arXiv subjects

J. J. Palacios

Publications and source records attributed to J. J. Palacios.

At least 37 records · Page 2Linked to original sources

arXiv2018

Observation of a well-defined hybridization gap and in-gap states on the SmB6 (001) surface

The rise of topology in condensed matter physics has generated strong interest in identifying novel quantum materials in which topological protection is driven by electronic correlations. Samarium hexaboride is a Kondo insulator for which it has been proposed that a band inversion between $5d$ and $4f$ bands gives rise to topologically protected surface states. However, unambiguous proof of the existence and topological nature of these surface states is still missing, and its low-energy electronic structure is still not fully established. Here we present a study of samarium hexaboride by ultra-low-temperature scanning tunneling microscopy and spectroscopy. We obtain clear atomically resolved topographic images of the sample surface. Our tunneling spectra reveal signatures of a hybridization gap with a size of about $8\ \mathrm{meV}$ and with a reduction of the differential conductance inside the gap by almost half, and surprisingly, several strong resonances below the Fermi level. The spatial variations of the energy of the resonances point towards a microscopic variation of the electronic states by the different surface terminations. High-resolution tunneling spectra acquired at $100\ \mathrm{mK}$ reveal a splitting of the Kondo resonance, possibly due to the crystal electric field.

cond-mat.str-el↗

arXiv2017

High current density electrical breakdown of TiS3 nanoribbon-based field-effect transistors

The high field transport characteristics of nanostructured transistors based on layered materials are not only important from a device physics perspective but also for possible applications in next generation electronics. With the growing promise of layered materials as replacements to conventional silicon technology, we study here the high current density properties of the layered material titanium trisulfide (TiS3). We observe high breakdown current densities up to 1.7 10^6 A/cm^2 in TiS3 nanoribbon-based field-effect transistors which are among the highest found in semiconducting nanomaterials. Investigating the mechanisms responsible for current breakdown, we perform a thermogravimetric analysis of bulk TiS3 and compare the results with density functional theory (DFT) and Kinetic Monte Carlo calculations. We conclude that oxidation of TiS3 and subsequent desorption of sulfur atoms plays an important role in the electrical breakdown of the material in ambient conditions. Our results show that TiS3 is an attractive material for high power applications and lend insight to the thermal and defect activated mechanisms responsible for electrical breakdown in nanostructured devices.

cond-mat.mes-hall↗

arXiv2016

Electronic Transport in Gadolinium Atomic-Size Contacts

We report on the fabrication, transport measurements, and density functional theory (DFT) calculations of atomic size contacts made out of gadolinium (Gd). Gd is known to have local moments mainly associated with $f$ electrons. These coexist with itinerant $s$ and $d$ bands that account for its metallic character. Here we explore whether and how the local moments influence electronic transport properties at the atomic scale. Using both Scanning Tunneling Microscope (STM) and lithographic Mechanically Controllable Break Junction (MCBJ) techniques under cryogenic conditions, we study the conductance of Gd when only few atoms form the junction between bulk electrodes made out of the very same material. Thousands of measurements shows that Gd has an average lowest conductance, attributed to an atom-size contact, below $\frac{2e^2}{h}$. Our DFT calculations for monostrand chains anticipate that the $f$ bands are fully spin polarized and insulating, and that the conduction may be dominated by $s$, $p$, and $d$ bands. DFT quantum transport calculations quantitatively reproduce the experimental results for zero bias and reveal that, while $s-p$ bands are dominant for transport, $d$ orbitals seem to have a relevant contribution in some cases.

cond-mat.mes-hall↗

arXiv2016

Local electroexfoliation of graphene with a STM tip

Graphite surfaces can be manipulated by several methods to create graphene structures of different shapes and sizes. Scanning tunneling microscopy (STM) can be used to create these structures either through mechanical contact between the tip and the surface or through electro-exfoliation. In the latter, the mechanisms involved in the process of exfoliation with an applied voltage are not fully understood. Here we show how a graphite surface can be locally exfoliated in a systematic manner by applying an electrostatic force with a STM tip at the edge of a terrace, forming triangular flakes several nanometers in length. We demonstrate, through experiments and simulations, how these flakes are created by a two-step process: first a voltage ramp must be applied at the edge of the terrace, and then the tip must be scanned perpendicularly to the edge. Ab-initio electrostatic calculations reveal that the presence of charges on the graphite surface weakens the interaction between layers allowing for exfoliation at voltages in the same range as those used experimentally. Molecular dynamics simulations show that a force applied locally on the edge of a step produces triangular flakes such as those observed under STM. Our results provide new insights towards surface modification that can be extended to other layered materials.

