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Paul H. M. van Loosdrecht

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

At least 19 recordsLinked to original sources

Tracking the Catastrophic Collapse of Hybrid Exciton-Phonon Order in a Quantum Material

Revealing the interactions binding electronic and lattice components of cooperative quantum order is central to sculpting new states of matter. This challenge is epitomized by the charge density wave material 1T-TiSe$_2$, where photoexcitation disrupts its presumed hybrid exciton-phonon order. This exposes a paradox: the electronic component collapses within femtoseconds while the periodic lattice distortion persists. If the lattice distortion outlives the excitonic condensate, were they truly intertwined? Here we resolve this by uncovering a low-frequency mode (approx. 0.13 THz) emerging only in the ordered state, signaling exciton-phonon coupling. This mode is consistent with a locked phason -- a collective excitation arising if coupling between the excitonic condensate and lattice reduces continuous phase symmetry to a discrete one, giving the excitonic Goldstone mode finite mass. This is captured by an effective theory describing a shared potential landscape. At a critical threshold, the collapse of excitonic order flattens the potential, triggering an exciton-phonon catastrophe: selective overheating of the charge density wave phonon, disappearance of the locked phason, and sudden loss of electronic coherence. Remarkably, the lattice distortion survives as a dynamically trapped, non-thermal remnant, confirmed by the anomalous temperature dependence of the phononic response. These findings demonstrate that coupled potential energy landscapes can be manipulated to selectively dismantle complex quantum orders, advancing material control through dynamical design.

physics.app-ph↗

Photoinduced Electronic Band Dynamics and Defect-mediated Surface Potential Evolution in PdSe$_2$

We use time- and angle-resolved photoemission spectroscopy (TR-ARPES) combined with density functional theory to investigate ultrafast carrier dynamics in low-symmetry layered semiconducting PdSe$_2$. The indirect bandgap is determined to be 0.55~eV. Following photoexcitation above this gap, we resolve a valence band shift and broadening, both lasting less than a picosecond, consistent with bandgap renormalization and carrier scattering, indicative of strong many-body interactions. Subsequently, hot carriers populate the conduction band minimum and are captured by defect states. A surface photovoltage (SPV) of $\sim$ 67~meV emerges, persisting for over 50~ps, driven by defect-assisted charge separation. The formation of native vacancies, promoted by the low-symmetry lattice, likely gives rise to the mid-gap states responsible for this long-lived SPV response. Detailed analysis of TR-ARPES spectra disentangles the contributions of bandgap renormalization, carrier scattering, defect states, and SPV. These findings establish PdSe$_2$ as a prototypical layered quantum material exhibiting exotic photoresponses on ultrafast timescales.

cond-mat.mes-hall↗

Unveiling Ultrafast Spin-Valley Dynamics and Phonon-Mediated Charge Transfer in MoSe$_{2}$/WSe$_{2}$ Heterostructures

We use helicity-resolved ultrafast transient absorption spectroscopy to study spin-valley polarization dynamics in a vertically stacked MoSe$_{2}$/WSe$_{2}$ heterostructure. The experimental findings reveal details of interlayer charge transfer on ultrafast timescales, showing that the spin-valley polarized state of photoexcited carriers is conserved during the charge transfer and formation of interlayer excitons. Our results confirm that phonon scattering mediates the interlayer charge transfer process, while a high phonon population at elevated temperatures causes a significant decrease in spin-valley selective charge transfer. Moreover, the experimental findings demonstrate the possibility that interlayer excitons and their spin-valley polarization can be probed in the optical response of intralayer excitons. These findings pave the way for ultrafast detection, control, and manipulation of spin-valley polarized excitons in transition metal dichalcogenide-based 2D heterostructures.

