Solid-State Dewetting: From Flat to Curved Substrates
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1 Solid-State Dewetting: From Flat to Curved Substrates Yan Wang with Prof. Weizhu Bao, Prof. David J. Srolovitz, Prof. Wei Jiang and Dr. Quan Zhao IMS, 2 May, 2018 Wang Yan (CSRC) Solid-State Dewetting 1 / 50
2 Outline 1 Introduction 2 Mathematical models Flat substrate Curved substrate 3 Numerical results 4 Summary and future works Wang Yan (CSRC) Solid-State Dewetting 2 / 50
3 Outline 1 Introduction 2 Mathematical models Flat substrate Curved substrate 3 Numerical results 4 Summary and future works Wang Yan (CSRC) Solid-State Dewetting 3 / 50
4 Background Wang Yan (CSRC) Solid-State Dewetting 4 / 50
5 Background Solid-state dewetting Thin films are generally metastable in the as-deposited state and will dewet or agglomerate to form arrays of islands when heated. This process occurs well below the melting temperature of the solid material. Figure: A schematic view of solid-state dewetting. Thin films dewet to form isolated islands when it remains in the solid state (M. Naffouti et al., 2017). Wang Yan (CSRC) Solid-State Dewetting 5 / 50
6 Application Suppress dewetting Thin films are basic components in many microelectronic and optoelectronic devices, and for these devices to function properly, the structural integrity of the thin films must be maintained. Dewetting destabilizes a thin film structure and limits the device reliability. Induce dewetting Ordered arrays of metal nanoparticles has a wide range of potential applications in plasmonics, magnetic memories, DNA detection and catalysis for nanowire and nanotube growth. Dewetting (template-assisted dewetting, dewetting of single crystal thin film) provides a easy way to produce ordered arrays of nanoparticles of controlled size and geometry. Wang Yan (CSRC) Solid-State Dewetting 6 / 50
7 Experimental results Dewetting on a flat substrate generally leads to disordered arrays of islands, the irregularities of dewetting morphologies have limited the application for fabrication of ordered structures. Figure: Dewetting of 30-nm-thick gold films on a flat substrate. (E. Jiran and C.V. Thompson, 1990). Wang Yan (CSRC) Solid-State Dewetting 7 / 50
8 Experimental results Dewetting on a flat substrate generally leads to disordered arrays of islands, the irregularities of dewetting morphologies have limited the application for fabrication of ordered structures. Figure: Dewetting of a single-crystal Si film on oxidized Si on a flat substrate. (R. Nuryadi et. al., 1990). Wang Yan (CSRC) Solid-State Dewetting 7 / 50
9 Experimental results Template-assisted dewetting, i.e., dewetting on a pre-patterned (curved) substrate can lead to formation of ordered structures. Figure: Template-assisted solid-state dewetting of gold films on oxidized silicon surfaces patterned with arrays of inverted pyramid shaped pits. (A.L. Giermann and C.V. Thompson, 2005). Wang Yan (CSRC) Solid-State Dewetting 7 / 50
10 Experimental results Template-assisted dewetting, i.e., dewetting on a pre-patterned (curved) substrate can lead to formation of ordered structures. Figure: Dewetting of Ni(100) (J. Ye and C.V. Thompson, 2011). Wang Yan (CSRC) Solid-State Dewetting 7 / 50
