Non-fullerene acceptors based organic solar cells represent the frontier of the field, owing to both the materials and morphology manipulation innovations. Non-radiative recombination loss ...suppression and performance boosting are in the center of organic solar cell research. Here, we developed a non-monotonic intermediate state manipulation strategy for state-of-the-art organic solar cells by employing 1,3,5-trichlorobenzene as crystallization regulator, which optimizes the film crystallization process, regulates the self-organization of bulk-heterojunction in a non-monotonic manner, i.e., first enhancing and then relaxing the molecular aggregation. As a result, the excessive aggregation of non-fullerene acceptors is avoided and we have achieved efficient organic solar cells with reduced non-radiative recombination loss. In PM6:BTP-eC9 organic solar cell, our strategy successfully offers a record binary organic solar cell efficiency of 19.31% (18.93% certified) with very low non-radiative recombination loss of 0.190 eV. And lower non-radiative recombination loss of 0.168 eV is further achieved in PM1:BTP-eC9 organic solar cell (19.10% efficiency), giving great promise to future organic solar cell research.
In this contribution, the effectiveness of an RbF post deposition treatment (PDT) is evaluated in dependence on the Cu content of the absorber layer of Cu(In,Ga)Se 2 solar cells. It is shown that the ...PDT only acts beneficially on the open-circuit voltage and fill factor (FF) on samples with rather high Cu content, while it deteriorates all parameters of the solar cells in samples with low Cu content. In order to clarify the behavior of the open-circuit voltage, the well-known exchange mechanism of Rb and Na during the PDT is analyzed as a function of the Cu content of the absorber layers and discussed in regard to theoretical publications. Furthermore, a model explaining the observed effect on the FF based on the formation of an RbInSe 2 (RIS) layer during the RbF-PDT is proposed. The model supposes that the RIS layer acts as a barrier for the photocurrent and therefore lowers the FF. It is evaluated theoretically in dependence of the properties of the RIS layer using one-dimensional solar cell capacitance simulator (SCAPS) simulations. Finally, the proposed model is also tested and confirmed experimentally by directly depositing RIS onto untreated Cu(In,Ga)Se 2 layers.
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.
It is shown that the dominant effect of electrostatic potential fluctuations in Cu(In,Ga)Se2 solar cells is linked to the local variations in the doping densities ND and the interface‐charge density NIF introduced via the buffer layer deposition or duration of RbF postdeposition treatment. Furthermore, light soaking was found to reduce electrostatic fluctuations in cells with Zn(O,S) buffer. To explain this, we proposed a model based on changes in charge states of defects at the CIGS/buffer interface.
The impact of a rubidium fluoride post deposition treatment (RbF‐PDT) on the material and device properties of Cu(In,Ga)Se2 (CIGS) thin films and corresponding solar cells is investigated. The ...structure and device properties of CIGS with different PDT duration are compared. With longer PDT duration, which equals a higher amount of RbF deposited on the CIGS absorber layer, a clear trade‐off is observed between increasing open‐circuit‐voltage (VOC) and decreasing fill factor (FF). An optimum of the PDT duration is found increasing the efficiency by about 0.8% (absolute) compared to the Rb‐free reference device. The mechanisms behind the increased VOC are explored by various characterization methods and identified as a combination of increased carrier concentration and reduced recombination rates in the device. Possible origins for these mechanisms are discussed. Furthermore numerical simulations are used to analyze the detrimental effect of the PDT on the FF. It is found that thermally activated alkali migration into the transparent front contact could create acceptor states there, which could explain the observed FF‐loss.
Varying the amount of RbF deposited on Cu(In,Ga)Se2 thin films, both the changes in material properties of the absorber layer and the electrical modifications of the corresponding solar cell devices are studied. A comprehensive model combining effects on both levels is proposed based on experimental data and numerical simulation under consideration of literature results.
All‐inorganic perovskites have emerged as promising photovoltaic materials due to their superior thermal stability compared to their heat‐sensitive hybrid organic–inorganic counterparts. In ...particular, CsPbI2Br shows the highest potential for developing thermally‐stable perovskite solar cells (PSCs) among all‐inorganic compositions. However, controlling the crystallinity and morphology of all‐inorganic compositions is a significant challenge. Here, a simple, thermal gradient‐ and antisolvent‐free method is reported to control the crystallization of CsPbI2Br films. Optical in situ characterization is used to investigate the dynamic film formation during spin‐coating and annealing to understand and optimize the evolving film properties. This leads to high‐quality perovskite films with micrometer‐scale grain sizes with a noteworthy performance of 17% (≈16% stabilized), fill factor (FF) of 80.5%, and open‐circuit voltage (VOC) of 1.27 V. Moreover, excellent phase and thermal stability are demonstrated even after extreme thermal stressing at 300 °C.
A spin‐forced (SF) method as a facile approach is proposed to control the crystallization kinetics of CsPbI2Br crystal growth, achieving a uniform, and high‐quality film. The perovskite film formation during spin‐coating and annealing is evaluated by optical in situ characterization. As a result, an efficiency of 17.0% with excellent thermal stability at 300 °C is achieved.
