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International Journal of Applied Mechanics
DOI: 10.1142/S1758825117501034
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A Combined Analytical-Numerical Investigation on Photo-Sensitive Hydrogel
Micro-Valves
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Arash Kargar-Estahbanaty, Mostafa Baghani*, Hamid Shahsavari, Ghader Faraji
School of Mechanical Engineering
College of Engineering, University of Tehran, Tehran, Iran
*baghani@ut.ac.ir
thermal sensitive hydrogels are described. Two benchmark problems common in micro-fluidic designs
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are solved using the presented theory, and the deformation and stress distributions are calculated. The
theory is implemented into a finite element (FE) framework through developing a user-defined
subroutine. To properly validate the finite element model, the FE results are compared with the
proposed analytical results. The confirmed numerical method is then employed to investigate two
different realistic micro-valve structures. The constructions are composed of three jacket-pillar
structures arranged in two different patterns. In this step, the nonlinear contact between the
components of structures and presumptive rigid walls are added to the thermo-mechanical deformation
of the photo sensitive micro-jackets. The contact length and contact pressure are investigated. By
calculating all necessary mechanical parameters, the analysis results can be utilized in the design
procedure of a photo sensitive micro-valve and pave the way for the industrial production of the next
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generation micro-fluidic devices.
Keywords: Photo-thermal sensitive; Photo sensitive; Hydrogel; Micro-valve; Analytic study; FEM
1. Introduction
A polymer network consists of polymer chains that are covalently crosslinked. When
a hydrophilic polymer network, having a tendency to mix in water, equilibrates with an
aqueous solution, it absorbs a huge amount of solvent and swells. The swollen state is
called hydrogel. The swelling process can be affected by many external stimuli e.g.,
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temperature [Mazaheri et al., 2016; Abdolahi et al., 2016], pH [Marcombe et al., 2010;
Hamzavi et al., 2016; Arbabi et al., 2017], light [Toh et al., 2014; Suzuki and Tanaka, 1990]
and electrical field [Fukunaga et al., 2008; Liu et al., 2015]. Some sort of hydrogels can be
stimulated via more than just one external field such as Photo-Thermal Sensitive (PTS)
hydrogels, influenced by either change in the temperature or light intensity [Suzuki, 1994].
Smart hydrogels are employed in the design of microsensors [Lee and Braun, 2003; Shin
et al., 2010] and actuators [Morimoto and Ashida, 2015; Ionov, 2013; Liu et al., 2016].
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cylindrical jacket. While the volume of the core is fixed, the pillar volume may vary by a
change in the stimulus. Using this structure, self-adjusted devices can be designed in which
flow channel outlet alters as a result of stimulus variation [Mazaheri et al., 2015].
Understanding hydrogels swelling behavior is crucial in these applications. Different
field theories of hydrogels have been introduced to explain the swelling phenomenon.
These theories account for the effect of deformation of the network, migration of solvent,
and swelling thermodynamics of hydrogels [Baek and Pence, 2011; Hong et al., 2009]. The
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proposed theory, firstly introduced to model neutral hydrogels, extended to the thermal
sensitive hydrogels through imposing the temperature variation effects on the energy
function [Cai and Suo, 2011; Ding et al., 2013]. Based on these theories, PTS hydrogels
model were developed, possessing an energy function which not only accounts for the
influence of the temperature, but also imposes the effect of irradiated light intensity [Toh
et al., 2014]. In this model, a photochemical energy was added to the energy density and
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in the light of Planck–Einstein relation, the effect of the light irradiation on the temperature
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In this study, in the formulation section, the free energy of photo-thermal sensitive
hydrogels is briefly introduced and governing equations are developed for homogeneous
and inhomogeneous swelling of PTS hydrogels. The result section is organized as follows:
At the first step, we analyze homogeneous swelling of a solid cylinder and inhomogeneous
swelling of a jacket-pillar mechanism analytically for various material and geometrical
parameters, making use of nonlinear field theory of hydrogels. Then, we implement the
presented material model into a FE framework, employing a user-defined subroutine. Two
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patterns studied analytically in the previous step, are solved by FEM. The deformation and
stresses calculated by the analytical method are compared with those of numerical
simulations (FEM). At the second step, two proposed patterns of multi-jacket valves are
analyzed numerically. In this step, the contact between different components of a micro-
fluidic structure and its influence on the coupled thermo-mechanical behavior of hydrogel
valve is studied. Comparing the configurations, a design method for a photo sensitive
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hydrogel micro-valve is achieved. At the final section, we present a summary and draw
conclusions.
