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Bifurcation-based embodied logic and autonomous

actuation
Yijie Jiang1, Lucia M. Korpas1 & Jordan R. Raney1

Many plants autonomously change morphology and function in response to environmental

stimuli or sequences of stimuli. In contrast with the electronically-integrated sensors,
1234567890():,;

actuators, and microprocessors in traditional mechatronic systems, natural systems embody

these sensing, actuation, and control functions within their compositional and structural
features. Inspired by nature, we embody logic in autonomous systems to enable them to
respond to multiple stimuli. Using 3D printable fibrous composites, we fabricate structures
with geometries near bifurcation points associated with a transition between bistability and
monostability. When suitable stimuli are present, the materials swell anisotropically. This
forces a key geometric parameter to pass through a bifurcation, triggering rapid and large-
amplitude self-actuation. The actuation time can be programmed by varying structural
parameters (from 0.6 to 108 s for millimeter-scale structures). We demonstrate this bioin-
spired control strategy with examples that respond to their environment according to their
embodied logic, without electronics, external control, or tethering.

1 Department of Mechanical Engineering and Applied Mechanics, 220 S 33rd St., University of Pennsylvania, Philadelphia, PA 19104, USA. Correspondence
and requests for materials should be addressed to J.R.R. (email: raney@[Link])

