*Adv Sci (Weinh) ; 5(2): 1700365, 2018 02.*

##### RESUMO

The integrity of phonon transport properties of large graphene (linear and curved) grain boundaries (GBs) is investigated under the influence of structural and dynamical disorder. To do this, density functional tight-binding (DFTB) method is combined with atomistic Green's function technique. The results show that curved GBs have lower thermal conductance than linear GBs. Its magnitude depends on the length of the curvature and out-of-plane structural distortions at the boundary, having stronger influence the latter one. Moreover, it is found that by increasing the defects at the boundary, the transport properties can strongly be reduced in comparison to the effect produced by heating up the boundary region. This is due to the large reduction of the phonon transmission for in-plane and out-of-plane vibrational modes after increasing the structural disorder in the GBs.

*Nano Lett ; 17(4): 2589-2595, 2017 04 12.*

##### RESUMO

The critical points and the corresponding singularities in the density of states of crystals were first classified by Van Hove with respect to their dimensionality and energy-momentum dispersions. Here, different from saddle-point Van Hove singularities, the occurrence of a continuum of critical points, which give rise to strong singularities in two-dimensional elemental hexagonal lattices, is shown using a minimal tight-binding formalism. The model predicts quartic energy-momentum dispersions despite quadratic or linear ones, which is also the origin of the strong singularity. Starting with this model and using first-principles density functional theory calculations, a family of novel two-dimensional materials that actually display such singularities are identified and their extraordinary features are investigated. The strong singularity gives rise to ferromagnetic instability with an inverse-square-root temperature dependence and the quartic dispersion is responsible for a steplike transmission spectrum, which is a characteristic feature of one-dimensional systems. Because of the abrupt change in transmission at the band edge, these materials have temperature-independent thermopower and enhanced thermoelectric efficiencies. Nitrogene has exceptionally high thermoelectric efficiencies at temperatures down to 50 K, which could make low-temperature thermoelectric applications possible.

*Nanotechnology ; 27(35): 355705, 2016 Sep 02.*

##### RESUMO

Electronic, phononic, and thermoelectric transport properties of single layer black- and blue-phosphorene structures are investigated with first-principles based ballistic electron and phonon transport calculations employing hybrid functionals. The maximum values of room temperature thermoelectric figure of merit, ZT corresponding to armchair and zigzag directions of black-phosphorene, â¼0.5 and â¼0.25, are calculated as rather smaller than those obtained with first-principles based semiclassical Boltzmann transport theory calculations. On the other hand, the maximum value of room temperature ZT of blue-phosphorene is predicted to be substantially high and remarkable values as high as 2.5 are obtained for elevated temperatures. Besides the fact that these figures are obtained at the ballistic limit, our findings mark the strong possibility of high thermoelectric performance of blue-phosphorene in new generation thermoelectric applications.

*Phys Chem Chem Phys ; 15(33): 13951-8, 2013 Sep 07.*

##### RESUMO

Quantum interference (QI) effects in molecular devices have drawn increasing attention over the past years due to their unique features observed in the conductance spectrum. For the further development of single molecular devices exploiting QI effects, it is of great theoretical and practical interest to develop simple methods controlling the emergence and the positions of QI effects like anti-resonances or Fano line shapes in conductance spectra. In this work, starting from a well-known generic molecular junction with a side group (T-shaped molecule), we propose a simple graphical method to visualize the conditions for the appearance of quantum interference, Fano resonances or anti-resonances, in the conductance spectrum. By introducing a simple graphical representation (parabolic diagram), we can easily visualize the relation between the electronic parameters and the positions of normal resonant peaks and anti-resonant peaks induced by quantum interference in the conductance spectrum. This parabolic model not only can predict the emergence and energetic position of quantum interference from a few electronic parameters but also can enable one to know the coupling between the side group and the main conduction channel from measurements in the case of orthogonal basis. The results obtained within the parabolic model are validated using density-functional based quantum transport calculations in realistic T-shaped molecular junctions.

##### Assuntos

Modelos Moleculares , Teoria Quântica , Elétrons*Sci Rep ; 3: 1632, 2013.*

##### RESUMO

Topology is familiar mostly from mathematics, but also natural sciences have found its concepts useful. Those concepts have been used to explain several natural phenomena in biology and physics, and they are particularly relevant for the electronic structure description of topological insulators and graphene systems. Here, we introduce topologically distinct graphene forms - graphene spirals - and employ density-functional theory to investigate their geometric and electronic properties. We found that the spiral topology gives rise to an intrinsic Rashba spin-orbit splitting. Through a Hamiltonian constrained by space curvature, graphene spirals have topologically protected states due to time-reversal symmetry. In addition, we argue that the synthesis of such graphene spirals is feasible and can be achieved through advanced bottom-up experimental routes that we indicate in this work.

