Abstract
The development of a fast and reliable whispering gallery mode (WGM) simulator capable of generating spectra that are comparable with experiment is an important step forward for designing microresonators. We present a new model for generating WGM spectra for multilayer microspheres, which allows for an arbitrary number of concentric dielectric layers, and any number of embedded dipole sources or uniform distributions of dipole sources to be modeled. The mode excitation methods model embedded nanoparticles, or fluorescent dye coatings, from which normalized power spectra with accurate representation of the mode coupling efficiencies can be derived. In each case, the emitted power is expressed conveniently as a function of wavelength, with minimal computational load. The model makes use of the transfer-matrix approach, incorporating improvements to its stability, resulting in a reliable, general set of formulae for calculating whispering gallery mode spectra. In the specific cases of the dielectric microsphere and the single-layer coated microsphere, our model simplifies to confirmed formulae in the literature.
© 2017 Optical Society of America
1. Introduction
Due to their guidance of optical whispering gallery modes (WGMs), dielectric microspheres have attracted a lot of interest in different fields of research, such as remote atmospheric sensing [1, 2], biosensing technologies [3–5], photonic band-gap devices [6, 7], fluorescence spectroscopy [8–10], nonlinear optics [11–16], superscattering [17], and metamaterial perfect absorbers [18,19]. The extensive literature on these applications, together with the numerous theoretical works on light scattering from microspheres [1,2,9,20–26] based on Mie scattering [27], clearly demonstrate a continually growing interest in this field of research. Technological advances have led to new possibilities for using microspheres with several dielectric layers, coatings of active materials, or doped with fluorescence nanoparticles [28,29]. The excitation of WGM resonances of microspheres can also occur in numerous ways, such as via phase-matched optical waveguides [6,30] or fiber tapers [31–34], prism coupling [35], fluorescence emission of incorporated nanoparticles [36–38], or active material coatings [39]. As a result, there is now a necessity to have more advanced models, as well as efficient numerical simulation tools, for describing these resonators and their excitation schemes accurately.
Simulation techniques are required for the interpretation of measured whispering gallery mode (WGM) spectra obtained from optical resonators. They may be used to identify the polarizations of the modes in a given WGM spectrum [40], and provide insight into how they can be used for sensing applications [25,41–43]. Furthermore, the ability to calculate the underlying geometric parameters of a given resonator based solely on its spectrum [44] by scanning over a wide parameter space makes the development of a fast, reliable and general model for resonators of high importance.
The derivation of a model that contains multiple layers of concentric spheres has, until now, not been treated comprehensively. The development of a WGM spectrum model by Chew [20,45] considered spherical dielectric particles with embedded dipole sources, with the motivation being the modeling of Raman and fluorescence scattering. The Chew model was then extended to include a uniform distribution of dipole sources placed on the surface of a sphere [9]. A multilayer variant to the Chew model exists, but contains no derivation of the power spectrum [45]. Meanwhile, a generalization of Mie scattering theory, developed for spherical concentric ‘onion’ resonators, is constrained to external ray excitation [21–23], and does not provide emitted power spectra with which to compare to WGM resonances.
Analytic models typically make use of the transfer-matrix approach [2], which is faster and more convenient to construct mathematically than the multilayer Chew model. However, this approach suffers from numerical instabilities for certain parameter values [46], and needs to be treated carefully. More recent work on single-layer coated microspheres clearly separates the spectrum into TE and TM modes, and calculates the resonance positions [24,26]. Note that, in the case of [2], the labeling of the TE and TM modes has been interchanged. The key result of the present work is the derivation of a model for multilayer microsphere resonators, which may include dipole sources in any layer, or an active layer of sources. The model is able to generate the wavelength positions of the TE and TM modes, and calculate the emitted power spectrum, from a formalism that is general for any excitation strategy, unlike previous works [2].
