arXiv subjects

Alexander Högele

Publications and source records attributed to Alexander Högele.

At least 19 recordsLinked to original sources

arXiv2026

Insights into the Nature of Quantum Emitters in Electron-Irradiated hexagonal Boron Nitride

Quantum emitters in hexagonal boron nitride (hBN) have emerged as a promising solid-state platform for quantum technology applications. However, a persistent challenge in the field is the unclear origin of many observed emission lines, particularly in the visible range, which can be difficult to distinguish from signals arising from organic or process-induced contamination during sample preparations and handling. This ambiguity limits both the reproducibility of emitter generation and the reliable identification of truly intrinsic quantum defects. This work provides a step-by-step framework to assess whether quantum emitters in electron-irradiated hBN are associated with organic contaminants introduced during sample preparation. We employ hyperspectral imaging, thermal annealing, and oxygen plasma etching to investigate the origin of the green-yellow emitters in electron-irradiated hBN. The combined results not only rule out organic contamination as the source of emission but also provide insight into the spectral variability, thermal stability, and vertical localization of the emitters generated in electron-irradiated hBN that was created without any pre- or post-processing. In addition, our experiments demonstrate the feasibility of creating stable emitters in hBN with thicknesses below 10 nm. These findings provide practical guidance for the identification and controlled implementation of hBN-based single-photon emitters in quantum photonic devices.

physics.optics↗

arXiv2026

Charge Tunable Optical Nonlinearity of Moiré Exciton-Polaritons

Transition metal dichalcogenides represent a versatile platform to study strong light-matter interactions based on excitons and electrons in ordered lattices. Twist-engineering of moiré structures further enables the manipulation of the polaritonic nonlinearities via engineering the exciton landscape on the nanoscale. In this work, we demonstrate in-situ control of the optical saturation-based nonlinearity of moiré exciton-polaritons by phase space restriction via charge doping. Strong exciton-photon coupling is established in a gate-controllable MoTe$_2$-MoSe$_2$ heterobilayer, embedded in a spectrally-tunable open cavity. A small gate voltage can effectively lower the necessary polariton density by one order of magnitude to achieve a similar nonlinear saturation effect as in the charge-neutral case. Our microscopic description successfully explains the observed phenomena in the framework of Pauli blocking for the moiré superlattices with charge preoccupation.

cond-mat.mes-hall↗

arXiv2026

Optical switching of magnetic order in few-layer CrSBr

Manipulating magnetism with light is crucial for both fundamental understanding and technological advancements of information storage devices. The layered antiferromagnet CrSBr, part of the recently emerging class of two-dimensional van der Waals magnets, offers a unique path towards optical control of magnetism via magneto-excitons, which allow optical readout of the spin alignment and also provide a strong absorption channel. Here, we use exciton absorption and photoluminescence to demonstrate optical switching of the magnetic order in bi- and trilayer CrSBr. Using a continuous-wave laser with a power as low as a few microwatts at near-critical external magnetic fields, we demonstrate both local and remote switching of the magnetic configuration in extended lateral domains and further employ this mechanism to deterministically prepare the zero-field magnetic configuration. Our results establish optical switching as a useful means of controlling magnetism in CrSBr, with potential applications in magneto-optoelectronic devices.

cond-mat.mes-hall↗

arXiv2026

Optimizing strong light-matter coupling of plasmonic lattices and monolayer semiconductors

Exciton-polaritons provide a versatile platform for the study of a wide range of phenomena, including polariton lasers, topological polaritons, and bosonic condensation. Transition metal dichalcogenide monolayers host excitons with large oscillator strength and binding energies constituting a robust matter constituent that forms polaritons from cryogenic to room temperature when embedded in optical microcavities. Plasmonic nanoparticles arranged in lattice geometries offer strong field-confinement and high quality factors. However, the high sensitivity of monolayer excitons to strain and dielectric disorder necessitates encapsulation in atomically flat hBN to ensure a high optical quality, rendering plasmonics more challenging. Here, we employ our recently developed fabrication method for embedding gold nanodisk arrays into van der Waals heterostructures and compare two samples with opposite layer order. We observe that strain and etching-induced surface contamination can reduce the exciton quality and thus the light-matter interaction strength significantly. Our fabrication approach reduces interfacial irregularities and enables homogeneous large-area polariton lattices for a wide range of applications, such as polarization-control or topological polaritonics.

