arXiv subjects

Stefano Sanvito

Publications and source records attributed to Stefano Sanvito.

At least 91 records · Page 5Linked to original sources

arXiv2016

Evidence for pressure-induced node-pair annihilation in Cd3As2

As an intermediate state in the topological phase diagram, Dirac semimetals are of particular interest as a platform for studying topological phase transitions under external modulations. Despite a growing theoretical interest in this topic, it remains a substantial challenge to experimentally tune the system across topological phase transitions. Here, we investigate the Fermi surface evolution of Cd3As2 under high pressure through magnetotransport. A sudden change in Berry phase occurs at 1.3 GPa along with the unanticipated shrinkage of the Fermi surface, which occurs well below the structure transition point (~2.5 GPa). High pressure X-ray diffraction also reveals an anisotropic compression of the Cd3As2 lattice around a similar pressure. Corroborated by the first-principles calculations we show that an axial compression will shift the Dirac nodes towards the Brillouin zone center and eventually introduces a finite energy gap. The ability to tune the node position, a vital parameter of Dirac semimetals, can have dramatic impacts on the corresponding topological properties such as the Fermi arc surface states and the chiral anomaly. Our study demonstrates axial compression as an efficient approach for manipulating the band topology and exploring the critical phenomena near the topological phase transition in Cd3As2.

cond-mat.mtrl-sci↗

arXiv2016

First-principles spin-transfer torque in CuMnAs$|$GaP$|$CuMnAs junctions

We demonstrate that an all-antiferromagnetic tunnel junction with current perpendicular to the plane geometry can be used as an efficient spintronics device with potential high frequency operation. By using state-of-the-art density functional theory combined with quantum transport, we show that the Néel vector of the electrodes can be manipulated by spin-transfer torque. This is staggered over the two different magnetic sublattices and can generate dynamics and switching. At the same time the different magnetization states of the junction can be read by standard tunnelling magnetoresistance. Calculations are performed for CuMnAs$|$GaP$|$CuMnAs junctions with different surface terminations between the anti-ferromagnetic CuMnAs electrodes and the insulating GaP spacer. In particular we find that the torque remains staggered regardless of the termination, while the magnetoresistance depends on the microscopic details of the interface.

cond-mat.mes-hall↗

arXiv2016

Non-equilibrium magnetic fields in ab initio spin dynamics

Starting from the continuity equation for the magnetization in time-dependent spin-density functional theory, we derive an expression for the effective time-dependent magnetic fields driving the out-of-equilibrium spin dynamics in magnetic systems. We evaluate these, so called, kinetic magnetic fields in the ultrafast demagnetization response to optical pulse excitations of ferromagnetic iron-based materials, namely Fe$_6$ cluster and bulk bcc Fe. We identify spatial "hot spots" where the demagnetization is particularly enhanced as a result of the increased kinetic torque.

cond-mat.mes-hall↗

arXiv2016

Observation of quasi-two-dimensional Dirac fermions in ZrTe5

Since the discovery of graphene, layered materials have attracted extensive interests owing to their unique electronic and optical characteristics. Among them, Dirac semimetal, one of the most appealing categories, has been a long-sought objective in layered systems beyond graphene. Recently, layered pentatelluride ZrTe5 was found to host signatures of Dirac semimetal. However, the low Fermi level in ZrTe5 strongly hinders a comprehensive understanding of the whole picture of electronic states through photoemission measurements, especially in the conduction band. Here, we report the observation of Dirac fermions in ZrTe5 through magneto-optics and magneto-transport. By applying magnetic field, we observe a square-root-B dependence of inter-Landau-level resonance and Shubnikov-de Haas (SdH) oscillations with non-trivial Berry phase, both of which are hallmarks of Dirac fermions. The angular-dependent SdH oscillations show a clear quasi-two-dimensional feature with highly anisotropic Fermi surface and band topology, in stark contrast to the 3D Dirac semimetal such as Cd3As2. This is further confirmed by the angle-dependent Berry phase measurements and the observation of bulk quantum Hall plateaus. The unique band dispersion is theoretically understood: the system is at the critical point between a 3D Dirac semimetal and a topological insulator phase. With the confined interlayer dispersion and reducible dimensionality, our work establishes ZrTe5 as an ideal platform for exploring exotic physical phenomena of Dirac fermions.

