TY - JOUR A1 - Stolterfoht, Martin A1 - Le Corre, Vincent M. A1 - Feuerstein, Markus A1 - Caprioglio, Pietro A1 - Koster, Lambert Jan Anton A1 - Neher, Dieter T1 - Voltage-Dependent Photoluminescence and How It Correlates with the Fill Factor and Open-Circuit Voltage in Perovskite Solar Cells JF - Acs energy letters N2 - Optimizing the photoluminescence (PL) yield of a solar cell has long been recognized as a key principle to maximize the power conversion efficiency. While PL measurements are routinely applied to perovskite films and solar cells under open circuit conditions (V-OC), it remains unclear how the emission depends on the applied voltage. Here, we performed PL(V) measurements on perovskite cells with different hole transport layer thicknesses and doping concentrations, resulting in remarkably different fill factors (FFs). The results reveal that PL(V) mirrors the current-voltage (JV) characteristics in the power-generating regime, which highlights an interesting correlation between radiative and nonradiative recombination losses. In particular, high FF devices show a rapid quenching of PL(V) from open-circuit to the maximum power point. We conclude that, while the PL has to be maximized at V-OC at lower biases < V-OC the PL must be rapidly quenched as charges need to be extracted prior to recombination. Y1 - 2019 U6 - https://doi.org/10.1021/acsenergylett.9b02262 SN - 2380-8195 VL - 4 IS - 12 SP - 2887 EP - 2892 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 - TY - GEN A1 - Caprioglio, Pietro A1 - Stolterfoht, Martin A1 - Wolff, Christian Michael A1 - Unold, Thomas A1 - Rech, Bernd A1 - Albrecht, Steve A1 - Neher, Dieter T1 - On the relation between the open‐circuit voltage and quasi‐Fermi level splitting in efficient perovskite solar cells T2 - Postprints der Universität Potsdam Mathematisch-Naturwissenschaftliche Reihe N2 - Today's perovskite solar cells (PSCs) are limited mainly by their open‐circuit voltage (VOC) due to nonradiative recombination. Therefore, a comprehensive understanding of the relevant recombination pathways is needed. Here, intensity‐dependent measurements of the quasi‐Fermi level splitting (QFLS) and of the VOC on the very same devices, including pin‐type PSCs with efficiencies above 20%, are performed. It is found that the QFLS in the perovskite lies significantly below its radiative limit for all intensities but also that the VOC is generally lower than the QFLS, violating one main assumption of the Shockley‐Queisser theory. This has far‐reaching implications for the applicability of some well‐established techniques, which use the VOC as a measure of the carrier densities in the absorber. By performing drift‐diffusion simulations, the intensity dependence of the QFLS, the QFLS‐VOC offset and the ideality factor are consistently explained by trap‐assisted recombination and energetic misalignment at the interfaces. Additionally, it is found that the saturation of the VOC at high intensities is caused by insufficient contact selectivity while heating effects are of minor importance. It is concluded that the analysis of the VOC does not provide reliable conclusions of the recombination pathways and that the knowledge of the QFLS‐VOC relation is of great importance. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 774 KW - electro‐optical materials KW - perovskite solar cells KW - photovoltaic devices KW - thin films Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-437595 SN - 1866-8372 IS - 774 ER - TY - GEN A1 - Wolff, Christian Michael A1 - Caprioglio, Pietro A1 - Stolterfoht, Martin A1 - Neher, Dieter T1 - Nonradiative recombination in perovskite solar cells BT - the role of interfaces T2 - Postprints der Universität Potsdam Mathematisch-Naturwissenschaftliche Reihe N2 - Perovskite solar cells combine high carrier mobilities with long carrier lifetimes and high radiative efficiencies. Despite this, full devices suffer from significant nonradiative recombination losses, limiting their VOC to values well below the Shockley–Queisser limit. Here, recent advances in understanding nonradiative recombination in perovskite solar cells from picoseconds to steady state are presented, with an emphasis on the interfaces between the perovskite absorber and the charge transport layers. Quantification of the quasi‐Fermi level splitting in perovskite films with and without attached transport layers allows to identify the origin of nonradiative recombination, and to explain the VOC of operational devices. These measurements prove that in state‐of‐the‐art solar cells, nonradiative recombination at the interfaces between the perovskite and the transport layers is more important than processes in the bulk or at grain boundaries. Optical pump‐probe techniques give complementary access to the interfacial recombination pathways and provide quantitative information on transfer rates and recombination velocities. Promising optimization strategies are also highlighted, in particular in view of the role of energy level alignment and the importance of surface passivation. Recent record perovskite solar cells with low nonradiative losses are presented where interfacial recombination is effectively overcome—paving the way to the thermodynamic efficiency limit. T3 - Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe - 772 KW - interfacial recombination KW - open‐circuit voltage KW - perovskite solar cells KW - photoluminescence Y1 - 2019 U6 - http://nbn-resolving.de/urn/resolver.pl?urn:nbn:de:kobv:517-opus4-437626 SN - 1866-8372 IS - 772 ER -