Emulsion-based, resonant infrared matrix-assisted pulsed laser evaporation (RIR-MAPLE) has been demonstrated as an alternative technique to deposit conjugated polymer films for photovoltaic applications; yet, a fundamental understanding of how the emulsion target characteristics translate into film properties and solar cell performance is unclear. Such understanding is crucial to enable the rational improvement of organic solar cell (OSC) efficiency and to realize the expected advantages of emulsionbased RIR-MAPLE for OSC fabrication. In this paper, the effect of the primary solvent used in the emulsion target is studied, both experimentally and theoretically, and it is found to determine the conjugated polymer cluster size in the emulsion as well as surface roughness and internal morphology of resulting polymer films. By using a primary solvent with low solubility-in-water and low vapor pressure, the surface roughness of deposited P3HT and PCPDTBT polymer films was reduced to 10 nm, and the efficiency of P3HT:PC 61 BM OSCs was increased to 3.2% (∼100 times higher compared to the first MAPLE OSC demonstration [Caricato, A. P.; et al. Appl. Phys. Lett. 2012, 100, 073306]). This work unveils the mechanism of polymer film formation using emulsion-based RIR-MAPLE and provides insight and direction to determine the best ways to take advantage of the emulsion target approach to control film properties for different applications.

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Multifunctional films combining switchable biocidal and fouling release properties were deposited on substrates using RIR-MAPLE.

Some of the most exciting materials research in the 21st century attempts to resolve the challenge of simulating, synthesizing, and characterizing new materials with unique properties designed from first principles. Achievements in such development for organic and organic-inorganic hybrid materials make them important options for electronic and/or photonic devices because they can impart multi-functionality, flexibility, transparency, and sustainability to emerging systems, such as wearable electronics. Functional organic materials include small molecules, oligomers, and polymers, while hybrid materials include inorganic nanomaterials (such as zero-dimensional quantum dots, one-dimensional carbon nanotubes, or two-dimensional nanosheets) combined with organic matrices. A critically important step to implementing new electronic and photonic devices using such materials is the processing of thin films. While solution-based processing is the most common laboratory technique for organic and hybrid materials, vacuum-based deposition has been critical to the commercialization of organic light emitting diodes based on small molecules, for example. Therefore, it is desirable to explore vacuum-based deposition of organic and hybrid materials that include larger macromolecules, such as polymers. This review article motivates the need for physical vapor deposition of polymeric and hybrid thin films using matrix-assisted pulsed laser evaporation (MAPLE), which is a type of pulsed laser deposition. This review describes the development of variations in the MAPLE technique, discusses the current understanding of laser-target interactions and growth mechanisms for different MAPLE variations, surveys demonstrations of MAPLE-deposited organic and hybrid materials for electronic and photonic devices, and provides a future outlook for the technique.

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Resonant-infrared, matrix-assisted pulsed laser evaporation (RIR-MAPLE) has been used to deposit blended, organic thin-films with nanoscale domain sizes of constituent polymers, small molecules, or colloidal nanoparticles. In the emulsion-based RIR-MAPLE process, the target contains a nonpolar, organic solvent phase and a polar, water phase. The emulsion properties have a direct impact on the nanoscale morphology of single-component organic thin films, while the morphology of blended, organic thin films also depends on the RIR-MAPLE deposition mode. In addition to these fundamental aspects, applications of blended organic films (organic solar cells, anti-reflection coatings, and multi-functional surfaces) deposited by emulsion-based RIR-MAPLE are presented. Importantly, domain sizes in the blended films are critical to thin-film functionality.