arXiv subjects

P. H. M. van Loosdrecht

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

At least 37 records · Page 2Linked to original sources

arXiv2019

Fingerprints of Kitaev physics in the magnetic excitations of honeycomb iridates

In the quest for realizations of quantum spin liquids, the exploration of Kitaev materials - spin-orbit entangled Mott insulators with strong bond-directional exchanges - has taken center stage. However, in these materials the local spin-orbital j=1/2 moments typically show long-range magnetic order at low temperature, thus defying the formation of a spin-liquid ground state. Using resonant inelastic x-ray scattering (RIXS), we here report on a proximate spin liquid regime with clear fingerprints of Kitaev physics in the magnetic excitations of the honeycomb iridates alpha-Li2IrO3 and Na2IrO3. We observe a broad continuum of magnetic excitations that persists up to at least 300K, more than an order of magnitude larger than the magnetic ordering temperatures. We prove the magnetic character of this continuum by an analysis of the resonance behavior. RIXS measurements of the dynamical structure factor for energies within the continuum show that dynamical spin-spin correlations are restricted to nearest neighbors. Notably, these spectroscopic observations are also present in the magnetically ordered state for excitation energies above the conventional magnon excitations. Phenomenologically, our data agree with inelastic neutron scattering results on the related honeycomb compound RuCl3, establishing a common ground for a proximate Kitaev spin-liquid regime in these materials.

cond-mat.str-el↗

arXiv2019

Coupled dynamics of long-range and internal spin cluster order in Cu$_{2}$OSeO$_{3}$

Cu$_4$ triplet clusters form the relevant spin entity for the formation of long-range magnetic order in the cluster magnet Cu$_2$OSeO$_3$. Using time-resolved Raman spectroscopy, we probed photoinduced spin and lattice dynamics in this Mott insulator. Multiple ps-decade spin-lattice relaxation dynamics is observed, evidencing a separation of the order parameter dynamics into disordering of long-range and internal spin cluster order. Our study exemplifies the double order parameter dynamics of generalized molecular crystals of charge, spin, and orbital nature.

cond-mat.str-el↗

arXiv2019

Dynamical resonance quench and Fano interference in spontaneous Raman scattering from quasiparticle and collective excitations

Time-resolved spontaneous Raman spectroscopy serves as a probe for incoherent quasiparticle and collective excitation dynamics, and allows to distinguish symmetry changes across a photoinduced phase transition through the inelastic light scattering selection rules. Largely unexplored is the role of the Raman resonance enhancement in the time-domain, and the transient interaction between scattering from quasiparticles and collective excitations, with the latter interaction leading to a Fano interference. In this work, we report on the observation of a phonon Raman tensor quench and Fano interference after strong photoexcitation of an intrinsic semiconductor. We observed a dynamic phonon scattering rate asymmetry and spectral asymmetry through simultaneous detection of both the anti-Stokes and Stokes response. The asymmetric phonon scattering rate is ascribed to the combined effect of the transient phonon population and the reduction of the phonon Raman tensor resulting from the photoexcited hole population. This same hole population results in a strong enhancement of the Fano spectral asymmetry.

cond-mat.mtrl-sci↗

arXiv2019

Resonant inelastic x-ray incarnation of Young's double-slit experiment

Young's archetypal double-slit experiment forms the basis for modern diffraction techniques: the elastic scattering of waves yields an interference pattern that captures the real-space structure. Here, we report on an inelastic incarnation of Young's experiment and demonstrate that resonant inelastic x-ray scattering (RIXS) measures interference patterns which reveal the symmetry and character of electronic excited states in the same way as elastic scattering does for the ground state. A prototypical example is provided by the quasi-molecular electronic structure of insulating Ba3CeIr2O9 with structural Ir dimers and strong spin-orbit coupling. The double 'slits' in this resonant experiment are the highly localized core levels of the two Ir atoms within a dimer. The clear double-slit-type sinusoidal interference patterns that we observe allow us to characterize the electronic excitations, demonstrating the power of RIXS interferometry to unravel the electronic structure of solids containing, e.g., dimers, trimers, ladders, or other superstructures.

cond-mat.str-el↗

arXiv2018

Temperature dependent percolation mechanism for conductivity in Y$_{0.63}$Ca$_{0.37}$TiO$_3$ revealed by a microstructure study

