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Photothermal Bimorph Actuators with In-Built Cooler


for Light Mills, Frequency Switches, and Soft Robots
Jingjing Li, Rui Zhang, Linlin Mou, Monica Jung de Andrade, Xiaoyu Hu, Kaiqing Yu,
Jinkun Sun, Tianjiao Jia, Yuanyuan Dou, Hong Chen, Shaoli Fang, Dong Qian,
and Zunfeng Liu*

hygroscopic seed dispersal,[2] tendril


Photothermal bimorph actuators are widely used for smart devices, which curling of climbing plants,[3] and trap
are generally operated in a room temperature environment, therefore a low closure of carnivorous plants.[4] Inspired
temperature difference for actuation without deteriorating the performance by these natural organisms, soft robots,
is preferred. The strategy for the actuator is assembling a broadband-light smart control, and motor system have
been developed based on artificial
absorption layer for volume expansion and an additional water evaporation
bimorph actuators.[5] Photothermal actua-
layer for cooling and volume shrinkage on a passive layer. The response tors and devices are highly desirable in
time and temperature-change-normalized bending speed under NIR, white, the field of bionics and material science
and blue light illumination are at the same level of high performance, fast because of the specific advantages such
photothermal actuators based on polymer or polymer composites. The as wireless remote control, abundant light
classical beam theory and finite element simulations are also conducted to source, and non-electromagnetic distur-
bance.[6] For instance, a soft robot made by
understand the actuation mechanism of the actuator. A new type of light reduced graphene oxide-carbon nanotube/
mill is designed based on a wing-flapping mechanism and a light-modulated polydimethylsiloxane (rGO-CNT/PDMS)
frequency switch. A fast-walking robot (with a speed of 26 mm s−1) and a composite film can move forward at
fast-and-strong mechanical gripper with a large weight-lifting ratio (≈2142), an average speed of 1.6 cm s−1.[7] A soft
respectively, are also demonstrated. gripper was designed based on sodium
alginate/WS2 actuator with a high weight-
lifting ratio of 500.[8] A light mill was devel-
oped based on liquid crystal actuators.[9]
1. Introduction Although limited success has been reported, the performance
of photothermally driven smart devices is still not acceptable
In nature, many animals and plants demonstrate multi- for practice due to the limitations of bending speed, bending
modal locomotor capabilities using asymetrical expansion of amplitude, and symmetrical reversibility of the photothermal
bilayer structures, such as wing flapping of birds and insects,[1] actuators.[10] Generally large temperature-difference is generally
used to achieve large bending amplitude in actuation.[11] As we
J. Li, L. Mou, X. Hu, K. Yu, J. Sun, T. Jia, Y. Dou, Dr. Z. Liu know, most of the smart devices are used at room temperature
State Key Laboratory of Medicinal Chemical Biology in daily life, therefore it is highly desirable to operate the photo-
Key Laboratory of Functional Polymer Materials thermal actuator under relatively small temperature change
College of Pharmacy without deteriorating the actuation performance.[12] Moreover,
Nankai University
Tianjin 300071, China devices that can be controlled via a broad spectrum of light
E-mail: liuzunfeng@nankai.edu.cn are strongly preferred for different operation conditions and
R. Zhang, Prof. D. Qian needs.[13] Additionally, the potential applications of bimorph
Department of Mechanical Engineering actuators should be very broad but currently still largely unex-
University of Texas at Dallas plored,[9] for example, photothermal switch with frequency
Richardson, TX 75080, USA
modulation has not been realized, which is important for fre-
Dr. M. Jung de Andrade, Dr. S. Fang
Alan G. MacDiarmid NanoTech Institute
quency signal transmission and communication.
University of Texas at Dallas In most of conventional bilayer photothermal actuators, it is
Richardson, TX 75080, USA composed of a thermal expansion layer and a passive layer, and
Prof. H. Chen the actuator bends to the passive layer upon heat generated by
School of Materials Science and Energy Engineering light irradiation due to the mismatch in coefficient of thermal
Foshan University expansion (CTE).[10] Attempts have been made to increase the
Foshan 528325, China
bending speed, response time, and bending amplitude of the
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/adfm.201808995.
bimorph actuators by increasing the difference in CTE or
the temperature difference between the two layers and reducing
DOI: 10.1002/adfm.201808995 the thickness.[5c,11]

