Universität Stuttgart

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    Direct electron beam patterning of electro-optically active PEDOT:PSS
    (2024) Doshi, Siddharth; Ludescher, Dominik; Karst, Julian; Floess, Moritz; Carlström, Johan; Li, Bohan; Mintz Hemed, Nofar; Duh, Yi-Shiou; Melosh, Nicholas A.; Hentschel, Mario; Brongersma, Mark; Giessen, Harald
    The optical and electronic tunability of the conductive polymer poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) has enabled emerging applications as diverse as bioelectronics, flexible electronics, and micro- and nano-photonics. High-resolution spatial patterning of PEDOT:PSS opens up opportunities for novel active devices in a range of fields. However, typical lithographic processes require tedious indirect patterning and dry etch processes, while solution-processing methods such as ink-jet printing have limited spatial resolution. Here, we report a method for direct write nano-patterning of commercially available PEDOT:PSS through electron-beam induced solubility modulation. The written structures are water stable and maintain the conductivity as well as electrochemical and optical properties of PEDOT:PSS, highlighting the broad utility of our method. We demonstrate the potential of our strategy by preparing prototypical nano-wire structures with feature sizes down to 250 nm, an order of magnitude finer than previously reported direct write methods, opening the possibility of writing chip-scale microelectronic and optical devices. We finally use the high-resolution writing capabilities to fabricate electrically-switchable optical diffraction gratings. We show active switching in this archetypal system with >95 % contrast at CMOS-compatible voltages of +2 V and -3 V, offering a route towards highly-miniaturized dynamic optoelectronic devices.
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    From two‐photon grayscale lithography to scalable replication : enabling complex aspherical micro‐optics for mass production
    (2025) Wagner, Stefan; Siegle, Leander; Haeusler, Stephan; Flad, Philipp; Hentschel, Mario; Guenther, Thomas; Zimmermann, André; Giessen, Harald
    The evolution of complex micro‐optics from prototyping to scalable manufacturing is a key challenge for modern imaging, sensing, and photonic systems. Two‐photon polymerization grayscale lithography (2GL) revolutionized the fabrication of micro‐optics by combining aspherical lenses with micro‐features enabling performance increases, weight reduction, aberration correction, and beam shaping. Its scalability for mass production, however, remains a key limitation. In this study, the replication and integration of 3D printed optics are demonstrated through electroplating and injection molding processes, enabling high‐volume production without sacrificing precision. Advancements in replicating complex micro‐optics fabricated via 2GL are presented by designing and 3D printing a diffractive, aspherical micro‐lens array. In relation to their size, these optics are almost impossible to produce with common techniques such as precision turning. The topography, beam profiles, and imaging quality of the 3D printed master are compared to the replicated lens array. By combining 2GL 3D printing and injection molding, micro‐optical mass production of arbitrary geometries is enabled. It is highlighted how this approach unlocks new opportunities for scalable production, addressing disparities between rapid prototyping and industrial manufacturing of micro‐optics.
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    Mass-producible micro-optical elements by injection compression molding and focused ion beam structured titanium molding tools
    (2020) Ristok, Simon; Roeder, Marcel; Thiele, Simon; Hentschel, Mario; Guenther, Thomas; Zimmermann, André; Herkommer, Alois; Giessen, Harald
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    Electron-driven photon sources for correlative electron-photon spectroscopy with electron microscopes
    (2020) Christopher, Joshua; Taleb, Masoud; Maity, Achyut; Hentschel, Mario; Giessen, Harald; Talebi, Nahid
    Electron beams in electron microscopes are efficient probes of optical near-fields, thanks to spectroscopy tools like electron energy-loss spectroscopy and cathodoluminescence spectroscopy. Nowadays, we can acquire multitudes of information about nanophotonic systems by applying space-resolved diffraction and time-resolved spectroscopy techniques. In addition, moving electrons interacting with metallic materials and optical gratings appear as coherent sources of radiation. A swift electron traversing metallic nanostructures induces polarization density waves in the form of electronic collective excitations, i.e., the so-called plasmon polariton. Propagating plasmon polariton waves normally do not contribute to the radiation; nevertheless, they diffract from natural and engineered defects and cause radiation. Additionally, electrons can emit coherent light waves due to transition radiation, diffraction radiation, and Smith-Purcell radiation. Some of the mechanisms of radiation from electron beams have so far been employed for designing tunable radiation sources, particularly in those energy ranges not easily accessible by the state-of-the-art laser technology, such as the THz regime. Here, we review various approaches for the design of coherent electron-driven photon sources. In particular, we introduce the theory and nanofabrication techniques and discuss the possibilities for designing and realizing electron-driven photon sources for on-demand radiation beam shaping in an ultrabroadband spectral range to be able to realize ultrafast few-photon sources. We also discuss our recent attempts for generating structured light from precisely fabricated nanostructures. Our outlook for the realization of a correlative electron-photon microscope/spectroscope, which utilizes the above-mentioned radiation sources, is also described.
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    Dynamic beam control based on electrically switchable nanogratings from conducting polymers
    (2023) Lee, Yohan; Karst, Julian; Ubl, Monika; Hentschel, Mario; Giessen, Harald
    Surging interests in point-of-device miniaturization have led to the development of metasurface-based optical components. Here, we demonstrate an electrically-driven ultracompact beam controller in the infrared spectral range. The effect benefits from diffraction gratings consisting of the commercially available conductive polymer PEDOT:PSS, which exhibits metal-to-insulator transition characteristics upon electrical biasing. By combining several metagratings with different superlattice periods in electrically isolated areas, our device enables diffraction beams at 16 and 33.5° when applying voltages of only ±1 V. Furthermore, no diffraction is realized by switching off the plasmonic property of the gratings. Dynamic control of electromagnetic wave via the presented platforms could be transformative for sensing, imaging, and communication applications.
