The creation of new families of intermetallic or Zintl-phase compounds with high-spin orbit elements has attracted a considerable amount of interest due to the presence of unique electronic, magnetic, and topological phenomena in these materials. Here, we establish the synthesis and structural and electronic characterization of KMgBi single crystals having a new structure type. KMgBi crystallizes in space group having unit cell parameters = 4.
View Article and Find Full Text PDFTwo-dimensional (2D) materials have drawn immense interests in scientific and technological communities, owing to their extraordinary properties and their tunability by gating, proximity, strain and external fields. For electronic applications, an ideal 2D material would have high mobility, air stability, sizable band gap, and be compatible with large scale synthesis. Here we demonstrate air stable field effect transistors using atomically thin few-layer PdSe sheets that are sandwiched between hexagonal BN (hBN), with large saturation current > 350 μA/μm, and high field effect mobilities of ~ 700 and 10,000 cm/Vs at 300 K and 2 K, respectively.
View Article and Find Full Text PDFThe exploration of quantum materials in which an applied thermo/electrical/magnetic field along one crystallographic direction produces an anisotropic response has led to unique functionalities. Along these lines, KMgBi is a layered, narrow gap semiconductor near a critical state between multiple Dirac phases due to the presence of a flat band near the Fermi level. The valence band is highly anisotropic with minimal cross-plane dispersion, which, in combination with an isotropic conduction band, enables axis-dependent conduction polarity.
View Article and Find Full Text PDFAxis-dependent conduction polarity (ADCP) is a unique electronic phenomena in which the charge polarity of carrier conduction can differ from p-type to n-type depending on the direction of travel through the crystal. Most materials that exhibit ADCP are metals, and very few semiconducting materials exhibit this effect. Here, we establish that PdSe, a ∼0.
View Article and Find Full Text PDFTopologically protected magnon surface states are highly desirable as an ideal platform to engineer low-dissipation spintronics devices. However, theoretical prediction of topological magnons in strongly correlated materials proves to be challenging because the ab initio density functional theory calculations fail to reliably predict magnetic interactions in correlated materials. Here, we present a symmetry-based approach, which predicts topological magnons in magnetically ordered crystals, upon applying external perturbations such as magnetic/electric fields and/or mechanical strains.
View Article and Find Full Text PDFControl of magnetism has attracted interest in achieving low-power and high-speed applications such as magnetic data storage and spintronic devices. Two-dimensional magnets allow for control of magnetic properties using the electric field, electrostatic doping and strain. In two-dimensional atomically thin magnets, a non-volatile all-optical method would offer the distinct advantage of switching magnetic states without application of an external field.
View Article and Find Full Text PDFKagome magnets possess several novel nontrivial topological features owing to the strong correlation between topology and magnetism that extends to their applications in the field of thermoelectricity. Conventional thermoelectric (TE) devices use the Seebeck effect to convert heat into electrical energy. In contrast, transverse thermoelectric devices based on the Nernst effect are attracting recent attention due to their unique transverse geometry, which uses a single material to eliminate the need for a multitude of electrical connections compared to conventional TE devices.
View Article and Find Full Text PDFSpin-orbit torque (SOT)-driven deterministic control of the magnetic state of a ferromagnet with perpendicular magnetic anisotropy is key to next-generation spintronic applications including non-volatile, ultrafast and energy-efficient data-storage devices. However, field-free deterministic switching of perpendicular magnetization remains a challenge because it requires an out-of-plane antidamping torque, which is not allowed in conventional spin-source materials such as heavy metals and topological insulators due to the system's symmetry. The exploitation of low-crystal symmetries in emergent quantum materials offers a unique approach to achieve SOTs with unconventional forms.
View Article and Find Full Text PDFThe development of thermally robust, air-stable, exfoliatable two-dimensional van der Waals ferromagnetic materials with high transition temperatures is of great importance. Here, we establish a family of magnetic alloys, CrPtTe ( ≤ 0.45), that combines the stability of the late transition metal dichalcogenide PtTe with magnetism from Cr.
View Article and Find Full Text PDFMethyl-substituted germanane is an emerging material that has been proposed for novel applications in optoelectronics, photoelectrocatalysis, and biosensors. It is a two-dimensional semiconductor with a strong above-gap fluorescence associated with water intercalation. Here, we use time-resolved photoluminescence spectroscopy to understand the mechanism causing this fluorescence.
View Article and Find Full Text PDFMoiré engineering of van der Waals magnetic materials can yield new magnetic ground states via competing interactions in moiré superlattices. Theory predicts a suite of interesting phenomena, including multiflavour magnetic states, non-collinear magnetic states, moiré magnon bands and magnon networks in twisted bilayer magnetic crystals, but so far such non-trivial magnetic ground states have not emerged experimentally. Here, by utilizing the stacking-dependent interlayer exchange interactions in two-dimensional magnetic materials, we demonstrate a coexisting ferromagnetic (FM) and antiferromagnetic (AF) ground state in small-twist-angle CrI bilayers.
View Article and Find Full Text PDFPolytypism, the ability of materials to form crystal structures with different stacking sequences, occasionally causes materials with the same stoichiometry and similar local structures to have profoundly different properties. Herein, we discover a metastable 13-layer trigonal (13T) polytype of CaGaGe, a layered intermetallic phase comprised of [GaGe] honeycombs separated by Ca. 13T-CaGaGe is synthesized from arc-melting the elements, and its structure is elucidated via neutron powder diffraction.
