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On the stability of inhomogeneous fluids under acoustic fields

Varun Kumar Rajendran\aff1    Aravind Ram S P    Karthick Subramani\aff1 \corresp karthick@iiitdm.ac.in \aff1Department of Mechanical Engineering, Indian Institute of Information Technology, Design and Manufacturing, Kancheepuram, Chennai-600127, India
Abstract

In this work, we present the stability theory for inhomogeneous fluids subjected to standing acoustic fields. Starting from the first principles, the stability criterion is established for two fluids of different acoustic impedance separated by a plane interface. Through stability theory and numerical simulations we show that, in the presence of interfacial tension, the relocation of high-impedance fluid from anti-node to node occurs when the acoustic force overcomes interfacial tension force, which is in agreement with recent microchannel experiments. Furthermore, we establish an acoustic Bond number that characterizes stable (Boa<1Bo_{a}<1) and relocation (Boa>1Bo_{a}>1) regimes. Remarkably, it is found that the critical acoustic energy density required for relocation can be significantly reduced by increasing the channel height which could help design acoustofluidic microchannel devices that handle immiscible fluids.

1 Introduction

When an acoustic field encounters inhomogeneity, it exerts acoustic radiation force on it. Here by inhomogeneity, we mean non-uniform or discontinuous variation of physical properties in a system such as particles/cells suspended in fluid, emulsions, co-flowing streams of miscible or immiscible fluids, and fluid subjected to a temperature gradient. The acoustic forces acting on inhomogeneity are extensively studied in microscale flows, and this field is known as ’microscale acoustofluidics’(Friend & Yeo, 2011). Over the last two decades, acoustofluidics has found a wide range of applications in biological(Ahmed et al., 2016; Iranmanesh et al., 2015; Collins et al., 2015; Christakou et al., 2013; Lakshmanan et al., 2020), chemical(Shi et al., 2009; Xie et al., 2020), and medical(Li et al., 2015; Lu et al., 2019; Zhang et al., 2020) sciences.

Recently, the relocation and stabilization of inhomogeneous co-flowing fluid streams in microchannels has gained the attention of the research community which is evident from the following works. Through silicon-glass microchannel experiments, Deshmukh et al. (2014) could relocate high-impedance sodium chloride solution to node (center) and low-impedance water to anti-node (sides). Also, they could stabilize high-impedance fluid at the center (and low-impedance fluid to the sides) against gravity stratification using acoustic forces. In addition to the above experiments on miscible fluids, Hemachandran et al. (2019) demonstrated the relocation of immiscible fluids using acoustic fields by overcoming the interfacial tension forces. Followed by this, Karlsen et al. (2018) showed that acoustic forces acting on stable inhomogeneous fluid configuration could effectively suppress the boundary-driven Rayleigh streaming in the bulk. The theoretical framework and understanding of the above non-linear acoustic forces on inhomogeneous fluids are provided by Rajendran et al. (2022); Karlsen et al. (2016, 2018). Other notable works on the practical applications of acoustic forces on co-flowing inhomogeneous fluids include iso-acoustic focusing of cells (Augustsson et al., 2016), acoustic focusing of sub-micron particles (Van Assche et al., 2020; Gautam et al., 2018), tweezing and patterning of inhomogeneous fluids in a microchannel (Karlsen & Bruus, 2017; Baudoin et al., 2020), rapid mixing of fluids using an alternating multinode method (Pothuri et al., 2019), reversible stream-droplet transition in a microfluidic co-flowing immiscible system (Hemachandran et al., 2021). Despite the above recent advancements and practical importance, the criterion at which the inhomogeneous fluid system becomes unstable or stable under acoustic fields has not been clearly established. This paper aims to establish the stability criterion of inhomogeneous co-flowing fluids subjected to standing acoustic wave fields.

In this work, using linear stability analysis, we derive the dispersion relation that governs the stability of inhomogeneous fluids (with and without interfacial tension) under acoustic body force. We study the various parameters such as the initial arrangement of fluids, the position of the interface with respect to the node, acoustic energy density, the height of the channel, and surface tension to establish the necessary and sufficient conditions for relocation and stability. For fluids with interfacial tension, a non-dimensional number called acoustic Bond number is obtained theoretically which characterizes stable and unstable (relocation) regime. Also, we deduce a relation between critical acoustic energy density and the height of the channel which paves a way for relocating fluids with higher interfacial tension (𝒪(101(\mathcal{O}(10^{1} to 102)mN/m)10^{2})mN/m) in a microchannel. Furthermore, numerical simulations are carried out using generalized acoustic body force which agrees well with the derived theoretical stability criterion.

2 Physics of the problem

The hydrodynamics of the inhomogeneous fluids involved in this study is governed by the mass-continuity and momentum equations (Landau & Lifshitz, 1987),

ρt+(ρV)=0,\displaystyle\frac{\partial\rho}{\partial t}+\bm{\nabla\cdot}(\rho\textbf{\emph{V}})=0, (1a)
ρDVDt=P+η2V+βη(V)+fac.\displaystyle\rho\frac{D\textbf{\emph{V}}}{Dt}=-\bm{\nabla}P+\eta\nabla^{2}\textbf{\emph{V}}+\beta\eta\bm{\nabla}(\bm{\nabla\cdot}\textbf{\emph{V}})+\textbf{\emph{f}}_{ac}. (1b)

where ρ\rho represents density, V represents the velocity vector field, PP represents the pressure field, η\eta is the dynamic viscosity of the fluid, β=(ξ/η)+(1/3)\beta=(\xi/\eta)+(1/3), ξ\xi is the bulk viscosity, and D/DtD/Dt denotes the material derivative (D/Dt=t+VD/Dt=\partial_{t}+\textbf{V}\bm{\cdot\nabla}). Here the body force fac\textbf{\emph{f}}_{ac} is only due to acoustics. The gravitational body force is neglected since it is dominated by acoustic force in microscale flows. The acoustic body force fac\textbf{\emph{f}}_{ac} is given as (Rajendran et al., 2022)

