We developed a new method to accurately extract the singlet exciton diffusion length in organic semiconductors by blending them with a low concentration of methanofullerene[6,6]-phenyl-C 61butyric acid methyl ester (PCBM). The dependence of photoluminescence (PL) decay time on the fullerene concentration provides information on both exciton diffusion and the nanocomposition of the blend. Experimentally measured PL decays of blends based on two narrow band gap dithiophenebenzothiadiazole polymers, C-PCPDTBT and Si-PCPDTBT, were modeled using a Monte Carlo simulation of 3D exciton diffusion in the blend. The simulation software is available for download. The extracted exciton diffusion length is 10.5 AE 1 nm in both narrow band gap polymers, being considerably longer than the 5.4 AE 0.7 nm that was measured with the same technique in the model compound poly(3-hexylthiophene) as a reference. Our approach is simple, fast and allows us to systematically measure and compare exciton diffusion length in a large number of compounds.
The temperature dependence of the exciton dynamics in a conjugated polymer is studied using time-resolved spectroscopy. Photoluminescence decays were measured in heterostructured samples containing a sharp polymer-fullerene interface, which acts as an exciton quenching wall. Using a 1D diffusion model, the exciton diffusion length and diffusion coefficient were extracted in the temperature range of 4-293 K. The exciton dynamics reveal two temperature regimes: in the range of 4-150 K, the exciton diffusion length (coefficient) of approximately 3 nm (approximately 1.5 x 10 (-4) cm2/s) is nearly temperature independent. Increasing the temperature up to 293 K leads to a gradual growth up to 4.5 nm (approximately 3.2 x 10 (-4) cm2/ s). This demonstrates that exciton diffusion in conjugated polymers is governed by two processes: an initial downhill migration toward lower energy states in the inhomogenously broadened density of states, followed by temperature activated hopping. The latter process is switched off below 150 K.
Nanocrystal/fullerene derivative inorganic-organic hybrid photodetectors exhibiting high detectivity for near-IR wavelengths and a linear power dependence are produced. The ultrafast electron transfer from the PbS crystals to the fullerene opens a new route to obtaining efficient photodetectors that are appealing, cost-effective alternatives to the currently available technology
Temperature‐dependent studies of the electrical and optical properties of cross‐linked PbS nanocrystal (NC) solar cells can provide deeper insight into their working mechanisms. It is demonstrated that the overall effect of temperature on the device efficiency originates from the temperature dependence of the open‐circuit voltage and the short‐circuit current, while the fill factor remains approximately constant. Extensive modeling provides signs of band‐like transport in the inhomogeneously coupled NC active layer and shows that the charge transport is dominated by diffusion. Moreover, via low temperature absorption and photoluminescence (PL) measurements, it is shown that the optical properties of PbS thin films before and after benzenedithiol (BDT) treatment exhibit very distinct behavior. After BDT treatment, both the optical density (OD) and PL are shifted to lower energies, indicating the occurrence of electronic wave function overlap between adjacent NCs. Decrease of the temperature leads to additional red‐shift of the OD and PL spectra, which is explained by the well‐known temperature dependence of the PbS NCs' bandgap. Moreover, BDT treated PbS NCs show unusual properties, such as decrease of the PL signal and broadening of the spectra at low temperatures. These features can be attributed to the partial relaxation of the quantum confinement and the opening of new radiative and nonradiative pathways for recombination at lower temperatures due to the presence of trap states.
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