cond-mat.mes-hall↗

arXiv2025

Cavity-mediated exciton hopping in a dielectrically engineered polariton system

Exciton-polaritons - coherently hybridized states of excitons and photons - are instrumental for solid-state nonlinear optics and quantum simulations. To enable engineered polariton energy landscapes and interactions, local control over the particle-like states can be achieved by tuning the properties of the exciton constituent. Monolayer transition metal dichalcogenides stand out in this respect, as they readily allow for a deterministic, flexible and scalable control of excitons, and thus of hybrid exciton-polaritons, via environmental dielectric engineering. Here, we demonstrate the realization of mesoscopic exciton-polariton domains in a structured dielectric exciton environment, and establish an effective long-range exciton hopping in the dispersive regime of cavity-coupling. Our results represent a crucial step toward interacting polaritonic networks and quantum simulations in exciton-polariton lattices based on dielectrically tailored two-dimensional semiconductors.

cond-mat.mes-hall↗

arXiv2025

Deterministic and Scalable Quantum Light Generation in DNA Origami-Programmed Organic Molecule-MoS$_2$ Monolayer Hybrids

The functionalization of atomically-thin transition metal dichalcogenides (TMDs) with organic molecules is a promising approach for realizing nanoscale optoelectronic devices with tailored functionalities, such as quantum light generation or p-n junctions. However, achieving precise control over the molecules' positioning on the 2D material remains a significant challenge. Here, we overcome the limitations of solution- and vapor-deposition methods and use a DNA origami placement technique to spatially arrange thiol molecules on a chip surface at the single-molecule level with high assembly yields. We successfully integrated MoS$_2$ monolayers with micron-scale thiol-origami patterns, achieving single-photon emission from thiol-induced localized excitons in MoS$_2$. Our work lays a foundation for the chemical control of quantum emitters in atomically-thin semiconductors and enables the design and production of ultracompact 2D devices for quantum technologies.

cond-mat.mes-hall↗

arXiv2025

Control of atomic reconstruction and quasi-1D excitons in strain-engineered moiré heterostructures

In two-dimensional nearly commensurate heterostructures, strain plays a critical role in shaping electronic behavior. While previous studies have focused on random strain introduced during fabrication, achieving controlled structural design has remained challenging. Here, we demonstrate the deterministic creation of one-dimensional arrays from initially zero-dimensional triangular moiré patterns in MoSe$_2$-WSe$_2$ heterobilayers. This transformation, driven by the interplay of uniaxial strain and atomic reconstruction, results in one-dimensional confinement of interlayer excitons within domain walls, exhibiting near-unity linearly polarized emission related to the confinement-induced symmetry breaking. The width of the domain walls--and consequently the degree of exciton confinement--can be precisely tuned by the interlayer twist angle. By applying out-of-plane electric field, the confined excitons exhibit energy shifts exceeding 100~meV and changes in the fine-structure splitting by up to a factor of two. Our work demonstrates the potential of strain engineering for constructing designer moiré systems with programmable quantum properties, paving the way for future optoelectronic applications.

cond-mat.mes-hall↗

arXiv2024

Doping-control of excitons and magnetism in few-layer CrSBr

Magnetism in two-dimensional materials reveals phenomena distinct from bulk magnetic crystals, with sensitivity to charge doping and electric fields in monolayer and bilayer van der Waals magnet CrI3. Within the class of layered magnets, semiconducting CrSBr stands out by featuring stability under ambient conditions, correlating excitons with magnetic order and thus providing strong magnon-exciton coupling, and exhibiting peculiar magneto-optics of exciton-polaritons. Here, we demonstrate that both exciton and magnetic transitions in bilayer and trilayer CrSBr are sensitive to voltage-controlled field-effect charging, exhibiting bound exciton-charge complexes and doping-induced metamagnetic transitions. Moreover, we demonstrate how these unique properties enable optical probes of local magnetic order, visualizing magnetic domains of competing phases across metamagnetic transitions induced by magnetic field or electrostatic doping. Our work identifies few-layer CrSBr as a rich platform for exploring collaborative effects of charge, optical excitations, and magnetism.

cond-mat.mes-hall↗

arXiv2024

Correlated magnetism of moiré exciton-polaritons on a triangular electron-spin lattice

We demonstrate evidence of correlated magnetism for exciton-polaritons in a MoSe$_{2}$/WS$_{2}$ moiré heterostructure with near-parallel alignment subject to electron doping. In our experiments, interactions between electrons and moiré excitons are controlled electrostatically by field-effect doping, and the polaritonic regime of strong light-matter coupling is established in an open cryogenic microcavity. Remarkably, at filling fractions around one electron per moiré cell, we observe drastic and nonlinear enhancement of the effective polariton Landé factor as a hallmark of correlated magnetism, which is cavity-controlled via resonance tuning of light and matter polariton constituents. Our work establishes moiré van der Waals heterostructures as an outstanding platform for studies of correlated phenomena in the presence of strong light-matter coupling and many-body phases of lattice-ordered excitons, charges and spins.

cond-mat.mes-hall↗

arXiv2024

Cavity-enhanced photon indistinguishability at room temperature and telecom wavelengths