The format of the article is as follows. In Section 2, the mathematics of the problem is summarized, and the conventions used in the literature are harmonized. In solving the boundary value problem of a multilayer microsphere using the transfer-matrix approach, the resonance positions are calculated. The formulae for the normalized power as a function of wavelength are then derived for two main cases. The first case is mode excitation via a single dipole placed on the surface with any desired orientation, analogous to embedded nanoparticles. The second case is a uniform distribution of dipoles of random orientation, extending the work by Chew [9], which is analogous to a fluorescent dye coating as commonly used in biosensing applications [47, 48]. The distribution of dipoles can occur in any layer of the multilayer resonator. In Section 3, the formulae are shown to apply to specific cases, highlighting the differences between multilayer, single-layer and uncoated microsphere spectra. We showcase the results for active layer coated microspheres, and demonstrate the novelty of the unified multilayer model. A discussion of the implementation of the transfer-matrix algorithm is also included, demonstrating improvements made to the mean execution time. Tests showing that the model converges to the specific cases as the layer thickness becomes vanishingly small are given in the Appendix A.
2. Theory
In this section, we state the basic equations required to find the wavelength positions of the resonances, and the radiation power spectrum of a multilayer microsphere, with either dipole sources or active layers for the excitation method.
2.1. Geometry
We consider a microsphere with an arbitrary number of concentric layers, N. The refractive index distribution and thicknesses are illustrated in Fig. 1. It is assumed that each layer includes a dipole emitter located at position r′j, where j is the layer number and the prime symbol is specifically used for the position of the sources. We use the radial coordinate r when representing fields at an arbitrary point in space, and rj to specify unambiguously the radius of the boundary between the jth and j + 1th region. The outermost region is N + 1, extended to infinity, and the innermost region is 1, hence the radius of the inner region is r1 and rN is the boundary of region N.
2.2. Conventions
Considering the spherical symmetry of the problem, we use Vector Spherical Harmonics (VSH). Different conventions exist for the definition of VSH in the literature, e.g. atomic physics and electrodynamics (see [27] and [49]). We modify the definition given by Barrera [50],
where Ylm(θ, ϕ) are standard Scalar Spherical Harmonics [51], and l and m are the azimuthal quantum numbers. The vector functions Ylm(θ, ϕ), Ψlm(θ, ϕ), and Φlm(θ, ϕ) are orthonormal, and form a complete set (See Eqs. (68) and (69)), i.e. any vector field in spherical coordinates can be expanded based on these functions, where the coefficients , and can be found by using orthogonality relations (see Appendix A). Note that Ylm is in the radial direction and Ψlm and Φlm are in the transverse plane perpendicular to , and hence and represent the coefficients of the transverse field.2.3. Transfer matrix method
We solve Maxwell’s Equations (in Gaussian units),
taking into account the boundary conditions of the problem. In general, the total electric and magnetic field in each region j can be written as the sum of the fields due to the dipole in the layer, denoted Ejd, Hjd, and those associated with the reflection and transmission from other layers, denoted Ej, Hj. Hence and . The fields (Ej, Hj) can be written as [45]: Here, Aj, Bj, Cj and Dj are coefficients that are determined through the boundary conditions. Note that Aj and Bj describe the transverse component of Hj and thus the TM modes, whereas Cj and Dj describe the TE modes, as defined by Jackson [51]. In this notation, the TM modes are defined as the modes for which Hj has no component in the radial direction, whereas the TE modes are those for which Ej has no such radial component. Also, the choice of Bessel functions jl(kjr) and ensures that appropriate functions of r can be constructed for any layer, including the innermost and outermost regions. Using the properties of the orthonormal functions Ylm, Ψlm, and Φlm (Eqs. (68) through (70)), we rewrite Eqs. (4) and (5) as This explicitly shows that the electric and magnetic fields (Ej, Hj in the layer j are written in terms of the orthonormal function set Ylm(θ, ϕ), Ψlm, (θ, ϕ), and Φlm (θ, ϕ), in a form consistent with Eq. (2). The boundary conditions at the interfaces of the layers imply that transverse components of the fields are continuous, while there is a discontinuity in the normal components of the fields. We focus on transverse components of the fields, indicated by superscript (1) and (2) in Eq. (2), in layer j. We write them in a matrix form using Eqs. (6) and (7) where the block diagonal matrix and the vectors EHj and Aj are defined asIn arriving at Eq. (9) we have used c/njω = 1/kj, Riccati-Bessel and Riccati-Hankel functions, ψl(kjr) = kjrjl(kjr) and and their derivatives with respect to their arguments, and . Note that the determinant of 2 × 2 blocks, and , are given by
