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We report the band structure calculations and the experimental results of resistivity and magnetic susceptibility in a spin-1/2 (BEDT-TTF)$^{\bullet +}$ monomer Mott insulator (BEDT-TTF)Cu[N(CN)$_2$]$_2$. The band calculations indicate a Dirac semimetal state with nodal lines at the Fermi level. The resistivity and the magnetic susceptibility as functions of temperature are well interpreted in terms of the monomer Mott insulating state instead of the expected semimetal state probably owing to strong electron correlation. In addition, we find that an Arrhenius-type steep reduction of the paramagnetic susceptibility appears below approximately 25 K, which indicates a spin-singlet ground state., 4 pages, 5 figures. J. Phys. Soc. Jpn (2022) in press

Wide ranges of absorbance spectra were measured to elucidate a difference in the antiferro-electric (AF) ordering mechanisms below 50 and 168 K in Cs

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., Here the authors show second harmonic generation (SHG) from a centrosymmetric organic superconductor κ-(BEDT-TTF)2Cu[N(CN)2]Br. They find unusual temperature dependence and CEP-sensitive nature of the SHG which are explained in terms of nonlinear current.

We report the structure and physical properties of a new radical–cationic Mott insulator θ-(BEDT-BDT)PF6 (BEDT-BDT: benzo[1,2-g:4,5-g′]bis(thieno[2,3-b][1,4]dithiin)). The crystal structure belongs to a monoclinic system with a 1 : 1 donor/anion ratio. Based on this composition, the salt is considered a half-filled Mott insulator, in which the BEDT-BDT molecules form a θ mode arrangement. Owing to the strong electron correlation, the temperature dependence of the resistivity exhibits semiconducting behaviour. The static magnetic susceptibility first follows the Curie–Weiss law down to 15 K, but then follows the two-dimensional (2D) triangular Heisenberg model with J = 7.5 K below 15 K. Even at 2 K, this salt is paramagnetic and no magnetic order is formed. The tight-binding band calculation reveals a 2D Fermi surface. It is remarkable that θ-(BEDT-BDT)PF6 forms a 2D electronic structure without any 1,3-dithiol-2-ylidene units, unlike tetrathiafulvalene and tetrathiapentalene donors.

We present a systematic investigation of the low-frequency charge carrier dynamics in different charge states of the organic conductors $\theta$-(BEDT-TTF)$_2$$M$Zn(SCN)$_4$ with $M$=Rb,Tl, which result from quenching or relaxing the charge degrees of freedom on a geometrically frustrated triangular lattice. Due to strong electronic correlations these materials exhibit a charge-ordering transition, which can be kinetically avoided by rapid cooling resulting in a so-called charge-glass state without long-range order. The combination of fluctuation spectroscopy and a heat pulse method allows us to study and compare the resistance fluctuations in the low-resistive quenched and the high-resistive charge-ordered state, revealing striking differences in the respective noise magnitudes. For both compounds, we find strongly enhanced resistance fluctuations right at the metal-insulator transition and a broad noise maximum in the slowly cooled charge-crystal state with partly dominating two-level processes revealing characteristic activation energies.

Magnetic susceptibility and torque measurements have been performed for neutral BEDT-TTF crystals to investigate the diamagnetic properties. The diamagnetic susceptibility is found to be anisotropi...

A citrate pyrolysis technique is a unique route to prepare reactive precursor mixtures through an ignition process of concentrated aqueous solution. This procedure enables to synthesize highly homogeneous and fine powders for functional materials. The double-chain based superconductor Pr2Ba4Cu7O15−δ and double perovskite photocatalytic semiconductor Ba2Tb(Bi,Sb)O6 were synthesized by using the citrate pyrolysis technique. For the present sample with a reduction treatment for 72 h, a sharp superconducting transition appeared at an onset temperature Tc,on=26 K accompanied by a zero-resistance state at Tc,zero=22 K. The superconducting volume fraction estimated from the magnetization measurement showed an excellent value of ∼58%. Both reduction treatment in a vacuum and subsequent quenching procedure are needed to realize higher superconductivity due to further oxygen defects. The polycrystalline samples for Ba2Tb(Bi1−x,Sbx)O6 (x=0 and 0.5) were formed in the monoclinic and cubic crystal structures. We conducted the gaseous 2-propanol (IPA) and methylene blue (MB) degradation experiments under a visible light irradiation, to evaluate photocatalytic activities of the powder samples. For the Sb50% substituted sample, the highest performance of MB degradation was observed. The effect of Sb-substitution on the photocatalytic degradation of MB is in direct contrast to that on the IPA decomposition under visible light irradiation. The enhanced photocatalytic properties in the citrate samples are attributed to their morphology, where fine particles are homogeneously distributed with a submicron order.

