238 research outputs found
Room-temperature ferromagnetism in graphite driven by 2D networks of point defects
Ferromagnetism in carbon-based materials is appealing for both applications
and fundamental science purposes because carbon is a light and bio-compatible
material that contains only s and p electrons in contrast to traditional
ferromagnets based on 3d or 4f electrons. Here we demonstrate direct evidence
for ferromagnetic order locally at defect structures in highly oriented
pyrolytic graphite (HOPG) with magnetic force microscopy and in bulk
magnetization measurements at room temperature. Magnetic impurities have been
excluded as the origin of the magnetic signal after careful analysis supporting
an intrinsic magnetic behavior of carbon. The observed ferromagnetism has been
attributed to originate from unpaired electron spins localized at grain
boundaries of HOPG. Grain boundaries form two-dimensional arrays of point
defects, where their spacing depends on the mutual orientation of two grains.
Depending on the distance between these point defects, scanning tunneling
spectroscopy of grain boundaries showed two intense split localized states for
small distances between defects (< 4 nm) and one localized state at the Fermi
level for large distances between defects (> 4 nm).Comment: 19 pages, 5 figure
Electronic Instability in a Zero-Gap Semiconductor: The Charge-DensityWave in (TaSe4)(2)I
We report a comprehensive study of the paradigmatic quasi-1D compound (TaSe4)(2)I performed by means of angle-resolved photoemission spectroscopy (ARPES) and first-principles electronic structure calculations. We find it to be a zero-gap semiconductor in the nondistorted structure, with non-negligible interchain coupling. Theory and experiment support a Peierls-like scenario for the charge-density wave formation below T-CDW = 263 K, where the incommensurability is a direct consequence of the finite interchain coupling. The formation of small polarons, strongly suggested by the ARPES data, explains the puzzling semiconductor-to-semiconductor transition observed in transport at T-CDW.open114sciescopu
Electronic transport in polycrystalline graphene
Most materials in available macroscopic quantities are polycrystalline.
Graphene, a recently discovered two-dimensional form of carbon with strong
potential for replacing silicon in future electronics, is no exception. There
is growing evidence of the polycrystalline nature of graphene samples obtained
using various techniques. Grain boundaries, intrinsic topological defects of
polycrystalline materials, are expected to dramatically alter the electronic
transport in graphene. Here, we develop a theory of charge carrier transmission
through grain boundaries composed of a periodic array of dislocations in
graphene based on the momentum conservation principle. Depending on the grain
boundary structure we find two distinct transport behaviours - either high
transparency, or perfect reflection of charge carriers over remarkably large
energy ranges. First-principles quantum transport calculations are used to
verify and further investigate this striking behaviour. Our study sheds light
on the transport properties of large-area graphene samples. Furthermore,
purposeful engineering of periodic grain boundaries with tunable transport gaps
would allow for controlling charge currents without the need of introducing
bulk band gaps in otherwise semimetallic graphene. The proposed approach can be
regarded as a means towards building practical graphene electronics.Comment: accepted in Nature Material
First-Principles Study of the Electronic and Magnetic Properties of Defects in Carbon Nanostructures
Understanding the magnetic properties of graphenic nanostructures is
instrumental in future spintronics applications. These magnetic properties are
known to depend crucially on the presence of defects. Here we review our recent
theoretical studies using density functional calculations on two types of
defects in carbon nanostructures: Substitutional doping with transition metals,
and sp-type defects created by covalent functionalization with organic and
inorganic molecules. We focus on such defects because they can be used to
create and control magnetism in graphene-based materials. Our main results are
summarized as follows: i)Substitutional metal impurities are fully understood
using a model based on the hybridization between the states of the metal
atom and the defect levels associated with an unreconstructed D carbon
vacancy. We identify three different regimes, associated with the occupation of
distinct hybridization levels, which determine the magnetic properties obtained
with this type of doping; ii) A spin moment of 1.0 is always induced by