fac=ρ0v1v1=\displaystyle\textbf{\emph{f}}_{ac}=-\bm{\nabla\cdot}\langle\rho_{0}\textbf{\emph{v}}_{1}\textbf{\emph{v}}_{1}\rangle= (12(κ0|p1|2ρ0|v1|2))+[v1××(ρ0v1)]\displaystyle\left(\frac{1}{2}\bm{\nabla}\left(\kappa_{0}\langle|p_{1}|^{2}\rangle-\rho_{0}\langle|\textbf{\emph{v}}_{1}|^{2}\right\rangle)\right)+\biggl{[}\langle\textbf{\emph{v}}_{1}\times\bm{\nabla}\times(\rho_{0}\textbf{\emph{v}}_{1})\rangle\biggr{]}
+(12|p1|2κ012v12ρ0)\displaystyle+\left(-\frac{1}{2}\langle|p_{1}|^{2}\rangle\bm{\nabla}\kappa_{0}-\frac{1}{2}\langle\textbf{\emph{v}}_{1}^{2}\rangle\bm{\nabla}\rho_{0}\right) (2)
=\displaystyle= (f1)+[f2]+(f3).\displaystyle\ (\textbf{\emph{f}}_{1})+[\textbf{\emph{f}}_{2}]+(\textbf{\emph{f}}_{3}). (3)

where p1p_{1} and v1\textbf{\emph{v}}_{1} denote the first-order (fast time scale) pressure and velocity fields due to acoustic waves (see Appendix A) and \langle...\rangle is the time average in one oscillation period (the time average of two first-order fields u1v1\langle\textbf{\emph{u}}_{1}\textbf{\emph{v}}_{1}\rangle is defined as 12\frac{1}{2}Real(u1v1\textbf{\emph{u}}_{1}^{\star}\textbf{\emph{v}}_{1}), where \star denotes complex conjugation). The terms ρ0\rho_{0} and κ0\kappa_{0} denote the zeroth-order (background) density and compressibility of the fluid. In (2), the first term is a conservative or gradient term that induces pressure and not fluid flow, the second term is only dominant at boundary layers and is responsible for boundary-driven Rayleigh streaming and the third term is responsible for relocation and stabilization of inhomogeneous fluids. Hence, only the relevant third term (f3\textbf{\emph{f}}_{3} in (3)) is considered for theoretical analysis. For the standing acoustic wave applied along the X-direction, |p1|2=pa2sin2(kwx)\langle|p_{1}|^{2}\rangle=p_{a}^{2}\sin^{2}(k_{w}x), |v12|=pa2/(ρ02c02)cos2(kwx)\langle|\textbf{\emph{v}}_{1}^{2}|\rangle=p_{a}^{2}/(\rho_{0}^{2}c_{0}^{2})\cos^{2}(k_{w}x), kw=2\upi/λwk_{w}=2\upi/\lambda_{w} denotes the wavenumber (λw\lambda_{w} denotes the wavelength) and pap_{a} denotes the pressure amplitude. Then the relocation force frlf_{rl} can be well approximated in terms of impedance gradient as (Rajendran et al., 2022)

f3=frl=Eaccos(2kwx)Z^.\textbf{\emph{f}}_{3}=\textbf{\emph{f}}_{rl}=-E_{ac}\cos({2k_{w}x})\bm{\nabla}\hat{Z}. (4)

where Eac=pa2/(4ρavgcavg2)=(va2ρavg)/4E_{ac}=p_{a}^{2}/(4\rho_{avg}c_{avg}^{2})=(v_{a}^{2}\rho_{avg})/4 is the acoustic energy density, Z=ρ0c0Z=\rho_{0}c_{0} denotes impedance, c0c_{0} denotes background (zeroth-order) speed of sound in a medium, Z^=Z/zavg\hat{Z}=Z/z_{avg}, c^0=c0/cavg\hat{c}_{0}=c_{0}/c_{avg} and ρ^0=ρ0/ρavg\hat{\rho}_{0}=\rho_{0}/\rho_{avg}, where the subscript ’avg’ denotes the respective average quantities of fluid A and B.

Refer to caption
Figure 1: Inhomogeneous fluids (of different impedance ZAZ_{A} and ZBZ_{B}) separated by a plane interface subjected to a standing acoustic half-wave. In the absence of interfacial tension, the fluid system (a) is in an unstable equilibrium, (b) is in a stable equilibrium, (c) is in neutral equilibrium and (d) is in non-equilibrium state. In the presence of interfacial tension, the fluid system (a) is in a conditionally stable equilibrium, (b) is in stable equilibrium, (c) is in stable equilibrium and (d) is in a conditionally stable equilibrium. Note: (d) is not in the scope of this work.

2.1 Stability analysis of inhomogeneous fluids in the absence of interfacial tension

A two-dimensional fluid domain subjected to a standing acoustic half-wave in the X-direction, with two fluids separated by a sharp vertical interface as shown in figure 1.a-c is considered for the stability analysis. Before beginning the analysis, it is necessary to understand the equilibrium of the system in the absence of interfacial tension. In a completely enclosed domain, a fluid initially at rest (V=0\textbf{\emph{V}}=0) will remain at rest (or equilibrium) if the body force can be completely absorbed in pressure, frl=P\textbf{\emph{f}}_{rl}=\bm{\nabla}P from (1b) and (4). By taking the curl of the above relation, the condition for equilibrium is given as ×frl=0\bm{\nabla}\times\textbf{\emph{f}}_{rl}=0. Thus,

Eaczavg[x(cos(2kwx)zy)y(cos(2kwx)zx)]=0.-\frac{E_{ac}}{z_{avg}}\left[\frac{\partial}{\partial x}\left(\cos(2k_{w}x)\frac{\partial z}{\partial y}\right)-\frac{\partial}{\partial y}\left(\cos(2k_{w}x)\frac{\partial z}{\partial x}\right)\right]=0. (5)

It is clear from (5) that the given fluid configuration will be in an equilibrium state, only if the direction of the acoustic standing wave is normal to the fluid-fluid interface (the direction of the acoustic standing wave is parallel to the direction of the impedance gradient) as shown in figure 1(aa-cc). Since ×frl0\bm{\nabla}\times\textbf{\emph{f}}_{rl}\neq 0 for the configuration shown in figure 1(d)(d), it is not in equilibrium and tends to relocate to the stable configuration without any perturbations. The stability nature of the equilibrium configurations is analysed by imposing infinitesimal perturbations on the interface. Now we proceed to show that in the absence of interfacial tension, the configuration shown in figure 1(a)(a) is in unstable equilibrium (perturbations grow), figure 1(b)(b) is in stable equilibrium (perturbations decay), and figure 1(cc) is in neutral equilibrium (perturbations neither grow nor decay).

