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In photovoltaic devices, the bulk disorder introduced by grain boundaries (GBs) in polycrystalline silicon is generally considered to be detrimental to the physical stability and electronic transport of the bulk material. However, at the extremum of disorder, amorphous silicon is known to have a beneficially increased band gap and enhanced optical absorption. This study is focused on understanding and utilizing the nature of the most commonly encountered Σ3 GBs, in an attempt to balance incorporation of the advantageous properties of amorphous silicon while avoiding the degraded electronic transport of a fully amorphous system. A combination of theoretical methods is employed to understand the impact of ordered Σ3 GBs on the material properties and full-device photovoltaic performance.

Strain in a material induces shifts in vibrational frequencies, which is a probe of the nature of the vibrations and interatomic potentials, and can be used to map local stress/strain distributions via Raman microscopy. This method is standard for crystalline silicon devices, but due to lack of calibration relations, it has not been applied to amorphous materials such as hydrogenated amorphous silicon (a-Si:H), a widely studied material for thin-film photovoltaic and electronic devices. We calculated the Raman spectrum of a-Si:H \ab initio under different strains $\epsilon$ and found peak shifts $\Delta \omega = \left( -460 \pm 10\ \mathrm{cm}^{-1} \right) {\rm Tr}\ \epsilon$. This proportionality to the trace of the strain is the general form for isotropic amorphous vibrational modes, as we show by symmetry analysis and explicit computation. We also performed Raman measurements under strain and found a consistent coefficient of $-510 \pm 120\ \mathrm{cm}^{-1}$. These results demonstrate that a reliable calibration for the Raman/strain relation can be achieved even for the broad peaks of an amorphous material, with similar accuracy and precision as for crystalline materials., Comment: 12 pages, 3 figures + supplementary 8 pages, 4 figures

With the advent of high-bandgap perovskites, the opportunity now exists to make tandems with perovskites on top of silicon. We have prototyped a mechanically stacked tandem, achieving 17.9% certified efficiency using a perovskite cell with a silver nanowire mesh electrode. We have also prototyped a monolithically integrated tandem on silicon, with the two subcells electronically connected by band-to-band tunneling in the silicon. The primary challenges to propelling perovskite/silicon tandems into a high-efficiency (>25%) regime are spiro-OMeTAD parasitic absorption, perovskite crystal quality, stability of a perovskite with a 1.8 eV bandgap, perovskite environmental stability, and transparent electrode quality and stability.

In this work we aim to connect atomic structure to observed mobility through a series of experiments, leveraging computational simulations to correlate atomic-level phenomena with empirical mobility trends, providing insight into the shifting regimes of prevalent defects. The work is conducted in three main thrusts: First, through experimental measurements of a-Si:H hole mobility over a wide range of deposition conditions, we correlate the mobility with independent measurements of film intrinsic stress, and hydrogen concentration and bonding configuration. We show that the peak mobility values occur at moderately compressive values of stress, away from theextremaofeitherhydrogenbondingconcentration.Second, by extending our previous computational study of structural defects in a-Si:H to include variations in both biaxial stress and hydrogen concentration, we are able to hypothesize on the sources of defects in the various experimental conditions of the material, as well as design experiments to validate thesetheories.Finally,wedeconvolutethestressandhydrogen contents in our as-deposited films and thereby provide experimental evidence to corroborate our computational theories as to the dominant defects and their sources in the continuum of experimental samples produced.

Genetic programming is used to identify the structural features most strongly associated with hole traps in hydrogenated nanocrystalline silicon with very low crystalline volume fraction. The genetic programming algorithm reveals that hole traps are most strongly associated with local structures within the amorphous region in which a single hydrogen atom is bound to two silicon atoms (bridge bonds), near fivefold coordinated silicon (floating bonds), or where there is a particularly dense cluster of many silicon atoms. Based on these results, we propose a mechanism by which deep hole traps associated with bridge bonds may contribute to the Staebler-Wronski effect.

