We present a theory for the recombination of (charged) holons and doublons in one-dimensional organic Mott insulators, which is responsible for the decay of a photoexcited metallic state. Due to the charge-spin separation, the dominant mechanism for recombination at low density of charges involves a multi-phonon emission. We show that a reasonable coupling to phonons is sufficient to explain the fast recombination observed by pump-probe experiments in ET-F$_2$TCNQ, whereby we can also account for the measured pressure dependence of the recombination rate.
We present a calculation of the recombination rate of the excited holon-doublon pairs based on the two-dimensional model relevant for undoped cuprates which shows that fast processes, observed in pump-probe experiments on Mott-Hubbard insulators in picosecond range, can be explained even quantitatively with the multi-magnon emission. The precondition is the existence of the Mott-Hubbard bound exciton of the s-type. We find that its decay is exponentially dependent on the Mott-Hubbard gap and on the magnon energy, with a small prefactor which can be traced back to strong correlations and conseq…
Experiments performed over the last twenty years have revealed striking similarities between several two-dimensional (2D) fermion systems, including diluted two-dimensional electron liquids in semiconductors, 3He monolayers, and layered organic charge-transfer salts. These experimental results, together with recent theoretical advances, provide compelling evidence that strong electronic correlations - Wigner-Mott physics - dominate the universal features of the corresponding metal-insulator transitions (MIT). Here we review the recent theoretical work exploring quantum criticality of Mott and …
We present experimental evidences for a ferro-electric transition in the family of quasi one- dimensional conductors (TMTTF)2X. We interpret this new transition in the frame of the combined Mott-Hubbard state taking into account the double action of the spontaneous charge disproportionation on the TMTTF molecular stacks and of the X anionic potentials.
We investigated the effect of magnetic field on the highly correlated metal near the Mott transition in the quasi-two-dimensional layered organic conductor, $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl, by the resistance measurements under control of temperature, pressure, and magnetic field. It was demonstrated that the marginal metallic phase near the Mott transition is susceptible to the field-induced localization transition of the first order, as was predicted theoretically. The thermodynamic consideration of the present results gives a conceptual pressure-field phase diagram of the Mott transiti…
We study the Mott transition, antiferromagnetism and superconductivity in layered organic conductors using Cellular Dynamical Mean Field Theory for the frustrated Hubbard model. A d-wave superconducting phase appears between an antiferromagnetic insulator and a metal for $t^{\prime}/t=0.3-0.7 $, or between a nonmagnetic Mott insulator (spin liquid) and a metal for $t^{\prime}/t\geq 0.8$, in agreement with experiments on layered organic conductors including $κ$-(ET)$_{2}$Cu$_{2}$(CN)$_{3}$. These phases are separated by a strong first order transition. The phase diagram gives much insight into …
We consider the possibility that the electrons injected into organic field-effect transistors are strongly correlated. A single layer of acenes can be modelled by a Hubbard Hamiltonian similar to that used for the kappa-(BEDT-TTF)(2)X family of organic superconductors. The injected electrons do not necessarily undergo a transition to a Mott insulator state as they would in bulk crystals when the system is half-filled. We calculate the fillings needed for obtaining insulating states in the framework of the slave-boson theory and in the limit of large Hubbard repulsion, U. We also suggest that t…
The experimentally observed, ambipolar field-effect characteristics of Mott insulators are reproduced in the one-dimensional Hubbard model attached to a tight-binding model for source and drain electrodes. The formation of Schottky barriers, originating from the work-function difference, is taken into account by a potential satisfying the Poisson equation with an appropriate boundary condition. Then, these field-effect characteristics are shown to be related by unique current-voltage characteristics of metal-Mott-insulator interfaces.