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R
esponsiveness to environmental stimuli is vital to the times (and in sequences of defined actuation events). We
function and growth of plant life1–6. Natural morphological accomplish this by 3D printing self-actuating units consisting of
changes can take hours (e.g., for dispersal of seeds or laterally-constrained fibrous composite beams. We design the
environmental adaptation3–5) or less than a second (e.g., the beams to possess geometries near bifurcation points that govern
closing of the Venus flytrap, Dionaea muscipula, to capture their stability behavior. The beams swell anisotropically in the
prey6,7). These can also require multiple stimuli or a specific presence of suitable stimuli, causing a key geometric parameter
sequence of stimuli. For example, underlying the motion of the to move through a bifurcation point. This triggers rapid and
Venus flytrap is a complex sequence of sensing and actuation large-amplitude actuation at pre-defined times and in response
events. Hairs on the leaf lobes must be mechanically stimulated to multiple stimuli. Specifically, we use polydimethylsiloxane
multiple times within 20–30 s for the lobes to close. After partially (PDMS)-based and hydrogel-based materials to respond to non-
closing, the plant reassesses the size of any enclosed object and polar solvents and water, respectively.
awaits continued stimulation to determine whether to open (to
release the object) or to close the rest of the way (to begin
digestion)7,8. In traditional mechatronic systems, sensing, actua- Results
tion, and control are performed electronically. Complex natural General concept. Laterally-constrained beams, depending on
logic, however, is embodied in plants more directly through the their geometric parameters and boundary conditions, can exhibit
tools nature has at its disposal: stimuli-induced morphological very different mechanical responses, including cantilever-like
changes via material composition and the structural (geometric) bending, snap-through instabilities53, and bistability51,52,59. Each
organization. Recent work in soft robotics has shown the feasi- of these behaviors correspond to specific domains in a parameter
bility of embedding control logic in the structure of the robot space defined by beam geometry. For laterally-confined, tilted
itself (i.e., microfluid logic)9, opening the door for further nature- beams, these key geometric parameters are the inclination angle
inspired control systems, as we explore here. of the beam (θ) and its slenderness ratio (w/L, where w denotes
The ability of a material to adapt to its environment via the beam width and L denotes the beam length) (Fig. 1a). We
response to specific stimuli is of interest for numerous applica- used finite element simulations (discussed in detail later) to
tions, from robotics10–12 to medicine (e.g., drug delivery13,14). obtain the bistable and monostable energy curves in Fig. 1b
Synthetic active materials have been developed that actuate in (curves I and III, respectively), both with θ = 45o but with dif-
response to a variety of stimuli15–23, including chemical cues24, ferent w/L ratios (corresponding to points I and III in Fig. 1c). A
temperature10,11,25–31, light12,32–36, voltage37–39, and water40–42. bistable mechanical response is defined by a dual-well potential
Each of these stimuli-responsive materials has its own set of (Fig. 1b), with each well representing a stable morphology that
strengths as well as practical challenges that need to be addressed can be maintained without any applied force or continued input
for its use in autonomous applications. For example, thermally- of energy51,52. The two stable configurations are separated by an
activated shape changes, such as those associated with shape- energy barrier that, if traversed, produces an instability and a
memory polymers11,25,27,43,44, often require mechanical pro- rapid snap-through from one stable configuration to the other.
gramming and/or large thermal energy transfer to/from the The two stable wells are not at the same energy level because in
environment. Light- or voltage-responsive materials often require one configuration the beam is unstrained, and in the other it is
a stimulus of significantly larger magnitude than may be buckled (associated with strain energy). The size of the energy
encountered in the ambient environment (e.g., high illumination barrier, i.e., the depth of the second well (Eout in Fig. 1b), can be
intensity33,45 or high voltage37,38). Actuation via differential controlled by the geometry of the beams51,56,59. For a fixed θ, as
swelling (e.g., using bilayers42,46,47 or anisotropic composite w/L increases (i.e., as the beam becomes wider relative to its
materials40) requires diffusion of stimuli (e.g., solvents), which, length) the energy barrier decreases, reaching a value of zero at a
depending on sample volume and geometry, can take many specific value of w/L that defines a bifurcation point, B (at point II
minutes due to the intrinsic limits of the speed of diffusion40,41. in Supplementary Figure 1). For values of w/L larger than B, the
Moreover, in these examples, the material strain that is induced is beam is monostable, meaning it will return to its undeformed
a monotonic function of the amount of stimulus that is present, position (u = 0) if the applied force is removed. The critical value
rather than a discrete, sudden morphological change. of w/L = B changes as a function of θ, as represented by the
The active materials above achieve their responsiveness via orange line dividing bistable from monostable regions in Fig. 1c.
composition and microstructure, i.e., via the functionality Because of this sharp critical value, only a small nudge to the
intrinsic to the specific polymer matrix or (if a composite) to geometric parameters (e.g., via active materials) is necessary to
microstructural features, such as fiber alignment. However, the cross a bifurcation point and trigger rapid snap-through for the
geometric arrangement of the material is also vital to the overall purpose of actuation or movement. To accomplish this, we
actuation response. Natural systems like plants possess the same fabricate the beams using highly anisotropic composite materials,
speed limits associated with diffusion that synthetic materials do1. causing anisotropic swelling of the beams upon exposure to
When faster responses are required, however, plants increase the material-specific cues (e.g., water or non-polar solvents in our
rate of actuation using geometrically defined instabilities6, a initial work). As shown in Fig. 1b and c, for a beam fabricated
nonlinear mechanical phenomenon studied extensively48–50 in with geometry corresponding to point I (w/L < B) and placed in
structures, such as beams51–57 and shells29,46,58. Snap-through its buckled configuration, if it were to anisotropically swell to
instabilities are associated with rapid morphological changes. point III (w/L > B) it would have to pass through the bifurcation
These have been used in previous work to enhance the speed of point at point II (w/L=B=0.105), above which the beam is only
actuation in soft materials, including in response to diffusion. stable in its unbuckled configuration (u = 0). This forces a rapid
Examples include diffusion-induced actuation via doubly curved actuation event, rapidly releasing the strain energy from the beam
beams and multilayer shells with stiffness gradients46,57,58, and as it ceases to be bistable. Supplementary Movie 1 shows such an
structures composed of layers with orthogonal microstructure29. actuation event, recorded using a high-speed camera during
In this work, we combine anisotropic materials with bistable bifurcation (in this case, PDMS-glass fiber composite beams
structures to embody logic (AND, OR, and NAND) in 3D responding to toluene). The images in Fig. 1c demonstrate the
printable composite structures. These structures can be pro- rapid actuation (τ < 0.01 s) that occurs for any beam that traverses
grammed to respond to multiple stimuli and to actuate at specific such a bifurcation point. τ represents the amount of time it takes

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a b d
0.15 Bistable
L Monostable
Logic 1

Energy, E/C10wLd
w u module
Unstable Stable
 0.1 (max.) (min.) 0
Ι
Output
Eout
0.05
ΙΙΙ Input
Ein

AND
Stable 0.5 1 PDMS
u/Lsinθ
c 55
Bistability Monostability
θ (degrees)

50 Anisotropic Hydrogel
beam swelling
OR
Hydrogel
45
Ι ΙΙ ΙΙΙ

40
0.09 0.10 0.11 0.12 0.13
PDMS
w/L
NAND
1 + 1 0
t < t* 1 cm t = t* t > t* (Toluene applied) (Toluene applied) (Unit closes)