cond-mat.mes-hall↗

arXiv2016

Franckeite: a naturally occurring van der Waals heterostructure

The fabrication of van der Waals heterostructures, artificial materials assembled by individually stacking atomically thin (2D) materials, is one of the most promising directions in 2D materials research. Until now, the most widespread approach to stack 2D layers relies on deterministic placement methods which are cumbersome when fabricating multilayered stacks. Moreover, they tend to suffer from poor control over the lattice orientations and the presence of unwanted adsorbates between the stacked layers. Here, we present a different approach to fabricate ultrathin heterostructures by exfoliation of bulk franckeite which is a naturally occurring and air stable van der Waals heterostructure (composed of alternating SnS2-like and PbS-like layers stacked on top of each other). Presenting both an attractive narrow bandgap (<0.7 eV) and p-type doping, we find that the material can be exfoliated both mechanically and chemically down to few-layer thicknesses. We present extensive theoretical and experimental characterizations of the material's electronic properties and crystal structure, and explore applications for near-infrared photodetectors (exploiting its narrow bandgap) and for p-n junctions based on the stacking of MoS2 (n-doped) and franckeite (p-doped)

cond-mat.mes-hall↗

arXiv2016

Effective mass theory for the anisotropic exciton in 2D crystals: Application to phosphorene

We present a theoretical study of the exciton binding energy for anisotropic two-dimensional crystals. We obtain analytical expressions from variational wave functions in different limits of the screening length to exciton size ratio and compare them with numerical solutions, both variational and exact. As an example, we apply these results to phosphorene, a monolayer of black phosphorous. Aided by density functional theory calculations for the evaluation of the two-dimensional polarizability, our analytical solution for the exciton binding energy gives a result which is very close to the numerical ones and, in turn, is comparable to the experimental value, as recently reported.

cond-mat.mes-hall↗

arXiv2015

Resonant transport and electrostatic effects in single-molecule electrical junctions

In this contribution we demonstrate structural control over a transport resonance in HS(CH$_{2}$)$_{n}$[1,4 - C$_{6}$H$_{4}$](CH$_{2}$)$_{n}$SH (n = 1, 3, 4, 6) metal - molecule - metal junctions, fabricated and tested using the scanning tunnelling microscopy-based $I(z)$ method. The Breit-Wigner resonance originates from one of the arene $π$-bonding orbitals, which sharpens and moves closer to the contact Fermi energy as $n$ increases. Varying the number of methylene groups thus leads to a very shallow decay of the conductance with the length of the molecule. We demonstrate that the electrical behaviour observed here can be straightforwardly rationalized by analyzing the effects caused by the electrostatic balance created at the metal-molecule interface. Such resonances offer future prospects in molecular electronics in terms of controlling charge transport over longer distances, and also in single molecule conductance switching if the resonances can be externally gated.

cond-mat.mes-hall↗

arXiv2015

A theoretical study of the dynamics of atomic hydrogen on graphene bilayers

We present a theoretical study of the dynamics of H atoms adsorbed on graphene bilayers with Bernal stacking. First, through extensive density functional theory calculations, including van der Waals interactions, we obtain the activation barriers involved in the desorption and migration processes of a single H atom. These barriers, along with attempt rates and the energetics of H pairs, are used as input parameters in kinetic Monte Carlo simulations to study the time evolution of an initial random distribution of adsorbed H atoms. The simulations reveal that, at room temperature, H atoms occupy only one sublattice before they completely desorb or form clusters. This sublattice selectivity in the distribution of H atoms may last for sufficiently long periods of time upon lowering the temperature down to 0 C. The final fate of the H atoms, namely, desorption or cluster formation, depends on the actual relative values of the activation barriers which can be tuned by doping. In some cases a sublattice selectivity can be obtained for periods of time experimentally relevant even at room temperature. This result shows the possibility for observation and applications of the ferromagnetic state associated with such distribution.

cond-mat.mes-hall↗

arXiv2015

Susbtrate-Induced Stabilization and Reconstruction of Zigzag Edges in Graphene Nanoislands on Ni(111)

We combine experimental observations by scanning tunneling microscopy (STM) and density functional theory (DFT) to reveal the most stable edge structures of graphene on Ni(111) as well as the role of stacking-driven activation and suppression of edge reconstruction. Depending on the position of the outermost carbon atoms relative to hollow and on-top Ni sites, zigzag edges have very different energies. Triangular graphene nanoislands are exclusively bound by the more stable zigzag hollow edges. In hexagonal nanoislands, which are constrained by geometry to alternate zigzag hollow and zigzag top edges along their perimeter, only the hollow edge is stable whereas the top edges spontaneously reconstruct into the (57) pentagon-heptagon structure. Atomically-resolved STM images are consistent with either top-fcc or top-hcp epitaxial stacking of graphene and Ni sites, with the former being favored by DFT. Finally, we find that there is a one-to-one relationship between the edge type, graphene stacking, and orientation of the graphene islands.

