arXiv subjects
Publications and source records attributed to Xavier Cartoixà.
We present first-principles calculations of the thermal conductivity, ${\bm κ}$, of monolayer CrSBr, a van der Waals magnetic 2D material. We find a considerable thermal anisotropy, with a ratio $κ_{xx}/κ_{yy}$ of around 1.8. The anisotropy stems from a combined effect of phonon velocities and lifetimes and can be tuned by controlling the flake size by suppressing long mean path phonons.
We develop in this work a simple qualitative quantum electron transport model, in the strong light-matter coupling regime under dipole approximation, able to capture polaritonic signatures in the time-dependent electrical current. The effect of the quantized electromagnetic field in the displacement current of a resonant tunneling diode inside an optical cavity is analyzed. The original peaks of the bare electron transmission coefficient split into two new peaks due to the resonant electron-photon interaction, leading to coherent Rabi oscillations among the polaritonic states that are developed in the system in the strong coupling regime. This mimics known effects predicted by a Jaynes-Cummings model in closed systems, and shows how a full quantum treatment of electrons and electromagnetic fields may open interesting paths for engineering new THz electron devices. The computational burden involved in the multi-time measurements of THz currents is tackled by invoking a Bohmian description of the light-matter interaction. We also show that the traditional static transmission coefficient used to characterize DC quantum electron devices has to be substituted by a new displacement current coefficient in high-frequency AC scenarios.
We investigate the features arising from hydrodynamic effects in graphene and phosphorene devices with finite heat sources, using ab initio calculations to go beyond Callaway's model and inform a full linearized scattering operator, and solving the phonon Boltzmann transport equation through energy-based deviational Monte Carlo methods. We explain the mechanisms that create those hydrodynamic features, showing that boundary scattering and the relation of sample dimensions to the nonlocal length are the determinant factors, regardless of the relative importance of normal versus resistive scattering. From this point of view, the nonlocal length reflects the ability of scattering to randomize the heat flux, and we show that approximations made on the scattering operator may have, through the value of nonlocal length, qualitative consequences on the signatures of hydrodynamic behavior.
Without access to the full quantum state, modeling quantum transport in mesoscopic systems requires dealing with a limited number of degrees of freedom. In this work, we analyze the possibility of modeling the perturbation induced by the non-simulated degrees of freedom on the simulated ones as a transition between single-particle pure states. First, we show that Bohmian conditional wave functions (BCWF) allow a rigorous discussion of the dynamics of electrons inside open quantum systems in terms of such single-particle pure states, either under Markovian or non-Markovian conditions. Second, we discuss the practical application of the method for modeling light-matter interaction phenomena in a resonant tunneling device (RTD), where a single photon is interacting with a single electron. Third, we emphasize the importance of interpreting such scattering mechanism as a transition between initial and final single-particle BCWF with well-defined energies (rather than with well-defined momenta).
We present BTE-Barna (Boltzmann Transport Equation - Beyond the Rta for NAnosystems), a software package that extends the Monte Carlo (MC) module of the almaBTE solver of the Peierls-Boltzmann transport equation for phonons (PBTE) to work with nanosystems based on 2D materials with complex geometries. To properly capture how the phonon occupations evolve in momentum space as a result of scattering, we have supplemented the relaxation-time approximation with an implementation of the propagator for the full linearized version of the PBTE. The code can now find solutions for finite and extended devices under the effect of a thermal gradient, with isothermal reservoirs or with an arbitrary initial temperature distribution in space and time, writing out the temperature and heat flux distributions as well as their spectral decompositions. Besides the full deviational MC solver, a number of useful approximations for highly symmetric devices are also included.
Crystal phase engineering gives access to new types of superlattices where, rather than different materials, different crystal phases of the same material are juxtaposed. Here, by means of atomistic nonequilibrium molecular dynamics calculations, we study to what extent these periodic systems can be used to alter phonon transport, similarly to what has been predicted and observed in conventional superlattices based on heterointerfaces. We focus on twin superlattices in GaAs and InAs and highlight the existence of two different transport regimes: in one each interface behaves like an independent scatterer; in the other, a segment with a sufficiently large number of closely-spaced interfaces, is seen by propagating phonons as a metamaterial with its own thermal properties.
Raman spectroscopy is one of the most extended experimental techniques to investigate thin-layered 2D materials. For a complete understanding and modeling of the Raman spectrum of a novel 2D material, it is often necessary to combine the experimental investigation to density-functional-theory calculations. We provide the experimental proof of the fundamentally different behavior of polar 2D vs 3D systems regarding the effect of the dipole-dipole interactions, which in 2D systems ultimately lead to the absence of optical phonons splitting, otherwise present in 3D materials. We demonstrate that non-analytical corrections (NACs) should not be applied to properly model the Raman spectra of few-layered 2D materials, such as WSe$_{2}$ and h-BN, corroborating recent theoretical predictions [Nano Lett. 2017, 17 (6), 3758-3763]. Our findings are supported by measurements performed on tilted samples that allow increasing the component of photon momenta in the plane of the flake, thus unambiguously setting the direction of an eventual NAC. We also investigate the influence of the parity of the number of layers and of the type of layer-by-layer stacking on the effect of NACs on the Raman spectra.
