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Multi-mode heterodyned 5th-order infrared spectroscopy
摘要： Fifth-order multidimensional infrared spectroscopy with heterodyned detection was carried out in the three-beam dual-frequency configuration. Numerous 5th-order cross peaks were detected for the 4-azidobutyrate-N-hydroxysuccinimide ester compound in solution involving several vibrational modes ranging in frequency from 1045 to 2100 cm?1. Cross peaks involving overtones (2X/Z) and combination bands (XY/Z) among the tags, modes X and Y excited by the first two mid-IR laser pulses, and the reporter, modes Z excited by the third laser pulse, were acquired and the factors affecting the amplitude of 5th-order cross peaks are discussed. The 5th-order cross peaks were detected among modes that are spatially close (a few bonds apart) as well as for modes spatially separated by ca. 12 ? (eight bonds apart). In both cases, the waiting time dependences for the 3rd and 5th order cross peaks were found to be different. In particular, the waiting time at which the cross-peak maximum is reached, the decay time, and the value of a plateau at large waiting times were all differing strongly. The differences are explained by reduced sensitivity of the 5th-order signals to modes coupled weakly to the reporter mode and different relaxation dynamics involving overtone state of the tag. The ability of the 5th-order peaks to single out the modes coupled strongly to the reporter can help identifying specific energy relaxation and transport pathways, which will be useful for understanding energy transport dynamics in molecules. The absorptive 5th-order cross peaks were constructed which report on three-point correlation functions. It is shown that in addition to the triple-frequency correlation functions, a correlation of the frequencies with the mode coupling (anharmonicity) can be naturally measured by the 5th-order spectroscopy. The current limit for detecting 5th-order signals was estimated at the level of 1 × 10?3 in reduced anharmonicity, which is determined by the corresponding two-state anharmonicity divided by the reporter mode spectral width. Given the simplicity of recording the 5th-order cross peaks in the three-beam configuration, the approach carries a potential for a broad use.
关键词： vibrational modes,anharmonicity,heterodyned detection,fifth-order,multidimensional infrared spectroscopy,energy transport
更新于2025-09-23 15:22:29
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Photochemical dynamics under incoherent illumination: Light harvesting in self-assembled molecular J-aggregates
摘要： Transport phenomena in organic, self-assembled molecular J-aggregates have long attracted a great deal of attention due to their potential role in designing novel organic photovoltaic devices. A large number of theoretical and experimental studies have been carried out describing excitonic energy transfer in J-aggregates under the assumption that excitons are induced by a coherent laser-light source or initialized by a localized excitation on a particular chromophore. However, these assumptions may not provide an accurate description to assess the efficiency of J-aggregates, particularly as building blocks of organic solar cells. Under natural conditions, J-aggregates would be subjected to an incoherent source of light (as is sunlight), which would illuminate the whole photosynthetic complex rather than a single molecule. In this work, we present the first study of the efficiency of photosynthetic energy transport in self-assembled molecular aggregates under incoherent sunlight illumination. By making use of a minimalistic model of a cyanine dye J-aggregate, we demonstrate that long-range transport efficiency is enhanced when exciting the aggregate with incoherent light. Our results thus support the conclusion that J-aggregates are, indeed, excellent candidates for devices where efficient long-range incoherently induced exciton transport is desired, such as in highly efficient organic solar cells.
关键词： incoherent illumination,exciton transport,organic solar cells,J-aggregates,photosynthetic energy transport
更新于2025-09-23 15:19:57
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[ASME ASME 2018 International Technical Conference and Exhibition on Packaging and Integration of Electronic and Photonic Microsystems - San Francisco, California, USA (Monday 27 August 2018)] ASME 2018 International Technical Conference and Exhibition on Packaging and Integration of Electronic and Photonic Microsystems - Effect of Interfacial Thermal Conductance Between the Nanoparticles
摘要： Heat transport across nanostructured interfaces, such as between nanoparticles, has been of great interest for advanced thermal management. Interfacial thermal conductance, G, is central to understanding heat transport between nanoparticles that have a contact point between each other as well as the surrounded medium. In this study, we show that G dominates the heat transport compared to the conduction and radiation heat transfer modes between the nanoparticles for values higher than ~20 (MW/m2K). We also investigate the effect of radius of contact between the nanoparticles on the overall modes of heat transfer.
关键词： Nanoparticle Packings,Interfacial Thermal Conductance,Micro-Nanoscale Thermal Energy Transport
更新于2025-09-19 17:15:36
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Enhanced Energy Transfer in Doped Bifluorene Single Crystals: Prospects for Organic Lasers
摘要： Organic single crystals with long-range molecular order ensure enhanced carrier mobility and stability as well as emission outcoupling, which makes them attractive as gain medium for electrically pumped organic lasers. Unfortunately, effects of excitonic coupling introduce losses degrading optical performance in crystals, hence higher lasing thresholds are observed compared to amorphous films. Here, crystal doping strategy is investigated as a method to avoid pronounced reabsorption and annihilation losses associated with J-type excitonic coupling, while taking advantage of enhanced exciton transport for efficient energy transfer. Bifluorene-based derivatives linked with acetylene and ethylene rigid bridges are suitable as host and dopant system forming high-quality crystals doped at various concentrations (0.5–11.0%). Enhanced exciton transport in host crystal mediates picosecond host–dopant energy transfer enabling 100% transfer efficiency at lower doping concentrations compared to amorphous films. Amplified spontaneous emission threshold of 1.9 μJ cm?2 in 3.5% doped crystal is enabled by minimized exciton annihilation and emission reabsorption losses at optimal doping concentration.
关键词： long-range energy transport,organic single crystals,organic laser gain materials,amplified spontaneous emission,F?rster resonant energy transfer
更新于2025-09-12 10:27:22