Recently, Urai et al. [Phys. Rev. Lett. 124, 117204 (2020)] reported that an antiferromagnetic long-range-ordered state in $\ensuremath{\kappa}$-${(\mathrm{ET})}_{2}\mathrm{Cu}\mathrm{[N}{(\mathrm{CN})}_{2}\mathrm{]Cl}$ changes into a quantum spin liquid via an unconventional spin glass-like state as randomness is introduced by x-ray irradiation. Here, we focused on the spin glass-like state and conducted a detailed investigation into it using $^{13}\mathrm{C}$-NMR measurements on 150-h x-ray-irradiated $\ensuremath{\kappa}$-$({\mathrm{ET})}_{2}\mathrm{Cu}\mathrm{[N(}{\mathrm{CN})}_{2}\mathrm{]Cl}$. We found that the spin glass-like state is composed of two components: the major component inherits the spin structure of nonirradiated $\ensuremath{\kappa}$-$({\mathrm{ET})}_{2}\mathrm{Cu}\mathrm{[N(}{\mathrm{CN})}_{2}\mathrm{]Cl}$, whereas the minor component differs from that of nonirradiated $\ensuremath{\kappa}$-${(\mathrm{ET})}_{2}\mathrm{Cu}\mathrm{[N(}{\mathrm{CN})}_{2}\mathrm{]Cl}$. We also found that in the spin glass-like state, spin moments fluctuate very slowly around stable directions even at low temperatures, which is very likely related to the Griffiths physics.

We report the structural and physical properties of a new organic Mott insulator (BEDT-BDT)AsF6 (BEDT-BDT: benzo[1,2-g:4,5-g′]bis(thieno[2,3-b][1,4dithiin). This AsF6 salt has the same structure as the PF6 salt. Although the anions are disordered, the donor molecules form a θ-type arrangement. The temperature dependence of the resistivity exhibits semiconducting behavior. The static magnetic susceptibility follows Curie–Weiss law over a wide temperature range, however, below 25 K, the magnetic susceptibility is in agreement with a one-dimensional chain model with the exchange coupling J = 7.4 K. No structural phase transition was observed down to 93 K. At 270 K, the Fermi surface calculated by the tight-binding approximation is a two-dimensional cylinder, however, it is significantly distorted at 93 K. This is because the dihedral angles between the BEDT-BDT molecules become larger due to lattice shrinkage at low temperatures, which results in a smaller transfer integral (t1) along the stack direction. This slight change in the dihedral angle gives rise to a significant change in the electronic structure of the AsF6 salt. Radical-cation salts using BEDT-BDT, in which the highest occupied molecular orbital does not have a dominant sign throughout the molecule, are sensitive to slight differences in the overlap between the molecules, and their electronic structures are more variable than those of conventional θ-type conductors.

$\ensuremath{\kappa}\text{\ensuremath{-}}{(\mathrm{BEDT}\text{\ensuremath{-}}\mathrm{TTF})}_{2}\mathrm{Cu}[\mathrm{N}{(\mathrm{CN})}_{2}]\mathrm{Br} (\ensuremath{\kappa}\text{\ensuremath{-}}\mathrm{Br})$ is an organic superconductor that changes to an Anderson-type insulator due to the random defects introduced by x-ray irradiation. In this study, we directly investigated the effects of irradiation on the local structures in the anion layer of $\ensuremath{\kappa}\text{\ensuremath{-}}\mathrm{Br}$ using x-ray fluorescence holography. The local structures around the Cu atoms in the anion layer were directly reconstructed from holograms. Prior to radiation damage, the reconstruction clearly shows the atomic images of the Br and N atoms that are directly coordinated to Cu. In the irradiated samples, the N images in the reconstructions were strongly suppressed as a result of the positional fluctuations of N introduced by the defects induced by irradiation. Using the previously proposed ``bond-shifted'' model and the thermal vibration amplitudes calculated from molecular dynamics simulations, we simulated the holograms and the atomic reconstructions of the anion layer. The simulations show that the ``bond-shifted'' model, along with thermal vibrations at 100 K, suppresses the N atomic images, as was observed in the experimental reconstructions.