Ι: Bistable ΙΙ: Bifurcation (τ< 0.01 s) ΙΙΙ: Monostable

Fig. 1 Overview of bifurcation-based actuation. a Schematic and photo of beams, with key geometric parameters and boundary conditions. b The
normalized strain energy, E/(C10wLd), where C10 is a material parameter in the Holzapfel–Gasser–Ogden (HGO) model65 and d is the out-of-plane
thickness of the beam; plots are included for a bistable beam (red curve, I) and a monostable beam (black curve, III) as a function of normalized
displacement, u/Lsinθ, obtained via finite element simulations (Supplementary Note 5). Inset: photos of the undeformed (u = 0) and buckled
configurations, corresponding to the two stable points (energy minima) on the bistable curve; the monostable curve has only the single minimum at u = 0.
c Geometric phase diagram mapping geometric parameters to mechanical behavior, with schematic overlay indicating the transition from bistable to
monostable (point I to point III) due to anisotropic swelling of the beams. Also shown are representative images recorded with a high-speed camera during
actuation showing a unit when it is bistable (red), at the point of bifurcation when actuation occurs (green), and monostable (black). d A logic module
which can act as one of several types of logic gates depending on the contents of the module. An AND gate can be constructed by using a hydrogel valve
and a PDMS-GF15 bistable unit (requiring both water and toluene to switch from 0 to 1). An OR gate can be constructed by fabricating a composite bistable
unit from both PDMS-GF5 (blue) and hydrogel (transparent) materials (this actuates if either water or toluene is applied); a functionally-complete NAND
gate can be constructed by connecting two “input” bistable units to one “output” unit. In this case, only when toluene is applied to both input units will the
output unit close from 1 to 0 (i.e., 1+1→0)

for the actuation event (the release of the stored strain energy) approach allows the “embodiment” of complex control in this
once bifurcation is reached (as observed with a high-speed material-structure combination.
camera). Note, the value of w/L would remain unchanged during In Fig. 1d, we demonstrate modular embodied logic, in which a
swelling of an isotropic beam, and thus the bifurcation point mechanical logic module can produce AND, OR, or NAND
would not be reached horizontally. (Depending on the specific output in response to chemical inputs, depending on which
architecture, isotropic swelling could still lead to the crossing of a structures are placed inside the module. We produce an AND
bifurcation point via an increase in θ. However, since the gate by using a hydrogel valve and a PDMS-GF15 bistable unit
monostable/bistable boundary is nearly vertical, it would typically inside (Supplementary Figure 2). The actuation of this inner
require a larger degree of material swelling to do so.) bistable unit flips the output of the module from 0 to 1. However,
Supplementary Movies 1–3 demonstrate the feasibility of using to achieve this, water must be present (to make the hydrogel swell
changes to the environment to trigger snap-through and buckle, opening the valve) as well as toluene (to trigger the
instabilities35,44,46,60, as also observed in nature1. For example, actuation of the unit). We produce an OR gate by constructing a
Supplementary Movie 3 shows a hopper that autonomously bistable unit with out-of-plane arrangements of both PDMS-GF5
jumps out of the way when an undesired chemical (in this case, (blue) and hydrogel (transparent) materials. This bistable unit can
toluene) enters its environment. We note that this behavior actuate when either water or toluene is applied (Supplementary
occurs without discrete sensors, tethering, or mechatronic Movie 4). Finally, we produce a NAND gate by connecting two
actuators: the system’s combination of composition and structure units (corresponding to two inputs) and one output. The stiffness
is itself the sensor, control system, and actuator. By harnessing of these is tuned (via geometry) such that both inputs must
systems of 3D printable bistable, anisotropic beam units (each of actuate in order to close the output unit (i.e., 1+1→0). Otherwise,
which can be independently assigned its own choice of actuation the output unit remains open (Supplementary Movie 5). Since
timing and its own stimulus, as described later), our bioinspired NAND is a functionally complete logic gate, in principle any

