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F. Rivadulla

Publications and source records attributed to F. Rivadulla.

At least 19 recordsLinked to original sources
arXiv2021

Tuning Coherent-Phonon Heat Transport in LaCoO$_3$/SrTiO$_3$ Superlattices

Accessing the regime of coherent phonon propagation in nanostructures opens enormous possibilities to control the thermal conductivity in energy harvesting devices, phononic circuits, etc. In this paper we show that coherent phonons contribute substantially to the thermal conductivity of LaCoO3/SrTiO3 oxide superlattices, up to room temperature. We show that their contribution can be tuned through small variations of the superlattice periodicity, without changing the total superlattice thickness. Using this strategy, we tuned the thermal conductivity by 20% at room temperature. We also discuss the role of interface mixing and epitaxial relaxation as an extrinsic, material dependent key parameter for understanding the thermal conductivity of oxide superlattices.

cond-mat.mtrl-sci↗
arXiv2020

Electronic structure and magnetic exchange interactions of Cr-based van der Waals ferromagnets. A comparative study between CrBr3 and Cr2Ge2Te6

Low dimensional magnetism has been powerfully boosted as a promising candidate for numerous applications. The stability of the long-range magnetic order is directly dependent on the electronic structure and the relative strength of the competing magnetic exchange constants. Here, we report a comparative pressure-dependent theoretical and experimental study of the electronic structure and exchange interactions of two-dimensional ferromagnets CrBr3 and Cr2Ge2Te6 . While CrBr3 is found to be a Mott-Hubbard-like insulator, Cr2Ge2Te6 shows a charge-transfer character due to the broader character of the Te 5p bands at the Fermi level. This different electronic behaviour is responsible of the robust insulating state of CrBr3 , in which the magnetic exchange constants evolve monotonically with pressure, and the proximity to a metal-insulator transition predicted for Cr2Ge2Te6 , which causes a non-monotonic evolution of its magnetic ordering temperature. We provide a microscopic understanding for the pressure evolution of the magnetic properties of the two systems.

cond-mat.mtrl-sci↗
arXiv2019

Spin-Hall magnetoresistance in a low-dimensional magnetic insulator

We observe an unusual behavior of the spin Hall magnetoresistance (SMR) measured in a Pt ultra-thin film deposited on a ferromagnetic insulator, which is a tensile-strained LaCoO3 (LCO) thin film with the Curie temperature Tc=85K. The SMR displays a strong magnetic-field dependence below Tc, with the SMR amplitude continuing to increase (linearly) with increasing the field far beyond the saturation value of the ferromagnet. The SMR amplitude decreases gradually with raising the temperature across Tc and remains measurable even above Tc. Moreover, no hysteresis is observed in the field dependence of the SMR. These results indicate that a novel low-dimensional magnetic system forms on the surface of LCO and that the Pt/LCO interface decouples magnetically from the rest of the LCO thin film. To explain the experiment, we revisit the derivation of the SMR corrections and relate the spin-mixing conductances to the microscopic quantities describing the magnetism at the interface. Our results can be used as a technique to probe quantum magnetism on the surface of a magnetic insulator.

cond-mat.mes-hall↗
arXiv2018

Epitaxial stabilization of pulsed laser deposited Sr$_{n+1}$Ir$_n$O$_{3n+1}$ thin films: entangled effect of growth dynamics and strain

The subtle balance of electronic correlations, crystal field splitting and spin--orbit coupling in layered Ir$^{4+}$ oxides can give rise to novel electronic and magnetic phases. Experimental progress in this field relies on the synthesis of epitaxial films of these oxides. However, the growth of layered iridates with excellent structural quality is a great experimental challenge. Here we selectively grow high quality single--phase films of Sr$_2$IrO$_4$, Sr$_3$Ir$_2$O$_7$, and SrIrO$_3$ on various substrates from a single Sr$_3$Ir$_2$O$_7$ target by tuning background oxygen pressure and epitaxial strain. We demonstrate a complex interplay between growth dynamics and strain during thin film deposition. Such interplay leads to the stabilization of different phases in films grown on different substrates under identical growth conditions, which cannot be explained by a simple kinetic model. We further investigate the thermoelectric properties of the three phases and propose that weak localization is responsible for the low temperature activated resistivity observed in SrIrO$_3$ under compressive strain.

cond-mat.mtrl-sci↗
arXiv2017

Oxygen vacancies in strained SrTiO$_{3}$ thin films: formation enthalpy and manipulation

We report the enthalpy of oxygen vacancy formation in thin films of electron-doped SrTiO$_{3}$, under different degrees of epitaxial stress. We demonstrate that both compressive and tensile strain decrease this energy at a very similar rate, and promote the formation of stable doubly ionized oxygen vacancies. Moreover, we also show that unintentional cationic vacancies introduced under typical growth conditions, produce a characteristic rotation pattern of TiO$_6$ octahedra. The local concentration of oxygen vacancies can be modulated by an electric field with an AFM tip, changing not only the local electrical potential, but also producing a non-volatile mechanical response whose sign (up/down) can be reversed by the electric field.

