SUPPLEMENTARY INFORMATION The Effect of Contact Conditions on the Onset of Shear Instability in Cold-Spray Fanchao Meng, Huseyin Aydin, Stephen Yue, and Jun Song* Department of Mining and Materials Engineering, McGill University, Montréal, Québec H3A 0C5, Canada S1. Deformation Control Techniques To cope with the convergence challenges in cold-spray finite element simulations, many different deformation control techniques have been explored. For example, adaptive meshing has been largely adopted to confine the excessive mesh distortion [1-4] . However, very frequent remeshing in adaptive meshing can cause unrealistic deformation shapes for both the particle and substrate and non-conserving energy variations [1, 3-5], and thus is not adopted in our simulations. Figure S1 illustrates a typical deformation response in the particle/substrate contact using adaptive meshing frequency of 30 and mesh sweeps per increment of 1, showing a much smoothed “jetting” periphery compared with the one without adaptive meshing (see Fig.4 and Fig. 8 in the main text). Hourglass control and element distortion control have also been studied by Li et al. [5] as alternative deformation control techniques. As reported in Ref. [5], hourglass control with stiffness technique is particularly useful in problems using reduced integration elements, whose physical response will not be constrained under this control [5, 6] . The element distortion control can be employed to generate more realistic deformation shapes with good convergence if a small element distortion control is used (e.g., using a distortion length ratio < * Corresponding author: Jun Song. Email: jun.song2@mcgill.ca Tel.: +1 514-398-4592 Fax : +1 514-398-4492 Other Emails: fanchao.meng@mail.mcgill.ca (Fanchao Meng), huseyin.aydin@mcgill.ca (Huseyin Aydin), steve.yue@mcgill.ca (Stephen Yue). S1 0.1) [5, 6] . In addition, hourglass control and element distortion control can be used together to further improve the simulation convergence. In the present study, the effects of hourglass control with stiffness technique and element distortion control on the onset of shear instability were examined. Figure S2 plotted the temperature evolution of the corresponding most critical particle element under different deformation control techniques for a representative full-particle model with friction coefficient = 0.5. As shown in Fig. S2, the shear instability initiates around 32 ns when no control technique is used, being very close to onset time under the element distortion control (with distortion length ratio 0.1). However, under hourglass control with stiffness or hourglass control together with element distortion control, the shear instability is completely refrained. Consequently, element distortion control with distortion length ratio 0.1 is chosen for our simulations in this study. Fig. S1. Deformed particle/substrate configurations and temperature contours with adaptive meshing. The simulation is conducted using the half-particle model with the particle velocity being 500 m/s, friction coefficient being 0.5, and surface separation allowed. S2 Fig. S2. The simulated temperature evolution curves for the most critical particle element under different distortion control techniques (DC: distortion control; EDC: element distortion control; HGC: hourglass control). The simulation is conducted using the full-particle model with the particle velocity being 500 m/s, friction coefficient being 0.5, and surface separation allowed. S2. Frictional Dissipation In the work by Li et al. [5] , it was demonstrated that in cold spray, the thermal energy from frictional dissipation is negligible compared to the energy from plastic dissipation for low friction coefficients (i.e., < 0.4). In our study, we further examined the energy contribution from the frictional dissipation for intermediate and high values of friction coefficient, and found that the contribution remains negligible. Figure S3 plotted a representative energy evolution curve under friction coefficient μ = 4, showing the thermal energy generated by friction is order of magnitude smaller than the one coming from plastic deformation. Therefore we believe that friction dissipation does not modify the simulation results. The insignificant frictional dissipation likely is because a) the contacting surface is only limited between the particle outer surface and the substrate, and b) the relative sliding between particle/substrate is small. S3 Fig. S3. A representative energy evolution curve extracted from the