The effect of viscosity is neglected in the stability analysis, as it governs only the timescale of the phenomenon and does not contribute to the stability criterion. Although the physical properties are non-uniform in an inhomogeneous system, the fluid particles considered in the flow field have constant density ρ\rho, speed of sound cc, and impedance ZZ. Thus, the material derivative of all properties is zero, which includes the incompressibility condition (Dρ/Dt=ρ/t+Vρ=0)(D\rho/Dt=\partial\rho/\partial t+\textbf{\emph{V}}\bm{\cdot\nabla}\rho=0). By combining the incompressibility condition with (1a) and neglecting the viscosity, the governing equations (1) reduce to

Ux+Vy=0,\displaystyle\frac{\partial U}{\partial x}+\frac{\partial V}{\partial y}=0, (6a)
ρDUDt=PxEaccos(2kwx)zavgZx,\displaystyle\rho\frac{DU}{Dt}=-\frac{\partial P}{\partial x}-\frac{E_{ac}\cos({2k_{w}x})}{z_{avg}}\frac{\partial Z}{\partial x}, (6b)
ρDVDt=PyEaccos(2kwx)zavgZy,\displaystyle\rho\frac{DV}{Dt}=-\frac{\partial P}{\partial y}-\frac{E_{ac}\cos({2k_{w}x})}{z_{avg}}\frac{\partial Z}{\partial y}, (6c)
where U,VU,V are the X-component and Y-component of the velocity field V. Since the body force term is a function of impedance, the below impedance relation is required for the closure.
DZDt=Zt+UZx+VZy=0.\frac{DZ}{Dt}=\frac{\partial Z}{\partial t}+U\frac{\partial Z}{\partial x}+V\frac{\partial Z}{\partial y}=0. (6d)

Now, the flow fields are decomposed into an unperturbed zeroth-order stationary state and infinitesimal perturbations as U=u0+δu,V=v0+δv,P=p0+δp,ρ=ρ0+δρU=u_{0}+\delta u,\ V=v_{0}+\delta v,\ P=p_{0}+\delta p,\ \rho=\rho_{0}+\delta\rho and Z=z0+δzZ=z_{0}+\delta z. In this study, the variation of acoustic impedance is considered only in the X-direction (figure 1(aa-cc)), z0=z0(x)z_{0}=z_{0}(x). At the stationary state (u0=v0=0)(u_{0}=v_{0}=0), the unperturbed zeroth-order equations become, p0x=Eaccos(2kwx)zavgz0x\frac{\partial p_{0}}{\partial x}=-\frac{E_{ac}\cos({2k_{w}x})}{z_{avg}}\frac{\partial z_{0}}{\partial x} from 6b, p0x=0\frac{\partial p_{0}}{\partial x}=0 from 6c and z0t=0\frac{\partial z_{0}}{\partial t}=0 from 6d. Using the above zeroth order relations and neglecting the second-order terms in (6), the first-order perturbation equations governing the stability becomes

δux+δvy=0,\displaystyle\frac{\partial\delta u}{\partial x}+\frac{\partial\delta v}{\partial y}=0, (7a)
ρ0δut=δpxEaccos(2kwx)zavgδzx,\displaystyle\rho_{0}\frac{\partial\delta u}{\partial t}=-\frac{\partial\delta p}{\partial x}-\frac{E_{ac}\cos({2k_{w}x})}{z_{avg}}\frac{\partial\delta z}{\partial x}, (7b)
ρ0δvt=δpyEaccos(2kwx)zavgδzy,\displaystyle\rho_{0}\frac{\partial\delta v}{\partial t}=-\frac{\partial\delta p}{\partial y}-\frac{E_{ac}\cos({2k_{w}x})}{z_{avg}}\frac{\partial\delta z}{\partial y}, (7c)
(δz)t=δuz0x.\displaystyle\frac{\partial(\delta z)}{\partial t}=-\delta u\frac{\partial z_{0}}{\partial x}. (7d)

Analysing the disturbances into normal modes, the amplitude of the disturbances δu,δv,δρ,δp,\delta u,\ \delta v,\ \delta\rho,\ \delta p, and δz\delta z takes the following form

A(x,y,t)=A(x)exp(ikyy+nt),A(x,y,t)=A(x)exp(ik_{y}y+nt), (8)

where kyk_{y} is the wavenumber considered along the Y-direction. Applying the above amplitude relations in the form (8) in (7),

δux+ikyδv=0,\displaystyle\frac{\partial\delta u}{\partial x}+ik_{y}\delta v=0, (9a)
ρ0nδu=δpxEaccos(2kwx)zavgδzx,\displaystyle\rho_{0}n\delta u=-\frac{\partial\delta p}{\partial x}-\frac{E_{ac}\cos{\left(2k_{w}x\right)}}{z_{avg}}\frac{\partial\delta z}{\partial x}, (9b)
ρ0nδv=ikyδpikyEaccos(2kwx)zavgδz,\displaystyle\rho_{0}n\delta v=-ik_{y}\delta p-ik_{y}\frac{E_{ac}\cos{\left(2k_{w}x\right)}}{z_{avg}}\delta z, (9c)
nδz=δuz0x.\displaystyle n\delta z=-\delta u\frac{\partial z_{0}}{\partial x}. (9d)

The partial notation is dropped since the only derivatives in (9) are with respect to the xx coordinate. Multiplying by ikyik_{y} throughout (9c) and combining with (9a) and (9d), we obtain,

