arXiv subjects

S. Fratini

Publications and source records attributed to S. Fratini.

At least 19 recordsLinked to original sources

arXiv2023

Transient localization from the interaction with quantum bosons

We carefully revisit the electron-boson scattering problem, going beyond popular semi-classical treatments. By providing numerically exact results valid at finite temperatures, we demonstrate the existence of a regime of electron-boson scattering where quantum localization processes become relevant despite the absence of extrinsic disorder. Localization in the Anderson sense is caused by the emergent randomness resulting from a large thermal boson population, being effective at transient times before diffusion can set in. Compelling evidence of this transient localization phenomenon is provided by the observation of a distinctive displaced Drude peak (DDP) in the optical absorption and the ensuing suppression of conductivity. Our findings identify a general route for anomalous metallic behavior that can broadly apply in interacting quantum matter.

cond-mat.str-el↗

arXiv2022

A quantum theory of the nearly frozen charge glass

We study long-range interacting electrons on the triangular lattice using mixed quantum/classical simulations going beyond the usual classical descriptions of the lattice Coulomb fluid. Our results in the strong interaction limit indicate that the emergence and proliferation of quantum defects governs the low-temperature dynamics of this strongly frustrated system, in a way that crucially depends on the degree of anisotropy of the electronic structure. The present theoretical findings explain the phenomenology observed in the $\theta$-ET$_2$X charge ordering materials as they fall out of equilibrium. The approach devised here can be easily generalized to address other systems where charge frustration is lifted by quantum fluctuations.

cond-mat.str-el↗

arXiv2021

Displaced Drude peak and bad metal from the interaction with slow fluctuations

Scattering by slowly fluctuating degrees of freedom can cause a transient localization of the current-carrying electrons in metals, driving the system away from normal metallic behavior. We illustrate and characterize this general phenomenon by studying how signatures of localization emerge in the optical conductivity of electrons interacting with slow bosonic fluctuations. The buildup of quantum localization corrections manifests itself in the emergence of a displaced Drude peak (DDP), whose existence strongly alters the low frequency optical response and suppresses the d.c. conductivity. We find that for sufficiently strong interactions, many-body renormalization of the fluctuating field induced at metallic densities enhances electron localization and the ensuing DDP phenomenon in comparison with the well-studied low concentration limit. Our results are compatible with the frequent observation of DDPs in electronic systems where slowly fluctuating degrees of freedom couple significantly to the charge carriers.

cond-mat.str-el↗

arXiv2019

On dynamical localization corrections to band transport

Bloch-Boltzmann transport theory fails to describe the carrier diffusion in current crystalline organic semiconductors, where the presence of large-amplitude thermal molecular motions causes substantial dynamical disorder. The charge transport mechanism in this original situation is now understood in terms of a transient localization of the carriers' wavefunctions, whose applicability is however limited to the strong disorder regime. In order to deal with the ever-improving performances of new materials, we develop here a unified theoretical framework that includes transient localization theory as a limiting case, and smoothly connects with the standard band description when molecular disorder is weak. The theory, which specifically adresses the emergence of dynamical localization corrections to semiclassical transport, is used to determine a "transport phase diagram" of high-mobility organic semiconductors.

cond-mat.mtrl-sci↗

arXiv2018

Low-Energy Excitations in Quantum Spin-Liquids Identified by Optical Spectroscopy

The electrodynamic response of organic spin liquids with highly-frustrated triangular lattices has been measured in a wide energy range. While the overall optical spectra of these Mott insulators are governed by transitions between the Hubbard bands, distinct in-gap excitations can be identified at low temperatures and frequencies which we attribute to the quantum spin liquid state. For the strongly correlated $β^{\prime}$-EtMe$_3$\-Sb\-[Pd(dmit)$_2$]$_2$, we discover enhanced conductivity below $175~{\rm cm}^{-1}$, comparable to the energy of the magnetic coupling $J\approx 250$ K. For $ω\rightarrow 0$ these low-frequency excitations vanish faster than the charge-carrier response subject to Mott-Hubbard correlations, resulting in a dome-shape band peaked at 100~\cm. Possible relations to spinons, magnons and disorder are discussed.

