Searcharxiv⌕ Search

arXiv subjects

Paul H. M. van Loosdrecht

Publications and source records attributed to Paul H. M. van Loosdrecht.

34 records · Page 2Linked to original sources

Origin of the hump anomalies in the Hall resistance loops of ultrathin SrRuO$_3$/SrIrO$_3$ multilayers

The proposal that very small Néel skyrmions can form in SrRuO$_3$/SrIrO$_3$ epitaxial bilayers and that the electric field-effect can be used to manipulate these skyrmions in gated devices strongly stimulated the recent research of SrRuO$_3$ heterostructures. A strong interfacial Dzyaloshinskii-Moriya interaction, combined with the breaking of inversion symmetry, was considered as the driving force for the formation of skyrmions in SrRuO$_3$/SrIrO$_3$ bilayers. Here, we investigated nominally symmetric heterostructures in which an ultrathin ferromagnetic SrRuO$_3$ layer is sandwiched between large spin-orbit coupling SrIrO$_3$ layers, for which the conditions are not favorable for the emergence of a net interfacial Dzyaloshinskii-Moriya interaction. Previously the formation of skyrmions in the asymmetric SrRuO$_3$/SrIrO$_3$ bilayers was inferred from anomalous Hall resistance loops showing humplike features that resembled topological Hall effect contributions. Symmetric SrIrO$_3$/SrRuO$_3$/SrIrO$_3$ trilayers do not show hump anomalies in the Hall loops. However, the anomalous Hall resistance loops of symmetric multilayers, in which the trilayer is stacked several times, do exhibit the humplike structures, similar to the asymmetric SrRuO$_3$/SrIrO$_3$ bilayers. The origin of the Hall effect loop anomalies likely resides in unavoidable differences in the electronic and magnetic properties of the individual SrRuO$_3$ layers rather than in the formation of skyrmions.

cond-mat.mtrl-sci↗

Excitonic Transport and Intervalley Scattering in Exfoliated MoSe2 Monolayer Revealed by Four-Wave-Mixing Transient Grating Spectroscopy

Exciton intervalley scattering, annihilation and relaxation dynamics, and diffusive transport in a monolayer transition metal dichalcogenides are central to the functionality of devices based on them. This motivated us to investigate these properties in exfoliated high-quality monolayer MoSe2 using heterodyned nonlinear four-wave-mixing transient grating spectroscopy. While free exciton excitations are found to be long-lived (~230 ps), an extremely fast intervalley scattering ( less than 120 fs) is observed leading to a negligible valley polarization, consistent with steady state photoluminescence measurements. The exciton population decay shows an appreciable contribution from exciton-exciton annihilation reactions with an annihilation constant of ~ 0.01 cm2s-1, which in addition leads to an extra contribution to the transient grating response. The underlying excitonic dynamics were numerically modeled by including exciton-exciton annihilation, also in the diffusion equation, which allows extraction of the diffusion constant, D ~1.4 cm2s-1. Our results provide a method that allows for the disentanglement of the intricate dynamics involving many-body annihilation processes and a detailed characterization of the excitonic properties of monolayer MoSe2

cond-mat.mes-hall↗

Non-perturbative high-harmonic generation in the three-dimensional Dirac semimetal Cd$_3$As$_2$

Harmonic generation is a general characteristic of driven nonlinear systems, and serves as an efficient tool for investigating the fundamental principles that govern the ultrafast nonlinear dynamics. In atomic gases, high-harmonic radiation is produced via a three-step process of ionization, acceleration, and recollision by strong-field infrared laser. This mechanism has been intensively investigated in the extreme ultraviolet and soft X-ray regions, forming the basis of attosecond research. In solid-state materials, which are characterized by crystalline symmetry and strong interactions, yielding of harmonics has just recently been reported. The observed high-harmonic generation was interpreted with fundamentally different mechanisms, such as interband tunneling combined with dynamical Bloch oscillations, intraband thermodynamics and nonlinear dynamics, and many-body electronic interactions. Here, in a distinctly different context of three-dimensional Dirac semimetal, we report on experimental observation of high-harmonic generation up to the seventh order driven by strong-field terahertz pulses. The observed non-perturbative high-harmonic generation is interpreted as a generic feature of terahertz-field driven nonlinear intraband kinetics of Dirac fermions. We anticipate that our results will trigger great interest in detection, manipulation, and coherent control of the nonlinear response in the vast family of three-dimensional Dirac and Weyl materials.

