arXiv subjects

N. Yoneyama

Publications and source records attributed to N. Yoneyama.

At least 19 recordsLinked to original sources

arXiv2022

A Monomer Mott Insulator (BEDT-TTF)Cu[N(CN)$_2$]$_2$ as a Potential Nodal Line System

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.

cond-mat.str-el↗

arXiv2017

Crystallization and vitrification of electrons in a glass-forming charge liquid

Charge ordering (CO) is a phenomenon in which electrons in solids crystallize into a periodic pattern of charge-rich and charge-poor sites owing to strong electron correlations. This usually results in long-range order. In geometrically frustrated systems, however, a glassy electronic state without long-range CO has been observed. We found that a charge-ordered organic material with an isosceles triangular lattice shows charge dynamics associated with crystallization and vitrification of electrons, which can be understood in the context of an energy landscape arising from the degeneracy of various CO patterns. The dynamics suggest that the same nucleation and growth processes that characterize conventional glass-forming liquids guide the crystallization of electrons. These similarities may provide insight into our understanding of the liquid-glass transition.

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arXiv2017

Dimer-Mott and charge-ordered insulating states in the quasi-one-dimensional organic conductors $δ'_{P}$- and $δ'_{C}$-(BPDT-TTF)$_2$ICl$_2$

We investigated the electronic states of the quasi-one-dimensional organic conductors $δ'_{P}$-(BPDT-TTF)$_2$ICl$_2$ and $δ'_{C}$-(BPDT-TTF)$_2$ICl$_2$, both of which are insulating at room temperature owing to strong electron correlations. Through measurements of electrical resistivity, optical conductivity, and magnetic susceptibility, as well as band-structure calculations, we have revealed that the two materials possess completely different ground states, even though they have the same chemical composition and stacking configuration of the donor molecules. We have found that the $δ_P'$-type salt with an effective half-filled band behaves as a dimer-Mott (DM) insulator and exhibits a nonmagnetic transition at 25 K, whereas the $δ'_C$-type salt with a 3/4-filled band shows a charge ordering (CO) transition just above room temperature and becomes nonmagnetic below 20 K. The optical spectra of the $δ_P'$-type salt are composed of two characteristic bands due to intra- and interdimer charge transfers, supporting the DM insulating behavior arising from the strong on-site Coulomb interaction. By contrast, in the $δ'_C$-type salt, a single band characterizing the formation of CO arising from the off-site Coulomb interactions is observed. Upon lowering the temperature, the shape of the optical spectra in the $δ_C'$-type salt becomes asymmetric and shifts to much lower frequencies, suggesting the emergence of domain-wall excitations with fractional charges expected in a one-dimensional CO chain. The temperature dependence of the magnetic susceptibility of the $δ_P'$-type salt is well described by a 2D spin-1/2 Heisenberg AFM model on an anisotropic square lattice in the dimerized picture, while in the $δ_C'$-type salt, it can be explained by a 2D spin-1/2 Heisenberg AFM model on an anisotropic honeycomb lattice formed in the CO state.

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arXiv2014

Collective excitation of a short-range charge ordering in $θ$-$\mbox{(BEDT-TTF)}_2\mbox{CsZn(SCN)}_4$

We find a characteristic low-energy peak structure located in the range of 100-300 cm$^{-1}$ in the optical conductivity spectra of a quasi-two-dimensional organic compound with a triangular lattice, $θ$-$\mbox{(BEDT-TTF)}_2\mbox{CsZn(SCN)}_4$, in which two different types of short-range charge orderings (COs) coexist. Upon lowering the temperature, the low-energy peak becomes significant and shifts to much lower frequencies only for the polarization of ${E \parallel a}$, in contrast to the other broad electronic bands in the mid-infrared region. On introducing disorder, the low-energy peak is strongly suppressed in comparison with the broad electronic bands. This result indicates that the low-energy peak is attributed to a collective excitation that originates from the short-range CO with a relatively long-period $3\times3$ pattern. The present results shed light on the understanding of the low-energy excitation in the glassy electronic state, where the charge degrees of freedom remain at low temperatures.

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arXiv2013

Phonon-Spectrum Narrowing Induced by Ultrafast Charge Fluctuation in an Organic Dimer Mott Insulator

We have observed the characteristic temperature dependence of the intermolecular phonon spectrum in the organic dimer Mott insulator kappa-(ET)2Cu2(CN)3 exhibiting a dielectric anomaly at 30 K. The anomalous spectral narrowing of the 55 cm-1 phonon peak at 30 K was analyzed in terms of motional narrowing within the framework of a stationary Gaussian process, i. e., the phonon frequency is modulated by the ultrafast charge fluctuation. The spectral narrowing occurs because the time constant of the correlation time tau_c and the amplitude of the frequency modulation delta satisfy the relation tau_c<delta at 30 K. At temperatures below 30 K, the motional narrowing is disturbed by the increasing of tau_c, near the charge-glass or the short-range order at 6 K. On the other hand, for temperatures above 30 K, the motional narrowing is disturbed by the increase of delta with increasing temperature.

