SUPPLEMENTARY MATERIAL Multiscale modeling of oil uptake Jean-Michaël Vauvre, Anna Patsioura, Régis Kesteloot, Olivier Vitrac Jean-Michaël Vauvre INRA, UMR 1145 Ingénierie Procédés Alimentaires, F-91300 Massy, France AgroParisTech, UMR 1145 Ingénierie Procédés Alimentaires, F-91300 Massy, France McCain Alimentaire S.A.S., Parc d’entreprises de la Motte du Bois, 62440 Harnes, France Anna Patsioura INRA, UMR 1145 Ingénierie Procédés Alimentaires, F-91300 Massy, France AgroParisTech, UMR 1145 Ingénierie Procédés Alimentaires, F-91300 Massy, France Régis Kesteloot Régis Kesteloot conseil, 60 Avenue du Colonel Driant, 59130 Lambersart, France Olivier Vitrac INRA, UMR 1145 Ingénierie Procédés Alimentaires, F-91300 Massy, France AgroParisTech, UMR 1145 Ingénierie Procédés Alimentaires, F-91300 Massy, France Phone: +33169935063 Email: olivier.vitrac@agroparistech.fr Topical area Transport Phenomena and Fluid Mechanics Keywords Porous media, Spontaneous imbibition, Percolation model, Kinetic Monte-Carlo, Deep-frying 1 1 Common assumptions The optical configuration of the experiments on an inverted microscope is reproduced in Figure 1a-c. The aim of the 3D optical reconstruction was to rebuild the penetration depth of oil within each cell. The main idea was to work with averaged properties along a significant section, so-called Σ and of specific surface area AΣ, parallel to (x,y) so that composition effects could be related to an increase of the length of the optical path T (see Figure 1c), where fluorescent absorption and emission occurred. As a result, the attenuation of the z ,t excitation beam, E X , was assumed to be controlled by two effective absorption coefficients: one associated with the scattering of light due to diffusion and refraction through crossed semi-transparent phases, denoted s T ,t ; and one specifically associated to the specific absorption by fluorophores, denoted f T ,t . Due to the deep-UV excitation at 295 nm, absorbing fluorophores included phenolic residues in cell walls and 1,6-diphenyl-1,3,5hexatriene, they were denoted with subscripts 1 and 2, respectively. By noting that collected intensity was also limited by the scattering of emitted fluorescence, the following set of effective absorbing coefficients, denoted X and M , was used for excitation and emission respectively: X M where i i wall ,oil ,air T ,t s T ,t f T ,t T 1 1 x, y,z x , y , z ,t òwall s , wall òoil s ,oil dxdy dz T 0 A T 1 1 x, y, z x , y , z ,t òwall f 1c1,wall òoil f 2 c2,oil dxdy dz T 0 A T ,t s (1) T ,t are the volume fractions of each phase verifying òsolid òoil òair 1 ; {ci }i 1..2 are the volume concentrations in fluorophores and { f ,i }i 1,2 the corresponding specific fluorescent absorption coefficients; { ns ,i }i wall ,oil are the non-fluorescent absorption coefficients and were assumed independent of the emission wavelength without loss of generality. Similarly, en effective quantum fluorescence yield, denoted , was assumed to vary with the local composition in the horizontal plane z at time t. It related the local excitation intensity z ,t absorbed to generate fluorescence, E Xf , to the local intensity of the fluorescence emission, z ,t EMf as: T ,t T ,t dEMf T ,t dEXf T 1 0 x, y , z wall A ò x , y , z ,t 1 Xf 1c1, wall òoil 2 Xf 2c2,oil dxdy dz s T ,t (2) Since the volume fraction of cell walls remained unchanged during experiment, the invasion of oil of the considered plane caused an increase of the measured fluorescence. 2 T ,t with time and consequently, to Figure 1. Simplified description of excitation and emission pathways. a) Experimental setup, where the incident excitation EX0 is scattered by the sample (intensity EXs) and used to generate fluorescence (intensity EXf). The residual excitation EX is lost at the top of the sample. The corresponding emission of fluorescence (EMf) is scattered by the sample (intensity EMs). Only the fraction enclosed within the solid angle (with intensity I) is measured by the detector. b) Scheme of the local conversion of excitation into fluorescent emission. c) Corresponding light paths T are as used in Eq. (7). d) Honeycomb arrangement of cells; e) and corresponding step-wise integration of absorption and emission intensities when oil fills successively cells of layer 1 (step 1) and of layer 2 (step 2). It is important to notice that air is not represented as it is associated to s Ki 0 . 