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We here have designed trilayered photothermal actuators NIR region (400−2600 nm), whereas the PET and acrylic
containing a cooling layer, which also enhance the actuation layer exhibit almost no absorption in this range, indicating
performance by water evaporation-induced volume shrinking. It that the ink layer may have strong photothermal effect. Then
can achieve fast responses of 0.36, 0.20, and 0.27 s under NIR, photothermal experiments are carried out on the IPAT-0 film
white, and blue light, respectively, at relatively small temperature under NIR irradiation. The temperature increased from 25.0 to
changes (9.9, 4.9, and 12.8 °C). The trilayered photothermal actu- 53.7 °C over 5 s (heating of 28.7 °C) for the IPAT-0 film under
ator achieves higher bending speed (71.1 cm−1 s−1 and 725ο s−1) 100 mW cm−2 NIR irradiation, while much lower temperature
at much lower temperature increase (9.9 and 4.9 °C) under NIR change (4.5 °C) was found in the PET film (Figure 1d) under
and white light than the equivalent bilayered actuator without a the same conditions, indicating strong photothermal effect
cooling layer. We designed a light-modulated electrical switch of the ink layer. Compared with the IPAT-0 film, a much less
with frequency modulation and a new type of light mill based rise in temperature from 25.0 to 37.1 °C over 5 s (heating of
on a wing-flapping mechanism. We further demonstrated the 12.1 °C) was observed for the IPAT-2 film under the same con-
application of trilayered actuator as a soft crawl robot with a fast ditions, demonstrating strong cooling effect of the acrylic layer.
speed (≈26 mm s−1) and a fast-and-strong mechanical gripper To research the origin of this cooling effect of the acrylic
with a large weight-lifting ratio (≈2142), respectively. layer, we investigated the water-evaporation dynamics of the
IPAT-2 film, which showed that the acrylic layer lost 5.1 wt%
in water over 6 s when it was exposed to 50 mW cm−2 NIR
2. Results and Discussion irradiation (Figure S3, Supporting Information). In contrast,
the absence of an acrylic layer in the IPAT-0 film caused it to
2.1. Physical Properties and Actuation Mechanism exhibit minimal water loss (0.8 wt%) under the same condi-
of the Actuators tions (Figure S3, Supporting Information). Therefore, photo-
thermally induced water evaporation in acrylic layer resulted
The thermal expansion layer is constituted by a carbon black in lower temperature rise in IPAT-2 than that in IPAT-0. By
slurry, which absorbs a broad spectrum of light and converts it switching off NIR illumination, the film can be restored to its
to heat, and polyethylene terephthalate (PET) film is used as a original mass by adsorbing water from the air (Figure S4a,b,
passive layer. The cooling layer is made by coating waterborne Supporting Information), indicating a reversible water adsorp-
acrylic adhesive on the other side of the PET film, which can tion/desorption in acrylic layer. The fast reabsorption of water
produce water desorption upon heating. The water evapora- may be ascribed to the high affinity of the acrylic layer to water.
tion results in decrease of film temperature, accompanied by In order to elaborate the interaction mechanism of water mol-
volume shrinkage, which can increase the bending amplitude ecules in the acrylic layer, we investigated the Fourier transform
of the actuator. It is worth mentioning that this acrylic layer also infrared (FTIR) spectrum of the acrylic layer at water-adsorption
has a certain adhesion, so it can increase the interaction force and freeze-dried states (Figure S5, Supporting Information).
between the film and the object when used as a smart gripper. The absorption band at 3417 cm−1 of the freeze-dried acrylic
Briefly, this photothermal trilayered actuator containing an layer is attributed to the stretching vibration of the hydroxyl
in-built cooling system was prepared as follows. A shading ink groups (−OH), and the FTIR spectrum of the wet acrylic layer
containing carbon black was coated on a PET film to form a black has a redshift at 3448 cm−1, indicating strong interaction
ink layer, and then an acrylic adhesive was coated on the other between adsorption water molecule and the hydroxyl groups.[14]
side of the PET film to form different thickness, as shown in We then measured the thermal expansion coefficient of each
Figure 1a. The thickness of the ink, PET, and acrylic adhesive is layer in the IPAT-2 actuator to understand their mechanical
about 1.2, 1.6, and 2 µm, respectively (Figure 1b). The scanning function in actuation. The results show that there is large
electron microscopy (SEM) image of the ink surface shows that a mismatch in CTE between the ink layer (106 × 10−6 K−1) and
large number of carbon black particles are deposited on the sur- the PET layer (40 × 10−6 K−1), which would result in bending
face of ink layer (Figure 1c). We refer to such an ink-PET-acrylic toward the PET side upon light irradiation. We experimentally
trilayered actuator as an IPAT-x, where the notation x indicates measured the volume change of the acrylic layer upon heating
that the film thickness of the acrylic layer is x µm. The IPAT-0 in air, and the results showed that the volume decreased
denotes an ink-PET bilayered structure, which is used as a con- due to water evaporation. Therefore, an equivalent CTE of the
trol sample to study the function of the acrylic layer (Figure S1, acrylic layer is introduced here and determined as a negative
Supporting Information). Similarly, a PET-acrylic bilayered value of −2.8  × 10−3 K−1 (Figure S6, Supporting Information).
(PAB) film was prepared to study the function of the ink layer, This shrinking of the acrylic layer might enhance the bending
where the thickness of the acrylic layer is 2 µm. Unless other- actuation of the IPAT-2 actuator. Therefore, it is expected that
wise specified, IPAT-2 and IPAT-0 actuators are used for further the IPAT-2 film can generate bending actuation under light
investigations in this paper. irradiation, as schematic illustrated in Figure 1e.
In order to investigate the photothermal effect of the ink
layer and the cooling effect of the acrylic layer, the following
characterizations are carried out on the IPAT-2, IPAT-0, and 2.2. Photothermal Actuation under NIR, White, and Blue Light
PAB films. UV–vis absorption is first carried out on the ink
layer, the PET layer, and the acrylic layer, as shown in Figure S2 Based on the strong light absorption of the ink layer in a
in the Supporting Information. The ink layer shows strong broadband spectrum, photothermal actuation of the IPAT-2
absorption over a wide spectral band from the visible to the actuator was investigated under irradiation of different types of

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Figure 1.  Fabrication and characterization of IPAT-x actuator. a) Schematic illustration of the fabrication process of the IPAT-x actuator. b) Cross-
sectional SEM image of the IPAT-2 actuator. c) SEM image of the ink surface. d) Temperature as a function of time for the ink layer of IPAT-2, IPAT-0, and
PAB films under 100 mW cm−2 NIR irradiation (760−2600 nm). e) Schematic illustration of an IPAT-x actuator showing the synergistic effect between
the photothermal expansion of an ink layer and the shrinkage of an acrylic layer via water evaporation.