cond-mat.str-el↗

arXiv2017

Quantum Spin Liquids Unveil the Genuine Mott State

The Widom line identifies the locus in the phase diagram where a supercritical gas crosses over from gas-like to a more liquid-like behavior. A similar transition exists in correlated electron liquids, where the interplay of Coulomb repulsion, bandwidth and temperature triggers between the Mott insulating state and an incoherent conduction regime. Here we explore the electrodynamic response of three organic quantum spin liquids with different degrees of effective correlation, where the absence of magnetic order enables unique insight into the nature of the genuine Mott state down to the most relevant low-temperature region. Combining optical spectroscopy with pressure-dependent dc transport and theoretical calculations, we succeeded to construct a phase diagram valid for all Mott insulators on a quantitative scale. In the vicinity of the low-temperature phase boundary, we discover metallic fluctuations within the Mott gap, exhibiting enhanced absorption upon cooling that is not present in antiferromagnetic Mott insulators. Our findings reveal the phase coexistence region and Pomeranchuk-like anomaly of the Mott transition, previously predicted but never observed.

cond-mat.str-el↗

arXiv2015

Multiorbital kinetic effects on charge ordering of frustrated electrons on the triangular lattice

The role of the multiorbital effects on the emergence of frustrated electronic orders on the triangular lattice at half filling is investigated through an extended spinless fermion Hubbard model. By using two complementary approaches, unrestricted Hartree-Fock and exact diagonalizations, we unravel a very rich phase diagram controlled by the strength of both local and off-site Coulomb interactions and by the interorbital hopping anisotropy ratio $t'/t$. Three robust unconventional electronic phases, a pinball liquid, an inverse pinball liquid, and a large-unit-cell $\sqrt{12} \times \sqrt{12}$ droplet phase, are found to be generic in the triangular geometry, being controlled by the band structure parameters. The latter are also stabilized in the isotropic limit of our microscopic model, which recovers the standard SU(2) spinful extended single-band Hubbard model.

cond-mat.str-el↗

arXiv2015

The transient localization scenario for charge transport in crystalline organic materials

Charge transport in crystalline organic semiconductors is intrinsically limited by the presence of large thermal molecular motions, which are a direct consequence of the weak van der Waals inter-molecular interactions. These lead to an original regime of transport called \textit{transient localization}, sharing features of both localized and itinerant electron systems. After a brief review of experimental observations that pose a challenge to the theory, we concentrate on a commonly studied model which describes the interaction of the charge carriers with inter-molecular vibrations. We present different theoretical approaches that have been applied to the problem in the past, and then turn to more modern approaches that are able to capture the key microscopic phenomenon at the origin of the puzzling experimental observations, i.e. the quantum localization of the electronic wavefuntion at timescales shorter than the typical molecular motions. We describe in particular a relaxation time approximation which clarifies how the transient localization due to dynamical molecular motions relates to the Anderson localization realized for static disorder, and allows us to devise strategies to improve the mobility of actual compounds. The relevance of the transient localization scenario to other classes of systems is briefly discussed.

cond-mat.mtrl-sci↗

arXiv2013

Anisotropic intrinsic spin relaxation in graphene due to flexural distortions

We propose an intrinsic spin scattering mechanism in graphene originated by the interplay of atomic spin-orbit interaction and the local curvature induced by flexural distortions of the atomic lattice. Starting from a multiorbital tight-binding Hamiltonian with spin-orbit coupling considered non-perturbatively, we derive an effective Hamiltonian for the spin scattering of the Dirac electrons due to flexural distortions. We compute the spin lifetime due to both flexural phonons and ripples and we find values in the microsecond range at room temperature. Interestingly, this mechanism is anisotropic on two counts. First, the relaxation rate is different for off-plane and in-plane spin quantization axis. Second, the spin relaxation rate depends on the angle formed by the crystal momentum with the carbon-carbon bond. In addition, the spin lifetime is also valley dependent. The proposed mechanism sets an upper limit for spin lifetimes in graphene and will be relevant when samples of high quality can be fabricated free of extrinsic sources of spin relaxation.

