Quantification of chirality based on electric toroidal monopole.

Chirality ubiquitously appears in nature; however, its quantification remains obscure owing to the lack of microscopic description at the quantum-mechanical level. We propose a way of evaluating chirality in terms of the electric toroidal monopole, a practical entity of time-reversal even pseudoscalar (parity-odd) objects reflecting relevant electronic wave functions. For this purpose, we analyze a twisted methane molecule at the quantum-mechanical level, showing that the electric toroidal monopoles become a quantitative indicator for chirality. In the twisted methane, we clarify that the handedness of chirality corresponds to the sign of the expectation value of the electric toroidal monopole and that the most important ingredient is the modulation of the spin-dependent imaginary hopping between the hydrogen atoms, while the relativistic spin-orbit coupling within the carbon atom is irrelevant for chirality.

Giant spin polarization and a pair of antiparallel spins in a chiral superconductor.

Chiral molecules can exhibit spin-selective charge emission, which is known as chirality-induced spin selectivity1,2. Despite the constituent light elements of the molecules, their spin polarization can approach or even exceed that of typical ferromagnets. This powerful capability may lead to applications in the chiral spintronics2 field. Although the origin of spin selectivity is elusive, two microscopic phenomena have been suggested based on experimental results: effective enhancement of spin-orbit interactions3 and chirality represented by a pair of oppositely polarized spins4,5. However, the hypotheses remain to be verified. Here we report the simultaneous observation of these two phenomena in an organic chiral superconductor by magnetoresistance measurements in the vicinity of the superconducting transition temperature. A pair of oppositely polarized spins is demonstrated by spatially mapping the spin polarity in an electric alternating current excitation. The obtained spin polarization exceeds that of the Edelstein effect6-10 by several orders of magnitude, which indicates an effective enhancement of the spin-orbit interaction. Our results demonstrate a solid-state analogue of spin accumulations assumed for chiral molecules, and may provide clues to the origin of their molecular counterparts. In addition, the innovative capability of spin-current sourcing will invigorate superconducting spintronics research11.

Terahertz-field-induced polar charge order in electronic-type dielectrics.

Ultrafast electronic-phase change in solids by light, called photoinduced phase transition, is a central issue in the field of non-equilibrium quantum physics, which has been developed very recently. In most of those phenomena, charge or spin orders in an original phase are melted by photocarrier generations, while an ordered state is usually difficult to be created from a non-ordered state by a photoexcitation. Here, we demonstrate that a strong terahertz electric-field pulse changes a Mott insulator of an organic molecular compound in κ-(ET)2Cu[N(CN)2]Cl (ET = bis(ethylenedithio)tetrathiafulvalene), to a macroscopically polarized charge-order state; herein, electronic ferroelectricity is induced by the collective intermolecular charge transfers in each dimer. In contrast, in an isostructural compound, κ-(ET)2Cu2(CN)3, which shows the spin-liquid state at low temperatures, a similar polar charge order is not stabilized by the same terahertz pulse. From the comparative studies of terahertz-field-induced second-harmonic-generation and reflectivity changes in the two compounds, we suggest the possibility that a coupling of charge and spin degrees of freedom would play important roles in the stabilization of polar charge order.

Petahertz non-linear current in a centrosymmetric organic superconductor.

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 quasi-particles. 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 many-body 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.

Mott transition by an impulsive dielectric breakdown.

The transition of a Mott insulator to metal, the Mott transition, can occur via carrier doping by elemental substitution, and by photoirradiation, as observed in transition-metal compounds and in organic materials. Here, we show that the application of a strong electric field can induce a Mott transition by a new pathway, namely through impulsive dielectric breakdown. Irradiation of a terahertz electric-field pulse on an ET-based compound, κ-(ET) 2Cu[N(CN) 2]Br (ET:bis(ethylenedithio)tetrathiafulvalene), collapses the original Mott gap of ∼30 meV with a ∼0.1 ps time constant after doublon-holon pair productions by quantum tunnelling processes, as indicated by the nonlinear increase of Drude-like low-energy spectral weights. Additionally, we demonstrate metallization using this method is faster than that by a femtosecond laser-pulse irradiation and that the transition dynamics are more electronic and coherent. Thus, strong terahertz-pulse irradiation is an effective approach to achieve a purely electronic Mott transition, enhancing the understanding of its quantum nature.