cond-mat.mtrl-sci↗
arXiv2016

Thermodynamic conditions during growth determine the magnetic anisotropy in epitaxial thin-films of La$_{0.7}$Sr$_{0.3}$MnO$_{3}$

The suitability of a particular material for use in magnetic devices is determined by the process of magnetization reversal/relaxation, which in turn depends on the magnetic anisotropy. Therefore, designing new ways to control magnetic anisotropy in technologically important materials is highly desirable. Here we show that magnetic anisotropy of epitaxial thin-films of half-metallic ferromagnet La$_{0.7}$Sr$_{0.3}$MnO$_{3}$ (LSMO) is determined by the proximity to thermodynamic equilibrium conditions during growth. We performed a series of X-ray diffraction and ferromagnetic resonance (FMR) experiments in two different sets of samples: the first corresponds to LSMO thin-films deposited under tensile strain on (001) SrTiO$_{3}$ by Pulsed Laser Deposition (PLD; far from thermodynamic equilibrium); the second were deposited by a slow Chemical Solution Deposition (CSD) method, under quasi-equilibrium conditions. Thin films prepared by PLD show a in-plane cubic anisotropy with an overimposed uniaxial term. A large anisotropy constant perpendicular to the film plane was also observed in these films. However, the uniaxial anisotropy is completely suppressed in the CSD films. The out of plane anisotropy is also reduced, resulting in a much stronger in plane cubic anisotropy in the chemically synthesized films. This change is due to a different rotation pattern of MnO$_{6}$ octahedra to accomodate epitaxial strain, which depends not only on the amount of tensile stress imposed by the STO substrate, but also on the growth conditions. Our results demonstrate that the nature and magnitude of the magnetic anisotropy in LSMO can be tuned by the thermodynamic parameters during thin-film deposition.

cond-mat.mtrl-sci↗
arXiv2015

Electron degeneracy and intrinsic magnetic properties of epitaxial Nb:SrTiO$_3$ thin-films controlled by defects

We report thermoelectric power experiments in e-doped thin films of SrTiO$_3$ (STO) which demonstrate that the electronic band degeneracy can be lifted through defect management during growth. We show that even small amounts of cationic vacancies, combined with epitaxial stress, produce a homogeneous tetragonal distortion of the films, resulting in a Kondo-like resistance upturn at low temperature, large anisotropic magnetoresistance, and non-linear Hall effect. Ab-initio calculations confirm a different occupation of each band depending on the degree of tetragonal distortion. The phenomenology reported in this paper for tetragonally distorted e-doped STO thin films, is similarto that observed in LaAlO$_3$/STO interfaces and magnetic STO quantum wells.

cond-mat.mtrl-sci↗
arXiv2013

Magnetic Field Induced Transition in Vanadium Spinels

We study vanadium spinels $A$V$_2$O$_4$ ($A$ = Cd, Mg) in pulsed magnetic fields up to 65 T. A jump in magnetization at $μ_0 H \approx$ 40 T is observed in the single-crystal MgV$_2$O$_4$, indicating a field induced quantum phase transition between two distinct magnetic orders. In the multiferroic CdV$_2$O$_4$, the field-induced transition is accompanied by a suppression of the electric polarization. By modeling the magnetic properties in the presence of strong spin-orbit coupling characteristic of vanadium spinels, we show that both features of the field-induced transition can be successfully explained by including the effects of the local trigonal crystal field.

cond-mat.str-el↗
arXiv2012

Tuning the thermoelectric properties of SrTiO3 by controlled oxygen doping

We report the thermoelectric properties (Seebeck coefficient, thermal conductivity, and electrical resistivity) of lightly doped single crystals of (001)-oriented SrTiO3 (STO). Hall effect measurements show that electron doping around 10^-5 carriers per unit cell can be achieved by vacuum annealing of the crystals under carefully controlled conditions. The steep density of states near the Fermi energy of STO at this doping level (confirmed by ab initio calculations) retains an unusually large Seebeck coefficient, in spite of an increase in the electronic conductivity by several orders of magnitude. This effect, combined with a decrease in thermal conductivity due to vacancy disorder scattering makes intrinsic doping in STO (and other materials) an alternative strategy to optimize its thermoelectric figure of merit.

cond-mat.str-el↗
arXiv2010

Nonmonotonic Evolution of the Blocking Temperature in Dispersions of Superparamagnetic Nanoparticles

We use a Monte Carlo approach to simulate the influence of the dipolar interaction on assemblies of monodisperse superparamagnetic $γ-Fe_{2}O_{3}$ nanoparticles. We have identified a critical concentration c*, that marks the transition between two different regimes in the evolution of the blocking temperature ($T_{B}$) with interparticle interactions. At low concentrations (c < c*) magnetic particles behave as an ideal non-interacting system with a constant $T_{B}$. At concentrations c > c* the dipolar energy enhances the anisotropic energy barrier and $T_{B}$ increases with increasing c, so that a larger temperature is required to reach the superparamagnetic state. The fitting of our results with classical particle models and experiments supports the existence of two differentiated regimes. Our data could help to understand apparently contradictory results from the literature.

