alphaFeedback

You’re reading v1 — jump to latest

WorksPhysics and Astronomy

Kinematic and rheological equivalence of steady shearing and planar extensional flows

AI contributions
Not recorded for this paper
View details

Abstract

Steady shearing and planar extension are commonly viewed as two distinct types of flow field, especially in the context of probing the rheology of complex fluids. By leveraging the kinematic equivalence between the two flows, we derive an effective extension rate experienced by a material element which removes the rotational component of the shearing flow. This enables reconstruction of the steady planar extensional viscosity of an unknown fluid using only material functions measured in a steady shearing flow, revealing a deep rheological equivalence between the two deformation histories. We demonstrate this equivalency through phenomenological and microscopically motivated frame-invariant constitutive models as well as using experimental data obtained with a viscoelastic polymer solution and a polymer melt.

The nonlinear canonical rheology of complex fluids is typically characterized in homogeneous flow fields such as simple shear and pure extension. These two flows probe different aspects of the microstructure through different stretch histories, and in general, one cannot be predicted from the other [1, 2]. Although shear flows are routinely employed in a torsional rheometer to obtain material functions such as the shear viscosity and the first normal stress coefficient, steady extensional flows have been more difficult to achieve [3]. Nevertheless, extensional flows are essential for understanding many polymer processing operations [4], as well as filament breakup [5], fracture [6] and jetting phenomena [7]. Furthermore, in flows with mixed kinematics, the extensional component will often dominate at high strain rates [8].

It is commonly assumed that planar elongation probes nonlinear material responses that are independent of those probed by shearing deformations [9]. However, generating true planar extensional flows has posed a major challenge experimentally, especially compared to implementing uniaxial or biaxial extensional deformations. Various devices have been developed for generating uniaxial elongation, though these deformations are typically transient and inhomogeneous. Examples include the use of converging flows [9] or the rotating clamp Meissner apparatus [10] for viscous polymer melts, and filament stretching configurations [5] such as Dripping onto Substrate [11], and jetting devices such as ROJER [7] for less viscous materials. The only bespoke devices able to generate planar extensional flow for dilute polymer solutions are the OSCER microfluidic device [12] and a modified filament stretching device [13]. The difficulties in generating planar extensional flow, especially at sufficiently high extension rates to achieve large microstructural deformations, have led to few published studies.

More broadly, flow fields can be classified kinematically using invariants of frame-invariant tensors such as the strain rate γ˙\dot{\boldsymbol{\gamma}} and the Finger strain B\mathbf{B}. Because of fluid incompressibility, the first invariant of γ˙\dot{\boldsymbol{\gamma}} is zero, and the third invariant of B\mathbf{B} is always unity. The remaining two invariants for each tensor thus form two separate maps of all physically realizable flows. Such maps were first put forth by Sawyers [14] in terms of the Finger strain tensor, and have been popularized by Chong, Perry and Cantwell [15] for classifying turbulent flow fields in terms of the strain rate tensor. Both representations are featured in the classic textbook by Bird et al. [16] and are summarized in the SI. These maps are bounded by uniaxial and biaxial extensional flows, but interestingly, simple shear flow and planar extension reside on the same invariant lines and are thus kinematically indistinguishable. This raises a more fundamental question about whether a mapping exists between steady shear material functions and the steady planar extensional viscosity. In this Letter, we show that for any materially objective constitutive equation, the steady planar extensional viscosity can be completely determined from the steady shear viscosity and the first normal stress difference. This relationship reveals that the two flows, although ostensibly distinct, are kinematically equivalent. Our key development is to systematically remove the contribution of rotation from the shearing flow, by defining an “effective extension rate” to establish this equivalence. This establishes an accessible route to infer steady planar extensional behavior from steady shear measurements alone, and opens avenues for understanding the physics inherent in a complex fluid subjected to two flows previously thought to be distinct.

In a recent study, Hillebrand et al. [17] have shown that suspensions of elastic discs and solutions of long flexible polymers, described respectively by the Oldroyd-A and Oldroyd-B models, produce identical velocity fields in any planar 2D flow. Our finding builds on this development, since both constitutive models generate identical shear stress and first normal stress differences in shear flow, and we show more broadly that the rheological material functions defined in planar extensional flows are kinematically connected to those in steady shear flow, once the rate of rotation has been accounted for.

By symmetry arguments, the extra stress tensor σ\boldsymbol{\sigma} in any planar flow (i.e. including simple shear and planar extensional flow) has the following form:

σ=(σ11σ120σ12σ22000σ33)(1)\boldsymbol{\sigma} = \begin{pmatrix} \sigma_{11} & \sigma_{12} & 0 \\ \sigma_{12} & \sigma_{22} & 0 \\ 0 & 0 & \sigma_{33} \end{pmatrix} \tag*{(1)}

