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Title: RNi{sub 8}Si{sub 3} (R=Gd,Tb): Novel ternary ordered derivatives of the BaCd{sub 11} type

Abstract

The title compounds have been synthesized and characterized both from the structural and magnetic point of view. Both crystallize in a new monoclinic structure strictly related to the tetragonal BaCd{sub 11} type. The structure was solved by means of X-ray single-crystal techniques for GdNi{sub 8}Si{sub 3} and confirmed for TbNi{sub 8}Si{sub 3} on powder data; the corresponding lattice parameters (obtained from Guinier powder patterns) are a=6.3259(2), b=13.7245(5), c=7.4949(3) Å, β=113.522(3)°, V{sub cell}=596.64(3) Å{sup 3} and a=6.3200(2), b=13.6987(4), c=7.4923(2) Å, β=113.494(2)°, V{sub cell}=594.88(2) Å{sup 3}. The symmetry relationship between the tI48-I4{sub 1}/amd BaCd{sub 11} aristotype and the new ordered mS48-C2/c GdNi{sub 8}Si{sub 3} derivative is described via the Bärnighausen formalism within the group theory. The large Gd–Gd (Tb–Tb) distances, mediated via Ni–Si network, likely lead to weak magnetic interactions. Low-field magnetization vs temperature measurements indicate weak and field-sensitive antiferromagnetic ground state, with ordering temperatures of 3 K in GdNi{sub 8}Si{sub 3} and about 2–3 K in TbNi{sub 8}Si{sub 3}. On the other hand, the isothermal field-dependent magnetization data show the presence of competing interactions in both compounds, with a field-induced ferromagnetic behavior for GdNi{sub 8}Si{sub 3} and a ferrimagnetic-like behavior in TbNi{sub 8}Si{sub 3} at the ordering temperature T{sub C/N} ofmore » about (or slightly higher than) 3K. The magnetocaloric effect, quantified in terms of isothermal magnetic entropy change ΔS{sub m}, has the maximum values of –19.8 J(kg K){sup −1} (at 4 K for 140 kOe field change) and −12.1 J(kg K){sup −1} (at 12 K for 140 kOe field change) in GdNi{sub 8}Si{sub 3} and TbNi{sub 8}Si{sub 3}, respectively. - Graphical abstract: GdNi{sub 8}Si{sub 3} and TbNi{sub 8}Si{sub 3} compounds are isostructural, and crystallize in a new monoclinic type strictly related to the tetragonal BaCd{sub 11} structure. The large R–R interatomic distances mediated via Ni–Si network lead to a weak magnetism in both compounds. - Highlights: • Novel RNi{sub 8}Si{sub 3} (R=Gd, Tb) compounds have been synthesized and characterized. • GdNi{sub 8}Si{sub 3} and TbNi{sub 8}Si{sub 3} are isostructural compounds, belonging to a new monoclinic structure type. • The monoclinic GdNi{sub 8}Si{sub 3} type is an ordered derivative of the tetragonal BaCd{sub 11} type. • The large R–R interatomic distances mediated via Ni–Si network lead to a weak magnetism. • Both compounds GdNi{sub 8}Si{sub 3} and TbNi{sub 8}Si{sub 3} show antiferromagnetic-like order around 3 K.« less

Authors:
 [1];  [2];  [3];  [4]; ;  [1];  [2];  [5];  [6]
  1. Department of Chemistry, University of Genova, Via Dodecaneso 31, 16146 Genova (Italy)
  2. (Italy)
  3. Department of Chemistry, Moscow State University, Leninskie Gory, House 1, Building 3, Moscow, GSP-2 119992 (Russian Federation)
  4. Department of Petrology, Geological Faculty, Moscow State University, Leninskie Gory, Moscow 119992 (Russian Federation)
  5. Indian Institute of Technology Madras, Chennai 600036 (India)
  6. Departamento de Física Teórica e Experimental, Universidade Federal do Rio Grande do Norte, Natal 59082-970 (Brazil)
Publication Date:
OSTI Identifier:
22577756
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Solid State Chemistry; Journal Volume: 233; Other Information: Copyright (c) 2015 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ANTIFERROMAGNETISM; ENTROPY; GROUND STATES; INTERACTIONS; INTERATOMIC DISTANCES; LATTICE PARAMETERS; MAGNETIC PROPERTIES; MAGNETIZATION; MONOCLINIC LATTICES; MONOCRYSTALS; NICKEL SILICIDES; POWDERS; RARE EARTHS; TEMPERATURE MEASUREMENT; TETRAGONAL LATTICES; X RADIATION

