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The present work provides an overview of radiative performance losses in thin-film solar cells, focusing on those related to the open-circuit voltage, using (Ag,Cu)(In,Ga)Se2 devices as examples. The microscopic origins of these losses are outlined, highlighting the presence of compositional variations, strain, and inhomogeneously distributed point defects on various length scales as contributors to band-gap and electrostatic potential fluctuations, which both contribute to the broadening of the absorption edge in the absorptance or quantum efficiency spectra of the semiconductor absorber layer or the completed solar-cell device. The relationship between this broadening and Urbach tails is discussed. It is shown that the photovoltaic band-gap energy as well as the broadening can be reliably determined from the arithmetic mean and standard deviation extracted from Gaussian fits to the first derivative of the absorptance or quantum efficiency spectra around the absorption edge. The more enhanced the broadening, the more the local maximum in the luminescence spectrum shifts to smaller energies with respect to the band-gap energy of the absorber layer, as verified for about 30 (Ag,Cu)(In,Ga)Se2 solar cells. [ABSTRACT FROM AUTHOR]

A new method for efficiently converting electron backscatter diffraction data obtained using serial sectioning by focused ion beam of a polycrystalline thin film into a computational, three-dimensional (3D) structure is presented. The reported data processing method results in a more accurate representation of the grain surfaces, reduced computer memory usage, and improved processing speed compared to traditional voxel methods. The grain structure of a polycrystalline absorption layer from a high-efficiency Cu(In,Ga)Se2 solar cell (19.5%) is reconstructed in 3D and the grain size and surface distribution is investigated. The grain size distribution is found to be best fitted by a log-normal distribution. We further find that the grain size is determined by the [Ga]/([Ga] + [In]) ratio in vertical direction, which was measured by glow discharge optical emission spectroscopy. Finally, the 3D model derived from the structural information is applied in optoelectronic simulations, revealing insights into the effects of grain boundary recombination on the open-circuit voltage of the solar cell. An accurate 3D structure like the one obtained with our method is a prerequisite for a detailed understanding of mechanical properties and for advanced optical and electronic simulations of polycrystalline thin films. [ABSTRACT FROM AUTHOR]

A dimethylformamide (DMF) and thiourea (TU)‐based ink deposition route is used to fabricate narrow bandgap (≈1.0 eV) CuIn(S,Se)2 (CISSe) films with Cu‐poor ([Cu]/[In] = 0.85), stoichiometric ([Cu]/[In] = 1.0), and Cu‐rich ([Cu]/[In] = 1.15) compositions for photovoltaic applications. Characterization of KCN‐ or (NH4)2S‐treated Cu‐rich absorber films using X‐ray diffraction and scanning electron microscopy confirms the removal of copper‐selenide phases from the film surface, while electron backscatter diffraction measurements and depth‐dependent energy‐dispersive X‐ray spectroscopy indicate remnant copper‐selenides in the absorber layer bulk. Contrary to best practice for vacuum‐processed cells, optimum [Cu]/[In] ratios appear to be stoichiometric, rather than Cu‐poor, in DMF–TU‐based CISSe devices. Accordingly, stoichiometric film compositions yield large‐grained (≈2 μm) absorber layers with smooth absorber surfaces (root mean square roughness <20 nm) and active area device efficiencies of 13.2% (without antireflective coating). Notably, these devices reach 70.0% of the Shockley–Queisser limit open‐circuit voltage (i.e., 526 mV at Eg of 1.01 eV), which is among the highest for ink‐based CISSe devices. [ABSTRACT FROM AUTHOR]

Outstanding optoelectronic properties of mixed tin‐lead perovskites are the cornerstone for the development of high‐efficiency all‐perovskite tandems. However, recombination losses in Sn‐Pb perovskites still limit the performance of these perovskites, necessitating more fundamental research. Here, rubidium iodide is employed as an additive for methylammonium‐free Sn‐Pb perovskites. It is first investigated the effect of the RbI additive on the perovskite composition, crystal structure, and element distribution. Quasi‐Fermi level splitting and transient photoluminescence measurements reveal that the RbI additive reduces recombination losses and increases carrier lifetime of the perovskite films. This finding is attributed to an approximately ten‐fold reduction in the defect density following RbI treatment, as probed using constant final state yield photoelectron spectroscopy. Additionally, the concentration of Sn vacancies is also reduced, and the perovskite film becomes less p‐type both in the bulk and at the interface towards the electron contact. Thus, the conductivity for electrons increases, improving carrier extraction. As a result, the open‐circuit voltage of RbI‐containing solar cells improves by 61 mV on average, with the best efficiency >20%. This comprehensive study demonstrates that RbI is effective at reducing recombination losses and carrier trapping, paving way for a new approach to Sn‐Pb perovskite solar cell research. [ABSTRACT FROM AUTHOR]