Meaningful material functions are always defined in terms of the system’s response (i.e. the output) divided by a measure of the imposed deformation history (input) [18]. For steady shear, we define 1 as the flow direction and 2 as the velocity gradient direction (Figure 1a). The only non-zero component of the velocity field is v1=γ˙x2v_1 = \dot{\gamma}x_2. Hence, the shear viscosity is defined as η(γ˙)≡σ12/γ˙\eta(\dot{\gamma}) \equiv\sigma_{12}/\dot{\gamma}, and rheologists also measure the first normal stress difference N1=σ11−σ22N_1 = \sigma_{11} - \sigma_{22} and the second normal stress difference N2=σ22−σ33N_2 = \sigma_{22} - \sigma_{33}. For steady homogeneous planar extensional flow, we define 1 as the extension direction and 2 as the compression direction (Figure 1b). The velocity field has two non-zero components v1=ϵ˙x1v_1 = \dot{\epsilon}x_1 and v2=−ϵ˙x2v_2 = -\dot{\epsilon}x_2. The steady planar extensional viscosity is defined by ηP1(ϵ˙)≡(σ11−σ22)/ϵ˙\eta_{P1}(\dot{\epsilon}) \equiv(\sigma_{11} - \sigma_{22})/\dot{\epsilon}. For completeness, we also define a second planar extensional viscosity ηP2(ϵ˙)≡(σ33−σ22)/ϵ˙\eta_{P2}(\dot{\epsilon}) \equiv(\sigma_{33} - \sigma_{22})/\dot{\epsilon}. Note that from symmetry arguments based on reversing the flow direction (such that γ˙→−γ˙\dot{\gamma} \to-\dot{\gamma} or ϵ˙→−ϵ˙\dot{\epsilon} \to-\dot{\epsilon}), we expect that the normal stress difference N1N_1 in steady shear is an even function of the applied shear rate, (σ11−σ22)∼γ˙2(\sigma_{11} - \sigma_{22}) \sim\dot{\gamma}^{2}, whereas the corresponding quantity in planar extensional flow is an odd function of the imposed extension rate, i.e. (σ11−σ22)∼ϵ˙(\sigma_{11} - \sigma_{22}) \sim\dot{\epsilon} [16].

Schematic of stresses and principal axes in steady shear and planar extensional flow

Figure 1. (a) The different stresses σ11\sigma_{11}, σ22\sigma_{22} and σ12\sigma_{12} acting on a fluid element in steady shear flow. The principal stresses σ1(t)\sigma_1(t) and σ2(t)\sigma_2(t) and their corresponding eigenvectors e1′\mathbf{e}'_1 and e2′\mathbf{e}'_2 are shown at an arbitrary time tt for a given flow strength γ˙\dot{\gamma}. (b) The principal stresses σ1\sigma_1 and σ2\sigma_2 at time tt in a planar extensional flow. The orientation of the eigenvectors do not evolve in time. (c) A schematic depicting the projection of the imposed strain rate onto the principal axes of stress in shear flow for two different flow strengths γ˙1\dot{\gamma}_1, γ˙2\dot{\gamma}_2. The principal stress difference at each instance is Δσ=σ1−σ2=N12+4σ122\Delta\sigma= \sigma_1-\sigma_2 = \sqrt{N_1^2 + 4\sigma_{12}^2}.

The extra stress tensor for any planar flow can also be expressed in terms of three principal stresses σ1\sigma_1, σ2\sigma_2 and σ3\sigma_3 when rotated into its principal axes:

σ′=(σ1000σ2000σ3)(2)\boldsymbol{\sigma}' = \begin{pmatrix} \sigma_1 & 0 & 0 \\ 0 & \sigma_2 & 0 \\ 0 & 0 & \sigma_3 \end{pmatrix} \tag*{(2)}

In planar extensional flow, the stress tensor is already diagonal since σ12=0\sigma_{12} = 0, hence σ1=σ11\sigma_1 = \sigma_{11}, σ2=σ22\sigma_2 = \sigma_{22} and σ3=σ33\sigma_3 = \sigma_{33}. It is frequently described by rheologists as a ‘shear-free’ flow [16], but is also referred to as ‘pure shear’ by solid mechanicians [19]. In simple shear flow, the eigenvalues of σ\boldsymbol{\sigma} are [20]:

σ1=12(σ11+σ22+(σ11−σ22)2+4σ122)(3)\sigma_1 = \frac{1}{2}\left(\sigma_{11} + \sigma_{22} + \sqrt{(\sigma_{11} - \sigma_{22})^2 + 4\sigma_{12}^2}\right) \tag*{(3)}
σ2=12(σ11+σ22−(σ11−σ22)2+4σ122)(4)\sigma_2 = \frac{1}{2}\left(\sigma_{11} + \sigma_{22} - \sqrt{(\sigma_{11} - \sigma_{22})^2 + 4\sigma_{12}^2}\right) \tag*{(4)}
σ3=σ33(5)\sigma_3 = \sigma_{33} \tag*{(5)}

When shearing deformations are expressed in this coordinate frame, we can define a principal stress difference Δσ≡(σ1−σ2)=N12+4σ122\Delta\sigma\equiv(\sigma_1-\sigma_2) = \sqrt{N_1^2 + 4\sigma_{12}^2} (see Figure 1c). As the shear flow strength increases, the microstructure becomes increasingly aligned with the 1 direction, and this can be quantified by an orientation angle χ=12tan⁡−1(2σ12/N1)\chi= \frac{1}{2}\tan^{-1}(2\sigma_{12}/N_1) that decreases from 45∘45^\circ towards 0∘0^\circ [20].

The question is thus: can we define a composite viscosity function that maps the material responses determined in shear and is consistent with the true planar extensional viscosity ηP1=(σ11−σ22)/ϵ˙\eta_{P1} = (\sigma_{11} - \sigma_{22})/\dot{\epsilon} defined in Figure 1?