11 Schematic illustration xc, l xc r are the contact points γ VS, γ FS are vapor/substrate and film/substrate interfacial energy densities (usually treated as constants) γ FV = γ(θ) is the film/vapor interfacial energy density, where θ is the normal angle of the film/vapor interface Wang Yan (CSRC) Solid-State Dewetting 8 / 50
12 Film/vapor interfacial energy densities The smooth case: γ(θ) C 2 ([ π, π]) Isotropic case: γ(θ) is a constant. Weakly anisotropic case: γ(θ) := γ(θ) + γ (θ) > 0, θ [ π, π]. Strongly anisotropic case: γ(θ) < 0 for some θ [ π, π]. The cusped case: γ(θ) is piecewise smooth (C 2 ) and not differentiable at finite points. Figure: Different energy densities. Wang Yan (CSRC) Solid-State Dewetting 9 / 50
13 Equilibrium problem Energy minimization problem (J. Gibbs, 1878; G. Wulff, 1901; J. Taylor, 1974; I. Fonseca and S. Müller, 1991; R. Kaischew, 1950; W. Winterbottom, 1967; W. Bao et al., 2017) min Ω W = ( ) γ FV dγ FV + γfs γ VS dγfs Γ FV Γ } FS {{} Substrate Energy s.t. Ω = const. Wang Yan (CSRC) Solid-State Dewetting 10 / 50
14 Dynamic problem Surface diffusion (mass transport) (W. Mullins, 1957; J. Cahn and D. Hoffman, 1974) Chemical potential: Mass flux: µ = Ω 0 δw δγ, J = D sν k B T e s µ, Normal velocity: V n = Ω 0 s J = D sνω 0 k B T e 2 s µ. Wang Yan (CSRC) Solid-State Dewetting 11 / 50
15 Dynamic problem Surface diffusion (mass transport) Moving contact line At the equilibrium state, the following (isotropic) Young equation should be satisfied (T. Young, 1805): γ VS = γ FS + γ 0 cos θ i. Vapor γ V S γ F V γ 0 θ i γ F S Film Substrate Wang Yan (CSRC) Solid-State Dewetting 11 / 50
16 Existing models/methods 1 Sharp interface model/methods: D. Srolovitz and S. Safran (1986): Isotropic, cylindrically symmetric case; H. Wong et al. (2000): Isotropic, semi-infinite step in 2D, and a marker-particle method P. Du et al. (2010): Isotropic, cylindrical wire Wang et al. (2015); Jiang et al., (2016); Bao et al., (2017): Anisotropic case in 2D, and a parametric finite element method 2 Phase field model: Isotropic case (W. Jiang et al., 2012; M. Naffouti et al., 2017); Weakly anisotropic case (M. Dziwnik et al., 2017) 3 Others (e.g. E. Dornel et al., 2006; L. Klinger and E. Rabkin, 2011; R.V. Zucker et al., 2013; O. Pierre-Louis et al., 2009; T. Lee et al., 2015) Wang Yan (CSRC) Solid-State Dewetting 12 / 50
17 Objective Mathematical modeling Rigorously derive the sharp interface model; Include the interfacial anisotropy; Consider both flat and curved substrates. Numerical simulation Equilibrium; Morphological evolution; Template-assisted dewetting;... Wang Yan (CSRC) Solid-State Dewetting 13 / 50
18 Outline 1 Introduction 2 Mathematical models Flat substrate Curved substrate 3 Numerical results 4 Summary and future works Wang Yan (CSRC) Solid-State Dewetting 14 / 50
19 Outline 1 Introduction 2 Mathematical models Flat substrate Curved substrate 3 Numerical results 4 Summary and future works Wang Yan (CSRC) Solid-State Dewetting 15 / 50
20 Thermodynamic variation: Perturbation n θ τ Γ ǫ = Γ + ǫϕ(s)n + ǫψ(s)τ Γ Vapor Film x l c Substrate x r c Derive the model via thermodynamic variation; Perturb Γ in both normal and tangent directions; ψ(s) is an arbitrary function, and ϕ(s) satisfies L ϕ(s)ds = 0. 0 Wang Yan (CSRC) Solid-State Dewetting 16 / 50
