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    <id>61832</id>
    <completedYear/>
    <publishedYear>2024</publishedYear>
    <thesisYearAccepted/>
    <language>eng</language>
    <pageFirst>1</pageFirst>
    <pageLast>8</pageLast>
    <pageNumber/>
    <edition/>
    <issue/>
    <volume/>
    <type>preprint</type>
    <publisherName>Cornell University</publisherName>
    <publisherPlace>Ithaca, NY</publisherPlace>
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    <contributingCorporation/>
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    <title language="eng">Localization of Hybridized Surface Plasmon Modes on Random Gold Nanoparticle Assemblies</title>
    <abstract language="eng">Assemblies of plasmonic nanoparticles (NPs) support hybridized modes of localized surface plasmons (LSPs), which delocalize in geometrically well-ordered arrangements. Here, the hybridization behavior of LSPs in geometrically completely disordered arrangements of Au NPs fabricated by an e-beam synthesis method is studied. Employing electron energy loss spectroscopy in a scanning transmission electron microscope in combination with numerical simulations, the disorder-driven spatial and spectral localization of the coupled LSP modes that depend on the NP thickness is revealed. Below 0.4nm sample thickness (flat NPs), localization increases towards higher hybridized LSP mode energies. In comparison, above 10nm thickness, a decrease of localization (an increase of delocalization) with higher mode energies is observed. In the intermediate thickness regime, a transition of the energy dependence of the localization between the two limiting cases, exhibiting a transition mode energy with minimal localization, is observed. This behavior is mainly driven by the energy and thickness dependence of the polarizability of the individual NPs.</abstract>
    <parentTitle language="eng">arxiv.org</parentTitle>
    <identifier type="doi">10.48550/arXiv.2410.10514</identifier>
    <identifier type="urn">urn:nbn:de:kobv:b43-618323</identifier>
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    <licence>Creative Commons - CC BY-NC-ND - Namensnennung - Nicht kommerziell - Keine Bearbeitungen 4.0 International</licence>
    <author>Mohammed Fayis Kalady</author>
    <author>Johannes Schultz</author>
    <author>Kristina Weinel</author>
    <author>Daniel Wolf</author>
    <author>Axel Lubk</author>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Plasmonics</value>
    </subject>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Electron-Energy Loss Spectroscopy</value>
    </subject>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Discrete Dipole Approximation</value>
    </subject>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Nanoparticles</value>
    </subject>
    <collection role="ddc" number="620">Ingenieurwissenschaften und zugeordnete Tätigkeiten</collection>
    <collection role="institutes" number="">5 Werkstofftechnik</collection>
    <collection role="institutes" number="">5.1 Mikrostruktur Design und Degradation</collection>
    <collection role="themenfelder" number="">Material</collection>
    <collection role="fulltextaccess" number="">Datei für die Öffentlichkeit verfügbar ("Open Access")</collection>
    <collection role="literaturgattung" number="">Graue Literatur</collection>
    <collection role="themenfelder" number="">Advanced Materials</collection>
    <collection role="unnumberedseries" number="">Preprints der BAM</collection>
    <thesisPublisher>Bundesanstalt für Materialforschung und -prüfung (BAM)</thesisPublisher>
    <file>https://opus4.kobv.de/opus4-bam/files/61832/arxiv_2410.10514v1.pdf</file>
  </doc>
  <doc>
    <id>61833</id>
    <completedYear/>
    <publishedYear>2024</publishedYear>
    <thesisYearAccepted/>
    <language>eng</language>
    <pageFirst>1</pageFirst>
    <pageLast>2</pageLast>
    <pageNumber/>
    <edition/>
    <issue/>
    <volume>129</volume>
    <type>article</type>
    <publisherName>EDP Sciences</publisherName>
    <publisherPlace>Les Ulis</publisherPlace>
    <creatingCorporation/>
    <contributingCorporation/>
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    <title language="eng">Fabrication of 2-dimensional disordered assemblies of gold nanoparticles and investigation of localized surface plasmon resonances</title>
    <abstract language="eng">Interaction of electromagnetic waves, such as electron beams or light, with conductive material can lead to localized surface plasmon resonances (LSPRs) where the incoming energy can be deposited in a collective excitation of electrons of the conduction band, which in turn can result in coherent localized plasmon oscillations. LSPR in metallic nanostructures, such as nanoparticles (NPs), which are sensitive to geometry, material composition and environment, are currently utilized in a wide range of applications, such as surface-enhanced Raman spectroscopy, plasmonic wave guides, improved solar cells, on-chip particle accelerators and nanoantennas. A host of studies that focus on plasmonic NPs ranging from single NPs with several shapes (cubic, spherical, tetrahedral) over 1D assemblies of NPs such as chains, to ordered 2D assemblies of NPs show an increase of the complexity regarding the hybridization behavior of LSPRs eventually lead to delocalized Surface Plasmons. Furthermore, Anderson predicted in 1977 the absence of diffusion or delocalization of waves in disordered systems, which has been discussed as the underlying mechanism for LSPRs localization in disordered metallic thin films and ultrathin 2D networks. Our aim is to further develop these studies on the surface plasmon localization in disordered structures by (1) developing a novel NPs assembly fabrication method that allows fabricating disordered assemblies of NPs of a wide range of NPs sizes, and (2) probing the LSPR with high-resolution electron energy-loss spectroscopy (EELS). Moreover, the dominant dipolar interaction between the NPs, also facilitates an efficient numerical modeling of these systems, which in comparison with the experiments allows for an in-depth study of the impact of various geometric parameters as well as retardation and life-time damping on the observed localization behavior.&#13;
