arXiv subjects

Andres Arnau

Publications and source records attributed to Andres Arnau.

9 recordsLinked to original sources

arXiv2022

The Role of the Magnetic Anisotropy in Atomic-Spin Sensing of 1D Molecular Chains

One-dimensional metal-organic chains often possess a complex magnetic structure susceptible to be modified by a alteration of their chemical composition. The possibility to tune their magnetic properties provides an interesting playground to explore quasiparticle interactions in low-dimensional systems. Despite the great effort invested so far, a detailed understanding of the interactions governing the electronic and magnetic properties of the low-dimensional systems is still incomplete. One of the reasons is the limited ability to characterize their magnetic properties at the atomic scale. Here, we provide a comprehensive study of the magnetic properties of metal-organic one-dimensional (1D) coordination polymers consisting of 2,5-diamino-1,4-benzoquinonediimine ligands coordinated with Co or Cr atoms synthesized in ultra-high vacuum conditions on a Au(111) surface. A combination of an integral X-ray spectroscopy with local-probe inelastic electron tunneling spectroscopy corroborated by multiplet analysis, density functional theory, and inelastic electron tunneling simulations enable us to obtain essential information about their magnetic structure, including the spin magnitude and orientation at the magnetic atoms, as well as the magnetic anisotropy.

cond-mat.mes-hall↗

arXiv2019

Tunable energy and mass renormalization from homothetic Quantum dot arrays

Quantum dot arrays in the form of molecular nanoporous networks are renown for modifying the electronic surface properties through quantum confinement. Here we show that, compared to the pristine surface state, the fundamental energy of the confined states can exhibit downward shifts accompanied by a lowering of the effective masses simultaneous to the appearance of tiny gaps at the Brillouin zone boundaries. We observed these effects by angle resolved photoemission for two self-assembled homothetic (scalable) Co-coordinated metal-organic networks. Complementary scanning tunneling spectroscopy measurements confirmed these findings. Electron plane wave expansion simulations and density functional theory calculations provide insight into the nature of this phenomenon, which we assign to metal-organic overlayer-substrate interactions in the form of adatom-substrate hybridization. The absence to date of the experimental band structure resulting from single adatom metal-coordinated nanoporous networks has precluded the observation of the significant surface state renormalization reported here, which we infer are general of low interacting and well-defined adatom arrays.

physics.chem-ph↗

arXiv2019

On the validity of the Arrhenius picture in two-dimensional submonolayer growth

For surface-mediated processes, such as on-surface synthesis, epitaxial growth and heterogeneous catalysis, a constant slope in the Arrhenius diagram of the corresponding rate of interest against inverse temperature, $\log R$ {\it vs} $1/k_B T$, is traditionally interpreted as the existence of a bottleneck elementary reaction (or rate-determining step), whereby the constant slope (or apparent activation energy, $E_{app}^{R}$) reflects the value of the energy barrier for that reaction. Here, we show that a constant value of $E_{app}^{R}$ can be obtained even if control shifts from one elementary reaction to another. In fact, we show that $E_{app}^{R}$ is a weighted average and the leading elementary reaction will change with temperature while the actual energy contribution for every elementary reaction will contain, in addition to the traditional energy barrier, a configurational term directly related to the number of local configurations where that reaction can be performed. For this purpose, we consider kinetic Monte Carlo simulations of two-dimensional submonolayer growth at constant deposition flux, where the rate of interest is the tracer diffusivity. In particular, we focus on the study of the morphology, island density and diffusivity by including a large variety of single-atom, multi-atom and complete-island diffusion events for two specific metallic heteroepitaxial systems, namely, Cu on Ni(111) and Ni on Cu(111), as a function of coverage and temperature.

cond-mat.mtrl-sci↗

arXiv2019

Large effect of the metal substrate on the magnetic anisotropy of Co on hexagonal Boron Nitride

We combine x-ray absorption spectroscopy (XAS), x-ray magnetic circular dichroism (XMCD) and x-ray magnetic linear dichroism (XMLD) data with first principles density functional theory (DFT) calculations and a multiorbital many body Hamiltonian approach to understand the electronic and magnetic properties of Co atoms adsorbed on h-BN/Ru(0001) and h-BN/Ir(111). The XAS line shape reveals, for both substrates, an electronic configuration close to $3d^8$, corresponding to a spin $S = 1$. Magnetic field dependent XMCD data show large (14 meV) out-of-plane anisotropy on h-BN/Ru(0001), while it is almost isotropic (tens of $μ$eV) on h-BN/Ir(111). XMLD data together with both DFT calculations and the results of the multiorbital Hubbard model suggest that the dissimilar magnetic anisotropy originates from different Co adsorption sites, namely atop N on h-BN/Ru(0001) and 6-fold hollow on h-BN/Ir(111).