cond-mat.mes-hall↗

arXiv2012

Electronic transport and quantum localization effects in organic semiconductors

We explore the charge transport mechanism in organic semiconductors based on a model that accounts for the thermal intermolecular disorder at work in pure crystalline compounds, as well as extrinsic sources of disorder that are present in current experimental devices. Starting from the Kubo formula, we develop a theoretical framework that relates the time-dependent quantum dynamics of electrons to the frequency-dependent conductivity. The electron mobility is then calculated through a relaxation time approximation that accounts for quantum localization corrections beyond Boltzmann theory, and allows us to efficiently address the interplay between highly conducting states in the band range and localized states induced by disorder in the band tails. The emergence of a "transient localization" phenomenon is shown to be a general feature of organic semiconductors, that is compatible with the bandlike temperature dependence of the mobility observed in pure compounds. Carrier trapping by extrinsic disorder causes a crossover to a thermally activated behavior at low temperature, which is progressively suppressed upon increasing the carrier concentration, as is commonly observed in organic field-effect transistors. Our results establish a direct connection between the localization of the electronic states and their conductive properties, formalizing phenomenological considerations that are commonly used in the literature.

cond-mat.mtrl-sci↗

arXiv2012

Molecular fingerprints in the electronic properties of crystalline organic semiconductors: from experiment to theory

By comparing photoemission spectroscopy with a non-perturbative dynamical mean field theory extension to many-body ab initio calculations, we show in the prominent case of pentacene crystals that an excellent agreement with experiment for the bandwidth, dispersion and lifetime of the hole carrier bands can be achieved in organic semiconductors provided that one properly accounts for the coupling to molecular vibrational modes and the presence of disorder. Our findings rationalize the growing experimental evidence that even the best band structure theories based on a many-body treatment of electronic interactions cannot reproduce the experimental photoemission data in this important class of materials.

cond-mat.mtrl-sci↗

arXiv2011

Geometrical frustration effects on charge-driven quantum phase transitions

The interplay of Coulomb repulsion and geometrical frustration on charge-driven quantum phase transitions is explored. The ground state phase diagram of an extended Hubbard model on an anisotropic triangular lattice relevant to quarter-filled layered organic materials contains homogeneous metal, 'pinball' and three-fold charge ordered metallic phases. The stability of the 'pinball' phase occurring for strong Coulomb repulsions is found to be strongly influenced by geometrical frustration. A comparison with a spinless model reproduces the transition from the homogeneous metallic phase to a pinball liquid, which indicates that the spin correlations should play a much smaller role than the charge correlations in the metallic phase close to the charge ordering transition. Spin degeneracy is, however, essential to describe the dependence of the system on geometrical frustration. Based on finite temperature Lanczos diagonalization we find that the effective Fermi temperature scale, T*, of the homogeneous metal vanishes at the quantum phase transition to the ordered metallic phase driven by the Coulomb repulsion. Above this temperature scale 'bad' metallic behavior is found which is robust against geometrical frustration in general. Quantum critical phenomena are not found whenever nesting of the Fermi surface is strong, possibly indicating a first order transition instead. 'Reentrant' behavior in the phase diagram is encountered whenever the 2kF-CDW instability competes with the Coulomb driven three-fold charge order transition. The relevance of our results to the family of quarter-filled materials: theta-(BEDT-TTF)2X is discussed.