Hydrogen‐doped In2O3 (In2O3:H) is highly conductive while maintaining extraordinary transparency, thus making it a very attractive material for applications in optoelectronic devices such as (multijunction) solar cells or light‐emitting devices. However, the corresponding metal/In2O3:H contacts may exhibit undesirably high resistances, significantly deteriorating device performance. To gain insight into the underlying efficiency‐limiting mechanism, hard X‐ray photoelectron spectroscopy is employed to in‐situ monitor annealing‐induced changes in the chemical structure of the Ag/In2O3:H interface system that is further complemented by ex‐situ electron microscopy analyses and contact resistance measurements. The observed evolution of the Ag‐ and In‐related photoelectron line intensities can be explained by significant intermixing across the Ag/In2O3:H interface. The corresponding lineshape broadening of the Ag 3d spectra is attributed to the formation of Ag2O and AgO, which becomes significant at temperatures above approximately 160 °C. However, after annealing to 300 °C, instead of the formation of an insulating AgOx interfacial layer, it is found i) In to be rather homogeneously distributed in the complete Ag/In2O3:H stack, ii) Ag diffusing into the In2O3:H, and iii) an improvement of the contact resistance rather than its often‐reported deterioration. [ABSTRACT FROM AUTHOR]

Polycrystalline Cu(In,Ga)Se2 (CIGSe) thin‐film solar cells exhibit gradual onset in their external quantum efficiency (EQE) spectra whose shape can be affected by various CIGSe material properties. Apart from influences on the charge‐carrier collection, a broadening of the EQE onset leads to enhanced radiative losses in open‐circuit voltage (Voc). In the present work, Gaussian broadening of parameters describing the EQE onset of thin‐film solar cells, represented by the standard deviation, 휎total, was evaluated to study the impacts of the effective band‐gap energy, the electron diffusion length, and the Ga/In gradient in the CIGSe absorber. It is shown that 휎total can be disentangled into contributions of these material properties, in addition to a residual component 휎residual. Effectively, 휎total depends only on a contribution related to the Ga/In gradient as well as on 휎residual. The present work highlights the connection of this compositional gradient, the microstructure in the polycrystalline CIGSe absorber, and the luminescence emission with the residual component 휎residual. It is demonstrated that a flat band‐gap with no compositional gradient in the bulk of the CIGSe absorber is essential to obtain the lowest 휎total values and thus result in lower recombination losses and gains in Voc. [ABSTRACT FROM AUTHOR]

Copper indium selenide chalcopyrite-structure alloys with gallium (CIGS) are unique among the highest performing photovoltaic (PV) semiconductor technologies. They are structurally disordered, nonstoichiometric materials that have been engineered to achieve remarkably low bulk nonradiative recombination levels. Nevertheless, their performance can be further improved. This review adopts a fundamental thermodynamic perspective to comparatively assess the root causes of present limitations on CIGS PV performance. The topics of selectivity and passivation of contacts to CIGS and its multinary alloys are covered, highlighting pathways to maximizing the electrochemical potential between those contacts under illumination. An overview of absorber growth methods and resulting properties is also provided. We recommend that CIGS researchers consider strategies that have been successfully implemented in the more mature wafer-based GaAs and Si PV device technologies, based on the paradigm of an idealized PV device design using an isotropic absorber with minimal nonradiative recombination, maximal light trapping, and both electron-selective and hole-selective passivated contacts. We foresee that CIGS technology will reach the 25% efficiency level within the next few years through enhanced collection and reduced recombination. To significantly impact power-generation applications, cost-effective, manufacturable solutions are also essential. [ABSTRACT FROM AUTHOR]