Citation Formats

Pani, M., E-mail: marcella@chimica.unige.it, Institute SPIN-CNR, Corso Perrone 24, 16152 Genova, Morozkin, A.V., Yapaskurt, V.O., Provino, A., Manfrinetti, P., Institute SPIN-CNR, Corso Perrone 24, 16152 Genova, Nirmala, R., and Malik, S.K.. RNi{sub 8}Si{sub 3} (R=Gd,Tb): Novel ternary ordered derivatives of the BaCd{sub 11} type. United States: N. p., 2016. Web. doi:10.1016/J.JSSC.2015.11.004.
Pani, M., E-mail: marcella@chimica.unige.it, Institute SPIN-CNR, Corso Perrone 24, 16152 Genova, Morozkin, A.V., Yapaskurt, V.O., Provino, A., Manfrinetti, P., Institute SPIN-CNR, Corso Perrone 24, 16152 Genova, Nirmala, R., & Malik, S.K.. RNi{sub 8}Si{sub 3} (R=Gd,Tb): Novel ternary ordered derivatives of the BaCd{sub 11} type. United States. doi:10.1016/J.JSSC.2015.11.004.
Pani, M., E-mail: marcella@chimica.unige.it, Institute SPIN-CNR, Corso Perrone 24, 16152 Genova, Morozkin, A.V., Yapaskurt, V.O., Provino, A., Manfrinetti, P., Institute SPIN-CNR, Corso Perrone 24, 16152 Genova, Nirmala, R., and Malik, S.K.. Fri . "RNi{sub 8}Si{sub 3} (R=Gd,Tb): Novel ternary ordered derivatives of the BaCd{sub 11} type". United States. doi:10.1016/J.JSSC.2015.11.004.
@article{osti_22577756,
title = {RNi{sub 8}Si{sub 3} (R=Gd,Tb): Novel ternary ordered derivatives of the BaCd{sub 11} type},
author = {Pani, M., E-mail: marcella@chimica.unige.it and Institute SPIN-CNR, Corso Perrone 24, 16152 Genova and Morozkin, A.V. and Yapaskurt, V.O. and Provino, A. and Manfrinetti, P. and Institute SPIN-CNR, Corso Perrone 24, 16152 Genova and Nirmala, R. and Malik, S.K.},
abstractNote = {The title compounds have been synthesized and characterized both from the structural and magnetic point of view. Both crystallize in a new monoclinic structure strictly related to the tetragonal BaCd{sub 11} type. The structure was solved by means of X-ray single-crystal techniques for GdNi{sub 8}Si{sub 3} and confirmed for TbNi{sub 8}Si{sub 3} on powder data; the corresponding lattice parameters (obtained from Guinier powder patterns) are a=6.3259(2), b=13.7245(5), c=7.4949(3) Å, β=113.522(3)°, V{sub cell}=596.64(3) Å{sup 3} and a=6.3200(2), b=13.6987(4), c=7.4923(2) Å, β=113.494(2)°, V{sub cell}=594.88(2) Å{sup 3}. The symmetry relationship between the tI48-I4{sub 1}/amd BaCd{sub 11} aristotype and the new ordered mS48-C2/c GdNi{sub 8}Si{sub 3} derivative is described via the Bärnighausen formalism within the group theory. The large Gd–Gd (Tb–Tb) distances, mediated via Ni–Si network, likely lead to weak magnetic interactions. Low-field magnetization vs temperature measurements indicate weak and field-sensitive antiferromagnetic ground state, with ordering temperatures of 3 K in GdNi{sub 8}Si{sub 3} and about 2–3 K in TbNi{sub 8}Si{sub 3}. On the other hand, the isothermal field-dependent magnetization data show the presence of competing interactions in both compounds, with a field-induced ferromagnetic behavior for GdNi{sub 8}Si{sub 3} and a ferrimagnetic-like behavior in TbNi{sub 8}Si{sub 3} at the ordering temperature T{sub C/N} of about (or slightly higher than) 3K. The magnetocaloric effect, quantified in terms of isothermal magnetic entropy change ΔS{sub m}, has the maximum values of –19.8 J(kg K){sup −1} (at 4 K for 140 kOe field change) and −12.1 J(kg K){sup −1} (at 12 K for 140 kOe field change) in GdNi{sub 8}Si{sub 3} and TbNi{sub 8}Si{sub 3}, respectively. - Graphical abstract: GdNi{sub 8}Si{sub 3} and TbNi{sub 8}Si{sub 3} compounds are isostructural, and crystallize in a new monoclinic type strictly related to the tetragonal BaCd{sub 11} structure. The large R–R interatomic distances mediated via Ni–Si network lead to a weak magnetism in both compounds. - Highlights: • Novel RNi{sub 8}Si{sub 3} (R=Gd, Tb) compounds have been synthesized and characterized. • GdNi{sub 8}Si{sub 3} and TbNi{sub 8}Si{sub 3} are isostructural compounds, belonging to a new monoclinic structure type. • The monoclinic GdNi{sub 8}Si{sub 3} type is an ordered derivative of the tetragonal BaCd{sub 11} type. • The large R–R interatomic distances mediated via Ni–Si network lead to a weak magnetism. • Both compounds GdNi{sub 8}Si{sub 3} and TbNi{sub 8}Si{sub 3} show antiferromagnetic-like order around 3 K.},
doi = {10.1016/J.JSSC.2015.11.004},
journal = {Journal of Solid State Chemistry},
number = ,
volume = 233,
place = {United States},
year = {Fri Jan 15 00:00:00 EST 2016},
month = {Fri Jan 15 00:00:00 EST 2016}
}