physics.app-ph↗

THz Control of Exchange Mode in a Ferrimagnetic Cavity

The interaction of terahertz (THz) radiation with high-frequency spin resonances in complex magnetic materials is central for modern ultrafast magnonics. Here we demonstrate strong variations of the excitation efficiency of the sub-THz exchange magnon in a single crystal ferrimagnet (Gd,Bi)$_3$Fe$_5$O$_{12}$. An enhancement of the exchange magnon amplitude is observed when its frequency matches an eigenmode of the cavity created by the sample interfaces. Moreover, this enhancement is accompanied by a 5-fold decrease in effective damping of the exchange mode. The THz-exchange magnon interaction in the cavity is analyzed within the developed Landau-Lifshitz-Gilbert formalism for three coupled magnetization sublattices and cavity-enhanced THz field. This work presents a novel approach for the THz excitation of spin dynamics in ferrimagnets and outlines promising pathways for the controlled optimization of light-spin coupling in single crystals.

cond-mat.other↗

Tuning the interlayer coupling in La0.7Sr0.3Mn0.95Ru0.05O3 / LaNiO3 multilayers with perpendicular magnetic anisotropy

In ferromagnetic oxide epitaxial multilayers, magnetic properties and interlayer coupling are determined by a variety of factors. Beyond the contribution of interlayer exchange coupling, strain and interfacial effects, such as structural reconstructions or charge transfer, play significant roles, resulting in complex magnetic behaviour. In this study the interlayer coupling of ferromagnetic La0.7Sr0.3Mn0.95Ru0.05O3 (LSMRO) layers (8 nm thick) was investigated, when separated by epitaxial spacers of paramagnetic metallic LaNiO3 (LNO), in stacks exhibiting perpendicular magnetic anisotropy. By varying the thickness of the spacer, it was found that the coupling between two LSMRO layers changes from antiferromagnetic (with a 4 unit cell thick LNO spacer) to ferromagnetic (with a 6 unit cells thick LNO spacer). For multilayers comprising five LSMRO layers and a 4 unit cell thick LNO spacer, the antiferromagnetic coupling was preserved. However, the effective magnetic anisotropy changed, causing the magnetization to cant more towards the in-plane direction. This behavior was corroborated by X-ray magnetic circular dichroism (XMCD) investigations at the Mn and Ni L3-edges. The XMCD results indicated that the 4 unit cells thick LNO spacer in the multilayer become magnetically ordered, closely following the magnetization of adjacent LSMRO layers.

cond-mat.mtrl-sci↗

Resonance-Induced Anomalies in Temperature-Dependent Raman Scattering of PdSe$_{2}$

We report a comprehensive Raman study of the phonon behaviour in PdSe$_2$ in the temperature range of 5 K to 300 K. A remarkable change in the Raman spectrum is observed at 120 K: a significant enhancement of the out-of-plane phonon A$^{1}_{g}$ mode, accompanied by a suppression of the in-plane A$^{2}_{g}$ and B$^{2}_{1g}$ modes. This intriguing behavior is attributed to a temperature-dependent resonant excitation effect. The results are supported by density functional theory (DFT) calculations, which demonstrate that the electron-phonon coupling for the phonon modes varies and is strongly associated with the relevant electronic states. Furthermore, nonlinear frequency shifts are identified in all modes, indicating the decay of an optical phonon into multiple acoustic phonons. The study of Raman emission reported here, complemented by linear optical spectroscopy, reveals an unexpected scenario for the vibrational properties of PdSe$_2$ that holds substantial promise for future applications in PdSe$_2$-based optoelectronics.

cond-mat.str-el↗

Ultrafast Optical Control of Exciton Diffusion in WSe$_2$/Graphene Heterostructures Revealed by Heterodyne Transient Grating Spectroscopy

Using heterodyne transient grating spectroscopy, we observe a significant enhancement of exciton diffusion within a monolayer WSe$_2$ stacked on top of graphene. We further demonstrate that the diffusion dynamics can be optically tuned on the ultrafast time scale (i.e. a few picoseconds) by altering the photoexcited charge carrier density in graphene. The results reveal that, on a time scale of a few picoseconds, the effective diffusion constant in the WSe$_2$/graphene heterostructure is approximately 40 cm$^2 $/s, representing a substantial improvement over the 2 cm$^2 $/s typical for an isolated monolayer of WSe$_2$. The enhanced diffusion can be understood in terms of a transient screening of impurities, charge traps, and defect states in WSe$_2$ by photoexcited charge carriers in graphene. Furthermore, we observe that the diffusion within WSe$_2$ is affected by interlayer interactions, like charge transfer, exhibiting different dynamic states depending on the incident excitation fluence. These findings underscore the dynamic nature of screening and diffusion processes in heterostructures of 2D semiconductors and graphene and provide valuable insights for future applications of these systems in ultrafast optoelectronic devices.