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gated logic could be achieved via combinations of these. To chain criteria above, but requires some rheological tuning of the
the logic gates into more complex systems, the mechanical materials to allow printing (Fig. 2b–d and Supplementary
response from one gate (the output) could be used either to Figure 3). In this work, we make use of two materials that
indicate when to perform a manual pour, or to automatically respond to two distinct stimuli: a PDMS-based material (contain-
open a chamber to allow fluid movement to the next gate (e.g., ing short glass fibers to provide anisotropy), which swells in the
the input solvents for the NAND gate could be either manually presence of non-polar solvents, such as toluene or hexane; and a
poured or introduced automatically via suitable channel design). hydrogel-based matrix (containing cellulose fibrils to provide
anisotropy) that swells in the presence of water. Our PDMS ink
Materials and fabrication. In the remainder of this article, we formulation (see Methods) shows the rheological properties
outline how to achieve this behavior, and demonstrate utility via desired for DIW, including a decrease in apparent viscosity
several use cases. with increasing shear rate (Fig. 2b) and a viscoelastic yielding
To achieve the general strategy outlined above, the ideal behavior that is characterized by a high storage modulus (G')
materials would meet the following requirements: First, each when the shear stress is low (allowing the material to maintain its
material must swell in response to a defined stimulus, e.g., water, shape and to behave like an elastic solid) and a defined yield stress
non-polar solvents, temperature, light, etc. (in this work, we above which the storage modulus suddenly drops (allowing
demonstrate the use of the first two of these stimuli, but any flowability through the nozzle) (Fig. 2c). A similar rheological
would work). Second, the materials swell anisotropically to alter profile is observed for the hydrogel material (Supplementary
the key geometric parameter (w/L) when exposed to their stimuli, Figure 3). Because of the alignment of the fibers during extrusion
allowing a well-controlled approach to move through a bifurca- (Fig. 2d), a high degree of mechanical anisotropy can be
tion. Third, the materials should be sufficiently elastic to maintain achieved. We characterize this by printing tensile specimens with
a buckled configuration (maximum material strain of εmax < 0.15) fiber alignment both parallel with (“Longitudinal”) and perpen-
without prohibitive time-dependent relaxation, as it is this stored dicular to (“Transverse”) the loading direction, subsequently
elastic energy that enables the actuation event. Finally, the testing these under quasistatic tension (see Methods) (Fig. 2e).
materials (or material precursors) must be patternable with high Since the glass fibers are much shorter than the beam length, the
structural fidelity, since the mechanical response of the beams is Halpin–Tsai model64 is used, with the best fit corresponding to a
determined by precise values of geometric parameters. matrix stiffness of Em = 2.96 MPa and a fiber stiffness of Ef =
While 3D printers make it relatively easy to achieve sufficient 52.13 GPa (details in Supplementary Note 3). With increasing
structural fidelity of the beams (the fourth point above), most glass fiber volume fraction, the longitudinal stiffness, EL, increases
conventional 3D printers are unable to simultaneously achieve much more than the transverse value, ET (Fig. 2e), as expected for
the other requirements61. Direct ink writing (DIW) is an short fiber composites. With 15 vol% glass fibers, significant
extrusion-based 3D printing technique61,62 which offers a large mechanical anisotropy (EL/ET = 10.8) is obtained while good
degree of materials flexibility, and is ideal for producing printability is maintained. Additional tensile tests on swollen
anisotropic materials (fibers align due to material shear in the samples and stress relaxation tests are shown in Supplementary
nozzle40,63 (Fig. 2a)). This approach allows us to meet all four Figure 4.

a b 105 c 108
Viscosity (Pa•s)

104 106
Moduli (Pa)

103 104

102 102
G′ (Storage modulus)
G″ (Loss modulus)
101 100 2
100 102 10 103 104
Strain rate (1/s) Shear stress (Pa)

d e 60
Longitudinal
Transverse
50 Fit by Halpin-Tsai model
64
Stiffness (MPa)

40

30

20

10
100 μm
0
0 5 10 15
Vol% of glass fibers

Fig. 2 Direct ink writing (DIW) of PDMS-glass fiber composites. a Schematic of extrusion of PDMS ink during DIW 3D printing, leading to alignment of
glass fibers. b, c Rheological characterization of the PDMS-GF ink shows shear-thinning and yield-stress behavior, respectively. d An optical micrograph
showing material printed using PDMS-GF ink (15 vol% glass fibers), with alignment of glass fibers along the print direction. e Stiffness of PDMS-GF
composites (after curing of printed structures) as a function of the volume fraction of glass fibers and the fiber orientation, based on tensile testing of
printed specimens (“Longitudinal” and “Transverse” indicate printing and fiber orientation that is parallel with or perpendicular to the loading direction,
respectively), and fit using the Halpin–Tsai model64

