Reduced-dimensional perovskites (RDPs) are widely used to bolster the stability of perovskite photovoltaics by forming quantum well (QW) structures and impact device performance by tuning QW width distribution. However, there is a lack of understanding about how the phase distribution affects the carrier localization and electron−phonon coupling, as well as their influences on charge dynamics. Herein, we employ a simple strategy to control the crystallization kinetics of RDP films by varying the sequence of incorporating the large organic salt, 2-thiopheneethylammonium iodide (TEAI), in the two-step fabrication method. When incorporating TEAI at the first step, the formation of the TEA-related intermediate phase promotes the preferential directional growth of RDPs with n ≥ 3. Due to the low energy disorder with the preferred energy landscape, the enhanced electron−phonon coupling in RDPs extends the charge recombination lifetime and ensures effective charge collection. The resultant inverted RDP devices achieve an efficiency of 21.0%, accompanied by enhanced operational stability.O rganic−inorganic hybrid perovskite solar cells (PSCs), with an efficiency of over 25%, are compelling candidates for the production of nextgeneration photovoltaics. 1,2 The soft nature of halide perovskites results in electron−phonon interaction with the polaron formation, which has been proposed as a possible explanation for their interesting physical properties. 3−7 However, the associated crystalline defects, in turn, cause it to easily degrade under heat, light, and moisture exposure, resulting in relatively poor stability. 8−10 Stabilizing PSCs is becoming the most pressing issue before commercialization. 11,12 Besides developing methylammonium-free materials, 13,14 composition engineering through incorporating large organic cations into the A-site to form reduced-dimensional (2D and quasi-2D) perovskites (RDPs) has garnered great success. 15,16 For example, a Ruddlesden−Popper (RP) or Dion−Jacobson phase with a quantum well (QW) structure has been demonstrated to strengthen both thermal and environmental stability. 17,18 In
photovoltaic into the windows provides an effective approach to improving building energy efficiency by reducing heat conversion in summer and heat losses in winter. [5] Besides, near-infrared transparent solar cells can be applied to the top cells in tandem devices to exceed the Shockley-Queisser (S-Q) efficiency limit of single-junction cells. [6,7] Many types of light-absorbing materials has been considered for the semitransparent application, including chalcopyrite-, CdTe-, perovskite-, organic-, and dye-sensitized-based systems. [8] Among all the next-generation absorbing materials, semitransparent perovskite solar cells (ST-PSCs) are an ideal candidate due to their tunable bandgaps, high absorption coefficients, excellent physical properties, and low fabrication cost. These appealing advantages make ST-PSCs worth further study for applications in BIPV and tandem devices. The performance evaluation of ST-PSCs can be comprehensively evaluated by light utilization efficiency (LUE), achieved from power conversion efficiency (PCE) coupled with average photopic transmittance (APT) values. [9,10] In Lunt's model, APT is independent of the visible wavelength range and only reflects the photopic response of the human eye. [11] In general, the APT value is lower than the average transmittance (AVT) value, but it avoids overestimation and is consistent with perceived transparency of the window. [12,13] Apparently, PCE and APT are two competing parameters to restrict each other, which makes their optimizations more challenging than that of traditional opaque devices. Achieving an optimum trade-off between transparency and efficiency requires more elaborate and innovative work. Generally, ST-PSCs are composed of a thin perovskite active layer, transparent electrodes, and charge transport layers.To date, many studies have focused on various perovskite fabrication methods [14,15] and device architectures [16][17][18] to increase transparency and color neutrality. Reducing the thickness of the perovskite active layer is the most direct way to improve device transparency. Nevertheless, ultrathin perovskite absorbers are accompanied by nonhomogeneous film coverage due to the formation of voids and pinholes, [19] resulting in shunting paths and nonradiative recombination losses in the final device. Another strategy for achieving highly transparent perovskite films relies on perovskite microstructure engineering, such as
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