cond-mat.mes-hall↗

Impulsive Fermi magnon-phonon resonance in antiferromagnetic $CoF_{2}$

Understanding spin-lattice interactions in antiferromagnets is one of the most fundamental issues at the core of the recently emerging and booming fields of antiferromagnetic spintronics and magnonics. Recently, coherent nonlinear spin-lattice coupling was discovered in an antiferromagnet which opened the possibility to control the nonlinear coupling strength and thus showing a novel pathway to coherently control magnon-phonon dynamics. Here, utilizing intense narrow band terahertz (THz) pulses and tunable magnetic fields up to 7 T, we experimentally realize the conditions of the Fermi magnon-phonon resonance in antiferromagnetic $CoF_{2}$. These conditions imply that both the spin and the lattice anharmonicities harvest energy transfer between the subsystems, if the magnon eigenfrequency $f_{m}$ is twice lower than the frequency of the phonon $2f_{m}=f_{ph}$. Performing THz pump-infrared probe spectroscopy in conjunction with simulations, we explore the coupled magnon-phonon dynamics in the vicinity of the Fermi-resonance and reveal the corresponding fingerprints of an impulsive THz-induced response. This study focuses on the role of nonlinearity in spin-lattice interactions, providing insights into the control of coherent magnon-phonon energy exchange.

cond-mat.mes-hall↗

Magnetic Anisotropy and Its Structural Origins in Ru-Substituted Manganite Films

Controlling magnetic anisotropy (MA) is important in a variety of applications including magnetic memories, spintronic sensors, and skyrmion-based data distribution. The perovskite manganite family provides a fertile playground for complex, intricate, and potentially useful structure-magnetism relations. Here we report on the MA that emerges in 10% Ru substituted $La_{0.7}Sr_{0.3}MnO_{3}$ (Ru-LSMO) films for which strong perpendicular magnetization and anisotropic in-plane magnetization are found. These moderately compressively strained films possess a rich microstructure, consisting of coherently strained phase which evolves into a one dimensional (1D) periodically-modulated structure above a critical thickness. We illustrate how 10% Ru substitution plays a crucial role behind the observed MA, and how the structural distortion and 1D periodic structural modulation produce the anisotropic in-plane magnetization. We highlight the practical significance of the observed MA, which could pave the way towards the realization of cutting-edge oxide-based room temperature spintronic memory devices.

cond-mat.mtrl-sci↗

Chiral excitations and the intermediate-field spin-liquid regime in the Kitaev magnet $α$-RuCl$_3$

In the Kitaev magnet $α$-RuCl$_3$, the existence of a magnetic-field-induced quantum spin liquid phase and of anyonic excitations are discussed controversially. We address this elusive, exotic phase via helicity-dependent Raman scattering and analyze the Raman optical activity of excitations as a function of magnetic field and temperature. The hotly debated field regime between 7.5 T and 10.5 T is characterized by clear spectroscopic signatures such as a plateau of the Raman optical activity of the dominant, chiral spin-flip excitation. This provides direct evidence for the existence of a distinct intermediate field regime compatible with a quantum spin liquid phase.

cond-mat.str-el↗

Disentangling the magneto-optic Kerr effect of manganite epitaxial heterostructures

Magneto-optic Kerr effect can probe the process of magnetization reversal in ferromagnetic thin films and thus be used as an alternative to magnetometry. Kerr effect is wavelength-dependent and the Kerr rotation can reverse sign, vanishing at particular wavelengths. We investigate epitaxial heterostructures of ferromagnetic manganite, La$_{0.7}$Sr$_{0.3}$Mn$_{0.9}$Ru$_{0.1}$O$_3$, by polar Kerr effect and magnetometry. The manganite layers are separated by or interfaced with a layer of nickelate, NdNiO$_3$. Kerr rotation hysteresis loops of trilayers, with two manganite layers of different thickness separated by a nickelate layer, have intriguing humplike features, when measured with light of 400 nm wavelength. By investigating additional reference samples we disentangle the contributions of the individual layers to the loops: we show that the humps originate from the opposite sense of the Kerr rotation of the two different ferromagnetic layers, combined with the additive behavior of the Kerr signal.

