Rearrangement of van der Waals stacking and formation of a singlet state at T = 90 K in a cluster magnet

Sheckelton, John P.; Plumb, Kemp W.; Trump, Benjamin A.; Broholm, Collin L.; McQueen, Tyrel M.

doi:10.1039/C6QI00470A

Title: Rearrangement of van der Waals stacking and formation of a singlet state at T = 90 K in a cluster magnet

Journal Article · Sun Jan 01 00:00:00 EST 2017 · Inorganic Chemistry Frontiers (Online)

DOI:https://doi.org/10.1039/C6QI00470A· OSTI ID:1397289

Sheckelton, John P.; Plumb, Kemp W.; Trump, Benjamin A.; Broholm, Collin L.; McQueen, Tyrel M.

Insulating Nb3Cl8 is a layered chloride consisting of two-dimensional triangular layers of Seff = 1/2 Nb3Cl13 clusters at room temperature. Magnetic susceptibility measurement show a sharp, hysteretic drop to a temperature independent value below T = 90 K. Specific heat measurements show that the transition is first order, with ΔS ≈ 5 J K-1 mol-1 f.u.-1, and a low temperature T-linear contribution originating from defect spins. Neutron and X-ray diffraction show a lowering of symmetry from trigonal P[3 with combining macron]m1 to monoclinic C2/m symmetry, with a change in layer stacking from –AB–AB– to –AB'–BC'–CA'– and no observed magnetic order. This lowering of symmetry and rearrangement of successive layers evades geometric magnetic frustration to form a singlet ground state. It is the lowest temperature at which a change in stacking sequence is known to occur in a van der Waals solid, occurs in the absence of orbital degeneracies, and suggests that designer 2-D heterostructures may be able to undergo similar phase transitions.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI ID:: 1397289

Journal Information:: Inorganic Chemistry Frontiers (Online), Vol. 4, Issue 3; ISSN 2052-1553

Publisher:: Royal Society of Chemistry

Country of Publication:: United States

Language:: ENGLISH

References (52)