We have performed optical microscopy, micro-photoelectron spectroscopy, and micro-Raman scattering measurements on Y$_{0.63}$Ca$_{0.37}$TiO$_3$ single crystals in order to clarify the interplay between the microstructure and the temperature dependent electronic transport mechanisms in this material. Optical microscopy observations reveal dark and bright domain patterns on the surface with length scales of the order of several to a hundred micrometers showing a pronounced temperature dependent evolution. Spatially resolved photoelectron spectroscopy measurements show the different electronic character of these domains. Using micro-Raman spectroscopy, we observe a distinct temperature dependence of the crystal structure of these domains. On the basis of these findings the different domains are assigned to insulating and metallic volume fractions, respectively. By decreasing the temperature, the volume fraction of the conducting domains increases, hence allowing the electrons to percolate through the sample at temperatures lower than $\sim$150 K.

cond-mat.str-el↗

arXiv2018

Optically driven collective spin excitations and magnetization dynamics in the Néel-type skyrmion host GaV$_4$S$_8$

GaV$_4$S$_8$ is a multiferroic semiconductor hosting magnetic cycloid (Cyc) and Néel-type skyrmion lattice (SkL) phases with a broad region of thermal and magnetic stability. Here, we use time-resolved magneto-optical Kerr spectroscopy and micro-magnetic simulations to demonstrate the coherent generation of collective spin excitations in the Cyc and SkL phases driven by an optically-induced modulation of uniaxial anisotropy. Our results shed light on spin-dynamics in anisotropic materials hosting skyrmions and pave a new pathway for the optical control of their magnetic order.

cond-mat.str-el↗

arXiv2018

A tunable time-resolved spontaneous Raman spectroscopy setup for probing ultrafast collective excitation and quasiparticle dynamics in quantum materials

We present a flexible and efficient ultrafast time-resolved spontaneous Raman spectroscopy setup to study collective excitation and quasi-particle dynamics in quantum matter. The setup has a broad energy tuning range extending from the visible to near infrared spectral regions for both the pump excitation and Raman probe pulses. Additionally, the balance between energy and time-resolution can be controlled. A high light collecting efficiency is realized by high numerical aperture collection optics and a high-throughput flexible spectrometer. We demonstrate the functionality of the setup with a study of the zone-center longitudinal optical phonon and hole continuum dynamics in silicon, and discuss the role of the Raman tensor in time-resolved Raman scattering. In addition, we show evidence for unequal phonon softening rates at different high symmetry points in the Brillouin zone of silicon by means of detecting pump-induced changes in the two-phonon overtone spectrum. Demagnetization dynamics in the helimagnet Cu2OSeO3 is studied by observing softening and broadening of a magnon after photo-excitation, underlining the unique power of measuring transient dynamics in the frequency domain, and the feasibility to study phase transitions in quantum matter.

cond-mat.mtrl-sci↗

arXiv2015

Revealing puddles of electrons and holes in compensated topological insulators

Three-dimensional topological insulators harbour metallic surface states with exotic properties. In transport or optics, these properties are typically masked by defect-induced bulk carriers. Compensation of donors and acceptors reduces the carrier density, but the bulk resistivity remains disappointingly small. We show that measurements of the optical conductivity in BiSbTeSe$_2$ pinpoint the presence of electron-hole puddles in the bulk at low temperatures, which is essential for understanding DC bulk transport. The puddles arise from large fluctuations of the Coulomb potential of donors and acceptors, even in the case of full compensation. Surprisingly, the number of carriers appearing within puddles drops rapidly with increasing temperature and almost vanishes around 40 K. Monte Carlo simulations show that a highly non-linear screening effect arising from thermally activated carriers destroys the puddles at a temperature scale set by the Coulomb interaction between neighbouring dopants, explaining the experimental observation semi-quantitatively. This mechanism remains valid if donors and acceptors do not compensate perfectly.

cond-mat.mes-hall↗

arXiv2015

Temperature-dependent and anisotropic optical response of layered Pr$_{0.5}$Ca$_{1.5}$MnO$_{4}$ probed by spectroscopic ellipsometry