The adoption of amorphous silicon based solar cells has been drastically hindered by the low efficiency of these devices, which is mainly due to a low hole mobility. It has been shown that using both crystallized and amorphous silicon layers in solar cells leads to an enhancement of the device performance. In this study the crystallization of a-Si prepared by PECVD under various growth conditions has been investigated. The growth stresses in the films are determined by measuring the curvature change of the silicon substrate before and after film deposition. Localized crystallization is induced by exposing a-Si films to focused 532 nm laser beam of power ranging from 0.08 to 8 mW. The crystallization process is monitored by recording the Raman spectra after various exposures. The results suggest that growth stresses in the films affect the minimum laser power (threshold power). In addition, a detailed analysis of the width and position of the Raman signal indicates that the silicon grains in the crystallized regions are of few nm diameter.

Hydrogenated amorphous silicon (a-Si:H) refers to a broad class of atomic configurations, sharing a lack of long-range order, but varying significantly in material properties, including optical constants, porosity, hydrogen content, and intrinsic stress. It has long been known that deposition conditions affect microstructure, but much work remains to uncover the correlation between these parameters and their influence on electrical, mechanical, and optical properties critical for high-performance a-Si:H photovoltaic devices. We synthesize and augment several previous models of deposition phenomena and ion bombardment, developing a refined model correlating plasma-enhanced chemical vapor deposition conditions (pressure and discharge power and frequency) to the development of intrinsic stress in thin films. As predicted by the model presented herein, we observe that film compressive stress varies nearly linearly with bombarding ion momentum and with a (\ensuremath{-}1/4) power dependence on deposition pressure, that tensile stress is proportional to a reduction in film porosity, and the net film intrinsic stress results from a balance between these two forces. We observe the hydrogen-bonding configuration to evolve with increasing ion momentum, shifting from a void-dominated configuration to a silicon-monohydride configuration. Through this enhanced understanding of the structure-property-process relation of a-Si:H films, improved tunability of optical, mechanical, structural, and electronic properties should be achievable.

Low hole mobility severely limits the conversion efficiencies of amorphous silicon (a-Si) solar cells. Previously it has been proposed that carrier mobility can be improved by introducing certain types of stress into thin films. In this work we explore a range of deposition conditions allowing the formation of intrinsic stresses varying from −924 MPa compressive to 386 MPa tensile. We then discuss the origins of these stresses due to ion bombardment, presenting a model correlating our deposition parameters with our observed stress measurements. In doing so we elucidate the non-linear relationship between deposition pressure and the films intrinsic stress.

With the advent of efficient high-bandgap metal-halide perovskite photovoltaics, an opportunity exists to make perovskite/silicon tandem solar cells. We fabricate a monolithic tandem by developing a silicon-based interband tunnel junction that facilitates majority-carrier charge recombination between the perovskite and silicon sub-cells. We demonstrate a 1 cm2 2-terminal monolithic perovskite/silicon multijunction solar cell with a VOC as high as 1.65 V. We achieve a stable 13.7% power conversion efficiency with the perovskite as the current-limiting sub-cell, and identify key challenges for this device architecture to reach efficiencies over 25%.

While low hole mobilities limit the current collection and efficiency of hydrogenated amorphous silicon (a-Si:H) photovoltaic devices, attempts to improve mobility of the material directly have stagnated. Herein, we explore a method of utilizing nanostructuring of a-Si:H devices to allow for improved hole collection in thick absorber layers. This is achieved by etching an array of 150 nm diameter holes into intrinsic a-Si:H and then coating the structured material with p-type a-Si:H and a conformal zinc oxide transparent conducting layer. The inclusion of these nanoholes yields relative power conversion efficiency (PCE) increases of ∼45%, from 7.2 to 10.4% PCE for small area devices. Comparisons of optical properties, time-of-flight mobility measurements, and internal quantum efficiency spectra indicate this efficiency is indeed likely occurring from an improved collection pathway provided by the nanostructuring of the devices. Finally, we estimate that through modest optimizations of the design and fabrication, PCEs of beyond 13% should be obtainable for similar devices.