Thermal conductivity and specific heat of the linear chain cuprate ${Sr}_{2} {CuO}_{3} :$ Evidence for thermal transport via spinons Sologubenko, A. V.; Felder, E.; Giannò, K. Physical Review B, Vol. 62, Issue 10 https://doi.org/10.1103/PhysRevB.62.R6108	journal	September 2000
Ubiquitous Interplay Between Charge Ordering and High-Temperature Superconductivity in Cuprates da Silva Neto, E. H.; Aynajian, P.; Frano, A. Science, Vol. 343, Issue 6169 https://doi.org/10.1126/science.1243479	journal	December 2013
Superconductivity at 39 K in magnesium diboride Nagamatsu, Jun; Nakagawa, Norimasa; Muranaka, Takahiro Nature, Vol. 410, Issue 6824 https://doi.org/10.1038/35065039	journal	March 2001
$S = \frac{1}{2}$ chains and spin-Peierls transition in TiOCl Seidel, Alexander; Marianetti, Chris A.; Chou, F. C. Physical Review B, Vol. 67, Issue 2 https://doi.org/10.1103/PhysRevB.67.020405	journal	January 2003
Spin-singlet state formation in the cluster Mott insulator ${GaNb}_{4} S_{8}$ studied by $μ SR$ and NMR spectroscopy Waki, T.; Kajinami, Y.; Tabata, Y. Physical Review B, Vol. 81, Issue 2 https://doi.org/10.1103/PhysRevB.81.020401	journal	January 2010
Charge ordering in a quasi-two-dimensional organic conductor Miyagawa, K.; Kawamoto, A.; Kanoda, K. Physical Review B, Vol. 62, Issue 12 https://doi.org/10.1103/PhysRevB.62.R7679	journal	September 2000
Single crystal growth and characterization of nearly stoichiometric LiVO2 Tian, W.; Chisholm, M. F.; Khalifah, P. G. Materials Research Bulletin, Vol. 39, Issue 9 https://doi.org/10.1016/j.materresbull.2004.03.024	journal	July 2004
Structure and Properties of Functional Oxide Thin Films: Insights From Electronic-Structure Calculations Rondinelli, James M.; Spaldin, Nicola A. Advanced Materials, Vol. 23, Issue 30 https://doi.org/10.1002/adma.201101152	journal	July 2011
Synthesis, Structure, and Magnetic Properties of NaTiO ₂ Clarke, S. J.; Fowkes, A. J.; Harrison, A. Chemistry of Materials, Vol. 10, Issue 1 https://doi.org/10.1021/cm970538c	journal	January 1998
Experimental and Theoretical Electronic Structure Investigations on α-Nb ₃ Cl ₈ and the Intercalated Phase β‘-NaNb ₃ Cl ₈ Kennedy, John Rory; Adler, Peter; Dronskowski, Richard Inorganic Chemistry, Vol. 35, Issue 8 https://doi.org/10.1021/ic951348b	journal	January 1996
Observation of the spin-Peierls transition in linear ${Cu}^{2 +}$ (spin-1/2) chains in an inorganic compound ${CuGeO}_{3}$ Hase, Masashi; Terasaki, Ichiro; Uchinokura, Kunimitsu Physical Review Letters, Vol. 70, Issue 23 https://doi.org/10.1103/PhysRevLett.70.3651	journal	June 1993
Experimental Realization of a Three-Dimensional Topological Insulator, Bi₂Te₃ Chen, Y. L.; Analytis, J. G.; Chu, J.-H. Science, Vol. 325, Issue 5937, p. 178-181 https://doi.org/10.1126/science.1173034	journal	June 2009
Emergent Honeycomb Lattice in ${LiZn}_{2} {Mo}_{3} O_{8}$ Flint, Rebecca; Lee, Patrick A. Physical Review Letters, Vol. 111, Issue 21 https://doi.org/10.1103/PhysRevLett.111.217201	journal	November 2013
Orbital Ordering in a Two-Dimensional Triangular Lattice Pen, H. F.; van den Brink, J.; Khomskii, D. I. Physical Review Letters, Vol. 78, Issue 7 https://doi.org/10.1103/PhysRevLett.78.1323	journal	February 1997
Valence bond liquid phase in the honeycomb lattice material ${Li}_{2} Ru O_{3}$ Kimber, Simon A. J.; Mazin, I. I.; Shen, Juan Physical Review B, Vol. 89, Issue 8 https://doi.org/10.1103/PhysRevB.89.081408	journal	February 2014
Scattering Continuum and Possible Fractionalized Excitations in $α − {RuCl}_{3}$ Sandilands, Luke J.; Tian, Yao; Plumb, Kemp W. Physical Review Letters, Vol. 114, Issue 14 https://doi.org/10.1103/PhysRevLett.114.147201	journal	April 2015
γ-Nb₃Cl₈ - a New Stacking Variant Formed from the Thermal Decomposition of Intercalated β'-NaNb₃Cl₈ Kennedy, J. R.; Simon, André Materials Science Forum, Vol. 91-93 https://doi.org/10.4028/www.scientific.net/MSF.91-93.183	journal	January 1992
