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Spatially resolved 3D carrier-lifetime maps were measured using 2P tomography to uncover carrier dynamics at buried structures in CdTe thin-films photovoltaics. When thin-film CdTe solar cells are initially deposited, we observe increased nonradiative carrier recombination at GBs throughout the 3D volume of the film, which is most pronounced in the critical junction region where small nucleation grains form at the buried CdTe/CdS interface. The data on CdTe films treated by exposure to CdCl2vapor reveal that a critical function of the treatment is to reduce surface, interface and GB recombination throughout the entirety of these polycrystalline films. The CdCl2treatment may also compensate CdTe films, making it difficult to exceed a hole density of 1015m-3and achieve higher current density and efficiency.

Accurately measuring the bulk minority carrier lifetime is one of the greatest challenges in evaluating photoactive materials used in photovoltaic cells. One-photon time-resolved photoluminescence decay measurements are commonly used to measure lifetimes of direct bandgap materials. However, because the incident photons have energies higher than the bandgap of the semiconductor, most carriers are generated close to the surface, where surface defects cause inaccurate lifetime measurements. Here we show that two-photon absorption permits sub-surface optical excitation, which allows us to decouple surface and bulk recombination processes even in unpassivated samples. Thus with two-photon microscopy we probe the bulk minority carrier lifetime of photovoltaic semiconductors. We demonstrate how the traditional one-photon technique can underestimate the bulk lifetime in a CdTe crystal by 10× and show that two-photon excitation more accurately measures the bulk lifetime. Finally, we generate multi-dimensional spatial maps of optoelectronic properties in the bulk of these materials using two-photon excitation.

Tandem solar cells (TSCs), which use two or more materials to absorb sunlight, have achieved power conversion efficiencies of >25% versus 11-20% for commercialized single junction solar cell modules. The key to widespread commercialization of TSCs is to develop the wide-band, top solar cell that is both cheap to fabricate and has a high open-circuit voltage (i.e. >1V). Previous work in TSCs has generally focused on using expensive processing techniques with slow growth rates resulting in costs that are two orders of magnitude too expensive to be used in conventional solar cell modules. The objective of the PLANT PV proposal was to investigate the feasibility of using Ag(In,Ga)Se2 (AIGS) as the wide-bandgap absorber in the top cell of a thin film tandem solar cell (TSC). Despite being studied by very few in the solar community, AIGS solar cells have achieved one of the highest open-circuit voltages within the chalcogenide material family with a Voc of 949mV when grown with an expensive processing technique (i.e. Molecular Beam Epitaxy). PLANT PV's goal in Phase I of the DOE SBIR was to 1) develop the chemistry to grow AIGS thin films via solution processing techniques to reduce costs and 2) fabricate new devicemore » architectures with high open-circuit voltage to produce full tandem solar cells in Phase II. PLANT PV attempted to translate solution processing chemistries that were successful in producing >12% efficient Cu(In,Ga)Se2 solar cells by replacing copper compounds with silver. The main thrust of the research was to determine if it was possible to make high quality AIGS thin films using solution processing and to fully characterize the materials properties. PLANT PV developed several different types of silver compounds in an attempt to fabricate high quality thin films from solution. We found that silver compounds that were similar to the copper based system did not result in high quality thin films. PLANT PV was able to deposit AIGS thin films using a mixture of solution and physical vapor deposition processing, but these films lacked the p-type doping levels that are required to make decent solar cells. Over the course of the project PLANT PV was able to fabricate efficient CIGS solar cells (8.7%) but could not achieve equivalent performance using AIGS. During the nine-month grant PLANT PV set up a variety of thin film characterization tools (e.g. drive-level capacitance profiling) at the Molecular Foundry, a Department of Energy User Facility, that are now available to both industrial and academic researchers via the grant process. PLANT PV was also able to develop the back end processing of thin film solar cells at Lawrence Berkeley National Labs to achieve 8.7% efficient CIGS solar cells. This processing development will be applied to other types of thin film PV cells at the Lawrence Berkeley National Labs. While PLANT PV was able to study AIGS film growth and optoelectronic properties we concluded that AIGS produced using these methods would have a limited efficiency and would not be commercially feasible. PLANT PV did not apply for the Phase II of this grant.« less