&#13;
To synthesize 2D disordered assemblies of gold NPs on a TEM transparent silicon oxide substrate, a new synthesis routine was developed. This procedure is based on sublimation and redeposition of a gold microparticle precursor induced by an electron beam in a scanning electron microscope (SEM) operated at 30 kV. To characterize the assembly of synthesized NPs in terms of size, shape and spreading over the substrate, TEM measurements were conducted subsequently. To study LSPRs experimentally, EELS in scanning transmission electron microscopy (STEM) mode was carried out. The numerical modelling of LSPRs was performed using a self-consistent dipole model.&#13;
&#13;
The synthesized 2D disordered gold NPs assemblies exhibit a gradient in the NPs mean size, which ranges from 100 nm close to the precursor location down to 2 nm at a distance of more than 20 µm from the precursor location. Additionally, the interparticle distance between the gold NPs increases with increasing distance to the precursor location.&#13;
&#13;
The experimental investigation as well as the numerical simulation of the LSPRs demonstrate a localization behavior that decreases toward larger energies, which is driven by the disorder of the NPs assembly (mainly the random particle distance). That localization behavior stays in contrast to what was found in ultrathin 2D gold networks showing increasing of localization towards higher LSPRs energies. By varying the geometric parameters of the NPs assembly in the simulation, we could identify the NPs thickness as the parameter, that determines the energy-dependence of the localization. Specifically, a critical thickness of approx. 10 nm separates the two localization regimes, which correlates to the energy of the dipole mode resonance crucially depending on the thickness of the NPs.&#13;
&#13;
2D disordered assemblies of gold NPs of a wide range of NPs sizes and distances can be synthesized directly on thin substrates facilitating structural characterization and EELS measurements in a TEM. It could be shown that such assemblies exhibit LSPRs with a localization behavior that may be tuned by the NPs sizes (including thickness) and interparticle distances. The proposed synthesis of random NPs assemblies opens new avenues for fundamental studies on Anderson localization in disordered plasmonic structures as well as its applications such as surface-enhanced Raman spectroscopy where localization behavior must be tuned to specific wave lengths.</abstract>
    <parentTitle language="eng">BIO Web of Conferences</parentTitle>
    <identifier type="doi">10.1051/bioconf/202412932007</identifier>
    <identifier type="urn">urn:nbn:de:kobv:b43-618330</identifier>
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    <enrichment key="eventName">17th European Microscopy Congress (EMC 2024)</enrichment>
    <enrichment key="eventPlace">Copenhagen, Denmark</enrichment>
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    <licence>Creative Commons - CC BY - Namensnennung 4.0 International</licence>
    <author>Kristina Weinel</author>
    <author>Johannes Schultz</author>
    <author>Mohammed Fayis Kalady</author>
    <author>Daniel Wolf</author>
    <author>Leonardo Agudo Jácome</author>
    <author>Axel Lubk</author>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Scanning electron microscopy</value>
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    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Gold nanoparticle synthesis</value>
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    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Disordered assemblies</value>
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    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Localized surface plasmon resonances</value>
    </subject>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Transmission electron microscopy</value>
    </subject>
    <collection role="ddc" number="620">Ingenieurwissenschaften und zugeordnete Tätigkeiten</collection>
    <collection role="institutes" number="">5 Werkstofftechnik</collection>
    <collection role="institutes" number="">5.1 Mikrostruktur Design und Degradation</collection>
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    <collection role="literaturgattung" number="">Verlagsliteratur</collection>
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    <collection role="unnumberedseries" number="">Wissenschaftliche Artikel der BAM</collection>
    <collection role="themenfelder" number="">Advanced Materials</collection>
    <thesisPublisher>Bundesanstalt für Materialforschung und -prüfung (BAM)</thesisPublisher>
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