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  1. Article ; Online: Architecture Controls Phonon Propagation in All-Solid Brush Colloid Metamaterials.

    Cang, Yu / Sainidou, Rebecca / Rembert, Pascal / Matyjaszewski, Krzysztof / Bockstaller, Michael / Graczykowski, Bartlomiej / Fytas, George

    Small (Weinheim an der Bergstrasse, Germany)

    2023  Volume 20, Issue 13, Page(s) e2304157

    Abstract: Brillouin light scattering and elastodynamic theory are concurrently used to determine and interpret the hypersonic phonon dispersion relations in brush particle solids as a function of the grafting density with perspectives in optomechanics, heat ... ...

    Abstract Brillouin light scattering and elastodynamic theory are concurrently used to determine and interpret the hypersonic phonon dispersion relations in brush particle solids as a function of the grafting density with perspectives in optomechanics, heat management, and materials metrology. In the limit of sparse grafting density, the phonon dispersion relations bear similarity to polymer-embedded colloidal assembly structures in which phonon dispersion can be rationalized on the basis of perfect boundary conditions, i.e., isotropic stiffness transitions across the particle interface. In contrast, for dense brush assemblies, more complex dispersion characteristics are observed that imply anisotropic stiffness transition across the particle/polymer interface. This provides direct experimental validation of phonon propagation changes associated with chain conformational transitions in dense particle brush materials. A scaling relation between interface tangential stiffness and crowding of polymer tethers is derived that provides a guideline for chemists to design brush particle materials with tailored phononic dispersion characteristics. The results emphasize the role of interfaces in composite materials systems. Given the fundamental relevance of phonon dispersion to material properties such as thermal transport or mechanical properties, it is also envisioned that the results will spur the development of novel functional hybrid materials.
    Language English
    Publishing date 2023-11-16
    Publishing country Germany
    Document type Journal Article
    ZDB-ID 2168935-0
    ISSN 1613-6829 ; 1613-6810
    ISSN (online) 1613-6829
    ISSN 1613-6810
    DOI 10.1002/smll.202304157
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  2. Article: Origin of the Acoustic Bandgaps in Hypersonic Colloidal Phononics: The Role of the Elastic Impedance

    Cang, Yu / Sainidou, Rebecca / Rembert, Pascal / Magnabosco, Giulia / Still, Tim / Vogel, Nicolas / Graczykowski, Bartlomiej / Fytas, George

    Journal of physical chemistry. 2022 Aug. 23, v. 126, no. 34

    2022  

    Abstract: How phonons propagate in nanostructures determines the flow of elastic and thermal energy in dielectric materials. However, a reliable theoretical prediction of the phonon dispersion relation requires experimental verification both near to and far from ... ...

    Abstract How phonons propagate in nanostructures determines the flow of elastic and thermal energy in dielectric materials. However, a reliable theoretical prediction of the phonon dispersion relation requires experimental verification both near to and far from the Brillouin zone of the nanostructure. We report on the experimental hypersonic phonon dispersion of hard (SiO₂) and soft (polymer) fcc colloidal crystals infiltrated in liquid polydimethylsiloxane with different elastic impedance contrast using Brillouin light spectroscopy. We discuss the distinct differences with first-principles full elastodynamic calculations involving a multiple-scattering theory. Interparticle contacts strongly impact the long-wavelength speed of sound and the nature of the particle vibration resonance-induced hybridization hypersonic bandgap. The absence of the order-induced Bragg bandgap in SiO₂ and its presence in soft opals cannot be fully accounted for by the theory, limiting its predictive power. Bridging the elasticity of the two colloidal crystals with suitable SiO₂ core–shell (polymer) particles reveals an unprecedented crossover behavior in the dispersion relation. In view of many conversational parameters, the control tuning of phonon propagation in soft matter-based hypersonic phononics remains challenging.
    Keywords acoustics ; hybridization ; liquids ; nanomaterials ; physical chemistry ; polydimethylsiloxane ; prediction ; spectroscopy ; thermal energy ; vibration
    Language English
    Dates of publication 2022-0823
    Size p. 6575-6584.
    Publishing place American Chemical Society
    Document type Article
    ISSN 1520-5207
    DOI 10.1021/acs.jpcb.2c03923
    Database NAL-Catalogue (AGRICOLA)

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  3. Article ; Online: Origin of the Acoustic Bandgaps in Hypersonic Colloidal Phononics: The Role of the Elastic Impedance.

