Search

The hole‐transporting material (HTM), poly (3,4‐ethylene dioxythiophene) poly(styrene sulfonate) (PEDOT : PSS), is the most widely used material in the realization of high‐efficiency organic solar cells (OSCs). However, the stability of PEDOT : PSS‐based OSCs is quite poor, arising from its strong acidity and hygroscopicity. In addition, PEDOT : PSS has an absorption in the infrared region and high highest occupied molecular orbital (HOMO) energy level, thus limiting the enhancement of short‐circuit current density (Jsc) and open‐circuit voltage (Voc), respectively. Herein, two asymmetric self‐assembled molecules (SAMs), namely BrCz and BrBACz, were designed and synthesized as HTM in binary OSCs based on the well‐known system of PM6 : Y6, PM6 : eC9, PM6 : L8‐BO, and D18 : eC9. Compared with BrCz, BrBACz shows larger dipole moment, deeper work function and lower surface energy. Moreover, BrBACz not only enhances photon harvesting in the active layer, but also minimizes voltage losses as well as improves interface charge extraction/ transport. Consequently, the PM6 : eC9‐based binary OSC using BrBACz as HTM exhibits a champion efficiency of 19.70 % with a remarkable Jsc of 29.20 mA cm−2 and a Voc of 0.856 V, which is a record efficiency for binary OSCs so far. In addition, the unencapsulated device maintains 95.0 % of its original efficiency after 1,000 hours of storage at air ambient, indicating excellent long‐term stability. [ABSTRACT FROM AUTHOR]

The main obstacles to promoting the commercialization of perovskite solar cells (PSCs) include their record power conversion efficiency (PCE), which still remains below the Shockley–Queisser limit, and poor long‐term stability, attributable to crystallographic defects in perovskite films and open‐circuit voltage (Voc) loss in devices. In this study, potassium (4‐tert‐butoxycarbonylpiperazin‐1‐yl) methyl trifluoroborate (PTFBK) was employed as a multifunctional additive to target and modulate bulk perovskite defects and carrier dynamics of PSCs. Apart from simultaneously passivating anionic and cationic defects, PTFBK could also optimize the energy‐level alignment of devices and weaken the interaction between carriers and longitudinal optical phonons, resulting in a carrier lifetime of greater than 3 μs. Furthermore, it inhibited non‐radiative recombination and improved the crystallization capacity in the target perovskite film. Hence, the target rigid and flexible p‐i‐n PSCs yielded champion PCEs of 24.99 % and 23.48 %, respectively. More importantly, due to hydrogen bonding between formamidinium and fluorine, the target devices exhibited remarkable thermal, humidity, and operational tracking at maximum power point stabilities. The reduced Young's modulus and residual stress in the perovskite layer also provided excellent bending stability for flexible target devices. [ABSTRACT FROM AUTHOR]

Comprehensive Summary Inverted (p‐i‐n) perovskite solar cells (PSCs) are favored by researchers owing to their superior compatibility with flexible substrates and tandem device fabrication. Additionally, the hole transport layer (HTL) serves as a template for perovskite growth, which is critical for enhancing the device performance. However, the current research on how the HTL promotes perovskite crystallization is insufficient. Here, 4PADCB, a self‐assembled monolayer (SAM) hole transport material, was optimized as a superior template for perovskite growth through comparative analysis; accordingly, compact perovskite film with vertical growth was prepared. The better matched energy level alignment between 4PADCB and perovskite suppressed nonradiative recombination at the interface and enabled rapid hole extraction. Moreover, high‐quality perovskite film growth on 4PADCB exhibited lower Young's modulus and less residual stress. By integrating 4PADCB into p‐i‐n PSCs, the optimal device achieved a power conversion efficiency of 24.80%, with an open‐circuit voltage of 1.156 V, thus achieving the best rank among devices without perovskite post‐treatment, additives, dopants, or intermediate layers. Furthermore, the unencapsulated device demonstrated exceptional thermostability and photostability under maximum power point tracking. Thus, this work provides a new understanding for the development of novel SAMs and perovskite growth, and it is expected to further improve device performance. [ABSTRACT FROM AUTHOR]