21 Thermodynamic variation: Perturbation n θ τ Γ ǫ = Γ + ǫϕ(s)n + ǫψ(s)τ Γ Vapor Film x l c Substrate x r c We express Γ = (x(s), y(s)), Γ ɛ = (x ɛ (s), y ɛ (s)) = (x(s) + ɛu(s), y(s) + ɛv(s)). Then the increments along the y axis at the two contact points must be zero, i.e., v(0) = v(l) = 0. Wang Yan (CSRC) Solid-State Dewetting 16 / 50
22 Thermodynamic variation 1 The total interfacial energy before perturbation is: W = γ(θ) dγ + (γ FS γ VS )(xc r xc) l = Γ L 0 γ(θ) ds + (γ FS γ VS )(x r c x l c). The total free energy W ɛ of the new curve Γ ɛ as follows: W ɛ = = Γɛ γ(θ ɛ ) dγ ɛ + ( γ FS γ VS ) [ (x rc + ɛu(l) ) ( x lc + ɛu(0) )] L 0 ( γ arctan ( y s + ɛv s ) ) (x s + ɛu s ) x s + ɛu 2 + (y s + ɛv s ) 2 ds s + ( γ FS γ VS ) [ ( x r c + ɛu(l) ) ( x l c + ɛu(0) )]. Wang Yan (CSRC) Solid-State Dewetting 17 / 50
23 Thermodynamic variation 2 dw ɛ dɛ = ɛ=0 L ( ) γ (θ) + γ(θ) κ ϕ ds 0 [ + γ(θd l ) cos θl d γ (θd l ) sin θl d + ( ) ] γ FS γ VS u(0) [ γ(θd r ) cos θr d γ (θd r ) sin θr d + ( ) ] γ FS γ VS u(l). Chemical potential: δw ( ) µ = Ω 0 δγ = Ω 0 γ(θ) + γ (θ) κ, Surface normal velocity: V n = D sνω 0 k B T e 2 µ s 2. Wang Yan (CSRC) Solid-State Dewetting 18 / 50
24 Thermodynamic variation 2 dw ɛ dɛ = ɛ=0 L ( ) γ (θ) + γ(θ) κ ϕ ds 0 [ + γ(θd l ) cos θl d γ (θd l ) sin θl d + ( ) ] γ FS γ VS u(0) [ γ(θd r ) cos θr d γ (θd r ) sin θr d + ( ) ] γ FS γ VS u(l). Assuming that the moving process of the contact point can be taken as an energy gradient flow: dx l c(t) dt dx r c (t) dt = η δw δxc l = η δw δxc r [ = η γ(θd l ) cos θl d γ (θd l ) sin θl d + ( ) ] γ FS γ VS, [ = η γ(θd r ) cos θr d γ (θd r ) sin θr d + ( ) ] γ FS γ VS. Wang Yan (CSRC) Solid-State Dewetting 18 / 50
25 Governing equation According to the thermodynamic principle, we have the following dimensionless sharp-interface model for weakly anisotropic solid-state dewetting problems: X t = V nn = 2 µ s 2 n ( ) µ = γ(θ) + γ (θ) κ, where κ = ss x s y s x ss y is the curvature. Wang Yan (CSRC) Solid-State Dewetting 19 / 50
26 Boundary conditions 1 Contact Point Condition (BC1) y(xc, l t) = 0, y(xc r, t) = 0. 2 Relaxed Contact Angle Condition (BC2) where dx l c dt = ηf (θl d ), dx r c dt = ηf (θr d ), f (θ) := γ(θ) cos θ γ (θ) sin θ σ, with σ := γ VS γ FS γ 0. 3 Zero-Mass Flux Condition (BC3) µ s (x l c, t) = 0, µ s (x r c, t) = 0. Wang Yan (CSRC) Solid-State Dewetting 20 / 50
27 Regularization X t = 2 [( ) ] s 2 γ(θ) + γ (θ) κ n, Well-posed in the isotropic and weakly anisotropic cases, i.e., γ(θ) := γ(θ) + γ (θ) > 0 for all θ [0, 2π]; Ill-posed in the strongly anisotropic case where γ(θ) may become negative for some θ. In order to regularize the equation, a high order regularization term can be added to the free energy (M.E. Gurtin and M.E. Jabbour, 2002; S. Torabi et al., 2009): W w = ε2 2 Γ κ 2 dγ Wang Yan (CSRC) Solid-State Dewetting 21 / 50
28 Governing equation (strong anisotropy) By calculating the variation of the regularized interfacial energy W + W w, we can form the dimensionless model for the strongly anisotropic case as: µ = X t = V nn = 2 µ s 2 n, ( γ(θ) + γ (θ) )κ ε (κ 2 ss + κ3 2 where κ = ss x s y s x ss y is the curvature. ), Wang Yan (CSRC) Solid-State Dewetting 22 / 50
