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Marco Gruenewald

Publications and source records attributed to Marco Gruenewald.

5 recordsLinked to original sources

Tuning of Photoexcited Electron Dynamics at Monolayer h-BN/Metal Interfaces by Corrugation

Atomic-scale corrugation in two-dimensional materials can modify interfacial electronic coupling, yet its influence on ultrafast carrier relaxation remains poorly established. Here, we compare image potential states (IPS) at monolayer h-BN/Ir(111) and h-BN/Pt(111) interfaces using structural characterization and time-resolved two-photon photoemission spectroscopy. Consistent with literature, h-BN is strongly corrugated on Ir(111) but comparatively flat on Pt(111). The first (n = 1) and second (n = 2) IPS appears at similar energies on both substrates, whereas their relaxation dynamics differ markedly. On h-BN/Ir(111), the IPS decay is response-limited (<20 fs), while h-BN/Pt(111) exhibits lifetimes of 56 fs (n = 1) and 75 fs (n = 2). The lifetime contrast is most consistently explained by corrugation-enhanced overlap of the IPS wavefunction with the metal substrate, which accelerates electron decay. These results indicate that atomic-scale corrugation is an effective physical parameter for tuning ultrafast electron dynamics at two-dimensional material and metal interfaces.

cond-mat.mtrl-sci

Bottom-up realization of a type-II organic-TMD heterointerface: Pentacene on monolayer WS2

Stacked van der Waals heterostructures based on transition metal dichalcogenides (TMDs) exhibit a rich variety of exotic interfacial phenomena. Substituting one component with an organic semiconductor (OSC) enables the design of hybrid heterostructures with tunable functionalities for optoelectronic, photovoltaic, and spintronic applications. In this work, exploiting scanning tunneling spectroscopy (STS), photoemission orbital tomography (POT) and G0W0 electronic structure calculations, we experimentally and theoretically demonstrate the self-assembly of an ordered single layer of pentacene (5A) above monolayer WS2, exhibiting a type-II (staggered) band alignment in the hybrid 5A/WS2 interface. Central to this result is the synthesis of extended, atomically flat WS2 - an essential prerequisite for a highly ordered and electronically homogeneous OSC/TMD interface - which can only be reliably achieved via bottom-up growth, most notably molecular beam epitaxy (MBE). We realize this by leveraging Au(111) as an atomically clean and conductive sample for epitaxial growth - a necessary requirement for reliable and comparable STS/POT characterizations. The high quality of the synthesized heterostructure, together with its type-II band alignment, establishes pentacene/WS2 as a model system for orbital-resolved studies of charge transfer, energy-level renormalization, and non-equilibrium interfacial processes in hybrid organic-inorganic-2D heterostructures.

cond-mat.mtrl-sci

Lifshitz Transition and Band Structure Evolution in Alkali Metal Intercalated 1Tprime-MoTe2

In van der Waals materials, coupling between adjacent layers is weak, and consequently interlayer interactions are weakly screened. This opens the possibility to profoundly modify the electronic structure, e.g., by applying electric fields or with adsorbates. Here, we show for the case of the topologically trivial semimetal 1Tprime-MoTe2 that potassium dosing at room temperature significantly transforms its band structure. With a combination of angle-resolved photoemission spectroscopy, scanning tunneling microscopy, x-ray photoemission spectroscopy, and density functional theory we show that i) for small concentrations of K, 1Tprime-MoTe2 undergoes a Lifshitz transition with the electronic structure shifting rigidly, and ii) for larger K concentrations 1Tprime-MoTe2 undergoes significant band structure transformation. Our results demonstrate that the origin of this electronic structure change stems from alkali metal intercalation.

cond-mat.mtrl-sci

Atomically Thin Metal-Dielectric Heterostructures by Atomic Layer Deposition

Heterostructures increasingly attracted attention over the past several years to enable various optoelectronic and photonic applications. In this work, atomically thin interfaces of Ir/Al2O3 heterostructures compatible with micro-optoelectronic technologies are reported. Their structural and optical properties were determined by spectroscopic and microscopic techniques (XRR, XPS, HRTEM, spectroscopic ellipsometry, and UV/VIS/NIR spectrophotometry). The XRR and HRTEM analyses reveal a layer-by-layer growth mechanism of Ir in atomic scale heterostructures, which is different from the typical island-type growth of metals on dielectrics. Alongside, XPS investigations imply the formation of Ir-O-Al bonding at the interfaces for lower Ir concentrations, in contrast to the nanoparticle core-shell structure formation. Precisely tuning the ratio of the constituents ensures the control of the dispersion profile along with a transition from effective dielectric to metallic heterostructures. The Ir coating thickness was varied ranging from a few Å to films of about 7 nm in the heterostructures. The transition has been observed in the structures containing individual Ir coating thicknesses of about 2-4 nm. Following this, show epsilon-near-zero metamaterials with tunable dielectric constants by precisely varying the composition of such heterostructures. Overall, a comprehensive study on structural and optical properties of the metal-dielectric interface of Ir/Al2O3 heterostructures was addressed indicating an extension of the material portfolio available for optical system design.

physics.app-ph

Tuning exciton recombination rates in doped transition metaldichalcogenides

Monolayer transition metal dichalcogenides (TMDs) are direct gap semiconductors that hold great promise for advanced applications in photonics and optoelectronics. Understanding the interplay between their radiative and non-radiative recombination pathways is thus of crucial importance not only for fundamental studies but also for the design of future nanoscale on-chip devices. Here, we investigate the interplay between doping and exciton-exciton annihilation (EEA) and their impact on the photoluminescence quantum yield in different TMD samples and related heterostructures. We demonstrate that the EEA threshold increases in highly doped samples, where the radiative and non-radiative recombination of trions dominates.

cond-mat.mes-hall