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Mechanical behavior. In prior work on the bistability of laterally- The anisotropy in stiffness imparted by the alignment of the
constrained beams51, the relationship between beam geometry glass fibers produces anisotropic swelling when the material is
(the two key geometric parameters θ and w/L) and the exposed to a suitable solvent (Fig. 4). To characterize this, we
stability behavior (e.g., bistable or monostable) was considered measured L and w of the printed beams during exposure to the
material-independent. However, this conclusion implicitly solvent under an optical microscope. Since PDMS swells strongly
assumed that the material was isotropic. In fact, the degree of in non-polar solvents, we used toluene as the stimulus66. When
material anisotropy is also essential for determining the allowed to become fully saturated by toluene (at time t = ts), the
stability. Using experiments and finite element analysis (FEA), isotropic PDMS matrix (no glass fibers) swells until each linear
we locate the boundary between regions of monostability and dimension has increased by 42%, corresponding to a swelling
bistability in the geometric phase diagram (e.g., Fig. 1c) for the ratio of η = 1.42 (see Fig. 4a and Supplementary Note 6). The
more general case, in which the material anisotropy is allowed mechanical anisotropy produced by aligned fibers (e.g., in PDMS-
to vary. We first fit an anisotropic hyperelastic mechanical GF composites) significantly reduces the swelling ratio in the
model, the Holzapfel–Gasser–Ogden (HGO) model65, to our direction of fiber alignment (longitudinal direction), ηL = Ls/L0.
experimental tensile data for the case of 15 vol% glass fibers The magnitude of this reduction increases as the volume fraction
(Supplementary Figure 5a) and then use this to conduct a para- of the fibers (and concomitantly the degree of anisotropy)
metric study (Fig. 3). The results (Fig. 3a, b) indicate that a beam increases. In contrast, there is only a slight reduction in the
with θ = 45° is bistable if w/L is less than 0.105 (i.e., the second swelling ratio in the direction perpendicular to the fibers (the
energy well exists, and therefore the quantity Eout can be defined transverse swelling ratio, ηT = ws/w0) relative to the isotropic case
and is nonzero), and monostable otherwise (Supplementary (see Fig. 4a), since the fibers do not provide significant
Note 5). This is consistent with our experimentally-determined reinforcement perpendicular to their alignment. The swelling
phase boundary between 0.102 < w/L < 0.108 (Supplementary anisotropy (defined as ηT/ηL) therefore increases with increasing
Note 4). We develop a more complete phase diagram by sys- fiber volume fraction (Fig. 4b). Accordingly, w will increase more
tematically varying θ and w/L and determining the normalized than L upon exposure to a solvent, and the key geometric
energy barrier Eout/(C10wLd) (Fig. 3c), which is very different parameter w/L that defines the nonlinear behavior of the beam
from the isotropic case51. As discussed more in Supplementary can be altered merely by exposing it to a suitable solvent. The
Note 5, the phase boundary depends strongly on the degree of swelling anisotropy (ηT/ηL) also determines the range in
anisotropy (see Fig. 3d and Supplementary Figure 5c, with k1 = 0 parameter space, Δw/L, through which the geometry of a beam
indicating isotropy and increasing k1 indicating increasing ani- is able to move based on such swelling. The choice of the initial
sotropy). For a beam of fixed length, L, the greater the degree of beam geometry w0/L0 at fabrication determines whether this
material anisotropy, the thinner the beam must be to be bistable range is sufficient to bring the beam’s geometry through the
(Supplementary Note 5). bifurcation (i.e., the k1 = 10 phase boundary in Fig. 3d for our 15

a 0.25 b
0.06
0.2 u 0.12
Force, F/C10cosθLd
Energy, E/C10wLd

0.11
0.15 0.105 0.04
0.1
0.095
0.09
0.1
0.08 0.02
0.07
0.05 w/L
0

0
0 0.5 1 1.5 0 0.5 1 1.5
u/Lsinθ u/Lsinθ

c Energy barrier, Eout/C10wLd d 60

k1
0.014
60 10
55
0.012 6
55
3
0.01 50
θ (degrees)

1
50
θ (degrees)

0
0.008 45
45
0.006
40 40
0.004
35
35
0.002
30
0 30
0.08 0.1 0.12 0.1 0.15 0.2
w/L w/L

Fig. 3 Finite element analysis to determine the phase boundary for anisotropic materials. a, b Energy and force, respectively, as a function of displacement,
for a beam with θ = 45o and a w/L ratio varying from 0.07 to 0.12. The dashed box indicates bistable w/L values. c Energy barrier, Eout, necessary for a
buckled beam to snap back to its undeformed configuration (the gray region indicates that the beam is monostable). d The phase boundaries as a function
of anisotropy, where k1=0 indicates an isotropic material and increasing k1 indicates increasing anisotropy (i.e., larger stiffness ratio EL/ET); everything to
the left of a particular line is bistable for that value of k1

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a 1.6 b c 1.4
Transverse, ηT = w/w0
1.5 1.3
Longitudinal, ηL = L/L0

