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Hexakis(n-alkyloxy)triphenylene) (HATn) consisting of an aromatic triphenylene core and alkyl side chains are model discotic liquid crystal (DLC) systems forming a columnar mesophase. In the mesophase, the molecules of HATn self-assemble in columns, which has one-dimensional high charge carrier mobility along the columns. Here, a homologous series of HATn with different length of the alkyl chain (n=5,6,8,10,12) is investigated using differential scanning calorimetry (DSC), broadband dielectric spectroscopy (BDS) and advanced calorimetric techniques including fast scanning calorimetry (FSC) and specific heat spectroscopy (SHS). The investigation of the phase behavior was done utilizing DSC experiments and the influence of the alkyl chain length on the phase behavior was revealed. By the dielectric investigations a γ-relaxation due to localized fluctuations as well as two glassy dynamics the αcore and αalkyl relaxation were observed in the temperature range of the plastic crystalline phase. Moreover, the observed glassy dynamics were further studied employing advanced calorimetry. All observed relaxation processes are attributed to the possible specific molecular fluctuations and discussed in detail. From the results a transition at around n=8 from a rigid constrained (n=5,6) to a softer system (n=10,12) on a molecular lenght scale was revealed with increasing alkyl chain length. A counterbalance of two competing effects of a polyethylene like behavior of the alkyl chains in the intercolumnar domains and self-organized confinement is discussed in the context of a hindered glass transition. The results were confirmed by in- and quasielastic neutron scattering
Hexakis(n-alkyloxy)triphenylene) (HATn) consisting of an aromatic triphenylene core and alkyl side chains are model discotic liquid crystal (DLC) systems forming a columnar mesophase. In the mesophase, the molecules of HATn self-assemble in columns, which has one-dimensional high charge carrier mobility along the columns. Here, a homologous series of HATn with different length of the alkyl chain (n=5,6,8,10,12) is investigated using differential scanning calorimetry (DSC), broadband dielectric spectroscopy (BDS) and advanced calorimetric techniques including fast scanning calorimetry (FSC) and specific heat spectroscopy (SHS). The investigation of the phase behavior was done utilizing DSC experiments and the influence of the alkyl chain length on the phase behavior was revealed. By the dielectric investigations probing the molecular mobility, a γ-relaxation due to localized fluctuations as well as two glassy dynamics the αcore and αalkyl relaxation were observed in the temperature range of the plastic crystalline phase. Moreover, the observed glassy dynamics were further studied employing advanced calorimetry. All observed relaxation processes are attributed to the possible specific molecular fluctuations and discussed in detail. From the results a transition at around n=8 from a rigid constrained (n=5,6) to a softer system (n=10,12) on a molecular lenght scale was revealed with increasing alkyl chain length. A counterbalance of two competing effects of a polyethylene like behavior of the alkyl chains in the intercolumnar domains and self-organized confinement is discussed in the context of a hindered glass transition.
A selected series of dipole functionalized triphenylene-based discotic liquid crystals (DLCs) was synthesized and investigated in a systematic way to reveal the phase behavior and molecular dynamics. The later point is of particular importance to understand the charge transport in such systems which is the key property for their applications such as organic field effect transistors, solar cells or as nanowires in molecular electronics, and also to tune the properties of DLCs. The mesomorphic properties were studied by polarizing optical microscopy, X-ray diffraction, and differential scanning calorimetry, which were compared to the corresponding unfunctionalized DLC. The molecular dynamics were investigated by a combination of state-of-the-art broadband dielectric spectroscopy (BDS) and advanced calorimetry such as fast scanning calorimetry (FSC) and specific heat spectroscopy (SHS). Besides localized fluctuations, surprisingly multiple glassy dynamics were detected for all materials for the first time. Glassy dynamics were proven for both processes unambiguously due to the extraordinary broad frequency range covered. The α1-process is attributed to fluctuations of the alky chains in the intercolumnar space because a polyethylene-like glassy dynamics is observed. This corresponds to a glass transition in a confined three-dimensional space. The α2-process found at temperatures lower than α1-process, is assigned to the fluctuation of translational in plane movements of the triphenylene core inside distorted columns. This can be considered as a glass transition of a one-dimensional fluid. Therefore, obtained results are of general importance to understand the glass transition, which is an unsolved problem of condensed matter science.