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1.
Phys Rev Lett ; 131(7): 076901, 2023 Aug 18.
Artigo em Inglês | MEDLINE | ID: mdl-37656841

RESUMO

We report ultrafast x-ray scattering experiments of the quasi-1D charge density wave (CDW) material (TaSe_{4})_{2}I following ultrafast infrared photoexcitation. From the time-dependent diffraction signal at the CDW sidebands we identify a 0.11 THz amplitude mode derived primarily from a transverse acoustic mode of the high-symmetry structure. From our measurements we determine that this mode interacts with the valence charge indirectly through another collective mode, and that the CDW system in (TaSe_{4})_{2}I has a composite nature supporting multiple dynamically active structural degrees of freedom.

2.
Phys Rev Lett ; 129(12): 127601, 2022 Sep 16.
Artigo em Inglês | MEDLINE | ID: mdl-36179158

RESUMO

We use an x-ray free-electron laser to study the lattice dynamics following photoexcitation with ultrafast near-UV light (wavelength 266 nm, 50 fs pulse duration) of the incipient ferroelectric potassium tantalate, KTaO_{3}. By probing the lattice dynamics corresponding to multiple Brillouin zones through the x-ray diffuse scattering with pulses from the Linac Coherent Light Source (LCLS) (wavelength 1.3 Å and <10 fs pulse duration), we observe changes in the diffuse intensity associated with a hardening of the transverse acoustic phonon branches along Γ to X and Γ to M. Using force constants from density functional theory, we fit the quasiequilibrium intensity and obtain the instantaneous lattice temperature and density of photoexcited charge carriers. The density functional theory calculations demonstrate that photoexcitation transfers charge from oxygen 2p derived π-bonding orbitals to Ta 5d derived antibonding orbitals, further suppressing the ferroelectric instability and increasing the stability of the cubic, paraelectric structure.

3.
Phys Rev Lett ; 116(19): 196401, 2016 May 13.
Artigo em Inglês | MEDLINE | ID: mdl-27232028

RESUMO

We use angle resolved photoemission spectroscopy, Raman spectroscopy, low energy electron diffraction, and x-ray scattering to reveal an unusual electronically mediated charge density wave (CDW) in K_{0.9}Mo_{6}O_{17}. Not only does K_{0.9}Mo_{6}O_{17} lack signatures of electron-phonon coupling, but it also hosts an extraordinary surface CDW, with T_{S_CDW}=220 K nearly twice that of the bulk CDW, T_{B_CDW}=115 K. While the bulk CDW has a BCS-like gap of 12 meV, the surface gap is 10 times larger and well in the strong coupling regime. Strong coupling behavior combined with the absence of signatures of strong electron-phonon coupling indicates that the CDW is likely mediated by electronic interactions enhanced by low dimensionality.

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