2 Photon counting balance As the speed of light is much faster than the percolation of oil, both excitation of light and emission fluorescence fluxes were assumed at steady state. By choosing the top surface as reference position z 0 , inverse modeling aims at relating the thickness of the optical path, T, 3 I z 0 z ,t T where fluorescence occurs, with the intensity of the fluorescence I T ,t dz collected t by the detector. The variation of the fluorescent intensity generated when the optical path is T,t I increased of dT, , is related to the variation of the intensity absorbed and emitted by T t T ,t the fluorophores, E Xf EMf T ,t and T T t , respectively, via Eq. (2) and the following photon t balances: I T ,t T t , measured I T ,t T t , emited light in direction of the detector T ,t T EMf 4 T s T ,t I T ,t T I T ,t t t , scattered light in direction of the detector T 4 T ,t (3) T ,t E Xf T s T ,t I T ,t t where T is the solid angle, which the lens makes with Σ at position z. Similarly, the photon balance applied to the excitation beam leads to a variation of the light flux, lost by the top of the sample, E XT ,t , as: T t T ,t E Xf E XT ,t T t T s T ,t E X T ,t (4) t z T ,t 4 and 1, yields to a generalized Beer-Lambert law written as the photon balance between the absorbed and emitted light fluxes: The linear combination of Eqs. (3) and (4), respectively to the weights K d K T ,t EXT ,t I T ,t dT t dK T ,t T ,t EX s dT t T ,t K T ,t T ,t EXT ,t I T ,t (5) It is worth noticing that Eq. (5) neglects the effect of wavelength on attenuation constant T ,t . It can be integrated along T as soon as variables are separable, that is when K T ,t can be assumed constant. According to Eq. (11) in 1, the variation of the solid angle associated to a source much smaller than the detector (lens) and close to the detector is indeed 1 T C , where C is the thickness of the quartz coverslip (0.17 mm) 1 2 2 4 2 T C Rlens s and Rlens is the diameter of the lens (12 mm). By considering thin cell layers (total thickness of 300 µm), the variation of between z 0 and z T is low. The variation of t is of 6%. When the optical absorption and composition properties vary significantly along T, the strategy will consist in decomposing the integral over N successive optical paths such as N T Ti . When K is constant on each domain and equal to K i , one gets: i 1 4 Ti N Ki EXT ,t I T ,t i 1 Ti1 T ,t Ki E X I T ,t N Ti i 1 Ti1 Ti ,t s (6) dT with T0 0 . It is worth noticing that Eq. (6) is commutative for all optical paths with similar thicknesses and optical properties. As a result, a step-wise integration procedure can be devised by collecting all phases with similar optical properties and filling homogeneously the capillary: oil or cell walls. This strategy is illustrated in Figure 1d-e as an equivalent dissipative network for excitation and emission. Pure air does not have significant effect on light scattering T ,t Ki 0 . If N is now the number of dense phases assumed because it is associated to s to be homogeneous, Eq. (6) is integrated as: N Ki E XTi ,t I Ti ,t ln s ,i Ti K E Ti1 ,t I Ti1 ,t i 1 i 1 i X N (7) with Ti the length of the optical path for each solid phase i, intensity at top surface I 0,t 0 , 0,t incident excitation at bottom surface EX EX 0 and apparent scattering coefficient s ,i for the phase i. 3 Application of Eq. (7) to the identification of the oil front z Eq. (7) is used with the following convention: i 1 for bottom cell wall, and i 2 for oil. The position of the oil front, z, is defined in this study as the equivalent thickness of the optical path filled with oil, T2 z , regardless oil is on the top or at the bottom of the considered cell. According to Eq. (7), two sensors should be required to retrieve unambiguously z: one T ,t sensor to measure the collected fluorescence, I N , and another to measure the transmitted T ,t light across the product, EX N . In this study, we inferred a reconstitution strategy based on the sequential observations on the cell filling process using a single detector and reported in Patsioura, et al. 2. For each stack of two cells (see Figure 1c), the inverse problem –finding the position of the oil front– was broken into two sequential problems: finding z when only a cell of the first layer was partly filled with oil and finding z z1 when the cells of the top layer are already filled with oil and where z1 is the position on the cell wall between the top layer (layer 1) and the bottom layer (layer 2). Step 1: For 0 t t z1 , only optical paths crossing the layer 1 are considered: N 2 in Eq. (7) with i 1 for the bottom cell wall between layers 1 and 2 (see Figure 1d) and i 2 for the oil filling the top cell. For t t z , the top cell is saturated (filled) with oil. 1 Step 2: For t t z tlag , where tlag is a significant lag time, we get N 3 in Eq. (7) with 1 i 1 for cell wall, i 2 for oil height in the top cell with T2 z1 and i 3 for oil height in the bottom cell with T3 z . The application of Eq. (7) for the top cell leads to: z z K 2 EX ,2 I 2 t t K1EX 0 exp s ,1 0 t t z1 t exp s ,2 z with t T1 0 z z1 5 (8) Under low scattering and low fluorescent conditions (i.e. f ,i z s ,i z 0 for i = 1, 2), the right-hand side in Eq. (8) becomes exp s ,i z t 1 s ,i z t s ,i 2 z t 2 . As a z , result, the transmitted light and collected fluorescence across a single cell, EX ,2 and I 2 t z t respectively, are approximated by a linear function of z t . 4 Literature Cited 1. Shelyuto V. Exact analytic results for the solid angle in systems with axial symmetry. Z. angew. Math. Phys. 1989;40(4):608-612. 2. Patsioura A, Vauvre JM, Kesteloot R, Jamme F, Hume P, Vitrac O. Microscopic imaging of biphasic air-oil flow in French-fries using Synchrotron radiation. submitted to AIChE J. 2014. 6