cond-mat.mtrl-sci↗

arXiv2015

Modeling contact formation between atomic-sized gold tips via molecular dynamics

The formation and rupture of atomic-sized contacts is modelled by means of molecular dynamics simulations. Such nano-contacts are realized in scanning tunnelling microscope and mechanically controlled break junction experiments. These instruments routinely measure the conductance across the nano-sized electrodes as they are brought into contact and separated, permitting conductance traces to be recorded that are plots of conductance versus the distance between the electrodes. One interesting feature of the conductance traces is that for some metals and geometric configurations a jump in the value of the conductance is observed right before contact between the electrodes, a phenomenon known as jump-to-contact. This paper considers, from a computational point of view, the dynamics of contact between two gold nano-electrodes. Repeated indentation of the two surfaces on each other is performed in two crystallographic orientations of face-centred cubic gold, namely (001) and (111). Ultimately, the intention is to identify the structures at the atomic level at the moment of first contact between the surfaces, since the value of the conductance is related to the minimum cross-section in the contact region. Conductance values obtained in this way are determined using first principles electronic transport calculations, with atomic configurations taken from the molecular dynamics simulations serving as input structures.

cond-mat.mes-hall↗

arXiv2014

Theory of projections with non-orthogonal basis sets: Partitioning techniques and effective Hamiltonians

Here we present a detailed account of the fundamental problems one encounters in projection theory when non-orthogonal basis sets are used for representation of the operators. In particular, we re-examine the use of projection operators in connection with the calculation of projected (or reduced) Green's functions and associated physical quantities such as the local density of states (LDOS), local charge, and conductance. The unavoidable ambiguity in the evaluation of the LDOS and charge is made explicit with the help of simple examples of metallic nanocontacts while the conductance, within certain obvious limits, remains invariant against the type of projection. We also examine the procedure to obtain effective Hamiltonians from reduced Green's functions. For completeness we include a comparison with results obtained with block-orthogonal basis sets where both direct and dual spaces are used.

cond-mat.mes-hall↗

arXiv2014

Isolation and characterization of few-layer black phosphorus

Isolation and characterization of mechanically exfoliated black phosphorus flakes with a thickness down to two single-layers is presented. A modification of the mechanical exfoliation method, which provides higher yield of atomically thin flakes than conventional mechanical exfoliation, has been developed. We present general guidelines to determine the number of layers using optical microscopy, Raman spectroscopy and transmission electron microscopy in a fast and reliable way. Moreover, we demonstrate that the exfoliated flakes are highly crystalline and that they are stable even in free-standing form through Raman spectroscopy and transmission electron microscopy measurements. A strong thickness dependence of the band structure is found by density functional theory calculations. The exciton binding energy, within an effective mass approximation, is also calculated for different number of layers. Our computational results for the optical gap are consistent with preliminary photoluminescence results on thin flakes. Finally, we study the environmental stability of black phosphorus flakes finding that the flakes are very hydrophilic and that long term exposure to air moisture etches black phosphorus away. Nonetheless, we demonstrate that the aging of the flakes is slow enough to allow fabrication of field-effect transistors with strong ambipolar behavior. Density functional theory calculations also give us insight into the water-induced changes of the structural and electronic properties of black phosphorus.

cond-mat.mes-hall↗

arXiv2014

Anomalous exchange interaction between intrinsic spins in conducting graphene systems

We address the nature and possible observable consequences of singular one-electron states that appear when strong defects are introduced in the metallic family of graphene, namely, metallic carbon nanotubes and nanotori. In its simplest form, after creating two defects on the same sublattice, a state may emerge at the Fermi energy presenting very unusual properties: It is unique, normalizable, and features a wave function equally distributed around both defects. As a result, the exchange coupling between the magnetic moments generated by the two defects is anomalous. The intrinsic spins couple ferromagnetically, as expected, but do not present an antiferromagnetic excited state at any distance. We propose the use of metallic carbon nanotubes as a novel electronic device based on this anomalous coupling between spins which can be useful for the robust transmission of magnetic information at large distances.