Magnetic structures of organic Mott insulators X[Pd(dmit)2]2 (X=Me4P, Me4Sb), of which electronic states are located near quantum spin liquid (X=EtMe3Sb), are demonstrated by 13C NMR. Antiferromagnetic spectra and nuclear relaxations show two distinct magnetic moments within each Pd(dmit)2 molecule, which cannot be described by single band dimer-Mott model and requires intramolecular electronic correlation. This unconventional fragmentation of S = 1/2 electron spin with strong quantum fluctuation is presumably caused by nearly degenerated intramolecular multiple orbitals, and shares a notion o…
Unconventional superconductivity typically occurs in materials in which a small change of a parameter such as bandwidth or doping leads to antiferromagnetic or Mott insulating phases. As such competing phases are approached, the properties of the superconductor often become increasingly exotic. For example, in organic superconductors and underdoped high-$T_\mathrm{c}$ cuprate superconductors a fluctuating superconducting state persists to temperatures significantly above $T_\mathrm{c}$. By studying alloys of quasi-two-dimensional organic molecular metals in the $κ$-(BEDT-TTF)$_2$X family, we r…
An organic Mott insulator, $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl, was investigated by resistance measurements under continuously controllable He gas pressure. The first-order Mott transition was demonstrated by observation of clear jump in the resistance variation against pressure. Its critical endpoint at 38 K is featured by vanishing of the resistive jump and critical divergence in pressure derivative of resistance, $|\frac{1}{R}\frac{\partial R}{\partial P}|$, which are consistent with the prediction of the dynamical mean field theory and have phenomenological correspondence with the liquid…
The phase diagram of the organic superconductor $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$Cl has been investigated by ultrasonic velocity measurements under helium gas pressure. Different phase transitions were identified trough several elastic anomalies characterized from isobaric and isothermal sweeps. Our data reveal two crossover lines that end on the critical point terminating the first-order Mott transition line. When the critical point is approached along these lines, we observe a dramatic softening of the velocity which is consistent with a diverging compressibility of the electronic degrees of fr…
Close to the Mott transition, lattice degrees of freedom react to the softening of electron degrees of freedom. This results in a change of lattice spacing, a diverging compressibility and a critical anomaly of the sound velocity. These effects are investigated within a simple model, in the framework of dynamical mean-field theory. The results compare favorably to recent experiments on the layered organic κ-(BEDT-TTF)_2Cu[N(CN)_2]Cl conductor . We predict that effects of a similar magnitude are expected for V2O3, despite the much larger value of the elastic modulus of this material.
High-$T_{\rm C}$ superconductors show anomalous transport properties in their normal states, such as the bad-metal and pseudogap behaviors. To discuss their origins, it is important to speculate whether these behaviors are material-dependent or universal phenomena in the proximity of the Mott transition, by investigating similar but different material systems. An organic Mott transistor is suitable for this purpose owing to the adjacency between the two-dimensional Mott insulating and superconducting states, simple electronic properties, and high doping/bandwidth tunability in the same sample.…
We present the carrier transport properties in the vicinity of a doping-driven Mott transition observed at a field-effect transistor (FET) channel using a single crystal of the typical two-dimensional organic Mott insulator $κ$-(BEDT-TTF)$_2$CuN(CN)$_2$Cl ($κ$-Cl).The FET shows a continuous metal$-$insulator transition (MIT) as electrostatic doping proceeds. The phase transition appears to involve two-step crossovers, one in Hall measurement and the other in conductivity measurement. The crossover in conductivity occurs around the conductance quantum $e^2/h$ , and hence is not associated with …
We use midinfrared pulses with stable carrier-envelope phase offset to drive molecular vibrations in the charge transfer salt ET-F2TCNQ, a prototypical one-dimensional Mott insulator. We find that the Mott gap, which is probed resonantly with 10 fs laser pulses, oscillates with the pump field. This observation reveals that molecular excitations can coherently perturb the electronic on-site interactions (Hubbard U) by changing the local orbital wave function. The gap oscillates at twice the frequency of the vibrational mode, indicating that the molecular distortions couple quadratically to the …
