lattice for x ⩽ 0.5
journal, January 1983


Photoconductivity in BiFeO3 thin films
journal, March 2008

  • Basu, S. R.; Martin, L. W.; Chu, Y. H.
  • Applied Physics Letters, Vol. 92, Issue 9
  • DOI: 10.1063/1.2887908

Superconducting Dome in a Gate-Tuned Band Insulator
journal, November 2012


A strong ferroelectric ferromagnet created by means of spin–lattice coupling
journal, August 2010

  • Lee, June Hyuk; Fang, Lei; Vlahos, Eftihia
  • Nature, Vol. 466, Issue 7309
  • DOI: 10.1038/nature09331

2D Ising-Like Ferromagnetic Behaviour for the Lamellar Cr 2 Si 2 Te 6 Compound: A Neutron Scattering Investigation
journal, January 1995


Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998

  • Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.
  • Physical Review B, Vol. 57, Issue 3, p. 1505-1509
  • DOI: 10.1103/PhysRevB.57.1505

Lattice dynamics of layered MP X 3 ( M= Mn,Fe,Ni,Zn; X= S,Se) compounds
journal, December 1988


Topological Insulator Materials
journal, October 2013

  • Ando, Yoichi
  • Journal of the Physical Society of Japan, Vol. 82, Issue 10, Article No. 102001
  • DOI: 10.7566/JPSJ.82.102001

Spectroscopic Signature of the Superparamagnetic Transition and Surface Spin Disorder in CoFe 2 O 4 Nanoparticles
journal, May 2012

  • Sun, Qi -C.; Birkel, Christina S.; Cao, Jinbo
  • ACS Nano, Vol. 6, Issue 6
  • DOI: 10.1021/nn301276q

CrXTe 3 (X = Si, Ge) nanosheets: two dimensional intrinsic ferromagnetic semiconductors
journal, January 2014

  • Li, Xingxing; Yang, Jinlong
  • Journal of Materials Chemistry C, Vol. 2, Issue 34
  • DOI: 10.1039/C4TC01193G

Spin and orbital ordering in Y 1 x La x VO 3
journal, December 2011


Crystallographic, magnetic and electronic structures of a new layered ferromagnetic compound Cr 2 Ge 2 Te 6
journal, January 1995


Bond-length fluctuations and the spin-state transition in L CoO 3 ( L = La , Pr, and Nd)
journal, April 2004


Synthesis and crystal structure of a new layered phase: The chromium hexatellurosilicate Cr2Si2Te6
journal, March 1988


An interpretation of the magnetic properties of the perovskite-type mixed crystals La1−xSrxCoO3−λ
journal, August 1958


Magnetic and Electric Phase Control in Epitaxial EuTiO 3 from First Principles
journal, December 2006


Superexchange interaction and symmetry properties of electron orbitals
journal, July 1959


A density-functional study of the adsorption of methane-thiol on the (111) surfaces of the Ni-group metals: II. Vibrational spectroscopy
journal, June 2010


Unusually Strong Orbit-Lattice Interactions in the R V O 3 Perovskites
journal, November 2004


Molybdenum disulphide/titanium dioxide nanocomposite-poly 3-hexylthiophene bulk heterojunction solar cell
journal, April 2012

  • Shanmugam, Mariyappan; Bansal, Tanesh; Durcan, Chris A.
  • Applied Physics Letters, Vol. 100, Issue 15
  • DOI: 10.1063/1.3703602

The crystal structure of Cr2Si2Te6: Corrigendum
journal, November 1988


Transition-metal dichalcogenides for spintronic applications: Spintronics beyond graphene
journal, August 2014

  • Zibouche, Nourdine; Kuc, Agnieszka; Musfeldt, Janice
  • Annalen der Physik, Vol. 526, Issue 9-10
  • DOI: 10.1002/andp.201400137

Single-layer MoS2 transistors
journal, January 2011

  • Radisavljevic, B.; Radenovic, A.; Brivio, J.
  • Nature Nanotechnology, Vol. 6, Issue 3, p. 147-150
  • DOI: 10.1038/nnano.2010.279

Bilbao Crystallographic Server : Useful Databases and Tools for Phase-Transition Studies
journal, January 2003


A ferromagnetic insulating substrate for the epitaxial growth of topological insulators
journal, September 2013

  • Ji, Huiwen; Stokes, R. A.; Alegria, L. D.
  • Journal of Applied Physics, Vol. 114, Issue 11
  • DOI: 10.1063/1.4822092

MoS 2 Nanosheet Phototransistors with Thickness-Modulated Optical Energy Gap
journal, June 2012

  • Lee, Hee Sung; Min, Sung-Wook; Chang, Youn-Gyung
  • Nano Letters, Vol. 12, Issue 7
  • DOI: 10.1021/nl301485q

Filled Skutterudite Antimonides: A New Class of Thermoelectric Materials
journal, May 1996


Theory of the Role of Covalence in the Perovskite-Type Manganites [ La ,   M ( II ) ] Mn O 3
journal, October 1955


Complex thermoelectric materials
book, October 2010


Voltage- and time-dependent valence state transition in cobalt oxide catalysts during the oxygen evolution reaction
journal, April 2020


Reducing Dzyaloshinskii-Moriya interaction and field-free spin-orbit torque switching in synthetic antiferromagnets
journal, May 2021


Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect
journal, February 2020


A strong ferroelectric ferromagnet created by means of spin–lattice coupling
journal, July 2011

  • Lee, June Hyuk; Fang, Lei; Vlahos, Eftihia
  • Nature, Vol. 476, Issue 7358
  • DOI: 10.1038/nature10219

Topological Insulator Materials
text, January 2013


Works referencing / citing this record:

Metal Thio- and Selenophosphates as Multifunctional van der Waals Layered Materials
journal, August 2017

  • Susner, Michael A.; Chyasnavichyus, Marius; McGuire, Michael A.
  • Advanced Materials, Vol. 29, Issue 38
  • DOI: 10.1002/adma.201602852

Intrinsic Van Der Waals Magnetic Materials from Bulk to the 2D Limit: New Frontiers of Spintronics
journal, May 2019


Intrinsic Negative Magnetoresistance in Van Der Waals FeNbTe 2 Single Crystals
journal, February 2019


Van der Waals 2D Transition Metal Tellurides
journal, August 2019

  • Su, Jianwei; Liu, Kailang; Wang, Fakun
  • Advanced Materials Interfaces, Vol. 6, Issue 19
  • DOI: 10.1002/admi.201900741

Magnetic Entropy Scaling in Ferromagnetic Semiconductor CrGeTe 3
journal, June 2019


Effect of Coulomb Interactions on the Electronic and Magnetic Properties of Two-Dimensional CrSiTe3 and CrGeTe3 Materials
journal, September 2018


Spin–lattice and electron–phonon coupling in 3d/5d hybrid Sr3NiIrO6
journal, August 2019


Thickness-dependent magnetic order in CrI3 single crystals
journal, September 2019


Critical behavior of the quasi-two-dimensional semiconducting ferromagnet CrSiTe3
journal, September 2016

  • Liu, Bingjie; Zou, Youming; Zhang, Lei
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep33873

Spin dynamics, electronic, and thermal transport properties of two-dimensional CrPS 4 single crystal
journal, January 2016

  • Pei, Q. L.; Luo, X.; Lin, G. T.
  • Journal of Applied Physics, Vol. 119, Issue 4
  • DOI: 10.1063/1.4940948

Effects of hydrostatic pressure on spin-lattice coupling in two-dimensional ferromagnetic Cr 2 Ge 2 Te 6
journal, February 2018

  • Sun, Y.; Xiao, R. C.; Lin, G. T.
  • Applied Physics Letters, Vol. 112, Issue 7
  • DOI: 10.1063/1.5016568

First-principles study the single-layer transition metal trihalide CrXSe 3 (X  =  Sn, Ge, Si) as monolayer ferromagnetic semiconductor
journal, November 2019

  • Shen, Zihan; Fan, Xiaoli; Yang, Danxi
  • Journal of Physics: Condensed Matter, Vol. 32, Issue 8
  • DOI: 10.1088/1361-648x/ab462a

Electrically tunable exchange splitting in bilayer graphene on monolayer Cr 2 X 2 Te 6 with X = Ge, Si, and Sn
journal, July 2018

  • Zollner, Klaus; Gmitra, Martin; Fabian, Jaroslav
  • New Journal of Physics, Vol. 20, Issue 7
  • DOI: 10.1088/1367-2630/aace51

Magneto-elastic coupling in a potential ferromagnetic 2D atomic crystal
journal, June 2016


Electric field effect in multilayer Cr 2 Ge 2 Te 6 : a ferromagnetic 2D material
journal, May 2017


First-principles studies of spin-phonon coupling in monolayer C r 2 G e 2 T e 6
journal, December 2019


Magnetic dimerization in the frustrated spin ladder Li 2 Cu 2 O ( SO 4 ) 2
journal, November 2017


Anisotropic magnetic entropy change in Cr 2 X 2 Te 6 ( X = Si and Ge )
journal, January 2019


Emergence of Kondo lattice behavior in a van der Waals itinerant ferromagnet, Fe 3 GeTe 2
journal, January 2018


Nearly room temperature ferromagnetism in a magnetic metal-rich van der Waals metal
journal, January 2020


Two-dimensional magnetic crystals and emergent heterostructure devices
journal, February 2019


Ab Initio Study of Optoelectronic and Magnetic Properties of Ternary Chromium Chalcogenides
journal, November 2018

  • Ong, Marc; Hammouri, Mahmoud; Jishi, Radi A.
  • Advances in Materials Science and Engineering, Vol. 2018
  • DOI: 10.1155/2018/3762451

Magnetic ground state of semiconducting transition metal trichalcogenide monolayers
text, January 2015

  • Sivadas, Nikhil; Daniels, Matthew W.; Swendsen, Robert
  • Carnegie Mellon University
  • DOI: 10.1184/r1/6507131.v1

Magnetic ground state of semiconducting transition metal trichalcogenide monolayers
text, January 2015


Gate-controllable magneto-optic Kerr effect in layered collinear antiferromagnets
text, January 2016


Spin-lattice and electron-phonon coupling in 3$d$/5$d$ hybrid Sr$_3$NiIrO$_6$
text, January 2019


Thickness-dependent magnetic order in CrI$_3$ single crystals
text, January 2019


Dimensional crossover in a layered ferromagnet detected by spin correlation driven distortions
journal, April 2019