light including NIR, white, and blue light at relative humidity temperature change. Since the bending of the IPAT actuator
(RH) of ≈ 25%. In order to explore the cooling effect and the under NIR illumination does not result in a circular arc struc-
volume-shrinking effect of the acrylic layer on the actuation, the ture, the maximum curvature (κ) of the actuator under NIR
actuation behavior of the IPAT-0 actuator was also investigated illumination is used to evaluate the actuation performance in
under the same conditions. the following.[16] Also the response time (t), temperature change
(ΔT), and speed (v  =  κ/t) to reach the maximum bending
are discussed. The IPAT-2 actuator reached a plateau curvature
2.2.1. Photothermal Actuation of IPAT Actuators under NIR of 7.6 cm−1 within 0.36 s, corresponding to a large bending
Light speed of 71.1 cm−1 s−1, upon exposure to 150 mW cm−2 NIR
illumination as the temperature increased from 25.0 to 34.9 °C,
It is well known that NIR light has a stronger photothermal and the actuator then returned to the initial state within
effect than short-wavelength light as well as relatively strong 0.44 s (Figure 2b). It can be concluded that the bending cur-
penetration and is widely used in photoheating.[15] Therefore, vature increases with increasing temperature in this dynamic
the actuation performance of IPAT actuators are first character- process, and the bending curvature increase with temperature
ized under NIR irradiation (760−2600 nm). Unless otherwise change (Figure 2d). The NIR light having a light intensity of
specified, the dimensions of the IPAT actuator investigated are 100–300 mW cm−2 are good enough for photothermal heating
10 mm × 1 mm. Figure  2a and Figure S7 in the Supporting and are mostly used to initiate photothermal actuation,[11a] so we
Information show the recorded optical and infrared images, investigated the actuation of IPAT-2 under 90–150 mW cm−2.
indicating a fast and reversible actuation process and a small The bending curvature and corresponding temperature of the

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Figure 2. NIR-light actuation of IPAT-2 actuators. a) Photographs of an IPAT-2 actuator during an actuation cycle driven by NIR light
(150 mW cm−2). b) Time dependence of the bending curvature and temperature of an IPAT-2 actuator exposed to NIR light when the light
is switched on and off. The dotted line indicates the NIR light is switched off. c) Finite element analysis results for the effective stress
distribution associated with bending actuation for an IPAT-2 actuator. d) Experimental data and the classical beam theoretical analysis of
the bending curvature as a function of the temperature change for IPAT-2 and IPAT-0 actuators. The error bar indicates standard deviations
calculated by five parallel tests. e) Experimental data and the classical beam theoretical analysis of the bending curvature and the measured
temperature for an IPAT-2 actuator as a function of the NIR-light light intensity. The error bar indicates standard deviations calculated by five
parallel tests.

actuator are plotted as a function of time and light intensity in change to reach the maximum bending (+9.9  °C) is one of
Figure 2e, and the bending curvature and temperature change the lowest temperature change, such as CNT-paper/biaxially
increased linearly with light intensity. oriented polypropylene (BOPP) actuator (37.7 °C),[20] and
Below we compared the performance of the IPAT actua- GO-polydopamine/rGO actuator (17 °C).[16] The actuation
tors with previously published actuators under NIR irradiation curvature (7.6 cm−1) and speed (71.1 cm−1 s−1) are also at the
(Table S1, Supporting Information). Compared with other NIR same level of the NIR-responsive actuators based on polymer
photothermal bimorph actuators, the response time (0.36 s) of or polymer composites.[11b,17,21] The fast forwarding (0.36 s) and
our IPAT-2 actuator is comparable to some actuators such as reversing (0.44 s) bending actuation indicates high symmetrical
graphene oxide (GO)/polyvinylidene fluoride (PVDF) (0.3 s),[17] reversibility comparable to other best symmetrical bimorph
rGO/GO actuator (0.73 s),[18] and CNT/polyethylene actuator actuators. This symmetrical switching-on and switching-off
(1.43 s),[11b] and longer than the VO2/metallic CNT (2.4 ms),[19a] time is preferred when the actuator is used as remote smart
and W-VO2-CNT (29 ms) actuators.[19c] The temperature control, soft robotics, grippers, and electrical switches.

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Figure 3.  White light and blue light actuation of IPAT-2 actuators. a,b) Photographs of an IPAT-2 actuator during an actuation cycle driven by white
light and blue light (30 mW cm−2). c) Repeatable actuation of an IPAT-2 actuator for 10 000 cycles (The inset is time dependence of the bending
angle and temperature of an IPAT-2 actuator exposed to white light when the light is switched on and off, and the arrow indicates the light was
switched off ). d) Time dependence of the bending angle and temperature of an IPAT-2 actuator exposed to blue light when the light is switched
on and off. e) Bending angle of an IPAT-2 actuator as a function of actuation frequency under white light and blue light illumination (The inset
is the schematic illustration of the bending angle for the IPAT-2 actuator). f ) Comparison of the actuation temperature difference and response
time of an IPAT-2 actuator under irradiation with NIR light and visible light with results from the literature. The literatures with available and
accurate values of response time and temperature change and the response time less than 10 s were selected. Reproduced with permission.[5a]
Copyright 2017, Wiley-VCH. Reproduced with permission.[5e] Copyright 2017, Royal Society of Chemistry. Reproduced with permission.[7]
Copyright 2015, Wiley-VCH. Reproduced with permission.[11a] Copyright 2016, Wiley-VCH. Reproduced with permission.[11b] Copyright 2018,
American Chemical Society. Reproduced with permission[13a] Copyright 2014, Nature. Reproduced with permission.[16] Copyright 2015, Science.
Reproduced with permission.[19a] Copyright 2017, Science. Reproduced with permission.[19b] Copyright 2015, American Chemical Society.
Reproduced with permission.[19c] Copyright 2017, American Chemical Society. Reproduced with permission.[20] Copyright 2018, Royal Society of
Chemistry. Reproduced with permission.[25a] Copyright 2016, American Chemical Society. Reproduced with permission.[25b] Copyright 2018, Royal
Society of Chemistry.