We report the influence of the field effect on the dc resistance and Hall coefficient in the strain-induced Mott insulating state of an organic superconductor $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br. Conductivity obeys the formula for activated transport $σ_{\Box} = σ_{0}\exp(-W/k_{B}T)$, where $σ_{0}$ is a constant and $W$ depends on the gate voltage. The gate voltage dependence of the Hall coefficient shows that, unlike in conventional FETs, the effective mobility of dense hole carriers ($\sim1.6\times 10^{14}$ cm$^{-2}$) is enhanced by a positive gate voltage. This implies that carrier doping…
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 c…
We study the continuous bandwidth-controlled Mott transition in the two-dimensional single-band Hubbard model with a focus on the critical scaling behavior of charge and spin degrees of freedom. Using plaquette cluster dynamical mean-field theory, we find charge and spin criticality consistent with experimental results for organic conductors. In particular, the charge degree of freedom measured via the local density of states at the Fermi level shows a smoother transition than expected for the Ising universality class and in single-site dynamical mean-field theory, revealing the importance of …
We investigate the dynamics of correlated charge carriers in the vicinity of the Mott metal-to-insulator transition in various of the title quasi-two-dimensional organic charge-transfer salts by means of fluctuation (noise) spectroscopy. The observed $1/f$-type fluctuations are quantitatively very well described by a phenomenological model based on the concept of non-exponetial kinetics. The main result is a correlation-induced enhancement of the fluctuations accompanied by a substantial shift of spectral weight to low frequencies close to the Mott critical endpoint. This sudden slowing down o…
Discontinuous changes of the lattice parameters at the Mott metal-insulator transition are detected by high-resolution dilatometry on deuterated crystals of the layered organic conductor $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br. The uniaxial expansivities uncover a striking and unexpected anisotropy, notably a zero-effect along the in-plane c-axis along which the electronic interactions are relatively strong. A huge thermal expansion anomaly is observed near the end-point of the first-order transition line enabling to explore the critical behavior with very high sensitivity. The analysis yields c…
Femtosecond relaxation of photo-excited quasiparticles in the one dimensional Mott insulator ET-F2TCNQ are measured as a function of external pressure, which is used to tune the electronic structure. By fitting the static optical properties and measuring femtosecond decay times at each pressure value, we correlate the relaxation rates with the electronic bandwidth t and on the intersite correlation energy V. The scaling of relaxation times with microscopic parameters is different than for metals and semiconductors. The competition between localization and delocalization of the Mott-Hubbard exc…
Quantum entanglement effects between the electronic spin and charge degrees of freedom are examined in an organic molecular solid, termed a dimer-Mott insulating system, in which molecular dimers are arranged in a crystal as fundamental units. A low energy effective model includes an antisymmetric exchange interaction, as one of the dominant magnetic interactions. This interaction favors a 90 degree spin configuration, and competes with the Heisenberg-type exchange interaction. Stabilities of the magnetic ordered phases are examined by using the spin-wave theory, as well as the Schwinger-boson…
We present key issues of related phenomenons of the Ferroelectricity and the Charge Disproportionation in organic metals. In (TMTTF_2X the dielectric susceptibility demonstrates clear cases of the ferroelectric and anti-ferroelectric phase transitions. Both the susceptibility and the conductivity prove independence and occasional coexistence of "structurless" ferroelectric transitions and usual "anionic" ones. Their sequence gives access to physics of three types of solitons emerging upon cooling via several steps of symmetry breaking. The theory invokes a concept of the Combined Mott-Hubbard …
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 M…
The physics of quantum many-body systems have been studied using bulk correlated materials, and recently, moiré superlattices formed by atomic bilayers have appeared as a novel platform in which the carrier concentration and the band structures are highly tunable. In this brief review, we introduce an intermediate platform between those systems, namely, a band-filling- and bandwidth-tunable electric double-layer transistor based on a real organic Mott insulator $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl. In the proximity of the bandwidth-control Mott transition at half filling, both electron and ho…