chemical functionalization when a molecule chemisorbs on a graphene layer via a
single C-C (or other weakly polar) covalent bond. The magnetic coupling between
adsorbates shows a key dependence on the sublattice adsorption site. This
effect is similar to that of H adsorption, however, with universal character;
iii) The spin moment of substitutional metal impurities can be controlled using
strain. In particular, we show that although Ni substitutionals are
non-magnetic in flat and unstrained graphene, the magnetism of these defects
can be activated by applying either uniaxial strain or curvature to the
graphene layer. All these results provide key information about formation and
control of defect-induced magnetism in graphene and related materials.Comment: 40 pages, 17 Figures, 62 References; Chapter 2 in Topological
Modelling of Nanostructures and Extended Systems (2013) - Springer, edited by
A. R. Ashrafi, F. Cataldo, A. Iranmanesh, and O. Or
Band structure engineering in (Bi1-xSbx)2Te3 ternary topological insulators
Three-dimensional (3D) topological insulators (TI) are novel quantum
materials with insulating bulk and topologically protected metallic surfaces
with Dirac-like band structure. The spin-helical Dirac surface states are
expected to host exotic topological quantum effects and find applications in
spintronics and quantum computation. The experimental realization of these
ideas requires fabrication of versatile devices based on bulk-insulating TIs
with tunable surface states. The main challenge facing the current TI materials
exemplified by Bi2Se3 and Bi2Te3 is the significant bulk conduction, which
remains unsolved despite extensive efforts involving nanostructuring, chemical
doping and electrical gating. Here we report a novel approach for engineering
the band structure of TIs by molecular beam epitaxy (MBE) growth of
(Bi1-xSbx)2Te3 ternary compounds. Angle-resolved photoemission spectroscopy
(ARPES) and transport measurements show that the topological surface states
exist over the entire composition range of (Bi1-xSbx)2Te3 (x = 0 to 1),
indicating the robustness of bulk Z2 topology. Most remarkably, the systematic
band engineering leads to ideal TIs with truly insulating bulk and tunable
surface state across the Dirac point that behave like one quarter of graphene.
This work demonstrates a new route to achieving intrinsic quantum transport of
the topological surface states and designing conceptually new TI devices with
well-established semiconductor technology.Comment: Minor changes in title, text and figures. Supplementary information
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Graphene for spintronics: giant Rashba splitting due to hybridization with Au
Graphene in spintronics has so far primarily meant spin current leads of high
performance because the intrinsic spin-orbit coupling of its pi-electrons is
very weak. If a large spin-orbit coupling could be created by a proximity
effect, the material could also form active elements of a spintronic device
such as the Das-Datta spin field-effect transistor, however, metal interfaces
often compromise the band dispersion of massless Dirac fermions. Our
measurements show that Au intercalation at the graphene-Ni interface creates a
giant spin-orbit splitting (~100 meV) in the graphene Dirac cone up to the
Fermi energy. Photoelectron spectroscopy reveals hybridization with Au-5d
states as the source for the giant spin-orbit splitting. An ab initio model of
the system shows a Rashba-split dispersion with the analytically predicted
gapless band topology around the Dirac point of graphene and indicates that a
sharp graphene-Au interface at equilibrium distance will account for only ~10
meV spin-orbit splitting. The ab initio calculations suggest an enhancement due
to Au atoms that get closer to the graphene and do not violate the sublattice
symmetry.Comment: 16 pages (3 figures) + supplementary information 16 pages (14
figures
Emergence of non-centrosymmetric topological insulating phase in BiTeI under pressure
The spin-orbit interaction affects the electronic structure of solids in
various ways. Topological insulators are one example where the spin-orbit
interaction leads the bulk bands to have a non-trivial topology, observable as
gapless surface or edge states. Another example is the Rashba effect, which
lifts the electron-spin degeneracy as a consequence of spin-orbit interaction
under broken inversion symmetry. It is of particular importance to know how
these two effects, i.e. the non-trivial topology of electronic states and
Rashba spin splitting, interplay with each other. Here we show, through
sophisticated first-principles calculations, that BiTeI, a giant bulk Rashba
semiconductor, turns into a topological insulator under a reasonable pressure.