δp=ρ0nky2dδudx+Eaccos(2kwx)zavgδundz0dx.\delta p=-\rho_{0}\frac{n}{{k_{y}}^{2}}\frac{d\delta u}{dx}+E_{ac}\frac{\cos(2k_{w}x)}{z_{avg}}\frac{\delta u}{n}\frac{dz_{0}}{dx}. (10)

substituting (9d) and (10) in (9b) results in,

ddx(ρ0dδudx)ρ0ky2δu=Eac2kwδuzavgky2n2dz0dxsin(2kwx).\frac{d}{dx}\left(\rho_{0}\frac{d\delta u}{dx}\right)-\rho_{0}k_{y}^{2}\delta u=-E_{ac}\frac{2k_{w}\delta u}{z_{avg}}\frac{k_{y}^{2}}{n^{2}}\frac{dz_{0}}{dx}\sin(2k_{w}x). (11)

Considering two uniform fluids of different impedance ZAZ_{A} and ZBZ_{B} separated by interfaces positioned at xsx_{s},

z0=zA+(zBzA)H(xxs),z_{0}=z_{A}+(z_{B}-z_{A})H(x-x_{s}), (12a)
dz0dx=(zBzA)δ(xxs),\frac{dz_{0}}{dx}=(z_{B}-z_{A})\delta(x-x_{s}), (12b)

where H(xxs)H(x-x_{s}) is the Heaviside step function at x=xsx=x_{s} and δ(xxs)\delta(x-x_{s}) is the Dirac’s δ\delta-function at x=xsx=x_{s}. Substituting (12b) in (11),

ddx(ρ0dδudx)ρ0ky2δu=Eac2kwδuzavgky2n2sin(2kwx)(zBzA)δ(xxs).\frac{d}{dx}\left(\rho_{0}\frac{d\delta u}{dx}\right)-\rho_{0}k_{y}^{2}\delta u=-E_{ac}\frac{2k_{w}\delta u}{z_{avg}}\frac{k_{y}^{2}}{n^{2}}\sin(2k_{w}x)(z_{B}-z_{A})\delta(x-x_{s}). (13)

Equation (13) is the governing differential equation for the stability of inhomogeneous fluids (without interfacial tension). For a uniform region on either side of the interface(s) where there are no discontinuities in the impedance, the governing equation (13) reduces to

d2δudx2ky2δu=0.\frac{d^{2}\delta u}{dx^{2}}-k_{y}^{2}\delta u=0. (14)

The solution of (14) is of the form δu=C1eky(xxs)+C2eky(xxs)\delta u=C_{1}e^{k_{y}(x-x_{s})}+C_{2}e^{-k_{y}(x-x_{s})} where C1,C2C_{1},C_{2} are constants. Since δu\delta u must vanish at the boundaries, we can write the solution as,

δuB=Ceky(xxs)(x<xs),\delta u_{B}=Ce^{k_{y}(x-x_{s})}\quad\quad(x<x_{s}), (15a)
δuA=Ceky(xxs)(x>xs),\delta u_{A}=Ce^{-k_{y}(x-x_{s})}\quad\quad(x>x_{s}), (15b)

where the constant CC in (15) is chosen to ensure continuity in velocity across the interfaces. For the solution at the interface (x=xs)(x=x_{s}), we integrate (13) along infinitesimal distance (dx0)(dx\approx 0), the second term in the left-hand side of the equation is zero and the remaining terms are,

Δ(ρ0dδusdx)=Eac2kwδuszavgky2n2(zBzA)(sin(2kwx)δ(xxs))𝑑x,\Delta\left(\rho_{0}\frac{d\delta u_{s}}{dx}\right)=-E_{ac}\frac{2k_{w}\delta u_{s}}{z_{avg}}\frac{k_{y}^{2}}{n^{2}}(z_{B}-z_{A})\int{\left(\sin(2k_{w}x)\delta(x-x_{s})\right)dx}, (16)

where δus\delta u_{s} is the value of δu\delta u at x=xsx=x_{s}. Using, (15) and the Dirac delta identity f(x)δ(xa)𝑑x=f(a)\int f(x)\delta(x-a)dx=f(a) to solve for eigenvalue nn in (16).

ρA(kyδus)ρB(kyδus)=Eac2kwδuszavgky2n2(zBzA)sin(2kwxs),\rho_{A}(-k_{y}\delta u_{s})-\rho_{B}(k_{y}\delta u_{s})=-E_{ac}\frac{2k_{w}\delta u_{s}}{z_{avg}}\frac{k_{y}^{2}}{n^{2}}(z_{B}-z_{A})\sin(2k_{w}x_{s}), (17)

Rearranging (17), the dispersion relation nn for the stability problem becomes

n=kyρA+ρBϕEac(zBzA)sin(2kwxs).n=\sqrt{\frac{k_{y}}{\rho_{A}+\rho_{B}}\phi E_{ac}(z_{B}-z_{A})\sin(2k_{w}x_{s})}. (18)

where ϕ=2kw/zavg\phi=2k_{w}/z_{avg}. The dispersion relation (18) establishes the acoustic stability criterion when inhomogeneous fluids (without interfacial tension) in a microchannel are subjected to a standing acoustic wave. If the eigenvalue nn is imaginary in (18), then the configuration is in a stable equilibrium and the configuration is in an unstable equilibrium when the eigenvalue nn is real. For a standing acoustic half-wave, in (18), the values of kyρB+ρA,ϕ\frac{k_{y}}{\rho_{B}+\rho_{A}},\phi and EacE_{ac} are always positive. Thus, the sign of zBzAz_{B}-z_{A} (initial configuration of the fluids) and sin(2kwxs)\sin(2k_{w}x_{s}) (relative location of the interface with respect to the standing acoustic wave) decide the nature of the eigenvalue in (18). zBzAz_{B}-z_{A} is positive when high-impedance fluid is present to the right of the interface, and negative when high-impedance fluid is present to the left of the interface. sin(2kwxs)\sin(2k_{w}x_{s}) has a negative value to the left of the node (xsx_{s} is negative), a positive value to the right of the node (xsx_{s} is positive) and zero when the interface coincides with the node (centre of the microchannel) or anti-node (sides of the microchannel) (xs=0)(x_{s}=0).