cond-mat.mes-hall↗

arXiv2014

Hydrogenation-induced ferromagnetism on graphite surfaces

We calculate the electronic structure and magnetic properties of hydrogenated graphite surfaces using van der Waals density functional theory (DFT) and model Hamiltonians. We find, as previously reported, that the interaction between hydrogen atoms on graphene favors adsorption on different sublattices along with an antiferromagnetic coupling of the induced magnetic moments. On the contrary, when hydrogenation takes place on the surface of graphene multilayers or graphite (Bernal stacking), the interaction between hydrogen atoms competes with the different adsorption energies of the two sublattices. This competition may result in all hydrogen atoms adsorbed on the same sublattice and, thereby, in a ferromagnetic state for low concentrations. Based on the exchange couplings obtained from the DFT calculations, we have also evaluated the Curie temperature by mapping this system onto an Ising-like model with randomly located spins. Remarkably, the long-range nature of the magnetic coupling in these systems makes the Curie temperature size dependent and larger than room temperature for typical concentrations and sizes.

cond-mat.mes-hall↗

arXiv2013

Kondo effect and spin quenching in high-spin molecules on metal substrates

Using a state-of-the art combination of density functional theory and impurity solver techniques we present a complete and parameter-free picture of the Kondo effect in the high-spin ($S=3/2$) coordination complex known as Manganese Phthalocyanine adsorbed on the Pb(111) surface. We calculate the correlated electronic structure and corresponding tunnel spectrum and find an asymmetric Kondo resonance, as recently observed in experiments. Contrary to previous claims, the Kondo resonance stems from only one of three possible Kondo channels with origin in the Mn 3d-orbitals, its peculiar asymmetric shape arising from the modulation of the hybridization due to strong coupling to the organic ligand. The spectral signature of the second Kondo channel is strongly suppressed as the screening occurs via the formation of a many-body singlet with the organic part of the molecule. Finally, a spin-1/2 in the 3d-shell remains completely unscreened due to the lack of hybridization of the corresponding orbital with the substrate, hence leading to a spin-3/2 underscreened Kondo effect.

cond-mat.mes-hall↗

arXiv2013

Understanding the structure of the first atomic contact in Gold

We have studied experimentally the phenomena of jump-to-contact (JC) and jump-out-of-contact (JOC) in gold electrodes. JC can be observed at the first contact when the two metals approach each other while JOC occurs in the last contact before breaking. When the indentation depth between the electrodes is limited to a certain value of conductance, a highly reproducible behaviour in the evolution of the conductance can be obtained for hundreds of cycles of formation and rupture. Molecular dynamics simulations of this process show how the two metallic electrodes are shaped into tips of a well-defined crystallographic structure formed through a mechanical annealing mechanism. We report a detailed analysis of the atomic configurations obtained before contact and rupture of these stable structures and obtained their conductance using first-principlesquantum transport calculations. These results help us understand the values of conductance obtained experimentally in the JC and JOC phenomena and improve our understanding of atomic-sized contacts and the evolution of their structural characteristics.

cond-mat.mes-hall↗

arXiv2013

Topologically protected quantum transport in locally exfoliated bismuth at room temperature

We report electrical conductance measurements of Bi nanocontacts created by repeated tip-surface indentation using a scanning tunneling microscope at temperatures of 4 K and 300 K. As a function of the elongation of the nanocontact we measure robust, tens of nanometers long plateaus of conductance G0 = 2e^2/h at room temperature. This observation can be accounted for by the mechanical exfoliation of a Bi(111) bilayer, a predicted QSH insulator, in the retracing process following a tip-surface contact. The formation of the bilayer is further supported by the additional observation of conductance steps below G0 before break-up at both temperatures. Our finding provides the first experimental evidence of the possibility of mechanical exfoliation of Bi bilayers, of the existence of the QSH phase in a two-dimensional crystal, and, most importantly, of the observation of the QSH phase at room temperature.

cond-mat.mes-hall↗

arXiv2012

Manipulation of the magnetic ground state of individual manganese phtalocyanines by coordination to CO molecules

We show that the magnetic state of individual manganese phthalocyanine (MnPc) molecules on a Bi(110) surface is modified when the Mn2+ center coordinates to CO molecules adsorbed on top. Using scanning tunneling spectroscopy we identified this change in magnetic properties from the broadening of a Kondo-related zero-bias anomaly when the CO-MnPc complex is formed. The original magnetic state can be recovered by selective desorption of individual CO molecules. First principle calculations show that the CO molecule reduces the spin of the adsorbed MnPc from S = 1 to S = 1=2 and strongly modifies the respective screening channels, driving a transition from an underscreened Kondo state to a state of mix-valence.

cond-mat.mes-hall↗