This material is shown to exhibit several unique features such as, a highly
pressure-tunable giant Rashba spin splitting, an unusual pressure-induced
quantum phase transition, and more importantly the formation of strikingly
different Dirac surface states at opposite sides of the material.Comment: 5 figures are include
Spin-half paramagnetism in graphene induced by point defects
Using magnetization measurements, we show that point defects in graphene -
fluorine adatoms and irradiation defects (vacancies) - carry magnetic moments
with spin 1/2. Both types of defects lead to notable paramagnetism but no
magnetic ordering could be detected down to liquid helium temperatures. The
induced paramagnetism dominates graphene's low-temperature magnetic properties
despite the fact that maximum response we could achieve was limited to one
moment per approximately 1000 carbon atoms. This limitation is explained by
clustering of adatoms and, for the case of vacancies, by losing graphene's
structural stability.Comment: 14 pages, 14 figure
Realization of a Tunable Artificial Atom at a Supercritically Charged Vacancy in Graphene
The remarkable electronic properties of graphene have fueled the vision of a
graphene-based platform for lighter, faster and smarter electronics and
computing applications. One of the challenges is to devise ways to tailor its
electronic properties and to control its charge carriers. Here we show that a
single atom vacancy in graphene can stably host a local charge and that this
charge can be gradually built up by applying voltage pulses with the tip of a
scanning tunneling microscope (STM). The response of the conduction electrons
in graphene to the local charge is monitored with scanning tunneling and Landau
level spectroscopy, and compared to numerical simulations. As the charge is
increased, its interaction with the conduction electrons undergoes a transition
into a supercritical regime 6-11 where itinerant electrons are trapped in a
sequence of quasi-bound states which resemble an artificial atom. The
quasi-bound electron states are detected by a strong enhancement of the density
of states (DOS) within a disc centered on the vacancy site which is surrounded
by halo of hole states. We further show that the quasi-bound states at the
vacancy site are gate tunable and that the trapping mechanism can be turned on
and off, providing a new mechanism to control and guide electrons in grapheneComment: 18 pages and 5 figures plus 14 pages and 15 figures of supplementary
information. Nature Physics advance online publication, Feb 22 (2016
In-Plane Orbital Texture Switch at the Dirac Point in the Topological Insulator Bi2Se3
Topological insulators are novel macroscopic quantum-mechanical phase of
matter, which hold promise for realizing some of the most exotic particles in
physics as well as application towards spintronics and quantum computation. In
all the known topological insulators, strong spin-orbit coupling is critical
for the generation of the protected massless surface states. Consequently, a
complete description of the Dirac state should include both the spin and
orbital (spatial) parts of the wavefunction. For the family of materials with a
single Dirac cone, theories and experiments agree qualitatively, showing the
topological state has a chiral spin texture that changes handedness across the
Dirac point (DP), but they differ quantitatively on how the spin is polarized.
Limited existing theoretical ideas predict chiral local orbital angular
momentum on the two sides of the DP. However, there have been neither direct
measurements nor calculations identifying the global symmetry of the spatial
wavefunction. Here we present the first results from angle-resolved
photoemission experiment and first-principles calculation that both show,
counter to current predictions, the in-plane orbital wavefunctions for the
surface states of Bi2Se3 are asymmetric relative to the DP, switching from
being tangential to the k-space constant energy surfaces above DP, to being
radial to them below the DP. Because the orbital texture switch occurs exactly
at the DP this effect should be intrinsic to the topological physics,
constituting an essential yet missing aspect in the description of the
topological Dirac state. Our results also indicate that the spin texture may be
more complex than previously reported, helping to reconcile earlier conflicting
spin resolved measurements
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