    Cang, Yu / Sainidou, Rebecca / Rembert, Pascal / Magnabosco, Giulia / Still, Tim / Vogel, Nicolas / Graczykowski, Bartlomiej / Fytas, George

    The journal of physical chemistry. B

    2022  Volume 126, Issue 34, Page(s) 6575–6584

    Abstract: How phonons propagate in nanostructures determines the flow of elastic and thermal energy in dielectric materials. However, a reliable theoretical prediction of the phonon dispersion relation requires experimental verification both near to and far from ... ...

    Abstract How phonons propagate in nanostructures determines the flow of elastic and thermal energy in dielectric materials. However, a reliable theoretical prediction of the phonon dispersion relation requires experimental verification both near to and far from the Brillouin zone of the nanostructure. We report on the experimental hypersonic phonon dispersion of hard (SiO
    Language English
    Publishing date 2022-08-23
    Publishing country United States
    Document type Journal Article
    ISSN 1520-5207
    ISSN (online) 1520-5207
    DOI 10.1021/acs.jpcb.2c03923
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  4. Article: Thermomechanical Properties and Glass Dynamics of Polymer-Tethered Colloidal Particles and Films

    Cang, Yu / Alonso-Redondo Elena / Bockstaller Michael R / Fytas George / Lee Jaejun / Matyjaszewski Krzysztof / Rembert Pascal / Reuss Anna N / Sainidou Rebecca / Yan Jiajun / Zhang Jianan

    Macromolecules. 2017 Nov. 14, v. 50, no. 21

    2017  

    Abstract: Polymer-tethered colloidal particles (aka “particle brush materials”) have attracted interest as a platform for innovative material technologies and as a model system to elucidate glass formation in complex structured media. In this contribution, ... ...

    Abstract Polymer-tethered colloidal particles (aka “particle brush materials”) have attracted interest as a platform for innovative material technologies and as a model system to elucidate glass formation in complex structured media. In this contribution, Brillouin light scattering is used to sequentially evaluate the role of brush architecture on the dynamical properties of brush particles in both the individual and assembled (film) state. In the former state, the analysis reveals that brush–brush interactions as well as global chain relaxation sensitively depend on grafting density; i.e., more polymer-like behavior is observed in sparse brush systems. This is interpreted to be a consequence of more extensive chain entanglement. In contrast, the local relaxation of films does not depend on grafting density. The results highlight that relaxation processes in particle brush-based materials span a wider range of time and length scales as compared to linear chain polymers. Differentiation between relaxation on local and global scale is necessary to reveal the influence of molecular structure and connectivity on the aging behavior of these complex systems.
    Keywords chemical structure ; colloids ; glass ; light scattering ; models ; polymers
    Language English
    Dates of publication 2017-1114
    Size p. 8658-8669.
    Publishing place American Chemical Society
    Document type Article
    ZDB-ID 1491942-4
    ISSN 1520-5835 ; 0024-9297
    ISSN (online) 1520-5835
    ISSN 0024-9297
    DOI 10.1021%2Facs.macromol.7b01752
    Database NAL-Catalogue (AGRICOLA)

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  5. Article ; Online: Role of Polymer Graft Architecture on the Acoustic Eigenmode Formation in Densely Polymer-Tethered Colloidal Particles.

    Schneider, Dirk / Schmitt, Michael / Hui, Chin Ming / Sainidou, Rebecca / Rembert, Pascal / Matyjaszewski, Krzysztof / Bockstaller, Michael R / Fytas, George

    ACS macro letters

    2014  Volume 3, Issue 10, Page(s) 1059–1063

    Abstract: The concurrent evaluation of the vibration eigenfrequencies in densely polymer-tethered particle systems ("particle brushes") by Brillouin light scattering and elastodynamic theory reveals a distinctive change of acoustic eigenmode formation associated ... ...