cond-mat.mtrl-sci↗

Correlating the nanoscale structural, magnetic and magneto-transport properties in SrRuO3-based perovskite oxide ultra-thin films

We investigated the structural and magnetic properties of bare SrRuO$_3$ (SRO) ultra-thin films and SrRuO$_3$/SrIrO$_3$/SrZrO$_3$ (SRO/SIO/SZO: RIZ) trilayer heterostructures between 10 K and 80 K, by comparing macroscopic data using magneto-optical Kerr effect (MOKE) and magneto-transport (anomalous Hall effect: AHE), with nanoscale fingerprints when applying non-contact scanning force microscopy (nc-SFM) and magnetic force microscopy (MFM). SRO and RIZ ultra-thin films were epitaxially grown at 650C onto vicinal SrTiO$_3$ (100) single-crystalline substrates to a nominal thickness of 4 and 4/2/2 unit cells (uc), respectively. Our correlated analysis allows associating topographic sample features of overgrown individual layers to their residual magnetization, as is shown here to be relevant for interpreting the macroscopic AHE data. Although the hump-like features in the AHE suggest a magnetically extured skyrmion phase to exist around 55 K associated to the topological Hall effect (THE), both our MOKE and MFM data cannot support this theory. In contrast, our SFM/MFM local-scale analysis finds the local coercive field to be strongly dependent on the effective layer thickness and stoichiometry in both the SRO and RIZ samples, with huge impact on the local band-structure. In fact, it is these variations that in turn mimic a potential THE through anomalies in the AHE resistivity loops.

physics.app-ph↗

Incoherent phonon population and exciton-exciton annihilation in monolayer WS2 revealed by time-resolved spontaneous Raman scattering

Atomically thin layer transition metal dichalcogenides have been intensively investigated for their rich optical properties and potential applications in nano-electronics. In this work, we study the incoherent optical phonon and exciton population dynamics in monolayer WS2 by time-resolved spontaneous Raman scattering spectroscopy. Upon excitation of the exciton transition, both the Stokes and anti-Stokes optical phonon scattering strength exhibit a large reduction. Based on the detailed balance, the optical phonon population is retrieved, which shows an instant build-up and a relaxation lifetime of around 4 ps at an exciton density E12 cm-2. The corresponding optical phonon temperature rises by 25 K, eventually, after some 10s of picoseconds, leading to a lattice heating by only around 3 K. The exciton relaxation dynamics extracted from the transient vibrational Raman response shows a strong excitation density dependence, signaling an important bi-molecular contribution to the decay. The exciton relaxation rate is found to be (70 ps)-1 and exciton-exciton annihilation rate 0.1 cm2s-1. These results provide valuable insight into the thermal dynamics after optical excitation and enhance the understanding of the fundamental exciton dynamics in two-dimensional transition metal materials.

cond-mat.mtrl-sci↗

Phonon mode calculations and Raman spectroscopy of the bulk-insulating topological insulator BiSbTeSe$_2$

The tetradymite compound BiSbTeSe$_2$, is one of the most bulk-insulating three-dimensional topological insulators, which makes it important in the topological insulator research. It is a member of the solid-solution system Bi$_{2-x}$Sb$_x$Te$_{3-y}$Se$_y$, for which the local crystal structure, such as the occupation probabilities of each atomic site, is not well understood. We have investigated the temperature and polarization dependent spontaneous Raman scattering in BiSbTeSe$_2$, revealing a much higher number of lattice vibrational modes than predicted by group theoretical considerations for the space group R$\bar{3}$m corresponding to an ideally random solid-solution situation. The density functional calculations of phonon frequencies show a very good agreement with experimental data for parent material Bi$_2$Te$_3$, where no disorder effects were found. In comparison to Bi$_2$Te$_3$ the stacking disorder in BiSbTeSe$_2$, causes a discrepancy between theory and experiment. Combined analysis of experimental Raman spectra and DFT calculated phonon spectra for different types of atomic orders showed coexistence of different sequences of layers in the material and that those with Se in the center and a local order of Se-Bi-Se-Sb-Te, are the most favored.