Indistinguishable single photons in the telecom-bandwidth of optical fibers are indispensable for long-distance quantum communication. Solid-state single photon emitters have achieved excellent performance in key benchmarks, however, the demonstration of indistinguishability at room-temperature remains a major challenge. Here, we report room-temperature photon indistinguishability at telecom wavelengths from individual nanotube defects in a fiber-based microcavity operated in the regime of incoherent good cavity-coupling. The efficiency of the coupled system outperforms spectral or temporal filtering, and the photon indistinguishability is increased by more than two orders of magnitude compared to the free-space limit. Our results highlight a promising strategy to attain optimized non-classical light sources.

cond-mat.mes-hall↗

arXiv2024

Metasurface of strongly coupled excitons and nanoplasmonic arrays

Metasurfaces allow to manipulate light at the nanoscale. Integrating metasurfaces with transition metal dichalcogenide monolayers provides additional functionality to ultrathin optics, including tunable optical properties with enhanced light-matter interactions. In this work, we demonstrate the realization of a polaritonic metasurface utilizing the sizable light-matter coupling of excitons in monolayer WSe2 and the collective lattice resonances of nanoplasmonic gold arrays. To this end, we developed a novel fabrication method to integrate gold nanodisk arrays in hexagonal boron nitride and thus simultaneously ensure spectrally narrow exciton transitions and their immediate proximity to the near-field of array surface lattice resonances. In the regime of strong light-matter coupling, the resulting van der Waals metasurface exhibits all key characteristics of lattice polaritons, with a directional and linearly-polarized far-field emission profile dictated by the underlying nanoplasmonic lattice. Our work can be straightforwardly adapted to other lattice geometries, establishing structured van der Waals metasurfaces as means to engineer polaritonic lattices.

physics.optics↗

arXiv2024

Hybrid moiré excitons and trions in twisted MoTe$_2$-MoSe$_2$ heterobilayers

We report experimental and theoretical studies of MoTe$_2$-MoSe$_2$ heterobilayers with rigid moiré superlattices controlled by the twist angle. Using an effective continuum model that combines resonant interlayer electron tunneling with stacking-dependent moiré potentials, we identify the nature of moiré excitons and the dependence of their energies, oscillator strengths and Landé $g$-factors on the twist angle. Within the same framework, we interpret distinct signatures of bound complexes among electrons and moiré excitons in nearly collinear heterostacks. Our work provides fundamental understanding of hybrid moiré excitons and trions in MoTe$_2$-MoSe$_2$ heterobilayers, and establishes the material system as a prime candidate for optical studies of correlated phenomena in moiré lattices.

cond-mat.mes-hall↗

arXiv2024

Implementation of the bilayer Hubbard model in a moiré heterostructure

Moiré materials provide a unique platform for studies of correlated many-body physics of the Fermi-Hubbard model on triangular spin-charge lattices. Bilayer Hubbard models are of particular significance with regard to the physics of Mott insulating states and their relation to unconventional superconductivity, yet their experimental implementation in moiré systems has so far remained elusive. Here, we demonstrate the realization of a staggered bilayer triangular lattice of electrons in an antiparallel MoSe$_{2}$/WS$_{2}$ heterostructure. The bilayer lattice emerges due to strong electron confinement in the moiré potential minima and the near-resonant alignment of conduction band edges in MoSe$_{2}$ and WS$_{2}$. As a result, charge filling proceeds layer-by-layer, with the first and second electron per moiré cell consecutively occupying first the MoSe$_{2}$ and then the WS$_{2}$ layer. We describe the observed charging sequence by an electrostatic model and provide experimental evidence of spin correlations on the vertically offset and laterally staggered bilayer lattice, yielding absolute exciton Landé factors as high as $600$ at lowest temperatures. The bilayer character of the implemented spin-charge lattice allows for electrostatic tunability of Ruderman-Kittel-Kasuya-Yosida magnetism, and establishes antiparallel MoSe$_{2}$/WS$_{2}$ heterostructures as a viable platform for studies of bilayer Hubbard model physics with exotic magnetic phases on frustrated lattices.

cond-mat.str-el↗

arXiv2024

Field-induced hybridization of moiré excitons in MoSe$_2$/WS$_2$ heterobilayers

We study experimentally and theoretically the hybridization among intralayer and interlayer moiré excitons in a MoSe$_2$/WS$_2$ heterostructure with antiparallel alignment. Using a dual-gate device and cryogenic white light reflectance and narrow-band laser modulation spectroscopy, we subject the moiré excitons in the MoSe$_2$/WS$_2$ heterostack to a perpendicular electric field, monitor the field-induced dispersion and hybridization of intralayer and interlayer moiré exciton states, and induce a cross-over from type I to type II band alignment. Moreover, we employ perpendicular magnetic fields to map out the dependence of the corresponding exciton Landé $g$-factors on the electric field. Finally, we develop an effective theoretical model combining resonant and non-resonant contributions to moiré potentials to explain the observed phenomenology, and highlight the relevance of interlayer coupling for structures with close energetic band alignment as in MoSe$_2$/WS$_2$.

