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.

Hole-Transporting Vanadium-Containing Oxide (V2O5-x) Interlayers Enhance Stability of α-FAPbI3-Based Perovskite Solar Cells (∼23%).

Perovskite solar cells (PSCs) have attracted tremendous interest due to their outstanding intrinsic photovoltaic properties, such as absorption coefficients, exciton binding energies, and long carrier lifetimes. Although the power conversion efficiency (PCE) of PSCs is close to the Si solar cells' PCE, device stability remains a challenge. In particular, the device stability is more critical in n-i-p normal structured PSCs, which show a higher efficiency than p-i-n inverted ones, simply because of the much lower stability of 2,2',7,7'-tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9'-spirobifluorene (Spi). To prevent the devices from degrading performances arising both from perovskite's degradation and Spi instability, we prepare atomic layer deposition (ALD)-grown transition metal oxides for hole transport with efficient n-i-p PSCs. We demonstrate low-temperature (Tdep = 45 °C)-grown amorphous ALD-V2O5-x with oxygen-deficient traps on top of Spi as an interlayer, which prevents the devices' degradation in performance. By blocking moisture and oxygen, ALD-V2O5-x was able to greatly improve the devices' stability by preserving the photovoltaic α-FAPbI3 phase while suppressing both Li ion diffusion from the additive and Au ions from the electrode. As a result, we successfully fabricate PSCs with passivation/hole-transporting bifunctional Spi/ALD-V2O5-x interlayers without sacrificing photovoltaic performances, and the device stability is significantly improved.