It is attractive to alloy Cu(In,Ga)Se2 solar‐cell absorbers with Ag (ACIGSe), since they lead to similar device performances as the Ag‐free absorber layers, while they can be synthesized at much lower deposition temperatures. However, a KF post‐deposition treatment (PDT) of the ACIGSe absorber surface is necessary to achieve higher open‐circuit voltages (Voc). The present work provides microscopic insights to the effects of this KF PDT, employing correlative scanning‐electron microscope techniques on identical positions of cross‐sectional specimens of the cell stacks. We found that the increase in Voc after the KF PDT can be explained by the removal of Cu‐poor, Ag‐poor, and Ga‐rich regions near the ACIGSe/CdS interface. The KF PDT leads, when optimally doped, to a very thin K‐Ag‐Cu‐Ga‐In‐Se layer between ACIGSe and CdS. If the KF dose is too large, we find that Cu‐poor and K‐rich regions form near the ACIGSe/CdS interface with enhanced nonradiative recombination which explains a decrease in the Voc. This effect occurs in addition to the presence of a (K,Ag,Cu)InSe2 intermediate layer, that might be responsible for limiting the short‐current density of the solar cells due to a current blocking behavior. [ABSTRACT FROM AUTHOR]

High‐efficiency Cu(In,Ga)Se2 (CIGS) thin‐film solar cells are based on polycrystalline CIGS absorber layers, which contain grain boundaries, stacking faults, and dislocations. While planar defects in CIGS layers have been investigated extensively, little is still known about the impact of dislocations on optoelectronic properties of CIGS absorbers. Herein, evidence for an optoelectronic inactivity of dislocations in these thin films is given, in contrast to the situation at grain boundaries. This unique behavior is explained by the extensive elemental redistribution detected around dislocation cores, which is connected with the dislocation strain field, probably leading to a shift of defect states toward the band edges. [ABSTRACT FROM AUTHOR]

Interface recombination at the absorber surface impedes the efficiency of a solar cell with an otherwise excellent absorber. The internal voltage or quasi‐Fermi‐level splitting (qFLs) measures the quality of the absorber. Interface recombination reduces the open‐circuit voltage (VOC) with respect to the qFLs. A facile solution‐based sulfur postdeposition treatment (S‐PDT) is explored to passivate the interface of CuInS2 grown under Cu‐rich conditions, which show excellent qFLs values, but much lower VOCs. The absorbers are treated in S‐containing solutions at 80 °C. Absolute calibrated photoluminescence and current–voltage measurements demonstrate a reduction of the deficit between qFLs and VOC by almost one‐third compared with the untreated device. Temperature dependence of the open‐circuit voltage shows increased activation energy for the dominant recombination path, indicating less interface recombination. In addition, capacitance transients reveal the presence of slow metastable defects in the untreated solar cell. The slow response is considerably reduced by the S‐PDT, suggesting passivation of these slow metastable defects. The results demonstrate the effectiveness of solution‐based S‐treatment in passivating defects, presenting a promising strategy to explore and reduce defect states near the interface of chalcogenide semiconductors. [ABSTRACT FROM AUTHOR]

In Cu(In,Ga)Se2 (CIGS) thin‐film solar cells, laterally inhomogeneous distributions of point defects may induce electrostatic potential fluctuations and thus reduce the open‐circuit voltage (Voc). In the present work, we investigate possible origins of fluctuating potentials and estimate the amplitude of fluctuations and Voc losses in solar cells with various [Ga] in the CIGS absorber, with different buffer layers and with different durations of an RbF postdeposition treatment (PDT). Electron‐beam‐induced current measurements were employed to study the local difference in the width of the space‐charge region (wSCR). It is shown that the amplitude of fluctuations in the wSCR depends significantly on the choice of buffer system and on the duration of the RbF PDT. In addition, energy‐dispersive X‐ray spectroscopy and cathodoluminescence measurements reveal that band‐gap fluctuations do not have substantial impact on the device performance. Finally, some of the investigated cells were exposed to light soaking, which was found to be a means to reduce the detected electrostatic potential fluctuations and also to increase the effective electron diffusion length in the CIGS absorber for a part of the investigated cells. [ABSTRACT FROM AUTHOR]

