142 research outputs found
Long-range charge density wave proximity effect at cuprate-manganate interfaces
The interplay between charge density waves (CDWs) and high-temperature
superconductivity is currently under intense investigation. Experimental
research on this issue is difficult because CDW formation in bulk copper-oxides
is strongly influenced by random disorder, and a long-range-ordered CDW state
in high magnetic fields is difficult to access with spectroscopic and
diffraction probes. Here we use resonant x-ray scattering in zero magnetic
field to show that interfaces with the metallic ferromagnet
LaCaMnO greatly enhance CDW formation in the optimally
doped high-temperature superconductor YBaCuO (), and that this effect persists over several tens of nm. The wavevector
of the incommensurate CDW serves as an internal calibration standard of the
charge carrier concentration, which allows us to rule out any significant
influence of oxygen non-stoichiometry, and to attribute the observed phenomenon
to a genuine electronic proximity effect. Long-range proximity effects induced
by heterointerfaces thus offer a powerful method to stabilize the charge
density wave state in the cuprates, and more generally, to manipulate the
interplay between different collective phenomena in metal oxides.Comment: modified version published in Nature Material
Orbital control of noncollinear magnetic order in nickelate heterostructures
We have used resonant x-ray diffraction to develop a detailed description of
antiferromagnetic ordering in epitaxial superlattices based on two-unit-cell
thick layers of the strongly correlated metal LaNiO3. We also report reference
experiments on thin films of PrNiO3 and NdNiO3. The resulting data indicate a
spiral state whose polarization plane can be controlled by adjusting the Ni
d-orbital occupation via two independent mechanisms: epitaxial strain and
quantum confinement of the valence electrons. The data are discussed in the
light of recent theoretical predictions.Comment: 5 pages, 3 figure
Long-range transfer of electron-phonon coupling in oxide superlattices
The electron-phonon interaction is of central importance for the electrical
and thermal properties of solids, and its influence on superconductivity,
colossal magnetoresistance, and other many-body phenomena in
correlated-electron materials is currently the subject of intense research.
However, the non-local nature of the interactions between valence electrons and
lattice ions, often compounded by a plethora of vibrational modes, present
formidable challenges for attempts to experimentally control and theoretically
describe the physical properties of complex materials. Here we report a Raman
scattering study of the lattice dynamics in superlattices of the
high-temperature superconductor and the
colossal-magnetoresistance compound that suggests
a new approach to this problem. We find that a rotational mode of the MnO
octahedra in experiences pronounced
superconductivity-induced lineshape anomalies, which scale linearly with the
thickness of the layers over a remarkably long range of
several tens of nanometers. The transfer of the electron-phonon coupling
between superlattice layers can be understood as a consequence of long-range
Coulomb forces in conjunction with an orbital reconstruction at the interface.
The superlattice geometry thus provides new opportunities for controlled
modification of the electron-phonon interaction in complex materials.Comment: 13 pages, 4 figures. Revised version to be published in Nature
Material
Giant phonon anomalies and central peak due to charge density wave formation in YBaCuO
The electron-phonon interaction is a major factor influencing the competition
between collective instabilities in correlated-electron materials, but its role
in driving high-temperature superconductivity in the cuprates remains poorly
understood. We have used high-resolution inelastic x-ray scattering to monitor
low-energy phonons in YBaCuO (superconducting
K), which is close to a charge density wave (CDW) instability. Phonons in a
narrow range of momentum space around the CDW ordering vector exhibit extremely
large superconductivity-induced lineshape renormalizations. These results imply
that the electron-phonon interaction has sufficient strength to generate
various anomalies in electronic spectra, but does not contribute significantly
to Cooper pairing. In addition, a quasi-elastic "central peak" due to CDW
nanodomains is observed in a wide temperature range above and below ,
suggesting that the gradual onset of a spatially inhomogeneous CDW domain state
with decreasing temperature is a generic feature of the underdoped cuprates
Advances in ab-initio theory of Multiferroics. Materials and mechanisms: modelling and understanding
Within the broad class of multiferroics (compounds showing a coexistence of
magnetism and ferroelectricity), we focus on the subclass of "improper
electronic ferroelectrics", i.e. correlated materials where electronic degrees
of freedom (such as spin, charge or orbital) drive ferroelectricity. In
particular, in spin-induced ferroelectrics, there is not only a {\em
coexistence} of the two intriguing magnetic and dipolar orders; rather, there
is such an intimate link that one drives the other, suggesting a giant
magnetoelectric coupling. Via first-principles approaches based on density
functional theory, we review the microscopic mechanisms at the basis of
multiferroicity in several compounds, ranging from transition metal oxides to
organic multiferroics (MFs) to organic-inorganic hybrids (i.e. metal-organic
frameworks, MOFs)Comment: 22 pages, 9 figure
Mottness at finite doping and charge instabilities in cuprates