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    Towards fiber-coupled plasmonic perfect absorber superconducting nanowire photodetectors for the near- and mid-infrared
    (2023) Mennle, Sandra; Karl, Philipp; Ubl, Monika; Ruchka, Pavel; Weber, Ksenia; Hentschel, Mario; Flad, Philipp; Giessen, Harald
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    Dielectric Mie voids : confining light in air
    (2023) Hentschel, Mario; Koshelev, Kirill; Sterl, Florian; Both, Steffen; Karst, Julian; Shamsafar, Lida; Weiss, Thomas; Kivshar, Yuri; Giessen, Harald
    Manipulating light on the nanoscale has become a central challenge in metadevices, resonant surfaces, nanoscale optical sensors, and many more, and it is largely based on resonant light confinement in dispersive and lossy metals and dielectrics. Here, we experimentally implement a novel strategy for dielectric nanophotonics: Resonant subwavelength localized confinement of light in air. We demonstrate that voids created in high-index dielectric host materials support localized resonant modes with exceptional optical properties. Due to the confinement in air, the modes do not suffer from the loss and dispersion of the dielectric host medium. We experimentally realize these resonant Mie voids by focused ion beam milling into bulk silicon wafers and experimentally demonstrate resonant light confinement down to the UV spectral range at 265 nm (4.68 eV). Furthermore, we utilize the bright, intense, and naturalistic colours for nanoscale colour printing. Mie voids will thus push the operation of functional high-index metasurfaces into the blue and UV spectral range. The combination of resonant dielectric Mie voids with dielectric nanoparticles will more than double the parameter space for the future design of metasurfaces and other micro- and nanoscale optical elements. In particular, this extension will enable novel antenna and structure designs which benefit from the full access to the modal field inside the void as well as the nearly free choice of the high-index material for novel sensing and active manipulation strategies.
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    Electrically switchable metallic polymer metasurface device with gel polymer electrolyte
    (2023) Jong, Derek de; Karst, Julian; Ludescher, Dominik; Floess, Moritz; Moell, Sophia; Dirnberger, Klaus; Hentschel, Mario; Ludwigs, Sabine; Braun, Paul V.; Giessen, Harald
    We present an electrically switchable, compact metasurface device based on the metallic polymer PEDOT:PSS in combination with a gel polymer electrolyte. Applying square-wave voltages, we can reversibly switch the PEDOT:PSS from dielectric to metallic. Using this concept, we demonstrate a compact, standalone, and CMOS compatible metadevice. It allows for electrically controlled ON and OFF switching of plasmonic resonances in the 2-3 µm wavelength range, as well as electrically controlled beam switching at angles up to 10°. Furthermore, switching frequencies of up to 10 Hz, with oxidation times as fast as 42 ms and reduction times of 57 ms, are demonstrated. Our work provides the basis towards solid state switchable metasurfaces, ultimately leading to submicrometer-pixel spatial light modulators and hence switchable holographic devices.
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    Tailored optical functionality by combining electron‐beam and focused gold‐ion beam lithography for solid and inverse coupled plasmonic nanostructures
    (2020) Hentschel, Mario; Karst, Julian; Giessen, Harald
    Plasmonics is a field uniquely driven by advances in micro‐ and nanofabrication. Many design ideas pose significant challenges in their experimental realization and test the limits of modern fabrication techniques. Here, the combination of electron‐beam and gold ion‐beam lithography is introduced as an alternative and highly versatile route for the fabrication of complex and high fidelity plasmonic nanostructures. The capability of this strategy is demonstrated on a selection of planar as well as 3D nanostructures. Large area and extremely accurate structures are presented with little to no defects and errors. These structures exhibit exceptional quality in shape fidelity and alignment precision. The combination of the two techniques makes full use of their complementary capabilities for the realization of complex plasmonic structures with superior optical properties and functionalities as well as ultra‐distinct spectral features which will find wide application in plasmonics, nanooptics, metasurfaces, plasmonic sensing, and similar areas.
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    Electro-active metaobjective from metalenses-on-demand
    (2022) Karst, Julian; Lee, Yohan; Floess, Moritz; Ubl, Monika; Ludwigs, Sabine; Hentschel, Mario; Giessen, Harald
    Switchable metasurfaces can actively control the functionality of integrated metadevices with high efficiency and on ultra-small length scales. Such metadevices include active lenses, dynamic diffractive optical elements, or switchable holograms. Especially, for applications in emerging technologies such as AR (augmented reality) and VR (virtual reality) devices, sophisticated metaoptics with unique functionalities are crucially important. In particular, metaoptics which can be switched electrically on or off will allow to change the routing, focusing, or functionality in general of miniaturized optical components on demand. Here, we demonstrate metalenses-on-demand made from metallic polymer plasmonic nanoantennas which are electrically switchable at CMOS (complementary metal-oxide-semiconductor) compatible voltages of ±1 V. The nanoantennas exhibit plasmonic resonances which can be reversibly switched ON and OFF via the applied voltage, utilizing the optical metal-to-insulator transition of the metallic polymer. Ultimately, we realize an electro-active non-volatile multi-functional metaobjective composed of two metalenses, whose unique optical states can be set on demand. Overall, our work opens up the possibility for a new level of electro-optical elements for ultra-compact photonic integration.