cond-mat.mtrl-sci↗

Ellipticity control of terahertz high-harmonic generation in a Dirac semimetal

We report on terahertz high-harmonic generation in a Dirac semimetal as a function of the driving-pulse ellipticity and on a theoretical study of the field-driven intraband kinetics of massless Dirac fermions.Very efficient control of third-harmonic yield and polarization state is achieved in electron-doped Cd$_3$As$_2$ thin films at room temperature. The observed tunability is understood as resulting from terahertz-field driven intraband kinetics of the Dirac fermions. Our study paves the way for exploiting nonlinear optical properties of Dirac matter for applications in signal processing and optical communications.

cond-mat.mtrl-sci↗

Nonequilibrium dynamics of $α$-RuCl$_{3}$ -- a time-resolved magneto-optical spectroscopy study

We present time-resolved magneto-optical spectroscopy on the magnetic Mott-Hubbard-insulating Kitaev spin liquid candidate $α$-RuCl$_3$ to investigate the nonequilibrium dynamics of its antiferromagnetically ordered zigzag groundstate after photoexcitation. A systematic study of the transient magnetic linear dichroism under different experimental conditions (temperature, external magnetic field, photoexcitation density) gives direct access to the dynamical interplay of charge excitations with the zigzag ordered state on ultrashort time scales. We observe a rather slow initial demagnetization (few to 10s of ps) followed by a long-lived non-thermal antiferromagnetic spin-disordered state (100$-$1000s of ps), which can be understood in terms of holons and doublons disordering the antiferromagnetic background after photoexcitation. Varying temperature and fluence in the presence of an external magnetic field reveals two distinct photoinduced dynamics associated with the zigzag and quantum paramagnetic disordered phases. The photo-induced non-thermal spin-disordered state shows universal compressed-exponential recovery dynamics related to the growth and propagation of zigzag domains on nanosecond time scales, which is interpreted within the framework of the Fatuzzo-Labrune model for magnetization reversal. The study of nonequilibrium states in strongly correlated materials is a relatively unexplored topic, but our results are expected to be extendable to a large class of Mott-Hubbard insulator materials with strong spin-orbit coupling.

cond-mat.str-el↗

Thickness and temperature dependence of the atomic-scale structure of SrRuO$_3$ thin films

Due to the strong lattice-property relationships which exist in complex oxide epitaxial layers, their electronic and magnetic properties can be modulated by structural distortions induced at the atomic scale. The modification and control can be affected at coherent heterointerfaces by epitaxial strain imposed by the substrate or by structural modifications to accommodate the film-substrate symmetry mismatch. Often these act in conjunction with a strong dependence on the layer thickness, especially for ultrathin layers. Moreover, as a result of these effects, the temperature dependence of the structure may deviate largely from that of the bulk. The temperature-dependent structure of 3 to 44 unit cell thick ferromagnetic SrRuO$_3$ films grown on Nb-doped SrTiO$_3$ substrates are investigated using a combination of high-resolution synchrotron X-ray diffraction and high-resolution electron microscopy. This aims to shed light on the intriguing magnetic and magnetotransport properties of epitaxial SRO layers, subjected to extensive investigations lately. The oxygen octahedral tilts and rotations are found to be strongly dependent on the temperature, the film thickness, and the distance away from the film-substrate interface. As a striking manifestation of the coupling between magnetic order and lattice structure, the Invar effect is observed below the ferromagnetic transition temperature in epitaxial layers as thin as 8 unit cells, similar to bulk ferromagnetic SrRuO$_3$.

cond-mat.mtrl-sci↗

Magnetic interlayer coupling between ferromagnetic SrRuO$_3$ layers through a SrIrO$_3$ spacer

