Self‐assembled monolayers (SAMs) have emerged as effective carrier transport layers in perovskite (PVK) solar cells because of their unique ability to manipulate interfacial property, as well as simple processing and scalable fabrication. However, the defects and pinholes derived from their sensitive adsorption process inevitably deteriorate the final device performance. Herein, a sputtered nickel oxide (NiOx) interlayer is used as a seed layer to promote the adsorption of the [2‐(3,6‐dimethoxy‐9H‐carbazol‐9‐yl)ethyl]phosphonic acid (MeO‐2PACz) SAM on the indium tin oxide (ITO) substrate. The promoted adsorption is attributed to the enhanced tridentate binding between MeO‐2PACz and NiOx relative to the conventional bidentate binding between MeO‐2PACz and ITO. In addition, the NiOx modification can simultaneously improve the passivation ability and hole‐selectivity of the MeO‐2PACz, provide a favorable energy‐level alignment at the ITO/PVK interface, and prevent a direct contact between PVK and ITO. As a consequence, this NiOx‐seeded MeO‐2PACz hole transport layer enables a significantly enhanced power conversion efficiency of 19.9% in comparison with 18.4% of the control device. This work provides an effective strategy to improve the performance of the SAM‐based photoelectric device.
A fundamental theory including photoelectric response, ion migration and photon recycling effects for back-contact perovskite solar cells is established.
Wide bandgap (E g ) mixed-halide perovskite has attracted much attention for applications in photovoltaic devices. However, devices featuring this type of perovskite are often subject to a large voltage deficit due to the occurrence of phase segregation, which limits the relevant devices' access to high performances. Here, the correlation of the phase segregation and voltage losses for wide-E g mixed-halide perovskite solar cells (PSCs) is clarified by experiments and simulations. Taking 1.67 eV E g mixed-halide perovskite as an example, it is confirmed experimentally that the control devices produce a poor physical morphology, a locally widened E g , and an inferior electrical response. By suppressing the phase segregation, the open-circuit voltage (V oc ) can be boosted from 1.15 to 1.20 V, which is a high value for the 1.67 eV E g mixed-halide PSCs. An electrical simulation of phase segregation reveals that the performance degeneration can be attributed to the bulk recombination due to the energy level mismatch of the varied E g s. Moreover, a theoretical perspective is produced to expatiate on the strategies for the high V oc of wide-E g PSCs. This study brings deep guidance to unlock the potential for high-performance mix-halide PSCs.
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