cond-mat.mtrl-sci↗

arXiv2016

Femtosecond spin current pulses generated by the non-thermal spin-dependent Seebeck effect and interacting with ferromagnets in spin valves

Using the sensitivity of magneto-induced second harmonic generation to spin currents (SC), we demonstrate in Fe/Au/Fe/MgO(001) pseudo spin valves the generation of 250 fs-long SC pulses. Their temporal profile indicates that superdiffusive hot electron transport across a sub-100~nm Au layer is close to the ballistic limit and the pulse duration is primarily determined by the thermalization time of laser-excited hot carriers in Fe. Considering the calculated spin-dependent Fe/Au interface transmittance we conclude that a non-thermal spin-dependent Seebeck effect is responsible for the generation of ultrashort SC pulses. We also show that hot electron spins rotate upon interaction with non-collinear magnetization at the Au/Fe interface, which holds high potential for future spintronic devices.

physics.optics↗

arXiv2015

Raman Characterization of Platinum Diselenide Thin Films

Platinum diselenide (PtSe2) is a newly discovered 2D material which is of great interest for applications in electronics and catalysis. PtSe2 films were synthesized by thermally-assisted selenization of predeposited platinum films and scanning transmission electron microscopy revealed the crystal structure of these films to be 1T. Raman scattering of these films was studied as a function of film thickness, laser wavelength and laser polarization. Eg and A1g Raman active modes were identified using polarization measurements in the Raman setup. These modes were found to display a clear position and intensity dependence with film thickness, for multiple excitation wavelengths, and their peak positions agree with simulated phonon dispersion curves for PtSe2. These results highlight the practicality of using Raman spectroscopy as a prime characterization technique for newly-synthesized 2D materials.

cond-mat.mtrl-sci↗

arXiv2015

Designing a fully-compensated half-metallic ferrimagnet

Recent experimental work on Mn2RuxGa demonstrates its potential as a compensated ferrimagnetic half-metal (CFHM).Here we present a set of high-throughput ab initio density functional theory calculations and detailed experimental characterisation, that enable us to correctly describe the nominal Mn2RuxGa thin films, in particular with regard to site-disorder and defects. We then construct models that accurately capture all the key features of the Mn-Ru-Ga system, including magnetic compensation and the spin gap at the Fermi level. We find that electronic doping is neccessary, which is achieved with a Mn/Ga ratio smaller than two. Our study shows how composition and substrate-induced biaxial strain can be combined to design the first room-temperature CFHM.

cond-mat.mtrl-sci↗

arXiv2015

The role of spin-orbit interaction in the ultrafast demagnetization of small iron clusters

The ultra-fast demagnetization of small iron clusters initiated by an intense optical excitation is studied with time-dependent spin density functional theory (TDSDFT). In particular we investigate the effect of the spin-orbit interaction on the onset of the demagnetization process. It is found that the initial rate of coherent spin loss is proportional to the square of the atomic spin-orbit coupling constant, $λ$. A simplified quantum spin model comprising spin-orbit interaction and a local time-dependent magnetic field is found to be the minimal model able to reproduce our {\it ab initio} results. The model predicts the $λ^2$ dependence of the onset rate of demagnetization when it is solved either numerically or analytically in the linear response limit. Our findings are supported by additional TDSDFT simulations of clusters made of Co and Ni.

cond-mat.mes-hall↗

arXiv2015

Charge transfer energies of benzene physisorbed on a graphene sheet from constrained density functional theory

Constrained density functional theory (CDFT) is used to evaluate the energy level alignment of a benzene molecule as it approaches a graphene sheet. Within CDFT the problem is conveniently mapped onto evaluating total energy differences between different charge-separated states, and it does not consist in determining a quasi-particle spectrum. We demonstrate that the simple local density approximation provides a good description of the level aligmnent along the entire binding curve, with excellent agreement to experiments at an infinite separation and to GW calculations close to the bonding distance. The method also allows us to explore the effects due to the presence of graphene structural defects and of multiple molecules. In general all our results can be reproduced by a classical image charge model taking into account the finite dielectric constant of graphene.