A key element to tailor the properties of magnetic multilayers is the coupling between the individual magnetic layers. In case of skyrmion hosting multilayers, coupling of skyrmions across the magnetic layers is highly desirable. Here the magnetic interlayer coupling was studied in epitaxial all-oxide heterostructures of ferromagnetic perovskite SrRuO$_3$ layers separated by spacers of the strong spin-orbit coupling oxide SrIrO$_3$. This combination of oxide layers is being discussed as a potential candidate system to host Néel skyrmions. First order reversal curve (FORC) measurements were performed in order to distinguish between magnetic switching processes of the individual layers and to disentangle the signal of soft magnetic impurities from the samples$'$ signal. Additionally, FORC investigations enabled to determine whether the coupling between the magnetic layers is ferromagnetic or antiferromagnetic. The observed interlayer coupling strength was weak for all the heterostructures, with SrIrO$_3$ spacers between 2 monolayers and 12 monolayers thick.

cond-mat.mtrl-sci↗

Magneto-optical study of metamagnetic transitions in the antiferromagnetic phase of $α$-RuCl$_3$

$α$-RuCl$_3$ is a promising candidate material to realize the so far elusive quantum spin liquid ground state. However, at low temperatures, the coexistence of different exchange interactions couple the effective pseudospins into an antiferromagnetically zigzag (ZZ) ordered state. The low-field evolution of spin structure is still a matter of debate and the magnetic anisotropy within the honeycomb planes is an open and challenging question. Here, we investigate the evolution of the ZZ order parameter by second-order magneto-optical effects, the magnetic linear dichroism and magnetic linear birefringence. Our results clarify the presence and nature of metamagnetic transitions in the ZZ phase of $α$-RuCl$_3$. Our experimental observations show the presence of initial magnetic domain repopulation followed by a spin-flop transition for small in-plane applied magnetic fields ($\approx$ 1.6 T) along specific crystallographic directions. In addition, using a magneto-optical approach, we detected the recently reported emergence of a field-induced intermediate phase before suppressing the ZZ order. Our results disclose the details of various angle-dependent in-plane metamagnetic transitions quantifying the bond-anisotropic interactions present in $α$-RuCl$_3$

cond-mat.str-el↗

Band-selective third-harmonic generation in superconducting MgB$_2$: Possible evidence for Higgs amplitude mode in the dirty limit

We report on time-resolved linear and nonlinear terahertz spectroscopy of the two-band superconductor MgB$_2$ with the superconducting transition temperature $T_c \approx 36$ K. Third-harmonic generation (THG) is observed below $T_c$ by driving the system with intense narrowband THz pulses. For the pump-pulse frequencies $f=$ 0.3, 0.4, and 0.5 THz, temperature-dependent evolution of the THG signals exhibits a resonance maximum at the temperatures with the resonance conditions $2f=2Δ_π(T)$ fulfilled, for the dirty-limit superconducting gap $2Δ_π$. In contrast, for $f=$ 0.6 and 0.7 THz with $2f>2Δ_π(T\rightarrow0)=1.03$ THz, the THG intensity increases monotonically with decreasing temperature. Moreover, for $2f<2Δ_π(T\rightarrow0)$ the THG is found nearly isotropic with respect to the pump-pulse polarization. These results suggest a predominant contribution of the driven Higgs amplitude mode of the dirty-limit $π$-band superconducting gap, pointing to the importance of scattering for observation of the Higgs mode in superconductors.

cond-mat.supr-con↗

Relaxation dynamics of the optically driven nonequilibrium states in the electron- and hole-doped topological-insulator materials $(Bi_{1-x}Sb_{x})_{2}Te_{3}$

We report on time-resolved mid-infrared-pump terahertz-transmission-probe studies of the topological-insulator materials $(Bi_{1-x}Sb_{x})_{2}Te_{3}$, in which by varying x charge carriers are chemically tuned to be of n-type or p-type. Relaxation dynamics is found to be different in various aspects for transitions below or above the bandgap, which are selectively excited by changing the pump-pulse energy. For the below-bandgap excitation, an exponential decay of the pump-probe signals is observed, which exhibits linear dependence on the pump-pulse fluence. In contrast, the relaxation dynamics for the above-bandgap excitation is characterized by a compressed exponential decay and nonlinear fluence dependence at high pump flunences, which reflects interaction of the excited nonequilibrium states.

cond-mat.mtrl-sci↗