To answer this question, we define an effective extension rate ϵ˙eff\dot{\epsilon}_{\mathrm{eff}} by projecting the imposed deformation rate field onto the evolving principal axes of the resulting stress tensor. For general deformations, the symmetric strain rate tensor is defined as γ˙=∇v+∇vT\dot{\boldsymbol{\gamma}} = \nabla\mathbf{v} + \nabla\mathbf{v}^{T}, in which ∇v\nabla\mathbf{v} is the velocity gradient tensor. In planar extensional flow, this tensor is diagonal and can be expressed compactly as γ˙=2ϵ˙e1e1−2ϵ˙e2e2\dot{\boldsymbol{\gamma}} = 2\dot{\epsilon}\mathbf{e}_1\mathbf{e}_1 - 2\dot{\epsilon}\mathbf{e}_2\mathbf{e}_2. Therefore, the eigenvectors of the strain rate tensor and the stress tensor (cf. Eq. 2) are always coincident and fixed with time. On the other hand, the strain rate tensor in simple shear is γ˙=γ˙e1e2+γ˙e2e1\dot{\boldsymbol{\gamma}} = \dot{\gamma}\mathbf{e}_1\mathbf{e}_2 + \dot{\gamma}\mathbf{e}_2\mathbf{e}_1. As we show schematically in Figure 1c, the eigenvectors of the strain rate tensor are always fixed in time (even in a transient shear experiment) and rotated 45∘45^\circ anticlockwise from the flow axis e1\mathbf{e}_1. However, the eigenvectors of the stress tensor change their orientation at a rate that is dependent on the evolution of the stress field given by the material’s constitutive response. The full expressions for the time-dependent eigenvectors of the stress tensor are provided in the SI. Since the principal axes of the strain rate tensor and the principal axes of the stress tensor are not coincident, the proper way to define the effective extension rate that is aligned in the direction of the stress is to find the projection of the imposed deformation rate onto the direction of the principal axes of the stress tensor, as we sketch in Figure 1c.

We define the normalized eigenvectors of the stress tensor as e1′e'_1, e2′e'_2, and e3′e'_3. By rotating the strain rate tensor into this coordinate frame and extracting the 11 component of the resultant tensor, the “effective extension rate” can be shown to be (see details in the SI):

ϵ˙eff=12e1′⋅γ˙⋅e1′=γ˙σ12Δσ(6)\dot{\epsilon}_{\mathrm{eff}} = \frac{1}{2} \mathbf{e}'_1 \cdot\dot{\boldsymbol{\gamma}} \cdot\mathbf{e}'_1 = \frac{\dot{\gamma}\sigma_{12}}{\Delta\sigma} \tag*{(6)}

This is the main finding of this Letter. The factor of 1/2 arises because we constrain the “flow strength”, measured by the second invariant of the strain rate tensor, to be equivalent for both simple shear flow and planar extension. In simple shear flow, IIγ˙=tr⁡(γ˙2)=2γ˙2II_{\dot{\gamma}} = \operatorname{tr}(\dot{\gamma}^2) = 2\dot{\gamma}^2, while in a general planar extension, IIγ˙=8ϵ˙2II_{\dot{\gamma}} = 8\dot{\epsilon}^2. Equating the two flow strengths, for internal consistency we have ϵ˙eff=γ˙/2\dot{\epsilon}_{\mathrm{eff}} = \dot{\gamma}/2.

This effective extension rate ϵ˙eff\dot{\epsilon}_{\mathrm{eff}} now isolates the stretching component of the shear flow projected onto a deforming material element at time tt by removing the vorticity inherent to a simple shearing deformation. This then leads to a proper definition of an equivalent composite planar extensional viscosity:

η[P1]≡σ1−σ2ϵ˙eff=N12+4σ122γ˙σ12=4η(γ˙)[1+(N12σ12)2](7)\eta_{[P1]} \equiv\frac{\sigma_1-\sigma_2}{\dot{\epsilon}_{\mathrm{eff}}} = \frac{N_1^2+4\sigma_{12}^2}{\dot{\gamma}\sigma_{12}} = 4\eta(\dot{\gamma})\left[1+\left(\frac{N_1}{2\sigma_{12}}\right)^2\right] \tag*{(7)}

where we have substituted η(γ˙)≡σ12/γ˙\eta(\dot{\gamma}) \equiv\sigma_{12}/\dot{\gamma} in the last equality. We show that when this new composite function is plotted against the effective extension rate, we can completely reconstruct the a priori unknown steady planar extensional viscosity curve, using only steady shear data.

An expression for the second planar extensional viscosity can also be obtained by dividing the appropriate principal stress difference by the effective extension rate:

η[P2]≡σ3−σ2ϵ˙eff=(Δσ)(−N1−2N2+Δσ)2γ˙σ12(8)\eta_{[P2]} \equiv\frac{\sigma_3-\sigma_2}{\dot{\epsilon}_{\mathrm{eff}}} = \frac{(\Delta\sigma)(-N_1-2N_2+\Delta\sigma)}{2\dot{\gamma}\sigma_{12}} \tag*{(8)}

However, Petrie [21] has shown that ηP2\eta_{P2} becomes vanishingly small compared to ηP1\eta_{P1} in planar extension for most rheological models. Furthermore, it is more difficult to measure N2N_2 in a rheometer [22] especially since its magnitude is often much smaller than N1N_1. In view of these limitations, the rest of this Letter focuses on the dominant planar extensional viscosity η[P1]\eta_{[P1]}. Further results on η[P2]\eta_{[P2]} are provided in the SI.