This overview describes the progressive results of the superconducting critical temperature in bulk nanostructured metals (niobium, vanadium and tantalum) processed by high-pressure torsion (HPT). Bulk nanostructured superconductors provide a new route to control superconducting property, because ultrafine-grain structures with a high density of grain boundaries, dislocations, and other crystalline defects modify the superconducting order parameter. The critical temperature Tc in Nb increases with the evolution of grain refinement owing to the quantum confinement of electrons in ultrafine grains. In V and Ta, however, Tc decreases at a certain HPT revolution number (i.e. at certain strain levels). The different behaviour of Tc in the three materials is explained by the competition effect between the quantum size effect and disorder effect; these effects are characterized by the parameters of grain size, electron mean free path, and superconducting coherence length.

"Secondary doping" in poly(3,4-ethylenedioxy-thiophene):poly(styrenesulfonate) (PEDOT:PSS) is quite effective and a frequently used method for the conductivity enhancement. This simple approach, the addition of co-solvents to the PEDOT:PSS solution before film fabrication, is an essential way to derive the high electrical performance of PEDOT:PSS, but the mechanism still remains unclear. In this study, nanoscale structural changes synchronized with the conductivity enhancement via secondary doping in PEDOT:PSS films were investigated. During secondary doping with ethylene glycol near the critical dopant concentration, non-crystalized PEDOT molecules uncoupled from PSS chains and then underwent nano-crystallization. These structural changes might be the key driving force for conductivity enhancement via secondary doping., 9 pages, 7 figures, accepted for publication in J. Phys. Chem. C

Metal-organic frameworks (MOFs), which are self-assemblies of metal ions and organic ligands, provide a tunable platform to search a new state of matter. A two-dimensional (2D) perfect kagome lattice, whose geometrical frustration is a key to realizing quantum spin liquids, has been formed in the ${\pi}$-${d}$ conjugated 2D MOF [Cu$_{3}$(C$_{6}$S$_{6}$)]$_{n}$ (Cu-BHT). The recent discovery of its superconductivity with a critical temperature $T_{\rm c}$ of 0.25\,kelvin raises fundamental questions about the nature of electron pairing. Here, we show that Cu-BHT is a strongly correlated unconventional superconductor with extremely low superfluid density. A nonexponential temperature dependence of superfluid density is observed, indicating the possible presence of superconducting gap nodes. The magnitude of superfluid density is much smaller than those in conventional superconductors, and follows the Uemura's relation of strongly correlated superconductors. These results imply that the unconventional superconductivity in Cu-BHT originates from electron correlations related to spin fluctuations of kagome lattice., Comment: 4 figures

The mechanism of unconventional superconductivity, such as high-temperature-cuprate, Fe-based, and heavy-fermion superconductors, has been studied as a central issue in condensed-matter physics. Spin fluctuations, instead of phonons, are considered to be responsible for the formation of Cooper pairs, and many efforts have been made to confirm this mechanism experimentally. Although a qualitative consensus seems to have been obtained, experimental confirmation has not yet been achieved. This is owing to a lack of the quantitative comparison between theory and experiments. Here, we show a semi-quantitative comparison between the superconducting-transition temperature ($T_{\rm SC}$) and spin fluctuations derived from the nuclear magnetic resonance (NMR) experiment on the ferromagnetic (FM) superconductor UCoGe, in which the FM fluctuations and superconductivity are tunable by external fields. The enhancement and abrupt suppression of $T_{\rm SC}$ by applied fields, as well as the pressure variation of $T_{\rm SC}$ around the FM criticality are well understood by the change in the FM fluctuations on the basis of the single-band spin-triplet theoretical formalism. The present comparisons strongly support the theoretical formalism of spin-fluctuation-mediated superconductivity, particularly in UCoGe., Comment: 10 pages, 8 pages. To be published in Phys. Rev. B