cond-mat.mes-hall↗

arXiv2018

Magnetic properties of metal-organic coordination networks based on 3d transition metal atoms

The magnetic anisotropy and exchange coupling between spins localized at the positions of 3d transition metal atoms forming two-dimensional metal-organic coordination networks (MOCNs) grown on the Au(111) metal surface are studied. In particular, we consider MOCNs made of Ni or Mn metal centers linked by TCNQ (7,7,8,8-tetracyanoquinodimethane) organic ligands, which form rectangular networks with 1:1 stoichiometry. Based on the analysis of X-ray magnetic circular dichroism (XMCD) data taken at T= 2.5 K, we find that Ni atoms in the Ni-TCNQ MOCNs are coupled ferromagnetically and do not show any significant magnetic anisotropy, while Mn atoms in the Mn-TCNQ MOCNs are coupled antiferromagnetically and do show a weak magnetic anisotropy with in-planemagnetization. We explain these observations using both amodelHamiltonian based on mean-fieldWeiss theory and density functional theory calculations that include spin-orbit coupling. Our main conclusion is that the antiferromagnetic coupling between Mn spins and the in-plane magnetization of the Mn spins can be explained neglecting effects due to the presence of the Au(111) surface, while for Ni-TCNQ the metal surface plays a role in determining the absence of magnetic anisotropy in the system.

cond-mat.mes-hall↗

arXiv2014

Modeling Ferro- and Antiferromagnetic Interactions in Metal-Organic Coordination Networks

Magnetization curves of two rectangular metal-organic coordination networks formed by the organic ligand TCNQ (7,7,8,8-tetracyanoquinodimethane) and two different (Mn and Ni) 3d transition metal atoms [M(3d)] show marked differences that are explained using first principles density functional theory and model calculations. We find that the existence of a weakly dispersive hybrid band with M(3d) and TCNQ character crossing the Fermi level is determinant for the appearance of ferromagnetic coupling between metal centers, as it is the case of the metallic system Ni-TCNQ but not of the insulating system Mn-TCNQ. The spin magnetic moment localized at the Ni atoms induces a significant spin polarization in the organic molecule; the corresponding spin density being delocalized along the whole system. The exchange interaction between localized spins at Ni centers and the itinerant spin density is ferromagnetic. Based on two different model Hamiltonians, we estimate the strength of exchange couplings between magnetic atoms for both Ni- and Mn-TCNQ networks that results in weak ferromagnetic and very weak antiferromagnetic correlations for Ni- and Mn-TCNQ networks, respectively.

physics.chem-ph↗

arXiv2011

Simulation of inelastic electron tunneling spectroscopy of single molecules with functionalized tips

The role of the tip in inelastic electron tunneling spectroscopy (IETS) performed with scanning tunneling microscopes (STM) is theoretically addressed via first-principles simulations of vibrational spectra of single carbon monoxide (CO) molecules adsorbed on Cu(111). We show how chemically functionalized STM tips modify the IETS intensity corresponding to adsorbate modes on the sample side. The underlying propensity rules are explained using symmetry considerations for both the vibrational modes and the molecular orbitals of the tip and sample. This suggests that single-molecule IETS can be optimized by selecting the appropriate tip orbital symmetry.

cond-mat.mes-hall↗

arXiv2010

Characterization of single-molecule pentanedithiol junctions by inelastic electron tunneling spectroscopy and first-principles calculations

We study pentanedithiol molecular junctions formed by means of the break-junction technique with a scanning tunneling microscope at low temperatures. Using inelastic electron tunneling spectroscopy and first-principles calculations, the response of the junction to elastic deformation is examined. We show that this procedure makes a detailed characterization of the molecular junction possible. In particular, our results indicate that tunneling takes place through just a single molecule.

cond-mat.mes-hall↗

arXiv2006

Determination of Compton profiles at solid surfaces from first-principles calculations

Projected momentum distributions of electrons, i.e. Compton profiles above the topmost atomic layer have recently become experimentally accessible by kinetic electron emission in grazing-incidence scattering of atoms at atomically flat single crystal metal surfaces. Sub-threshold emission by slow projectiles was shown to be sensitive to high-momentum components of the local Compton profile near the surface. We present a method to extract momentum distribution, Compton profiles, and Wigner and Husimi phase space distributions from ab-initio density-functional calculations of electronic structure. An application for such distributions to scattering experiments is discussed.

cond-mat.other↗