Inelastic fluids exhibit no normal stress differences, N1=N2=0N_1 = N_2 = 0. In the Newtonian limit, σ12=η0γ˙\sigma_{12} = \eta_0\dot{\gamma} in shear flow, and the planar extensional viscosity η[P1]\eta_{[P1]} predicted from (7) is four times the shear viscosity η0\eta_0, in agreement with the well-known Trouton ratio Tr=ηP1/η0=4Tr = \eta_{P1}/\eta_0 = 4 in planar extensional flow. Similarly, due to its inelasticity (N1→0N_1 \to0), a generalized Newtonian fluid will always have a planar extensional viscosity that is four times the shear viscosity, even if it shear thins. Numerical simulations on a suspension of solid spherical particles, which flows like an inelastic fluid, in planar extension [23] have also shown that the Trouton ratio remains at four at large extension rates.

With the insight of (7), we are able to replicate the steady state planar extensional viscosity curves for a wide range of constitutive models. We first show that this composite material function is valid for a phenomenological nonlinear model based on polymer network formation and destruction, the Phan-Thien Tanner (PTT) model [24]. Specifically, the linear PTT model has similarities to the widely used FENE-P model for polymer solutions when the flows are steady [25]. It has the equation:

σ▽+(1+ετη0tr⁡(σ))σ=η0γ˙(9)\overset{\triangledown}{\boldsymbol{\sigma}} + \left(1+\frac{\varepsilon\tau}{\eta_0}\operatorname{tr}(\boldsymbol{\sigma})\right)\boldsymbol{\sigma} = \eta_0\dot{\boldsymbol{\gamma}} \tag*{(9)}

where the operator (⋅▽\overset{\triangledown}{\cdot}) indicates the upper convected derivative σ▽=DσDt−(∇v)T⋅σ−σ⋅∇v\overset{\triangledown}{\boldsymbol{\sigma}} = \frac{D\boldsymbol{\sigma}}{Dt} - (\nabla\mathbf{v})^T\cdot\boldsymbol{\sigma} - \boldsymbol{\sigma}\cdot\nabla\mathbf{v}, and τ\tau is the relaxation time of the fluid. The model nonlinearity is controlled by a parameter ε\varepsilon, which is a measure of the enhanced rate of rupture events in the transient entangled network, and the model simplifies to the quasilinear Upper Convected Maxwell (UCM) model when ε=0\varepsilon= 0. To solve for the stress tensor σ\boldsymbol{\sigma}, we consider the start-up of steady shear γ˙(t)=γ˙0H(t)\dot{\gamma}(t)=\dot{\gamma}_0\mathcal{H}(t) and planar extensional flow ϵ˙(t)=ϵ˙0H(t)\dot{\epsilon}(t)=\dot{\epsilon}_0\mathcal{H}(t), where H(t)\mathcal{H}(t) is the Heaviside step function. We define an accumulated Hencky strain for extensional flow, ∫0tϵ˙(t′) dt′\int_0^t \dot{\epsilon}(t')\,dt' and an accumulated strain for shear flow ∫0tγ˙(t′) dt′=γ˙0t\int_0^t \dot{\gamma}(t')\,dt'=\dot{\gamma}_0t. As we show in Figure 2(a), the shear stress growth coefficient [18] η+=σ12(t)/γ˙0\eta^+ = \sigma_{12}(t)/\dot{\gamma}_0 evolves nonlinearly with shear strain and saturates. In extensional flow the stress difference is larger, but ηP1+\eta^+_{P1} also saturates at large Hencky strains. Our new composite material function η[P1]+\eta^+_{[P1]} closely follows this material response and, importantly, saturates at exactly the same value. The dimensionless ratio of the extension rate ϵ˙eff(t)/γ˙0\dot{\epsilon}_{\mathrm{eff}}(t)/\dot{\gamma}_0 (Figure 2(b)) decreases from an initial value of 1/21/2 and plateaus to a steady value at large strains. The predictions from

Transient and steady shear and planar extensional viscosity curves for the linear PTT model

Figure 2. (a) Transient shear and planar extensional viscosity for the linear PTT model (η0=1\eta_0 = 1 Pa.s, τ=1\tau= 1 s, ε=0.1\varepsilon= 0.1) as a function of accumulated strain. A step shear rate γ˙0=5\dot{\gamma}_0 = 5 s−1^{-1} or an extension rate ϵ˙0=0.97\dot{\epsilon}_0 = 0.97 s−1^{-1} was applied. The predictions of the UCM model are shown as dotted lines. The steady state values of these curves (star symbols) correspond to a single point on the graph of the steady viscosities, shown in (c). The variation of the effective extension rate, normalized by the applied strain rate, are shown against (b) time, and (d) strain rate.

the UCM model, which is the universal asymptotic limit at low strain rates, are shown as dotted lines, emphasizing the transition from linear to nonlinear fluid response at high shear rates (γ˙τ≫1\dot{\gamma}\tau\gg1) and large strains. The UCM model does not predict a steady extensional viscosity at dimensionless extension rates beyond τϵ˙0>12\tau\dot{\epsilon}_0 > \frac{1}{2}.