As the bending curvature and bending speed depend on com- under NIR irradiation (Figure 3f and Table S1, Supporting Info
plicated parameters of the actuators, including the mechanical rmation).[5e,11a,b,16,20]
properties, dimensions, temperature change, etc., it is difficult
to make absolute comparisons with literatures by normalizing Role of the Cooling Layer on Actuation: In Section 2.1, we
these values. We here focus on the actuation performance by found that the acrylic layer had a cooling effect and exhibited
considering temperature change using temperature-change- volume shrinking via water evaporation under heating. It is
normalized curvature (κΔT  =  κ/ΔT) and speed (vΔT  =  v/ΔT), hypothesized that this water-evaporation-induced cooling may
obtaining values of 0.76 cm−1  °C−1 and 7.18 cm−1 s−1  °C−1, decrease the temperature change during actuation and the
respectively. These values are at the same level of photothermal volume shrinking may synergistically increase the bending
bimorph actuators based on polymer or polymer composites amplitude of the actuator. Below we investigated the bending

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curvature, temperature change, and long-term stability of the The thickness of the acrylic layer has a great influence on the
trilayered actuator with those of the equivalent bilayered actu- actuation performance. When the thickness of the acrylic layer
ator without a cooling layer, in order to investigate the function is 7 µm, the bending curvature is about 8.2 cm−1. However,
of the acrylic layer. too thick acrylic layer (15 µm) deteriorates the bending ampli-
The temperature change and bending curvature of the IPAT-2 tude possibly due to the decrease in actuation temperature
actuator are +9.9 °C and 7.6 cm−1 under 150 mW cm−2 NIR change, which is consistent with the theoretical simulations
irradiation, which is 0.5 and 1.43 times as those of the IPAT-0 (Figure S16, Supporting Information).
actuator, respectively (Figure 2b). This verifies the cooling effect
and synergistic volume shrinking effect of the acrylic layer. The
relatively low actuation temperature change resulting from the 2.2.2. White-Light and Blue-Light Photothermal Actuation
acrylic layer also improves the cycling stability of the IPAT-2
actuator. The IPAT-2 actuator exhibited excellent and steady cur- The IPAT-2 actuator can also generate bending actuation in the
vature performance over 100 cycles under 150 mW cm−2 NIR sunlight without any optical focusing system. To better inves-
light, whereas the IPAT-0 actuator showed obvious degrada- tigate sunlight-induced actuation of the actuator, white light
tion in its curvature after only ≈50 actuation cycles (Figure S8, here is used for simulated sunlight. Moreover, actuation under
Supporting Information). high-energy short-wave light, such as blue light, is investigated,
To further investigate the influence of the acrylic layer for which is often applied for lighting and precise control due to
the IPAT actuators. We measured the actuation performance of strong focusing.[24] By considering the absorption over a wide
the IPAT-2 and IPAT-0 actuators under different RH (Figure S9, spectrum for the ink layer in the IPAT film, we studied the
Supporting Information). It can be observed that varying actuation performance of IPAT actuators under white and blue
humidity conditions have little effect on the actuation perfor- light, respectively.
mance (temperature difference, speed, and amplitude) of the The IPAT-2 actuator bent under white light (400−600 nm)
IPAT-0 actuator. For the IPAT-2 actuator, the curvature and actu- with a more tightly focused illumination spot (6.0 mm)
ation speed decreased slightly accompanied by a small increase (Figure 3a). It reaches a maximum bending angle of 142° within
of temperature change with increase in humidity. This may be 0.20 s at a bending speed of 725°s−1 under 30 mW cm−2
due to the fact that water evaporation from the IPAT-2 actuator (0.3 sun) white-light irradiation, with temperature change of
became slow at relatively high RH, and resulted in the decrease +4.9  °C (Figure 3c). The actuation performance is superior to
in volume shrinkage. the IPAT-0 actuator (Figure S17, Supporting Information). The
response time (0.20 s), and temperature-change-normalized
Theoretical Analysis: The bending actuation of an IPAT-0 bending angle (29 °C−1) and speed (148° s−1  °C−1) are at the
actuator is induced by the mismatch in CTE between the same level of high performance, fast white-light driven actua-
different layers upon heating due to light irradiation, while tors based on polymer or polymer composites (in Table S3,
the thermal contraction of the acrylic layer due to the water Supporting Information).[5a,7,13a,25] However, the response time
loss upon heating synergistically enhances the actuation per- is larger than the reported VO2/metallic CNT (2.0 ms)[19a] and
formance of the IPAT-2 film. In order to quantitatively study VO2/CNT (3.3 ms).[19b] An interesting oscillation behavior
the mechanism of volume shrinking of the acrylic layer on the is observed under white light illumination due to the self-
bending actuation, we carried out theoretical analysis on trilay- shadowing effect of the IPAT-2 film (inset of Figure 3c).[26] A
ered and bilayered actuators. cycling test showed that no obvious degradation was observed
First, a transient heat transfer analysis was conducted to for 10 000 cycles under 30 mW cm−2 white-light (Figure 3c).
quantify the temperature change of the IPAT actuator as a Larger bending angle can be obtained by impinging the position
function of the light intensity and exposure time (Note S1 further from the free end (Figure S18, Supporting Information)
and Table S2, Supporting Information). Figure S10 in the and by increasing the light intensity (Figure S19, Supporting
Supporting Information shows that the theoretical calculations Information). Fast periodic actuation can be generated under
are almost consistent with the experimental measurement for square-wave light illumination and the bending angle decreased
IPAT-2 and IPAT-0 films when they are fixed and free to bend. with increasing actuation frequency (Figure 3e).
Thus, the established analytical formulation is suitable for Although few successful reports about photothermal
calculating the thermal response of the IPAT actuators. Both the actuation under blue light have been published,[27] there
theoretical and numerical solutions show good agreement with have no efforts to decrease the temperature change used for
the experimental data (Figure 2c and Figures S11−S15 in the actuation. We now present the investigation of photothermal
Supporting Information). Then a thermomechanical analysis actuation of IPAT-2 under blue-light illumination (Figure 3b).
of bending curvature as a function of temperature change The actuation behavior of an IPAT-2 actuator was studied
for IPAT-2 and IPAT-0 actuators was conducted using the under 30 mW cm−2 blue-light illumination at a wavelength of
classical beam theory (Figure 2d and Note S2, Supporting 450 nm and spot size of 4.0 mm. The IPAT-2 actuator achieved
Information).[22,23] By combining the above photothermal and a maximum bending angle of 124° within 0.24 s at a bending
thermal-mechanical analysis by the classical beam theory, the speed of 625° s−1, with a temperature change of 12.8 °C (from
effect of light intensity on the maximum curvature of the IPAT-2 25.0 to 37.8 °C) (Figure 3d). The bending angle decreased with
actuator was investigated. The calculated results agree well with increasing the actuation frequency (Figure 3e) and increased
the experimental observations, and the maximum curvature is with increasing blue-light intensity (Figure S20, Supporting
almost linearly proportional to the light intensity (Figure 2e). Information). To elucidate the generality of acrylic layer on the

