Irfan Habib

Abstract:

Obtaining micron-thick perovskite films of high quality is key to realizing efficient and stable positive (p)-intrinsic (i)-negative (n) perovskite solar cells^1,2, but it remains a challenge. Here we report an effective method for producing high-quality, micron-thick formamidinium-based perovskite films by forming coherent grain boundaries, in which high-Miller-index-oriented grains grow on the low-Miller-index-oriented grains in a stabilized atmosphere. The resulting micron-thick perovskite films, with enhanced grain boundaries and grains, showed stable material properties and outstanding optoelectronic performances. The small-area solar cells achieved efficiencies of 26.1%. The 1-cm² devices and 5 cm × 5 cm mini-modules delivered efficiencies of 24.3% and 21.4%, respectively. The devices processed in a stabilized atmosphere presented a high reproducibility across all four seasons. The encapsulated devices exhibited superior long-term stability under both light and thermal stressors in ambient air.

Abstract:

Free charge generation after photoexcitation of donor or acceptor molecules in organic solar cells generally proceeds via (1) formation of charge transfer states and (2) their dissociation into charge separated states. Research often either focuses on the first component or the combined effect of both processes. Here, we provide evidence that charge transfer state dissociation rather than formation presents a major bottleneck for free charge generation in fullerene-based blends with low energetic offsets between singlet and charge transfer states. We investigate devices based on dilute donor content blends of (fluorinated) ZnPc:C60 and perform density functional theory calculations, device characterization, transient absorption spectroscopy and time-resolved electron paramagnetic resonance measurements. We draw a comprehensive picture of how energies and transitions between singlet, charge transfer, and charge separated states change upon ZnPc fluorination. We find that a significant reduction in photocurrent can be attributed to increasingly inefficient charge transfer state dissociation. With this, our work highlights potential reasons why low offset fullerene systems do not show the high performance of non-fullerene acceptors.

Abstract:

This dataset contains snapshots of the fitting of spectroscopic ellipsometry data using CompleteEase and NEXAFS data using QANT (Igor). This data was used in my thesis titled "An exploration of vacuum evaporable non-fullerene acceptors for use in organic solar cells and molecular orientation in evaporated thin films".

Abstract:

The record power conversion efficiency of solution-processed organic solar cells (OSCs) has almost doubled since non-fullerene acceptors (NFAs) replaced fullerene derivatives as the best-performing acceptor molecules. The successful transition from C60 to NFAs is still pending for vacuum-thermal evaporated (VTE) OSCs, not least because most NFAs are too large to be evaporated without breaking. Due to VTE’s relevance in terms of industrial manufacturing, discovering high-performing VTE NFAs is a major opportunity for OSCs. Here, we fabricate evaporated OSCs based on the NFA BTIC-H known from solution processing. This A–D–A molecule has an unfused bithiophene core, 1,1-dicyanomethylene-3-indanone end groups, and hexyl side chains, making it small enough to be evaporated well. We pair BTIC-H with four commonly used evaporated donors—DCV5T-Me(3,3), DTDCPB, HB194, and SubNc—in planar heterojunctions. We observe appreciable photocurrents and a voltage loss of ∼0.8 V, matching that of corresponding C60 devices. Donor:BTIC-H bulk heterojunctions likely face charge collection issues due to unfavorable microstructure. Our work demonstrates one of few NFA based evaporated OSCs with encouraging performance results and gives one potential starting point for molecule design of further NFAs suitable for VTE.

Abstract:

The advent of nonfullerene acceptors (NFAs) enabled records of organic photovoltaics (OPVs) exceeding 19% power conversion efficiency in the laboratory. However, high-efficiency NFAs have so far only been realized in solution-processed blends. Due to its proven track record in upscaled industrial production, vacuum thermal evaporation (VTE) is of prime interest for real-world OPV commercialization. Here, we combine the benchmark solution-processed NFA Y6 with three different evaporated donors in a bilayer (planar heterojunction) architecture. We find that voltage losses decrease by hundreds of millivolts when VTE donors are paired with the NFA instead of the fullerene C₆₀, the current standard acceptor in VTE OPVs. By showing that evaporated small-molecule donors behave much like solution-processed donor polymers in terms of voltage loss when combined with NFAs, we highlight the immense potential for evaporable NFAs and the urgent need to direct synthesis efforts toward making smaller, evaporable compounds.