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Aljoscha Söll

Publications and source records attributed to Aljoscha Söll.

7 recordsLinked to original sources

Direct Nanoscale Pyroelectric Characterization of a CuInP${}_2$S${}_6$ van der Waals Nanogenerator

Pyroelectric energy conversion offers a route for harvesting time-dependent thermalfluctuations that are abundant in natural and technological environments. Twodimensional ferroelectrics are particularly attractive for this purpose because reduced dimensionality enables ultrathin, mechanically compliant device architectures. Here, we demonstrate direct nanoscale pyroelectric characterization of an out-of-plane van der Waals nanogenerator based on CuInP2S6 (CIPS) encapsulated between few-layer graphene electrodes. A scanning thermal microscopy (SThM) probe is employed as a localized nanoscale heat source while the electrically generated response is measured in situ through the device electrodes. Harmonic detection isolates the pyroelectric signal from parasitic first-harmonic electromechanical contributions, while finite-element thermal modeling combined with probe calibration enables direct determination of the local pyroelectric coefficient from the measured electrical response. Beyond quantitative characterization, the spatially resolved measurements directly identify electrically inactive regions associated with device defects, revealing local performance-limiting features that remain hidden in conventional spatially averaged pyroelectric measurements. The presented approach establishes a versatile platform for quantitative nanoscale pyroelectric characterization and the optimization of van der Waals pyroelectric devices.

cond-mat.mes-hall↗

Interplay of Cl Substitution and He$^{+}$ Irradiation in CrSBr$_{1-x}$Cl$_{x}$

Two-dimensional magnetic semiconductors provide a promising platform for exploring the interplay between disorder, lattice dynamics, and resonant light--matter interactions. Among them, CrSBr exhibits strong in-plane anisotropy and pronounced resonance-enhanced Raman scattering. Here, we investigate the effects of Cl substitution and He$^{+}$ irradiation on the vibrational response of CrSBr using polarization-resolved Raman spectroscopy. Cl substitution activates additional phonon modes associated with local symmetry breaking, while He$^{+}$ irradiation introduces distinct defect-related scattering channels and enhanced phonon broadening. The combined effects of alloy disorder and externally introduced defects lead to strong anisotropic reconstruction of the Raman spectra and modification of the nonlinear Raman response under near-resonant 1.96 eV excitation. Power-dependent measurements reveal robust superlinear scaling of both intrinsic and substitution-induced phonon modes, indicating persistent resonance-enhanced electron--phonon coupling even in defect-engineered samples.

cond-mat.mes-hall↗

Deep-Subwavelength and Broadband Quarter-Wave Retardation in Ultrathin Hyperbolic MoOCl2

The miniaturization of polarization-controlling optical components is one of the central pursuits in nanophotonics. While traditional anisotropic materials require large propagation lengths to achieve the desired phase shifts, metasurfaces mitigate this size constraint but often introduce narrow operational bandwidths and high fabrication complexities. To bridge this gap, we introduce MoOCl2 as a promising material for ultracompact and broadband phase retardation. Building on its giant optical anisotropy, we experimentally demonstrate MoOCl2 quarter-wave plates with thicknesses of 77 nm and 98 nm. These flakes exhibit achromatic quarter-wave retardation across broad visible (445 - 525 nm) and near-infrared (730 - 945 nm) spectral windows, surpassing the fundamental thickness and bandwidth limitations of both conventional optical materials and artificial nanostructures. Moreover, MoOCl2 waveplates demonstrate up to lambda/4500 retardance tolerance at central wavelengths. As a result, this study establishes MoOCl2 as a building block for ultracompact polarization optics.

physics.optics↗

Robust phonon engineering and symmetry-selective lattice dynamics in CrSBr$_{1-x}$Cl$_{x}$