cond-mat.mes-hall↗

arXiv2015

Gate-tunable quantum oscillations in ambipolar Cd3As2 thin films

Electrostatic doping in materials can lead to various exciting electronic properties, such as metal-insulator transition and superconductivity, by altering the Fermi level position or introducing exotic phases. Cd3As2, a three-dimensional (3D) analog of graphene with extraordinary carrier mobility, was predicted to be a 3D Dirac semimetal, a feature confirmed by recent experiments. However, most research so far has been focused on metallic bulk materials that are known to possess ultra-high mobility and giant magnetoresistance but limited carrier transport tunability. Here, we report on the first observation of a gate-induced transition from band conduction to hopping conduction in single-crystalline Cd3As2 thin films via electrostatic doping by solid electrolyte gating. The extreme charge doping enables the unexpected observation of p-type conductivity in a 50 nm-thick Cd3As2 thin film grown by molecular beam epitaxy. More importantly, the gate-tunable Shubnikov-de Haas (SdH) oscillations and the temperature-dependent resistance reveal a unique band structure and bandgap opening when the dimensionality of Cd3As2 is reduced. This is also confirmed by our first-principles calculations. The present results offer new insights towards nanoelectronic and optoelectronic applications of Dirac semimetals in general, and provide new routes in the search for the intriguing quantum spin Hall effect in low-dimension Dirac semimetals, an effect that is theoretically predicted but not yet experimentally realized.

cond-mat.mtrl-sci↗

arXiv2015

Spin-valve Effect in NiFe/MoS2/NiFe Junctions

Two-dimensional (2D) layered transition metal dichalcogenides (TMDs) have been recently proposed as appealing candidate materials for spintronic applications owing to their distinctive atomic crystal structure and exotic physical properties arising from the large bonding anisotropy. Here we introduce the first MoS2-based spin-valves that employ monolayer MoS2 as the nonmagnetic spacer. In contrast with what expected from the semiconducting band-structure of MoS2, the vertically sandwiched-MoS2 layers exhibit metallic behavior. This originates from their strong hybridization with the Ni and Fe atoms of the Permalloy (Py) electrode. The spin-valve effect is observed up to 240 K, with the highest magnetoresistance (MR) up to 0.73% at low temperatures. The experimental work is accompanied by the first principle electron transport calculations, which reveal an MR of ~ 9% for an ideal Py/MoS2/Py junction. Our results clearly identify TMDs as a promising spacer compound in magnetic tunnel junctions and may open a new avenue for the TMDs-based spintronic applications.

cond-mat.mtrl-sci↗

arXiv2015

An in- and ex-situ TEM study into the oxidisation of titanium (IV) sulphide

The degradation of liquid dispersed titanium (IV) sulphide (TiS$_2$) is studied from the point of view of oxidisation. TiS$_2$ is a layered two-dimensional nanomaterial, with potential for energy storage applications. However, flakes in dispersion were observed to degrade. We examined two oxidisation routes: deionised water at room temperature and oxygen gas within the temperature range 150-350°C. Water was seen to slowly oxidise flakes inwards from the edge, forming an amorphous oxide, a result comparable to the state of flakes which degraded within the original dispersion. Oxygen gas was seen to rapidly oxidise entire flakes to a polycrystalline oxide, when heated 275 °C and above. Degradation was studied with scanning transmission electron microscopy (STEM), energy dispersed x-ray spectroscopy (EDX) and electron energy-loss spectroscopy (EELS). Density Functional Theory calculations have shown oxidisation by both water and gas molecules to be thermodynamically favourable.

cond-mat.mtrl-sci↗

arXiv2015

Charge carrier mobility in hybrid halide perovskites

The charge transport properties of hybrid halide perovskites are investigated with a combination of density functional theory including van der Waals interaction and the Boltzmann theory for diffusive transport in the relaxation time approximation. We find the mobility of electrons to be in the range 5-10 cm$^2$V$^{-1}$s$^{-1}$ and that for holes within 1-5 cm$^2$V$^{-1}$s$^{-1}$, where the variations depend on the crystal structure investigated and the level of doping. Such results, in good agreement with recent experiments, set the relaxation time to about 1 ps, which is the time-scale for the molecular rotation at room temperature. For the room temperature tetragonal phase we explore two possible orientations of the organic cations and find that the mobility has a significant asymmetry depending on the direction of the current with respect to the molecular axis. This is due mostly to the way the PbI$_3$ octahedral symmetry is broken. Interestingly we find that substituting I with Cl has minor effects on the mobilities. Our analysis suggests that the carrier mobility is probably not a key factor in determining the high solar-harvesting efficiency of this class of materials.