cond-mat.str-el↗

Photo-induced magnetization enhancement in two-dimensional weakly anisotropic Heisenberg magnets

By comparing the photo-induced magnetization dynamics in simple layered systems we show how light-induced modifications of the magnetic anisotropy directly enhance the magnetization. It is observed that the spin precession in (CH3NH3)2CuCl4, initiated by a light pulse, increases in amplitude at the critical temperature TC. The phenomenon is related to the dependence of the critical temperature on the axial magnetic anisotropy. The present results underline the possibility and the importance of the optical modifications of the anisotropy, opening new paths toward the control of the magnetization state for ultrafast memories.

cond-mat.mtrl-sci↗

Thermal conductivity of anisotropic spin - 1/2 two leg ladder:Green's function approach

We study the thermal transport of a spin-1/2 two leg antiferromagnetic ladder in the direction of legs. The possible effect of spin-orbit coupling and crystalline electric field are investigated in terms of anisotropies in the Heisenberg interactions on both leg and rung couplings. The original spin ladder is mapped to a bosonic model via a bond-operator transformation where an infinite hard-core repulsion is imposed to constrain one boson occupation per site. The Green's function approach is applied to obtain the energy spectrum of quasi-particle excitations responsible for thermal transport. The thermal conductivity is found to be monotonically decreasing with temperature due to increased scattering among triplet excitations at higher temperatures. A tiny dependence of thermal transport on the anisotropy in the leg direction at low temperatures is observed in contrast to the strong one on the anisotropy along the rung direction, due to the direct effect of the triplet density. Our results reach asymptotically the ballistic regime of the spin - 1/2 Heisenberg chain and compare favorably well with exact diagonalization data.

cond-mat.str-el↗

The Role of Driving Energy and Delocalised States for Charge Separation in Organic Semiconductors

The electron-hole pair created via photon absorption in organic photoconversion systems must overcome the Coulomb attraction to achieve long-range charge separation. We show that this process is facilitated through the formation of excited, delocalized band states. In our experiments on organic photovoltaic cells, these states were accessed for a short time (<1ps) via IR optical excitation of electron-hole pairs bound at the heterojunction. Atomistic modelling showed that the IR photons promote bound charge pairs to delocalised band states, similar to those formed just after singlet exciton dissociation, which indicates that such states act as the gateway for charge separation. Our results suggest that charge separation in efficient organic photoconversion systems, occurs through hot-state charge delocalisation rather than energy-gradient-driven intermolecular hopping.

cond-mat.mes-hall↗

Magneto-absorption spectra of hydrogen-like yellow exciton series in cuprous oxide: excitons in strong magnetic fields

We study the absorption spectra of the yellow excitons in Cu$_2$O in high magnetic fields using polarization-resolved optical absorption measurements with a high frequency resolution. We show that the symmetry of the yellow exciton results in unusual selection rules for the optical absorption of polarized light and that the mixing of ortho- and para- excitons in magnetic field is important. Our calculation of the energies of the yellow exciton series in an arbitrary magnetic field gives an excellent fit to experimental data and allows us to understand the complex structure of excitonic levels and their magnetic field dependence, which resolves the old-standing disagreement between the results of optical absorption and cyclotron resonance measurements.

cond-mat.mtrl-sci↗

Magnetodielectric and magnetoelastic coupling in TbFe3(BO3)4

We have studied the magnetodielectric and magnetoelastic coupling in TbFe3(BO3)4 single crystals by means of capacitance, magnetostriction and Raman spectroscopy measurements. The data reveal strong magnetic field effects on the dielectric constant and on the macroscopic sample length which are associated to long range magnetic ordering and a field-driven metamagnetic transition. We discuss the coupling of the dielectric, structural, and magnetic order parameters and attribute the origin of the magnetodielectric coupling to phonon mode shifts according to the Lyddane-Sachs-Teller (LST) relation.