We investigate the low-frequency charge-carrier dynamics of a molecular dimer-Mott insulator ${\ensuremath{\beta}}^{\ensuremath{'}}\ensuremath{-}{(\mathrm{BEDT}\ensuremath{-}\mathrm{TTF})}_{2}{\mathrm{ICl}}_{2}$, where the freezing of charge fluctuations on the dimers gives rise to electronic ferroelectricity. We show that conductance fluctuation (noise) spectroscopy allows one to probe changes in the dielectric properties at elevated temperatures, where samples are even still in the conductive regime. Our results explain the formation of electric polarization states leading to glassy and relaxor-type ferroelectric behavior that is frequently observed in these systems. The onset of distinct two-level fluctuations and changes of the underlying $1/f$-type noise indicate the formation of nanoscale polar regions, the dynamics of which depends on the applied electric fields. Conductance noise spectroscopy therefore is a suitable tool for investigating the onset of electric-polarization dynamics in molecular and other, inorganic charge-driven ferroelectrics.

We present a $^{35}$Cl NMR study for spin $S=1/2$ perfect kagome antiferromagnet Ca-kapellasite (CaCu$_{3}$(OH)$_{6}$Cl$_{2}\cdot$0.6H$_{2}$O) with a magnetic transition at $T^{\ast}=7.2$ K. The static magnetic structure in the ground state has been determined to be a chirality-ordered $Q=0$ state, which is selected by a finite Dzyaloshinskii-Moriya interaction. The low-energy magnetic excitations in the ordered state are investigated by the nuclear spin-lattice relaxation rate measurement. We detect a weakly temperature dependent contribution in the magnetic fluctuations perpendicular to the kagome plane in addition to the dispersive spin-wave contribution in the kagome plane. The low-energy magnetic excitations from the coplanar spin structure are attributed to the zero mode originating from the flat band in this kagome antiferromagnet., Comment: 5 pages, 5 figures

In phases III and IV of Cs

Perovskite oxides $AB{\mathrm{O}}_{3}$ containing heavy B-site elements are a class of candidate materials to host topological metals with a large spin-orbit interaction. In contrast to the band insulator $\mathrm{BaSn}{\mathrm{O}}_{3}$, the semimetal $\mathrm{BaPb}{\mathrm{O}}_{3}$ is proposed to be a typical example with an inverted band structure, the conduction band of which is composed of mainly the $\mathrm{O}\text{\ensuremath{-}}2p$ orbital. In this paper, we exemplify a band-gap modification by systematic structural, optical, and transport measurements in $\mathrm{BaS}{\mathrm{n}}_{1\ensuremath{-}x}\mathrm{P}{\mathrm{b}}_{x}{\mathrm{O}}_{3}$ films. A sudden suppression of the conductivity and an enhancement of the weak antilocalization effect at $x=0.9$ indicate the presence of a singular point in the electronic structure as a signature of the band inversion. Our findings provide an intriguing platform for combining topological aspects and electron correlation in perovskite oxides based on band-gap engineering.

Solid-state physics and soft-matter physics have been developed independently, with little mutual exchange of the underlying physical concepts. However, after many studies of correlated electron systems, it has been recognized that correlated electrons (especially in Mott-transition systems) in solid matter sometimes show behavior similar to "structured fluids" in soft matter; that is, the electrons exhibit long-length self-organization (but without long-range order) and slow dynamics, which is inevitable for the long-length structures. The essential question is this: what condition causes such behavior in solid matter? We focused on an organic Mott-transition system and demonstrated that the electrons of this system fluctuate very slowly only when the following two factors are met simultaneously: (i) the electronic system is on the metal and Mott-insulator boundary and (ii) the system is subject to quenched disorder. This electronic state with slow dynamics under this condition can be explained by the concept of the "(electronic) Griffiths phase." This concept will potentially be a key in connecting solid-state physics with soft-matter physics.