where the Wronskian is defined as Using Eq. (19) in [2], it can be shown that . We write the fields Ejd(r), Hjd(r) due to a dipole located in the layer j and at position r′j in a similar way as Eq. (8), and hence we modify the field equations in [20] to write Here, θ(r) is a step function [θ(r) = 0 for r < 0 and θ(r) = 1 for r ≥ 0] that ensures the correct Bessel function jl(kjr) or is selected to evaluate the fields at point r either when (shown by subscript L in ajL) or (shown by subscript H in ajH), respectively. The vectors EHjd, ajL and ajH are given by where the coefficients ajEL, ajML, ajEH and ajML take the form [20]: The dipole coefficients ajEL and ajEH contribute to the TM modes, whereas ajML and ajMH contribute to the TE modes [27,51], which has caused confusion in the literature [2]. Here, we use the subscripts E and M of the dipole coefficients to indicate their origin in the electric and magnetic multipole expansions, respectively. The symbol indicates derivatives with respect to the position , and P is the dipole moment vector. Establishing field components in the layer j, we can construct the total field as the sum of fields in Eqs. (8) and (14), i.e., where the superscript T indicates total fields in layer j. The continuity of the transverse components of the electric and magnetic fields at the interface of regions j and j + 1 leads to Equation (20) can be used recursively to connect the coefficients in the outermost region, N + 1, to the innermost region, 1, leading to where matrix T(N + 1, j) is defined by Note that T(N + 1, j) is always composed of repetitive blocks of matrices in the form of . Explicitly writing this matrix, it can be found that The sub-matrices and take the form for and GR=µj+1nj+1 in the case of GTM, and GL= µj+1nj and GL= µjnj+1 in the case of GTE.The constant vector is given by
The sum in Eq. (27) is effectively over the regions that contain dipoles, since terms associated with regions with no dipoles are zero. Equation (22) can be inverted to obtain A1 in terms of AN+1 as follows, Note that the constant vector , contains information about the structure through the scattering matrix T, and information about the dipole sources, through ajH and ajL. However, matrices T(N + 1, 1) and T−1(N + 1, 1) are independent of any source, and depend only on the parameters of the structure. Thus they represent the scattering matrix of the entire structure. To avoid confusion between the elements of matrices T(N + 1, 1) and T(N + 1, j), from now on, we use T ≡ T(N + 1, 1) and Tj ≡ T(N + 1, j) for j ≠ 1. The matrices of the form T(N + 1, j) are block diagonal matrices, since they have been built based on block diagonal matrices M. We define matrix and henceIn the innermost region, the coefficients of Hankel functions in Eq. (4) and (5) are zero, and hence the vector A1 has the form A1 = (A1, 0, C1, 0). Using this, Eq. (28) can be solved to find AN+1 in terms of A1 and C1 as
The coefficients AN+1 = (AN+1, BN+1, CN+1, DN+1) determine the fields in the region N + 1, i.e., the outermost region, and hence are the scattering coefficients of the whole system of the microsphere and its sources. These coefficient are the same as an and bn coefficients of Mie scattering, and represent different magnetic and electric dipole moments (BN+1 corresponds to an, and DN+1 corresponds to bn). Once the values of the field coefficients in the outermost layer are known from Eqs. (30) through (33), the coefficients in any other layer, Aj, can be calculated recursively from Eq. (21). Then, Eqs. (6) and (7) may be used to calculate the total fields, Ej and Hj.Equations (30) through (33) are general, and can be used for a range of scenarios:
- If there are no sources (i.e. no dipoles in the structure and no incident wave) then , and from the above equations one can find the ratios BN+1/AN+1 and DN+1/CN+1, which determine all the far field scattering coefficients. From these ratios one can find the TM and TE resonances of the structure, respectively (see Sections 7.1 and 7.2).
- If there are dipole sources in the structure, then, without loss of generality, we can choose AN+1 = CN+1 = 0, solve for A1 and C1 from Eqs. (30) and (32) and then find BN+1 and DN+1 from Eqs. (31) and (33), respectively. This is due to the fact that the total emitted power must be the same in both the near and far fields.
- If there is only an incident field, then , and AN+1 and CN+1 are known from the incident wave expansion, and in turn A1 and C1 are known, which means that BN+1 and DN+1 are also known.
