Kinetic-Controlled Crystallization of α-FAPbI3 Inducing Preferred Crystallographic Orientation Enhances Photovoltaic Performance.

Crystallization kinetic controls the crystallographic orientation, inducing anisotropic properties of the materials. As a result, preferential orientation with advanced optoelectronic properties can enhance the photovoltaic devices' performance. Although incorporation of additives is one of the most studied methods to stabilize the photoactive α-phase of formamidinium lead tri-iodide (α-FAPbI3 ), no studies focus on how the additives affect the crystallization kinetics. Along with the role of methylammonium chloride (MACl) as a "stabilizer" in the formation of α-FAPbI3 , herein, the additional role as a "controller" in the crystallization kinetics is pointed out. With microscopic observations, for example, electron backscatter diffraction and selected area electron diffraction, it is examined that higher concentration of MACl induces slower crystallization kinetics, resulting in larger grain size and [100] preferred orientation. Optoelectronic properties of [100] preferentially oriented grains with less non-radiative recombination, a longer lifetime of charge carriers, and lower photocurrent deviations in between each grain induce higher short-circuit current density (Jsc ) and fill factor. Resulting MACl40 mol% attains the highest power conversion efficiency (PCE) of 24.1%. The results provide observations of a direct correlation between the crystallographic orientation and device performance as it highlights the importance of crystallization kinetics resulting in desirable microstructures for device engineering.

Measurement of Quantum Yields of Monolayer TMDs Using Dye-Dispersed PMMA Thin Films.

In general, the quantum yields (QYs) of monolayer transition metal dichalcogenides (1L-TMDs) are low, typically less than 1% in their pristine state, significantly limiting their photonic applications. Many methods have been reported to increase the QYs of 1L-TMDs; however, the technical difficulties involved in the reliable estimation of these QYs have prevented the general assessment of these methods. Herein, we demonstrate the estimation of the QYs of 1L-TMDs using a poly methyl methacrylate (PMMA) thin film embedded with rhodamine 6G (R6G) as a reference specimen for measuring the QYs of 1L-TMDs. The PMMA/R6G composite films with thicknesses of 80 and 300 nm demonstrated spatially homogeneous emissions with the incorporation of well-dispersed R6G molecules, and may, therefore, be used as ideal reference specimens for the QY measurement of 1L-TMDs. Using our reference specimens, for which the QY ranged from 5.4% to 22.2% depending on the film thickness and R6G concentrations, we measured the QYs of the exfoliated or chemical vapor deposition (CVD)-grown 1L-WS2, -MoSe2, -MoS2, and -WSe2 TMDs. The convenient procedure proposed in this study for preparing the thin reference films and the simple protocol for the QY estimation of 1L-TMDs may enable accurate comparisons of the absolute QYs between the 1L-TMD samples, thereby enabling the development of a method to improve the QY of 1L-TMDs.