Prof Yen-Hung Lin

Abstract:

Multivalent, resonance-stabilized amidinium ligands enable stronger chemical coordination and reduced deprotonation compared with conventional monovalent ammonium ligands in low-dimensional perovskites. Here, we introduce a controllable one- to two-dimensional (1D-to-2D) structural transition strategy by systematically tuning ligand conformation, thereby modulating hydrogen bonding, π-π stacking, and basicity to elucidate the relationship between molecular structure, interfacial interactions, and resulting dimensionality. The 1D-amidinium perovskite structure, with its pronounced geometric anisotropy, impedes uniform surface coverage and defect passivation. In contrast, the 2D-amidinium perovskite forms a continuous, homogeneous interfacial layer, enabling more effective defect passivation and favorable energy-level alignment. With dimensionality control, inverted 3D/2D-amidinium perovskite solar cells deliver 25.4% power conversion efficiency (1.1 square centimeters, steady-state certified) and maintain >95% of their initial efficiency after 1100 hours of continuous 1-sun operation at 85°C.

Abstract:

Perovskite solar cells (PSCs) are emerging as a particularly promising technology to enhance the world’s renewable energy generation capacity. As PSCs are transitioning from research to industrial-scale production, there is an important opportunity to establish sustainable manufacturing pathways. Here, we present a closed-loop framework for the development of environmentally sustainable PSCs and highlight strategies to achieve this vision. First, we analyse the sourcing of raw materials and compare two established PSC fabrication techniques, vapour-phase deposition and solution processing, evaluating their respective advantages and limitations in terms of economic feasibility and environmental impact. Second, we examine solution processing methods, focusing on solvent system design for the preparation of high-quality perovskite films and on the use of non-hazardous or less-hazardous solvents. Third, we examine potential lead-release concerns during PSC operation and discuss approaches to minimize associated environmental risks. Fourth, we summarize effective recycling methods for main PSC components to support a circular production model. Finally, we identify key challenges and outline future research directions to achieve fully sustainable, closed-loop PSC technologies.

Abstract:

Achieving efficient and stable formamidinium lead iodide (FAPbI3) perovskite solar cells (PSCs) requires integrated control of crystallization kinetics and defect suppression. While ionic liquids (IL) have shown promise as multifunctional additives, their rational design remains challenging. Here, we develop an attention-focus graph neural network (GNN) framework that combines the molecular features of IL with device-level characteristics of FAPbI3 PSCs. Our model identifies N-methyl-N-butylpyrrolidinium bis(trifluoromethylsulfonyl)imide ([MBPY][TFSI]) as an ideal dual-functional passivator. The [MBPY]⁺, acting as a Lewis base, passivates undercoordinated Pb²⁺ via Pb-N coordination bonds, whereas the [TFSI]⁻ anion mitigates interfacial defects via hydrogen bonding with FA⁺. It is found that the [MBPY]⁺ cation not only suppresses non-radiative recombination but also enhances the moisture resistance of the perovskite layer due to its hydrophobic alkyl chains. With the synergetic effect of [MBPY]⁺ and [TFSI]⁻ additives, the PSCs achieve a power conversion efficiency (PCE) of 25.03% with an open circuit voltage of 1.182 V, and retain 90.5% of their initial PCE after 1200 h storage at room temperature in air atmosphere (35% relative humidity). This work contributes to ongoing computational and experimental efforts in accelerating the exploration and prediction of potential ionic liquid passivation materials for perovskite solar cells. (Figure presented.).

Abstract:

The rational design of perovskite heterojunctions is crucial for advancing the efficiency and operational stability of perovskite solar cells (PSCs). However, conventional methods face challenges in precisely controlling interfacial phase purity at the nanoscale and achieving conformal heterojunction coverage. Herein, we report a 'soft-soft' interaction-guided strategy to tailor perovskite heterojunction formation by introducing dimethyl sulfide (DMS) as a soft Lewis base additive in the organic cation solution. The resulting DMS-modulated PSCs achieve a remarkable power conversion efficiency (PCE) of up to 26.70%, with a certified PCE of 26.48%. The devices exhibit exceptional operational stability, retaining over 94% of their initial PCE after 2000 h of maximum power point tracking under continuous 1-sun illumination (ISOS-L-1 protocol). Furthermore, the universality of this 'soft-soft' interaction strategy is validated across a range of diverse perovskite compositions and ligand systems, demonstrating its potential for scalable and reproducible PSC fabrication.

Abstract:

As the demand for edge platforms in artificial intelligence increases, including mobile devices and security applications, the surge in data influx into edge devices often triggers interference and suboptimal decision-making. There is a pressing need for solutions emphasizing low power consumption and cost-effectiveness. In-sensor computing systems employing memristors face challenges in optimizing energy efficiency and streamlining manufacturing due to the necessity for multiple physical processing components. Here, we introduce low-power organic optoelectronic memristors with synergistic optical and mV-level electrical tunable operation for a dynamic "control-on-demand" architecture. Integrating signal sensing, featuring, and processing within the same memristors enables the realization of each in-sensor analogue reservoir computing module, and minimizes circuit integration complexity. The system achieves 97.15% fingerprint recognition accuracy while maintaining a minimal reservoir size and ultra-low energy consumption. Furthermore, we leverage wafer-scale solution techniques and flexible substrates for optimal memristor fabrication. By centralizing core functionalities on the same in-sensor platform, we propose a resilient and adaptable framework for energy-efficient and economical edge computing.