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1 advances.sciencemag.org/cgi/content/full/4/4/eaar5762/dc1 Supplementary Materials for Near-infrared light responsive dynamic wrinkle patterns The PDF file includes: Fudong Li, Honghao Hou, Jie Yin, Xuesong Jiang Published 6 April 2018, Sci. Adv. 4, eaar5762 (2018) DOI: /sciadv.aar5762 section S1. Experimental section section S2. Results and discussion fig. S1. Image of CNT-PDMS that retains good transparency. fig. S2. UV-vis-NIR spectrum of CNT-PDMS. fig. S3. The temperature variation during NIR on/off switch monitored by an infrared camera. fig. S4. Temperature variation during NIR light radiation with different intensities monitored by an infrared camera. fig. S5. Temperature variation during 365-nm UV light radiation. fig. S6. Temperature variation during the exposure of green laser beam. fig. S7. The synthesis route to PSF. fig. S8. The synthesis route to AN. fig. S9. The synthesis route to PAN. fig. S10. Wrinkles occur through NIR radiation. fig. S11. Various wrinkles across different scales. fig. S12. Various functional polymers served as the skin layers, including PSF, PMMA, PAN and gelatin. fig. S13. Control experiments of the NIR-driven dynamic wrinkle pattern. fig. S14. UV-vis spectra of dimerization of PAN. fig. S15. The evolution process of PAN/CNT-PDMS wrinkles during NIR on/off cycles. fig. S16. The extinction/formation process of the circular wrinkle pattern via NIR on/off switch. fig. S17. The influence of the morphology and size of wrinkles and the laser beam on the diffraction patterns. Legends for movies S1 to S3

2 Other Supplementary Material for this manuscript includes the following: (available at advances.sciencemag.org/cgi/content/full/4/4/eaar5762/dc1) movie S1 (.mp4 format). Video of the fully wrinkled pattern s disappearance/formation behavior. movie S2 (.mp4 format). Video of the striped wrinkled pattern s disappearance/formation cycle. movie S3 (.mp4 format). Video of the diffraction ring/light spot switch corresponding to the wrinkled/wrinkle-free state of surface pattern.

3 section S1. Experimental section fig. S1. Image of CNT-PDMS that retains good transparency. The CNT content in the composited CNT-PDMS is approximately 0.05%. 1.5 Absorption Wavelength (nm) fig. S2. UV-vis-NIR spectrum of CNT-PDMS.

fig. S3. The temperature variation during NIR on/off switch monitored by an infrared camera.

Temperature variation during NIR light radiation with different intensities monitored by an

5 W/cm 2, 1.0 W/cm 2 and 0.75 W/cm 2, respectively. fig. S5.

4 fig. S3. The temperature variation during NIR on/off switch monitored by an infrared camera. The CNT contents in the composited CNT-PDMS is 0.05%. NIR light intensity is 1.5 W/cm 2. fig. S4. Temperature variation during NIR light radiation with different intensities monitored by an infrared camera. The CNT content in CNT-PDMS is 0.05%. The NIR light intensity in (a-c) is 1.5 W/cm 2, 1.0 W/cm 2 and 0.75 W/cm 2, respectively. fig. S5. Temperature variation during 365-nm UV light radiation. The CNT content in CNT- PDMS is 0.05%. The UV light intensity is approximately 15 mw/cm 2.

5 fig. S6. Temperature variation during the exposure of green laser beam. The CNT content in CNT-PDMS is 0.05%. The wavelength of green laser is 532 nm. fig. S7. The synthesis route to PSF.

6 fig. S8. The synthesis route to AN. (a) The synthesis route to AN. (b) 1 H NMR spectrum of AN in d-dmso. fig. S9. The synthesis route to PAN.

7 section S2. Results and discussion 2.1 Surface pattern and the applied strain to trigger wrinkle formation in the bilayer system According to linear bucking theory, the amplitude and wavelength of wrinkle is given as Equation S1 and S2 (S1) Here, (S2) refers to the critical strain to trigger wrinkle formation and is given as Equation S3 (S3) Then adapt Equation S1 to Equation S4 (S4) Both sides of Equation S4 were taken as the natural logarithm and with the proper deformation, we can obtain Equation S5 relating wrinkle amplitude A to the applied strain (13) (S5) 2.2 The critical strain of the formation and erasure of the NIR-driven dynamic wrinkle system According to linear bucking theory, the critical strain to trigger wrinkle formation in filmsubstrate bilayer system is given as following equation, (S3), (S6), where subscript f and s refer to the skin layer and the substrate of the bilayer system; represent in-plane modulus, Young s modulus and Poisson s ratio, respectively (2-5). In our experiments, the parameters for PSF and CNT-PDMS are: The resulting critical strain is approximately 1.3% according to Equation S3. The applied strain when the bilayer system is radiated by NIR is calculated via Equation S7, (S7), where refer to the coefficient of thermal expansion and temperature variation. Since, Equation S7 can be simplified as (S8). Here,

When temperature increased from room temperature to 80 and then cooled to room temperature, wrinkle occurred to minimize the total energy of the system.