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In this section, we represent a model for PTS hydrogels, firstly developed by Toh et al.
(2014). Fig. 1 illustrates a polymeric gel submerged in an aqueous solution. The solution
chemical potential is µs. An external traction load Ti and a body force Bi are exerted to the
gel. Also, an external source illuminates light to the network. The effect of the light
irradiation is considered by introducing parameter µ p called the photo-chemical potential.
Considering large deformation theory, in the thermodynamic framework, the change in the
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WdV T x dS B x dV
i i i i s C s dV p C p dV (1)
Solvent
Drain
Light
Irradiation Solvent
Absorption
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Mechanical M
Load
ˆ
WdV T x dS B x dV
i i i i
(2)
Now, we use the constrained equations to define Cs and Cp. It should be considered that
stress caused by external loads do not influence the gel volume change significantly, and
the only factor that makes change in the hydrogel volume is the amount of absorbed fluid.
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[Suzuki and Tanaka, 1990] demonstrated that a change in temperature due to irradiation
is proportional to polymer volume fraction ( ) and light intensity (I 0 ) as:
I 0 (4)
where is a proportionality constant. In addition, the hydrogel heat capacity can be
considered as the volumetric weight of capacity of its constituents as ([Toh et al., 2014]):
c ( g ) c ( net ) c (w ) (1 ) (5)
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where cgel, cw and cnet are volumetric heat capacity of gel, water and polymer network,
respectively.
The light irradiated to the system causes a change in the hydrogel temperature. With
1 / J , employing Eqs. (4) and (5) and applying conservation of energy, we assume
light energy density as E hfC p and change in the hydrogel energy density as E c gel
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cw c net cw I 0 (6)
Cp ( )
J J2 hf
Considering the calculated constraints and using the stretch free energy as Neo-
Hookean and taking the free energy of mixing in the Flory-Huggins format, the modified
free energy function could be expressed in the following form:
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1 kT J 1 (8)
Wˆ NkT (I1 3 2ln(J)) (J 1)(ln( ) ( 0 12 ))
2 J J J
I 0 cw c net cw J 1
kT ( ) s ( )
hf J J2
where k is the Stefan-Boltzmann constant and T is the temperature of the hydrogel. The
parameters J and I 1 may be defined as J= 12 3 and I 1 1 2 3 using principal
2 2 2
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stretches. 0 and 1 are mixing parameters and are determined via the following relations
[Afroze et al., 2000]:
0 (B 0T A0 ), 1 (B1T A1 ) (9)
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where A0, A1, B0 and B1 are experimental constants and is a fitted parameter which
depends on the molar fraction of the light sensitive nano-particles [Toh et al., 2014].
Consequently, we define nominal first Piola stresses as:
Wˆ (10)
Pi
i
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In the following sections, we employ the energy equation provided in Eq.(8) to solve
two benchmark problems, applicable in micro-fluidic design: homogeneous swelling of a
hydrogel cylinder and the inhomogeneous swelling of a PTS jacket coated on a rigid
cylindrical pillar. In the results section, the solutions are utilized in design of a photo
sensitive microvalve. The calculated analytical results are also used to validate FEM results
in the results section.
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of a single variable λ:
2 1
W 1 / 2 Nv 2 2 1 3 2ln 2 2 1 ln 2 2 12 0 (11)
I 0 cw c net cw
hf 2 4
The lateral stretch (λ) can be calculated through minimizing the free energy with
respect to its single variable ( W / 0 ). The homogenous swelling of a solid cylinder
is solved in results section for various material parameters.
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causes the hydrogel shell to swell. A and B are corresponding values for the shell inner and
outer radii in the initial configuration, respectively. Keeping fixed the inner radius A in the
deformation process, the outer radius is changed from B to b as a result of the swelling.
Since the solvent is water, the chemical properties of which is fixed in the whole
investigation, from now on, we put chemical potential equal to zero in the equations. Since
the cylinder is constrained in the axial direction, it justifies a plane strain condition.
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b
B Reducing
Light r(R)
R
A Intensity
A
Rigid
Pillar
Hydrogel
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Jacket
(a)
(b)
Fig. 2. (a) Initial and (b) final configuration of the jacket-pillar structure.
