arXiv subjects

Roberto D'Agosta

Publications and source records attributed to Roberto D'Agosta.

At least 19 recordsLinked to original sources

arXiv2026

Fano Resonances in Mismatched C$_3$N Nanoribbon Junctions

Mismatched junctions formed by two C$_3$N zigzag nanoribbons of different widths provide a useful setting for studying quantum interference effects involving edge state transport. A crucial ingredient for this interference to appear is, besides the presence of edge states, the formation of localized interface states at the mismatched interface of the junction. At the level of a tight-binding model it is shown that, by means of an external gate potential, one of the edge state energy bands can selectively be shifted into the energy range of the localized interface states. The resulting coupling between the edge and localized interface states gives rise to pronounced Fano resonances in both the density of states and the transmission spectrum with line shapes well described by the canonical Fano formula. Furthermore, it is found that the geometrical mismatch of the junction not only determines the number of resonances but also the energetic orientation of their asymmetric line shapes. These results identify mismatched C$_3$N nanojunctions as a tunable and robust platform for engineering interference-driven transport.

cond-mat.mes-hall↗

arXiv2023

Thermoelectric efficiency in multiterminal quantum thermal machines from steady-state density functional theory

The multi-terminal generalization of the steady-state density functional theory for the description of electronic and thermal transport (iq-DFT) is presented. The linear response regime of the framework is developed leading to exact expressions for the many-body transport coefficients and thermoelectric efficiency purely in terms of quantities accessible to the framework. The theory is applied to a multi-terminal interacting quantum dot in the Coulomb blockade regime for which accurate parametrizations of the exchange-correlation kernel matrix are given. The thermoelectric efficiency and output power of the multi-terminal system are studied. Surprisingly, the strong-interaction limit of these quantities can be understood in terms of the non-interacting one.

cond-mat.mes-hall↗

arXiv2022

Strongly anisotropic strain-tunability of excitons in exfoliated ZrSe$_3$

We study the effect of uniaxial strain on the band structure of ZrSe$_3$, a semiconducting material with a marked in-plane structural anisotropy. By using a modified 3-point bending test apparatus, thin ZrSe$_3$ flakes were subjected to uniaxial strain along different crystalline orientations monitoring the effect of strain on their optical properties through micro-reflectance spectroscopy. The obtained spectra showed excitonic features that blueshift upon uniaxial tension. This shift is strongly dependent on the direction along which the strain is being applied. When the flakes are strained along the b-axis, the exciton peak shifts at ~ 60-95 meV/%, while along the a-axis, the shift only reaches ~ 0-15 meV/%. Ab initio calculations were conducted to study the influence of uniaxial strain, applied along different crystal directions, on the band structure and reflectance spectra of ZrSe$_3$, exhibiting a remarkable agreement with the experimental results.

cond-mat.mtrl-sci↗

arXiv2021

Thermoelectric transport within density functional theory

A new formalism to describe steady-state electronic and thermal transport in the framework of density functional theory is presented. A one-to-one correspondence is proven between the three basic variables of the theory, i.e., the density on as well as the electrical and heat currents through the junction, and the three basic potentials, i.e., the local potential in as well as the DC bias and thermal gradient across the junction. Consequently, the Kohn-Sham system of the theory requires three exchange-correlations potentials. In linear response, the new formalism leads to exact expressions for the many-body transport coefficients (both electrical and thermal conductances and Seebeck coefficient) in terms of both the corresponding Kohn-Sham coefficients and derivatives of the exchange-correlations potentials. The theory is applied to the Single Impurity Anderson Model, and an accurate analytic parametrization for these derivatives in the Coulomb blockade regime is constructed through reverse engineering.

cond-mat.mes-hall↗

arXiv2021

In-plane anisotropic optical and mechanical properties of two-dimensional MoO$_3$