8 When temperature increased from room temperature to 80 and then cooled to room temperature, wrinkle occurred to minimize the total energy of the system. The corresponding practical strain ( ) is approximately 1.8% ( ). As a result, the critical elimination strain is. When the wrinkle was eliminated via radiation by NIR for 20 s, the temperature variation is approximately 20 ( ) and the corresponding applied strain ( ) is approximately 0.6% according to Equation S7, which has exceeded the critical elimination strain ( ) and consequently causes wrinkle elimination. 2.3 Wrinkle formation triggered by NIR radiation fig. S10. Wrinkles occur through NIR radiation. A smooth surface converts into wrinkled state through NIR radiation for 2.5 min and then cooling to room temperature. The CNT content is approximately 0.05% in CNT-PDMS. NIR intensity is 1.5 W/cm 2.

2.4 The wrinkle patterns across different scales fig. S11.

The thickness is 45 nm, 77 nm, 122 nm and 173 nm, respectively.

9 2.4 The wrinkle patterns across different scales fig. S11. Various wrinkles across different scales. (a-d) AFM images and related profile images that green lines pass through by controlling the thickness of the skin layer. The thickness is 45 nm, 77 nm, 122 nm and 173 nm, respectively. (e) Wavelength (red square, left vertical axis) and amplitude (black triangle, right vertical axis) as a function of the thickness of the skin layer.

NIR intensity is 1.5 W/cm 2. Scale bar is 100 m. 2.6 Control experiments to explore the factors to determine the rate of erasure/generation cycle fig.

10 2.5 Varieties of functional polymers as the skin layer materials fig. S12. Various functional polymers served as the skin layers, including PSF, PMMA, PAN and gelatin. The CNT content is approximately 0.05%. NIR intensity is 1.5 W/cm 2. Scale bar is 100 m. 2.6 Control experiments to explore the factors to determine the rate of erasure/generation cycle fig. S13. Control experiments of the NIR-driven dynamic wrinkle pattern. (a-f) Optical images of extinction/formation cycle of PSF/CNT-PDMS wrinkle system. The CNT content is

11 0.025%. (g) Optical images of winkle pattern transformation. The CNT extent is 0.01%. The NIR light intensity is 1.5 W/cm 2. (h-i) The effect of NIR light intensity on the rate of extinction/formation process. The light intensity is 1.0 W/cm 2 and 0.75 W/cm 2, respectively. The CNT content is 0.05%. The scale bar is 100 m. 2.7 Dimerization dynamics of PAN min 5 min 15 min 45 min 85 min 145 min Absorbance Wavelength (nm) fig. S14. UV-vis spectra of dimerization of PAN. Experimental condition: the toluene solution of PAN was spin-coated on quartz plate, and the sample was radiated by 365 nm UV-light under nitrogen protection. 2.8 Various resulted spatially controllable wrinkle patterns via varying photomasks fig. S15. The evolution process of PAN/CNT-PDMS wrinkles during NIR on/off cycles. The CNT content is approximately 0.05%. NIR intensity is 1.5 W/cm 2.

$The influence of the morphology and size of wrinkles and the laser beam on the diffraction patterns.$

12 fig. S16. The extinction/formation process of the circular wrinkle pattern via NIR on/off switch. The CNT content is approximately 0.05%. NIR intensity is 1.5 W/cm Dynamic gratings fig. S17. The influence of the morphology and size of wrinkles and the laser beam on the diffraction patterns. The wavelength of green laser and red laser is 532 nm and nm, respectively. The scale bar is 100 m.

13 Movies movie S1. Video of the fully wrinkled pattern s disappearance/formation behavior. movie S2. Video of the striped wrinkled pattern s disappearance/formation cycle. movie S3. Video of the diffraction ring/light spot switch corresponding to the wrinkled/wrinkle-free state of surface pattern.

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