Therefore, the longitudinal stretch is assumed to be constant and equal to unity. Due to
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dPr Pr P (12)
0
dR R
where Pr and Pθ denote normal and hoop nominal stresses, respectively, and R is the
element radius at the reference state. Substituting λr and λθ as normal and tangential
stretches, respectively, the parameters I1 and J can be replaced in Eqs. (8) and (10),
successively to calculate the radial and hoop stresses as:
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dr (R ) r (R ) (15)
r ,
dR R
Putting the stretches defined in Eq. (15) into the stress equations (Eq. (13) and Eq. (14))
and substituting the nominal stresses in equilibrium equation (Eq. (12)), we arrive at a
second order nonlinear ODE for r(R):
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(16)
C 2 (r,r,R) rC1 (r,r) C 0 r,r,R 0
C 0 (r )4 r 1 R
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5 6
C 1 r r N 2C L cw 2 N 1 r 6C L c net cw r
4
5 4 3
C2 r r r RN 2C L cw 2 N 1 r
2
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where 0 1 J , J r R r and C L I 0 hf .
The boundary conditions of the second order ODE (Eq.(16)) are as follow:
r (R ) A at R A , r (R ) 0 at R B (17)
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The boundary conditions impose no displacement condition on the inner radius and the
stress-free condition on the outer radius.
A semi-analytical solution is employed to calculate r(R) distribution in different
temperatures and light intensities. The calculations are performed through employing the
finite difference technique. Trapezoid method is employed as the based scheme and
Richardson extrapolation is added as the enhancement scheme, resulting in high-accuracy
results when the error term has a predictable format [Burden and Faires, 1989]. A 100000-
element mesh is used to solve the nonlinear Boundary Value Problem (BVP). A linear
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distribution is implemented as an initial guess for the BVP. Interested readers can see
[Baghani et al., 2016] for further study about Richardson extrapolation. Furthermore, a
detailed discussion of the numerical method is available at [Ascher et al., 1995]and [Ascher
and Petzold, 1998].
(CPE4H) where mesh independency is examined. The channel walls are modeled as a
discrete rigid. A normal “hard” contact is defined between the surfaces. The intensity is
expressed as a predefined field and introduced by the TEMP phrase in the UHYPER.
Instead of defining a rigid pillar, the inner radius of the jacket is fixed in order to simulate
the rigid pillar influence.
3. Numerical Results
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In this section, the method provided in the previous section is employed to design a
photo-sensitive micro-valve. We utilize material parameter of PNIPAAM temperature
sensitive hydrogel incorporated with 5% light absorbing nano-particles. The utilized
material parameters are listed in Table 1 and are held constant during the whole
investigation. The temperature variation can affect the mechanical behavior of the micro-
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valve, but it is not the case here. Therefore, we set the temperature fixed at 309K. The
whole study can be conducted at any other temperature. Firstly, the numerical method is
verified for several cases of homogeneous and inhomogeneous deformations. The results
are compared with those of the proposed analytical analysis and a parametric study is
performed. In the next step, more realistic sketches with more mechanical complexities are
analyzed with the aid of the numerical method.
Table 1. Material parameters
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PARAMETER VALUE REFERENCE
A0 -12.947 [Afroze et al., 2000]
B0 0.04496K
1 [Afroze et al., 2000]
A1 17.92 [Afroze et al., 2000]
B1 0.0569K
1 [Afroze et al., 2000]
α 1 [Suzuki and Tanaka, 1990]
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2
0.6m K .W
[Suzuki and Tanaka, 1990]
F
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6.1434 10 Hz
14
H 34
6.626 10 m .kg . s
2 1 [Toh et al., 2014]
cnet 2.4 10 J . m . K
7 3 1 [Birgersson et al., 2008]
cw 4.18 10 J . m . K
6 3 1 [Birgersson et al., 2008]
c cu 3.44 10 J . m . K
6 3 1 [Toh et al., 2014]
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As depicted in Fig. 3., a hydrogel solid cylinder can swell freely by decreasing the light
intensity. The analytical results are calculated solving Eq.(11) in different light intensities
for three different polymer network densities (Nυ). Numerical results are computed solving
a one-fourth cylinder and imposing symmetric conditions. It is observed that decreasing
Nυ causes larger stretches in the cylinder to be generated. The swelling ratio undergoes
severe changes in lower intensities. Therefore, it is better to restrict the photo sensitive
micro-valves actuation area in the vicinity of the zero intensity, which results in more
sensitive valves. As one may observe from Fig.3, the numerical results agree with the
analytical solution in all the cases.
