Carrier multiplication by singlet exciton fission enhances photovoltaic conversion efficiencies in organic solids. This decay of one singlet exciton into two triplet states allows the extraction of up to two electrons per harvested photon and, hence, promises to overcome the Shockley–Queisser limit. However, the microscopic mechanism of singlet exciton fission, especially the relation between molecular packing and electronic response, remains unclear, which therefore hampers the systematic improvement of organic photovoltaic devices. For the model system perfluoropentacene, we experimentally show that singlet exciton fission is greatly enhanced for a slip-stacked molecular arrangement by addressing different crystal axes featuring different packing schemes. This reveals that the fission process strongly depends on the intermolecular coupling: slip-stacking favors delocalization of excitations and allows for efficient exciton fission, while face-to-edge molecular orientations commonly found in the prevailing herringbone molecular stacking patterns even suppress it. Furthermore, we clarify the controversially debated role of excimer states as intermediary rather than competitive or precursory. Our detailed findings serve as a guideline for the design of next-generation molecular materials for application in future organic light-harvesting devices exploiting singlet exciton fission.
The photoluminescence from a Ga͑AsBi͒ sample is investigated as a function of pump power and lattice temperature. The disorder-related features are analyzed using a Monte Carlo simulation technique. A two-scale approach is introduced to separately account for cluster localization and alloy disorder effects. The corresponding characteristic energy scales of 11 and 45 meV are deduced from the detailed comparison between experiment and simulation.
Graphene has unique optical and electronic properties that make it attractive as an active material for broadband ultrafast detection. We present here a graphene-based detector that shows 40-picosecond electrical rise time over a spectral range that spans nearly three orders of magnitude, from the visible to the far-infrared. The detector employs a large area graphene active region with interdigitated electrodes that are connected to a log-periodic antenna to improve the long-wavelength collection efficiency, and a silicon carbide substrate that is transparent throughout the visible regime. The detector exhibits a noise-equivalent power of approximately 100 µW·Hz -½ and is characterized at wavelengths from 780 nm to 500 µm.
Temperature-dependent photoluminescence in a Ga(AsBi) structure is modelled in an excitonic hopping model and compared to experiment. It is shown that theory and experiment cannot be brought into agreement when using a single energy scale. Thus, a second energy scale is introduced, resulting in a good agreement between theory and experiment. The two scales are identified with spatially large alloy disorder and additional cluster states subdividing this first scale
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