Molybdenum trioxide (MoO$_3$) in-plane anisotropy has increasingly attracted the attention of the scientific community in the last few years. Many of the observed in-plane anisotropic properties stem from the anisotropic refractive index and elastic constants of the material but a comprehensive analysis of these fundamental properties is still lacking. Here we employ Raman and micro-reflectance measurements, using polarized light, to determine the angular dependence of the refractive index of thin MoO$_3$ flakes and we study the directional dependence of the MoO$_3$ Young's modulus using the buckling metrology method. We found that MoO$_3$ displays one of the largest in-plane anisotropic mechanical properties reported for 2D materials so far.

cond-mat.mtrl-sci↗

arXiv2020

Large birefringence and linear dichroism in TiS3 nanosheets

TiS3 nanosheets have proven to be promising candidates for ultrathin optoelectronic devices due to their direct narrow band-gap and the strong light-matter interaction. In addition, the marked in-plane anisotropy of TiS3 is appealing for the fabrication of polarization sensitive optoelectronic devices. Herein, we study the optical contrast of TiS3 nanosheets of variable thickness on SiO2/Si substrates, from which we obtain the complex refractive index in the visible spectrum. We find that TiS3 exhibits very large birefringence, larger than that of well-known strong birefringent materials like TiO2 or calcite, and linear dichroism. These findings are in qualitative agreement with ab initio calculations that suggest an excitonic origin for the birefringence and linear dichroism of the material.

cond-mat.mtrl-sci↗

arXiv2020

Tunable Photodetectors via in situ Thermal Conversion of TiS$_3$ to TiO$_2$

In two-dimensional materials research, oxidation is usually considered as a common source for the degradation of electronic and optoelectronic devices or even device failure. However, in some cases a controlled oxidation can open the possibility to widely tune the band structure of 2D materials. In particular, we demonstrate the controlled oxidation of titanium trisulfide (TiS$_3$), a layered semiconductor that has attracted much attention recently thanks to its quasi-1D electronic and optoelectronic properties and its direct bandgap of 1.1 eV. Heating TiS$_3$ in air above 300 °C gradually converts it into TiO$_2$, a semiconductor with a wide bandgap of 3.2 eV with ap-plications in photo-electrochemistry and catalysis. In this work, we investigate the controlled thermal oxidation of individual TiS$_3$ nanoribbons and its influence on the optoelectronic properties of TiS$_3$-based photodetectors. We observe a step-wise change in the cut-off wavelength from its pristine value ~1000 nm to 450 nm after subjecting the TiS$_3$ devices to subsequent thermal treatment cycles. Ab-initio and many-body calculations confirm an increase in the bandgap of titanium oxysulfide (TiO$_{2-x}$S$_x$) when increasing the amount of oxygen and reducing the amount of sulfur.

physics.app-ph↗

arXiv2019

Steady-state density functional theory for thermoelectric effects

The recently proposed density functional theory for steady-state transport (i-DFT) is extended to include temperature gradients between the leads. Within this framework, a general and exact expression is derived for the linear Seebeck coefficient which can be written as the sum of the Kohn-Sham coefficient and an exchange-correlation contribution. The formalism is applied to the single-impurity Anderson model for which approximate exchange-correlation functionals are suggested for temperatures both above and below the Kondo temperature. A certain structural property of the exchange-correlation potentials in the Coulomb blockade regime allows to recover an earlier result expressing the Seebeck coefficient in terms of quantities of equilibrium density functional theory. The numerical i-DFT results are compared to calculations with the numerical renormalization group over a wide range of temperatures finding a reasonable agreement while i-DFT comes at a much lower computational cost.

cond-mat.str-el↗

arXiv2017

Electronics and optoelectronics of quasi-one dimensional layered transition metal trichalcogenides

