By using femtosecond transient absorption spectroscopy with visible pump and IR probe to observe generation of injected electrons, we could directly observe plasmon-induced electron transfer from 10 nm gold nanodots to TiO2 nanocrystalline film. It was revealed that the reaction time was within 240 fs and the yield was about 40%.
We designed and synthesized new alkyl-functionalized organic dyes, MK-1 and MK-2, for dye-sensitized solar cells (DSSCs). Based on the MK-2 dye, a high performance of efficiency (eta, 7.7%; short-circuit current density Jsc = 14.0 mA cm-2, open-circuit voltage Voc = 0.74 V, and fill factor FF = 0.74) was achieved under AM 1.5 G irradiation (100 mW cm-2). Remarkably, the relatively higher Voc for DSSCs based on MK-1 and MK-2 dyes, which have long alkyl chains, were observed among the organic dyes caused by the increasing of the electron lifetime in the conduction band of TiO2. Our molecular design of alkyl-functionalized dyes strongly suggests the promising performance of molecular photovoltaics based on organic dyes.
Novel organic dyes (MK dyes), which have a carbazole derivative as an electron donor and a cyanoacrylic acid moiety (dC(sCtN)COOH) as an electron acceptor and an anchoring group, connected with n-hexyl-substituted oligothiophenes as a π-conjugated system, were designed and synthesized for application in dye-sensitized solar cells (DSSCs), which are one of the promising molecular photovoltaics. The photovoltaic performance of the DSSCs based on MK dyes markedly depends on the molecular structure of the dyes in terms of the number and position of n-hexyl chains and the number of thiophene moieties. Retardation of charge recombination caused by the existence of n-hexyl chains linked to the thiophene groups resulted in an increase in electron lifetime. As a consequence, an improvement of open-circuit photovoltage (V oc ) and hence the solar-to-electric power conversion efficiency (η) of DSSCs was achieved upon addition of n-hexyl chains to the thiophene groups. In addition, the adsorption condition (amount of dye molecules and/or dye aggregate thickness) on the nanoporous TiO 2 electrode, depending on the number of hexyl chains, strongly affected the performance of DSSCs. A larger amount and/or thicker aggregate of dye molecules brought about longer electron lifetime, which resulted in higher V oc , and slower diffusion of I 3 ions in the nanoporous TiO 2 electrode, which led to lower short-circuit photocurrent (J sc ) and fill factor (FF). In the result of thorough investigation on the series of MK dyes, a DSSC based on MK-2 consisting of n-hexyl-substituted quarter-thiophene produced 8.3% of η (J sc ) 15.22 mA cm -2 , V oc ) 0.73 V, and FF ) 0.75) under 100 mW cm -2 simulated AM1.5G solar irradiation.
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