As per the above arguments, the inhomogeneous system in figure 1(aa) is in an unstable equilibrium as eigenvalue nn is real, and the system in figure 1(bb) is in a stable equilibrium as eigenvalue nn is imaginary. It can be concluded from the above discussion and figures 2(aa-ii) and 2(aa-iiii) that, a system is said to be acoustically stable (unstable) if the initial configuration of the fluids is in such a way that the low (high) impedance fluid is present at the anti-node(s) and the high (low) impedance fluid is present at the node(s). This conclusion is consistent with the demonstration of acoustic relocation of fluids within a microchannel by Deshmukh et al. (2014). For the case where the interface coincides with the node, sin(2kwxs)=0\sin(2k_{w}x_{s})=0. Thus, the system is in a neutral equilibrium (n=0n=0) as shown in figures 1(cc) and 2(aa-iiiiii). The above analysis can be easily extended to an inhomogeneous system consisting of multiple interfaces. In this case, the eigenvalues evaluated at the fluid interfaces govern the nature of the system. Figure 2(bb) shows the stability of two interface systems that are widely used in acoustofluidic applications. It can be seen from figure 2(bb-ii) that when high impedance fluid is at the sides (anti-nodes), the eigenvalue at both the interfaces (IF1(IF_{1} and IF2)IF_{2}) is real and hence the system is in unstable equilibrium. The system is in stable equilibrium in figure 2(bb-iiii), as the eigenvalue at both interfaces is imaginary.

Refer to caption
Figure 2: Different inhomogeneous fluid configurations commonly used in microfluidics and their equilibrium nature. a) Single interface configurations; b) Double interface configurations. Equations (1) and (2) are used to calculate nn for fluids without interfacial tension and with interfacial tension.

2.2 Stability analysis of inhomogeneous fluids in the presence of interfacial tension

Proceeding to solve for immiscible fluids, the effect of surface tension must be accounted for. The discontinuity in impedance occurring in the interfaces (xsx_{s}) is modelled by including the interfacial tension effects in the X momentum equation (9b) as, (Chandrasekhar, 1961)

ρ0nδu=δpxEaccos(2kwx)zavgδzxky2sTδxsδ(xxs).\rho_{0}n\delta u=-\frac{\partial\delta p}{\partial x}-\frac{E_{ac}\cos{\left(2k_{w}x\right)}}{z_{avg}}\frac{\partial\delta z}{\partial x}-k_{y}^{2}\sum_{s}T\delta x_{s}\delta(x-x_{s}). (19)

where TT is the interfacial tension and δxs\delta x_{s} denotes the perturbation of the interfaces and ddtδxs=δusδxs=δusn\frac{d}{dt}\delta x_{s}=\delta u_{s}\implies\delta x_{s}=\frac{\delta u_{s}}{n}. The governing differential equation for stability between inhomogeneous fluids with interfacial tension is obtained similar to the case without interfacial tension, as in the previous §\S 2.1,

ddx(ρ0dδudx)ρ0ky2δu=Eac2kwδuzavgky2n2sin(2kwx)(zBzA)δ(xxs)+ky2n2sky2(Tδus)δ(xxs),\frac{d}{dx}\left(\rho_{0}\frac{d\delta u}{dx}\right)-\rho_{0}k_{y}^{2}\delta u=-E_{ac}\frac{2k_{w}\delta u}{z_{avg}}\frac{k_{y}^{2}}{n^{2}}\sin(2k_{w}x)(z_{B}-z_{A})\delta(x-x_{s})\\ +\frac{k_{y}^{2}}{n^{2}}\sum_{s}{k_{y}^{2}\left(T\delta u_{s}\right)\delta(x-x_{s})}, (20)

Integrating (20) across an infinitesimal distance (dx0dx\approx 0) and solving for the dispersion relation nn,

n=kyρ1+ρ2(ϕEac(zBzA)sin(2kwxs)ky2T).n=\sqrt{\frac{k_{y}}{\rho_{1}+\rho_{2}}\left(\phi E_{ac}(z_{B}-z_{A})\sin(2k_{w}x_{s})-k_{y}^{2}T\right)}. (21)

Equation (21) establishes the acoustic stability criterion when fluids with interfacial tension are subjected to a standing acoustic wave. It can be seen from (21) that the interfacial tension (T)(T) and wavenumber of the perturbation (ky)(k_{y}) play a role in the stability of immiscible fluids.

In the presence of interfacial tension (T>0T>0), the fluid system shown in figure 1(bb) is always stable, as the negative sign of (zBzA)sin(2kwxs)(z_{B}-z_{A})\sin(2k_{w}x_{s}) results in an imaginary eigenvalue nn in (21). Whereas, for the fluid system shown in figure 1(aa), the sign of (zBzA)sin(2kwxs)(z_{B}-z_{A})\sin(2k_{w}x_{s}) is positive in (21). Thus, the system is conditionally stable, and the stability is determined by the relative magnitudes of ϕEac(zBzA)sin(2kwxs)\phi E_{ac}(z_{B}-z_{A})\sin(2k_{w}x_{s}) and ky2Tk_{y}^{2}T. The fluid system (figure 1(aa) becomes unstable (nn is real) if the acoustic force density FrlF_{rl} (ϕEac(zBzA)sin(2kwxs)\phi E_{ac}(z_{B}-z_{A})\sin(2k_{w}x_{s})) dominates (or is greater than) the interfacial force density FintF_{int} (ky2Tk_{y}^{2}T) and becomes stable (nn is imaginary) if the interfacial force density dominates the acoustic force density. For the case where the interface coincides with the node (sin(2kwxs)=0\sin(2k_{w}x_{s})=0 and eigenvalue nn is imaginary) and the system is in a stable equilibrium, as shown in figures 1(cc) and 2(aa-iiiiii).