overall particle/substrate model. The simulation is conducted using the full-particle model with the particle velocity being 500 m/s, friction coefficient being 4, and surface separation allowed. S3. Perturbation Induced Axi-asymmetric Deformation When the full-particular model is used in the simulation, axi-asymmetric deformation may happen (see Fig. 5). This axi-asymmetry is in essence induced by the numerical randomness which serves as a perturbation. The perturbation would affect the exact details of the temperature evolution, e.g., onset time of shear instability, just as those details can be easily influenced by contact conditions. This is exactly the reason why the onset of shear instability cannot be used as a precise indication of bonding. However, the perturbation (due to numerical randomness or other sources) is not expected to modify the physics of the problem. As discussed in the manuscript, the trends shown in Figs. 9 and 10 reflect the actual deformation characteristics (i.e., physics), which remain unchanged regardless of the presence of perturbation. S4 To further illustrate this point, we performed a series of simulations with manually introduced perturbations. Below we demonstrated two case studies, shown in Figs. S4 and S5, corresponding to simulations with friction coefficient being 0.25 and 8 respectively (both with surface separation allowed). In both cases the system was perturbed by removing a rectangular region of a thickness of only one element (0.0006 mm) on the substrate (see Fig. S4). From the simulation results we can see that though the general features remain similar, the exact details of the temperature evolution are altered. In particular for the case with = 0.25, the introduction of the perturbation is seen to delay the onset of shear instability on the left side of the particle, while for the case with = 8 the perturbation is shown to sway the (side of) occurrence for axisymmetry as illustrated in Fig. S5c. Incorporating the data from those simulations into Figs. 9-10 (see Figs. S6 and S7), we note that they nicely collapse into the previously observed trends, confirming that the underlying physics remains intact. Fig. S4. The schematic particle/substrate model constructed for the FEA simulation with exaggerated particle size. Red rectangular region with height of 0.0006 mm (one element size in this study) is deleted in order to apply a small geometrical perturbation. S5 Fig. S5. (a) Deformed particle/substrate configurations and temperature contours at the onset of shear instability in models without (top row) and with perturbation (bottom row). Temperature evolution curves for the most critical particle element and its corresponding symmetric element at friction coefficient equal to (b) 0.25 and (c) 8 for the full-particle model with and without perturbation. The acronyms L and R represent the two symmetric elements from the left and right sides of the particle with one being the most critical particle element and the other being its symmetric element. S6 Fig. S6. (a) Onset time and (b) von Mises stress versus the ̅̅̅̅̅̅̅̅ 𝑃𝐸𝐸𝑄 at the onset of shear instability for models with different contact conditions with (open symbols) and without (solid symbols) normal constraint. The dashed line in (a) is drawn to guide the eyes while the line in (b) represents the linear fitting of data. The red triangles are data calculated from simulations with added perturbation. ̃ 𝑃 (see Eq. 3) versus the onset time at the onset of shear instability for Fig. S7. The energy measure, 𝑊 models with different contact conditions with (open symbols) and without (solid symbols) normal constraint. The dashed line represents the linear fitting of data. The red triangles are data calculated from simulations with added perturbation. S7 References 1. 2. 3. 4. 5. 6. H. Assadi, F. Gärtner, T. Stoltenhoff, and H. Kreye, Bonding Mechanism in Cold Gas Spraying, Acta Mater., 2003, 51(15), p. 4379-4394 M. Grujicic, J.R. Saylor, D.E. Beasley, W.S. DeRosset, and D. Helfritch, Computational Analysis of the Interfacial Bonding Between Feed-Powder Particles and the Substrate in the Cold-Gas Dynamic-Spray Process, Appl. Surf. Sci., 2003, 219(3), p. 211-227 S. Guetta, M.-H. Berger, F. Borit, V. Guipont, M. Jeandin, M. Boustie, Y. Ichikawa, K. Sakaguchi, and K. Ogawa, Influence of Particle Velocity on Adhesion of Cold-Sprayed Splats, J. Therm. Spray Technol., 2009, 18(3), p. 331-342 P.C. King, G. Bae, S.H. Zahiri, M. Jahedi, and C. 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