Abstract: The unprecedented speed at which the performance of solar cells based on solution‐processed perovskite thin films has increased, in some ways, appears to violate conventional understanding of device optimization. The relatively poor coverage of the TiO2 electron transport layer by the absorber should cause shunting of the cell. This, however, is not the case. In this paper, it is attempted to explain this “discrepancy.” Insights into coverage, morphology, local elemental composition, and spatially resolved electronic structure of CH3NH3PbI(3−x)Clx perovskite absorbers wet‐chemically deposited on planar compact TiO2 electron transport material (ETM) are revealed. Microscopy images indicate an incomplete coverage of the ETM. Depending on the degree of coverage, a variation in iodine oxidation and metallic lead formation is found. With the electronic structure of the absorber and the ETM established experimentally and taking literature on the commonly used hole transport material spiro‐MeOTAD into account, it is revealed that excellent charge selectivity occurs at the interfaces between the absorber and both the hole and electron transport layers. It can also be surmised that, crucially, any direct interface between the TiO2 and spiro‐MeOTAD would be characterized by a large recombination barrier preventing shunts; to some extent minimizing the negative effects of absorber pinholes. [ABSTRACT FROM AUTHOR]

In the present work, a brief overview is given on how to apply transmission (TEM) as well as scanning electron microscopy (SEM) and their related techniques (electron diffraction, energy-dispersive X-ray spectrometry, electron energy-loss spectroscopy, electron holography; electron backscatter diffraction, electron-beam-induced current, cathodoluminescence) for the analysis of interfaces between individual layers or extended structural defects in a thin-film stack. All examples given in the present work were recorded on Cu(In, Ga)Se 2 thin film solar cells, however, the shown experimental approaches may be used on any similar thin-film semiconductor device. A particular aspect is the application of various techniques on the same identical specimen area, in order to enhance the insight into structural, compositional, and electrical properties. For (aberration-corrected) TEM, the spatial resolutions of such measurements can be as low as on the subnanometer scale. However, when dealing with semiconductor devices, it is often necessary to characterize electrical and optoelectronic properties at larger scales, of few 10 nm up to even mm, for which SEM is more appropriate. At the same time, these larger scales provide also enhanced statistics of the analysis. In the present review, it is also outlined how to apply SEM techniques in combination with scanning-probe and optical microscopy, on the same identical positions. Altogether, a multiscale toolbox is provided for the thorough analysis of structure-property relationships in thin-film solar cells using correlative microscopy approaches. [ABSTRACT FROM AUTHOR]

The present contribution is a summary of an event that was organized as a special evening session in Symposium V “Chalcogenide Thin-Film Solar Cells” at the E-MRS 2016 Spring Meeting, Lille, France. The presentations in this session were given by the coauthors of this paper. These authors present retrospectives of key developments in the field of Cu(In,Ga)(S,Se) 2 solar cells as they themselves had witnessed in their laboratories or companies. Also, anecdotes are brought up, which captured interesting circumstances in that evolutionary phase of the field. Because the focus was on historical perspectives rather than a comprehensive review of the field, recent developments intentionally were not addressed. [ABSTRACT FROM AUTHOR]

We study the sequential fabrication of Cu(In,Ga)Se2 (CIGSe) absorber layers by using an atmospheric pressure selenization with a process duration of only a few minutes and the utilization of elemental selenium vapor from independent Se sources. This technology could proof to be an industrially relevant technology for the fabrication of thin-film solar cells. Controlling the amount of Se provided during the selenization of metal precursors is shown to be an effective measure to adjust the Ga in-depth distribution. A reduced Se supply for CIGSe formation leads to a more homogeneous Ga distribution within the absorber. The underlying growth dynamics is investigated by interrupting the selenization at different times. At first, CIGSe formation occurs in accordance with previously suggested growth paths and Ga segregates at the Mo back contact. Between 520 and 580 °C, the growth dynamics differs distinctly, and In and Ga distribute far more uniformly within the absorber depth. We also studied the impact of the precursor architecture. The best performing precursor in terms of efficiency of the respective solar cells was a multilayer with 22 In/CuGa/In triple layers. Simple bilayers stacks lead to films of higher roughness and correlated shunting. By optimizing the precursor architecture and the Ga in-depth distribution in the CIGSe layer, a conversion efficiency of up to 15.5% (active area) could be achieved. To our knowledge, this is the highest reported efficiency for sulfur free CIGSe-based solar cells utilizing fast (few minutes) atmospheric processes and elemental Se vapor. Copyright © 2017 John Wiley & Sons, Ltd. [ABSTRACT FROM AUTHOR]