Now, for conditionally stable configuration, we proceed to find the minimum energy density required to relocate the fluid systems in figures 1(aa) and 2(bb-ii) with interfacial tension (T>0T>0). Since the interface height, hh is finite, this leads to the quantization of the possible modes ky=khn=nπ/hk_{y}=k_{h_{n}}=n\pi/h. The minimum (critical) acoustic energy density (Ecr)(E_{cr}) required to relocate the fluid system is decided by the first conceivable mode, kh1=kh=π/hk_{h_{1}}=k_{h}=\pi/h and the critical acoustic energy density is obtained by limiting the eigenvalue nn to zero in (21). Thus,

Ecr=kh2Tzavgsin(2kwxs)2kw(zBzA).E_{cr}=\frac{k_{h}^{2}Tz_{avg}}{sin(2k_{w}x_{s})2k_{w}(z_{B}-z_{A})}. (22)

If the applied energy density EacE_{ac} is less than the critical energy density EcrE_{cr} (Eac<EcrE_{ac}<E_{cr}), the interfacial tension succeeds in stabilizing a potentially unstable configuration. The same system becomes unstable and eventually relocates to a stable configuration when Eac>EcrE_{ac}>E_{cr}. The above discussions on the equilibrium nature of different inhomogeneous fluid configurations (with and without interfacial tension) are clearly summarised in figure 2.

3 Numerical results and discussion

In this section (§\S 3), we numerically analyze the stability of inhomogeneous fluids (with and without interfacial tension) under acoustic fields and compare them with the results obtained by the theoretical analysis in the previous section (§\S 2). At first, we study the stability and relocation using acoustic relocation force frl\textbf{\emph{f}}_{rl} (4) where the acoustic energy density is assumed to be constant (as the variation of first-order pressure and velocity are not considered). We further extend the numerical analysis using the generalized acoustic body force fac\textbf{\emph{f}}_{ac} (2) where the first-order pressure and velocity vary during relocation (thus EacE_{ac} varies) (Rajendran et al., 2022).

The numerical analysis is carried out on a two-dimensional fluid domain of height h=160μmh=160\ \mu m and width w=360μmw=360\ \mu m in COMSOL Multiphysics 6.0. For this study, the fluids mineral oil (Z=1.23MPas/m)(Z=1.23\ MPa\ s/m) and silicone oil (Z=0.961MPas/m)(Z=0.961\ MPa\ s/m) are used. A mesh refinement procedure, similar to those employed by Rajendran et al. (2022) is used to confirm that the numerical findings are not affected by grid size. Three different fluid configurations are considered for the study, namely,

  • High-Low-High (HLH) configuration where the high impedance fluid is present at the anti-nodes (sides) and the low impedance fluid is present at the node (center) as shown in figure 3(aa).

  • Low-High-Low (LHL) configuration where the low impedance fluid is present at the anti-nodes (sides) and the high impedance fluid is present at the node (center) as shown in figure 3(bb).

  • High-Low (HL) configuration where the high impedance fluid occupies the domain to the left of the center of the microchannel and the low impedance fluid occupies the domain to the right of the center of the microchannel as shown in figure 3(cc).

For the sake of brevity, the configurations shown in figures 2(aa-ii) (or 1) and 2(aa-iiii) are not discussed explicitly as their stability and relocation are captured by HLH and LHL configurations. The Low-High (LH) configuration is also not discussed, as it would be analogous to the HL configuration. For all the analyses, the initial interface is perturbed and modelled as xs(y)=A0cos(2πhy+h2)x_{s}(y)=A_{0}\cos\left(\frac{2\pi}{h}y+\frac{h}{2}\right), where A0=0.01hA_{0}=0.01h is the perturbation amplitude.

Refer to caption
Figure 3: Stabilization and relocation of inhomogeneous fluids using simplified body force (4) with constant EacE_{ac} - (a) High-Low-High (HLH) configuration, (b) Low-High-Low (LHL) configuration, (c) High-Low (HL) configuration

3.1 Numerical analysis of stability using constant acoustic energy density

For the numerical simulations shown in 3, we employ equation (4) as body force and assumed EacE_{ac} to be constant throughout the relocation process. The boundary condition for the analysis is no slip at the walls and the pressure is constrained at a point (bottom left corner of the channel). In the absence of interfacial tension (T=0mN/m)(T=0\ mN/m), it is observed that for any Eac>0E_{ac}>0, the HLH configuration undergoes relocation to a stable LHL configuration as in figure 3(aa) (the simulation is shown for EacE_{ac} =80=80 J/m3J/m^{3}). In this case, the magnitude of EacE_{ac} only influences the timescale of the relocation process by competing with the viscosity. While, in the presence of interfacial tension, T=1mN/mT=1\ mN/m, the HLH fluid configuration remained stable for all energy densities below 88J/m388\ J/m^{3}, and relocation is observed for all energy densities above 89J/m389\ J/m^{3}. These simulations are in close agreement with the critical acoustic energy density Ecr=88.78J/m3E_{cr}=88.78\ J/m^{3} predicted by (22) for mineral-silicon oil combination. Simulation results of other fluid combinations shown in figure 5 also agree with (22). When the applied EacE_{ac} is just above EcrE_{cr}, the fluids take a much longer time to relocate. Thus for convenience, the simulation is shown for Eac=120J/m3E_{ac}=120\ J/m^{3} in figure 3(aa).

For LHL configuration with and without interfacial tension (T0T\geq 0), for any Eac>0E_{ac}>0, the relocation of fluid is not observed, and the system remained stable as shown in figure 3(bb) (the simulation is shown for EacE_{ac} =120=120 J/m3J/m^{3}). In the HL configuration, the node of the standing acoustic half-wave coincides with the fluid-fluid interface. Here for fluids with interfacial tension, relocation is not observed for any Eac>0E_{ac}>0, and the fluid system remained stable (figure 3(cc)). Whereas, for fluids without interfacial tension, the HL configuration is observed to be in neutral equilibrium (figure 3(cc)). These simulation results of unstable, stable, and neutral equilibrium of inhomogeneous fluids (figure 3) are in agreement with the stability criteria (from (18) and (21)) that we established theoretically in §\S 2.