    Abstract The concurrent evaluation of the vibration eigenfrequencies in densely polymer-tethered particle systems ("particle brushes") by Brillouin light scattering and elastodynamic theory reveals a distinctive change of acoustic eigenmode formation associated with polymer graft modification of colloidal particles. The eigenfrequencies of particle brushes reveal a characteristic red-shift compared to uniform core-shell particles that can only be rationalized by assuming imperfect boundary conditions and anisotropic elastic properties of the graft layer. The distinct characteristics of vibration modes in particle brush materials provide direct evidence for the implications of chain confinement on the nanomechanical properties of tethered chains. The results highlight a rich and hitherto unexplored parameter-space for controlling properties and interactions in particle-brush based systems that could spur the development of hybrid materials with novel functionalities.
    Language English
    Publishing date 2014-10-06
    Publishing country United States
    Document type Journal Article
    ISSN 2161-1653
    ISSN (online) 2161-1653
    DOI 10.1021/mz500433h
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  6. Article: Thermomechanical Properties and Glass Dynamics of Polymer-Tethered Colloidal Particles and Films.

    Cang, Yu / Reuss, Anna N / Lee, Jaejun / Yan, Jiajun / Zhang, Jianan / Alonso-Redondo, Elena / Sainidou, Rebecca / Rembert, Pascal / Matyjaszewski, Krzysztof / Bockstaller, Michael R / Fytas, George

    Macromolecules

    2017  Volume 50, Issue 21, Page(s) 8658–8669

    Abstract: Polymer-tethered colloidal particles (aka "particle brush materials") have attracted interest as a platform for innovative material technologies and as a model system to elucidate glass formation in complex structured media. In this contribution, ... ...

    Abstract Polymer-tethered colloidal particles (aka "particle brush materials") have attracted interest as a platform for innovative material technologies and as a model system to elucidate glass formation in complex structured media. In this contribution, Brillouin light scattering is used to sequentially evaluate the role of brush architecture on the dynamical properties of brush particles in both the individual and assembled (film) state. In the former state, the analysis reveals that brush-brush interactions as well as global chain relaxation sensitively depend on grafting density; i.e., more polymer-like behavior is observed in sparse brush systems. This is interpreted to be a consequence of more extensive chain entanglement. In contrast, the local relaxation of films does not depend on grafting density. The results highlight that relaxation processes in particle brush-based materials span a wider range of time and length scales as compared to linear chain polymers. Differentiation between relaxation on local and global scale is necessary to reveal the influence of molecular structure and connectivity on the aging behavior of these complex systems.
    Language English
    Publishing date 2017-10-30
    Publishing country United States
    Document type Journal Article
    ZDB-ID 3436-8
    ISSN 0024-9297
    ISSN 0024-9297
    DOI 10.1021/acs.macromol.7b01752
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  7. Article: Efficient generation of propagating plasmons by electron beams.

    Cai, Wei / Sainidou, Rebecca / Xu, Jingjun / Polman, A / García de Abajo, F Javier

    Nano letters

    2009  Volume 9, Issue 3, Page(s) 1176–1181

    Abstract: We report highly efficient generation of propagating plasmons by electron beams in planar films, planar dielectric cavities, metallic wires, and nanoparticle waveguides. Electron-induced plasmon excitation is investigated in (1) gold thin films, both ... ...

    Abstract We report highly efficient generation of propagating plasmons by electron beams in planar films, planar dielectric cavities, metallic wires, and nanoparticle waveguides. Electron-induced plasmon excitation is investigated in (1) gold thin films, both free-standing or supported on a silica substrate, (2) gold-silica-gold planar cavities, (3) gold nanowires, and (4) gold nanoparticle arrays. We obtain excitation yields as high as 10(- 2) plasmons per incoming electron over the visible and near-infrared range. Symmetric and antisymmetric plasmon modes are found to be more easily excited in thick and thin films, respectively, and in particular leaky plasmons in supported films are shown to be excited with very large probability exceeding one plasmon per electron. Generation of guided plasmons in metallic particle arrays is also proved to be attainable by aiming the electron at one end of the waveguide. The temporal evolution and spectral distribution of excited plasmons are discussed as well. Our results provide full support for the application of electron bombardment to excite propagating plasmons with high efficiency, thus solving the standing problem of plasmon generation at designated locations.
    MeSH term(s) Algorithms ; Electrons ; Gold/chemistry ; Metal Nanoparticles/chemistry ; Metals/chemistry ; Models, Statistical ; Nanotechnology/methods ; Nanowires/chemistry ; Scattering, Radiation ; Time Factors
    Chemical Substances Metals ; Gold (7440-57-5)
    Language English
    Publishing date 2009-02-18
    Publishing country United States
    Document type Journal Article ; Research Support, Non-U.S. Gov't
    ISSN 1530-6984
    ISSN 1530-6984
    DOI 10.1021/nl803825n
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  8. Article ; Online: Anisotropic elasticity of quasi-one-component polymer nanocomposites.