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actuation performance, the actuation behavior of the IPAT-2 shrinking induced by water evaporation under NIR irradiation
actuators driven by blue light are also compared with IPAT-0, as and thus increased actuation amplitude of the IPAT-2 film.
shown in Figure S21 in the Supporting Information. Similar
to the white light actuation, the IPAT-2 actuator showed larger
bending angle, faster actuation speed, and smaller temperature 2.3. Applications of IPAT Actuators
increment than those of the IPAT-0 actuator under white and
blue light. The response time and temperature change of the 2.3.1. Photothermal Frequency Switch
IPAT-2 actuator under white and blue light are at the same level
of high performance, fast photothermal actuators based on Different from the simple on/off switch, frequency switch can
polymer or polymer composites shown in Figure 3f. be used to switch on or off the circuit in the particular fre-
quency, which shows potential applications in communication
system. We demonstrate here a photothermal actuator-based
2.2.3. Helically Coiled IPAT Actuators frequency switch by taking advantage of the fast response speed
of the actuator.
In plants, there are many helically coiled movements, including A diffuse-reflective photoelectric-switch sensor, which is
the helical motion of tendrils and twisting of wood cells.[28] normally in the open state and generally used to control the
Helical actuators have been created by shaping the film to a on/off status of the electrical circuit, is adopted to construct
helical coil and exhibit promising applications in robots and the frequency switch. An IPAT-2 film was mounted on the
artificial muscles.[29] It is critical to further enhance the actua- side of the sensor, and it would cover the sensing part of the
tion performance of helical actuators for practical applications, sensor with NIR light irradiating on the film (Figure S29,
such as high rotation angle, fast response, and symmetrical Supporting Information). The light emitted by the transmitter
reversibility. By considering the fast actuation of IPAT-2 actuator of the photoelectric sensor was then reflected by the IPAT-2
at a relatively low temperature change, here we prepared IPAT- actuator and received by the photoelectric sensor. In this way,
based helical actuators (Figure S22, Supporting Information) a light-emitting diode (LED) could be lit on within 0.26 s and
and studied their rotation angle and speed as well as the tem- lit off within 0.14 s with NIR switched on and off, respec-
perature change as a function of time under NIR illumination. tively (Movie S1, Supporting Information). This switch can be
The IPAT-2 helical actuator with 1 mm coil diameter reached operated at a frequency up to 3 Hz by periodically switching on
a plateau of 288° cm−1 within 0.36 s with a temperature change and off the NIR light. It may be applied for sending frequency
of 17 °C when 150 mW cm−2 NIR light was switched on and signals for transmission, communication, and control by using
returned to the initial state within 0.72 s when the NIR light light. As currently the frequency is still low compared to other
was switched off (Figure S23, Supporting Information). Our approaches, further improving the frequency is possible by
IPAT-2 actuator shows faster response compared to other means of downsizing the actuator to micrometer to nanometer
helically coiled actuators.[24,30] The maximum rotation speed scale and increasing the modulus of the film.
was ≈150 r.p.m., and there was no significant degradation after
100 cycles (Figure S24, Supporting Information). The rotation
angle increased with a smaller coil diameter and a higher light 2.3.2. Mechanical Gripper
intensity (Figures S25 and S26, Supporting Information). As a
comparison, the IPAT-0 coil exhibited a smaller rotation angle Mechanical grippers are widely used in robotic systems for
(280° cm−1) and a slower response time (0.84 s) compared to grasping and lifting objects using mechanically actuated fin-
the IPAT-2 actuator, indicating the volume shrinking of the gers, and flexible actuators are preferred to enable such fingers
acrylic layer (Figure S27, Supporting Information). to handle objects of different shapes. The currently reported
mechanical grippers are limited by the small weight-lifting ratio
due to the limited interaction force between the fingers and the
2.2.4. Light-Induced Actuating Stress Generation object as well as the slow response time. Our IPAT-2 actuator
is a good candidate for use in a mechanical gripper due to the
The light-induced actuating stress of the IPAT-2 and IPAT-0 large bending amplitude and fast response time under light
actuators under NIR illumination with different light inten- irradiation and the fact that the acrylic layer of the IPAT-2 film
sities was measured by using an Instron mechanical tester can provide a strong adhesive force when holding an object.
(Figure S28, Supporting Information). Both ends of the film The strong mechanical properties of the IPAT-2 actuator played
(50 mm in length and 5 mm in width) were fastened to the a certain role in holding the load without broken when it was
machine in uniaxial testing mode, and ≈0.5 N force was applied gripped on the film via the acrylic layer. Here, we demonstrated
to keep it taut. The NIR illumination time is about ≈0.2 s. The an IPAT-based mechanical gripper that can grasp objects made
actuating stress induced in the actuator mainly originated from of different materials, including metal balls and polymer foams,
the expansion of the ink layer. It can be observed that the actu- under NIR irradiation (Figure 4a).
ating stress increased with increase of power density, which An IPAT-based gripper consisting of two IPAT-2 actuators
might be attributed to the large expansion of the ink layer. The (0.17 mg for the two actuators) was shown to be able to grasp
actuating stress of the IPAT-2 actuator is higher than that of and lift a copper ball of 0.3642 g within 0.37 s under NIR irra-
IPAT-0 actuator, which should be ascribed to the contribution diation of 150 mW cm−2 and quickly released it within 0.13 s
from the acrylic layer. The acrylic layer can generate volume by switching off the light (Figure 4b). This corresponds to a

