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Item type:Publication, Access status: with files , Gold Nanoparticles with N-Heterocyclic Carbene/Triphenylamine Surface Ligands: Stable and Electrochromically Active Hybrid Materials for OptoelectronicsOrganic-hybrid particle-based materials are increasingly important in (opto)electronics, sensing, and catalysis due to their printability and stretchability as well as their potential for unique synergistic functional effects. However, these functional properties are often limited due to poor electronic coupling between the organic shell and the nanoparticle. N-heterocyclic carbenes (NHCs) belong to the most promising anchors to achieve electronic delocalization across the interface, as they form robust and highly conductive bonds with metals and offer a plethora of functionalization possibilities. Despite the outstanding potential of the conductive NHC-metal bond, synthetic challenges have so far limited its application to the improvement of colloidal stabilities, disregarding the potential of the conductive anchor. Here, NHC anchors are used to modify redox-active gold nanoparticles (AuNPs) with conjugated triphenylamines (TPA). The resulting AuNPs exhibit excellent thermal and redox stability benefiting from the robust NHC-gold bond. As electrochromic materials, the hybrid materials show pronounced color changes from red to dark green, a highly stable cycling stability (1000 cycles), and a fast response speed (5.6 s/2.1 s). Furthermore, TPA-NHC@AuNP exhibits an ionization potential of 5.3 eV and a distinct out-of-plane conductivity, making them a promising candidate for application as hole transport layers in optoelectronic devices.Publicationtype: Journal Article27 32 - Some of the metrics are blocked by yourconsent settings
Item type:Publication, Access status: with files , Coherent phase change in interstitial solutions : a hierarchy of instabilitiesMetal hydrides or lithium ion battery electrodes can take the form of interstitial solid solutions with a miscibility gap. This work discusses theory approaches for locating, in temperature-composition space, coherent phase transformations during the charging/discharging of such systems and for identifying the associated transformation mechanisms. The focus is on the simplest scenario, where instabilities derive from the thermodynamics of the bulk phase alone, considering strain energy as the foremost consequence of coherency and admitting for stress relaxation at free surfaces. The extension of the approach to include capillarity is demonstrated by an example. The analysis rests on constrained equilibrium phase diagrams that are informed by geometry- and dimensionality-specific mechanical boundary conditions and on elastic instabilities–again geometry-specific–as implied by the theory of open-system elasticity. It is demonstrated that some scenarios afford the analysis of chemical stability to be based entirely on a linear stability analysis of the mechanical equilibrium, which provides closed-form solutions in a straightforward manner. Attention is on the impact of the system geometry (infinitely extended or of finite size) and on the chemical (closed or open system) and mechanical (incoherent or coherent) boundary conditions. Transformation mechanism maps are suggested for documenting the findings. The maps reveal a hierarchy of instabilities, which depend strongly on each of the above characteristics. Specifically, realistic, finite-sized systems differ qualitatively from idealized systems of infinite extension. Among the transformation mechanisms exposed by the analysis are a uniform switchover to the other phase when the open system reaches its chemical spinodal, practical coherent nucleation, as well as chemo-elastically coupled spontaneous buckling modes, which may take the form of either, single-phase or dual-phase states.Publicationtype: Journal Article20 18