    Voudouris, Panayiotis / Choi, Jihoon / Gomopoulos, Nikos / Sainidou, Rebecca / Dong, Hongchen / Matyjaszewski, Krzysztof / Bockstaller, Michael R / Fytas, George

    ACS nano

    2011  Volume 5, Issue 7, Page(s) 5746–5754

    Abstract: The in-plane and out-of-plane elastic properties of thin films of "quasi-one-component" particle-brush-based nanocomposites are compared to those of "classical" binary particle-polymer nanocomposite systems with near identical overall composition using ... ...

    Abstract The in-plane and out-of-plane elastic properties of thin films of "quasi-one-component" particle-brush-based nanocomposites are compared to those of "classical" binary particle-polymer nanocomposite systems with near identical overall composition using Brillouin light scattering. Whereas phonon propagation is found to be independent of the propagation direction for the binary particle/polymer blend systems, a pronounced splitting of the phonon propagation velocity along the in-plane and out-of-plane film direction is observed for particle-brush systems. The anisotropic elastic properties of quasi-one-component particle-brush systems are interpreted as a consequence of substrate-induced order formation into layer-type structures and the associated breaking of the symmetry of the film. The results highlight new opportunities to engineer quasi-one-component nanocomposites with advanced control of structural and physical property characteristics based on the assembly of particle-brush materials.
    Language English
    Publishing date 2011-07-26
    Publishing country United States
    Document type Journal Article ; Research Support, Non-U.S. Gov't ; Research Support, U.S. Gov't, Non-P.H.S.
    ISSN 1936-086X
    ISSN (online) 1936-086X
    DOI 10.1021/nn201431w
    Database MEDical Literature Analysis and Retrieval System OnLINE

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  9. Article ; Online: Extraordinary all-dielectric light enhancement over large volumes.

    Sainidou, Rebecca / Renger, Jan / Teperik, Tatiana V / González, María U / Quidant, Romain / García de Abajo, F Javier

    Nano letters

    2010  Volume 10, Issue 11, Page(s) 4450–4455

    Abstract: We present resonant dielectric structures exhibiting arbitrarily large optical field enhancement, only limited by fabrication imperfections. Three different arrangements are investigated, based upon dielectric waveguides, dielectric particle arrays, and ... ...

    Abstract We present resonant dielectric structures exhibiting arbitrarily large optical field enhancement, only limited by fabrication imperfections. Three different arrangements are investigated, based upon dielectric waveguides, dielectric particle arrays, and a combination of these two structures. Experimental confirmation of enhancement in a waveguide resonator is achieved by measuring the luminescence of quantum dots dispersed in the hot optical region of the structure. The performance of these systems can be readily controlled by simply changing geometrical parameters, which allows obtaining remarkable values of the intensity enhancement approaching 105 relative to the incident intensity over large volumes under feasible experimental conditions. This opens new avenues for all-optical switching and biosensing.
    MeSH term(s) Computer-Aided Design ; Equipment Design ; Equipment Failure Analysis ; Light ; Luminescent Measurements/instrumentation ; Quantum Dots ; Refractometry/instrumentation ; Scattering, Radiation
    Language English
    Publishing date 2010-10-18
    Publishing country United States
    Document type Journal Article ; Research Support, Non-U.S. Gov't
    ISSN 1530-6992
    ISSN (online) 1530-6992
    DOI 10.1021/nl102270p
    Database MEDical Literature Analysis and Retrieval System OnLINE

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