Roberto D'Agosta

Enhanced thermoelectric properties in hybrid graphene/boron nitride nanoribbons

The thermoelectric properties of hybrid graphene/boron nitride nanoribbons (BCNNRs) are investigated using the nonequilibrium Green’s function approach. We find that the thermoelectric figure of merit (ZT ) can be remarkably enhanced by periodically embedding hexagonal BN (h-BN) into graphene nanoribbons (GNRs). Compared to pristine GNRs, the ZT for armchair-edged BCNNRs with width index 3p + 2 is enhanced 10–20 times, while the ZT of nanoribbons with other widths is enhanced by just 1.5–3 times. As for zigzag-edge nanoribbons, the ZT is enhanced 2–3 times. This improvement comes from the combined increase in the Seebeck coefficient and the reduction in the thermal conductance outweighing the decrease in the electrical conductance. In addition, the effect of the component ratio of h-BN on the thermoelectric transport properties is discussed. These results qualify BCNNRs as a promising candidate for building outstanding thermoelectric devices.

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.

Thermoelectric properties of atomically thin silicene and germanene nanostructures

The thermoelectric properties in one- and two-dimensional silicon and germanium structures have been investigated using first-principle density functional techniques and linear response for the thermal and electrical transport. We have considered here the two-dimensional silicene and germanene, together with nano-ribbons of different widths. For the nano-ribbons, we have also investigated the possibility of nano-structuring these systems by mixing silicon and germanium. We found that the figure of merit at room temperature of these systems is remarkably high, up to 2.5.

Thermoelectric properties of atomic-thin silicene and germanene nano-structures

The thermoelectric properties in one- and two-dimensional silicon and germanium structures have been investigated using first-principle density functional techniques and linear response for the thermal and electrical transport. We have considered here the two-dimensional silicene and germanene, together with nano-ribbons of different widths. For the nano-ribbons, we have also investigated the possibility of nano-structuring these systems by mixing silicon and germanium. We found that the figure of merit at room temperature of these systems is remarkably high, up to 2.5.

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 qualitative agreement with the observed experimental optical transmittance.

Electronic Bandgap and Exciton Binding Energy of Layered Semiconductor TiS3

A study of the electronic and optical bandgap is presented 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. Scanning tunneling spectroscopy and photoelectrochemical measurements are combined with random phase approximation and Bethe–Salpeter equation calculations to obtain the electronic and optical bandgaps and thus the exciton binding energy. Experimental values are found 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.

Towards a dynamical approach to the calculation of the figure of merit of thermoelectric nanoscale devices

Research on thermoelectrical energy conversion, the reuse of waste heat produced by some mechanical or chemical processes to generate electricity, has recently gained some momentum. The calculation of the electronic parameters entering the figure of merit of this energy conversion, and therefore the discovery of efficient materials, is usually performed starting from Landauers approach to quantum transport coupled with Onsagers linear response theory. As it is well known, this approach suffers from certain serious drawbacks. Here, we discuss alternative dynamical methods that can go beyond the validity of Landauers/Onsagers approach for electronic transport. They can be used to validate the predictions of Landauers/Onsagers approach and to investigate systems for which this approach has been shown to be unsatisfactory.

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 theoretical approach where we replace the temperature gradient with controllable external blackbody radiations. The theory recovers known physical results, for example, the linear relation between the thermal current and the temperature difference of two blackbodies. Furthermore, our theory is not limited to the linear regime and goes beyond accounting for nonlinear effects and transient phenomena. Since the present theory is general and can be adapted to describe both electron and phonon dynamics, it provides a first step toward a unified formalism for investigating thermal and electronic transport.

Application of a time-convolutionless stochastic Schrödinger equation to energy transport and thermal relaxation

Quantum stochastic methods based on effective wave functions form a framework for investigating the generally non-Markovian dynamics of a quantum-mechanical system coupled to a bath. They promise to be computationally superior to the master-equation approach, which is numerically expensive for large dimensions of the Hilbert space. Here, we numerically investigate the suitability of a known stochastic Schrödinger equation that is local in time to give a description of thermal relaxation and energy transport. This stochastic Schrödinger equation can be solved with a moderate numerical cost, indeed comparable to that of a Markovian system, and reproduces the dynamics of a system evolving according to a general non-Markovian master equation. After verifying that it describes thermal relaxation correctly, we apply it for the first time to the energy transport in a spin chain. We also discuss a portable algorithm for the generation of the coloured noise associated with the numerical solution of the non-Markovian dynamics.

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 nonorthogonal atomic basis sets. As a check on the correctness of the method we investigate a perfect atomic wire of Cu atoms and a perfect nonorthogonal 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 interlevel 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