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tangential stresses at the final configuration (I0=0) are depicted in Fig. 5. The analytical
Cauchy stress is calculated by pushing forward the nominal stresses in Eq.(13) and (14). (
i i Pi / J ).
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Fig. 3. Stretch versus the light intensity for homogeneous swelling of PTS hydrogel cylinder. ‘ANL’ stands
for the analytical results and ‘FEM’ stands for finite element results.
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Fig. 4. Normalized outer radius of the jacket-pillar as a function of intensity for different radius ratios and
Nυ=0.001. ‘ANL’ stands for the analytical results and ‘FEM’ stands for finite element analysis results.
It is observed that the maximum values of both stresses occur at the inner radius, due
to the confinement. In addition, increasing Nυ results in an increase in the maximum radial
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and tangential stresses. The figure shows an excellent agreement between the analytical
stress prediction and FEM results. At the first sight, it may be conceived that lower network
densities might be the best choices, but it should be mentioned that a lower Nυ causes a
less stiff hydrogel [Morimoto and Ashida, 2015]. As the stiffness and rigidity decreases,
the valve leaks at a lower inlet pressure which is a disadvantage in micro-valve design
[Arbabi et al., 2017; Zhang et al., 2012]. Fig. 6. illustrates normalized stress contours for
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Fig. 5. Normalized stress distribution versus the normalized initial radius. Lines and circles stand for the
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analytical and numerical radial stresses, and diamonds denote the numerical tangential stresses.
From now on, we utilize the verified numerical method to analyze more realistic and
complex valve configurations. The numerical method can predict the interaction between
the thermo-mechanical response of hydrogels as well as the nonlinear contact between
different components of the valve. The parameters such as contact length and contact
pressure distribution are also considered. Since the dominant phenomenon in the hydrogel
valves time response, is fluid diffusion [Beebe et al., 2000], employing multiple smaller
hydrogel jackets can enhance the valve performance considerably. Fig. 7. demonstrates
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two different patterns proposed for a hydrogel multi-jacket micro-valve. The patterns are
called Inline (IL) and Upstream (US), respectively. The patterns dimensions are also shown
in Fig. 7. The configurations are designed so that, they pass an equal fluid flux at the open
condition when the inlet pressure is the same [Arbabi et al., 2017]. As one may observe,
although the US pattern possesses bigger valves, it passes an equal volume of fluid due to
its more hydrodynamic shape. The valves initial and final intensities are the same for both
cases. At the initial configuration, the valves are exposed to a 300 mw light irradiation. The
intensity is reduced to zero in the final configuration. The total deformation contour is also
displayed in Fig. 7. As depicted, US configuration contours undergo larger total
displacements.
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A considerable concern in the micro-valve design, is the sealing problem. In order to avoid
the leakage in the channel, enough contact length and pressure should be achieved in the
closed condition. Fig. 8. (a) and (b) demonstrate the contact between valves and walls, and
between the adjacent valves, respectively. The contact length is plotted versus the light
intensity in the vicinity of the closed condition (I0=0). From Fig. 8.(a) and (b), it is observed
that the hydrodynamic (US) configuration possesses a larger contact length, which makes
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it a more reliable valve. Additionally, in this case, the wall contact initiation occurred in a
higher intensity, comparing with IL configuration. As it is observed in Fig. 8, by reducing
less than 10mw in the intensity, the valve contact length can be increased from zero to 200
µm. It shows that the valve is highly sensitive to the light illumination which makes it a
suitable choice for micro-fluidic applications.
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Fig. 6. Normalized stress distribution contour for (a) numerical radial, (b) numerical tangential, (c)
analytical radial and (d) analytical tangential stresses for Nυ=0.001
In the following, Fig. 9. (a) and (b) depict normalized contact pressure distribution for
the IL configuration in the wall-and-valve contact (contact between rigid walls and their
nearby valves) and the valve-and-valve case (contact between two adjacent valves),
respectively. Locations at which two different contacts occurs are demonstrated in Fig. 7.