We represent the steady state responses of this dynamical system over a wide range of deformation rates in fig:2c. We show that the trajectories of the three transient stress growth coefficients each evolve towards the corresponding steady state attractors. Importantly, our new composite material function η[P1]\eta_{[P1]} (determined from transient shear properties alone) converges to the same value as ηP1\eta_{P1} (obtained from planar extension). This is because the effective extension rate begins at γ˙/2\dot{\gamma}/2 at low strain rates, and later decreases (in a model-dependent way) because ϵ˙eff/γ˙→σ12/N1\dot{\epsilon}_{\mathrm{eff}}/\dot{\gamma} \to\sigma_{12}/N_1 at high strain rates ((6)). Asymptotic analysis of the linear PTT model at large strain rates [26] gives σ12∼η0(2ετ2)−1/3γ˙1/3\sigma_{12} \sim\eta_0(2\varepsilon\tau^2)^{-1/3}\dot{\gamma}^{1/3} and N1∼η0(ετ/2)−1/3γ˙2/3N_1 \sim\eta_0(\varepsilon\tau/2)^{-1/3}\dot{\gamma}^{2/3}, hence as shown by the dashed line in fig:2d, ϵ˙eff/γ˙∼(4/ε)−1/3(τγ˙)−1/3\dot{\epsilon}_{\mathrm{eff}}/\dot{\gamma} \sim(4/\varepsilon)^{-1/3}(\tau\dot{\gamma})^{-1/3}.

These conclusions are further supported by numerical calculations (fig:3a). The planar extensional viscosity ηP1(ϵ˙)\eta_{P1}(\dot{\epsilon}) increases due to the coil-stretch transition [27] at a critical extension rate corresponding to a critical Weissenberg number Wic=τϵ˙c=12Wi_c = \tau\dot{\epsilon}_c = \frac{1}{2}. The material response softens at higher extension rates, causing ηP1\eta_{P1} to saturate smoothly.

Our analysis also applies to microstructurally motivated polymer models. We illustrate this by considering a state-of-the-art continuum model for entangled polymer melts, the Rolie-Poly model [28]. In terms of the polymer configuration tensor c\mathbf{c} and the identity tensor I\mathbf{I}, the Rolie-Poly model is written as:

c˙=−1τd(c−I)−2ksτR(1−1λ)(c+βλ2δ(c−I))(10)\dot{\mathbf{c}} = -\frac{1}{\tau_d}(\mathbf{c}-\mathbf{I})-\frac{2k_s}{\tau_R}\left(1-\frac{1}{\lambda}\right)(\mathbf{c}+\beta\lambda^{2\delta}(\mathbf{c}-\mathbf{I})) \tag*{(10)}

where the disengagement time is τd\tau_d, and the chain stretch λ=tr⁡c/3\lambda= \sqrt{\operatorname{tr}\mathbf{c}/3} evolves separately with the Rouse time τR\tau_R. The number of entanglements per polymer chain ZZ is often used to describe the degree of entanglements in the melt, and controls the ratio τd/τR\tau_d/\tau_R [29, 30]. Two scalar model parameters β\beta and δ\delta modulate the effectiveness of convective constraint release and the chain sensitivity to stretching [31]. The finite extensibility of the polymer chains is incorporated using the Cohen-Padé approximation to the inverse Langevin function for the spring law [32], making the spring constant ksk_s a function of the maximum extensibility (Lmax⁡L_{\max}) of the polymer chain:

ks(λ)=(3−λ2/Lmax⁡2)(1−1/Lmax⁡2)(1−λ2/Lmax⁡2)(3−1/Lmax⁡2)(11)k_s(\lambda) = \frac{(3-\lambda^2/L_{\max}^2)(1-1/L_{\max}^2)}{(1-\lambda^2/L_{\max}^2)(3-1/L_{\max}^2)} \tag*{(11)}

The stress is related to the polymer configuration tensor c\mathbf{c}, the spring nonlinearity ksk_s and the plateau modulus GG:

σ=Gks(c−I)(12)\boldsymbol{\sigma} = G k_s(\mathbf{c}-\mathbf{I}) \tag*{(12)}

The entangled fluid described by the Rolie-Poly model exhibits shear thinning of the shear viscosity beyond Wid≡γ˙τd≳1Wi_d \equiv\dot{\gamma}\tau_d \gtrsim1 (fig:3b). Once again, our proposed composite material function η[P1]\eta_{[P1]} accurately replicates the entire planar extensional viscosity curve. At low WidWi_d, N1N_1 increases quadratically, but when N1≳σ12N_1 \gtrsim\sigma_{12}, nonlinear elastic effects grow substantially and η[P1]\eta_{[P1]} evolves non-monotonically. Physically, the initial decrease in ηP1\eta_{P1} is due to the deformation-induced orientation of the chains within their tubes, followed by a coil-stretch transition and a sharp increase in the tensile stress difference at a critical Weissenberg number based on the Rouse time ϵ˙cτR∼O(1)\dot{\epsilon}_c\tau_R \sim O(1) (or equivalently, Wic∼τd/τR∼3ZWi_c \sim\tau_d/\tau_R \sim3Z). Finally, ηP1\eta_{P1} saturates due to finite extensibility effects and this is also faithfully captured by η[P1]\eta_{[P1]}.

Steady planar extensional viscosity curves recreated using steady shear viscosity and first normal stress difference

Figure 3. Steady planar extensional viscosity curves recreated using the steady shear η(γ˙)\eta(\dot{\gamma}) and N1(γ˙)N_1(\dot{\gamma}) for (a) the linear PTT model (ε=0.1\varepsilon= 0.1, G=η0/τG = \eta_0/\tau) and (b) the Rolie-Poly model (τd/τR=5\tau_d/\tau_R = 5, β=0.1\beta= 0.1, δ=−0.5\delta= -0.5, Lmax⁡=10L_{\max} = 10). The lines are the extensional viscosity η(γ˙)\eta(\dot{\gamma}) (red), N1(γ˙)N_1(\dot{\gamma}) (blue) and the steady planar extensional viscosity ηP1(ϵ˙)\eta_{P1}(\dot{\epsilon}) (black). The symbols (▲\blacktriangle) are the new composite material function η[P1](ϵ˙eff)\eta_{[P1]}(\dot{\epsilon}_{\mathrm{eff}}) ((7)).