Van der Waals heterostructures and devices Liu, Yuan; Weiss, Nathan O.; Duan, Xidong Nature Reviews Materials, Vol. 1, Issue 9 https://doi.org/10.1038/natrevmats.2016.42	journal	July 2016
Experimental Realization of a Spin- $1 / 2$ Triangular-Lattice Heisenberg Antiferromagnet Shirata, Yutaka; Tanaka, Hidekazu; Matsuo, Akira Physical Review Letters, Vol. 108, Issue 5 https://doi.org/10.1103/PhysRevLett.108.057205	journal	January 2012
Possible valence-bond condensation in the frustrated cluster magnet LiZn2Mo3O8 Sheckelton, J. P.; Neilson, J. R.; Soltan, D. G. Nature Materials, Vol. 11, Issue 6 https://doi.org/10.1038/nmat3329	journal	May 2012
Anomalous dielectric response in the dimer Mott insulator $κ − {(BEDT-TTF)}_{2} {Cu}_{2} {(CN)}_{3}$ Abdel-Jawad, Majed; Terasaki, Ichiro; Sasaki, Takahiko Physical Review B, Vol. 82, Issue 12 https://doi.org/10.1103/PhysRevB.82.125119	journal	September 2010
Spin-Peierls transition in TiOCl Shaz, Mohammad; van Smaalen, Sander; Palatinus, Lukas Physical Review B, Vol. 71, Issue 10 https://doi.org/10.1103/PhysRevB.71.100405	journal	March 2005
Single crystal growth and physical properties of Kondo insulator YbB12 Iga, F.; Shimizu, N.; Takabatake, T. Journal of Magnetism and Magnetic Materials, Vol. 177-181 https://doi.org/10.1016/S0304-8853(97)00493-9	journal	January 1998
FAULTS, a new program for refinement of powder diffraction patterns from layered structures Casas-Cabanas, M.; Rodriguez-Carvajal, J.; Palacin, M. R. Zeitschrift für Kristallographie Supplements, Vol. 2006, Issue suppl_23_2006 https://doi.org/10.1524/zksu.2006.suppl_23.243	journal	June 2006
Atomically thin p–n junctions with van der Waals heterointerfaces Lee, Chul-Ho; Lee, Gwan-Hyoung; van der Zande, Arend M. Nature Nanotechnology, Vol. 9, Issue 9 https://doi.org/10.1038/nnano.2014.150	journal	August 2014
Structural and magnetic transitions in the Mott insulator GaNb4S8 Jakob, Stefanie; Müller, Helen; Johrendt, Dirk Journal of Materials Chemistry, Vol. 17, Issue 36 https://doi.org/10.1039/b704943a	journal	January 2007
Light-emitting diodes by band-structure engineering in van der Waals heterostructures Withers, F.; Del Pozo-Zamudio, O.; Mishchenko, A. Nature Materials, Vol. 14, Issue 3 https://doi.org/10.1038/nmat4205	journal	February 2015
Neutron scattering study of the charge-density wave transitions in $2 H - Ta {Se}_{2}$ and $2 H - Nb {Se}_{2}$ Moncton, D. E.; Axe, J. D.; DiSalvo, F. J. Physical Review B, Vol. 16, Issue 2 https://doi.org/10.1103/PhysRevB.16.801	journal	July 1977
Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet Banerjee, A.; Bridges, C. A.; Yan, J. -Q. Nature Materials, Vol. 15, Issue 7 https://doi.org/10.1038/nmat4604	journal	April 2016
Commensurability, Excitation Gap, and Topology in Quantum Many-Particle Systems on a Periodic Lattice Oshikawa, Masaki Physical Review Letters, Vol. 84, Issue 7 https://doi.org/10.1103/PhysRevLett.84.1535	journal	February 2000
Novel Phase Transition in Spin-1/2 Linear Chain Systems: NaTiSi ₂ O ₆ and LiTiSi ₂ O ₆ Isobe, Masahiko; Ninomiya, Emi; N. Vasil'ev, Alexander Journal of the Physical Society of Japan, Vol. 71, Issue 6 https://doi.org/10.1143/JPSJ.71.1423	journal	June 2002
Magnetic order in $α - {RuCl}_{3}$ : A honeycomb-lattice quantum magnet with strong spin-orbit coupling Sears, J. A.; Songvilay, M.; Plumb, K. W. Physical Review B, Vol. 91, Issue 14 https://doi.org/10.1103/PhysRevB.91.144420	journal	April 2015
Crystal Structures, Electronic Properties, and Pressure-Induced Superconductivity of the Tetrahedral Cluster Compounds GaNb ₄ S ₈ , GaNb ₄ Se ₈ , and GaTa ₄ Se ₈ Pocha, Regina; Johrendt, Dirk; Ni, Bingfang Journal of the American Chemical Society, Vol. 127, Issue 24 https://doi.org/10.1021/ja050243x	journal	June 2005
General atomic and molecular electronic structure system Schmidt, Michael W.; Baldridge, Kim K.; Boatz, Jerry A. Journal of Computational Chemistry, Vol. 14, Issue 11, p. 1347-1363 https://doi.org/10.1002/jcc.540141112	journal	November 1993