We have performed in-plane transport measurements on the two-dimensional organic salt $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl. A variable (gas) pressure technique allows for a detailed study of the changes in conductivity through the insulator-to-metal transition. We identify four different transport regimes as a function of pressure and temperature (corresponding to insulating, semi-conducting, ''bad metal'', and strongly correlated Fermi liquid behaviours). Marked hysteresis is found in the transition region, which displays complex physics that we attribute to strong spatial inhomogeneities. A…
Pressure-temperature phase diagram of the organic Mott insulator $κ$-(ET)$_2$Cu$_2$(CN)$_3$, a model system of the spin liquid on triangular lattice, has been investigated by $^1$H NMR and resistivity measurements. The spin-liquid phase is persistent before the Mott transition to the metal or superconducting phase under pressure. At the Mott transition, the spin fluctuations are rapidly suppressed and the Fermi-liquid features are observed in the temperature dependence of the spin-lattice relaxation rate and resistivity. The characteristic curvature of Mott boundary in the phase diagram highli…
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 ta…
Changing the interactions between particles in an ensemble-by varying the temperature or pressure, for example-can lead to phase transitions whose critical behaviour depends on the collective nature of the many-body system. Despite the diversity of ingredients, which include atoms, molecules, electrons and their spins, the collective behaviour can be grouped into several families (called 'universality classes') represented by canonical spin models1. One kind of transition, the Mott transition2, occurs when the repulsive Coulomb interaction between electrons is increased, causing wave-like elec…
We extend our theory of electron--hole recombination in organic light emitting diodes to investigate the possibility that high energy singlet and triplet excited states with large electron--hole separations are generated in such processes, over and above the lowest singlet and triplet excitons. Our approach involves a time-dependent calculation of the interchain / intermolecular charge--transfer within model Hamiltonians that explicitly include electron-electron interactions between the $π$-electrons. We show that the electron--hole recombination reaction can be viewed as a tunneling process w…
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.
We have fabricated a metallic structure in an organic Mott insulator $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Cl. The periodic metallic domains of approximately 90$\times$90 $μ$m$^2$ obtained by X-ray irradiation through a molybdenum mesh mask are visualized by scanning microregion infrared reflectance spectroscopy technique. No deterioration by irradiation is found in a range of nanometer to micrometer scales. We demonstrate that the present processing method is applicable for the fabrication of molecular electronic devices.
The physics of the Mott metal-insulator transition (MIT) has attracted huge interest in the last decades. However, despite broad efforts, some key theoretical predictions are still lacking experimental confirmation. In particular, it is not clear whether the large coherent Fermi surface survives in immediate proximity to the bandwidth-controlled first-order MIT. A quantitative experimental verification of the predicted behavior of the quasiparticle effective mass, renormalized by many-body interactions, is also missing. Here we address these issues by employing organic $κ$-type salts as exempl…
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 …
The $\EtMeP$ and $\EtMeSb$ nearly triangular organic salts are distinguished from most other Pd[(dmit)$_2$] based salts, as they display valence bond and no long range order, respectively. Under pressure, a superconducting phase is revealed in EtMe$_3$P near the boundary of valence bond order. We use slave-rotor theory with an enlarged unit cell to study competition between uniform and broken translational symmetry states, offering a theoretical framework capturing the superconducting, valence bond order, spin liquid, and metallic phases on an isotropic triangular lattice. Our finite temperatu…
The band structure and magnetic properties of organic charge-transfer salt $λ$-(BEDSe-TTF)$_2$GaCl$_4$ (BEDSe-TTF: bis(ethylenediseleno)tetrathiafulvalene; abbreviated as $λ$-BEDSe) are investigated. The reported crystal structure is confirmed using X-ray diffraction measurements, and the transfer integrals are calculated. The degree of electron correlation $U/W$ ($U$: on-site Coulomb repulsion, $W$: bandwidth) of $λ$-BEDSe is larger than one and comparable to that of the isostructural Mott insulator $λ$-(ET)$_2$GaCl$_4$ (ET: bis(ethylenedithio)tetrathiafulvalene, abbreviated as $λ$-ET), where…
