Perovskite solar cells (PSCs) employing 3D organic-inorganic hybrid perovskite photoabsorbers have received tremendous progress with state-of-the-art power conversion efficiency (PCE) exceeding 25% during the last a dozen years. [1] However, ambient instability of 3D perovskite materials remains a critical obstacle for realistic applications of PSCs. [2,3] A strategy in addressing the poor stability is to reduce the structural dimensionality of perovskites via the introduction of long-chain organic ligands by forming Ruddlesden-Popper (RP) quasi-2D perovskites. [4,5] The organic ligands are bound to the 3D inorganic framework via coulombic interactions, resulting in a layered structure. The general formula of RP-2D perovskites takes the form of (L) 2 A n−1 Pb n I 3n+1 (n = 1, 2, 3, 4…) where A is the methylammonium (MA +), formamidinium (FA +), or cesium (Cs +) cations, L is the bulky organic ligands, e.g., butylammonium (BA +) or 2-phenylethylammonium (PEA +), and n is the number of layers in the [PbI 6 ] 4− octahedral sheets. [4-7] The incorporation of hydrophobic bulky organic ligands can not only enhance the stability of perovskites with minimized permeation of water molecules but also increase the formation energy of perovskites to mitigate thermal degradation and ion migration. [8-10] These merits alongside the quantum confinement have rendered quasi-2D perovskites great potentials for optoelectronic applications with a wide tunability on the bandgap or photophysical properties. [7] Unfavorably, quasi-2D perovskites are generally associated with a large exciton binding energy (hundreds of meV) due to the insulating nature of bulky organic ligands and the specific layered arrangement. [11,12] As a result, charge transport and extraction are hindered in quasi-2D PSCs. To date, the highest reported PCEs of quasi-2D PSCs (n ≤ 5) remain around 18%, [13-15] showing considerable performance gaps with regard to 3D-PSCs. The PCE (η) of photovoltaic cells is determined by the general relation, J V P FF sc oc light η = × × (V oc is the open-circuit voltage, FF is the fill factor, and P light is the illumination intensity). In quasi-2D PSCs, the relatively low J sc is more restrictive for Organic-inorganic hybrid quasi-2D perovskites have shown excellent stability for perovskite solar cells (PSCs), while the poor charge transport in quasi-2D perovskites significantly undermines their power conversion efficiency (PCE). Here, studies on water-controlled crystal growth of quasi-2D perovskites are presented to achieve high-efficiency solar cells. It is demonstrated that the (BA) 2 MA 4 Pb 5 I 16-based PSCs (n = 5) processed with water-containing precursors display an increased short-circuit current density (J sc) of 19.01 mA cm −2 and PCE over 15%. The enhanced performance is attributed to synergetic growths of the 3D and 2D phase components aided by the formed hydration (MAI•H 2 O), leading to modulations on the crystal orientation and phase distribution of various n-value components, which facilitate interphase charge tr...
Perovskite semiconductor nanocrystals have emerged as an excellent family of materials for optoelectronic applications, where biexciton interaction is essential for optical gain generation and quantum light emission. However, the strength of biexciton interaction remains highly controversial due to the entangled spectral features of the exciton- and biexciton-related transitions in conventional measurement approaches. Here, we tackle the limitation by using polarization-dependent two-dimensional electronic spectroscopy and quantify the excitation energy-dependent biexciton binding energy at cryogenic temperatures. The biexciton binding energy increases with excitation energy, which can be modeled as a near inverse-square size dependence in the effective mass approximation considering the quantum confinement effect. The spectral line width for the exciton–biexciton transition is much broader than that for the ground state to exciton transition, suggesting weakly correlated broadening between these transitions. These inhomogeneity effects should be carefully considered for the future demonstration of optoelectronic applications relying on coherent exciton–biexciton interactions.
Colloidal semiconductor nanoplatelets (NPLs) have recently emerged as highly promising optical gain medium because of their superior optical properties. Here, the shell‐thickness‐dependent optical gain properties of CdSe/CdS core/shell NPLs synthesized by high‐temperature growth are systematically investigated for the first time. The core/shell NPLs show the increased quantum yields and enhanced photostability as well as clear reduced emission blinking, thanks to the preferable passivation of nonradiative surface defects by the growth of the high‐quality CdS shells under high reaction temperature. Meanwhile, the amplified spontaneous emission (ASE) performance of CdSe/CdS NPLs indicates a nonmonotonic dependence on the shell thickness. The ASE threshold is achieved as low as ≈4.4 µJ cm−2 for thick‐shell NPLs with six monolayer CdS shells, and exhibiting ultrafast transient dynamics process (≈11 ps). Besides, an extremely long lifetime (>800 ps) and large bandwidth (>140 nm) of optical gain are observed by employing ultrafast transient absorption spectroscopy. Finally, a thick‐shell NPLs vertical cavity surface‐emitting laser is developed, which demonstrates spatially directional single‐mode operation with an ultralow lasing threshold of ≈1.1 µJ cm−2. These excellent results are attributed to the remarkable optical gain performance of core/shell NPLs and represent an important step toward practical NPL laser devices.
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