Rational strategy enabling large-area molecular ordering, are important for creating high-performance organic devices. We show that, upon one-step hot-pressing with uniaxially stretched Teflon sheets, a polymer brush carrying azobenzene-containing mesogenic side chains self-assembles into a freestanding film, where the polymer backbone aligns homeotropically to the film plane and the side chains align horizontally. Such a three-dimensionally ordered structure forms through translation of a one-dimensional molecular order of the Teflon sheet and propagates from the interface macroscopically on both sides of the film.

  The resultant wide-area bimorph configuration allows the polymer film to bend rapidly and reversibly when the azobenzene units are photoisomerized. This film provides us with a new class of molecular muscles and other three-dimensional devices.

LIGHT-DRIVEN ARTIFICIAL MUSCLES MADE OF MOLECULARLY ORDERED POLYMER BRUSHES