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arXiv2013

Relaxor ferroelectricity induced by electron correlations in a molecular dimer Mott insulator

We have investigated the dielectric response in an antiferromagnetic dimer-Mott insulator beta'-(BEDT-TTF)2ICl2 with square lattice, compared to a spin liquid candidate kappa-(BEDT-TTF)2Cu2(CN)3. Temperature dependence of the dielectric constant shows a peak structure obeying Curie-Weiss law with strong frequency dependence. We found an anisotropic ferroelectricity by pyrocurrent measurements, which suggests the charge disproportionation in a dimer. The ferroelectric actual charge freezing temperature is related to the antiferromagnetic interaction, which is expected to the charge-spin coupled degrees of freedom in the system.

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arXiv2013

Collective excitation of electric dipole on molecular dimer in organic dimer-Mott insulator

The terahertz (THz) response in 10-100 cm^-1 was investigated in an organic dimer-Mott (DM) insulator kappa-(ET)_2Cu_2(CN)_3 that exhibits a relaxor-like dielectric anomaly. 30 cm^-1 band in the optical conductivity was attributable to collective excitation of the intra-dimer electric dipoles which are formed by an electron correlation. We succeeded in observing photoinduced enhancement of this 30 cm^-1 band, reflecting the growth of the electric dipole cluster in the DM phase. Such optical responses in kappa-(ET)_2Cu_2(CN)_3 reflect instability near the boundary between the DM-ferroelectric charge ordered phases.

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arXiv2011

Suppression of superconductivity by non-magnetic disorder in organic superconductor $κ$-(BEDT-TTF)$_{2}$Cu(NCS)$_{2}$

The suppression of superconductivity by nonmagnetic disorder is investigated systematically in the organic superconductor $κ$-(BEDT-TTF)$_2$Cu(NCS)$_2$. We introduce a nonmagnetic disorder arising from molecule substitution in part with deuterated BEDT-TTF or BMDT-TTF for BEDT-TTF molecules and molecular defects introduced by X-ray irradiation. A quantitative evaluation of the scattering time $τ_{\rm dHvA}$ is carried out by de Haas-van Alphen (dHvA) effect measurement. A large reduction in $T_{\rm c}$ with a linear dependence on $1/τ_{\rm dHvA}$ is found in the small-disorder region below $1/τ_{\rm dHvA} \simeq$ 1 $\times$ 10$^{12}$ s$^{-1}$ in both the BMDT-TTF molecule-substituted and X-ray-irradiated samples. The observed linear relation between $T_{\rm c}$ and $1/τ_{\rm dHvA}$ is in agreement with the Abrikosov-Gorkov (AG) formula, at least in the small-disorder region. This observation is reasonably consistent with the unconventional superconductivity proposed thus far for the present organic superconductor. A deviation from the AG formula, however, is observed in the large-disorder region above $1/τ_{\rm dHvA} \simeq$ 1 $\times$ 10$^{12}$ s$^{-1}$, which reproduces the previous transport study (J. G. Analytis {\it et al.}: Phys. Rev. Lett. {\bf 96} (2006) 177002). We present some interpretations of this deviation from the viewpoints of superconductivity and the inherent difficulties in the evaluation of scattering time.

cond-mat.supr-con↗

arXiv2010

Electron localization near Mott transition in organic superconductor $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}]$Br

The effect of disorder on the electronic properties near the Mott transition is studied in an organic superconductor $κ$-(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.

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arXiv2008

Optical probe of carrier doping by X-ray irradiation in organic dimer Mott insulator $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}]$Cl

We investigated the infrared optical spectra of an organic dimer Mott insulator $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl, which was irradiated with X-rays. We observed that the irradiation caused a large spectral weight transfer from the mid-infrared region, where interband transitions in the dimer and Mott-Hubbard bands take place, to a Drude part in a low-energy region; this caused the Mott gap to collapse. The increase of the Drude part indicates a carrier doping into the Mott insulator due to irradiation defects. The strong redistribution of the spectral weight demonstrates that the organic Mott insulator is very close to the phase border of the bandwidth-controlled Mott transition.

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arXiv2008

Mott transition and superconductivity in the strongly correlated organic superconductor $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}]$Br

The magnetic field effect on the phase diagram of the organic Mott system $κ$-(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.

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arXiv2007

X-ray Irradiation-induced Carrier Doping Effects in Organic Dimer-Mott Insulators

We report X-ray irradiation-induced carrier doping effects on the electrical conductivity in the organic dimer-Mott insulators $κ$-(ET)$_{2}$$X$ with $X =$ Cu[N(CN)$_{2}$]Cl and Cu$_{2}$(CN)$_{3}$. For $κ$-(ET)$_{2}$Cu[N(CN)$_{2}$]Cl, we have observed a large decrease of the resistivity by 40 % with the irradiation at 300 K and the metal-like temperature dependence down to about 50 K. The irradiation-induced defects expected at the donor molecule sites might cause a local imbalance of the charge transfer in the crystal. Such molecular defects result in the effective doping of carriers into the half-filled dimer-Mott insulators.