cond-mat.mes-hall↗

arXiv2023

Exciton-exciton interactions in van der Waals heterobilayers

Exciton-exciton interactions are key to understanding non-linear optical and transport phenomena in van der Waals heterobilayers, which emerged as versatile platforms to study correlated electronic states. We present a combined theory-experiment study of excitonic many-body effects based on first-principle band structures and Coulomb interaction matrix elements. Key to our approach is the explicit treatment of the fermionic substructure of excitons and dynamical screening effects for density-induced energy renormalization and dissipation. We demonstrate that dipolar blue shifts are almost perfectly compensated by many-body effects, mainly by screening-induced self-energy corrections. Moreover, we identify a crossover between attractive and repulsive behavior at elevated exciton densities. Theoretical findings are supported by experimental studies of spectrally-narrow interlayer excitons in atomically-reconstructed, hBN-encapsulated MoSe$_2$/WSe$_2$ heterobilayers. Both theory and experiment show energy renormalization on a scale of a few meV even for high injection densities in the vicinity of the Mott transition. Our results revise the established picture of dipolar repulsion dominating exciton-exciton interactions in van der Waals heterostructures and open up opportunities for their external design.

cond-mat.mes-hall↗

arXiv2023

Non-linear and negative effective diffusivity of optical excitations in moiré-free heterobilayers

Interlayer exciton diffusion is studied in atomically-reconstructed MoSe2/WSe2 heterobilayers with suppressed disorder. Local atomic registry is confirmed by characteristic optical absorption, circularly-polarized photoluminescence, and g-factor measurements. Using transient microscopy we observe propagation properties of interlayer excitons that are independent from trapping at moiré- or disorder-induced local potentials. Confirmed by characteristic temperature dependence for free particles, linear diffusion coefficients of interlayer excitons at liquid helium temperature and low excitation densities are almost 1000 times higher than in previous observations. We further show that exciton-exciton repulsion and annihilation contribute nearly equally to non-linear propagation by disentangling the two processes in the experiment and simulations. Finally, we demonstrate effective shrinking of the light-emission over time across several 100's of picoseconds at the transition from exciton- to the plasma-dominated regimes. Supported by microscopic calculations for bandgap renormalization to identify Mott threshold, this indicates transient crossing between rapidly expanding, short-lived electron-hole plasma and slower, long-lived exciton populations.

cond-mat.mes-hall↗

arXiv2023

Imaging lattice reconstruction in homobilayers and heterobilayers of transition metal dichalcogenides

Moiré interference effects have profound impact on the optoelectronic properties of vertical van der Waals structures. Here we establish secondary electron imaging in a scanning electron microscope as a powerful technique for visualizing registry-specific domains in vertical bilayers of transition metal dichalcogenides with common moiré phenomena. With optimal parameters for contrast-maximizing imaging of high-symmetry registries, we identify distinct crystal realizations of WSe$_2$ homobilayers and MoSe$_2$-WSe$_2$ heterobilayers synthesized by chemical vapor deposition, and demonstrate ubiquitous lattice reconstruction in stacking-assembled bilayers with near parallel and antiparallel alignment. Our results have immediate implications for the optical properties of registry-specific excitons in layered stacks of transition metal dichalcogenides, and demonstrate the general potential of secondary electron imaging for van der Waals twistronics.

cond-mat.mes-hall↗

arXiv2023

Lattice reconstruction in MoSe$_2$-WSe$_2$ heterobilayers synthesized by chemical vapor deposition

Vertical van der Waals heterostructures of semiconducting transition metal dichalcogenides realize moiré systems with rich correlated electron phases and moiré exciton phenomena. For material combinations with small lattice mismatch and twist angles as in MoSe$_2$-WSe$_2$, however, lattice reconstruction eliminates the canonical moiré pattern and instead gives rise to arrays of periodically reconstructed nanoscale domains and mesoscopically extended areas of one atomic registry. Here, we elucidate the role of atomic reconstruction in MoSe$_2$-WSe$_2$ heterostructures synthesized by chemical vapor deposition. With complementary imaging down to the atomic scale, simulations, and optical spectroscopy methods we identify the coexistence of moiré-type cores and extended moiré-free regions in heterostacks with parallel and antiparallel alignment. Our work highlights the potential of chemical vapor deposition for applications requiring laterally extended heterosystems of one atomic registry or exciton-confining heterostack arrays.

cond-mat.mes-hall↗