Influence of Substituent Position of 2D Cations on Orientation Enabling Efficient and Stable 3D/2D Perovskite Solar Cells Retaining 95% of the Initial Efficiency After 900h Under 1 Sun

Gunes, Ummugulsum; Yaylali, Figen Varlioglu; Karabag, Zeynep Gozukara; Gao, Xuerui; Syzgantseva, Olga A.; Karabag, Aliekber; Yildirim, Gulsevim Bensu; Tsoi, Konstantin; Shibayama, Naoyuki; Kanda, Hiroyuki; Rafieh, Alwani Imanah; Zhong, Liping; Züttel, Andreas; Dyson, Paul; Yerci, Selçuk; Nazeeruddin, Mohammad Khaja; Günbaş, Görkem

doi:10.2139/ssrn.4311126

Cited by 2 publications

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“…[38][39][40] To exemplify this we spin-coated phenethylammonium iodide (PEAI) on top of a Cs 0.05 (MA 0.05 FA 0.95 ) 0.95 Pb(I 0.95 Br 0.05 ) 3 "FAPI-rich" perovskite which is known to form a 2D layer on the surface. [41][42][43][44] As shown in Figure 7a,b, this improves the performance through a higher V OC although the J SC is slightly reduced. We speculate that this suppresses the minority carrier concentration at the critical interface which can, for example, alleviate the losses due to an energy level mismatch between the perovskite and the C 60 Considering that the as-prepared perovskite exhibits a QFLS-V OC mismatch, we speculate that C 60 layer is misaligned with respect to the perovskite.…”

Section: Low Mobility Perovskitementioning

confidence: 99%

Mismatch of Quasi–Fermi Level Splitting and V_oc in Perovskite Solar Cells

Warby,

Shah,

Thiesbrummel

et al. 2023

Advanced Energy Materials

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Perovskite solar cells have demonstrated low non‐radiative voltage losses and open‐circuit voltages (VOCs) that often match the internal voltage in the perovskite layer, i.e. the quasi‐Femi level splitting (QFLS). However, in many cases, the VOC differs remarkably from the internal voltage, for example in devices without perfect energy alignment. In terms of recombination losses, this loss often outweighs all non‐radiative recombination losses observed in photoluminescence quantum efficiency measurements by many orders of magnitude. As such, understanding this phenomenon is of great importance for further perovskite solar cell development and tackling stability issues. The classical theory developed for Si solar cells explains the QFLS‐VOC mismatch by considering the partial resistances/conductivities for majority and minority carriers. Here, the authors demonstrate that this generic theory applies to a variety of physical mechanisms that give rise to such a mismatch. Additionally, it is found that mobile ions can contribute to a QFLS‐VOC mismatch in realistic perovskite cells, and it is demonstrated that this can explain various key observations about light soaking and aging‐induced VOC losses. The findings in this paper shine a light on well‐debated topics in the community, identify a new degradation loss, and highlight important design principles to maximize the VOC for improved perovskite solar cells.

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Section: Low Mobility Perovskitementioning

confidence: 99%

Mismatch of Quasi–Fermi Level Splitting and V_oc in Perovskite Solar Cells

Warby,

Shah,

Thiesbrummel

et al. 2023

Advanced Energy Materials

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“…[ 38 ] We recently demonstrated the positional effect of methoxy (‐OMe) substituents on the orientation of 2D‐forming PEAI salts ( x ‐OMe‐PEAI salts ( x = o , m , p )) on 3D/2D perovskite films. [ 39 ] In the present work, a series of bulky organic cations based on the phenylethylammonium (PEA) framework with 3 different halogens (F, Cl, and Br) that vary significantly in their size and electronegativity were realized. For all halogens, the substituent position also varied ( ortho ( o ), meta ( m ), and para ( p ) positions) on the aromatic ring, yielding nine different x ‐XPEAI salts ( x = o , m , p ; X = F , Cl , Br ) toward understanding the effect of electronics and sterics on the performance of resulting 3D/2D perovskite solar cells.…”

Section: Introductionmentioning

confidence: 99%

Tuning 2D Perovskite Passivation: Impact of Electronic and Steric Effects on the Performance of 3D/2D Perovskite Solar Cells

Gozukara Karabag,

Karabag,

Gunes

et al. 2023

Advanced Energy Materials

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Surface passivation with 2D perovskites is a powerful strategy to achieve improved stability and performance in perovskite solar cells (PSCs). Various large organic cations have been successfully implemented, led by phenylethylammonium (PEA+) and its derivatives. However, systematic studies on large sets of cations to understand the effect of substituent position on 2D perovskite passivation and device performance are lacking. Herein, a collection of halogenated PEA+ iodide salts (x‐XPEAI where x: ortho (o), meta (m), para (p), X: F, Cl, Br) are synthesized by a facile method and deposited on top of 3D perovskite. The 2D perovskite layer formation is confirmed by X‐ray diffraction (XRD) and grazing‐incidence wide‐angle X‐ray scattering analyses for all cations, regardless of the nature and position of the halogen. Density functional theory analysis reveals that lower formation energies and higher interfacial dipoles achieved by m‐substituted cations are responsible for enhanced performance compared to their o‐ and p‐ counterparts. While the m‐BrPEAI‐treated device shows a champion efficiency of 23.42%, (VOC=1.13 V, FF=81.2%), considering average efficiencies, stability, and reproducibility, the treatment with m‐ClPEAI salt yields the best overall performance. This comprehensive study provides guidelines for understanding the influence of large cation modification on performance and stability of 3D/2D PSCs.

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Influence of Substituent Position of 2D Cations on Orientation Enabling Efficient and Stable 3D/2D Perovskite Solar Cells Retaining 95% of the Initial Efficiency After 900h Under 1 Sun

Cited by 2 publications

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Mismatch of Quasi–Fermi Level Splitting and V_oc in Perovskite Solar Cells

Mismatch of Quasi–Fermi Level Splitting and V_oc in Perovskite Solar Cells

Tuning 2D Perovskite Passivation: Impact of Electronic and Steric Effects on the Performance of 3D/2D Perovskite Solar Cells

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Influence of Substituent Position of 2D Cations on Orientation Enabling Efficient and Stable 3D/2D Perovskite Solar Cells Retaining 95% of the Initial Efficiency After 900h Under 1 Sun

Cited by 2 publications

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Mismatch of Quasi–Fermi Level Splitting and Voc in Perovskite Solar Cells

Mismatch of Quasi–Fermi Level Splitting and Voc in Perovskite Solar Cells

Tuning 2D Perovskite Passivation: Impact of Electronic and Steric Effects on the Performance of 3D/2D Perovskite Solar Cells

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Mismatch of Quasi–Fermi Level Splitting and V_oc in Perovskite Solar Cells

Mismatch of Quasi–Fermi Level Splitting and V_oc in Perovskite Solar Cells