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Electronic Supplementary Material (ESI) for Nanoscale. This journal is The Royal Society of Chemistry 2016 Electronic Supplementary Material (ESI) for Nanoscale. This journal is The Royal Society of Chemistry 2016 Supplementary Information Transparent actuators and robots based on single-layer superaligned carbon nanotube sheet and polymer composites Luzhuo Chen, a,b Mingcen Weng, a,b Wei Zhang,* a,b Zhiwei Zhou, c Yi Zhou, c Dan Xia, c Jiaxin Li, a,b Zhigao Huang, a,b Changhong Liu* c and Shoushan Fan c a Fujian Provincial Key Laboratory of Quantum Manipulation and New Energy Materials, College of Physics and Energy, Fujian Normal University, Fuzhou, 350007, China b Fujian Provincial Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Xiamen, 361005, China E-mail: wzhang721@163.com c Tsinghua-Foxconn Nanotechnology Research Center and Department of Physics, Tsinghua University, Beijing, 100084, China E-mail: chliu@mail.tsinghua.edu.cn S1

1. Transmittance spectra of the PET and BOPP film in the visible light wavelength region Fig. S1 Transmittance spectra of the PET and BOPP film in the visible light wavelength region. 2. SEM image showing the thickness of single-layer SACNT sheet coated with EVA in the trilayer actuator Fig. S2 SEM image showing the thickness of single-layer SACNT sheet coated with EVA in the trilayer actuator. S2

3. Calculation of curvature The curvature of the SACNT/PET/BOPP actuator is defined as the reciprocal radius (1/ρ). As the bending angle is given by the curvature 1/ρ is deduced as 1 θ = L ρ, (1) ρ = θ L. (2) Therefore, the curvature of the actuator can be calculated by achieving the bending angle and length of the actuator. The bending angle of the actuator is captured by using a digital camera. 4. Calculation of energy efficiency The energy efficiency of the transparent actuator can be defined as the generated elastic energy density divided by the electrical energy density. As the SACNT layer is very thin, our trilayer structure can be approximated to a bilayer structure of PET/BOPP. Thus, the elastic energy density of our actuator can be calculated by using the following equation: [1] W 1 = E 3t 3 2 3t 2 +t 3 +E 2 t 2 2 3t 3 +t 2 E 2 2 t 2 4 +E 3 2 t 3 4 +2E 2 E 3 t 2 t 3 2t 2 2 +2t 3 4 +3t 2 t 3 36E 2 E 3 t 2 2 t 3 2 t 3 +t 2 ( 1 ρ )2 (3) where W 1 is the elastic energy density, 1/ρ is the curvature (0.41 cm -1 ), t 2 and t 3 are the thickness of PET layer (80 µm) and BOPP layer (40 µm) respectively, E 2 and E 3 are the Young s modulus of PET layer and BOPP layer respectively. The Young s modulus of the PET layer and BOPP layer are 2.55 GPa and 1.10 GPa, which are measured by a material testing machine (Lloyd LR5k) with stretching rate of 0.5 mm min -1. The calculated elastic energy density is 3.4 10 4 J m -3. Assuming the actuation time of 30 s, S3

the total electrical energy density applied to the actuator is given by W 2 = p τ (4) where W 2 is the electrical energy density, p is the power density (14.37 mw mm -3 ), τ is the actuation time (30 s). The calculated electrical energy density is 4.3 10 8 J m -3. Hence, the energy efficiency η is given by The energy efficiency η is then calculated to be 0.008%. η = W 1 W 2 (5) 5. Control experiment Fig. S3 Pure thermal actuation of the SACNT/PET/BOPP actuator. The measured maximum curvatures for the pure thermal actuation are in accordance with those measured from electrothermal actuation experiments for the same temperature change. 6. Modeling of the SACNT/PET and PET/BOPP composites (1) Modeling of the SACNT/PET composite S4

We develop a model to analyze the bending performance of the SACNT/PET composite. Based on the bimetal thermostat equation of Timoshenko, [2] the curvature of the composite is given by 1 = 6 α 2 α 1 T T 0 1+m 2 ρ h(3 1+m 2 +(1+mn )(m 2 + 1 (6) )), mn where h is the total thickness of the composite, T is the temperature, T 0 is the initial temperature, α 1 is the CTE of CNT (3 ppm K -1 ), α 2 is the CTE of PET (38 ppm K -1 ),, (7) t 1 and t 2 are the thickness of SACNT layer and PET layer (80 µm) respectively, and, (8) E 1 and E 2 are the Young s modulus of SACNT layer and PET layer respectively. The SACNT layer is embedded in EVA resin and has a total thickness of 5 µm in the trilayer actuator. To simplify the modeling, we assumed that the thickness of SACNT layer t 1 is equivalent to a densified pure SACNT layer of ~50 nm. [3-4] The Young s modulus of SACNT layer is given as a constant of 2.2 GPa. [5] The Young s modulus of the PET layer is 2.55 GPa. (2) Modeling of the PET/BOPP composite We develop another model to analyze the bending performance of the PET/BOPP composite. Based on the bimetal thermostat equation of Timoshenko, [2] the curvature of the composite is given by S5, (9)

where h is the total thickness of the composite, T is the temperature, T 0 is the initial temperature, α 2 is the CTE of PET (38 ppm K -1 ), α 3 is the CTE of BOPP (137 ppm K -1 ),, (10) t 2 and t 3 are the thickness of PET layer (80 µm) and BOPP layer (40 µm)respectively, and, (11) E 2 and E 3 are the Young s modulus of PET layer (2.55 GPa) and BOPP layer (1.10 GPa) respectively. 7. Repeatability test Fig. S4 Cycle life of the SACNT/PET/BOPP actuator with a 0.1 Hz square wave voltage (0-20 V) for 10,000 cycles. As the repeatability test takes a long time, using the digital camera to capture the bending angle and then calculating the curvature is not efficient. Hence, a laser displacement sensor was used to record the free-end displacement of the actuator, which could demonstrate the repeatability of the actuator as well. D 0 represents the initial displacement value. S6

References: [1] E. Merced, X. Tan and N. Sepúlveda, Sensors Actuat. A- Phys., 2013, 196, 30. [2] S. Timoshenko, J. Opt. Soc. Am., 1925, 11, 233. [3] M. Zhang, S. Fang, A. A. Zakhidov, S. B. Lee, A. E. Aliev, C. D. Williams, K. R. Atkinson and R. H. Baughman, Science, 2005, 309, 1215. [4] K. Jiang, J. Wang, Q. Li, L. Liu, C. Liu and S. Fan, Adv. Mater., 2011, 23, 1154. [5] L. Zhang, G. Zhang, C. Liu, S. Fan, Nano Lett., 2012, 12, 4848. S7