Atomic substitution provides a controlled route to engineer lattice dynamics in low-symmetry two-dimensional materials. Here, by combining polarization-resolved Raman spectroscopy and first-principles calculations, we investigate the evolution of phonon characteristics in CrSBr$_{1-x}$Cl$_{x}$ ($0 \leq x \leq \sim 0.5$) upon partial substitution of Br with Cl atoms. Progressive Cl substitution of Br induces systematic shifts of parent CrSBr out-of-plane $A_\textrm{g}$ phonon modes and activates additional Raman features. These features persist across different polarization configurations and excitation energies, reflecting substitution-induced symmetry lowering and local lattice perturbations. Explicit supercell phonon calculations combined with Raman $Γ$-density-of-states simulations identify these features as symmetry-lowered descendants of parent modes arising from alloy disorder. Complementary strain-dependent calculations reveal that anisotropic lattice compression plays a key role in renormalizing Cr-S dominated phonons. Under near-resonant excitation, stimulated Raman scattering-like amplification remains observable with increasing Cl content, highlighting the resilience of anisotropic electron-phonon coupling in this system.

cond-mat.mtrl-sci↗

Anisotropic Phonon Dynamics and Directional Transport in Actinide van der Waals Semiconductor USe$_3$

Direction-dependent charge transport and optical responses are characteristic of van der Waals (vdW) materials with strong in-plane anisotropy. While transition-metal trichalcogenides (TMTCs) exemplify this behavior, heavier analogs remain largely unexplored. In this study we examine USe$_3$ as an anisotropic vdW material and a heavier analog of the well-studied TMTCs. We reveal strong in-plane anisotropy using polarization-resolved Raman spectroscopy, investigate strain-induced shifts of phonon modes, and quantify direction-dependent charge-carrier mobility through transport measurements on field-effect devices. First-principles calculations based on density-functional theory corroborate our findings, providing a theoretical basis for our experimental observations. Casting USe$_3$ as an actinide analog of a TMTC establishes a platform for exploring low-dimensional semiconductors that combine strong in-plane anisotropy with f-electron physics.

cond-mat.mtrl-sci↗

Lithium Intercalation in the Anisotropic van der Waals Magnetic Semiconductor CrSBr

Alkali metal intercalation is an important strategy for doping van der Waals materials. Lithium, in particular, was shown to achieve exceptional charge carrier densities, reaching levels at which fundamental electrical, optical, and magnetic material properties begin to be strongly modified. While lithium is known to be highly volatile, its migration dynamics in anisotropic layered crystals remain poorly understood. In this work, we investigate the intercalation of lithium in-between layers of the anisotropic magnetic semiconductor CrSBr. Using exfoliated crystals, we are able to monitor the dynamics of the intercalation process in real time through optical and electrical characterization methods. Our measurements reveal highly anisotropic migration of Lithium characterized by diffusion coefficients that differ by more than one order of magnitude along a- and b-directions. This finding is in good agreement with our molecular dynamics simulations which show trajectories of lithium atoms primarily follow the Br-chains in the a-direction. Beyond that, we find that partially covering CrSBr crystals by thin hexagonal boron nitride (hBN) flakes has a significant impact on the intercalation process, and that lithium strongly enhances the electrical conductivity along the a-axis. Our method offers a new platform for lithium diffusion studies and encourages further research to pursue the fabrication of lithium-doped devices.

cond-mat.mtrl-sci↗

Strong Exciton-Phonon Coupling as a Fingerprint of Magnetic Ordering in van der Waals Layered CrSBr

The layered, air-stable van der Waals antiferromagnetic compound CrSBr exhibits pronounced coupling between its optical, electronic, and magnetic properties. As an example, exciton dynamics can be significantly influenced by lattice vibrations through exciton-phonon coupling. Using low-temperature photoluminescence spectroscopy, we demonstrate the effective coupling between excitons and phonons in nanometer-thick CrSBr. By careful analysis, we identify that the satellite peaks predominantly arise from the interaction between the exciton and an optical phonon with a frequency of 118 cm-1 (~14.6 meV) due to the out-of-plane vibration of Br atoms. Power-dependent and temperature-dependent photoluminescence measurements support exciton-phonon coupling and indicate a coupling between magnetic and optical properties, suggesting the possibility of carrier localization in the material. The presence of strong coupling between the exciton and the lattice may have important implications for the design of light-matter interactions in magnetic semiconductors and provides new insights into the exciton dynamics in CrSBr. This highlights the potential for exploiting exciton-phonon coupling to control the optical properties of layered antiferromagnetic materials.

cond-mat.mtrl-sci↗