29 Boundary conditions (strong anisotropy) 1 Contact Point Condition (BC1) y(xc, l t) = 0, y(xc r, t) = 0. 2 Relaxed Contact Angle Condition (BC2) dx l c dt = ηf ε(θ l d ), dx r c dt = ηf ε(θ r d ), where f ε (θ) := γ(θ) cos θ γ (θ) sin θ σ ε 2 κ (θ) sin θ. s 3 Zero-Mass Flux Condition (BC3) µ s (x l c, t) = 0, 4 Zero-curvature Condition (BC4) µ s (x r c, t) = 0. κ(x l c, t) = 0, κ(x r c, t) = 0. Wang Yan (CSRC) Solid-State Dewetting 23 / 50
30 Outline 1 Introduction 2 Mathematical models Flat substrate Curved substrate 3 Numerical results 4 Summary and future works Wang Yan (CSRC) Solid-State Dewetting 24 / 50
31 Schematic illustration on a curved substrate n θ τ γ F V = γ(θ) Film Γ Vapor c l Substrate Γ sub c r Figure: A schematic illustration of a film island in two dimension. Interfacial energy densities: γ FV = γ(θ), γ FS and γ VS are contants. The interfacial energy: W = γ(θ) dγ + ( ) γ FS γ VS (cr c l ), Γ }{{} Substrate Energy Wang Yan (CSRC) Solid-State Dewetting 25 / 50
32 Thermodynamic variation Similarly, we can perturb the film/vapor interface and calculate the thermodynamic variation of the total interfacial energy as δw δγ = ( ) γ(θ) + γ (θ) κ, δw = γ(θ δc ex) r cos θin r γ (θex) r sin θin r + (γ FS γ VS ), r δw [ ] = γ(θ l δc ex) cos θin l γ (θex) l sin θin l + (γ FS γ VS ). l Wang Yan (CSRC) Solid-State Dewetting 26 / 50
33 Thermodynamic variation Similarly, we can perturb the film/vapor interface and calculate the thermodynamic variation of the total interfacial energy as δw δγ = ( ) γ(θ) + γ (θ) κ, δw = γ(θ δc ex) r cos θin r γ (θex) r sin θin r + (γ FS γ VS ), r δw [ ] = γ(θ l δc ex) cos θin l γ (θex) l sin θin l + (γ FS γ VS ). l Wang Yan (CSRC) Solid-State Dewetting 26 / 50
34 Model formulation The two-dimensional solid-state dewetting of a thin film on a rigid curved solid substrate can be described in the following dimensionless form by the sharp interface model (isotropic/weakly anisotropic case): X t = V nn = 2 µ s 2 n ( ) µ = γ(θ) + γ (θ) κ, where κ = ss x s y s x ss y is the curvature. Wang Yan (CSRC) Solid-State Dewetting 27 / 50
35 Boundary conditions for the weakly anisotropic case 1 Contact point condition (BC1) X(0, t) = X sub (c l ), X(L, t) = X sub (c r ). 2 Relaxed contact angle condition (BC2) dc l dt = ηf (θl ex, θ l in), where the binary function f is defined as dc r dt = ηf (θr ex, θ r in), f (θ ex, θ in ) := γ(θ ex ) cos θ in γ (θ ex ) sin θ in σ, with the dimensionless coefficient σ := (γ VS γ FS )/γ 0 = cos θ i. 3 Zero-mass flux condition (BC3) µ s (s = 0, t) = 0, µ (s = L, t) = 0, s Wang Yan (CSRC) Solid-State Dewetting 28 / 50
36 Outline 1 Introduction 2 Mathematical models Flat substrate Curved substrate 3 Numerical results 4 Summary and future works Wang Yan (CSRC) Solid-State Dewetting 29 / 50
37 Isotropic, short island L = 5,β = 0,σ = cos(3π/4) Wang Yan (CSRC) Solid-State Dewetting 30 / 50
38 Weakly anisotropic, short island L = 5,m = 4,β = 0.06,σ = cos(3π/4) Wang Yan (CSRC) Solid-State Dewetting 31 / 50
39 Strongly anisotropic, short island L = 5,m = 4,β = 0.2,σ = cos(3π/4) Wang Yan (CSRC) Solid-State Dewetting 32 / 50
40 Weakly anisotropic, long island L = 60,m = 4,β = 0.06,σ = cos(5π/6) Wang Yan (CSRC) Solid-State Dewetting 33 / 50
41 Critical length for pinch-off L or more L or more /sin( i /2) γ(θ) = cos(4θ), /sin( i /2) γ(θ) = cos(4θ) Wang Yan (CSRC) Solid-State Dewetting 34 / 50
