Focus on Perovskite Thin Films and Nanomaterials for Applications in Optoelectronic Devices

Metal halide perovskites have attracted increasing attention due to their superior optical and electrical characteristics, flexible tunability, and easy fabrication processes. Apart from their unprecedented successes in photovoltaic devices, lasing action is the latest exploitation of the optoelectronic performance of perovskites. Among the substantial body of research on the configuration design and light emission quality of perovskite lasers, the random laser is a very interesting stimulated emission phenomenon with unique optical characteristics. In this review article, we first comprehensively overview the development of perovskite-based optoelectronic devices and then focus our discussion on random lasing performance. After an introduction to the historical development of versatile random lasers and perovskite random lasers, we summarize several synthesis methods and discuss their material configurations and stability in synthesized perovskite materials. Following this, a theoretical approach is provided to explain the random lasing mechanism in metal halide perovskites. Finally, we propose future applications of perovskite random lasers, presenting conclusions as well as future challenges, such as quality stability and toxicity reduction, of perovskite materials with regard to practical applications in this promising field.

The properties of CH₃NH₃PbI₃ (MAPbI₃) crystalline thin films and the device performance of highly efficient MAPbI₃ photovoltaic cells are investigated by varying the temperature of the antisolvent from 20 °C to 50 °C during the washing enhanced nucleation (WEN) process. The surface, structural, optoelectronic and defect properties of the perovskite thin films are characterized through atomic-force microscopy, X-ray diffractometry and photoluminescence spectrometry. The experimental results show that changing the temperature of the antisolvent during the WEN process can manipulate the MAPbI₃ crystalline thin films from the (110)–(002) complex phase to a (002) preferred phase. It is noted that the highest power conversion efficient of the inverted MAPbI₃ photovoltaic cells is 19.30%, mainly due to the increased carrier collection efficiency and reduced carrier recombination when the temperature of the antisolvent is 30 °C.

Atomic-force microscopic images, x-ray diffraction patterns, Urbach energies and photoluminescence quenching experiments show that the interfacial contact quality between the hydrophobic [6,6]-phenyl-C₆₁-buttric acid methyl ester (PCBM) thin film and hydrophilic CH₃NH₃PbI₃ (MAPbI₃) thin film can be effectively improved by using a binary antisolvent mixture (toluene:dichloromethane or chlorobenzene:dichloromethane) in the anti-solvent mixture-mediated nucleation process, which increases the averaged power conversion efficiency of the resultant PEDOT:PSS (P3CT-Na) thin film based MAPbI₃ solar cells from 13.18% (18.52%) to 13.80% (19.55%). Beside, the use of 10% dichloromethane (DCM) in the binary antisolvent mixture results in a nano-textured MAPbI₃ thin film with multicrystalline micrometer-sized grains and thereby increasing the short-circuit current density and fill factor (FF) of the resultant solar cells. It is noted that a remarkable FF of 80.33% is achieved, which can be used to explain the stable photovoltaic performance without additional encapsulations.

In this work, we report a novel two-dimensional (2D) (SrBr)₂PbI₄ perovskite layered architecture, which were formed by the reaction of strontium bromide (SrBr₂), strontium iodide (SrI₂) and lead iodide (PbI₂). Formation of 2D (SrBr)₂PbI₄ was verified by small angle XRD peak at 6.4°, which corresponds to the layer distance of 13.78 Å. The best one of solar cells fabricated with Quasi-3D perovskite, (SrBr)₂FA₅₉Pb₆₀I₁₈₁ (n = 60), showed a power conversion efficiency (PCE) of 18.46% and retained 95% of the initial PCE at 1000 h in the dry air. Further, the 2D (SrBr)₂PbI₄ as the surface passivation layer on the 3D FAPbI₃ perovskite greatly reduced the defects at the perovskite/Spiro-OMeTAD interface, and the corresponding solar cells with FAPbI₃/(SrBr)₂PbI₄ 3D/2D structure achieved a PCE of 22.14% and over 90% retention of the original PCE at 1000 h. In short, this work provides an example of inorganic complex cations that can form 2D perovskites and achieve perovskite solar cells with high PCE and stabilization at the same time.

Carbon nanotubes (CNTs) were continuously grown on the surface of the moving carbon fiber by chemical vapor deposition method using a custom-designed production line to prepare composite reinforcements on a large-scale. The systematic study of different parameters affecting the CNT growth revealed simple growth kinetics, which helps to control the surface morphology and structural quality of CNTs. Since hydrogen maintains the activity of the catalyst, it promotes the growth of CNTs in a continuous process. The increase of acetylene partial pressure promotes the accumulation of amorphous or graphite carbon on the catalyst surface, resulting in the decrease of CNT growth rate when acetylene concentration reaches 40%. The growth temperature significantly affects the CNT diameter and structural quality. As the temperature increases, the crystallinity of the tube wall increases obviously, and the CNT diameter increases due to the aggregate growth of the catalyst particles. According to the Arrhenius formula, the apparent activation energy is observed to be 0.67 eV, which proves that both bulk diffusion and surface diffusion exist when activated carbon passes through the catalyst to form CNTs.