3.2 Numerical analysis of stability using generalized body force fac\textbf{f}_{ac}

Refer to caption
Figure 4: Stabilization and relocation of inhomogeneous fluids using generalized body force facf_{ac} (2) along with the first-order pressure field (|p1|=Real(p1p1)|p_{1}|=\sqrt{Real(p_{1}^{\star}p_{1})}) for different fluid configurations. 1-D actuation is imposed on (a-c), and 2-D actuation is imposed on (d). (a) HLH configuration remained stable up to Eac=85.58J/m3E_{ac}=85.58\ J/m^{3} (pa=0.67MPap_{a}=0.67\ MPa, d0d_{0} = 0.210.21 nmnm, ν=\nu= 1.731.73 MHzMHz). (b) HLH configuration undergoes relocation above Eac=86.22E_{ac}=86.22 J/m3J/m^{3} (pa=0.69MPap_{a}=0.69\ MPa, d0d_{0} = 0.220.22 nmnm, ν=\nu= 1.731.73 MHzMHz). Significant variation in |p1||p_{1}| during relocation is observed. (c) HL configuration where the fluid interface coincides with the node remained in stable equilibrium even at Eac=2334J/m3E_{ac}=2334\ J/m^{3} (pa=3.54MPap_{a}=3.54\ MPa, d0d_{0} = 2020 nmnm, ν=\nu= 1.731.73 MHzMHz). (d) Relocation of HL configuration due to 2-D wall actuation (pa=1.37MPa,d0=20nm,ν=2.1MHz)(p_{a}=1.37\ MPa,\ d_{0}=20\ nm,\ \nu=2.1\ MHz)

Thus far, in the theoretical stability analysis (§\S 2) as well as in the numerical simulations (§\S 3.1), a simplified equation frl\textbf{\emph{f}}_{rl} (4) is employed as a body force with the assumption of constant EacE_{ac} (the amplitudes of first-order fields pap_{a} and vav_{a} do not vary during relocation). In this section, the generalized acoustic body force fac\textbf{\emph{f}}_{ac} (2) is employed and the first-order fields required to calculate the above fac\textbf{\emph{f}}_{ac} are obtained from the wave equations (frequency domain - see appendix A) by actuating the channel walls at a frequency ν\nu with a wall displacement d0d_{0}. There are two reasons for using generalized acoustic body force fac\textbf{\emph{f}}_{ac}: 1. To show the relocation predicted by frl\textbf{\emph{f}}_{rl} and fac\textbf{\emph{f}}_{ac} is approximately the same. When we use much simpler frl\textbf{\emph{f}}_{rl} instead of the complex fac\textbf{\emph{f}}_{ac}, the first-order field equations are not required to be solved which will significantly reduce the computation time for simulation of relocation of inhomogeneous fluids. 2. To explain the previous microchannel experiments in immiscible fluid relocation (Hemachandran et al., 2019).

For one-directional (1-D) standing half-wave simulations, the sidewalls are actuated in phase at a displacement d0d_{0} at a frequency ν\nu. In laminar flow equations, the boundary conditions used are no-slip at all walls, and the pressure is constrained at a point (bottom left corner of the channel). To disregard the effect of streaming, the first-order acoustic fields (see Appendix A) are allowed to slip in the frequency domain.

Figure 6(aa), shows the HLH configuration subjected to 1-D standing half-wave by actuating sidewalls at a displacement d0d_{0} of 0.210.21 nmnm and a frequency ν\nu of 1.73MHz1.73\ MHz. In this case, it is observed that the resulting pressure amplitude PaP_{a} of 0.67MPa0.67\ MPa (EacE_{ac} = 85.58J/m385.58\ J/m^{3}), could not relocate the fluids in the HLH configuration and thus remains stable. Whereas, when the displacement is increased to 0.220.22 nmnm, the resulting pressure amplitude of Pa=0.69MPaP_{a}=0.69\ MPa (EacE_{ac} = 86.22J/m386.22\ J/m^{3}), could relocate the HLH configuration to a stable equilibrium as shown in figure 6(bb). From the above discussion, the critical acoustic energy density is found to be EcrE_{cr} = 85.9±0.3285.9\ \pm 0.32 J/m3J/m^{3}. This value of EcrE_{cr} obtained through generalized body force fac\textbf{\emph{f}}_{ac} is in close agreement (deviation of 3.24%3.24\%) with the simplified relocation force frlf_{rl} employed to derive stability criterion (§\S 2).

In the case of a 1-D standing half-wave, when the interface of the fluid coincides with the pressure node (xs=0x_{s}=0), for any EacE_{ac}, relocation is not observed using both fac\textbf{\emph{f}}_{ac} and frl\textbf{\emph{f}}_{rl} (figures 3(cc) and 4(cc) as predicted by the stability criteria (21). However, Hemachandran et al. (2019) through experiments demonstrated the relocation of fluids irrespective of the location of the vertical interface xsx_{s}. In their experiments, the frequency employed (2.12.1 MHzMHz) is far from the 1-D resonant half-wave frequency (ν\nu = 1.61.6 MHzMHz \approx cavg/2wc_{avg}/2w). In our previous work (Rajendran et al., 2022), we have shown that the above relocation is due to standing two-directional (2-D) acoustic wave (frequency ff == 2.1MHz2.1\ MHz between cavg/2wc_{avg}/2w and cavg/2hc_{avg}/2h) as shown in figure 4(dd). From figure 4(dd) it is clear that the pressure node is not vertical but inclined with respect to the fluid interface owing to the 2-D actuation (all four walls are actuated at d0d_{0}). The above 2-D relocation can be clearly explained by the fact that if the fluid interface and node are not perpendicular to each other, then ×frl\bm{\nabla}\times\textbf{\emph{f}}_{rl} 0\neq 0. This implies when a sufficient energy density is applied, the fluid system 4(dd) will not be in equilibrium and relocation begins without imposing any perturbations unlike the other relocation discussed in this work.

