- Award ID(s):
- Publication Date:
- NSF-PAR ID:
- Journal Name:
- Journal of Materials Chemistry A
- Page Range or eLocation-ID:
- 13043 to 13049
- Sponsoring Org:
- National Science Foundation
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Rapid thermal annealing of CH 3 NH 3 PbI 3 perovskite thin films by intense pulsed light with aid of diiodomethane additiveThe organic metal halide perovskite material is capable of high throughput manufacturing via traditional deposition processes used in roll-to-roll, yet thermal annealing post deposition may require long ovens. We report rapid annealed perovskite thin films using intense pulsed light (IPL) to initiate a radiative thermal response that is enabled by an alkyl halide additive that collectively improves the performance of a device processed in an ambient environment from a baseline of 10 to 16.5% efficiency. Previous reports on CH 3 NH 3 PbI 3 perovskite films using IPL processing achieved functional devices in milli-second time scales and are promising for high throughput manufacturing processes under ambient conditions. In this study, we found that the addition of diiodomethane (CH 2 I 2 ) as an additive to the methylammonium iodide (MAI)/lead iodide (PbI 2 ) precursor ink chemistry and subsequent IPL thermal annealing are inter-dependent. The concentration of CH 2 I 2 and IPL processing parameters have a direct effect on the surface morphology of the films and performance within a perovskite solar cell (PSC). The CH 2 I 2 dissociates under exposure to ultraviolet (UV) radiation from the IPL source liberating iodine ions in the film, influencing the perovskite formationmore »
Tunable optical properties and stability of lead free all inorganic perovskites (Cs 2 SnI x Cl 6−x )Organic–inorganic hybrid lead-based perovskites experience significant environmental instability under ambient moist air and are not environmentally benign due to the usage of toxic Pb. Here, we report a new approach to synthesize lead-free all inorganic perovskites (Cs 2 SnI x Cl 6−x ) using hydriodic acid (HI) demonstrating greatly enhanced environmental stability and tunable optical properties by controlling the I − /Cl − ratios. Single phase perovskites can be achieved with a low iodine or chlorine content, and a phase separation occurs in the binary system with closer iodine and chlorine dopings. UV-vis diffuse reflectance and photoluminescence measurements reveal tunable band gaps of Cs 2 SnI x Cl 6−x perovskites from the UV to the infrared region. The mixed halide perovskite with a lower chloride content shows significantly higher photoluminescence intensity. The thermal stability of mixed halide all-inorganic perovskites is continuously improved as the Cl content increases. The synthesis of Sn-based perovskites with tunable optical properties and environmental stability represents one step further toward the realization of the stable lead-free all inorganic perovskites.
Metal halide perovskites have emerged as the next generation of light emitting semiconducting materials due to their excellent properties such as tunable bandgaps, high photoluminescence quantum yield, and high color purity. Nickel oxide is a hole transport material that has been used in planar light emitting diodes (LEDs). In this paper, we develop a novel method for the large scale fabrication of metal halide perovskite nanowire arrays encapsulated inside nickel oxide nanotubes. We study the structural and spectral properties of these infiltrated perovskites nanowires and, to the best of our knowledge, for the first time report on a working LED device consisting of perovskites encapsulated inside nickel oxide nanotubes. Finally, we study the photoluminescence and electroluminescence of an LED with MAPbBr 3 inside nickel oxide nanotubes and obtain an outstanding current efficiency of 5.99 Cd A −1 and external quantum efficiency of 3.9% for the LED device.
In high fluence applications of lead halide perovskites for light-emitting diodes and lasers, multi-polaron interactions and associated Auger recombination limit the device performance. However, the relationship of the ultrafast and strongly lattice coupled carrier dynamics to nanoscale heterogeneities has remained elusive. Here, in ultrafast visible-pump infrared-probe nano-imaging of the photoinduced carrier dynamics in triple cation perovskite films, a ~20 % variation in sub-ns relaxation dynamics with spatial disorder on tens to hundreds of nanometer is resolved. We attribute the non-uniform relaxation dynamics to the heterogeneous evolution of polaron delocalization and increasing scattering time. The initial high-density excitation results in faster relaxation due to strong many-body interactions, followed by extended carrier lifetimes at lower densities. These results point towards the missing link between the optoelectronic heterogeneity and associated carrier dynamics to guide synthesis and device engineering for improved perovskites device performance.
The remarkable optoelectronic properties of metal halide perovskites have generated intense research interest over the last few years. The ability to control and manipulate the crystallisation and stoichiometry of perovskite thin-films has allowed for impressive strides in the development of highly efficient perovskite solar cells. However, being able to effectively modify the interfaces of metal halide perovskites, and to controllably p- or n-type dope the surfaces, may be key to further improvements in the efficiency and long-term stability of these devices. In this study, we use surface doping of the mixed-cation, mixed-halide perovskite FA 0.85 MA 0.15 Pb(I 0.85 Br 0.15 ) 3 (FA – formamidinium; MA – methylammonium) to improve the hole extraction from the perovskite solar cell. By treating the surface of the perovskite film with a strongly oxidizing molybdenum tris(dithiolene) complex, we achieve a shift in the work function that is indicative of p-doping, and a twofold increase in the total conductivity throughout the film. We probe the associated interfacial chemistry through photoelectron and solid-state nuclear magnetic resonance spectroscopies and confirm that charge-transfer occurs between the perovskite and dopant complex. The resulting p-doped interface constitutes a homojunction with increased hole-selectivity. With charge-selective layers, we show that thismore »