Spin-Orbital Short-Range Order on a Honeycomb-Based Lattice Nakatsuji, S.; Kuga, K.; Kimura, K. Science, Vol. 336, Issue 6081 https://doi.org/10.1126/science.1212154	journal	May 2012
Van der Waals heterostructures Geim, A. K.; Grigorieva, I. V. Nature, Vol. 499, Issue 7459, p. 419-425 https://doi.org/10.1038/nature12385	journal	July 2013
Electric Field Effect in Atomically Thin Carbon Films Novoselov, K. S. Science, Vol. 306, Issue 5696, p. 666-669 https://doi.org/10.1126/science.1102896	journal	October 2004
Electronics and optoelectronics of two-dimensional transition metal dichalcogenides Wang, Qing Hua; Kalantar-Zadeh, Kourosh; Kis, Andras Nature Nanotechnology, Vol. 7, Issue 11, p. 699-712 https://doi.org/10.1038/nnano.2012.193	journal	November 2012
Topological order and absence of band insulators at integer filling in non-symmorphic crystals Parameswaran, Siddharth A.; Turner, Ari M.; Arovas, Daniel P. Nature Physics, Vol. 9, Issue 5 https://doi.org/10.1038/nphys2600	journal	April 2013
Observation of Time-Reversal-Protected Single-Dirac-Cone Topological-Insulator States in ${Bi}_{2} {Te}_{3}$ and ${Sb}_{2} {Te}_{3}$ Hsieh, D.; Xia, Y.; Qian, D. Physical Review Letters, Vol. 103, Issue 14 https://doi.org/10.1103/PhysRevLett.103.146401	journal	September 2009
Spin Liquid State in the $S = 1 / 2$ Triangular Lattice ${Ba}_{3} {CuSb}_{2} O_{9}$ Zhou, H. D.; Choi, E. S.; Li, G. Physical Review Letters, Vol. 106, Issue 14 https://doi.org/10.1103/PhysRevLett.106.147204	journal	April 2011
Superconductivity at 38 K in the Iron Arsenide $({Ba}_{1 - x} K_{x}) {Fe}_{2} {As}_{2}$ Rotter, Marianne; Tegel, Marcus; Johrendt, Dirk Physical Review Letters, Vol. 101, Issue 10 https://doi.org/10.1103/PhysRevLett.101.107006	journal	September 2008
Spin gap and antiferromagnetic correlations in the Kondo insulator CeNiSn Mason, T. E.; Aeppli, G.; Ramirez, A. P. Physical Review Letters, Vol. 69, Issue 3 https://doi.org/10.1103/PhysRevLett.69.490	journal	July 1992
Superconducting and Magnetic Transitions in the Heavy-Fermion System U ${Ru}_{2}$ ${Si}_{2}$ Palstra, T. T. M.; Menovsky, A. A.; Berg, J. van den Physical Review Letters, Vol. 55, Issue 24 https://doi.org/10.1103/PhysRevLett.55.2727	journal	December 1985
Quantum spin Hall effect in two-dimensional transition metal dichalcogenides Qian, X.; Liu, J.; Fu, L. Science, Vol. 346, Issue 6215 https://doi.org/10.1126/science.1256815	journal	November 2014
Solid state chemistry of Nb3Cl8: Nb3TeCl7, mixed crystal formation, and intercalation Miller, Gordon J. Journal of Alloys and Compounds, Vol. 217, Issue 1 https://doi.org/10.1016/0925-8388(94)01298-V	journal	January 1995
A roadmap for graphene Novoselov, K. S.; Fal′ko, V. I.; Colombo, L. Nature, Vol. 490, Issue 7419 https://doi.org/10.1038/nature11458	journal	October 2012
Discrete trinuclear complexes of niobium and tantalum related to the local structure in niobium chloride, Nb3Cl8 Cotton, F. Albert; Diebold, Michael P.; Feng, Xuejun Inorganic Chemistry, Vol. 27, Issue 19 https://doi.org/10.1021/ic00292a029	journal	September 1988
Die Kristallstruktur der Verbindung Nb3Cl8 v. Schnering, H. -G.; Wöhrle, H.; Schäfer, H. Naturwissenschaften, Vol. 48, Issue 6 https://doi.org/10.1007/BF00639538	journal	January 1961
The chemistry of two-dimensional layered transition metal dichalcogenide nanosheets Chhowalla, Manish; Shin, Hyeon Suk; Eda, Goki Nature Chemistry, Vol. 5, Issue 4, p. 263-275 https://doi.org/10.1038/nchem.1589	journal	April 2013
Successive Orbital Ordering Transitions in ${NaVO}_{2}$ McQueen, T. M.; Stephens, P. W.; Huang, Q. Physical Review Letters, Vol. 101, Issue 16 https://doi.org/10.1103/PhysRevLett.101.166402	journal	October 2008
Single-layer MoS₂ transistors Radisavljevic, B.; Radenovic, A.; Brivio, J. Nature Nanotechnology, Vol. 6, Issue 3, p. 147-150 https://doi.org/10.1038/nnano.2010.279	journal	January 2011

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