Layered transition metal dichalcogenides (TMDs) represent a diverse, emerging source of two-dimensional (2D) nanostructures with broad application in optoelectronics and energy. In particular, tungsten disulfide (WS2) is an efficient visible light absorber with relatively high carrier mobilities and catalytic activity towards hydrogen evolution. While explanation of the quantum confinement and excitonic effects governing TMD optoelectronic properties has progressed in recent years, less is known about the ultra-fast photoresponse and carrier dynamics following light excitation. This work utilizes transient absorption spectroscopy, with pump tunability and broadband visible probing, to monitor the carrier dynamics of both CVD-grown monolayer and solution exfoliated WS2. Picosecond-scale features include simultaneous bleaching of excitonic states and a red-shifted absorption spectrum attributed to bandgap renormalization, while free carriers, defect trapped carriers, and recombination signatures are apparent at increasing pico- to nanosecond lifetimes. Features associated with excitons, trions, and photo-excited carriers exhibit strong dependence on local environmental factors. Moisture, oxygen, chemical dopants, and dielectric environment strongly affect the strength and decay lifetimes of these photo-excited species. These results highlight the importance of understanding and controlling these local environmental factors to the rational design and implementation of 2D TMDs optoelectronic device platforms.
Solid-state energy upconversion has many potential applications, from nonlinear photonics and biophotonics to expanding the spectrum available for solar energy harvest. In organic molecular systems, upconversion is frequently done in solution to mitigate aggregation-induced photoluminescence quenching or to facilitate the diffusion of triplet donors in Triplet-Triplet Annihilation (TTA) systems. Here we demonstrate an organic thin film upconversion system utilizing two-photon absorption (TPA) properties to improve upconversion efficiency. In blend films of Stilbene-420 and Rhodamine 6G we observe a tenfold increase in up-converted fluorescence compared to the fluorescence yield of TPA in pristine stilbene films. While TPA normally has quadratic dependence on excitation intensity, these blend films exhibit sub-quadratic intensity dependence, indicating a combination of linear and quadratic upconversion processes and dramatically improving upconversion efficiency at lower excitation intensities. This improvement in intensity dependence allows for relatively efficient upconversion upon excitation by a nanosecond laser pulse, in contrast to the more expensive femtosecond lasers generally required for excitation in TPA microscopy and similar systems. Time-resolved photoluminescence decay measurements reveal that all excited states involved in this upconversion process are singlets, which indicates the potential for reduced energy losses when compared to TTA upconversion systems and their inherent intersystem-crossing energy losses. We observe emission from both the Rhodamine 6G donor molecules and Stilbene-420 acceptor molecules, indicating the presence of prompt fluorescence from the donor as well as upconversion to the acceptor, and FRET losses from acceptor back to donor. By fitting to a kinetic model we extract rates for these competing processes.
We have theoretically and experimentally investigated the effects of Ag-grating electrode on the performance of polymer:fullerene based bulk heterojunction organic solar cells. First, an integrated numerical model has been developed, which is capable of describing both the optical and the electrical properties simultaneously. The Ag-grating patterned back electrode was then designed to enhance the absorption in sub-bandgap region of P3HT:PCBM binary devices. Laser interference lithography and metal lift-off technique were adopted to realize highly-uniform and large-area nanograting patterns. We measured almost 5 times enhancement of the external quantum efficiency at the surface plasmon resonance wavelength. However, the overall improvement in power conversion efficiency was not significant due to the low intrinsic absorption of active layer in this sub-bandgap region. We, then, investigated about the effect of surface plasmon on the ternary device of P3HT:Si-PCPDTBT:ICBA. It was demonstrated that the infrared absorption by the Si-PCPDTBT sensitizer can be substantially enhanced by matching the surface plasmon resonance to the sensitizer absorption band. Besides, we also observed an additional enhancement in the visible range which is due to the scattering effect of the gratings. An overall short-circuit current enhancement of up to 40% was predicted numerically. We have then fabricated the device by the lamination technique and observed a 30% increase in the short circuit current. Plasmon enhancement of sensitized organic solar cell presents a promising pathway to high-efficiency, broadband-absorbing polymer:fullerene bulk heterojunction organic solar cells.
We investigated the ability of silver thin metal films to enhance photovoltaic conversion efficiency in blends of
poly-3-hexylthiophene (P3HT) and methanofullerene [6,6]-phenyl C61-butyric acid methyl ester (PCBM). By varying
the thickness of the silver films and developing a new fabrication routine that involves annealing for long periods of time
at low temperatures, we were able to reproducibly enhance photoconversion in P3HT/PCBM devices. Photovoltaic
conversion efficiency was monitored using internal photon to current conversion efficiency (IPCE) and current-voltage
measurements. We observed that plasmonic materials were able to enhance the conversion efficiencies of organic, bulk
heterojunction devices. The relationship between the surface plasmon resonance wavelength and overall device
performance is also presented with IPCE data. These preliminary studies indicate that plasmonic enhancement in bulk
heterojunction devices show promise to improve the viability of organic solar cells.
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