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Herein, we report on the synthesis and investigation of two triazino-isoquinoline tetrafluoroborate electrolytes as hole-blocking layers in methylammonium triiodide perovskite photovoltaic devices with fullerene electron extraction layer. We find that increasing the thickness of the dipolar hole-blocking layer results in a gradual increase in the open-circuit voltage suggesting that aggregation of the molecules can enhance the dipole induced by the layer. This finding is confirmed by theoretical calculations demonstrating that while both molecules exhibit a similar dipole moment in their isolated state, this dipole is significantly enhanced when they aggregate. Ultra-violet photoemission spectroscopy measurements show that both derivatives exhibit a high ionisation potential of 7 eV, in agreement with their effective hole-blocking nature demonstrated by the devices. However, each of the molecules shows a different electron affinity due to the increased conjugation of one of the derivatives. While the change in electron transport level between the two derivatives is as high as 0.3 eV, the difference in the open-circuit voltage of both types of devices is negligible, suggesting that the electron transport level plays only a minor role in determining the open-circuit voltage of the device. Numerical device simulations confirm that the increase in built-in potential, arising from the high dipole of the electrolyte layer, compensates for the non-ideal energetic alignment of the charge transport levels, resulting in high VOC for a range of electron transport levels. Our study demonstrates that the application of small molecule electrolytes as hole-blocking layer in inverted architecture perovskite solar cells is a powerful tool to enhance the open-circuit voltage of the devices and provides useful guidelines for designing future generations of such compounds.
We explore the degradation behaviour under continuous illumination and direct oxygen exposure of inverted unencapsulated formamidinium(FA)0.83Cs0.17Pb(I0.8Br0.2)3, CH3NH3PbI3, and CH3NH3PbI3-xClx perovskite solar cells. We continuously test the devic
Engineering the energetics of perovskite photovoltaic devices through the deliberate introduction of dipoles to control the built-in potential of the devices offers the opportunity to enhance their performance without the need to modify the active la
In this perspective, we explore the insights into the device physics of perovskite solar cells gained from modeling and simulation of these devices. We discuss a range of factors that influence the modeling of perovskite solar cells, including the ro
Point defects in metal halide perovskites play a critical role in determining their properties and optoelectronic performance; however, many open questions remain unanswered. In this work, we apply impedance spectroscopy and deep-level transient spec
Solution-processed quantum dots (QDs) have a high potential for fabricating low cost, flexible and large-scale solar energy harvesting devices. It has recently been demonstrated that hybrid devices employing a single monovalent cation perovskite solu