In each of the examples above, simply observing either the flow curve of η(γ˙)\eta(\dot{\gamma}) or the evolution of N1(γ˙)N_1(\dot{\gamma}) with γ˙\dot{\gamma} does not clearly reveal the existence of this stretching phenomenon because of the increasing angle between the eigenvectors of the imposed deformation rate and the resulting stress difference. Evaluating the new composite material function ((7)) in terms of the measurable quantities in steady shear clearly reveals the physics of the coil-stretch transition, at no additional experimental cost. We show in the SI that η[P1]\eta_{[P1]} also fully captures the planar extensional flow response of other commonly used constitutive models such as the UCM, Giesekus, and exponential PTT models.

Finally, we illustrate the application of this composite planar extensional function experimentally. Due to the experimental difficulties in generating a steady planar extensional flow, data in the literature for ηP1\eta_{P1} is sparse. We perform steady shear experiments on a 2 wt% poly-isobutylene (PIB) fluid in a paraffin oil (solvent viscosity ηs=18\eta_s = 18 mPa.s) at 20°C in a strain-controlled rheometer (TA Instruments ARES-G2) using a 25 mm 0.1 rad cone and plate fixture. Semidilute entangled shear-thinning viscoelastic materials are widely used in industry as adhesives, coolants and lubricants. However, they are not viscous enough to characterize in extension using rotating clamp devices [33], and also too viscous for microfluidic experiments [12, 34].

This shear-thinning elastic polymer solution was studied in detail by More et al. [35] and has been characterized as being in the semi-dilute regime, with an overlap concentration c∗=0.3 wt%c^{*} = 0.3\ \mathrm{wt}\%. The data shown in Figure 4 is truncated at the critical shear rate γ˙c\dot{\gamma}_{c} beyond which elasto-inertial instabilities onset and the flow is no longer viscometric. For illustrative purposes, we show that a single mode Rolie-Poly model is able to describe the measured steady shear viscosity (●) and N1N_{1} (▲) data. The average molecular weight of the polydisperse dissolved PIB polymer is M≈106 g/molM \approx10^{6}\ \mathrm{g/mol}. The molecular weight between entanglements of the polymer melt Me,0≈7000 g/molM_{\mathrm{e},0} \approx7000\ \mathrm{g/mol} [36], the mass fraction of polymer ϕ=2 wt%\phi= 2\ \mathrm{wt}\%, and the solvent quality was determined by More et al. [35] from viscoelastic measurements to be ν=0.593\nu= 0.593. The material is a ‘barely entangled’ semidilute solution and the modified entanglement number in the solution [30] is Zsol=(M/Me,0)ϕ1/(3ν−1)≃0.7Z_{\mathrm{sol}} = (M/M_{\mathrm{e},0})\phi^{1/(3\nu-1)} \simeq0.7. Taking the first order truncation of the perturbation expansion by Likhtman and McLeish [29], τd/τR∼3Z=2.1\tau_{\mathrm{d}}/\tau_{\mathrm{R}} \sim3Z = 2.1. This is close to the best fit value τd/τR=1.3\tau_{\mathrm{d}}/\tau_{\mathrm{R}} = 1.3, and rationalizes the fit.

Experimental steady shear viscosity and first normal stress difference data for a 2 wt% PIB solution

Figure 4. Experimental steady shear η(γ˙)\eta(\dot{\gamma}) (●) and N1(γ˙)N_{1}(\dot{\gamma}) (▲) data for a 2 wt% PIB solution. The data is fitted to a one mode Rolie-Poly model (G=5.18 PaG = 5.18\ \mathrm{Pa}, τd=0.94 s\tau_{\mathrm{d}} = 0.94\ \mathrm{s}, τR=0.75 s\tau_{\mathrm{R}} = 0.75\ \mathrm{s}, β=1.28\beta= 1.28, δ=0.305\delta= 0.305, Lmax⁡=20L_{\max} = 20). The symbols (★) are the new composite material function η[P1](ϵ˙eff)\eta_{[P1]}(\dot{\epsilon}_{\mathrm{eff}}) and the Rolie-Poly model predictions for η(γ˙)\eta(\dot{\gamma}) (---), N1(γ˙)N_{1}(\dot{\gamma}) (⋅−⋅) and ηP1(ϵ˙)\eta_{P1}(\dot{\epsilon}) (—) are shown as lines.

The Rolie-Poly model predicts that the steady planar extensional viscosity (—) starts at 4η04\eta_{0} at low extension rates, and begins to increase at deformation rates ϵ˙∼2\dot{\epsilon} \sim2–5 s−15\ \mathrm{s}^{-1} due to the onset of chain stretching. We have shown in our theoretical analysis above that the ratio of the effective extension rate to the imposed shear rate decreases monotonically as the stresses in the fluid grow. As we show in Figure 4 by the stars, the new composite material function η[P1]\eta_{[P1]}, computed from the steady shear viscosity and N1N_{1} data and plotted as a function of ϵ˙eff\dot{\epsilon}_{\mathrm{eff}}, matches very well with the predicted ηP1\eta_{P1} curve.

viscosity and N1N_{1} data and plotted as a function of ϵ˙eff\dot{\epsilon}_{\mathrm{eff}}, matches very well with the predicted ηP1\eta_{P1} curve. The Trouton ratio Tr=ηP1(ϵ˙)/η0(γ˙)Tr = \eta_{P1}(\dot{\epsilon})/\eta_{0}(\dot{\gamma}) increases from Tr=4Tr = 4 at low extension rates to Tr≃50Tr \simeq50 at ϵ˙eff≃7 s−1\dot{\epsilon}_{\mathrm{eff}} \simeq7\ \mathrm{s}^{-1} (corresponding to the maximum shear rate γ˙≃80 s−1\dot{\gamma} \simeq80\ \mathrm{s}^{-1}).

