article published yes Miranda M. Sroda author Jaejun Lee author Younghoon Kwon author Friedrich J Stricker author 7aca2cfc-46cf-11f0-abd3-8c96b5186745 Minwook Park author Megan T. Valentine author Javier Read de Alaniz author We investigate the influence of the host matrix on the photothermally driven actuation performance of negatively photochromic, donor−acceptor Stenhouse adduct (DASA)-based polymers. Using a modular Diels−Alder “click” platform, we designed polymeric materials with varying DASA incorporation and investigated the relationships between the material composition and the resulting physical, mechanical, and photoswitching properties. We demonstrate that increasing the DASA concentration in polymer conjugates has a dramatic effect on the material’s physical and mechanical properties, such as the glass transition temperature (Tg) and elastic modulus, as well as the photoswitching properties, which are found to be highly dependent on Tg. We establish using a simple photoresponsive bilayer that actuation performance is controlled by the bilayer stiffness rather than the photochrome incorporation of DASA. Finally, we report and compare the light-induced property changes in Tg and the elastic modulus between the materials comprising the open or closed forms of DASAs. Our results demonstrate the importance of designing a material that is stiff enough to provide the mechanical strength required for actuation under load, but soft enough to reversibly switch at the operational temperature and provide key considerations for the development of application-geared photoswitchable materials. American Chemical Society2022 eng donor−acceptor Stenhouse adductsphotothermal actuationphoto-induced property changesnegative photochromismglass transition temperature 2637-610510.1021/acsapm.1c01108 41141-149 yes Sroda MM, Lee J, Kwon Y, et al. Role of material composition in photothermal actuation of DASA-based polymers. <i>ACS Applied Polymer Materials</i>. 2022;4(1):141-149. doi:<a href="https://doi.org/10.1021/acsapm.1c01108">10.1021/acsapm.1c01108</a> Sroda, M. M., Lee, J., Kwon, Y., Stricker, F. J., Park, M., Valentine, M. T., &#38; Read de Alaniz, J. (2022). Role of material composition in photothermal actuation of DASA-based polymers. <i>ACS Applied Polymer Materials</i>. American Chemical Society. <a href="https://doi.org/10.1021/acsapm.1c01108">https://doi.org/10.1021/acsapm.1c01108</a> M.M. Sroda, J. Lee, Y. Kwon, F.J. Stricker, M. Park, M.T. Valentine, J. Read de Alaniz, ACS Applied Polymer Materials 4 (2022) 141–149. Sroda, Miranda M., et al. “Role of Material Composition in Photothermal Actuation of DASA-Based Polymers.” <i>ACS Applied Polymer Materials</i>, vol. 4, no. 1, American Chemical Society, 2022, pp. 141–49, doi:<a href="https://doi.org/10.1021/acsapm.1c01108">10.1021/acsapm.1c01108</a>. M. M. Sroda <i>et al.</i>, “Role of material composition in photothermal actuation of DASA-based polymers,” <i>ACS Applied Polymer Materials</i>, vol. 4, no. 1. American Chemical Society, pp. 141–149, 2022. Sroda MM, Lee J, Kwon Y, Stricker FJ, Park M, Valentine MT, Read de Alaniz J. 2022. Role of material composition in photothermal actuation of DASA-based polymers. ACS Applied Polymer Materials. 4(1), 141–149. Sroda, Miranda M., Jaejun Lee, Younghoon Kwon, Friedrich J Stricker, Minwook Park, Megan T. Valentine, and Javier Read de Alaniz. “Role of Material Composition in Photothermal Actuation of DASA-Based Polymers.” <i>ACS Applied Polymer Materials</i>. American Chemical Society, 2022. <a href="https://doi.org/10.1021/acsapm.1c01108">https://doi.org/10.1021/acsapm.1c01108</a>. 218242026-05-06T10:59:35Z2026-05-11T07:46:45Z