View Article and Find Full Text PDFACS Appl Mater Interfaces
November 2021
Transition-metal-free Zintl-Klemm phases have received little attention as heterogeneous catalysis. Here, we show that a large family of structurally and electronically similar layered Zintl-Klemm phases built from honeycomb layers of group 13 triel (Tr) or group 14 tetrel (Tt) networks separated by electropositive cations (A) and having a stoichiometry of ATr or ATrTt (A = Ca, Ba, Y, La, Eu; Tr = Ga, In; Tt = Si, Ge) exhibit varying degrees of activity for the hydrogenation of phenylacetylene to styrene and ethylbenzene at 51 bar H and 40-100 °C across a variety of solvents. The most active catalysts contain Ga with, formally, a half-filled p orbital, and minimal bonding between neighboring Tr or TrTt layers.
View Article and Find Full Text PDFThe discovery of 2-dimensional (2D) materials, such as CrI, that retain magnetic ordering at monolayer thickness has resulted in a surge of both pure and applied research in 2D magnetism. Here, we report a magneto-Raman spectroscopy study on multilayered CrI, focusing on two additional features in the spectra that appear below the magnetic ordering temperature and were previously assigned to high frequency magnons. Instead, we conclude these modes are actually zone-folded phonons.
View Article and Find Full Text PDFRemarkable properties of two-dimensional (2D) layer magnetic materials, which include spin filtering in magnetic tunnel junctions and the gate control of magnetic states, were demonstrated recently. Whereas these studies focused on static properties, dynamic magnetic properties, such as excitation and control of spin waves, remain elusive. Here we investigate spin-wave dynamics in antiferromagnetic CrI bilayers using an ultrafast optical pump/magneto-optical Kerr probe technique.
View Article and Find Full Text PDFWe lay the foundation for determining the microscopic spin interactions in two-dimensional (2D) ferromagnets by combining angle-dependent ferromagnetic resonance (FMR) experiments on high quality CrI_{3} single crystals with theoretical modeling based on symmetries. We discover that the Kitaev interaction is the strongest in this material with K∼-5.2 meV, 25 times larger than the Heisenberg exchange J∼-0.
View Article and Find Full Text PDFThe recent discovery that specific materials can simultaneously exhibit n-type conduction and p-type conduction along different directions of the single crystal has the potential to impact a broad range of electronic and energy-harvesting technologies. Here, we establish the chemical design principles for creating materials with this behavior. First, we define the single-carrier and multicarrier mechanisms for axis-dependent conduction polarity and their identifying band structure fingerprints.
View Article and Find Full Text PDFInexpensive, transition metal-free intermetallic compounds have received almost no attention as heterogeneous catalysts. Here, we show that BaGa, a Zintl-Klemm compound composed of honeycomb sheets of Ga anions separated by Ba cations and known to react with H under moderate conditions to form a layered polyanionic hydride BaGaH, effectively catalyzes the hydrogenation of phenylacetylene into styrene and ethylbenzene under modest conditions (1-50 bar H, 40-100 °C). Remarkably, the catalytic activity of BaGa (surface specific activities up to 8390 h) is on the same order of magnitude as commercial Pd-based catalysts.
View Article and Find Full Text PDFStacking order can influence the physical properties of two-dimensional van der Waals materials. Here we applied hydrostatic pressure up to 2 GPa to modify the stacking order in the van der Waals magnetic insulator CrI. We observed an irreversible interlayer antiferromagnetic-to-ferromagnetic transition in atomically thin CrI by magnetic circular dichroism and electron tunnelling measurements.
View Article and Find Full Text PDFThe creation of 2D van der Waals materials with ferromagnetism above room temperature is an essential goal toward their practical utilization in spin-based applications. Recent studies suggest that intercalating lithium in exfoliated flakes of the ferromagnet FeGeTe induces a nonzero magnetization at ∼ 300 K. However, the nanoscale nature of such experiments precludes precise observations of structural and chemical changes upon intercalation.
View Article and Find Full Text PDFElectronic materials generally exhibit a single isotropic majority carrier type, electrons or holes. Some superlattice and hexagonal materials exhibit opposite conduction polarities along in-plane and cross-plane directions due to multiple electron and hole bands. Here, we uncover a material genus with this behaviour that originates from the Fermi surface geometry of a single band.
View Article and Find Full Text PDFWe discover the chemical composition of over 1000 materials that are likely to exhibit layered and 2D phases but have yet to be synthesized. This includes two materials our calculations indicate can exist in distinct structures with different band gaps, expanding the short list of 2D phase-change materials. Whereas databases of over 1000 layered materials have been reported, we provide the first full database of materials that are likely layered but are yet to be synthesized, providing a roadmap for the synthesis community.
View Article and Find Full Text PDFThe sp3-hybridized group 14 graphane analogues are a unique family of 2D materials in which every atom requires a terminal ligand for stability. Consequently, the optical, electronic, and thermal properties of these materials can be manipulated via covalent chemistry. Herein, we review the methodologies for preparing these materials, and compare their functionalization densities to Si/Ge(111) surfaces and other covalently terminated 2D materials.
View Article and Find Full Text PDFAs a 2D ferromagnetic semiconductor with magnetic ordering, atomically thin chromium tri-iodide is the latest addition to the family of two-dimensional (2D) materials. However, realistic exploration of CrI-based devices and heterostructures is challenging due to its extreme instability under ambient conditions. Here, we present Raman characterization of CrI and demonstrate that the main degradation pathway of CrI is the photocatalytic substitution of iodine by water.
View Article and Find Full Text PDFBeilstein J Nanotechnol
August 2017
Germanane, a hydrogen-terminated graphane analogue of germanium has generated interest as a potential 2D electronic material. However, the incorporation and retention of extrinsic dopant atoms in the lattice, to tune the electronic properties, remains a significant challenge. Here, we show that the group-13 element Ga and the group-15 element As, can be successfully doped into a precursor CaGe phase, and remain intact in the lattice after the topotactic deintercalation, using HCl, to form GeH.
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