The isolation of graphene and transition metal dichalcongenides has opened a veritable world to a great number of layered materials which can be exfoliated, manipulated, and stacked or combined at will. With continued explorations expanding to include other layered materials with unique attributes, it is becoming clear that no one material will fill all the post-silicon era requirements. Here we review the properties and applications of layered, quasi-one dimensional transition metal trichalcogenides (TMTCs) as novel materials for next generation electronics and optoelectronics. The TMTCs present a unique chain-like structure which gives the materials their quasi-one dimensional properties such as high anisotropy ratios in conductivity and linear dichroism. The range of band gaps spanned by this class of materials (0.2 eV- 2 eV) makes them suitable for a wide variety of applications including field-effect transistors, infrared, visible and ultraviolet photodetectors, and unique applications related to their anisotropic properties which opens another degree of freedom in the development of next generation electronics. In this review we survey the historical development of these remarkable materials with an emphasis on the recent activity generated by the isolation and characterization of atomically thin titanium trisulfide (TiS3).

cond-mat.mtrl-sci↗

arXiv2016

Strong quantum confinement effect in the optical properties of ultrathin α-In2Se3

The effect of quantum confinement in the optical absorption spectra of atomically thin α-In2Se3 crystals is studied, observing a huge thickness-dependent shift in the optical band gap of exfoliated α-In2Se3 flakes. The band gap variation reported here is among the largest found in semiconductor crystals and spans a region of the near-UV spectrum uncovered by other 2D semiconductors.

cond-mat.mes-hall↗

arXiv2016

Efficient simulations with electronic open boundaries

We present a reformulation of the Hairy Probe method for introducing electronic open boundaries that is appropriate for steady state calculations involving non-orthogonal atomic basis sets. As a check on the correctness of the method we investigate a perfect atomic wire of Cu atoms, and a perfect non-orthogonal chain of H atoms. For both atom chains we find that the conductance has a value of exactly one quantum unit, and that this is rather insensitive to the strength of coupling of the probes to the system, provided values of the coupling are of the same order as the mean inter-level spacing of the system without probes. For the Cu atom chain we find in addition that away from the regions with probes attached, the potential in the wire is uniform, while within them it follows a predicted exponential variation with position. We then apply the method to an initial investigation of the suitability of graphene as a contact material for molecular electronics. We perform calculations on a carbon nanoribbon to determine the correct coupling strength of the probes to the graphene, and obtain a conductance of about two quantum units corresponding to two bands crossing the Fermi surface. We then compute the current through a benzene molecule attached to two graphene contacts and find only a very weak current because of the disruption of the $π$-conjugation by the covalent bond between the benzene and the graphene. In all cases we find that very strong or weak probe couplings suppress the current.

cond-mat.mes-hall↗

arXiv2016

Titanium trisulfide (TiS3): a 2D semiconductor with quasi-1D optical and electronic properties

We present characterizations of few-layer titanium trisulfide (TiS3) flakes which, due to their reduced in-plane structural symmetry, display strong anisotropy in their electrical and optical properties. Exfoliated few-layer flakes show marked anisotropy of their in-plane mobilities reaching ratios as high as 7.6 at low temperatures. Based on the preferential growth axis of TiS3 nanoribbons, we develop a simple method to identify the in-plane crystalline axes of exfoliated few-layer flakes through angle resolved polarization Raman spectroscopy. Optical transmission measurements show that TiS3 flakes display strong linear dichroism with a magnitude (transmission ratios up to 30) much greater than that observed for other anisotropic two-dimensional (2D) materials. Finally, we calculate the absorption and transmittance spectra of TiS3 in the random-phase-approximation (RPA) and find that the calculations are in good agreement with the observed experimental optical transmittance.

cond-mat.mtrl-sci↗

arXiv2015

Density Functional Theory of the Seebeck coefficient in the Coulomb blockade regime

The Seebeck coefficient plays a fundamental role in identifying the efficiency of a thermoelectric device. Its theoretical evaluation for atomistic models is routinely based on Density Functional Theory calculations combined with the Landauer-Büttiker approach to quantum transport. This combination, however, suffers from serious drawbacks for devices in the Coulomb blockade regime. We show how to cure the theory through a simple correction in terms of the {\em temperature derivative} of the exchange correlation potential. Our results compare well with both rate equations and experimental findings on carbon nanotubes.

