188 research outputs found
Nonlinear electron-phonon coupling in doped manganites
We employ time-resolved resonant x-ray diffraction to study the melting of
charge order and the associated insulator-metal transition in the doped
manganite PrCaMnO after resonant excitation of a
high-frequency infrared-active lattice mode. We find that the charge order
reduces promptly and highly nonlinearly as function of excitation fluence.
Density functional theory calculations suggest that direct anharmonic coupling
between the excited lattice mode and the electronic structure drive these
dynamics, highlighting a new avenue of nonlinear phonon control
Nonlinear lattice dynamics as a basis for enhanced superconductivity in YBa2Cu3O6.5
THz-frequency optical pulses can resonantly drive selected vibrational modes
in solids and deform their crystal structure. In complex oxides, this method
has been used to melt electronic orders, drive insulator to metal transitions
or induce superconductivity. Strikingly, coherent interlayer transport strongly
reminiscent of superconductivity can be transiently induced up to room
temperature in YBa2Cu3O6+x. By combining femtosecond X-ray diffraction and ab
initio density functional theory calculations, we determine here the crystal
structure of this exotic non-equilibrium state. We find that nonlinear lattice
excitation in normal-state YBa2Cu3O6+x at 100 K causes a staggered
dilation/contraction of the Cu-O2 intra/inter- bilayer distances, accompanied
by anisotropic changes in the in-plane O-Cu-O bond buckling. Density functional
theory calculations indicate that these motions cause dramatic changes in the
electronic structure. Amongst these, the enhancement in the dx2-y2 character of
the in-plane electronic structure is likely to favor superconductivity.Comment: 28 pages, including Supplemen
Photoinduced suppression of the ferroelectric instability in PbTe
The interactions between electrons and phonons drive a large array of
technologically relevant material properties including ferroelectricity,
thermoelectricity, and phase-change behaviour. In the case of many group IV-VI,
V, and related materials, these interactions are strong and the materials exist
near electronic and structural phase transitions. Their close proximity to
phase instability produces a fragile balance among the various properties. The
prototypical example is PbTe whose incipient ferroelectric behaviour has been
associated with large phonon anharmonicity and thermoelectricity. Experimental
measurements on PbTe reveal anomalous lattice dynamics, especially in the soft
transverse optical phonon branch. This has been interpreted in terms of both
giant anharmonicity and local symmetry breaking due to off-centering of the Pb
ions. The observed anomalies have prompted renewed theoretical and
computational interest, which has in turn revived focus on the extent that
electron-phonon interactions drive lattice instabilities in PbTe and related
materials. Here, we use Fourier-transform inelastic x-ray scattering (FT-IXS)
to show that photo-injection of free carriers stabilizes the paraelectric
state. With support from constrained density functional theory (CDFT)
calculations, we find that photoexcitation weakens the long-range forces along
the cubic direction tied to resonant bonding and incipient ferroelectricity.
This demonstrates the importance of electronic states near the band edges in
determining the equilibrium structure.Comment: 9 page, 3 figure
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