Universität Stuttgart

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    Tailored nanocomposites for 3D printed micro-optics
    (2020) Weber, Ksenia; Werdehausen, Daniel; König, Peter; Thiele, Simon; Schmid, Michael; Decker, Manuel; Oliveira, Peter William de; Herkommer, Alois; Giessen, Harald
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    Nearly diffraction limited FTIR mapping using an ultrastable broadband femtosecond laser tunable from 1.33 to 8 µm
    (2017) Mörz, Florian; Semenyshyn, Rostyslav; Steinle, Tobias; Neubrech, Frank; Zschieschang, Ute; Klauk, Hagen; Steinmann, Andy; Giessen, Harald
    Micro-Fourier-transform infrared (FTIR) spectroscopy is a widespread technique that enables broadband measurements of infrared active molecular vibrations at high sensitivity. SiC globars are often applied as light sources in tabletop systems, typically covering a spectral range from about 1 to 20 µm (10 000 - 500 cm−1) in FTIR spectrometers. However, measuring sample areas below 40x40 µm2 requires very long integration times due to their inherently low brilliance. This hampers the detection of ultrasmall samples, such as minute amounts of molecules or single nanoparticles. In this publication we extend the current limits of FTIR spectroscopy in terms of measurable sample areas, detection limit and speed by utilizing a broadband, tabletop laser system with MHz repetition rate and femtosecond pulse duration that covers the spectral region between 1250 - 7520 cm−1 (1.33 - 8 µm). We demonstrate mapping of a 150x150 µm2 sample of 100 nm thick molecule layers at 1430 cm−1 (7 µm) with 10x10 µm2 spatial resolution and a scan speed of 3.5 µm/sec. Compared to a similar globar measurement an order of magnitude lower noise is achieved, due to an excellent long-term wavelength and power stability, as well as an orders of magnitude higher brilliance.
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    3D direct laser writing of highly absorptive photoresist for miniature optical apertures
    (2022) Schmid, Michael D.; Toulouse, Andrea; Thiele, Simon; Mangold, Simon; Herkommer, Alois; Giessen, Harald
    The importance of 3D direct laser writing as an enabling technology increased rapidly in recent years. Complex micro-optics and optical devices with various functionalities are now feasible. Different possibilities to increase the optical performance are demonstrated, for example, multi-lens objectives, a combination of different photoresists, or diffractive optical elements. It is still challenging to create fitting apertures for these micro optics. In this work, a novel and simple way to create 3D-printed opaque structures with a highly absorptive photoresist is introduced, which can be used to fabricate microscopic apertures increasing the contrast of 3D-printed micro optics and enabling new optical designs. Both hybrid printing by combining clear and opaque resists, as well as printing transparent optical elements and their surrounding opaque apertures solely from a single black resist by using different printing thicknesses are demonstrated.
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    Ultrathin monolithic 3D printed optical coherence tomography endoscopy for preclinical and clinical use
    (2020) Li, Jiawen; Thiele, Simon; Quirk, Bryden C.; Kirk, Rodney W.; Verjans, Johan W.; Akers, Emma; Bursill, Christina A.; Nicholls, Stephen J.; Herkommer, Alois; Giessen, Harald; McLaughlin, Robert A.
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    3D printed micro-optics for quantum technology: Optimised coupling of single quantum dot emission into a single-mode fibre
    (2021) Sartison, Marc; Weber, Ksenia; Thiele, Simon; Bremer, Lucas; Fischbach, Sarah; Herzog, Thomas; Kolatschek, Sascha; Jetter, Michael; Reitzenstein, Stephan; Herkommer, Alois; Michler, Peter; Portalupi, Simone Luca; Giessen, Harald
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    Short-range surface plasmonics: localized electron emission dynamics from a 60-nm spot on an atomically flat single-crystalline gold surface
    (2017) Frank, Bettina; Kahl, Philip; Podbiel, Daniel; Spektor, Grisha; Orenstein, Meir; Fu, Liwei; Weiss, Thomas; Horn-von Hoegen, Michael; Davis, Timothy J.; Meyer zu Heringdorf, Frank-Joachim; Giessen, Harald
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    Momentum space separation of quantum path interferences between photons and surface plasmon polaritons in nonlinear photoemission microscopy
    (2024) Dreher, Pascal; Janoschka, David; Giessen, Harald; Schützhold, Ralf; Davis, Timothy J.; Horn-von Hoegen, Michael; Meyer zu Heringdorf, Frank-Joachim
    Quantum path interferences occur whenever multiple equivalent and coherent transitions result in a common final state. Such interferences strongly modify the probability of a particle to be found in that final state, a key concept of quantum coherent control. When multiple nonlinear and energy-degenerate transitions occur in a system, the multitude of possible quantum path interferences is hard to disentangle experimentally. Here, we analyze quantum path interferences during the nonlinear emission of electrons from hybrid plasmonic and photonic fields using time-resolved photoemission electron microscopy. We experimentally distinguish quantum path interferences by exploiting the momentum difference between photons and plasmons and through balancing the relative contributions of their respective fields. Our work provides a fundamental understanding of the nonlinear photon-plasmon-electron interaction. Distinguishing emission processes in momentum space, as introduced here, could allow nano-optical quantum-correlations to be studied without destroying the quantum path interferences.
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    Quantitative determination of the electric field strength in a plasmon focus from ponderomotive energy shifts
    (2022) Dreher, Pascal; Janoschka, David; Neuhaus, Alexander; Frank, Bettina; Giessen, Harald; Horn-von Hoegen, Michael; Meyer zu Heringdorf, Frank-Joachim
    Spectroscopic photoemission microscopy is used to detect and quantify a ponderomotive shift in the energy of electrons that are emitted from a surface plasmon polariton focus. The focus is formed on an atomically flat Au(111) surface by an Archimedean spiral and is spatiotemporally separated from the circularly polarized light pulse used to excite the spiral. A spectroscopic analysis of electrons emitted from the focus exhibits a peaked above-threshold electron emission spectrum. From the shift of the peaks as function of laser power the field strength of the surface plasmon polariton was quantitatively determined without free parameters. Estimations of the Keldysh parameter γ = 4.4 and the adiabaticity parameter δ = 4700 indicate that electron emission occurs in a regime of multiplasmon absorption and nonlocalized surface plasmon fields.
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    Focused surface plasmon polaritons coherently couple to electronic states in above-threshold electron emission
    (2023) Dreher, Pascal; Janoschka, David; Frank, Bettina; Giessen, Harald; Meyer zu Heringdorf, Frank-Joachim
    When an intense light field strongly interacts with the band structure of a solid, the formation of hybrid light-matter quantum states becomes possible. Examples of such Floquet-Bloch states have been reported, but engineering of the band structure using Floquet states can suffer from dissipation and decoherence. Sustaining the necessary quantum coherence of the light-matter interactions requires robust electronic states in combination with strong fields of suitable polarization and frequency. Here, we explore the quantum coherent coupling of nano-focused surface plasmon polaritons (SPP) to distinct electronic states in the band structure of a solid. We observe above-threshold electron emission from the Au(111) Shockley surface state by the absorption of up to seven SPP quanta. Using time-resolved photoelectron spectroscopy the coherence of the interaction of the SPPs with the surface state during electron emission is investigated and the process is shown to be similar to light-driven above threshold electron emission. Ultimately, our work could render SPP-based Floquet engineering in nano-optical systems feasible.
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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.