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Register a new userStrong light-field effects driven by nearly single-cycle 7-fs light field in correlated organic conductors
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We have demonstrated transient charge localization effects with a driving high-frequency field of 7-fs, 1.5-cycle near infrared light in correlated organic conductors. In a layered organic conductor alpha-(BEDT-TTF)2I3 (BEDT-TTF: bis[ethylenedithio]-tetrathiafulvalene), a transient short-range charge order (CO) state is induced in a metallic phase. In contrast to such drastic change in the electronic state from the metal to the transient CO in alpha-(BEDT-TTF)2I3, dynamics of a field-induced reduction of a transfer integral are captured as a red shift of the plasma-like reflectivity edge in a quasi-one-dimensional organic conductor (TMTTF)2AsF6 (TMTTF: tetramethyltetrathiafulvalene). These studies on the field-induced charge localization have been motivated by the theory of dynamical localization on the basis of tight-binding models with no electron correlation under a strong continuous field. However, the results of pump-probe transient reflectivity measurements using nearly single-cycle 7-fs, 11 MV/cm pulses and the theoretical studies which are presented in this review indicate that the pulsed field contributes to the similar phenomenon with the help of a characteristic lattice structure and Coulomb repulsion.
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Polarization selectivity of light-field-induced charge localization was investigated in an organic metal alpha-(BEDT-TTF)2I3 with a triangular lattice. Dependences of transient reflectivity spectra on polarizations of the 7-fs pump and probe lights indicate that a short-range charge order (CO) is efficiently induced from the metallic phase for the pump polarization perpendicular to the 1010-type CO axis. Numerical solution of a time-dependent Schrodinger equation clarified that the 1010-CO is induced by field-induced re-distribution of charges cooperating with competing inter-site Coulomb repulsions in the triangular lattice.
The strong light-field effect of (TMTTF)2AsF6 was investigated utilizing 1.5-cycle, 7-fs infrared pulses. The ultarfast (20 fs) and large (40%) response of the plasma-like reflectivity edge (0.7 eV) was analyzed by the changes in omega_p=sqrt(ne2/(epsilon_0*epsilon(infty)*m)} (n: number of charges in the 1/4 filled-band, m: mass of charge, epsilon(infty): dielectric constants for high-frequency and vacuum, e: elementary charge). The 3% reduction in omega_p is attributed to the 6% increase in m. Furthermore, 20 fs oscillation of omega_p in the time domain indicates that the plasma-like edge is affected by the charge gap (0.2 eV) nature. Theoretical calculations suggest that the Coulomb repulsion plays an important role in the increase in m.
Intense light-field application to solids produces enormous/ultrafast non-linear phenomena such as high-harmonic generations 1, 2 and attosecond charge dynamics 3, 4. They are distinct from conventional photonics. However, main targets have been limited to insulators and semiconductors, although theoretical approaches have been made also for correlated metals and superconductors 5. Here, in a layered organic superconductor, a non-linear charge oscillation driven by a nearly single-cycle strong electric field of >10 megavolts /cm is observed as a stimulated emission. The charge oscillation is different from a linear response and ascribed to a polar charge oscillation with a period of 6 fs. This non-linear polar charge oscillation is enhanced by critical fluctuations near a superconducting transition temperature and a critical end point of first order Mott transitions. Its observation on an ultrafast timescale of 10 fs clarifies that the Coulomb repulsion plays an essential role in superconductivity of organic superconductors.
We report on an ultrafast photoinduced phase transition with a strikingly long-lived Martensitic anomaly driven by above-threshold single-cycle terahertz (THz) pulses in Nb$_3$Sn. A non-thermal, THz-induced depletion of low frequency conductivity indicates increased gap splitting of high energy $Gamma_{12}$ bands by removal of their degeneracies which enhances the Martensitic phase. In contrast, optical pumping leads to a $Gamma_{12}$ gap melting. Such light-induced non-equilibrium Martensitic instability persists up to a critical temperature $sim$100 K, i.e., more than twice the equilibrium temperature, and can be stabilized beyond technologically-relevant, nanosecond timescales. Together with first-principle simulations, we identify a compelling THz tuning of structural fluctuations via E$_u$ phonons to achieve a non-equilibrium ordering at high temperatures far exceeding those for equilibrium states.
We perform charge-induced absorption and electroluminescence spectroscopy in a polyfluorene organic magnetoresistive device. Our experiments allow us to measure the singlet exciton, triplet exciton and polaron densities in a live device under an applied magnetic field, and to distinguish between three different models that were proposed to explain organic magnetoresistance. These models are based on different spin-dependent interactions, namely exciton formation, triplet exciton-polaron quenching and bipolaron formation. We show that the singlet exciton, triplet exciton and polaron densities and conductivity all increase with increasing magnetic field. Our data are inconsistent with the exciton formation and triplet-exciton polaron quenching models.
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