Adv. Funct. Mater. 2019, 1808995 1808995  (7 of 11) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com www.afm-journal.de

Figure 4.  Mechanical gripper made from the IPAT-2 actuators used to grasp and release an object under NIR irradiation. a) Schematic illustration and
b,c) photographs of the gripper for grabbing a copper ball and a polymer foam. d) Comparison of weight-lifting ratio and response time of actuators.
WS2/SA: Reproduced with permission.[8] Copyright 2017, Wiley-VCH. GO-PDA-rGO: Reproduced with permission.[16] Copyright 2015, Science. CNT-paper/
BOPP: Reproduced with permission.[20] Copyright 2018, Royal Society of Chemistry. sG/PDMS: Reproduced with permission.[31a] Copyright 2014, Royal
Society of Chemistry. PVDF/single-walled carbon nanotube (SWCNT): Reproduced with permission.[31b] Copyright 2016, Wiley-VCH. Pentaerythritol
ethoxylate (PEE)/polypyrrole (PPy): Reproduced with permission.[31c] Copyright 2013, Science. Cellulose nanocrystal (CNC)/phenol-formaldehyde (PF):
Reproduced with permission.[31d] Copyright 2014, Wiley-VCH. poly(N-isopropyl acrylamide)/PPy: Reproduced with permission.[31e] Copyright 2015,
Wiley-VCH. SA/PNIPAM: Reproduced with permission.[31f ] Copyright 2015, American Chemical Society.

weight-lifting ratio of 2142 (m/m0, where m0 is the mass of the exploring new interaction force between the fingers and the
IPAT actuators and m is the mass of the lifted object). This object such as magnetism, and increasing the response speed.
ratio is higher than the previous record weight-lifting ratio of
500 achieved by a sodium alginate/WS2 actuator.[8] The response
time is also shorter than the record response time (2 s) offered 2.3.3. Soft Crawling Robot
by a graphene sponge/PDMS actuator (Figure 4d).[31] The IPAT-
based gripper could also be made to grasp and release a polymer Soft robots that can harvest light are preferred because they can
foam by using NIR light (Figure 4c and Movie S2, Supporting be controlled remotely and enable miniaturization by elimi-
Information). To investigate the effect of the mechanical prop- nating the need for external batteries. A light-driven bimorph
erties of the actuator film to the gripper performance, we actuator is a good candidate for such a robot because it can
prepared a mechanical gripper using IPAT-0 actuators, which mimic locomotion as found in nature. However, the relatively
can pick up the polymer foam under irradiation of NIR light. low speed of such actuators has limited the development of
This indicates that the mechanical properties of the actuator such crawling robots. Considering that our IPAT-2 actua-
also play an important role for mechanical grippers, as reported tors provide a fast bending speed under a low light intensity,
by Li’s group.[8] With its outstanding weight-lifting ratio, fast we reasoned that it should be possible to develop a crawling
response, remote controllability, and the ability to manipulate robot based on IPAT-2 actuator that can crawl forward on a flat
different materials, this smart gripper could be used in diverse substrate driven by white light.
applications in robotic systems. For practical applications, A bow-shaped IPAT-2 actuator was prepared by attaching ten
the selectivity and adhesion of the acrylic layer to different mate- layers of forest-drawn, super-aligned carbon nanotube (SACNT)
rials need to be tailored and investigated. Based on the reported sheets on the adhesive layer of an IPAT-2 film (7 mm × 2 cm)
fast response actuator, such as VO2/CNT (3.3 ms)[19b] and for reducing the adhesion.[32] When the front leg of the bow-
VO2/metallic CNT (2 ms),[19a] a mechanical gripper with fast shaped IPAT actuator was illuminated (30 mW cm−2), the robot
response speed would be developed. Future work on improving became almost flat, the frictional force on the front leg (F2)
the properties of the mechanical gripper would be increasing diminished, and the front leg moved forward (Figure 5a). Upon
the mechanical properties of the actuator in holding the object, removal of the light, the IPAT-2 actuator bent and recovered its