cond-mat.mtrl-sci↗

arXiv2015

Single atom anisotropic magnetoresistance on a topological insulator surface

We demonstrate single atom anisotropic magnetoresistance on the surface of a topological insulator, arising from the interplay between the helical spin-momentum-locked surface electronic structure and the hybridization of the magnetic adatom states. Our first-principles quantum transport calculations based on density functional theory for Mn on Bi$_2$Se$_3$ elucidate the underlying mechanism. We complement our findings with a two dimensional model valid for both single adatoms and magnetic clusters, which leads to a proposed device setup for experimental realization. Our results provide an explanation for the conflicting scattering experiments on magnetic adatoms on topological insulator surfaces, and reveal the real space spin texture around the magnetic impurity.

cond-mat.mes-hall↗

arXiv2015

Revealing the role of organic cations in hybrid halide perovskites CH3NH3PbI3

The hybrid halide perovskite CH$_{3}$NH$_{3}$PbI$_{3}$ has enabled solar cells to reach an efficiency of about 18\%, demonstrating a pace for improvements with no precedents in the solar energy arena. Despite such explosive progress, the microscopic origin behind the success of such material is still debated, with the role played by the organic cations in the light-harvesting process remaining unclear. Here van-der-Waals-corrected density functional theory calculations reveal that the orientation of the organic molecules plays a fundamental role in determining the material electronic properties. For instance, if CH$_{3}$NH$_{3}$ orients along a (011)-like direction, the PbI$_{6}$ octahedral cage will distort and the band gap will become indirect. Our results suggest that molecular rotations, with the consequent dynamical change of the band structure, might be at the origin of the slow carrier recombination and the superior conversion efficiency of CH$_{3}$NH$_{3}$PbI$_{3}$.

cond-mat.mtrl-sci↗

arXiv2015

Liquid exfoliation of solvent-stabilised black phosphorus: applications beyond electronics

Few layer black phosphorus is a new two-dimensional material which is of great interest for applications, mainly in electronics. However, its lack of stability severely limits our ability to synthesise and process this material. Here we demonstrate that high-quality, few-layer black phosphorus nanosheets can be produced in large quantities by liquid phase exfoliation in the solvent N-cyclohexyl-2-pyrrolidone (CHP). We can control nanosheet dimensions and have developed metrics to estimate both nanosheet size and thickness spectroscopically. When exfoliated in CHP, the nanosheets are remarkably stable unless water is intentionally introduced. Computational studies show the degradation to occur by reaction with water molecules only at the nanosheet edge, leading to the removal of phosphorus atoms and the formation of phosphine and phosphorous acid. We demonstrate that liquid exfoliated black phosphorus nanosheets are potentially useful in a range of applications from optical switches to gas sensors to fillers for composite reinforcement.

cond-mat.mes-hall↗

arXiv2014

Ab-initio transport across Bismuth Selenide surface barriers

We investigate the effect of potential barriers in the form of step edges on the scattering properties of Bi$_2$Se$_3$(111) topological surface states by means of large-scale ab-initio transport simulations. Our results demonstrate the suppression of perfect backscattering, while all other scattering processes, which do not entail a complete spin and momentum reversal, are allowed. Furthermore, we find that the spin of the surface state develops an out of plane component as it traverses the barrier. Our calculations reveal the existence of quasi-bound states in the vicinity of the surface barriers, which appear in the form of an enhanced density of states in the energy window corresponding to the topological state. For double barriers we demonstrate the formation of quantum well states. To complement our first-principles results we construct a two-dimensional low-energy effective model and show that band bending plays a significant role in the scattering process. Our findings are discussed in the context of a number of recent experimental works.

cond-mat.mes-hall↗

arXiv2014

Topological tuning in three-dimensional Dirac semimetals

We study with first-principles methods the interplay between bulk and surface Dirac fermions in three dimensional Dirac semimetals. By combining density functional theory with the coherent potential approximation, we reveal a topological phase transition in Na$_3$Bi$_{1-x}$Sb$_{x}$ and Cd$_3$[As$_{1-x}$P$_x$]$_2$ alloys, where the material goes from a Dirac semimetal to a trivial insulator upon changing Sb or P concentrations. Tuning the composition allows us to engineer the position of the bulk Dirac points in reciprocal space. Interestingly, the phase transition coincides with the reversal of the band ordering between the conduction and valence bands.

cond-mat.mes-hall↗