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Register a new userReal space imaging of the metal - insulator phase separation in the band width controlled organic Mott system $kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br
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Systematic investigation of the electronic phase separation on macroscopic scale is reported in the organic Mott system $kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br. Real space imaging of the phase separation is obtained by means of scanning micro-region infrared spectroscopy using the synchrotron radiation. The phase separation appears near the Mott boundary and changes its metal-insulator fraction with the substitution ratio $x$ in $kappa$-[($h$-BEDT-TTF)$_{1-x}$($d$-BEDT-TTF)$_{x}$]$_{2}$Cu[N(CN)$_{2}$]Br, of which band width is controlled by the substitution ratio $x$ between the hydrogenated BEDT-TTF molecule ($h$-BEDT-TTF) and the deuterated one ($d$-BEDT-TTF). The phase separation phenomenon observed in this class of organics is considered on the basis of the strongly correlated electronic phase diagram with the first order Mott transition.
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The magnetic field effect on the phase diagram of the organic Mott system $kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br in which the bandwidth was tuned by the substitution of deuterated molecules was studied by means of the resistivity measurements performed in magnetic fields. The lower critical point of the first-order Mott transition, which ended on the upper critical field $H_{rm c2}$-temperature plane of the superconductivity, was determined experimentally in addition to the previously observed upper critical end point. The lower critical end point moved to a lower temperature with the suppression of $T_{rm c}$ in magnetic fields and the Mott transition recognized so far as the $S$-shaped curve reached $T =$ 0 when $H > H_{rm c2}$ in the end.
The effect of disorder on the electronic properties near the Mott transition is studied in an organic superconductor $kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br, which is systematically irradiated by X-ray. We observe that X-ray irradiation causes Anderson-type electron localization due to molecular disorder. The resistivity at low temperatures demonstrates variable range hopping conduction with Coulomb interaction. The experimental results show clearly that the electron localization by disorder is enhanced by the Coulomb interaction near the Mott transition.
We performed $^{13}$C-NMR experiment and measured spin-lattice relaxation rate divided by temperature $1/T_{1}T$ near the superconducting (SC) transition temperature $T_{c}$ in $kappa$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br ($kappa$-Br salt), and $kappa$-(BEDT-TTF)$_{2}$Cu(NCS)$_{2}$ ($kappa$-NCS salt). We observed the reduction of $1/T_{1}T$ starting at the temperature higher than $T_c$ in $kappa$-Br salt. Microscopic observation of quasi-particle density of states in the fluctuating SC state revealed the effects of short-range Cooper pairs induced in the normal state to the quasi-particle density of states. We also performed systematic measurements in the fields both parallel and perpendicular to the conduction plane in $kappa$-Br and $kappa$-NCS salts, and confirmed that the reduction of $1/T_{1}T$ above $T_{c}$ is observed only in $kappa$-Br salt regardless of the external field orientation.
The interplane optical spectrum of the organic superconductor kappa-(BEDT-TTF)2Cu[N(CN)2]Br was investigated in the frequency range from 40 to 40,000 cm-1. The optical conductivity was obtained by Kramers-Kronig analysis of the reflectance. The absence of a Drude peak at low frequency is consistent with incoherent conductivity but in apparent contradiction to the metallic temperature dependence of the DC resistivity. We set an upper limit to the interplane transfer integral of tb = 0.1 meV. A model of defect-assisted interplane transport can account for this discrepancy. We also assign the phonon lines in the conductivity to the asymmetric modes of the ET molecule.
Electronic phase separation consisting of the metallic and insulating domains with 50 -- 100 $mu$m in diameter is found in the organic Mott system $kappa$-[($h$8-BEDT-TTF)$_{1-x}$($d$8-BEDT-TTF)$_{x}$]$_{2}$Cu[N(CN)$_{2}$]Br by means of scanning micro-region infrared spectroscopy using the synchrotron radiation. The phase separation appears below the critical end temperature 35 -- 40 K of the first order Mott transition. The observation of the macroscopic size of the domains indicates a different class of the intrinsic electronic inhomogeneity from the nano-scale one reported in the inorganic Mott systems such as High-$T_{c}$ copper and manganese oxides.
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