cond-mat.mes-hall↗
arXiv2010

Rapidly fluctuating orbital occupancy above the orbital ordering transition in spin-gap compounds

Several spin systems with low dimensionality develop a spin-dimer phase within a molecular orbital below TS, competing with long-range antiferromagnetic order. Very often, preferential orbital occupancy and ordering are the actual driving force for dimerization, as in the so-called orbitally-driven spin-Peierls compounds (MgTi2O4, CuIr2S4, La4Ru2O10, NaTiSi2O6, etc.). Through a microscopic analysis of the thermal conductivity k (T) in La4Ru2O10, we show that the orbital occupancy fluctuates rapidly above TS, resulting in an orbital-liquid state. The strong orbital-lattice coupling introduces dynamic bond-length fluctuations that scatter the phonons to produce a k (T) proportional to T (i.e. glass-like) above TS. This phonon-glass to phonon-crystal transition is shown to occur in other spin-dimer systems, like NaTiSi2O6, pointing to a general phenomenon.

cond-mat.str-el↗
arXiv2010

CdV2O4: A rare example of a collinear multiferroic spinel

By studying the dielectric properties of the geometrically frustrated spinel CdV2O4, we observe ferroelectricity developing at the transition into the collinear antiferromagnetic ground state. In this multiferroic spinel, ferroelectricity is driven by local magnetostriction and not by the more common scenario of spiral magnetism. The experimental findings are corroborated by ab-initio calculations of the electric polarization and the underlying spin and orbital order. The results point towards a charge rearrangement due to dimerization, where electronic correlations and the proximity to the insulator-metal transition play an important role.

cond-mat.str-el↗
arXiv2009

Study of the pressure effects in TiOCl by ab initio calculations

Electronic structure calculations on the low dimensional spin-1/2 compound TiOCl were performed at several pressures in the orthorhombic phase, finding that the structure is quasi-one-dimensional. The Ti3+ (d1) ions have one t2g orbital occupied (dyz) with a large hopping integral along the b direction of the crystal. The most important magnetic coupling is Ti-Ti along the b axis. The transition temperature (Tc) has a linear evolution with pressure, and at about 10 GPa this Tc is close to room temperature, leading to a room temperature spin-Peierls insulator-insulator transition, with an important reduction of the charge gap in agreement with the experiment. On the high-pressure monoclinic phase, TiOCl presents two possible dimerized structures, with a long or short dimerization. Long dimerized state occurs above 15 GPa, and below this pressure the short dimerized structure is the more stable phase.

cond-mat.str-el↗
arXiv2008

Identification of a Marginal Fermi-Liquid in Itinerant Ferromagnet CoS2

We report specific heat, resistivity and susceptibility measurements at different temperatures, magnetic fields, and pressures to provide solid evidence of CoS2 being a marginal Fermi liquid. The presence of a tricritical point in the phase diagram of the system provides an opportunity to test the spin fluctuation theory with a high limit of accuracy. A magnetic field suppresses the amplitude of the spin fluctuations and recovers conventional Fermi liquid behavior, connecting both states continuously.

cond-mat.str-el↗
arXiv2008

Enhanced dimerization of TiOCl under pressure: spin-Peierls - to - Peierls transition

We report high-pressure x-ray diffraction and magnetization measurements combined with ab-initio calculations to demonstrate that the high-pressure optical and transport transitions recently reported in TiOCl, correspond in fact to an enhanced Ti3+-Ti3+ dimerization existing already at room temperature. Our results confirm the formation of a metal-metal bond between Ti3+ ions along the b-axis of TiOCl, accompanied by a strong reduction of the electronic gap. The evolution of the dimerization with pressure suggests a crossover from the spin-Peierls to a conventional Peierls situation at high pressures.

cond-mat.str-el↗
arXiv2008

Homopolar bond formation in ZnV$_2$O$_4$ close to a metal-insulator transition

Electronic structure calculations for spinel vanadate ZnV$_2$O$_4$ show that partial electronic delocalization in this system leads to structural instabilities. These are a consequence of the proximity to the itinerant-electron boundary, not being related to orbital ordering. We discuss how this mechanism naturally couples charge and lattice degrees of freedom in magnetic insulators close to such a crossover. For the case of ZnV$_2$O$_4$, this leads to the formation of V-V dimers along the [011] and [101] directions that readily accounts for the intriguing magnetic structure of ZnV$_2$O$_4$.

cond-mat.str-el↗
arXiv2007

Enhanced Pressure Dependence of Magnetic Exchange in A2+[V2]O4 Spinels Approaching the Itinerant Electron Limit

We report a systematic enhancement of the pressure dependence of TN in A2+[V2]O4 spinels as the V-V separation approaches the critical separation for a transition to itinerant-electron behavior. An intermediate phase between localized and itinerant electron behavior is identified in Zn[V2]O4 and Mg[V2]O4 exhibiting mobile holes as large polarons. In Zn[V2]O4, cooperative ordering of V-V pairs below a Ts=TN does not totally suppress the V3+-ion spins at ambient pressure, but makes TN to decrease with pressure. Our results demonstrate that Zn[V2]O4 and Mg[V2]O4 are less localized than previously thought.

cond-mat.str-el↗