We have shown in this Letter that the steady planar extensional viscosity can be reconstructed purely from the rheological information contained in the steady shear viscosity and the first normal stress difference. This result follows from the congruity of the kinematics of the two flows (quantified in terms of both IIγII_{\gamma} and IIBII_{B}) and is independent of the material constitutive equation. We have illustrated this finding using classical nonlinear continuum models as well as a molecularly-informed reptation model. We have also demonstrated it using experimental data for a representative, weakly entangled, polymer solution which cannot be characterized in planar extension using other techniques. The dynamical response of a viscoelastic material in steady shear is entirely equivalent to that in planar extension when expressed in a suitable reference frame, but the principal stress difference is distributed between two material responses σ12\sigma_{12} and N1N_{1}. This is a step towards understanding planar extensional flows, and prompts a deeper re-evaluation of other previously published viscometric data in steady shear flows for which both σ12\sigma_{12} and N1N_{1} have been carefully measured.

Our new analysis augments the well-known Cox-Merz rule [37] — which states that for viscoelastic fluids, the nonlinear shear viscosity curve can be approximated by the magnitude of the complex viscosity obtained from linear viscoelasticity measurements as a function of angular frequency. The analogous concept here is that the nonlinear material response in one type of deformation (readily achievable in a torsional rheometer) enables prediction of the corresponding behavior in a very different (shear-free) flow. Moving forward, carefully resolved measurements of σ12(γ˙)\sigma_{12}(\dot{\gamma}) and N1(γ˙)N_{1}(\dot{\gamma}) performed in steady shear flow over a range of shear rates can be used to construct steady planar extensional viscosity curves and provide greater insight into physical mechanisms underpinning strain-rate stiffening or softening, such as coil-stretch transitions and chain alignment, without incurring the additional costs and difficulties of performing more complicated planar extensional experiments.

Acknowledgments

We acknowledge Lubrizol Corporation for financial support and for providing the PIB fluid, as well as the Non-Newtonian Fluids group at MIT for the highly enjoyable reading group on flow kinematics in Fall 2025. N.K. also acknowledges conference grant support from the National University of Singapore Overseas Graduate Scholarship (NUS-OGS).

