No Arabic abstract
Femtosecond reflection spectroscopy was performed on a perovskite-type manganite, Gd0.55Sr0.45MnO3, with the short-range charge and orbital order (CO/OO). Immediately after the photoirradiation, a large increase of the reflectivity was detected in the mid-infrared region. The optical conductivity spectrum under photoirradiation obtained from the Kramers-Kronig analyses of the reflectivity changes demonstrates a formation of a metallic state. This suggests that ferromagnetic spin arrangements occur within the time resolution (ca. 200 fs) through the double exchange interaction, resulting in an ultrafast CO/OO to FM switching.
In the mixed-valence manganites, a near-infrared laser typically melts the orbital and spin order simultaneously, corresponding to the photoinduced $d^{1}d^{0}$ $xrightarrow{}$ $d^{0}d^{1}$ excitations in the Mott-Hubbard bands of manganese. Here, we use ultrafast methods -- both femtosecond resonant x-ray diffraction and optical reflectivity -- to demonstrate that the orbital response in the layered manganite Nd$_{1-x}$Sr$_{1+x}$MnO$_{4}$ ($it{x}$ = 2/3) does not follow this scheme. At the photoexcitation saturation fluence, the orbital order is only diminished by a few percent in the transient state. Instead of the typical $d^{1}d^{0}$ $xrightarrow{}$ $d^{0}d^{1}$ transition, a near-infrared pump in this compound promotes a fundamentally distinct mechanism of charge transfer, the $d^{0}$ $ xrightarrow{}$ $d^{1}L$, where $it{L}$ denotes a hole in the oxygen band. This novel finding may pave a new avenue for selectively manipulating specific types of order in complex materials of this class.
Metallization of 1T-TaS2 is generally initiated at the domain boundary of charge density wave (CDW), at the expense of its long-range order. However, we demonstrate in this study that the metallization of 1T-TaS2 can be also realized without breaking the long-range CDW order upon surface alkali doping. By using scanning tunneling microscopy, we find the long-range CDW order is always persisting, and the metallization is instead associated with additional in-gap excitations. Interestingly, the in-gap excitation is near the top of the lower Hubbard band, in contrast to a conventional electron-doped Mott insulator where it is beneath the upper Hubbard band. In combination with the numerical calculations, we suggest that the appearance of the in-gap excitations near the lower Hubbard band is mainly due to the effectively reduced on-site Coulomb energy by the adsorbed alkali ions.
Through a combination of neutron diffraction and Landau theory we describe the spin ordering in the ground state of the quadruple perovskite manganite CaMn7O12 - a magnetic multiferroic supporting an incommensurate orbital density wave that onsets above the magnetic ordering temperature, TN1 = 90 K. The multi-k magnetic structure in the ground state was found to be a nearly-constant-moment helix with modulated spin helicity, which oscillates in phase with the orbital occupancies on the Mn3+ sites via trilinear magneto-orbital coupling. Our phenomenological model also shows that, above TN2 = 48 K, the primary magnetic order parameter is locked into the orbital wave by an admixture of helical and collinear spin density wave structures. Furthermore, our model naturally explains the lack of a sharp dielectric anomaly at TN1 and the unusual temperature dependence of the electrical polarisation.
We report coherent x-ray scattering studies of charge and orbital domains in manganite systems. The experiments were carried out on LaMnO_3 and Pr_{0.6}Ca_{0.4}MnO_3, with the incident photon energy tuned near the Mn K edge. At room temperature, the orbital speckle pattern of LaMnO_3 was observed to be constant over a timescale of at least minutes, which is indicative of static orbital domains on this timescale. For Pr_{0.6}Ca_{0.4}MnO_3, both charge and orbital speckle patterns were observed. The observation of the latter rules out the presence of fast orbital fluctuations, while long time series data-- on the order of several minutes-- were suggestive of slow dynamic behavior. In contrast, the charge order speckle patterns were static.
We report on the in-plane anisotropy of the electronic response in the spin/charge/orbital ordered phase of a half-doped layered-structure manganite. The optical conductivity spectra for a single domain of Eu$_{1/2}$% Ca$_{3/2}$MnO$_{4}$ unambiguously show the anisotropic charge dynamics which well corresponds to the theoretical calculation: the optical conductivity with the polarization along the zigzag ferromagnetic chain direction exhibits a smaller gap and a larger intensity at lower energies than that of the perpendicular polarization mostly due to the charge/orbital ordering and the associated quantum interference effect.