Triangular lattice quasi-two-dimensional Mott insulators based on BEDT-TTF molecule and its analogies present a possibility to produce exotic phases by coupling charge and spin degrees of freedom. In this work we discuss magnetic properties of one of such materials, $κ$-(BEDT-TTF)$_2$Hg(SCN)$_2$Cl, which is found at the border of the phase transition between a Mott insulator into a charge ordered state. Our magnetic susceptibility and cantilever magnetisation measurements demonstrate how the charge degree of freedom defines magnetic properties for few different charge phases observed in this m…
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…
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 suppress…
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-TT…
We theoretically analyse the process of charge recombination in the planar Mott-Hubbard insulators with the aim to explain short picosecond-range lifetime of photoexcited carriers, experimentally studied via pump-probe experiments on the undoped cuprates. The recombination mechanism consists of two essential ingredients: the formation of a metastable s-type bound holon-doublon pair, i.e. the Mott exciton, and the decay of such an excitonic state via the multimagnon emission. In spite of the large gap that requires many bosons to be emitted, latter process is fast due to large exchange scale an…
$^{1}$H NMR and static susceptibility measurements have been performed in an organic Mott insulator with nearly isotropic triangular lattice, $κ$-(BEDT-TTF)$_{2}$Cu$_{2}$(CN)$_{3}$, which is a model system of frustrated quantum spins. The static susceptibility is described by the spin $S$ = 1/2 antiferromagnetic triangular-lattice Heisenberg model with the exchange constant $J$ $\sim$ 250 K. Regardless of the large magnetic interactions, the $^{1}$H NMR spectra show no indication of long-range magnetic ordering down to 32 mK, which is four-orders of magnitude smaller than $J$. These results su…
We present ultra-high-resolution dilatometric studies in magnetic fields on a quasi-two-dimensional organic conductor $κ$-(D8-BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Br, which is located close to the Mott metal-insulator (MI) transition. The obtained thermal expansion coefficient, $α(T)$, reveals two remarkable features: (i) the Mott MI transition temperature $T_{MI}$ = (13.6 $\pm$ 0.6)\,K is insensitive to fields up to 10\,T, the highest applied field; (ii) for fields along the interlayer \emph{b}-axis, a magnetic-field-induced (FI) phase transition at $T_{FI}$ = (9.5 $\pm$ 0.5)\,K is observed above a …
We investigate the continuous variation of electronic states from a Fermi liquid to a quantum spin liquid induced by chemical substitution in the organic dimer-Mott system of $κ$-[(BEDSe-TTF)$_x$(BEDT-TTF)$_{1-x}$]$_2$Cu[N(CN)$_2$]Br. Electrical transport measurements reveal that the mixing of BEDSe-TTF into the BEDT-TTF layers induces a quantum Mott transition around $x$=0.10. Although a charge gap disappears at this point, magnetic susceptibility and heat capacity measurements indicate that fermionic low-energy excitations remain in the insulating salts, suggesting that fermionic spin excita…
Fluctuation spectroscopy is used to investigate the organic bandwidth-controlled Mott system $κ$-(BEDT-TTF)$_2$Cu[N(CN)$_2$]Cl. We find evidence for percolative-type superconductivity in the spatially inhomogeneous coexistence region of antiferromagnetic insulating and superconducting states which develops under pressure at low temperatures. When the superconducting transition is driven by a magnetic field, percolation seems to be dominated by unstable superconducting clusters upon approaching $T_c (B)$ from above, before a "classical" type of percolation is resumed at low fields, dominated by…
We use a novel Monte Carlo method to study the Mott transition in an anisotropic triangular lattice. The real space approach, retaining extended spatial correlations, allows an accurate treatment of non trivial magnetic fluctuations in this frustrated structure. Choosing the degree of anisotropy to mimic the situation in the quasi-two dimensional organics, $κ-$(BEDT-TTF)$_2$Cu[N(CN)$_2$]-X, we detect a wide pseudogap phase, with anomalous spectral and transport properties, between the `ungapped' metal and the `hard gap' Mott insulator. The magnetic fluctuations also lead to pronounced momentum…
Using Floquet dynamical mean-field theory, we study the high-harmonic generation in the time-periodic steady states of wide-gap Mott insulators under AC driving. In the strong-field regime, the harmonic intensity exhibits multiple plateaus, whose cutoff energies $ε_{\rm cut} = U + mE_0$ scale with the Coulomb interaction $U$ and the maximum field strength $E_0$. In this regime, the created doublons and holons are localized because of the strong field and the $m$-th plateau originates from the recombination of $m$-th nearest-neighbor doublon-holon pairs. In the weak-field regime, there is only …