Swelling anisotropy, ηT/ηL

Swelling ratios, ηT and ηL

1.4 1.3
1.2
1.3

(w/L)rel
1.2
1.2
1.1 w0 = 615 ± 13.2 μm

1.1 w0 = 732 ± 7.1 μm

1.1
w0 = 1216 ± 13.6 μm
1 1
Fit by equation (1)
0.9 1
0 5 10 15 0 5 10 15 0 0.5 1 1.5 2
Vol% of glass fibers Vol% of glass fibers t/ts

d w /L
0=
0 0.0983 w0/L0 = 0.0958

w0/L0 = 0.09

t* = Experimentally-measured actuation time

t* = 0 s t* = 6.19 ± 0.2 s t* = 12.7 ± 0.19 s t* = 28.33 ± 0.22 s
Toluene applied ^ ^ ^
(t* = 7.1 s) (t* = 13.4 s) (t* = 33.1 s)
^
t* = Predicted actuation time by equation (2)

Fig. 4 Control of actuation time. a Swelling ratio in the transverse (ηT = w/w0) and longitudinal (ηL = L/L0) directions for PDMS–GF composite materials
after submersion in toluene for one day. b Swelling anisotropy, ηT/ηL as a function of volume fraction of glass fibers. c The relative slenderness ratio (w/L)rel
as a function of time for beams with different initial widths (time is normalized by saturation time, ts, to account for the dependence of diffusion time on
volume of material). d Actuation time can be controlled by selecting specific values for the initial beam geometry, w0/L0. The measured time t* is given, as
well as the predicted time, ^t , as calculated from equation (2). The error bars are the standard deviations computed from multiple measurements

vol% PDMS-GF), as necessary to trigger an actuation event where the time ts = w02/8D is the time we expect the beam to be
(Fig. 1c). As a proof of concept, we provide simple demonstra- saturated (based on diffusion), and D is the diffusion coefficient
tions of such autonomous actuation in Supplementary Movies 2 of toluene in PDMS. Using equation (1) (Supplementary Note 7),
and 6 for material printed from PDMS-GF and exposed to the time at which we expect the beam geometry w/L to reach the
toluene. In Supplementary Movie 2, a bistable unit actuates and bifurcation point B (and hence to actuate) is
jumps dramatically due to the rapid release of strain energy from
the buckled beams. In Supplementary Movie 6, a bistable unit is ðBL0  w0 Þ2
^t  ¼  2 ð2Þ
integrated with the lid of a 3D printed box, and the strain energy 8D ηT  1
is harnessed to open the lid when an appropriate solvent is
encountered. In this case, the box remains closed when placed in
water, but when the water becomes contaminated by the addition (note, we use ^t  to indicate the time of actuation predicted by
of toluene, the beams actuate and open the box lid. Using this equation (2), and t* to indicate the measured time). Fig. 4d and
approach, for example, a box could float indefinitely in the ocean Supplementary Movie 7 demonstrate how different w0/L0 values
and wait to autonomously open to release a chemical or to obtain produce different t* in accordance with equation (2). We have
a sample when a particular pollutant is encountered, without printed samples with widths of 600–850 μm and lengths of 7–9
using batteries or sensors. mm. The actuation time for these can range from about 0.6 s to
108 s, which almost spans the range of theoretically predicted
Controlling the time of actuation. The distance between w0/L0 times (0–130 s) by equation (2).
and the bifurcation B will set a time interval between the intro- Since B and ηT are unitless and D is an intrinsic parameter, the
duction of the stimulus (t = 0) and the time at which the beam maximum actuation time for a beam with slenderness ratio w0/L0
actuates (t = t*). To quantify this time, we measured the changing would scale like w02. For example, if the beams were made an
value of w/L during solvent swelling (Fig. 4c) for the PDMS-GF15 order of magnitude smaller (e.g., around 85 μm in width) the
ink during submersion in toluene. We normalize the beam’s range of available actuation times would decrease from roughly
changing w/L ratio (see also Supplementary Figure 6 for non- 0–130 s to 0–1.3 s. For any length scale, the theoretical upper
normalized data) by the initial ratio w0/L0 to provide a relative bound of the actuation time is the time to saturation, ts = w02/8D,
value, (w/L)rel = (w/L)/(w0/L0), which, assuming simple diffusion, and the theoretical lower bound can be arbitrarily close to zero, as
can be derived (Supplementary Note 7) as w0/L0 can always be chosen to satisfy B-w0/L0 →0. In reality, small
( perturbations in environmental conditions and fabrication
pffiffiffiffiffiffiffiffiffiffiffi 
1 þ ðt=ts Þ ηT  1 ; t<ts limitations in beam geometry make infinitesimal ^t  unachievable
ðw=LÞrel ¼ ð1Þ and increase the uncertainty in experimental actuation time at
ηT ; t  ts these smaller values.