The intrinsic instability of underdoped copper oxides towards inhomogeneous states is one of the central puzzles of the physics of correlated materials. The influence of the Mott physics on the doping-temperature phase diagram of copper oxides represents a major issue that is subject of intense theoretical and experimental effort. Here, we investigate the ultrafast electron dynamics in prototypical single-layer Bi-based cuprates at the energy scale of the O-2p\u2192Cu-3d charge-transfer (CT) process. We demonstrate a clear evolution of the CT excitations from incoherent and localized, as in a Mott insulator, to coherent and delocalized, as in a conventional metal. This reorganization of the high-energy degrees of freedom occurs at the critical doping pcr 430.16 irrespective of the temperature, and it can be well described by dynamical mean field theory calculations. We argue that the onset of the low-temperature charge instabilities is the low-energy manifestation of the underlying Mottness that characterizes the p<pcr region of the phase diagram. This discovery sets a new framework for theories of charge order and low-temperature phases in underdoped copper oxides. ArXI
Intense paramagnon excitations in a large family of high-temperature superconductors
In the search for the mechanism of high-temperature superconductivity,
intense research has been focused on the evolution of the spin excitation
spectrum upon doping from the antiferromagnetic insulating to the
superconducting states of the cuprates. Because of technical limitations, the
experimental investigation of doped cuprates has been largely focused on
low-energy excitations in a small range of momentum space. Here we use resonant
inelastic x-ray scattering to show that a large family of superconductors,
encompassing underdoped YBaCuO and overdoped YBaCuO,
exhibits damped spin excitations (paramagnons) with dispersions and spectral
weights closely similar to those of magnons in undoped cuprates. %The results
are in excellent agreement with the spin excitations obtained by exact
diagonalization of the Hamiltonian on finite-sized clusters. The
comprehensive experimental description of this surprisingly simple spectrum
permits quantitative tests of magnetic Cooper pairing models. A numerical
solution of the Eliashberg equations for the magnetic spectrum of
YBaCuO reproduces its superconducting transition temperature
within a factor of two, a level of agreement comparable to Eliashberg theories
of conventional superconductors.Comment: Main text (11 pages, 4 figures) + supplementary information (4 pages,
4 figures, 1 table). An updated version will appear in Nature Physic
Surface Doping Quantum Dots with Chemically Active Native Ligands: Controlling Valence without Ligand Exchange
One remaining challenge in the field of colloidal semiconductor nanocrystal quantum dots is learning to control the degree of functionalization or valence per nanocrystal. Current quantum dot surface modification strategies rely heavily on ligand exchange, which consists of replacing the nanocrystal\u27s native ligands with carboxylate- or amine-terminated thiols, usually added in excess. Removing the nanocrystal\u27s native ligands can cause etching and introduce surface defects, thus affecting the nanocrystal\u27s optical properties. More importantly, ligand exchange methods fail to control the extent of surface modification or number of functional groups introduced per nanocrystal. Here, we report a fundamentally new surface ligand modification or doping approach aimed at controlling the degree of functionalization or valence per nanocrystal while retaining the nanocrystal\u27s original colloidal and photostability. We show that surface-doped quantum dots capped with chemically active native ligands can be prepared directly from a mixture of ligands with similar chain lengths. Specifically, vinyl and azide-terminated carboxylic acid ligands survive the high temperatures needed for nanocrystal synthesis. The ratio between chemically active and inactive-terminated ligands is maintained on the nanocrystal surface, allowing to control the extent of surface modification by straightforward organic reactions. Using a combination of optical and structural characterization tools, including IR and 2D NMR, we show that carboxylates bind in a bidentate chelate fashion, forming a single monolayer of ligands that are perpendicular to the nanocrystal surface. Moreover, we show that mixtures of ligands with similar chain lengths homogeneously distribute themselves on the nanocrystal surface. We expect this new surface doping approach will be widely applicable to other nanocrystal compositions and morphologies, as well as to many specific applications in biology and materials science
Molecular Chemistry to the Fore: New Insights into the Fascinating World of Photoactive Colloidal Semiconductor Nanocrystals
Colloidal semiconductor nanocrystals possess unique properties that are unmatched by other chromophores such as organic dyes or transition-metal complexes. These versatile building blocks have generated much scientific interest and found applications in bioimaging, tracking, lighting, lasing, photovoltaics, photocatalysis, thermoelectrics, and spintronics. Despite these advances, important challenges remain, notably how to produce semiconductor nanostructures with predetermined architecture, how to produce metastable semiconductor nanostructures that are hard to isolate by conventional syntheses, and how to control the degree of surface loading or valence per nanocrystal. Molecular chemists are very familiar with these issues and can use their expertise to help solve these challenges. In this Perspective, we present our group\u27s recent work on bottom-up molecular control of nanoscale composition and morphology, low-temperature photochemical routes to semiconductor heterostructures and metastable phases, solar-to-chemical energy conversion with semiconductor-based photocatalysts, and controlled surface modification of colloidal semiconductors that bypasses ligand exchange
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