cond-mat.str-el↗

arXiv2011

Band dispersion and electronic lifetimes in crystalline organic semiconductors

The consequences of several microscopic interactions on the photoemission spectra of crystalline organic semiconductors (OSC) are studied theoretically. It is argued that their relative roles can be disentangled by analyzing both their temperature and their momentum/energy dependence. Our analysis shows that the polaronic thermal band narrowing, that is the foundation of most theories of electrical transport in OSC, is inconsistent in the range of microscopic parameters appropriate for these materials. An alternative scenario is proposed to explain the experimental trends.

cond-mat.mtrl-sci↗

arXiv2011

Transient localization in crystalline organic semiconductors

A relation derived from the Kubo formula shows that optical conductivity measurements below the gap frequency in doped semiconductors can be used to probe directly the time-dependent quantum dynamics of charge carriers. This allows to extract fundamental quantities such as the elastic and inelastic scattering rates, as well as the localization length in disordered systems. When applied to crystalline organic semiconductors, an incipient electron localization caused by large dynamical lattice disorder is unveiled, implying a breakdown of semiclassical transport.

cond-mat.mtrl-sci↗

arXiv2010

The importance of intra-molecular electron spin relaxation in small molecular semiconductors

Electron spin relaxation rate (eSR) is investigated on several organic semiconductors of different morphologies and molecular structures, using avoided level crossing muon spectroscopy as a local spin probe. We find that two functionalized acenes (polycrystalline tri(isopropyl)silyl-pentacene and amorphous 5,6,11,12-tetraphenyltetracene) exhibit eSRs with an Arrhenius-like temperature dependence, each with two characteristic energy scales similar to those expected from vibrations. Polycrystalline tris(8-hydroxyquinolate)gallium shows a similar behavior. The observed eSR for these molecules is no greater than 0.85 MHz at 300 K. The variety of crystal structures and transport regimes that these molecules possess, as well as the local nature of the probe, strongly suggest an intra-molecular phenomenon general to many organic semiconductors, contrasting the commonly assumed spin relaxation models based on inter-molecular charge carrier transport.

cond-mat.mtrl-sci↗

arXiv2010

On the interface polaron formation in organic field-effect transistors

A model describing the low density carrier state in an organic single crystal FET with high-$κ$ gate dielectrics is studied. The interplay between charge carrier coupling with inter-molecular vibrations in the bulk of the organic material and the long-range interaction induced at the interface with a polar dielectric is investigated. This interplay is responsible for the stabilization of a polaronic state with an internal structure extending on few lattice sites, at much lower coupling strengths than expected from the polar interaction alone. This effect could give rise to polaron self-trapping in high-$κ$ organic FET's without invoking unphysically large values of the carrier interface interaction.

cond-mat.mtrl-sci↗

arXiv2009

Band-like motion and mobility saturation in organic molecular semiconductors

We analyze a model that accounts for the inherently large thermal lattice fluctuations associated to the weak van der Waals inter-molecular bonding in crystalline organic semiconductors. In these materials the charge mobility generally exhibits a "metallic-like" power-law behavior, with no sign of thermally activated hopping characteristic of carrier self-localization, despite apparent mean-free-paths comparable or lower than the inter-molecular spacing. Our results show that such puzzling transport regime can be understood from the simultaneous presence of band carriers and incoherent states that are dynamically localized by the thermal lattice disorder.

cond-mat.mtrl-sci↗

arXiv2009

Unconventional metallic conduction in two-dimensional Hubbard-Wigner lattices

The interplay between long-range and local Coulomb repulsion in strongly interacting electron systems is explored through a two-dimensional Hubbard-Wigner model. An unconventional metallic state is found in which collective low-energy excitations characteristic of the Wigner crystal induce a flow of electrical current despite the absence of one-electron spectral weight at the Fermi surface. Photoemission experiments on certain quarter-filled layered molecular crystals should observe a gap in the excitation spectrum whereas optical spectroscopy should find a finite Drude weight indicating metallic behavior.

cond-mat.str-el↗