References

  1. [1]C. J. S. Petrie, One hundred years of extensional flow, Journal of Non-Newtonian Fluid Mechanics 137, 1 (2006).DOI
  2. [2]R. Larson and P. S. Desai, Modeling the Rheology of Polymer Melts and Solutions, Annual Review of Fluid Mechanics 47, 47 (2015).
  3. [3]C. J. S. Petrie, Extensional viscosity: A critical discussion, Journal of Non-Newtonian Fluid Mechanics 137, 15 (2006).DOI
  4. [4]Q. Huang, When Polymer Chains Are Highly Aligned: A Perspective on Extensional Rheology, Macromolecules 55, 715 (2022).DOI
  5. [5]G. H. McKinley and T. Sridhar, Filament-Stretching Rheometry of Complex Fluids, Annual Review of Fluid Mechanics 34, 375 (2002).
  6. [6]T. A. Lima, N. J. Alvarez, S. E. Smith, K. V. Edmond, M. Gopinadhan, and F. E. Uysse, Unexpected Solidlike Fracture in Simple Liquids, Physical Review Letters 136, 124002 (2026).DOI
  7. [7]B. Keshavarz, V. Sharma, E. C. Houze, M. R. Koerner, J. R. Moore, P. M. Cotts, P. Threlfall-Holmes, and G. H. McKinley, Studying the effects of elongational properties on atomization of weakly viscoelastic solutions using Rayleigh Ohnesorge Jetting Extensional Rheometry (ROJER), Journal of Non-Newtonian Fluid Mechanics 222, 171 (2015).DOI
  8. [8]C. J. S. Petrie, Elongational Flows: Aspects of the behaviour of model elasticoviscous fluids (Pitman, London, 1979).
  9. [9]H. M. Laun and H. Schuch, Transient Elongational Viscosities and Drawability of Polymer Melts, Journal of Rheology 33, 119 (1989).DOI
  10. [10]P. Hachmann and J. Meissner, Rheometer for equibiaxial and planar elongations of polymer melts, Journal of Rheology 47, 989 (2003).DOI
  11. [11]J. Dinic, Y. Zhang, L. N. Jimenez, and V. Sharma, Extensional Relaxation Times of Dilute, Aqueous Polymer Solutions, ACS Macro Letters 4, 804 (2015).DOI
  12. [12]S. J. Howard, M. S. N. Oliveira, M. A. Alves, and G. H. McKinley, Optimized Cross-Slot Flow Geometry for Microfluidic Extensional Rheometry, Physical Review Letters 109, 128301 (2012).
  13. [13]D. A. Nguyen, K. P. Bhattacharjee, and T. Sridhar, Response of an entangled polymer solution to uniaxial and planar deformation, Journal of Rheology 59, 821 (2015).
  14. [14]K. N. Sawyers, On the possible values of the strain invariants for isochoric deformations, Journal of Elasticity 7, 99 (1977).DOI
  15. [15]M. S. Chong, A. E. Perry, and B. J. Cantwell, A general classification of three-dimensional flow fields, Physics of Fluids A: Fluid Dynamics 2, 765 (1990).DOI
  16. [16]R. B. Bird, R. C. Armstrong, and O. Hassager, Dynamics of Polymeric Liquids. Vol. 1: Fluid Mechanics., 2nd ed. (Wiley, New York, 1987).
  17. [17]F. Hillebrand, R. J. Hill, M. Davoodi, S. J. Haward, A. Q. Shen, R. J. Poole, and S. Varchanis, Flat Elastic Disc Suspensions Are Indistinguishable from Solutions of Long Flexible Polymers within Planar Incompressible Flows, Physical Review Letters 135, 024002 (2025).
  18. [18]Ad Hoc Committee on Official Nomenclature and Symbols, Official symbols and nomenclature of The Society of Rheology.DOI
  19. [19]L. Anand and S. Govindjee, Continuum Mechanics of Solids, 1st ed. (Oxford University Press, 2020).
  20. [20]A. S. Lodge, Elastic Liquids: An introductory vector treatment of finite-strain polymer rheology (Academic Press, New York, 1964).
  21. [21]C. J. S. Petrie, Some asymptotic results for planar extension, Journal of Non-Newtonian Fluid Mechanics 34, 37 (1990).
  22. [22]O. Maklad and R. Poole, A review of the second normal-stress difference; its importance in various flows, measurement techniques, results for various complex fluids and theoretical predictions, Journal of Non-Newtonian Fluid Mechanics 292, 104522 (2021).
  23. [23]O. Cheal and C. Ness, Rheology of dense granular suspensions under extensional flow, Journal of Rheology 62, 501 (2018).DOI
  24. [24]N. Phan-Thien and R. I. Tanner, A new constitutive equation derived from network theory, Journal of Non-Newtonian Fluid Mechanics 2, 353 (1977).
  25. [25]M. Davoodi, K. Zografos, P. J. Oliveira, and R. J. Poole, On the similarities between the simplified Phan-Thien–Tanner model and the finitely extensible nonlinear elastic dumbbell (Peterlin closure) model in simple and complex flows, Physics of Fluids 34, 033110 (2022).DOI
  26. [26]D. Shogin, Full linear Phan-Thien–Tanner fluid model: Exact analytical solutions for steady, startup, and cessation regimes of shear and extensional flows, Physics of Fluids 33, 123112 (2021).DOI
  27. [27]P. G. De Gennes, Coil-stretch transition of dilute flexible polymers under ultrahigh velocity gradients, The Journal of Chemical Physics 60, 5030 (1974).
  28. [28]A. E. Likhtman and R. S. Graham, Simple constitutive equation for linear polymer melts derived from molecular theory: Rolie–Poly equation, Journal of Non-Newtonian Fluid Mechanics 114, 1 (2003).
  29. [29]A. E. Likhtman and T. C. B. McLeish, Quantitative Theory for Linear Dynamics of Linear Entangled Polymers, Macromolecules 35, 6332 (2002).
  30. [30]J. Du, H. Ohtani, A. Kiziltas, K. Ellwood, and G. H. McKinley, Capillarity-Driven Thinning Dynamics of Entangled Polymer Solutions, Macromolecules 58, 7161 (2025).
  31. [31]G. A. J. Holroyd, S. J. Martin, and R. S. Graham, Analytic solutions of the Rolie Poly model in time-dependent shear, Journal of Rheology 61, 859 (2017).
  32. [32]K. K. Kabanemi and J.-F. Hétu, Nonequilibrium stretching dynamics of dilute and entangled linear polymers in extensional flow, Journal of Non-Newtonian Fluid Mechanics 160, 113 (2009).
  33. [33]M. L. Sentmanat, Miniature universal testing platform: from extensional melt rheology to solid-state deformation behavior, Rheologica Acta 43, 657 (2004).
  34. [34]S. J. Haward, S. Varchanis, G. H. McKinley, M. A. Alves, and A. Q. Shen, Extensional rheometry of mobile fluids. Part II: Comparison between the uniaxial, planar, and biaxial extensional rheology of dilute polymer solutions using numerically optimized stagnation point microfluidic devices, Journal of Rheology 67, 1011 (2023).
  35. [35]R. V. More, R. Patterson, E. Pashkovski, and G. H. McKinley, Elasto-inertial instability in torsional flows of shear- thinning viscoelastic fluids, Journal of Fluid Mechanics 985, A37 (2024).
  36. [36]H. J. Unididad, M. A. Goad, A. R. Bras, M. Zamponi, R. Faust, J. Allgaier, W. Pychhout-Hintzen, A. Wischnewski, D. Richter, and L. J. Fetters, Consequences of Increasing Packing Length on the Dynamics of Polymer Melts. Macromolecules 48, 6638 (2015).
  37. [37]W. P. Cox and E. H. Merz, Correlation of dynamic and steady flow viscosities, Journal of Polymer Science 28, 619 (1958).

Paper details

vlnc:W_4mmeqnht

published ·

added ·

Usage

views · 0

downloads · 0

A view counts once per browser per day, a download each time the PDF is requested.

CC BY 4.0

Original source

  • Physics and Astronomy

Not recorded for this paper · View statement →

Looking for related papers…
Contents