Optical freezing of charge motion in an organic conductor

Dynamical localization, i.e., reduction of the intersite electronic transfer integral t by an alternating electric field, E(omega) , is a promising strategy for controlling strongly correlated systems with a competing energy balance between t and the Coulomb repulsion energy. Here we describe a charge localization induced by the 9.3 MV/cm instantaneous electric field of a 1.5 cycle (7 fs) infrared pulse in an organic conductor alpha-(bis[ethylenedithio]-tetrathiafulvelene)_2I_3. A large reflectivity change of > 25% and a coherent charge oscillation along the time axis reflect the opening of the charge ordering gap in the metallic phase. This optical freezing of charges, which is the reverse of the photoinduced melting of electronic orders, is attributed to the 10% reduction of t driven by the strong, high-frequency (omega>t/h_bar) electric field.

Phonon-Spectrum Narrowing Induced by Ultrafast Charge Fluctuation in an Organic Dimer Mott Insulator

We have observed the characteristic temperature dependence of the intermolecular phonon spectrum in the organic dimer Mott insulator kappa-(ET)2Cu2(CN)3 exhibiting a dielectric anomaly at 30 K. The anomalous spectral narrowing of the 55 cm-1 phonon peak at 30 K was analyzed in terms of motional narrowing within the framework of a stationary Gaussian process, i. e., the phonon frequency is modulated by the ultrafast charge fluctuation. The spectral narrowing occurs because the time constant of the correlation time tau_c and the amplitude of the frequency modulation delta satisfy the relation tau_c<delta at 30 K. At temperatures below 30 K, the motional narrowing is disturbed by the increasing of tau_c, near the charge-glass or the short-range order at 6 K. On the other hand, for temperatures above 30 K, the motional narrowing is disturbed by the increase of delta with increasing temperature.

Collective excitation of electric dipole on molecular dimer in organic dimer-Mott insulator

The terahertz (THz) response in 10-100 cm^-1 was investigated in an organic dimer-Mott (DM) insulator kappa-(ET)_2Cu_2(CN)_3 that exhibits a relaxor-like dielectric anomaly. 30 cm^-1 band in the optical conductivity was attributable to collective excitation of the intra-dimer electric dipoles which are formed by an electron correlation. We succeeded in observing photoinduced enhancement of this 30 cm^-1 band, reflecting the growth of the electric dipole cluster in the DM phase. Such optical responses in kappa-(ET)_2Cu_2(CN)_3 reflect instability near the boundary between the DM-ferroelectric charge ordered phases.