*Sci Rep ; 3: 1228, 2013.*

##### RESUMO

We propose a hybrid nano-structuring scheme for tailoring thermal and thermoelectric transport properties of graphene nanoribbons. Geometrical structuring and isotope cluster engineering are the elements that constitute the proposed scheme. Using first-principles based force constants and Hamiltonians, we show that the thermal conductance of graphene nanoribbons can be reduced by 98.8% at room temperature and the thermoelectric figure of merit, ZT, can be as high as 3.25 at T = 800â K. The proposed scheme relies on a recently developed bottom-up fabrication method, which is proven to be feasible for synthesizing graphene nanoribbons with an atomic precision.

##### Assuntos

Grafite/química , Nanotubos de Carbono/química , Radioisótopos de Carbono/química , Temperatura , Condutividade Térmica*Adv Mater ; 23(39): 4471-90, 2011 Oct 18.*

##### RESUMO

Graphene has a multitude of striking properties that make it an exceedingly attractive material for various applications, many of which will emerge over the next decade. However, one of the most promising applications lie in exploiting its peculiar electronic properties which are governed by its electrons obeying a linear dispersion relation. This leads to the observation of half integer quantum hall effect and the absence of localization. The latter is attractive for graphene-based field effect transistors. However, if graphene is to be the material for future electronics, then significant hurdles need to be surmounted, namely, it needs to be mass produced in an economically viable manner and be of high crystalline quality with no or virtually no defects or grains boundaries. Moreover, it will need to be processable with atomic precision. Hence, the future of graphene as a material for electronic based devices will depend heavily on our ability to piece graphene together as a single crystal and define its edges with atomic precision. In this progress report, the properties of graphene that make it so attractive as a material for electronics is introduced to the reader. The focus then centers on current synthesis strategies for graphene and their weaknesses in terms of electronics applications are highlighted.

##### Assuntos

Eletrônica , Grafite/química , Metais/química , Nanotecnologia , Nanotubos de Carbono/química , Silício/química*Nano Lett ; 11(11): 4971-7, 2011 Nov 09.*

##### RESUMO

Outstanding thermal transport properties of carbon nanotubes (CNTs) qualify them as possible candidates to be used as thermal management units in electronic devices. However, significant variations in the thermal conductivity (κ) measurements of individual CNTs restrict their utilizations for this purpose. In order to address the possible sources of this large deviation and to propose a route to solve this discrepancy, we systematically investigate the effects of varying concentrations of randomly distributed multiple defects (single and double vacancies, Stone-Wales defects) on the phonon transport properties of armchair and zigzag CNTs with lengths ranging between a few hundred nanometers to several micrometers, using both nonequilibrium molecular dynamics and atomistic Green's function methods. Our results show that, for both armchair and zigzag CNTs, κ converges nearly to the same values with different types of defects, at all lengths considered in this study. On the basis of the detailed mean free path analysis, this behavior is explained with the fact that intermediate and high frequency phonons are filtered out by defect scattering, while low frequency phonons are transmitted quasi-ballistically even for several micrometer long CNTs. Furthermore, an analysis of variances in κ for different defect concentrations indicates that defect scattering at low defect concentrations could be the source of large experimental variances, and by taking advantage of the possibility to create a controlled concentration of defects by electron or ion irradiation, it is possible to standardize κ with minimizing the variance. Our results imply the possibility of phonon engineering in nanostructured graphene based materials by controlling the defect concentration.

##### Assuntos

Modelos Químicos , Nanotubos de Carbono/química , Nanotubos de Carbono/ultraestrutura , Simulação por Computador , Tamanho da Partícula , Condutividade Térmica , Vibração*ACS Nano ; 5(5): 3779-87, 2011 May 24.*

##### RESUMO

The influence of the structural detail and defects on the thermal and electronic transport properties of graphene nanoribbons (GNRs) is explored by molecular dynamics and non-equilibrium Green's function methods. A variety of randomly oriented and distributed defects, single and double vacancies, Stone-Wales defects, as well as two types of edge form (armchair and zigzag) and different edge roughnesses are studied for model systems similar in sizes to experiments (>100 nm long and >15 nm wide). We observe substantial reduction in thermal conductivity due to all forms of defects, whereas electrical conductance reveals a peculiar defect-type-dependent response. We find that a 0.1% single vacancy concentration and a 0.23% double vacancy or Stone-Wales concentration lead to a drastic reduction in thermal conductivity of GNRs, namely, an 80% reduction from the pristine one of the same width. Edge roughness with an rms value of 7.28 Å leads to a similar reduction in thermal conductivity. Randomly distributed bulk vacancies are also found to strongly suppress the ballistic nature of electrons and reduce the conductance by 2 orders of magnitude. However, we have identified that defects close to the edges and relatively small values of edge roughness preserve the quasi-ballistic nature of electronic transport. This presents a route of independently controlling electrical and thermal transport by judicious engineering of the defect distribution; we discuss the implications of this for thermoelectric performance.