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The ability to measure microsecond- and nanosecond-scale local dynamics below the diffraction limit with widely available atomic force microscopy hardware would enable new scientific studies in fields ranging from biology to semiconductor physics. However, commercially available scanning-probe instruments typically offer the ability to measure dynamics only on time scales of milliseconds to seconds. Here, we describe in detail the implementation of fast time-resolved electrostatic force microscopy using an oscillating cantilever as a means to measure fast local dynamics following a perturbation to a sample. We show how the phase of the oscillating cantilever relative to the perturbation event is critical to achieving reliable sub-cycle time resolution. We explore how noise affects the achievable time resolution and present empirical guidelines for reducing noise and optimizing experimental parameters. Specifically, we show that reducing the noise on the cantilever by using photothermal excitation instead of piezoacoustic excitation further improves time resolution. We demonstrate the discrimination of signal rise times with time constants as fast as 10 ns, and simultaneous data acquisition and analysis for dramatically improved image acquisition times.

Thin film solar cells made from Cu, Zn, Sn, and S/Se can be processed from solution to yield high-performing kesterite (CZTS or CZTSSe) photovoltaics. We present a microstructural study of solution-deposited CZTSSe films prepared by nanocrystal-based ink approaches using scanning probe microscopy (SPM) and scanning electron microscopy (SEM) coupled with energy dispersive X-ray spectroscopy (EDS). We correlate scanning Kelvin probe microscopy (SKPM) maps of local surface potential with SEM/EDS images of the exact same regions of the film, allowing us to relate observed variations in surface potential to local variations in stoichiometry. Specifically, we find a correlation between surface potential and the S/(S + Se) composition ratio. In particular, we find that regions with high S/(S + Se) ratios are often associated with regions of more negative surface potential and thus higher work function. The change in work function is larger than the expected change in the valence band position with these small changes in sulfur, and thus the data suggest an increase in acceptor-like defects with increasing sulfur. These findings provide new experimental insight into the microscopic relationships between composition, structure, and electronic properties in these promising photovoltaic materials.

We report strong exciton migration with an efficiency of 83.3% from a violet-emitting epitaxial quantum well (QW) to an energy gradient colloidal construct of layered green-and red-emitting nanocrystal quantum dots (NQDs) at room temperature, enabled by the interplay between the exciton population and the depopulation of states in the optical near field. Based on the density matrix formalization of near-field interactions, we theoretically model and demonstrate that the energy gradient significantly boosts the QW-NQDs exciton transfer rate compared to using mono-dispersed NQDs, which is in agreement with the observed experimental results. (C) 2012 American Institute of Physics. [http://dx.doi.org/10.1063/1.4724109]

We proposed and demonstrated architectural tuning of color chromaticity by controlling photoluminescence decay kinetics through nonradiative Förster resonance energy transfer in the heterostructure of layer-by-layer spaced CdTe nanocrystal (NC) solids. We achieved highly sensitive tuning by precisely adjusting the energy transfer efficiency from donor NCs to acceptor NCs via controlling interspacing between them at the nanoscale. By modifying decay lifetimes of donors from 12.05 to 2.96 ns and acceptors from 3.68 to 14.57 ns, we fine-tuned chromaticity coordinates from (x,y) = (0.575,0.424) to (0.632, 0.367). This structural adjustment enabled a postsynthesis color tuning capability, alternative or additive to using the size, shape, and composition of NCs. © 2009 American Institute of Physics.

We use a combination of experiment and modeling to explore the promise and limitations of using plasmon-resonant metal nanoparticles to enhance the device performance of organic photovoltaics (OPVs). We focus on optical properties typical of the current generation of low-bandgap donor polymers blended with the fullerene (6,6)-phenyl C71-butyric acid methyl ester (PC71BM) and use the polymer poly(indacenodithiophene-co-phenanthro[9,10-b]quinoxaline) (PIDT-PhanQ) as our test case. We model the optical properties and performance of these devices both in the presence and absence of a variety of colloidal silver nanoparticles. We show that for these materials, device performance is sensitive to the relative z-position and the density of nanoparticles inside the active layer. Using conservative estimates of the internal quantum efficiency for the PIDT-PhanQ/PC71BM blend, we calculate that optimally placed silver nanoparticles could yield an enhancement in short-circuit current density of over 31% when used with ∼ 80-nm-thick active layers, resulting in an absolute increase in power conversion efficiency of up to ∼2% for the device based on optical engineering.