Low temperature derived carbon electrodes are employed to fabricate low cost hole transport layer free perovskite solar cells, in which perovskite films annealed in glovebox and ambient air are used as the absorbers, respectively. Results suggest that the air annealed sample has bigger crystal grains and higher crystallinity, and the existence of a small amount of lead iodide which passivates grain boundaries contributes to a lower trap density. As a result, a maximum power conversion efficiency (PCE) of 13.07% was obtained on the air annealed device, which is higher than those of devices annealed in glovebox (11.25%). Furthermore, the stability of unencapsulated devices stored in wet (with humidity around 90% ± 5%) air atmosphere are investigated and the results prove that our devices exhibit good stability. In addition to rigid devices, flexible perovskite solar cells are also fabricated using the same procedure. The highest PCE of 11.53% is demonstrated on the champion flexible device, and 69% of its initial PCE can be maintained even after 2000 bending cycles with a bending radius of 2 mm. Our work provides a promising and simple rout for low-cost, air-stable, high-efficiency carbon perovskite solar cells for both large area production and flexible electronic devices industry.

In this paper, we used tannic acid (TA) functionalized carbon nanotubes (TCNTs), and silver nanowires (AgNWs) to construct a new type of transparent conductive film (TCF) with a double-layered conductive network structure. The hybrid film exhibits excellent light transmittance, high electrical conductivity, ultra-flexibility, and strong adhesion. These outstanding performances benefit from the filling and adhesion of hydrophilic TCNT layers to the AgNW networks. Besides, we introduced the post-treatment process of mechanical pressing and covering polymer conductive polymer PEDOT:PSS, which obtained three layers of TCNT/AgNW/PEDOT hybrid film and greatly improved the comprehensive properties. The hybrid film can reach a sheet resistance of 9.2 Ω sq⁻¹ with a transmittance of 83.4% at 550 nm wavelength, and a low root mean square (RMS) roughness (approximately 3.8 nm). After 10 000 bends and tape testing, the conductivity and transmittance of the hybrid film remain stable. The resistance of the film has no significant degradation after 14 d of exposure to high temperature of 85 °C and humidity of 85%, indicating excellent stability. The organic light-emitting diodes (OLEDs) with TCNT/AgNW/PEDOT hybrid film as anode exhibit high current density and luminosity, confirming this process has considerable potential application in photovoltaic devices.

Inorganic perovskite quantum dots (IPQDs) such as cesium lead halide (CsPbX₃, X = Cl, Br and I) quantum dots have attracted much attention for developing cadmium-free quantum light-emitting displays (QLEDs) based on outstanding light emission properties including narrow full width at half maximum (FWHM), tunable bandgap and ultrahigh (>90%) photoluminescence quantum yield (PLQY). Nevertheless, their poor stability under ambient conditions, at high temperature or under continuous light irradiation is the main problem for practical applications. In this study, a new method is proposed to effectively stabilize CsPbBr₃ IPQDs by synthesizing them with sulfate-functionalized cellulose nanocrystals (CNCs) at room temperature without using traditional quantum dot stabilizers such as oleylamine (OLA) and oleic acid (OA). The as-prepared CsPbBr₃ IPQD/CNC hybrid paper-like films are highly stable and the relative photoluminescence (PL) intensity can be maintained at 92% under continuous UV light (306 nm, 15 W) illumination for 130 h, >99% at high temperature (100 °C) for 130 h, and >99% in ambient conditions for 15 d. Additionally, the PLQY and FWHM of IPQD/CNC are 45.69% and 22 nm, respectively. The ultrahigh stability and narrow FWHM characteristics proposed here for IPQD/CNC hybrid films can provide new possibilities for practical applications in the future development of IPQD-related devices.

Commercially available Jeffamines (polyetheramine) with average molecular weights of 2000 and 3000 g mol⁻¹; one (M2005), two (D2000), and three (T3000) primary amino groups end-capping on the polyether backbone; and propylene oxide (PO) and ethylene oxide (EO) functionality were explored as additives for application in MAPbI₃ perovskite solar cells (PSCs). The results indicated that the embedding of Jeffamine additives effectively passivates the defects in the grain boundaries of perovskite through the coordination bonding between the nitrogen atom and the uncoordinated lead ion of perovskite. We fabricated p–i–n PSC devices with the structure of glass/indium tin oxide (ITO)/NiO_x/CH₃NH₃PbI₃ (with and without Jeffamine)/PC₆₁BM/BCP/Ag. We observed the interaction between the Jeffamine and perovskites. This interaction led to increased lifetimes of the carriers of perovskite, which enabled the construction of high-performance p–i–n PSCs. For the Jeffamine-D2000-derived device, we observed an increase in the power conversion efficiency from 14.5% to 16.8% relative to the control device. Furthermore, the mechanical properties of the perovskite films were studied. The interaction between the additive and perovskite reinforced the flexibility of the thin film, which may pave the way for stretchable optoelectronics.