Thin-film solar cells based on polycrystalline Cu(In,Ga)Se 2 absorbers exhibit record conversion efficiencies of up to 22.6%. There is still a lack of a quantitative connection between the grain-boundary character distribution (GBCD) and the corresponding electrical and optoelectronic properties. The present work uses microstructural data from a CuInSe 2 thin film acquired by electron backscatter diffraction (EBSD) to evaluate the GBCD. The most prominent features of the GBCD of CuInSe 2 are Σ3 twin boundaries and the Σ9 and Σ27a symmetric tilt grain boundaries. Moreover, combining EBSD with electron-beam-induced current and cathodoluminescence (measurements on the same identical area) on a CuInSe 2 /Mo/glass stack provide the means to relate the grain-boundary character with the corresponding electrical and optoelectronic signals across the grain boundary. In part, determining this relationship is accomplished by means of correlation analysis using measurement data from more than 100 grain boundaries. However, the crystallographic, electrical and optoelectronic data showed no strong correlations, which is attributed to atomic reconstruction found in atomic planes adjacent to planar defects in polycrystalline CuInSe 2 thin films and corresponding reductions of excess charge densities at these defects. [ABSTRACT FROM AUTHOR]

Si thin films on glass grown by liquid phase crystallization (LPC) exhibit large grains resembling those in multicrystalline Si wafers. The present work gives direct insight into how planar defects in LPC-Si thin films influence the device performance of the corresponding solar cells by acquiring electron-backscatter diffraction maps and measuring solar cell parameters on the same identical positions. By this approach, it was possible to demonstrate how low scanning velocities of the laser line during the crystallization lead to lower densities of grain boundaries, to improved charge-carrier diffusion lengths, and hence to improved device performances. [ABSTRACT FROM AUTHOR]

The present review gives an overview of the various reports on properties of line and planar defects in Cu(In,Ga)(S,Se)2 thin films for high-efficiency solar cells. We report results from various analysis techniques applied to characterize these defects at different length scales, which allow for drawing a consistent picture on structural and electronic defect properties. A key finding is atomic reconstruction detected at line and planar defects, which may be one mechanism to reduce excess charge densities and to relax deep-defect states from midgap to shallow energy levels. On the other hand, nonradiative Shockley-Read-Hall recombination is still enhanced with respect to defect-free grain interiors, which is correlated with substantial reduction of luminescence intensities. Comparison of the microscopic electrical properties of planar defects in Cu(In,Ga)(S,Se)2 thin films with two-dimensional device simulations suggest that these defects are one origin of the reduced open-circuit voltage of the photovoltaic devices. (© 2016 WILEY-VCH Verlag GmbH &Co. KGaA, Weinheim) [ABSTRACT FROM AUTHOR]

The gallium gradient in Cu(In,Ga)Se2 (CIGS) layers, which forms during the two industrially relevant deposition routes, the sequential and co-evaporation processes, plays a key role in the device performance of CIGS thin-film modules. In this contribution, we present a comprehensive study on the formation, nature, and consequences of gallium gradients in CIGS solar cells. The formation of gallium gradients is analyzed in real time during a rapid selenization process by in situ X-ray measurements. In addition, the gallium grading of a CIGS layer grown with an in-line co-evaporation process is analyzed by means of depth profiling with mass spectrometry. This gallium gradient of a real solar cell served as input data for device simulations. Depth-dependent occurrence of lateral inhomogeneities on the µm scale in CIGS deposited by the co-evaporation process was investigated by highly spatially resolved luminescence measurements on etched CIGS samples, which revealed a dependence of the optical bandgap, the quasi-Fermi level splitting, transition levels, and the vertical gallium gradient. Transmission electron microscopy analyses of CIGS cross-sections point to a difference in gallium content in the near surface region of neighboring grains. Migration barriers for a copper-vacancy-mediated indium and gallium diffusion in CuInSe2 and CuGaSe2 were calculated using density functional theory. The migration barrier for the InCu antisite in CuGaSe2 is significantly lower compared with the GaCu antisite in CuInSe2, which is in accordance with the experimentally observed Ga gradients in CIGS layers grown by co-evaporation and selenization processes. Copyright © 2014 John Wiley & Sons, Ltd. [ABSTRACT FROM AUTHOR]