42 Weakly anisotropic, semi-infinite island m = 4,β = 0.06,σ = cos(5π/6) Power-law for the retraction distance: l t 0.4 (H. Wong et al., 2000) Wang Yan (CSRC) Solid-State Dewetting 35 / 50
43 Power law Retraction distance 10 2 β = θ i = 5π/6 θ = 3π/4 i θ = 2π/3 i θ i = π/2 θ =π/3 i θ =π/4 i t Wang Yan (CSRC) Solid-State Dewetting 36 / 50
44 Hole: Dewetting I β = 0.06, m = 4, σ = cos(π/2). (a) d = Wang Yan (CSRC) Solid-State Dewetting 37 / 50
45 Hole: Wetting II β = 0.06, m = 4, σ = cos(π/2). (b) d = Wang Yan (CSRC) Solid-State Dewetting 38 / 50
46 Hole: Void III β = 0.06, m = 4, σ = cos(π/2). (c) d = Wang Yan (CSRC) Solid-State Dewetting 39 / 50
47 Hole Wang Yan (CSRC) Solid-State Dewetting 40 / 50
48 Equilibria on a sawtooth substrate Figure: (a1-a2): Two equilibrium shapes of thin films on a sawtooth substate with initial area A = 2. Wang Yan (CSRC) Solid-State Dewetting 41 / 50
49 Asymmetric equlibrium (a1) (b1) (a2) (b2) (a3) (b3) (a4) (b4) Figure: Evolution of thin films on a circular substrate (R = 20). (a) isotropic case, (b) weakly anisotropic case with m = 4, β = σ = 0.5 in both cases. The intrinsic (contact) angles in (b4) are (left) and (right) Wang Yan (CSRC) Solid-State Dewetting 42 / 50
50 Pinch-off (a) (b) (c) (d) Figure: Evolution of a large island with isotropic surface energy on a spherical substrate of radius R = 30. Film length L = 82, σ = 3/2. Wang Yan (CSRC) Solid-State Dewetting 43 / 50
51 Pinch-off L (a) 1 2 or more /sin( i /2) L (b) 1 2 or more /sin( i /2) R = 30 R = 60 Wang Yan (CSRC) Solid-State Dewetting 44 / 50
52 Pinch-off Assuming isotropic surface energy, for given R and θ i, we suggest that the critical pinch-off length can be predicted according to the following relation L = 320.2/R , R 10. (1) sin(θ i /2) Here, the radius is restricted to be larger than 10 since pinch-off won t occur for small R. Wang Yan (CSRC) Solid-State Dewetting 45 / 50
53 Movement on a sinusoidal substrate L = 5,β = 0,σ = cos(π/3) y = 4sin(x/4) Wang Yan (CSRC) Solid-State Dewetting 46 / 50
54 Templated solid-state dewetting Consider sinusoidal substates y = H sin(wx). Consider enough long films. (a) (b) (c) Figure: Dewetting of thin films with different length on a pre-patterned sinusoidal substrate. The lengths of the films are L = 100, 150 and 200. Wang Yan (CSRC) Solid-State Dewetting 47 / 50
55 Templated solid-state dewetting I II III IV (I) 1.2 (II) H [R0] (III) πω [1/R 0 ] Figure: Phase diagram of the four observed categories of solid-state dewetting of thin films on pre-patterned sinusoidal substrates y = H sin(wx) (IV) Wang Yan (CSRC) Solid-State Dewetting 48 / 50
56 Templated solid-state dewetting Wang Yan (CSRC) Solid-State Dewetting 48 / 50
57 Outline 1 Introduction 2 Mathematical models Flat substrate Curved substrate 3 Numerical results 4 Summary and future works Wang Yan (CSRC) Solid-State Dewetting 49 / 50
58 Summary and future works Summary Proposed sharp interface models for solid-state dewetting problems in 2D for both flat and curved substrates. Presented a series of numerical results to show the influence of anisotropy and curved substrates in solid-state dewetting. Future works Analysis for the physical laws that we observed or summarized from numerical studies. 3D simulations....
59 Summary and future works Thank You for Your Attention!
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