Sputter‐deposited GaOx (i.e., oxygen‐deficient gallium oxide) films are evaluated as a potential replacement for the standard CdS buffer layers in Cu(In,Ga)Se2 (CIGSe) based thin‐film photovoltaics. ...The energy level alignment at the GaOx/CIGSe and CdS/CIGSe interfaces are compared by means of direct and inverse photoemission. For the GaOx/CIGSe a (0.04 ± 0.07) eV (i.e., a small spike‐like) conduction band offset (CBO) and a (−3.21 ± 0.19) eV (i.e., a large cliff‐like) valence band offset (VBO) are found, which suggests a nearly ideal charge‐selective contact. The derived GaOx band gap of (4.80 ± 0.25) eV confirms its utility as a highly transparent buffer layer. However, the GaOx (with x derived to be 1.1 ± 0.1) exhibits considerable (presumably) defect‐related occupied states above the valence band maximum. It is proposed that these states may increase charge carrier recombination and decrease open circuit voltage in respective devices; also explaining why solar cells with standard CdS buffer outperform devices with GaOx buffer, despite less ideal electronic interface properties (CBO: (−0.18 ± 0.07) eV, VBO: (−0.98 ± 0.15) eV) and the smaller CdS band gap of (2.35 ± 0.22) eV.
The buried interfaces between GaOx and CdS buffers and CIGSe thin‐film photovoltaic absorbers are studied using direct and inverse photoemission to determine the energy level alignments between the valence band maxima and conduction band minima.
Distinguishing among different electrical loss mechanisms − such as interface and bulk recombination − is a common problem in thin film solar cells. In this work, we report a
J–V
measurement ...technique using different illuminating spectra to distinguish between these two recombination losses. The basic idea is to change the relative contribution of bulk recombination to the total losses of photo-generated charge carriers by generating them in different depths within the absorber layer using different spectral regions of the illuminating light. The use of modern LED sun-simulators allows an almost free design of illumination spectra at intensities close to 1 sun. The comparison of two simple
J–V
measurements, one recorded with illumination near the absorber's band-gap energy and one with light of higher energy, in combination with supporting measurements of the absorber properties, as well as device modeling, enables the extraction of the diffusion length and the interface recombination velocity. Using this technique, we show that in CIGS solar cells, an RbF post-deposition treatment does not only reduce interface recombination losses, as often reported, but also reduces bulk recombination in the CIGS absorber. Furthermore, we find that both cells, with and without RbF treatment, are dominantly affected by interface recombination losses.
Latest record efficiencies of Cu(In,Ga)Se2 (CIGSe) solar cells were achieved by means of a rubidium fluoride (RbF) post-deposition treatment (PDT). To understand the effect of the RbF-PDT on the ...surface chemistry of CIGSe and its interaction with sodium that is generally present in the CIGSe absorber, we performed an X-ray photoelectron spectroscopy (XPS) study on CIGSe thin films as-deposited by a three-stage co-evaporation process and after the consecutive RbF-PDT. The sample transfer from the deposition to the XPS analysis chamber was performed via an ultra-high vacuum transfer system. This allows to minimize air exposure, avoiding oxide formation on the CIGSe surface, especially for alkali-treated absorbers. Beside an expected reduction of Cu- and Ga-content at the surface of RbF-treated CIGSe films, we find that Rb penetrates the CIGSe and, contrary to fluorine, it is not completely removed by subsequent ammonia etching. The remaining Rb contribution at 110.0 eV binding energy, which appears after the RbF-PDT is similar to the one detected on a co-evaporated RbInSe2 reference sample and together with a new Se 3d contribution may hence belong to an Rb-In-Se secondary phase on the CIGSe surface. In addition, Na is driven towards the surface of the CIGSe absorber as a direct result of the RbF-PDT. This proves the ion-exchange mechanism in the absence of moisture and air/oxygen between heavy Rb atoms incorporated via PDT and lighter Na atoms supplied by the glass substrate. A remaining XPS signal of Na 1 s is observed after etching the vacuum transferred RbF-CIGSe sample, indicating that Rb and/or F are not as much a driving force for Na as oxygen usually is.
In this contribution we are analyzing and comparing the impact of two different alkali-fluorine post deposition treatments (KF and RbF) on the growth of chemical-bath-deposited CdS buffer layers on ...Cu(In,Ga)Se2 absorber layers for thin film solar cells. By combining Raman scattering, scanning electron microscopy, current-voltage analysis and measurements of the internal quantum efficiency we provide a comprehensive picture of this issue on the material and device level. We find that both PDTs lead to a better CdS-coverage of the surface of the CIGS, which leads to an improved junction quality at early growth stages compared to untreated devices. Furthermore the growth rate of the CdS is enhanced on KF-treated absorber layers while it is decreased on those treated with RbF (compared to the reference). This leads to a more stable behavior of RbF-treated devices after longer duration of the CdS deposition, while the KF-treated devices suffer from reduced fill factor and open circuit voltage. Furthermore we show that not only both PDTs but also the growth of the CdS lead to a reduction of the amount of the so called ordered defect compound, which is initially present at the surface of our absorber layers. This behavior indicates either the formation of CdCu -anti-sites or of a secondary phase at the interface.
•The effects of KF- and RbF-PDTs on the CIGS′ surface morphology are compared.•Both PDTs lead to a reduction of the Cu-poor phase at the surface of the CIGS.•An additional consumption of this phase is detected.•Both PDTs show an improved coverage of the surface of the CIGS by CdS.•The optimal CdS growth duration is found to be dependent on the PDT utilized.
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