Adv. Funct. Mater. 2019, 1808995 1808995  (8 of 11) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com www.afm-journal.de

Figure 5.  Demonstration of applications of an IPAT actuator as a soft walking robot and a light mill. a) Schematic illustration of the force analysis
during the light-driven actuation of a locomotive bimorph actuator. b) Photographs showing a walking robot crawling forward on a flat substrate with
white light sequentially switched on and off. The red dashed lines represent the starting position of the left edge of the robot, and the yellow and blue
dashed lines represent the final position of the left edge of the robot. c,d) Schematic illustration of a light mill driven by a wing-flapping mechanism.
e) The relationship between the actuator shape and the maximum rotational speed of the light-driven mill under NIR irradiation.

original shape. The front leg touched the surface at an angle and high cost, it will be highly favored that the blade can be
closer to perpendicular, so that the “foot” was relatively flat on made by general polymer materials. The rapid motion of the
the surface. In contrast, the rear leg lay at a more acute angle, blades plays a vital role in obtaining the continuous rotatory
reducing the surface contact of the rear “foot” relative to the front motion of the mill, which might be related to the low energy
one. Thus, the frictional force on the front leg (F2′) was larger density of light compared to the weight of the mill, inefficient
than that on the rear leg (F1′), and the rear leg moved forward transformation of light-to-kinetic energy, and the air resistance.
(Movie S3, Supporting Information). By sequentially switching Inspired by the fast response and large bending amplitude of
on and off the white light at a frequency of ≈0.4 Hz, the crawling the IPAT-2 film under small temperature change, we demon-
robot could be driven to move forward at an average speed of strated a light mill by means of light-induced aerodynamic
≈ 26 mm s−1 (Figure 5b), which is ≈1.6 times the current record propulsion based on a wing-flapping mechanism (Figure 5c,d).
value of 16 mm s−1 reported for an rGO-CNT/PDMS crawler-type Upon irradiation with periodic pulses of NIR light, the IPAT
robot driven by light,[7] and other thermally induced crawling actuators sequentially bent and unbent, thereby generating fast
robots.[33] However, the speed is lower than the soft robots based air flow under the actuators and providing thrust to drive the
on a rolling mechanism such as polycarbonate (PC)/CNTs motor rotation of the light mill (Movie S4, Supporting Information).
(60 mm s−1)[13a] and polydopamine modified reduced graphene Figure 5e shows the relationship between the shape of the
oxide-carbon nanotube layer/polyvinylidene fluoride (PDG-CNT/ IPAT-2 actuators and the maximum rotational speed of the light
PVDF (100 mm s−1).[34] This robot can continuously cover a dis- mill. The results indicate that square-shaped IPAT-2 actuators
tance of up to 5 cm in our experiment. This soft robot may find generated the fastest rotational speed of the light mill among
applications for crawling to a specific place for searching and all of the tested actuator shapes, including circles, triangles,
take actions by combining with other modules such as sensors, rectangles, and hexagons. This finding mimics the character-
antenna, and other devices. Future work may focus on improving istics of flying birds, such as peregrine falcons and ducks,
the capacities such as carrying load and multifunctionality. who typically use short wings to generate overall fast speed.
A light-driven mill with a cantilever length of 3.0 cm and
square-shaped IPAT-2 actuators could generate an average
2.3.4. Light-Driven Mill Based on a Wing-Flapping IPAT Actuator rotational speed of 19 r.p.m. under periodic pulses of
150 mW cm−2 NIR light with on and off time of 0.30 and 0.28 s,
A mill is a device that converts external energy including respectively, and the corresponding specific work capacity was
wind, water, and light energy into rotational energy by means 7.5  × 10−3 J kg−1. The flapping frequency can reach 0.2 Hz,
of blades.[9] With the only successful trial for light mill using which is lower than the liquid crystal network actuator (1 Hz).[9]
liquid crystal polymers, the investigation about the light mill is The relatively low rotational speed might be related to the large
largely unexplored. However, due to the complicated synthesis weight ratio of actuator to the whole device (1:13) compared

Adv. Funct. Mater. 2019, 1808995 1808995  (9 of 11) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com www.afm-journal.de