cond-mat.mtrl-sci↗

Mapping the B,T phase diagram of frustrated metamagnet CuFeO2

The magnetic phase diagram of CuFeO2 as a function of applied magnetic field and temperature is thoroughly explored and expanded, both for magnetic fields applied parallel and perpendicular to the material's c-axis. Pulsed field magnetization measurements extend the typical magnetic staircase of CuFeO2 at various temperatures, demonstrating the persistence of the recently discovered high field metamagnetic transition up to Tn2 ~ 11 K in both field configurations. An extension of the previously introduced phenomenological spin model used to describe the high field magnetization process (Phys. Rev. B, 80, 012406 (2009)) is applied to each of the consecutive low-field commensurate spin structures, yielding a semi-quantitative simulation and intuitive description of the entire experimental magnetization process in both relevant field directions with a single set of parameters.

cond-mat.mtrl-sci↗

Probing ultrafast symmetry breaking in photo-stimulated matter

The nature of a phase transition is inherently connected to the changes in the crystalline symmtry, which is typically probed by elastic or inelastic scattering with neutrons, electrons or photons. When such a phase transition is stimulated by light or other sudden perturbations the solid evolves along a non-equilibrium pathway of which the underlying physics is poorly understood. Here we use picosecond Raman scattering to study the photo-induced ultrafast dynamics in Peierls distorted Antimony. We find evidence for an ultrafast non-thermal reversible structural phase transition. Most surprisingly, we find evidence that this transition evolves toward a lower symmetry, in contrast to the commonly accepted rhombohedral-to-simple cubic transition path. Our study demonstrates the feasibility of ultrafast Raman scattering symmetry analysis of photo-induced non-thermal transient phases.

cond-mat.mtrl-sci↗

Dynamics of spin and orbital phase transitions in YVO3

YVO3 exhibits a well separated sequence of orbital and spin order transitions at 200 K and 116 K, followed by a combined spin-orbital reorientation at 77 K. It is shown that the spin order can be destroyed by a sufficiently strong optical pulse within less than 4 ps. In contrast, the orbital reordering transition from C-type to G-type orbital order is slower than 100 ps and goes via an intermediate nonthermal phase. We propose that the dynamics of phase transitions is subjected to symmetry relations between the associated phases.

cond-mat.str-el↗

Symmetry disquisition on the TiOX phase diagram

The sequence of phase transitions and the symmetry of in particular the low temperature incommensurate and spin-Peierls phases of the quasi one-dimensional inorganic spin-Peierls system TiOX (TiOBr and TiOCl) have been studied using inelastic light scattering experiments. The anomalous first-order character of the transition to the spin-Peierls phase is found to be a consequence of the different symmetries of the incommensurate and spin-Peierls (P$2_{1}/m$) phases. The pressure dependence of the lowest transition temperature strongly suggests that magnetic interchain interactions play an important role in the formation of the spin-Peierls and the incommensurate phases. Finally, a comparison of Raman data on VOCl to the TiOX spectra shows that the high energy scattering observed previously has a phononic origin.

cond-mat.str-el↗

Raman scattering from phonons and magnons in RFe3)BO3)4

Inelastic light scattering spectra of several members of the RFe3(BO3)4 family reveal a cascade of phase transitions as a function of temperature, starting with a structural, weakly first order, phase transition followed by two magnetic phase transitions. Those consist of the ordering of the Fe-spin sublattice revealed by all the compound, and a subsequent spin-reorientational transition for GdFe3(BO3)4. The Raman data evidence a strong coupling between the lattice and magnetic degrees of freedom in these borates. The Fe-sublattice ordering leads to a strong suppression of the low energy magnetic scattering, and a multiple peaked two-magnon scattering continuum is observed. Evidence for short-range correlations is found in the `paramagnetic' phase by the observation of a broad magnetic continuum in the Raman data, which persists up to surprisingly high temperatures.

cond-mat.str-el↗