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a Toluene introduced t=0 Toluene introduced

locked
Trap Lock

Trap

Lock
Unit 1
Unit 2 Unit 2 Unit 1
t=0

b t1* Unit 1 actuates

unlocked

Unlocked

t1*

c Mass added d

Trap closed

e Relocked f Mass added t2* Unit 2 actuates

locked

t2* Trap remains open

Fig. 5 A “flytrap” with embodied logic Close(Stoluene, Smass | tmass - t1 < t2 - t1 ). a Toluene is applied to a flytrap-inspired system which is prevented from
closing by a lock that is toggled by two actuating units. b The unit with larger w0/L0 actuates first (at time t1 ), which unlocks the lobe. c, d If a mechanical
load is applied while the flytrap is unlocked it closes. e, f Later, the second bistable unit actuates (at time t2 ) and relocks the lobe; adding a mechanical load
at this point has no effect

Despite the simplistic assumptions in the model, we found that be smaller or larger depending on the length scale of the system)
the average discrepancy between ^t  and t* was about 17% for after which the units can be reset to the higher-energy state by
samples designed to actuate more than 20 s after exposure to the compression (to buckle the beams again). We performed repeated
stimulus. As this time is reduced, the relative error of the model tests (actuation–drying–resetting–actuation) on five units and
increases. For example, for samples designed to actuate at times found that the intra-sample variability of actuation time is
less than 5 s after exposure to the stimulus, the relative error of the comparable with the inter-sample variability, as discussed above
model increases to about 44%. The high discrepancy for short (see Supplementary Table 2).
actuation times (<5 s) arises from several challenging factors: non-
uniform exposure to the chemical stimulus (not accounted for in Demonstrations of embodied logic. In addition to the control of
the model, which assumes instantaneous, uniform exposure); the actuation time, self-actuating systems that consist of multiple
particularly close proximity of the geometric parameters to a actuating units (each of which may be a different material, to
bifurcation point when short delay times are desired, correspond- respond to different stimuli) can be constructed. There are many
ing to a very small energy barrier; experimental uncertainty in ways that these can be arranged, leading to different possible
the precise location of the phase boundary (exacerbated by the system functions of varying complexity. We utilize a shorthand to
small energy barrier near bifurcation); and deviations in friction describe some of these possible functions: first, we indicate a
between the material and the substrate. At longer intervals of time functional event in bold followed in parentheses by the condition
(>5 s) these problems are diminished. In practice, this uncertainty that is necessary for that event to occur; example functions
would set a practical limit on how closely a sequence of ordered include Open and Close, referring, e.g., to the opening or closing
actuation events could be temporally spaced. of a box. Second, the application of a stimulus is indicated by the
If we allow time for the solvent to evaporate, the beams return symbol S with an appropriate subscript; here, stimuli can include
to their initial geometric parameters (w0/L0), and are once again Stoluene (which actuates PDMS-based materials), Swater (which
bistable (see Supplementary Figure 7, and Supplementary actuates hydrogel-based materials), and Smass (which refers to
Table 1). External energy is required to reset the units to the placing a mass on the structure). For example, Open(Swater)
higher-energy state in order to reuse them. At ambient would indicate that a structure should open when exposed to
conditions, the drying time is about 70 min (though this could water, which would be accomplished by using a hydrogel-based

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material to actuate. Finally, if multiple stimuli must occur within a Hydrogel

some time interval, this is indicated by a value assigned to Δt*. As actuated by water

a first example, we 3D print a box (see Methods) which is Lock PDMS

actuated by toluene
designed to autonomously open when exposed to toluene, but
then to close again after a defined interval of time (e.g., 20 s). This
behavior can be written as TimedOpen(Stoluene | Δt* = 20 s). To Example 1 Example 2

open and then close the box, we need two actuation events, which Stoluene PDMS Lid Stoluene PDMS
we accomplish by integrating two PDMS-GF actuating units with Swater Hydrogel Stoluene Hydrogel
the box, each with different values of w0/L0. These values are
chosen such that simultaneous exposure to toluene will cause
them to reach the phase boundary, B, 20 s apart. We show this
behavior in Supplementary Movie 8: after exposure to toluene,
b d
the right unit actuates first, opening the box. Then, after ~20 s, the
left unit actuates and closes the box. The second demonstration
mimics the rapid closing of the Venus flytrap when an object
(denoted Smass) is placed on a waiting ledge, with the added
requirement that the trap is only in operation if a chemical signal
(toluene) has been applied (see Supplementary Movie 9). We can
represent this behavior as Close(Stoluene ∧ Smass). The trap is
locked until a PDMS-based unit actuates, preventing the lobes *
thydrogel *
tPDMS
from closing until t ≥ t* even if a load is applied before then. Lock opened Lid jammed
Figure 5 shows a similar Venus flytrap-inspired example, but
with more complex control logic. In this example, there are two c e c
actuating units made from PDMS-GF, which are designed to Open