cond-mat.mes-hall↗

arXiv2015

Topological effects in magnetic platinum nano-particles

The magnetic properties of platinum nano-particles ranging in size from a few to up 300 atoms are investigated through first-principle calculations. It is found that the total magnetization depends strongly on the local atomic rearrangements, with an enhancement around five-fold axis. This is due to an elongation of the nearest neighbor distance together with a contraction of the 2$^{nd}$ distance, resulting in a net interatomic partial charge transfer from the atoms lying on the sub-surface layer (donor) towards the vertexes (acceptor).

cond-mat.mes-hall↗

arXiv2015

Electronic bandgap and exciton binding energy of layered semiconductor TiS3

We present a study of the electronic and optical bandgap in layered TiS3, an almost unexplored semiconductor that has attracted recent attention because of its large carrier mobility and inplane anisotropic properties, to determine its exciton binding energy. We combine scanning tunneling spectroscopy and photoelectrochemical measurements with random phase approximation and Bethe-Salpeter equation calculations to obtain the electronic and optical bandgaps and thus the exciton binding energy. We find experimental values for the electronic bandgap, optical bandgap and exciton binding energy of 1.2 eV, 1.07 eV and 130 meV, respectively, and 1.15 eV, 1.05 eV and 100 meV for the corresponding theoretical results. The exciton binding energy is orders of magnitude larger than that of common semiconductors and comparable to bulk transition metal dichalcogenides, making TiS3 ribbons a highly interesting material for optoelectronic applications and for studying excitonic phenomena even at room temperature.

cond-mat.mes-hall↗

arXiv2015

Strain induced bang-gap engineering in layered $\text{TiS}_3$

By combining {\it ab initio} calculations and experiments we demonstrate how the band gap of the transition metal tri-chalcogenide TiS$_3$ can be modified by inducing tensile or compressive strain. We show by numerical calculations that the electronic band gap of layered TiS$_3$ can be modified for monolayer, bilayer and bulk material by inducing either hydrostatic pressure or strain. In addition, we find that the monolayer and bilayer exhibits a transition from a direct to indirect gap when the strain is increased in the direction of easy transport. The ability to control the band gap and its nature can have an impact in the use of TiS$_3$ for optical applications. We verify our prediction via optical absorption experiments that present a band gap increase of up to 10\% upon tensile stress application along the easy transport direction.

cond-mat.mtrl-sci↗

arXiv2015

Time-dependent thermal transport theory

Understanding thermal transport in nanoscale systems presents important challenges to both theory and experiment. In particular, the concept of local temperature at the nanoscale appears difficult to justify. Here, we propose a novel theoretical approach where we replace the temperature gradient with controllable external black-body radiations. The theory recovers known physical results, for example the linear relation between the thermal current and the temperatures difference of two black-bodies. Furthermore, our theory is not limited to the linear regime and goes beyond accounting for non linear effects and transient phenomena. In the strong coupling and large temperature gradients, we show that there is a maximum energy current that the system can sustain and we recover the Kramers' turnover. Since the present theory is general and can be adapted to describe both electron and phonon dynamics, it provides a first step towards a unified formalism for investigating thermal and electronic transport.

cond-mat.mes-hall↗

arXiv2015

TiS3 transistors with tailored morphology and electrical properties

Control over the morphology of TiS3 is demonstrated by synthesizing 1D nanoribbons and 2D nanosheets. The nanosheets can be exfoliated down to a single layer. Through extensive characterization of the two morphologies, differences in the electronic properties are found and attributed to a higher density of sulphur vacancies in nanosheets which, according to density functional theory calculations, leads to an n-type doping.

cond-mat.mtrl-sci↗