38 research outputs found
Signatures of a Pressure-Induced Topological Quantum Phase Transition in BiTeI
We report the observation of two signatures of a pressure-induced topological
quantum phase transition in the polar semiconductor BiTeI using x-ray powder
diffraction and infrared spectroscopy. The x-ray data confirm that BiTeI
remains in its ambient-pressure structure up to 8 GPa. The lattice parameter
ratio c/a shows a minimum between 2.0-2.9 GPa, indicating an enhanced c-axis
bonding through pz band crossing as expected during the transition. Over the
same pressure range, the infrared spectra reveal a maximum in the optical
spectral weight of the charge carriers, reflecting the closing and reopening of
the semiconducting band gap. Both of these features are characteristics of a
topological quantum phase transition, and are consistent with a recent
theoretical proposal.Comment: revised final versio
High-pressure spectroscopic investigation of multiferroic Ni3TeO6
We combined diamond anvil cell techniques, infrared and Raman spectroscopies, and lattice dynamics calculations to explore the high pressure properties of multiferroic Ni3TeO6. Using a frequency trend analysis, we trace a subtle decrease in compressibility near 4 GPa to a minimum in the O-Ni2-O bond angle. This unique behavior emanates from the proximity of the Ni2 center in the Ni3-Ni2-Ni1-Te chain to a flexible pocket that is intrinsic to the crystal structure. At the same time, predicted trends in the superexchange pathways are consistent with greater antiferromagnetic character under compression, in line with both phase stability calculations and direct susceptibility measurements. These findings highlight opportunities for local structure control of corundumlike materials
Long-Range Ordered Carbon Clusters: A Crystalline Material with Amorphous Building Blocks
Solid-state materials can be categorized by their structures into crystalline (having periodic translation symmetry), amorphous (no periodic and orientational symmetry), and quasi-crystalline (having orientational but not periodic translation symmetry) phases. Hybridization of crystalline and amorphous structures at the atomic level has not been experimentally observed. We report the discovery of a long-range ordered material constructed from units of amorphous carbon clusters that was synthesized by compressing solvated fullerenes. Using x-ray diffraction, Raman spectroscopy, and quantum molecular dynamics simulation, we observed that, although carbon-60 cages were crushed and became amorphous, the solvent molecules remained intact, playing a crucial role in maintaining the long-range periodicity. Once formed, the high-pressure phase is quenchable back to ambient conditions and is ultra-incompressible, with the ability to indent diamond
Pressure-Induced Magnetic Crossover Driven by Hydrogen Bonding in CuF2(H2O)2(3-chloropyridine)
Hydrogen bonding plays a foundational role in the life, earth, and chemical sciences, with its richness and strength depending on the situation. In molecular materials, these interactions determine assembly mechanisms, control superconductivity, and even permit magnetic exchange. In spite of its long-standing importance, exquisite control of hydrogen bonding in molecule-based magnets has only been realized in limited form and remains as one of the major challenges. Here, we report the discovery that pressure can tune the dimensionality of hydrogen bonding networks in CuF2(H2O)2(3-chloropyridine) to induce magnetic switching. Specifically, we reveal how the development of exchange pathways under compression combined with an enhanced ab-plane hydrogen bonding network yields a three dimensional superexchange web between copper centers that triggers a reversible magnetic crossover. Similar pressure- and strain-driven crossover mechanisms involving coordinated motion of hydrogen bond networks may play out in other quantum magnets
Ionic high-pressure form of elemental boron
Boron is an element of fascinating chemical complexity. Controversies have
shrouded this element since its discovery was announced in 1808: the new
'element' turned out to be a compound containing less than 60-70 percent of
boron, and it was not until 1909 that 99-percent pure boron was obtained. And
although we now know of at least 16 polymorphs, the stable phase of boron is
not yet experimentally established even at ambient conditions. Boron's
complexities arise from frustration: situated between metals and insulators in
the periodic table, boron has only three valence electrons, which would favour
metallicity, but they are sufficiently localized that insulating states emerge.
However, this subtle balance between metallic and insulating states is easily
shifted by pressure, temperature and impurities. Here we report the results of
high-pressure experiments and ab initio evolutionary crystal structure
predictions that explore the structural stability of boron under pressure and,
strikingly, reveal a partially ionic high-pressure boron phase. This new phase
is stable between 19 and 89 GPa, can be quenched to ambient conditions, and has
a hitherto unknown structure (space group Pnnm, 28 atoms in the unit cell)
consisting of icosahedral B12 clusters and B2 pairs in a NaCl-type arrangement.
We find that the ionicity of the phase affects its electronic bandgap, infrared
adsorption and dielectric constants, and that it arises from the different
electronic properties of the B2 pairs and B12 clusters and the resultant charge
transfer between them.Comment: Published in Nature 453, 863-867 (2009
Probing Mechanical Properties of Graphene with Raman Spectroscopy
The use of Raman scattering techniques to study the mechanical properties of
graphene films is reviewed here. The determination of Gruneisen parameters of
suspended graphene sheets under uni- and bi-axial strain is discussed and the
values are compared to theoretical predictions. The effects of the
graphene-substrate interaction on strain and to the temperature evolution of
the graphene Raman spectra are discussed. Finally, the relation between
mechanical and thermal properties is presented along with the characterization
of thermal properties of graphene with Raman spectroscopy.Comment: To appear in the Journal of Materials Scienc