We have studied the finite bias transport properties of a 2H-1T' MoS$_2$ lateral metal-semiconductor (M-S) junction by non-equilibrium Green's functions calculations, aimed at contacting the 2D channel in a field effect transistor. Our results indicate that (a) despite the fundamentally different electrostatics of line and planar dipoles, the Schottky barrier heights respond similarly to changes in doping and applied bias in 2D and 3D M-S junctions, (b) 2H-1T' MoS$_2$ lateral junctions are free from Fermi level pinning, (c) armchair interfaces have superior contacting properties vs.\ zigzag interfaces, (d) 1T' contacts to $p$ channels will present a reduced contact resistance by a factor of 4-10 with respect to $n$ channels and (e) contacts to intermediately doped $n$ ($p$) channels operate in the field (thermionic) emission regime. We also provide an improved procedure to experimentally determine the emission regime in 2D material junctions.
Among the most common few-layers transition metal dichalcogenides (TMDs), WSe2 is the most challenging material from the lattice dynamics point of view. Indeed, for a long time the main two phonon modes (A1g and E12g) have been wrongly assigned. In the last few years, these two modes have been properly interpreted, and their quasi-degeneracy in the monolayer has been used for its identification. In this work, we show that this approach has a limited validity and we propose an alternative, more general approach, based on multi-phonon bands. Moreover, we show and interpret all the peaks (about 40) appearing in the Raman spectra of monolayers, bilayers, and trilayers of WSe2 by combining experimental wavelength- and polarization-dependent Raman studies with density-functional theory calculations providing the phonon dispersions, the polarization-resolved first-order Raman spectra, and the one- and two-phonon density of states. This complete study not only offers a method to distinguish between monolayers, bilayers, and trilayers with no need of optical images and atomic force microscopy, but it also sheds light on the interpretation of single and multi-phonon bands appearing in the inelastic light scattering experiments of layered WSe2; some of these bands were never observed before, and some were observed and uncertainly assigned. We promote the full understanding of the lattice dynamics of this material that is crucial for the realization of optoelectronics devices and of novel phononic metamaterials, such as TMDs superlattices.
We calculate the lattice thermal conductivity ($κ$) for cubic (zinc-blende) and hexagonal (wurtzite) phases for 8 semiconductors using $\textit{ab initio}$ calculations and solving the Phonon Boltzmann Transport Equation, explaining the different behavior of the ratio $κ_{\rm hex}/κ_{\rm cub}$ between the two phases. We show that this behavior depends on the relative importance of two antagonistic factors: anharmonicity, which we find to be always higher in the cubic phase; and the accessible phase space, which is higher for the less symmetric hexagonal phase. Based on that, we develop a method that predicts the most conducting phase---cubic or hexagonal---where other more heuristic approaches fail. We also present results for nanowires made of the same materials, showing the possibility to tune $κ_{\rm hex}/κ_{\rm cub}$ over a wide range by modifying their diameter, thus making them attractive materials for complex phononic and thermoelectric applications/systems.
We carry out a systematic study of the thermal conductivity of four single-layer transition metal dichalcogenides, MX$_2$ (M = Mo, W; X = S, Se) from first-principles by solving the Boltzmann Transport Equation (BTE). We compare three different theoretical frameworks to solve the BTE beyond the Relaxation Time Approximation (RTA), using the same set of interatomic force constants computed within density functional theory (DFT), finding that the RTA severely underpredicts the thermal conductivity of MS$_2$ materials. Calculations of the different phonon scattering relaxation times of the main collision mechanisms and their corresponding mean free paths (MFP) allow evaluating the expected hydrodynamic behaviour in the heat transport of such monolayers. These calculations indicate that despite of their low thermal conductivity, the present TMDs can exhibit large hydrodynamic effects, being comparable to those of graphene, especially for WSe$_2$ at high temperatures.
We study the ballistic transmission and the contact resistance ($R_c$) of a graphite-graphene contact in a top contact geometry from first principles. We find that the calculated $R_c$'s depend on the amount of graphene-graphite overlap, but quickly saturate for transfer lengths of the order of 20 Å. For contacts overlapping more than this transfer length, the $R_c$ can be lower than the 100 Ω$\cdot$μm mark. On the other hand, edge graphite-graphene contacts are expected to have very low contact resistance.
Channel length scaling in graphene field effect transistors (GFETs) is key in the pursuit of higher performance in radio frequency electronics for both rigid and flexible substrates. Although two-dimensional (2D) materials provide a superior immunity to Short Channel Effects (SCEs) than bulk materials, they could dominate in scaled GFETs. In this work, we have developed a model that calculates electron and hole transport along the graphene channel in a drift-diffusion basis, while considering the 2D electrostatics. Our model obtains the self-consistent solution of the 2D Poisson's equation coupled to the current continuity equation, the latter embedding an appropriate model for drift velocity saturation. We have studied the role played by the electrostatics and the velocity saturation in GFETs with short channel lengths L. Severe scaling results in a high degradation of GFET output conductance. The extrinsic cutoff frequency follows a 1/L^n scaling trend, where the index n fulfills n < 2. The case n = 2 corresponds to long-channel GFETs with low source/drain series resistance, that is, devices where the channel resistance is controlling the drain current. For high series resistance, n decreases down to n= 1, and it degrades to values of n < 1 because of the SCEs, especially at high drain bias. The model predicts high maximum oscillation frequencies above 1 THz for channel lengths below 100 nm, but, in order to obtain these frequencies, it is very important to minimize the gate series resistance. The model shows very good agreement with experimental current voltage curves obtained from short channel GFETs and also reproduces negative differential resistance, which is due to a reduction of diffusion current.