State
actuate 10 s apart (Fig. 5a). The first of these (which actuates at a b
t1 ) activates the system by removing the lock (as in Fig. 5b) while Closed
t
the second (which actuates at t2 ) re-locks the flytrap, once again *
thydrogel *
tPDMS
preventing it from closing. If a mass is placed on a platform in the Ex.1 S Applied
center of the flytrap at a time between t1 and t2 (i.e., when the
Open

State
lock is disengaged) the lobes will close (Fig. 5c, d and a d
Supplementary Movie 10). If the mass is placed on the platform *
tPDMS Closed
when the lock is engaged (e.g., after t2 , as in Fig. 5e, f and Lid opened
*
t
Ex.2 S Applied tPDMS
Supplementary Movie 11) it will have no effect. This functionality
is described by Close(Stoluene, Smass | tmass - t1 < t2 – t1 ), where the Fig. 6 Multimaterial responsive systems, e.g., Open(Swater ∧ Stoluene |
comma indicates an ordered list of stimuli, and t2 –t1 = 10 s. thydrogel < tPDMS ). a A box with a lid which is unlocked upon actuation of a
Finally in Fig. 6, we demonstrate a multi-stimuli-responsive hydrogel-based unit (at time thydrogel ) and subsequently opened upon
system67,68, which uses two materials that respond to two actuation of a PDMS-based unit (at time tPDMS ). b, c Example 1: if water is
orthogonal stimuli (i.e., hydrogel, which responds to water, and applied to the hydrogel-based unit and toluene to the PDMS-based unit, the
PDMS, which responds to a non-polar solvent such as toluene). lid is unlocked and then pushed open, successfully opening the box
We compose a box which follows the behavior Open(Swater ∧ (Supplementary Movie 12). d Example 2: if toluene is applied to both units,
 
Stoluene | thydrogel <tPDMS ), as shown in Fig. 6a. Application of Swater the PDMS-based unit actuates as it should, but because the hydrogel-based
causes the hydrogel-based unit to actuate, opening a lock (at time unit is unresponsive to toluene, the lock interferes and the lid remains

thydrogel ) that otherwise obstructs the opening of the lid. closed (Supplementary Movie 13). e Diagram representing the system logic
Application of Stoluene causes the PDMS-based unit to actuate and the behaviors of the system in Examples 1 and 2

(at time tPDMS ), pushing open the lid if it has been unlocked
(Fig. 6b, c and Supplementary Movie 12). If instead we apply only
toluene, the hydrogel-based lock does not respond, and the box alignment of the fibers during extrusion, the beams swell aniso-
remains closed even when the PDMS-based unit pushes on the lid tropically in the presence of suitable stimuli, triggering rapid and
(Fig. 6d, e and Supplementary Movie 13). This capability could be large-amplitude configuration changes at predetermined times (as
used, for example, to produce a sampling box that autonomously the geometric parameter w0/L0 passes a bifurcation point). Using
opens when it encounters an oil–water interface, without any solely architected soft materials as self-actuating functional ele-
external power or solid-state sensors and actuators. ments, our approach enables complex function and control of
These principles can be further extended to 2D or 3D by timing in response to multiple stimuli. We demonstrated several
designing more complicated arrangements of beams. As a autonomous responsive systems in this work as examples of our
demonstration of this, we manufactured 2D samples using approach, all performing their designated functions without
PDMS-based materials and illustrated autonomous deployment mechatronics, traditional control systems, or tethering. This
due to the presence of toluene (Supplementary Movie 14). includes a hopper that autonomously jumps when an undesired
chemical is introduced, a “flytrap” that only closes if mechanically
stimulated during a pre-programmed interval of time, and a box
Discussion that only opens if it encounters both non-polar solvents and
In summary, we have designed and 3D printed systems of self- water. While this work focuses on the autonomous release of
actuating structures capable of simple logic (AND, OR, and strain energy to produce precise actuation events, these concepts
NAND) and controlled timing of actuation in response to mul- could be integrated with more complex systems. For example,
tiple stimuli. We have accomplished this using PDMS-based and advances from soft robotics, such as the integration of pneumatic
hydrogel-based materials that respond to different environmental or chemical energy sources69, could allow the units to be
stimuli. Due to the use of short fiber composites and the autonomously reset to allow repeated actuation events. We also

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NATURE COMMUNICATIONS | [Link] ARTICLE

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