We study the temperature dependence as well as anisotropy of optical conductivity ($σ_1$) in the pseudocubic single crystal Pr$_{0.5}$Ca$_{1.5}$MnO$_{4}$ using spectrocopic ellipsometry. Three transition temperatures are observed and can be linked to charge-orbital ($T_{\rm CO/OO}$ $\sim$ 320 K), two-dimensional-antiferromagnetic (2D-AFM) ($\sim$ 200 K), and three-dimensional AFM ($T_{\rm N} \sim$ 125 K) orderings. Below $T_{\rm CO/OO}$, $σ_1$ shows a charge ordering peak ($\sim$0.8 eV) with a significant blue shift as the temperature decreases. Calculations based on a model that incorporates a static Jahn-Teller distortion and assumes the existence of a local charge imbalance between two different sublattices support this assignment and explain the blue shift. This view is further supported by the partial spectral weight analysis showing the onset of optical anisotropy at $T_{\rm CO/OO}$ in the charge-ordering region ($0.5-2.5$ eV). Interestingly, in the charge-transfer region ($2.5-4$ eV), the spectral weight shows anomalies around the $T_{\rm 2D-AFM}$ that we attribute to the role of oxygen-$p$ orbitals in stabilizing the CE-type magnetic ordering. Our result shows the importance of spin, charge, and lattice degrees of freedom in this layered manganite.

cond-mat.str-el↗

arXiv2014

Modelling Dynamical Fluorescent Micro Thermal Imaging of the Heat Diffusion in the La5Ca9Cu24O41 Spin Ladder Compound

The dynamical fluorescent microthermal imaging (FMI) experiment has been used to investigate the phonon-magnon interaction in the 1D Heisenberg antiferromagnet La5Ca9Cu24O41. This material shows highly anisotropic heat conductivity due to the efficient magnetic heat transport along the spin ladders in the compound. To extract information on the phonon-magnon interaction we modelled the dynamic heat transport experiment using a two temperature model approach, taking both the crystal as well as the PMMA/EuTTA fluorescent heat imaging layer into account. The simulations are carried out by the finite element method using COMSOL Multiphysics Heat Transfer Module. The results of the numerical calculations are expected to be used for the data analysis of the experimental studies.

cond-mat.mtrl-sci↗

arXiv2012

Hubbard exciton revealed by time-domain optical spectroscopy

We use broadband ultra-fast pump-probe spectroscopy in the visible range to study the lowest excitations across the Mott-Hubbard gap in the orbitally ordered insulator YVO3. Separating thermal and non-thermal contributions to the optical transients, we show that the total spectral weight of the two lowest peaks is conserved, demonstrating that both excitations correspond to the same multiplet. The pump-induced transfer of spectral weight between the two peaks reveals that the low-energy one is a Hubbard exciton, i.e. a resonance or bound state between a doublon and a holon. Finally, we speculate that the pump-driven spin-disorder can be used to quantify the kinetic energy gain of the excitons in the ferromagnetic phase.

cond-mat.str-el↗

arXiv2011

A road to hydrogenating graphene by a reactive ion etching plasma

We report the hydrogenation of single and bilayer graphene by an argon-hydrogen plasma produced in a reactive ion etching (RIE) system. Electronic transport measurements in combination with Raman spectroscopy are used to link the electric mean free path to the optically extracted defect concentration. We emphasize the role of the self-bias of the graphene in suppressing the erosion of the akes during plasma processing. We show that under the chosen plasma conditions the process does not introduce considerable damage to the graphene sheet and that hydrogenation occurs primarily due to the hydrogen ions from the plasma and not due to fragmentation of water adsorbates on the graphene surface by highly accelerated plasma electrons. For this reason the hydrogenation level can be precisely controlled. The hydrogenation process presented here can be easily implemented in any RIE plasma system.

cond-mat.mtrl-sci↗

arXiv2010

Quest for Order in Chaos: Hidden Repulsive Level Statistics in Disordered Quantum Nanoaggregates

The local distribution of exciton levels in disordered cyanine-dye-based molecular nano-aggregates has been elucidated using fluorescence line narrowing spectroscopy. The observation of a Wigner-Dyson-type level spacing distribution provides direct evidence of the existence of level repulsion of strongly overlapping states in the molecular wires, which is important for the understanding of the level statistics, and therefore the `functional properties, of a large variety of nano-confined systems.