3.3 Characterization of stable and unstable (relocation) regime

When the 1-D acoustic standing wave is imposed on fluids with interfacial tension, the configurations (figures 1(bb), 2(bb-ii), 3(aa) having high impedance fluid at the anti-node and the low impedance fluid at the node, become conditionally stable. From (21), it is evident that the stability of the above inhomogeneous fluid configurations is governed by the ratio of FrlF_{rl} and FintF_{int}, which is called as acoustic Bond number (BoaBo_{a}), given by

Boa=FrlFint=ϕEacΔZsin(2kwxs)kh2TBo_{a}=\frac{F_{rl}}{F_{int}}=\frac{\phi E_{ac}\Delta Z\sin\left(2k_{w}x_{s}\right)}{k_{h}^{2}T} (23)

The BoaBo_{a} that separates the stable and unstable region is called critical acoustic Bond number Boa,crBo_{a,cr}. From (21)

Boa,cr=1Bo_{a,cr}=1 (24)

For Boa>Boa,crBo_{a}>Bo_{a,cr}, the above configurations become unstable (relocation occurs), and for Boa<Boa,crBo_{a}<Bo_{a,cr} the configurations remain stable. Figure 5 shows the simulation results of different immiscible fluid combinations. The relocation and non-relocation regimes predicted by the simulations are in line with (24). It must also be noted that the fluids with higher interfacial tension require a higher acoustic force for relocation.

Refer to caption
Figure 5: Characterization of relocation and non-relocation regimes of immiscible fluids using acoustic Bond number BoaBo_{a}

3.4 Effect of the height of the channel on stability

Refer to caption
Figure 6: Effect of channel height on stability, (a) channel height h=80μmh=80\ \mu m - no relocation is observed as applied energy density (Eac=120J/m3)(E_{ac}=120\ J/m^{3}) is less than the critical energy density (Ecr=384J/m3)(E_{cr}=384\ J/m^{3}), (b) channel height h=160μmh=160\ \mu m - relocation is observed as applied energy density (Eac=120J/m3)(E_{ac}=120\ J/m^{3}) is high than the critical energy density (Ecr=88.78J/m3)(E_{cr}=88.78\ J/m^{3}). This demonstrates that the interfacial tension force weakens as the height of the channel increases and thus higher the height of the channel, the lower the EacE_{ac} required for relocation as (Ecr1/h2)(E_{cr}\propto 1/h^{2}).

The height of the channel hh plays a critical role in the stability of immiscible fluids. For a given EacE_{ac}, the increase in hh weakens the stabilizing effect of interfacial tension force, as analysed theoretically in §\S 2. From (22), it can be inferred that the critical acoustic energy density is inversely proportional to the square of the channel height (Ecr1/h2)(E_{cr}\propto 1/h^{2}). In figure 6(aa), for a microchannel of height h=80μmh=80\ \mu m consisting of mineral-silicone oil with interfacial tension T=1mN/mT=1\ mN/m, the fluid system is stable as the applied Eac(120J/m3E_{ac}\ (120\ J/m^{3}) is lower than the critical energy density (Ecr=384J/m3E_{cr}=384\ J/m^{3}). Whereas for h=160μmh=160\ \mu m and keeping the remaining parameters same, fluid relocation is observed as applied Eac(120J/m3)E_{ac}\ (120\ J/m^{3}) is higher than the critical energy density (Ecr=88.78J/m3)(E_{cr}=88.78\ J/m^{3}).

The above discussion on the effect of channel height on acoustic relocation has high relevance in practical applications. To relocate fluids with high interfacial tension of 𝒪(101102)\mathcal{O}(10^{1}-10^{2}) mN/mmN/m, in commonly used acoustofluidic channels of height ranging from 100μm100\ \mu m to 200μm200\ \mu m, the required EacE_{ac} becomes 𝒪(104)J/m3\approx\mathcal{O}(10^{4})\ J/m^{3}, which is very high compared to the EacE_{ac} employed in typical acoustofluidic experiments (𝒪(102103)\mathcal{O}(10^{2}-10^{3}) J/m3J/m^{3}). The equation (22) tells that the above problem can be solved by increasing the channel height as Eac1/h2E_{ac}\propto 1/h^{2}. Hence, the depth (height) of the channel is a crucial aspect to be considered during the fabrication of an acoustofluidic microchannel for handling high interfacial tension fluids.

4 Conclusion

We have theoretically established the stability criteria for inhomogeneous fluids subjected to standing acoustic fields, which is consistent with the previous experimental investigations on miscible (Deshmukh et al., 2014), (Karlsen et al., 2016), and immiscible fluids (Hemachandran et al., 2019). Numerical simulations on the same were carried out using simplified and generalized body force to understand the various parameters that contribute towards stability and relocation of fluids. However, the effect of boundary layer-driven streaming on relocation is neglected in this work, which will be addressed in an upcoming paper. The insights gained from this study can have potential applications in inhomogeneous fluid handling and particle manipulation in the field of acoustofluidics.

Appendix A First-order fields in the frequency domain

The first-order fields (fast timescale) on the frequency domain are written as

iωρ1=(ρ0v1)-i\omega\rho_{1}=\bm{\nabla}\cdot(\rho_{0}\textbf{\emph{v}}_{1}) (25a)
iωρ0v1=p1+η2v1+βη(v1)+fac-i\omega\rho_{0}\textbf{\emph{v}}_{1}=-\bm{\nabla}p_{1}+\eta\nabla^{2}\textbf{\emph{v}}_{1}+\beta\eta\bm{\nabla}(\bm{\nabla\cdot}\textbf{\emph{v}}_{1})+\textbf{\emph{f}}_{ac} (25b)
iωρ0κ0p1=iωρ1+v1ρ0-i\omega\rho_{0}\kappa_{0}p_{1}=-i\omega\rho_{1}+\textbf{\emph{v}}_{1}\cdot\nabla\rho_{0} (25c)
Also, combining equations (25a & 25c) we get
iωκ0p1=v1-i\omega\kappa_{0}p_{1}=-\nabla\cdot\textbf{\emph{v}}_{1} (25d)

where p1p_{1} is the first-order pressure field, ρ1\rho_{1} refers to first-order density field, v1\textbf{\emph{v}}_{1} is the first-order velocity field, ω\omega is the angular frequency, η\eta is the dynamic viscosity of the fluid, ξ\xi is the volume fluid viscosity, β=(ξ/η)+(1/3)\beta=(\xi/\eta)+(1/3), facf_{ac} is generalised body force and ZZ is impedance. The detailed analysis of first-order and second-order fields acting on inhomogeneous fluids is given in Rajendran et al. (2022).

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