2.4. Structure resonances
We consider the case where there are no sources-neither plane waves nor dipoles. Thus in Eqs. (31) through (32) and we can find
In the electric field of Eq. (4)BN+1 is the coefficient of the term and AN+1 is the coefficient of the jl(kr) term in the outermost region N + 1. Hence the ratio of BN+1/AN+1 should approach infinity near a resonance with a transverse magnetic component only. Similarly, in the magnetic field of Eq. (5)DN+1 is the coefficient of the term and CN+1 is the coefficient of the jl(kr) term, in the outer layer N + 1. In this case, the ratio of DN+1/CN+1 should approach infinity near a resonance with a transverse electric component only. As a result, both S21/S22 and S43/S44 → ∞, which means the TM and TE resonances of the structure can be found by setting These equations are in general multivalued, and for a given azimuthal quantum number l, the solutions to Eqs. (36) and (37) form the fundamental radial modes and their harmonics. Since the higher order harmonics have larger values of the Bessel function argument (kr) at their roots than the fundamental modes, all modes that appear within a wavelength range, including higher order modes, can be obtained. The numerical code associated with this paper (http://www.photonicsimulation.net) uses the optical and geometrical properties of any structure, to find the T matrix, and numerically solves Eqs. (36) and (37) for any given wavelengths range.2.5. Scattered power in the outer region
We are interested in calculating the total radiated power of the system. Thus, we need to calculate the fields as r → ∞. In the outermost region N + 1 and for r ≫ r′j, the total transverse parts of the fields in Eq. (18) are given by
In the limit of r → ∞, this equation leads to the following forms for the scattered fields, Note that in arriving at the above equation, we have used Eqs. (2), (9), and (10) and jl(kr) → 0 as r → ∞. The total scattered power through a sphere of radius r can then be calculated by where we have used the orthonormal properties of Ψlm(θ, ϕ) and Φlm(θ, ϕ) functions given in Eq. (68) through (70). Note that in the limit of r → ∞, exp(iz) and exp(iz) [2], and hence Equation (42) is general, where BN+1, DN+1, and can be calculated based on Eqs. (31), (33), (15), and (16) respectively. Note that if there is no dipole in the outermost region, then .2.6. A dipole in one layer
In this section, we assume that there exists only one dipole in the layer j, where j = 1,…, N + 1. Then, according to Scenario 2 of Section 2.3,
Then, using Eqs. (15), (27), and (29), we get based on which we can find where and whereNote that αl and βl correspond to the contributions from the TM modes, whereas γl and ζl correspond to the contributions from the TE modes. Equations (45) and (47) are general, and can be applied to a dipole in any layer j, including the innermost layer 1 or the outermost layer N + 1. Considering Eqs. (16) and (17), we can rewrite and , which appear in the total scattered power in Eq. (42), as
Using the properties of orthonormal functions Ylm, Ψlm, and Φlm(θ, ϕ), and Eq (70), we note the forms of and , where , , and are functions of , as in Eqs. (49) and (50). Hence we can use the properties of the dyadic products of Ylm, Ψlm, and Φlm, Eq. (71), to perform the summation over m and simplify and , which appear in Eq. (42),
Here, Pr, Pθ, and Pϕ are the polar components of the polarization vector P. Based on the above equation, we can find the total scattered power from a sphere as the sum of powers due to normal and transverse components of P,One can normalize the powers P⊥ and P∥ to powers radiated by a dipole in a bulk material with (nj, ϵj, µj), i.e. and to obtain
2.7. One active layer
In this section, we consider a multilayer structure where one of the layers consists of active material. In this context, we add randomly oriented and uniformly distributed dipoles, with density , into that layer. As a result, one must integrate Eqs. (54) and (55) with respect to , which is located within the layer j. Since dipoles are randomly oriented in the layer, we can write , where
where the volume of the shell is . If j = 1, then by convention, r0 is set to zero, as in that case the volume is simply the sphere bounded by the innermost radius. Similarly, The total power is then Defining a functional form where pl(z) and ql(z) can be any of ψ(x) = x jl(x) or , one can then find where rj and rj−1 are the radii of the upper and lower interfaces of the region j, respectively. Similarly, we can calculate With and now known, the total averaged power can be calculated from Eq. (63).3. Demonstration and discussion
We now consider several scenarios of interest that can be uniquely treated using this model. First, we examine the behavior of the WGM spectrum of a silica microsphere (with dispersion included [52]) coated with a single high refractive index layer (n2 = 1.7), surrounded by water (n3 = 1.33), as the thickness of the coating d is changed from 5 nm to 15 nm. This scenario corresponds to N = 2, where N is the number of layers, including the central silica sphere, and the high index layer. Figure 2 shows the results for an electric dipole placed just outside the surface, with an orientation perpendicular or parallel to the surface of the sphere. A range of wavelengths 0.59–0.61 µm is simulated, and the outer diameter is kept fixed at 25 µm. It is found that there is a systematic shift in the prominent WGM peaks towards higher wavelengths, as the thickness of the layer is increased. The free spectral range, however, remains largely unchanged over this range of wavelength values. In the limit d → 0, the results match the simple case of the Chew model, as anticipated [20].