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In this pattern, the valve-valve contact (Fig. 9.b) is initiated at a greater intensity (after
8mw) comparing with wall-valve contact (Fig. 9.a) which is started after 6mw. The
pressure distribution is mainly influenced by the contact theory we choose in the analysis
and since the theory used for the analysis is identical in the whole investigation, the other
pattern pressure distributions are also the same. Comparing the normalized contact pressure
(Fig. 9) with the radial and tangential stresses caused by constrained deformation (Fig. 5
and Fig. 6), we observe that deformational stresses and contact stresses are on the same
order. Thus, contact stresses are influential and should be involved in the stress analysis.
In the case of inline configuration, the influence of normalized outer radius of jackets on
maximum contact pressure and maximum contact length at final configuration (I0 0) is
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illustrated in Fig. 10. The other geometrical parameters such as channel length, valves
distance and jacket inner radius are held fixed and similar to Fig. 7.(a). The lines are the
lower order polynomial fitted to the numerical results with an acceptable value of
regression. The contact pressures are fitted with a second order polynomial
(a 2 x 2 a1 x a 0 ) and the contact length fitted with a third order one (a 3 x 3 a 2 x 2 a1 x a 0 )
, coefficient of which are listed in Table 2.
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Fig. 7. (a) Inline, (b) Upstream patterns in the initial (left-hand-side) and deformed (right-hand-side)
configurations. The total displacement contour, for the deformed configurations, is also provided. The
light intensity reduced form 300 mw to zero.
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Fig. 8.(a) wall-valve and (b) valve-valve contact length versus intensity for Nυ=0.001 and the two
configurations. ‘IL', ‘US’ stand for Inline and Upstream patterns, respectively.
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-3 -3
x 10 x 10
1 1.2
Normalized Contact Pressure [ /kT ]
Decreasing 1 Decreasing
0.8
Light Light
(a) Intensity 0.8
(b) Intensity
0.6
0.6
0.4
0.4
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0.2
0.2
0 0
-200 -150 -100 -50 0 50 100 150 200 -200 -150 -100 -50 0 50 100 150 200
Distance from the Center of Contact [ m ] Distance from the Center of Contact [ m ]
Fig. 9. (a) wall-valve and (b) valve-valve contact pressure versus the distance from the center of contact
for Nυ=0.001 and Inline configurations.
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-3
x 10
3 4
3.5 R:Wall-Valve
2.5 R:Wall-Valve (a) (b)
R:Valve-Valve
R:Valve-Valve 3
F:Wall-Valve
2 F:Wall-Valve
2.5 F:Valve-Valve
F:Valve-Valve
1.5 2
[/kT]
[Lc /a]
1.5
1
1
0.5
US
0.5
0 0
1.7 1.8 1.9 2 2.1 2.2 2.3 2.4 2.5 2.6 1.7 1.8 1.9 2 2.1 2.2 2.3 2.4 2.5 2.6
B/A B/A
Fig. 10. (a) Normalized maximum contact pressure and (b) maximum contact length versus the
normalized outer radius. ‘R’ and ‘F’ stands for numerical results and fitted curves, respectively
Parameter a0 a1 a2 a3
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maximum radial and tangential stresses occurred at the inner radius which was constrained,
where the maximum deformation took place at the outer radius. Increasing the jacket
thickness led to more stretches. Due to the symmetry, the stress distribution was also
symmetric and depended only on the radial position. Moreover, decreasing the network
density increased the deformation and decreased the stress values, but it also led to more
fragile hydrogels with lower stress endurance capability, that is not a desirable feature.
In the following, a user-defined subroutine (UHYPER) was developed and numerical
simulation of the benchmark problems was also conducted. The numerical simulation
results were verified comparing with the analytical calculations. In the next step, two
different patterns with more complexity were represented: two photo sensitive micro-
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valves were introduced by multi-jacket pillar structures which were also in contact with a
rigid wall. In this case, the nonlinear contact was added into the coupled thermo-
mechanical behavior of hydrogel pillar-jacket structure. The contact length and pressure
were investigated in both cases. The results depicted that the more hydrodynamic structure
can create a greater contact length. The contact pressure distribution was the same for both
cases and depended on the contact theory employed in the numerical simulations. At the
final step, we studied the effect of the jacket geometry on the maximum contact length and
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maximum contact pressure and the numerical results were fitted by the polynomials,
coefficients of which were also reported. According to our calculations, the contact
pressure values have a significant influence on the micro-valve stress distribution and
should be involved in analysis.
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