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arXiv2005

Phase separation in the vicinity of the surface of $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br by fast cooling

Partial suppression of superconductivity by fast cooling has been observed in the organic superconductor $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br by two means: a marked sample size effect on the magnetic susceptibility and direct imaging of insulating regions by scanning microregion infrared reflectance spectroscopy. Macroscopic insulating regions are found in the vicinity of the crystalline surface after fast cooling, with diameters of 50--100 $μ$m and depths of a few $μ$m. The very large in-plane penetration depth reported to date ($\sim$ 24--100 $μ$m) can be explained by the existence of the insulating regions.

cond-mat.supr-con↗

arXiv2005

Real space imaging of the metal - insulator phase separation in the band width controlled organic Mott system $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br

Systematic investigation of the electronic phase separation on macroscopic scale is reported in the organic Mott system $κ$-(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 $κ$-[($h$-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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arXiv2004

Imaging phase separation near the Mott boundary in the correlated organic superconductors $κ$-(BEDT-TTF)$_{2}$X

Electronic phase separation consisting of the metallic and insulating domains with 50 -- 100 $μ$m in diameter is found in the organic Mott system $κ$-[($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.

cond-mat.str-el↗

arXiv2003

Impurity Effect on the In-plane Penetration Depth of the Organic Superconductors $κ$-(BEDT-TTF)$_2X$ ($X$ = Cu(NCS)$_2$ and Cu[N(CN)$_2$]Br)

We report the in-plane penetration depth $λ_{\parallel}$ of single crystals $κ$-(BEDT-TTF)$_2X$ ($X=$ Cu(NCS)$_2$ and Cu[N(CN)$_2$]Br) by means of the reversible magnetization measurements under the control of cooling-rate. In $X$ = Cu(NCS)$_2$, $λ_{\parallel}(0)$ as an extrapolation toward $T$ = 0 K does not change by the cooling-rate within the experimental accuracy, while $T_{\textrm{c}}$ is slightly reduced. On the other hand, in $X$ = Cu[N(CN)$_2$]Br, $λ_{\parallel}(0)$ indicates a distinct increase by cooling faster. The different behavior of $λ_{\parallel}(0)$ on cooling-rate between the two salts is quantitatively explained in terms of the local-clean approximation (London model), considering that the former salt belongs to the very clean system and the later the moderate clean one. The good agreement with this model demonstrates that disorders of ethylene-group in BEDT-TTF introduced by cooling faster increase the electron(quasiparticle)-scattering, resulting in shorter mean free path.

cond-mat.supr-con↗

arXiv2003

Disorder Effect on the Vortex Pinning by the Cooling Process Control in the Organic Superconductor $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br

We investigate the influence of disorders in terminal ethylene groups of BEDT-TTF molecules (ethylene-disorders) on the vortex pinning of the organic superconductor $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Br. Magnetization measurements are performed under different cooling-processes. The second peak in the magnetization hysteresis curve is observed for all samples studied, and the hysteresis width of the magnetization becomes narrower by cooling faster. In contradiction to the simple pinning effect of disorder, this result shows the suppression of the vortex pinning force by introducing more ethylene-disorders. The ethylene-disorder domain model is proposed for explaining the observed result. In the case of the system containing a moderate number of the ethylene-disorders, the disordered molecules form a domain structure and it works as an effective pinning site. On the contrary, an excess number of the ethylene-disorders may weaken the effect of the domain structure, which results in the less effective pinning force on the vortices.

cond-mat.supr-con↗

arXiv2003

Electronic correlation in the infrared optical properties of the quasi two dimensional $κ$-type BEDT-TTF dimer system

The polarized optical reflectance spectra of the quasi two dimensional organic correlated electron system $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]$Y$, $Y =$ Br and Cl are measured in the infrared region. The former shows the superconductivity at $T_{\rm c} \simeq$ 11.6 K and the latter does the antiferromagnetic insulator transition at $T_{\rm N} \simeq$ 28 K. Both the specific molecular vibration mode $ν_{3}(a_{g})$ of the BEDT-TTF molecule and the optical conductivity hump in the mid-infrared region change correlatively at $T^{*} \simeq$ 38 K of $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br, although no indication of $T^{*}$ but the insulating behaviour below $T_{\rm ins} \simeq$ 50-60 K are found in $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl. The results suggest that the electron-molecular vibration coupling on the $ν_{3}(a_{g})$ mode becomes weak due to the enhancement of the itinerant nature of the carriers on the dimer of the BEDT-TTF molecules below $T^{*}$, while it does strong below $T_{\rm ins}$ because of the localized carriers on the dimer. These changes are in agreement with the reduction and the enhancement of the mid-infrared conductivity hump below $T^{*}$ and $T_{\rm ins}$, respectively, which originates from the transitions between the upper and lower Mott-Hubbard bands. The present observations demonstrate that two different metallic states of $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br are regarded as {\it a correlated good metal} below $T^{*}$ including the superconducting state and {\it a half filling bad metal} above $T^{*}$. In contrast the insulating state of $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl below $T_{\rm ins}$ is the Mott insulator.

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