TY - JOUR A1 - Kegelmann, Lukas A1 - Tockhorn, Philipp A1 - Wolff, Christian Michael A1 - Márquez, José A. A1 - Caicedo Dávila, Sebastián A1 - Korte, Lars A1 - Unold, Thomas A1 - Loevenich, Wilfried A1 - Neher, Dieter A1 - Rech, Bernd A1 - Albrecht, Steve T1 - Mixtures of Dopant-Free Spiro-OMeTAD and Water-Free PEDOT as a Passivating Hole Contact in Perovskite Solar Cells JF - ACS applied materials & interfaces N2 - Doped spiro-OMeTAD at present is the most commonly used hole transport material (HTM) in n-i-p-type perovskite solar cells, enabling high efficiencies around 22%. However, the required dopants were shown to induce nonradiative recombination of charge carriers and foster degradation of the solar cell. Here, in a novel approach, highly conductive and inexpensive water-free poly(3,4-ethylenedioxythiophene) (PEDOT) is used to replace these dopants. The resulting spiro-OMeTAD/PEDOT (SpiDOT) mixed films achieve higher lateral conductivities than layers of doped spiro-OMeTAD. Furthermore, combined transient and steady-state photoluminescence studies reveal a passivating effect of PEDOT, suppressing nonradiative recombination losses at the perovskite/HTM interface. This enables excellent quasi-Fermi level splitting values of up to 1.24 eV in perovskite/SpiDOT layer stacks and high open-circuit voltages (V-OC) up to 1.19 V in complete solar cells. Increasing the amount of dopant-free spiro-OMeTAD in SpiDOT layers is shown to enhance hole extraction and thereby improves the fill factor in solar cells. As a consequence, stabilized efficiencies up to 18.7% are realized, exceeding cells with doped spiro-OMeTAD as a HTM in this study. Moreover, to the best of our knowledge, these results mark the lowest nonradiative recombination loss in the V-OC (140 mV with respect to the Shockley-Queisser limit) and highest efficiency reported so far for perovskite solar cells using PEDOT as a HTM. KW - perovskite solar cell KW - selective contact KW - spiro-OMeTAD KW - PEDOT KW - recombination KW - passivation KW - quasi-Fermi level splitting Y1 - 2019 U6 - https://doi.org/10.1021/acsami.9b01332 SN - 1944-8244 SN - 1944-8252 VL - 11 IS - 9 SP - 9172 EP - 9181 PB - American Chemical Society CY - Washington ER - TY - JOUR A1 - Pisoni, Stefano A1 - Stolterfoht, Martin A1 - Lockinger, Johannes A1 - Moser, Thierry A1 - Jiang, Yan A1 - Caprioglio, Pietro A1 - Neher, Dieter A1 - Buecheler, Stephan A1 - Tiwari, Ayodhya N. T1 - On the origin of open-circuit voltage losses in flexible n-i-p perovskite solar cells JF - Science and technology of advanced materials : STAM N2 - The possibility to manufacture perovskite solar cells (PSCs) at low temperatures paves the way to flexible and lightweight photovoltaic (PV) devices manufactured via high-throughput roll-to-roll processes. In order to achieve higher power conversion efficiencies, it is necessary to approach the radiative limit via suppression of non-radiative recombination losses. Herein, we performed a systematic voltage loss analysis for a typical low-temperature processed, flexible PSC in n-i-p configuration using vacuum deposited C-60 as electron transport layer (ETL) and two-step hybrid vacuum-solution deposition for CH3NH3PbI3 perovskite absorber. We identified the ETL/absorber interface as a bottleneck in relation to non-radiative recombination losses, the quasi-Fermi level splitting (QFLS) decreases from similar to 1.23 eV for the bare absorber, just similar to 90 meV below the radiative limit, to similar to 1.10 eV when C-60 is used as ETL. To effectively mitigate these voltage losses, we investigated different interfacial modifications via vacuum deposited interlayers (BCP, B4PyMPM, 3TPYMB, and LiF). An improvement in QFLS of similar to 30-40 meV is observed after interlayer deposition and confirmed by comparable improvements in the open-circuit voltage after implementation of these interfacial modifications in flexible PSCs. Further investigations on absorber/hole transport layer (HTL) interface point out the detrimental role of dopants in Spiro-OMeTAD film (widely employed HTL in the community) as recombination centers upon oxidation and light exposure. [GRAPHICS] . KW - Perovskite solar cell KW - flexible KW - interface engineering KW - non-radiative recombination KW - quasi-Fermi level splitting Y1 - 2019 U6 - https://doi.org/10.1080/14686996.2019.1633952 SN - 1468-6996 SN - 1878-5514 VL - 20 SP - 786 EP - 795 PB - Taylor & Francis CY - Abingdon ER -