Universität Stuttgart
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Item Open Access Dimerization and oligomerization of DNA-assembled building blocks for controlled multi-motion in high-order architectures(2021) Xin, Ling; Duan, Xiaoyang; Liu, NaIn living organisms, proteins are organized prevalently through a self-association mechanism to form dimers and oligomers, which often confer new functions at the intermolecular interfaces. Despite the progress on DNA-assembled artificial systems, endeavors have been largely paid to achieve monomeric nanostructures that mimic motor proteins for a single type of motion. Here, we demonstrate a DNA-assembled building block with rotary and walking modules, which can introduce new motion through dimerization and oligomerization. The building block is a chiral system, comprising two interacting gold nanorods to perform rotation and walking, respectively. Through dimerization, two building blocks can form a dimer to yield coordinated sliding. Further oligomerization leads to higher-order structures, containing alternating rotation and sliding dimer interfaces to impose structural twisting. Our hierarchical assembly scheme offers a design blueprint to construct DNA-assembled advanced architectures with high degrees of freedom to tailor the optical responses and regulate multi-motion on the nanoscale.Item Open Access Transformable plasmonic helix with swinging gold nanoparticles(2022) Peil, Andreas; Zhan, Pengfei; Duan, Xiaoyang; Krahne, Roman; Garoli, Denis; M. Liz‐Marzán, Luis; Liu, NaControl over multiple optical elements that can be dynamically rearranged to yield substantial three‐dimensional structural transformations is of great importance to realize reconfigurable plasmonic nanoarchitectures with sensitive and distinct optical feedback. In this work, we demonstrate a transformable plasmonic helix system, in which multiple gold nanoparticles (AuNPs) can be directly transported by DNA swingarms to target positions without undergoing consecutive stepwise movements. The swingarms allow for programmable AuNP translocations in large leaps within plasmonic nanoarchitectures, giving rise to tailored circular dichroism spectra. Our work provides an instructive bottom‐up solution to building complex dynamic plasmonic systems, which can exhibit prominent optical responses through cooperative rearrangements of the constituent optical elements with high fidelity and programmability.Item Open Access Stabilizing γ‐MgH2 at nanotwins in mechanically constrained nanoparticles(2021) Kammerer, Jochen A.; Duan, Xiaoyang; Neubrech, Frank; Schröder, Rasmus R.; Liu, Na; Pfannmöller, MartinReversible hydrogen uptake and the metal/dielectric transition make the Mg/MgH2 system a prime candidate for solid‐state hydrogen storage and dynamic plasmonics. However, high dehydrogenation temperatures and slow dehydrogenation hamper broad applicability. One promising strategy to improve dehydrogenation is the formation of metastable γ‐MgH2. A nanoparticle (NP) design, where γ‐MgH2 forms intrinsically during hydrogenation is presented and a formation mechanism based on transmission electron microscopy results is proposed. Volume expansion during hydrogenation causes compressive stress within the confined, anisotropic NPs, leading to plastic deformation of β‐MgH2 via (301)β twinning. It is proposed that these twins nucleate γ‐MgH2 nanolamellas, which are stabilized by residual compressive stress. Understanding this mechanism is a crucial step toward cycle‐stable, Mg‐based dynamic plasmonic and hydrogen‐storage materials with improved dehydrogenation. It is envisioned that a more general design of confined NPs utilizes the inherent volume expansion to reform γ‐MgH2 during each rehydrogenation.Item Open Access Three-dimensional optical metamaterials(2009) Liu, Na; Giessen, Harald (Prof. Dr.)Metamamaterials have attracted a lot of attention due to their fascinating properties. Many proactical applications have been suggested such as negative refraction, perfect lens, and invisibility cloak. In order to create real materials, we need three-dimensional structures. These structures pose some challenges in fabrication as well as with regards to understanding their optical properties, especially the relevant coupling mechanisms between neighboring elements and layers. In this thesis, we are going to present the advantages and problems associated with different fabrication methods. We will discuss coupling between the elements, taking electric and magnetic dipoles as well as higher order multipoles into account. Longitudinal and transverse interactions as well as their interplay will be examined.Item Open Access Real-time tracking of coherent oscillations of electrons in a nanodevice by photo-assisted tunnelling(2024) Luo, Yang; Neubrech, Frank; Martin-Jimenez, Alberto; Liu, Na; Kern, Klaus; Garg, ManishCoherent collective oscillations of electrons excited in metallic nanostructures (localized surface plasmons) can confine incident light to atomic scales and enable strong light-matter interactions, which depend nonlinearly on the local field. Direct sampling of such collective electron oscillations in real-time is crucial to performing petahertz scale optical modulation, control, and readout in a quantum nanodevice. Here, we demonstrate real-time tracking of collective electron oscillations in an Au bowtie nanoantenna, by recording photo-assisted tunnelling currents generated by such oscillations in this quantum nanodevice. The collective electron oscillations show a noninstantaneous response to the driving laser fields with a T2 decay time of nearly 8 femtoseconds. The contributions of linear and nonlinear electron oscillations in the generated tunnelling currents were precisely determined. A phase control of electron oscillations in the nanodevice is illustrated. Functioning in ambient conditions, the excitation, phase control, and read-out of coherent electron oscillations pave the way toward on-chip light-wave electronics in quantum nanodevices.