to the literature (1:1), which may be improved by increase the of a Teflon rod (4.0 mm diameter and 35 mm long) via the adhesive
weight fraction of the actuators in the future investigations. force of the acrylic layer to the Teflon rod. The lengthwise direction of the
This rotational motion can sustain as long as the light pulse IPAT-2 films were placed parallel to the diameter direction of the Teflon
rod, and part of the length (2 mm) of each IPAT-2 film was attached to
is provided during our experimental time period. This light- the Teflon rod. To achieve a suitable adhesion force for capturing and
induced aerodynamic propulsion design based on a wing- releasing different objects, talcum powder (325 mesh) was casted on the
flapping mechanism may also be used in driving motors, or acrylic layer.
even used in morphing aircraft and other automated systems, The bow-shaped IPAT-2 robot was designed by attaching ten layers
by suitable aerodynamic design. of forest-drawn SACNT sheets on its acrylic side of the film (7 mm
long and 2 mm wide) to reduce its adhesion, and wrapped around a
4 mm diameter stainless-steel rod with the SACNT side on the outside,
and then annealed at 100 °C for 1 h to set the shape.
3. Conclusion The light mill was composed of two-part structure, with the top part
having six arms connected to a small hemispherical glass cap, which
In conclusion, we designed an innovative photothermal trilay- was placed on top of a vertically oriented needle. An IPAT-2 film was
ered bimorph actuator with an in-built layer for cooling and syn- mounted at the end of each individual arm.
ergistic volume shrinking via water evaporation upon heating. Characterizations: The thickness of the individual layer of the IPAT film
was measured from cross-sectional images acquired using a scanning
We achieved shorter response time, larger actuation amplitude,
electron microscope (ZEISS, MERLIN Compact, Germany). The
and faster actuation speed at a smaller temperature change, optical absorption spectrum was obtained by UV/vis/IR spectrometer
compared to the equivalent bilayered actuator without the (PerkinEelmer, Lambda 950). FTIR spectroscopy of the acrylic layer
cooling layer, under broad spectrum including NIR, white, and was performed on a spectrometer (Bruker, TENSOR 37, Germany).
blue light. We successfully showed the demonstration of a light The CTE was measured using a dilatometer (NETZSCH, DIL 402SE,
mill via a wing-flapping mechanism and a photothermal fre- Germany). The mechanical properties of the film were obtained using
quency switch as well as a fast-soft robot and a strong mechan- an Instron mechanical tester (Model 3365, China). An IR camera (FLIR
T440, American) was used to measure the temperature of the IPAT-2
ical gripper. On the basis of our approach, we recommend the and IPAT-0 actuators. The bending amplitude and response time of the
application of this trilayered concept in various actuator-related IPAT-2 and IPAT-0 actuators were measured from digital images (Adobe
devices from smart control to artificial intelligence. As the cur- Preclude CC 2015) captured by a video camera (Nikon, D5300, Japan).
rent design uses thin polymer film for fast heat transfer and The light intensity was measured using a solar power meter (LH-122,
thus shows weak mechanical properties, future work may be China) and an IR power meter (LH-129, China). Ambient temperature
carried out to improve the mechanical strength by use of inor- and RH were measured using a hygrometer (DT-615, China).
ganic materials, such as metals, semiconductors, or composites.

Supporting Information
4. Experimental Section Supporting Information is available from the Wiley Online Library or
from the author.
Preparation of IPAT and Helically Coiled Actuators: The IPAT-0 actuator
was fabricated by coating the commercially available shading ink (TJ-1830,
Tengjing Electronic Materials Co. Ltd, Shenzhen, China.) on the PET film
(Jiufanghe Co. Ltd, China, 1.6 µm) to form an ink layer (1.2 µm) by spin Acknowledgements
coating (3000 r min−1). The ink is composed of carbon black (3−5%),
polyurethane (30%) in the mixture solvents of ethyl acetate and acetone This work was supported by the National Key Research and
(20%/80%) provided by the supplier. In detail, first the PET film was Development Program of China2017YFB0307000, the National Natural
attached on the glass side by double-side tape. A certain amount of ink Science Foundation of China (grants U1533122 and 51773094), the
slurry was dropped on the PET film to form a uniform ink layer by spin Natural Science Foundation of Tianjin (Grant No. 18JCZDJC36800),
coating and then an IPAT-0 film was obtained by drying the film naturally. the Science Foundation for Distinguished Young Scholars of Tianjin
Similarly, the IPAT-x (x > 0) actuator was prepared by coating commercially (Grant No. 18JCJQJC46600), the Fundamental Research Funds
available waterborne acrylic adhesive (Hexiang Co. Ltd, China) on the PET for the Central Universities63171219, the Science and Technology
side of the IPAT-0 film to form an acrylic layer with different thickness by Support Program of ChangzhouCZ20170007, State Key Laboratory
spin coating (Figure S1, Supporting Information), the thickness can be for Modification of Chemical Fibers and Polymer Materials, Donghua
controlled by using different spin coating speed. Helically coiled actuators UniversityLK1704, and Eugene McDermott Graduate Fellows Program.
were prepared by wrapping the IPAT films having 5 cm length and 2 mm
width, with the ink layer inside around steel rods of different diameters
(1.0, 2.0, 4.0, and 6.0 mm) with a helical angle of +45° (left handedness)
or −45° (right handedness). Both ends of the film were fixed by polyimide Conflict of Interest
tape and then annealed in an oven at 120 °C for 4 h to set the shape. The authors declare no conflict of interest.
Fabrication of the Frequency Switch, Smart gripper, Walking Robot, and
Light Mill: The frequency switch was fabricated by taping the IPAT-2
film (10 mm long and 1 mm wide) vertically on the side of the diffuse-
reflective photoelectric sensor (model M6, Xiangming Inc, China) to Keywords
control an LED light. The light emitted from the transmitter was reflected
and received by the photoelectric sensor, and the electrical circuit was bending actuation, light mills, photothermal, soft robots, torsional actuation
connected. The frequency control of the LED was achieved by changing
the actuation frequency of the IPAT-2 actuator under NIR irradiation. Received: December 18, 2018
A smart gripper was produced by attaching two identical IPAT-2 films Revised: March 5, 2019
(12 mm long and 2 mm wide) to the opposite sides of the bottom end Published online:

Adv. Funct. Mater. 2019, 1808995 1808995  (10 of 11) © 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
www.advancedsciencenews.com www.afm-journal.de

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