Department of Chemistry and Chemical Biology, McMaster University, ON L8S 4M1, Canada.
John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138.
Proc Natl Acad Sci U S A. 2020 Feb 25;117(8):3953-3959. doi: 10.1073/pnas.1902872117. Epub 2020 Feb 6.
Next-generation photonics envisions circuitry-free, rapidly reconfigurable systems powered by solitonic beams of self-trapped light and their particlelike interactions. Progress, however, has been limited by the need for reversibly responsive materials that host such nonlinear optical waves. We find that repeatedly switchable self-trapped visible laser beams, which exhibit strong pairwise interactions, can be generated in a photoresponsive hydrogel. Through comprehensive experiments and simulations, we show that the unique nonlinear conditions arise when photoisomerization of spiropyran substituents in pH-responsive poly(acrylamide--acrylic acid) hydrogel transduces optical energy into mechanical deformation of the 3D cross-linked hydrogel matrix. A Gaussian beam self-traps when localized isomerization-induced contraction of the hydrogel and expulsion of water generates a transient waveguide, which entraps the optical field and suppresses divergence. The waveguide is erased and reformed within seconds when the optical field is sequentially removed and reintroduced, allowing the self-trapped beam to be rapidly and repeatedly switched on and off at remarkably low powers in the milliwatt regime. Furthermore, this opto-chemo-mechanical transduction of energy mediated by the 3D cross-linked hydrogel network facilitates pairwise interactions between self-trapped beams both in the short range where there is significant overlap of their optical fields, and even in the long range--over separation distances of up to 10 times the beam width--where such overlap is negligible.
下一代光子学设想了无电路、快速可重构的系统,其动力来自自陷光孤子光束及其粒子相互作用。然而,进展受到需要可逆响应材料的限制,这些材料可以承载这种非线性光学波。我们发现,在光响应水凝胶中可以产生可重复切换的自陷可见光激光束,其表现出强烈的两两相互作用。通过全面的实验和模拟,我们表明,当 pH 响应聚(丙烯酰胺-丙烯酸)水凝胶中的螺吡喃取代基的光异构化将光学能量转换为 3D 交联水凝胶基质的机械变形时,会出现独特的非线性条件。当局部的异构化诱导水凝胶收缩并排出水时,高斯光束会自捕获,产生一个瞬态波导,束缚光场并抑制发散。当光场依次移除和重新引入时,波导在几秒钟内被擦除和重新形成,允许自捕获光束以低至毫瓦级的功率在毫秒范围内快速、反复地开启和关闭。此外,通过 3D 交联水凝胶网络介导的这种光-化学-机械能量转换,有助于自捕获光束之间的两两相互作用,无论是在光学场有显著重叠的短程范围内,还是在光学场重叠可以忽略不计的远程范围内,甚至在分离距离达到光束宽度的 10 倍以上的远程范围内。