Novel electronic ferroelectricity in an organic charge-order insulator investigated with terahertz-pump optical-probe spectroscopy.

In electronic-type ferroelectrics, where dipole moments produced by the variations of electron configurations are aligned, the polarization is expected to be rapidly controlled by electric fields. Such a feature can be used for high-speed electric-switching and memory devices. Electronic-type ferroelectrics include charge degrees of freedom, so that they are sometimes conductive, complicating dielectric measurements. This makes difficult the exploration of electronic-type ferroelectrics and the understanding of their ferroelectric nature. Here, we show unambiguous evidence for electronic ferroelectricity in the charge-order (CO) phase of a prototypical ET-based molecular compound, α-(ET)2I3 (ET:bis(ethylenedithio)tetrathiafulvalene), using a terahertz pulse as an external electric field. Terahertz-pump second-harmonic-generation(SHG)-probe and optical-reflectivity-probe spectroscopy reveal that the ferroelectric polarization originates from intermolecular charge transfers and is inclined 27° from the horizontal CO stripe. These features are qualitatively reproduced by the density-functional-theory calculation. After sub-picosecond polarization modulation by terahertz fields, prominent oscillations appear in the reflectivity but not in the SHG-probe results, suggesting that the CO is coupled with molecular displacements, while the ferroelectricity is electronic in nature. The results presented here demonstrate that terahertz-pump optical-probe spectroscopy is a powerful tool not only for rapidly controlling polarizations, but also for clarifying the mechanisms of ferroelectricity.

Quasiparticles and Fermi liquid behaviour in an organic metal.

Many organic metals display exotic properties such as superconductivity, spin-charge separation and so on and have been described as quasi-one-dimensional Luttinger liquids. However, a genuine Fermi liquid behaviour with quasiparticles and Fermi surfaces have not been reported to date for any organic metal. Here, we report the experimental Fermi surface and band structure of an organic metal (BEDT-TTF)(3)Br(pBIB) obtained using angle-resolved photoelectron spectroscopy, and show its consistency with first-principles band structure calculations. Our results reveal a quasiparticle renormalization at low energy scales (effective mass m*=1.9 m(e)) and ω(2) dependence of the imaginary part of the self energy, limited by a kink at ~50 meV arising from coupling to molecular vibrations. The study unambiguously proves that (BEDT-TTF)(3)Br(pBIB) is a quasi-2D organic Fermi liquid with a Fermi surface consistent with Shubnikov-de Haas results.

Novel Pauli-paramagnetic quantum phase in a Mott insulator.

In Mott insulators, the strong electron-electron Coulomb repulsion localizes electrons. In dimensions greater than one, their spins are usually ordered antiferromagnetically at low temperatures. Geometrical frustrations can destroy this long-range order, leading to exotic quantum spin liquid states. However, their magnetic ground states have been a long-standing mystery. Here we show that a quantum spin liquid state in the organic Mott insulator EtMe(3)Sb[Pd(dmit)(2)](2) (where Et is C(2)H(5)-, Me is CH(3)-, and dmit is 1,3-dithiole-2-thione-4,5-dithiolate) with two-dimensional triangular lattice has Pauli-paramagnetic-like low-energy excitations, which are a hallmark of itinerant fermions. Our torque magnetometry down to low temperatures (30 mK) up to high fields (32 T) reveals distinct residual paramagnetic susceptibility comparable to that in a half-filled two-dimensional metal, demonstrating the magnetically gapless nature of the ground state. Moreover, our results are robust against deuteration, pointing toward the emergence of an extended 'quantum critical phase', in which low-energy spin excitations behave as in paramagnetic metals with Fermi surface, despite the frozen charge degree of freedom.

Extremely slow charge fluctuations in the metallic state of the two-dimensional molecular conductor theta-(BEDT-TTF)2RbZn(SCN)4.

Large charge disproportionation has been confirmed in the metallic state of a 1/4-filled organic conductor theta-(BEDT-TTF)2RbZn(SCN)4 by means of 13C-NMR analysis on a selectively 13C-enriched single crystal sample. By comparing the homogeneous and inhomogeneous linewidths, the temperature dependence of the extremely slow dynamics of charge fluctuations has been determined first. The exotic nature of the metallic state of this salt is discussed.