Nanocrystal-based Cu2Zn(SnyGe1-y)(SxSe4-x) (CZTGeSSe) thin-film solar cell absorbers with tunable band gap have been prepared. Maximum solar-conversion total area efficiencies of up to 9.4% are achieved with a Ge content of 30 at.%. Improved performance compared with similarly processed films of Cu2ZnSn(SxSe4-x) (CZTSSe, 8.4% efficiency) is achieved through controlling Ge loss from the bulk of the absorber film during the high-temperature selenization treatment, although some Ge loss from the absorber surface is still observed following this step. Despite limitations imposed by elemental losses present at the absorber surface, we find that Ge alloying leads to enhanced performance due to increased minority charge carrier lifetimes as well as reduced voltage-dependent charge carrier collection. Copyright © 2013 John Wiley & Sons, Ltd. [ABSTRACT FROM AUTHOR]

The correct version of the fourth sentence in the caption of Table 1 states "The I V i SB oc sb value in parentheses (720 mV) is the one for a CIGSe layer exhibiting band-gap fluctuations." instead of the original, incorrect "The I V i SB oc sb value in parentheses is the one for a CIGSe layer free of band-gap fluctuations.". The first sentence of the sixth paragraph of the subsection "Cathodoluminescence (CL) behavior of the CIGSe absorber" in Results contained an error and originally incorrectly read " I S i SB GB sb can be written as 1/4 I N i SB GB sb I i SB e sb I v i SB th sb ". The original version of this Article contained errors in Table 1. [Extracted from the article]

Thin-film solar cells based on polycrystalline absorbers have reached very high conversion efficiencies of up to 23-25%. In order to elucidate the limiting factors that need to be overcome for even higher efficiency levels, it is essential to investigate microscopic origins of loss mechanisms in these devices. In the present work, a high efficiency (21% without anti-reflection coating) copper indium gallium diselenide (CIGSe) solar cell is characterized by means of a correlative microscopy approach and corroborated by means of photoluminescence spectroscopy. The values obtained by the experimental characterization are used as input parameters for two-dimensional device simulations, for which a real microstructure was used. It can be shown that electrostatic potential and lifetime fluctuations exhibit no substantial impact on the device performance. In contrast, nonradiative recombination at random grain boundaries can be identified as a significant loss mechanism for CIGSe solar cells, even for devices at a very high performance level. Achieving higher efficiencies for thin-film solar cells always requires identification of the limiting factors. Here Krause et al. show that inhomogeneously distributed net doping or lifetime have little impact while recombination at grain boundaries is one of the main loss mechanisms for high performance Cu(In,Ga)Se2 solar cells. [ABSTRACT FROM AUTHOR]

Thin‐film solar cells based on Cu(In,Ga)Se2 (CIGSe) absorber layers reach conversion efficiencies of above 20%. One key to this success is the incorporation of alkali metals, such as Na and K, into the surface and the volume of the CIGSe thin film. The present work discusses the impact of Na and K on the grain‐boundary (GB) properties in CIGSe thin films, i.e., on the barriers for charge carriers, Φb, and on the recombination velocities at the GBs, sGB. First, the physics connected with these two quantities as well as their impact on the device performance are revised, and then the values for the barrier heights and recombination velocities are provided from the literature. The sGB values are measured by means of a cathodoluminescence analysis of Na‐/K‐free CIGSe layers as well as on CIGSe layers on Mo/sapphire substrates, which are submitted to only NaF or only KF postdeposition treatments. Overall, passivating effects on GBs by neither Na nor K can be confirmed. The GB recombination velocities seem to remain on the same order of magnitude, in average about 103–104 cm s−1, irrespective of whether CIGSe thin films are Na‐/K‐free or Na‐/K‐containing. [ABSTRACT FROM AUTHOR]

The present work describes the approach of how to determine local orientations in individual CuInSe2 grains from electron‐backscatter diffraction (EBSD) data, in spite of the very small deviation (0.3%) of the ratio of lattice constants of the tetragonal crystal structure, c/a, from the value in the pseudocubic case, 2. A dictionary‐based indexing algorithm is applied on each EBSD pattern, determining unambiguously the corresponding CuInSe2 crystal orientation of the tetragonal structure. The approach provided in the present work can be used to improve the studies of microstructure–property relationships in various relevant photovoltaic material systems with similar pseudosymmetrical crystal structures, such as kesterite‐type or halide‐perovskite thin films. [ABSTRACT FROM AUTHOR]