We report a novel insulator-insulator transition arising from the internal charge degrees of freedom in the two-dimensional quarter-filled organic salt beta-(meso-DMBEDT-TTF)2PF6. The optical conductivity spectra above Tc = 70 K display a prominent feature of the dimer-Mott insulator, characterized by a substantial growth of a dimer peak near 0.6 eV with decreasing temperature. The dimer-peak growth is rapidly quenched as soon as a peak of the charge order shows up below Tc, indicating a competition between the two insulating phases. Our infrared imaging spectroscopy has further revealed a spa…
We investigated the magnetism under a magnetic field in the quasi-two-dimensional organic Mott insulator $κ$-(BEDT-TTF)$_{2}$Cu[N(CN)$_{2}$]Cl through magnetization and $^{13}$C-NMR measurements. We found that in the nominally paramagnetic phase (i.e., above Néel temperature) the field-induced local moments have a staggered component perpendicular to the applied field. As a result, the antiferromagnetic transition well defined at a zero field becomes crossover under a finite field. This unconventional behavior is qualitatively reproduced by the molecular-field calculation for Hamiltonian inclu…
The phase diagram of the layered organic superconductor $κ$-(ET)$_{2}$Cu[N(CN)$_{2}$]Cl has been accurately measured from a combination of $^{1}$H NMR and AC susceptibility techniques under helium gas pressure. The domains of stability of antiferromagnetic and superconducting long-range orders in the pressure {\it vs} temperature plane have been determined. Both phases overlap through a first-order boundary that separates two regions of inhomogeneous phase coexistence. The boundary curve is found to merge with another first order line related to the metal-insulator transition in the paramagnet…
A weird electronic state accompanied with an anomalous superconducting precursor and/or exotic orders, called the pseudogap state, arises prior to a superconducting condensate in underdoped cuprates that are situated near Mott transition. Another way to make the system approach the Mott transition is the variation of bandwidth or correlation strength, which gives a new dimension to exploring this exotic state. Here we report nuclear magnetic resonance (NMR) studies on layered organic superconductors with half-filled bands whose widths are pressure-tuned near the Mott transition. The system sit…
It is widely recognised that the effect of doping into a Mott insulator is complicated and unpredictable, as can be seen by examining the Hall coefficient in high $T_{\rm c}$ cuprates. The doping effect, including the electron-hole doping asymmetry, may be more straightforward in doped organic Mott insulators owing to their simple electronic structures. Here we investigate the doping asymmetry of an organic Mott insulator by carrying out electric-double-layer transistor measurements and using cluster perturbation theory. The calculations predict that strongly anisotropic suppression of the spe…
Mott insulators are commonly pictured with electrons localized on lattice sites. Their low-energy degrees of freedom involve spins only. Here we observe emerging charge degrees of freedom in a molecule-based Mott insulator $κ$-(BEDT-TTF)$_2$Hg(SCN)$_2$Br, resulting in a quantum dipole liquid state. Electrons localized on molecular dimer lattice sites form electric dipoles that do not order at low temperatures and fluctuate with frequency detected experimentally in our Raman spectroscopy experiments. The heat capacity and Raman scattering response are consistent with a scenario where the compos…
We examine recombination processes of photocarriers in one-dimensional Mott insulators coupled to phonons. Performing density matrix renormalization group calculations, we find that, even for small electron-phonon coupling, many phonons are generated dynamically, which cause initial relaxation process after the irradiation. At the same time, spin-charge coupling coming from mixing of high- and low-energy states by the irradiation is suppressed. We discuss differences between Mott and band insulators in terms of relaxation dynamics.
The high harmonic spectrum of the Mott insulating Hubbard model has recently been shown to exhibit plateau structures with cutoff energies determined by $n$th nearest neighbor doublon-holon recombination processes. The spectrum thus allows to extract the on-site repulsion $U$. Here, we consider generalizations of the single-band Hubbard model and discuss the signatures of bosonic excitations in high harmonic spectra. Specifically, we study an electron-plasmon model which captures the essential aspects of the dynamically screened Coulomb interaction in solids and a multi-orbital Hubbard model w…