The thin vertical lines marking the position of the resonances, with the corresponding mode numbers and labels, are obtained from the structure resonance positions in Eqs. (36) and (37) for a two-layer microsphere, by setting N = 2 in our general formalism. This can be done in a straightforward way in the code associated with this paper (see pg. 10). The thick vertical lines indicate the resonance positions obtained from the Arnold formalism [24,26], which agree exactly. Note that in the case of the parallel excitation in Fig. 2(b), there is a small contribution from the TM mode as well, as expected from Eq. (55).
A silica microsphere of the same size, 25 µm, is then modeled as being coated with a polymer (PMMA) with dispersion incorporated through the Sellmeier equations for both materials [52,53], as shown in Fig. 3. Across the wavelength range of 0.59 to 0.61 µm, the refractive index of silica varies from 1.4584 to 1.4577, wheres the index of PMMA varies from 1.4913 to 1.4902, respectively. PMMA is simulated in this example because it can act as an active layer [47] and is a straightforward way of testing the functionality of the model. At the diameter considered, higher order modes are not strongly coupled to, and so both the TE and TM modes remain distinct, as can be seen in Fig. 3(a). The refractive index contrast between silica and PMMA is relatively small, and so the dependence of the mode positions on the thickness of the coating is more mild. A close-up view of the plot is shown in Fig. 3(b). The vertical lines indicate the full-width at half-maximum (FWHM) positions for a variety of peaks, from which the Q-factors can be extracted. The Q-factor is estimated directly from the width of a spectral peak δλ, centred around a wavelength λ0, through Q = λ0/δλ. Q-factors corresponding to a selection of TM and TE modes are also shown above each peak. Note that for the TM modes (the left three peaks) there is a decrease in the Q-factor as d increases, but for the TE modes there is an apparent increase in the Q-factor.
The sensitivity of the WGM peaks can be examined by varying the refractive index of the surrounding medium, n3. In Fig. 4(a), d = 10 nm, the mean TE peak shift leads to a sensitivity of S ≡ dλ/dn3 = 60.0 nm/R.I.U. For a surrounding index of 1.36, the TE and TM modes are broad and overlapping, and an extraction of the Q-factor using the FWHM approach will necessarily include contributions from both mode polarizations. This is a consequence of the fact that the Q-factors obtained from the spectrum include both intrinsic, non-radiative contributions from the geometry of the structure, and contributions from the relative coupling of the active layer to the modes. This makes it more difficult to separate nearby modes and define independent Q-factors. We also calculate a figure of merit (FOM), defined as Q.S [43], to assess the sensing performance of the microspheres. For a given sensitivity S, the value of Q chosen is the mean value of the peak as it shifts to its new position, as a function of n3. The inset of Fig. 4(a) shows a decrease in the FOM as a function of λ. In Fig. 4(b), d = 50 nm, both the sensitivity and the FOM are larger, with S = 63.3 nm/R.I.U.
The summation , in the expressions for P/P0(λ), is calculated to an upper bound, lmax, determined by a prescribed tolerance τ, so that
This prescription is sufficient so long as the behavior of P/P0 is convergent, which is usually the case, except for unstable parameter regions, described below. At each value of l > 1, the spherical Bessel and Hankel functions are calculated using the recursion relations, and function calls are minimized to improve the efficiency of the calculation.Examples of the scaling behavior of the execution times (T) for the functions P/P0(λ), with respect to wavelength, for numbers of layers N = 1, 2 and 3 are shown in Fig. 5 for a fixed outer diameter of 25 µm. The results are fairly insensitive to the layer thickness, allowing Fig. 5 to be a fairly accurate measure of the execution time for a given number of layers and prescribed tolerance, τ. It was found that the implementation of the recursion relations resulted in an improvement of approximately one order of magnitude in the execution time compared to function-call methods.