cond-mat.dis-nn↗

arXiv2010

Origin of the ESR spectrum in the Prussian Blue analogue RbMn[Fe(CN)6]*H2O

We present an ESR study at excitation frequencies of 9.4 GHz and 222.4 GHz of powders and single crystals of a Prussian Blue analogue (PBA), RbMn[Fe(CN)6]*H2O in which Fe and Mn undergoes a charge transfer transition between 175 and 300 K. The ESR of PBA powders, also reported by Pregelj et al. (JMMM, 316, E680 (2007)) is assigned to cubic magnetic clusters of Mn2+ ions surrounding Fe(CN)6 vacancies. The clusters are well isolated from the bulk and are superparamagnetic below 50 K. In single crystals various defects with lower symmetry are also observed. Spin-lattice relaxation broadens the bulk ESR beyond observability. This strong spin relaxation is unexpected above the charge transfer transition and is attributed to a mixing of the Mn3+ - Fe2+ state into the prevalent Mn2+ - Fe3+ state.

cond-mat.str-el↗

arXiv2010

Suppressed spin dephasing for 2D and bulk electrons in GaAs wires due to engineered cancellation of spin-orbit interaction terms

We report a study of suppressed spin dephasing for quasi-one-dimensional electron ensembles in wires etched into a GaAs/AlGaAs heterojunction system. Time-resolved Kerr-rotation measurements show a suppression that is most pronounced for wires along the [110] crystal direction. This is the fingerprint of a suppression that is enhanced due to a strong anisotropy in spin-orbit fields that can occur when the Rashba and Dresselhaus contributions are engineered to cancel each other. A surprising observation is that this mechanisms for suppressing spin dephasing is not only effective for electrons in the heterojunction quantum well, but also for electrons in a deeper bulk layer.

cond-mat.mes-hall↗

arXiv2010

Heat conductivity of the spin-Peierls compounds TiOCl and TiOBr

We report experimental results on the heat conductivity κof the S=1/2 spin chain compounds TiOBr and TiOCl for temperatures 5K<T<300K and magnetic fields up to 14. Surprisingly, we find no evidence of a significant magnetic contribution to κ, which is in stark contrast to recent results on S=1/2 spin chain cuprates. Despite this unexpected result, the thus predominantly phononic heat conductivity of these spin-Peierls compounds exhibits a very unusual behavior. In particular, we observe strong anomalies at the phase transitions Tc1 and Tc2. Moreover, we find an overall but anisotropic suppression of κin the intermediate phase which extends even to temperatures higher than Tc2. An external magnetic field causes a slight downshift of the transition at Tc1 and enhances the suppression of κup to Tc2. We interprete our findings in terms of strong spin-phonon coupling and phonon scattering arising from spin-driven lattice distortions.

cond-mat.str-el↗

arXiv2009

Optical probing of spin dynamics of two-dimensional and bulk electrons in a GaAs/AlGaAs heterojunction system

We present time-resolved Kerr rotation measurements of electron spin dynamics in a GaAs/AlGaAs heterojunction system that contains a high-mobility two-dimensional electron gas (2DEG). Due to the complex layer structure of this material the Kerr rotation signals contain information from electron spins in three different layers: the 2DEG layer, a GaAs epilayer in the heterostructure, and the underlying GaAs substrate. The 2DEG electrons can be observed at low pump intensities, using that they have a less negative g-factor than electrons in bulk GaAs regions. At high pump intensities, the Kerr signals from the GaAs epilayer and the substrate can be distinguished when using a barrier between the two layers that blocks intermixing of the two electron populations. This allows for stronger pumping of the epilayer, which results in a shift of the effective g-factor. Thus, three populations can be distinguished using differences in g-factor. We support this interpretation by studying how the spin dynamics of each population has its unique dependence on temperature, and how they correlate with time-resolved reflectance signals.

cond-mat.mes-hall↗

arXiv2009

High-field recovery of the undistorted triangular lattice in the frustrated metamagnet CuFeO2

Pulsed field magnetization experiments extend the typical metamagnetic staircase of CuFeO2 up to 58 T to reveal an additional first order phase transition at high field for both the parallel and perpendicular field configuration. Virtually complete isotropic behavior is retrieved only above this transition, indicating the high-field recovery of the undistorted triangular lattice. A consistent phenomenological rationalization for the field dependence and metamagnetism crossover of the system is provided, demonstrating the importance of both spin-phonon coupling and a small field-dependent easy-axis anisotropy in accurately describing the magnetization process of CuFeO2.

cond-mat.str-el↗