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Register a new userMolecular Quantum Materials: Electronic Phases and Charge Dynamics in Two-Dimensional Organic Solids
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This review provides a perspective on recent developments and their implications for our understanding of novel quantum phenomena in the physics of two-dimensional organic solids. We concentrate on the phase transitions and collective response in the charge sector, the importance of coupling of electronic and lattice degrees of freedom and stress an intriguing role of disorder. After a brief introduction to low-dimensional organic solids and their crystallographic structures, we focus on the dimensionality and interactions and emergent quantum phenomena. Important topics of current research in organic matter with sizeable electronic correlations are Mott metal-insulator phase transitions, charge order and ferroelectricity. Highly frustrated two-dimensional systems are established model compounds for studying the quantum spin liquid state and the competition with magnetic long-range order. There are also unique examples of quantum disordered state of magnetic and electric dipoles. Representative experimental results are complemented by current theoretical approaches.
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We observe charge-order fluctuations in the quasi-two-dimensional organic superconductor $beta^{primeprime}$-(BEDT-TTF)2 SF5 CH2 CF2 SO3 both by means of vibrational spectroscopy, locally probing the fluctuating charge order, and investigating the in
-plane dynamical response by infrared reflectance spectroscopy. The decrease of effective electronic interaction in an isostructural metal suppresses both charge-order fluctuations and superconductivity, pointing on their interplay. We compare the results of our experiments with calculations on the extended Hubbard model.
The ferromagnetic Kondo lattice model with an antiferromagnetic interaction between localized spins is a minimal description of the competing kinetic t and magnetic K energy terms which generate the rich physics of manganite systems. Motivated by the discovery in one dimension of homogeneous ``island phases, we consider the possibility of analogous phases in higher dimensions. We characterize the phases present at commensurate fillings, and consider in detail the effects of phase separation in all filling and parameter regimes. We deduce that island and flux phases are stable for intermediate values of K/t at the commensurate fillings n = 1/4, 1/3, 3/8, and 1/2. We discuss the connection of these results to the charge and magnetic ordering observed in a wide variety of manganite compounds.
Symmetry fractionalization describes the fascinating phenomena that excitations in a 2D topological system can transform under symmetry in a fractional way. For example in fractional quantum Hall systems, excitations can carry fractional charges while the electrons making up the system have charge one. An important question is to understand what symmetry fractionalization (SF) patterns are possible given different types of topological order and different symmetries. A lot of progress has been made recently in classifying the SF patterns, providing deep insight into the strongly correlated experimental signatures of systems like spin liquids and topological insulators. We review recent developments on this topic. First, it was shown that the SF patterns need to satisfy some simple consistency conditions. More interesting, it was realized that some seemingly consistent SF patterns are actually `anomalous, i.e. they cannot be realized in strictly 2D systems. We review various methods that have been developed to detect such anomalies. Applying such an understanding to 2D spin liquid allows one to enumerate all potentially realizable SF patterns and propose numerical and experimental probing methods to distinguish them. On the other hand, the anomalous SF patterns were shown to exist on the surface of 3D systems and reflect the nontrivial order in the 3D bulk. We review examples of this kind where the bulk states are topological insulators, topological superconductors, or have other symmetry protected topological orders.
On the basis of an analysis of a 3/4-filled two-dimensional (2D) extended Hubbard model under the fluctuation-exchange approximation, we find Coulomb frustrated phase separation (PS) in a region of nonzero temperature, where the quantum critical phenomenon of charge ordering (CO) dominates. In quasi-2D organic conductors on the verge of CO, this frustrated PS provides a mechanism for generating spatial inhomogeneity, which is characterized by an extremely slow relaxation and an intermediate length scale.
We report comprehensive Raman and infrared investigations of charge-order (CO) fluctuations in the organic metal $beta^{primeprime}$-(BEDT-TTF)$_2$SF$_5$CHFSO$_3$ and superconductor $beta^{primeprime}$-(BEDT-TTF)$_2$SF$_5$CH$_2$CF$_2$SO$_3$. The charge-sensitive vibrational bands have been analyzed through an extension of the well-known Kubo model for the spectral signatures of an equilibrium between two states. At room temperature, both salts exhibit charge fluctuations between two differently charged molecular states with an exchange frequency of about $6times10^{11} {rm s}^{-1}$. The exchange rate of the metallic salt remains roughly constant down to 10 K, while in the superconductor the exchange velocity starts to decrease below 200 K, and a frozen charge-ordered state emerges, and coexists with the charge-order fluctuation state down to the superconducting temperature. These findings are confronted with other existing spectroscopic experiments, and a tentative phase diagram is proposed for the $beta^{primeprime}$ BEDT-TTF quarter-filled salts.
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