4. Conclusion
A method for the modeling of whispering gallery modes in optical resonators, including various excitation scenarios that closely mirror experimental techniques, is an important step toward facilitating the design and analysis of novel resonator architectures. We developed an algorithm based on the solutions of the boundary value problem for multilayer spherical resonators, with improved execution times compared to standard functional methods. The model is able to handle an arbitrary number of concentric, spherical dielectric layers, and extract the resonance positions from the characteristic equation. Formulae for the power spectrum are derived for the case of a single dipole or an active layer source, and the behavior of the mode positions are examined for several different scenarios. Estimates of the computation time for the normalized emitted power at a single wavelength, and improvements to stability issues inherent in the transfer-matrix approach, have been discussed. The spectrum simulator reported represents an important step towards a general, fast and efficient method for extracting the underlying parameters and properties of a given resonator purely from its spectrum, simulating spectra over a wide parameter space, and predicting features of novel resonator designs for photonic band-gap devices and biosensing applications.
5. Appendix A: Properties of vector spherical harmonics (VSH)
The VSH are orthogonal in the usual three-dimensional sense,
and also orthonormal in the Hilbert space In addition, it can be shown that The following summation rules apply to dyadic products of the VSH:6. Appendix B: Relation between conventions
Depending on the application, different definitions have been used for the VSH. The following functions have been used in the literature
Comparing these equations with the orthonormal functions used here, Eqs. (1), we find,7. Appendix C: Examples
7.1. Example 1: A microsphere
For a microsphere, we set N = 1, and then using Eq. (23), the T matrix is
and hence we can use Eq. (25) and (26) with j = 1 to find By assuming µ1 = µ2, the TM and TE resonance conditions, T11 = 0 and T33 = 0, lead to Eqs. (79) and (80) exactly match Eqs. (19) and (13) in [25] and Eq. (4.53) in [27], respectively. It should be noted that in Eq. (33) of [2] the TE and TM modes are interchanged.7.1.1. Special case: A dipole in the outer region
Let us assume a dipole source is located in the outermost region, i.e., j = N + 1 = 2. Then from Eqs. (27) and (23) becomes
Using Eq. (45) and (47), we can find and in Having identified the coefficient αl, βl, γl, ζl, we can find the power due to normal and transverse components using Eq. (54) and (55) as Now since S = T−1, Eq. (29), then and In addition, and hence we can use Eq. (25) and (26) to find Having found the coefficients and , we can find and . Equations (86) and (88) are the same as Eqs. (6) and (7) of Chew [20].7.1.2. Special case: A dipole in the inner region
Let us assume a dipole in the innermost region, then N = 1, j = 1 and from Eqs. (15), (23) and (27) we find . Using Eq. (45) and (47), we can find and ,
According to Eq. (27)S = T−1(2, 1) hence (S22T22 + S21T12) = (S44T44 + S43T34) = 1 and as a result, and Now, since S = T−1(2, 1), then S22 = det(TTM)−1T11 and S44 = det(TTE)−1T33 and hence we can use Eqs. (25) and (26) to find Similarly, we find Thus, we can find and as for These are exactly the same as Eqs. (1, 3a) and Eq. (2,3) of Chew [9].7.1.3. Special case: A microsphere with an active inner region
Now assume that the inner region is filled with randomly oriented dipoles. Then, we can use Eqs. (63), (65), and (66) together with , βl = 0, ζ = 0, and , calculated in the previous section, to find
Note that in the case of a microsphere, r0is set to zero, as well as all functionals of the form Ψ[·](k1r0) = 0. Similarly, we can also find Having and , we find7.2. Example 2: A shell
If N = 2, i.e., a microsphere coated by a single layer, then using Eqs. (23), (25), and (26), we have the following T(3, 1) matrix:
One can find the TM and TE resonances of the structure by setting T11 = 0 and T33 = 0, respectively, from Eqs. (36) and (37) which results in the following resonances and where Eqs. (107) and (108) exactly match Eq. (7) in [26] and Eq. (10) in [24], respectively.A numerical comparison is shown in Fig. 6. The multilayer model for a single layer converges to the microsphere case for a vanishingly small layer coating, or a vanishingly small internal sphere size. It was found that both the limits converge to within numerical precision.
Funding
Australian Research Council (ARC) (FL130100044, CE140100003).
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