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.
Supplementary information forNonlinear charge oscillation driven by a single-cycle light field in an organic superconductor
Polarization selectivity of light-field-induced charge localization was investigated in an organic metal a-(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 Schrödinger 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.
Charge acceleration during an intense light field application to solids attracts much attention as elementary processes in high-harmonic generation and photoelectron emission. For manipulating such attosecond dynamics of charge, carrier-envelope-phase (CEP: relative phase between carrier oscillation of light field and its envelope function) control has been employed in insulators, nanometal and graphene. In superconducting materials, collective control of charge motion is expected because of its strongly coherent nature of quasiparticles. Here we report that, in a layered organic superconductor, a non-linear petahertz current driven by a single-cycle 6 femtosecond near infrared field shows up as second harmonic generation (SHG), which is in contrast to the common belief that even harmonics are forbidden in the centrosymmetric system. The SHG represents a CEP sensitive nature and an enhancement near the superconducting temperature. The result and its quantum manybody analysis indicate that a polarized current is induced by non-linear acceleration of charge, which is amplified by superconducting fluctuations. This will lead to petahertz functions of superconductors and of strongly correlated systems.
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