Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals

The realization of long-range ferromagnetic order in two-dimensional van der Waals crystals, combined with their rich electronic and optical properties, could lead to new magnetic, magnetoelectric and magneto-optic applications. In two-dimensional systems, the long-range magnetic order is strongly suppressed by thermal fluctuations, according to the Mermin–Wagner theorem; however, these thermal fluctuations can be counteracted by magnetic anisotropy. Previous efforts, based on defect and composition engineering, or the proximity effect, introduced magnetic responses only locally or extrinsically. Here we report intrinsic long-range ferromagnetic order in pristine Cr2Ge2Te6 atomic layers, as revealed by scanning magneto-optic Kerr microscopy. In this magnetically soft, two-dimensional van der Waals ferromagnet, we achieve unprecedented control of the transition temperature (between ferromagnetic and paramagnetic states) using very small fields (smaller than 0.3 tesla). This result is in contrast to the insensitivity of the transition temperature to magnetic fields in the three-dimensional regime. We found that the small applied field leads to an effective anisotropy that is much greater than the near-zero magnetocrystalline anisotropy, opening up a large spin-wave excitation gap. We explain the observed phenomenon using renormalized spin-wave theory and conclude that the unusual field dependence of the transition temperature is a hallmark of soft, two-dimensional ferromagnetic van der Waals crystals. Cr2Ge2Te6 is a nearly ideal two-dimensional Heisenberg ferromagnet and so will be useful for studying fundamental spin behaviours, opening the door to exploring new applications such as ultra-compact spintronics.

[1]  Q. Xue,et al.  Experimental Observation of the Quantum Anomalous Hall Effect in a Magnetic Topological Insulator , 2013, Science.

[2]  S. Louie,et al.  Tunable Magnetism and Half-Metallicity in Hole-Doped Monolayer GaSe. , 2014, Physical review letters.

[3]  F. Guinea,et al.  Missing atom as a source of carbon magnetism. , 2010, Physical review letters.

[4]  Shiyan Li,et al.  Gate-tunable phase transitions in thin flakes of 1T-TaS2. , 2014, Nature nanotechnology.

[5]  Xingao Gong,et al.  Magnetic properties and energy-mapping analysis. , 2013, Dalton transactions.

[6]  C. Vaz,et al.  Magnetism in ultrathin film structures , 2008 .

[7]  R. F. Willis,et al.  Thickness-dependent Curie temperatures of ultrathin magnetic films: effect of the range of spin-spin interactions. , 2001, Physical review letters.

[8]  R. A. Stokes,et al.  A ferromagnetic insulating substrate for the epitaxial growth of topological insulators , 2013 .

[9]  J. Fabian,et al.  Magnetic moment formation in graphene detected by scattering of pure spin currents. , 2012, Physical review letters.

[10]  N. Peres,et al.  Localized magnetic states in graphene. , 2008, Physical review letters.

[11]  G. Ouvrard,et al.  Crystallographic, magnetic and electronic structures of a new layered ferromagnetic compound Cr2Ge2Te6 , 1995 .

[12]  Kang L. Wang,et al.  Scale-invariant quantum anomalous Hall effect in magnetic topological insulators beyond the two-dimensional limit. , 2014, Physical review letters.

[13]  M I Katsnelson,et al.  Magnetic correlations at graphene edges: basis for novel spintronics devices. , 2007, Physical review letters.

[14]  N. Peres,et al.  Low-density ferromagnetism in biased bilayer graphene. , 2007, Physical review letters.

[15]  N. Mermin,et al.  Absence of Ferromagnetism or Antiferromagnetism in One- or Two-Dimensional Isotropic Heisenberg Models , 1966 .

[16]  Stefano de Gironcoli,et al.  Linear response approach to the calculation of the effective interaction parameters in the LDA + U method , 2004, cond-mat/0405160.

[17]  G. Gehring,et al.  The domain structure in ultrathin magnetic films , 1993 .

[18]  F. Xia,et al.  Ultrafast graphene photodetector , 2009, CLEO/QELS: 2010 Laser Science to Photonic Applications.

[19]  J. Petta,et al.  Large anomalous Hall effect in ferromagnetic insulator-topological insulator heterostructures , 2014, 1407.1432.

[20]  J. Keinonen,et al.  Spin-half paramagnetism in graphene induced by point defects , 2011, Nature Physics.

[21]  Zuocheng Zhang,et al.  Direct observation of the layer-dependent electronic structure in phosphorene. , 2016, Nature nanotechnology.

[22]  Andre K. Geim,et al.  The rise of graphene. , 2007, Nature materials.

[23]  M. Bloch Magnon Renormalization in Ferromagnets Near the Curie Point , 1962 .

[24]  H. Primakoff,et al.  Field dependence of the intrinsic domain magnetization of a ferromagnet , 1940 .

[25]  Li,et al.  Dimensional crossover in ultrathin Ni(111) films on W(110). , 1992, Physical review letters.

[26]  K. Hirakawa Kosterlitz‐Thouless transition in two‐dimensional planar ferromagnet K2CuF4 (invited) , 1982 .

[27]  José M. Gómez-Rodríguez,et al.  Atomic-scale control of graphene magnetism by using hydrogen atoms , 2016, Science.

[28]  Jing Shi,et al.  Proximity-induced ferromagnetism in graphene revealed by the anomalous Hall effect. , 2015, Physical review letters.

[29]  Stefano de Gironcoli,et al.  QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials , 2009, Journal of physics. Condensed matter : an Institute of Physics journal.

[30]  B. Hong,et al.  Exfoliation and Raman Spectroscopic Fingerprint of Few-Layer NiPS3 Van der Waals Crystals , 2016, Scientific Reports.

[31]  H. Ohno,et al.  Electric-field control of ferromagnetism , 2000, Nature.

[32]  Martin M. Fejer,et al.  Modified Sagnac interferometer for high-sensitivity magneto-optic measurements at cryogenic temperatures , 2006 .

[33]  Wei Han,et al.  Graphene spintronics. , 2014, Nature nanotechnology.

[34]  A. MacDonald,et al.  Theory of interedge superexchange in zigzag edge magnetism. , 2008, Physical review letters.

[35]  P. L. McEuen,et al.  The valley Hall effect in MoS2 transistors , 2014, Science.

[36]  M. Katsnelson,et al.  Room-temperature ferromagnetism in graphite driven by two-dimensional networks of point defects , 2009, 0910.2130.

[37]  A. Corciovei Spin-Wave Theory of Ferromagnetic Thin Films , 1963 .