A new method for efficiently converting electron backscatter diffraction data obtained using serial sectioning by focused ion beam of a polycrystalline thin film into a computational, three-dimensional (3D) structure is presented. The reported data processing method results in a more accurate representation of the grain surfaces, reduced computer memory usage, and improved processing speed compared to traditional voxel methods. The grain structure of a polycrystalline absorption layer from a high-efficiency Cu(In,Ga)Se2 solar cell (19.5%) is reconstructed in 3D and the grain size and surface distribution is investigated. The grain size distribution is found to be best fitted by a log-normal distribution. We further find that the grain size is determined by the [Ga]/([Ga] + [In]) ratio in vertical direction, which was measured by glow discharge optical emission spectroscopy. Finally, the 3D model derived from the structural information is applied in optoelectronic simulations, revealing insights into the effects of grain boundary recombination on the open-circuit voltage of the solar cell. An accurate 3D structure like the one obtained with our method is a prerequisite for a detailed understanding of mechanical properties and for advanced optical and electronic simulations of polycrystalline thin films. [ABSTRACT FROM AUTHOR]

The selenization of metallic Cu-Zn-Sn-Ge precursors is a promising route for the fabrication of low-cost and efficient kesterite thin-film solar cells. Nowadays, efficiencies of kesterite solar cells are still below 13%. For Cu(In,Ga)Se2 solar cells, the formation of compositional gradients along the depth of the absorber layer has been demonstrated to be a key requirement for producing thin-film solar cells with conversion efficiencies above the 22% level. No clear understanding has been reached so far about how to produce these gradients in an efficient manner for kesterite compounds, but among the possible candidates, Ge arises as one of the most promising ones. In the present work, we evaluate the potential of incorporating Ge in Cu2ZnSnSe4 to produce compositional gradients in kesterites. Synchrotron-based in situ energy-dispersive X-ray diffraction and X-ray fluorescence have been used to study the selenization of Cu-Zn-Sn-Ge metallic precursors. We propose a reaction mechanism for the incorporation of Ge atoms into the kesterite lattice after the formation of Cu2ZnSnSe4. Electron microscopy reveals that the annealing process leads to Cu2Zn(Sn,Ge)Se4 absorber layers with an increase of Ge content toward the back contact with independence of the original location of Ge in the precursor layer. The effect of the Ge gradient on the optoelectronic properties of the absorber layer has been evaluated with room-temperature cathodoluminescence. The implications of the results for the development of kesterite solar cells are discussed, with the aim of encouraging new synthesis routes for compositionally graded absorbers. [ABSTRACT FROM AUTHOR]

Cu 2 SnS 3 is investigated as a potential solar absorber material, which is known to exist in several polymorphs. In the present work, the transition to the most efficient monoclinic polymorph is investigated and an explanation is given why this one seems to be the best for solar cells. Cubic, mixed polymorphs and monoclinic polymorphs are synthesised with increasing temperature. Photoluminescence spectra of the mixed and cubic polymorphs show mainly defect emissions below the band-gap energy, while the monoclinic modification shows only one sharp peak, which is attributed to the conduction to valence band transition. The monoclinic polymorph also grows in combination with a secondary phase containing sodium, Na x CuSnS 3 , with x between 0.5 and 1. It exhibits a cubic (F43m) crystal structure like CuSn 3.75 S 8 and a band-gap of around 1.6 eV. Devices with absorber layers of monoclinic Cu 2 SnS 3 , in which Na x CuSnS 3 is either present or removed, gave similar power conversion efficiencies of above 1%. [ABSTRACT FROM AUTHOR]

Abstract: Light scattering is a monitoring method which enables in-situ controlling and studying of polycrystalline thin film deposition processes. One advantage of light scattering is that it is flexible in the location of the light source and the detector, which allows a certain margin in the substrate position or in the physical configuration of the deposition system. We have made a systematic investigation on the signal level of the laser light scattering on the case of a typical Cu(In,Ga)Se2 three-stage deposition process. Relationship between the distribution of the scattered light and the film structure was investigated. Generic suggestions for physical setup of light scattering systems have been described. [Copyright &y& Elsevier]