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Fluctuations and rare events in stochastic
                  aggregation

                                Colm Connaughton

             Mathematics Institute and Centre for Complexity Science,
                           University of Warwick, UK

Collaborators: R. Rajesh (Chennai), R. Tribe (Warwick), O. Zaboronski (Warwick).


 IUTAM Syposium - Common aspects of extreme events in
                         fluids
        University College Dublin July 2-6, 2012

                                                                             ./figures/warwickL



        http://www.slideshare.net/connaughtonc   Stochastic aggregation
Introduction to cluster-cluster aggregation (CCA)



                                                                 Many particles of one
                                                                 material dispersed in
                                                                 another.
                                                                 Transport: diffusive,
                                                                 advective, ballistic...
                                             Particles stick together on
                                             contact.
  Applications: surface and colloid physics, atmospheric
  science, biology, cloud physics, astrophysics...



                                                                                     ./figures/warwickL



          http://www.slideshare.net/connaughtonc   Stochastic aggregation
Mean-field model: Smoluchowski’s kinetic equation

  Cluster size distribution, Nm (t), satisfies the kinetic equation :
  Smoluchowski equation :

                                 m
  ∂Nm (t)             1
               =                     dm1 dm2 K (m1 , m2 )Nm1 Nm2 δ(m − m1 − m2 )
    ∂t                2      0
                            ∞
               −                 dm1 dm2 K (m, m1 )Nm Nm1 δ(m2 − m − m1 )
                        0
                      J
               +         δ(m − m0 )
                      m0

      Source of monomers: input mass flux J.
      Assumes no correlations.
      Very extensive literature on this equation.
                                                                              ./figures/warwickL



            http://www.slideshare.net/connaughtonc   Stochastic aggregation
Mass cascades in CCA with a source and sink

                                           Kernel is often homogeneous:
                                                       K (am1 , am2 ) = aβ K (m1 , m2 )

                                           Today we will mostly consider the con-
                                           stant kernel (β = 0):
                                                                    K (m1 , m2 ) = λ.
           K (m1 , m2 ) = 1.




  Stationary state for t → ∞, m                        m0 (White 1967):
                                                   √          β+3
                                  Nm = c               J m−    2    .

  Describes a cascade of mass from source at m0 to sink at large
  m. Analogous to the Richardson cascade in turbulence.      ./figures/warwickL



          http://www.slideshare.net/connaughtonc        Stochastic aggregation
Stochastic Particle System Model of Aggregation
  Consider a lattice in d dimensions with particles of integer
  masses. Nt (x, m)=number of particles of mass m on site x at
  time t.

      Diffusion:                 Nt (x, m) → Nt (x, m) − 1
                                 Nt (x + n, m) → Nt (x + n, m) + 1
      Rate:                      DNt (x, m)/2d
      Aggregation:               Nt (x, m1 ) → Nt (x, m1 ) − 1
                                 Nt (x, m2 ) → Nt (x, m2 ) − 1
                                 Nt (x, m1 + m2 ) → Nt (x, m1 + m2 ) + 1
      Rate:                      λNt (x, m1 )Nt (x, m2 )
      Injection:                 Nt (x, m) → Nt (x, m) + 1
      Rate:                      J
                                                                            ./figures/warwickL



          http://www.slideshare.net/connaughtonc   Stochastic aggregation
Path integral representation of correlation functions

  Stochastic particle system can be reformulated as a statistical
  field theory (Doi, Peliti, Zeldovich, Ovchinnikov, Cardy...)

                                                                       ¯
                          nm =              D[zm , zm ] zm e−Seff [zm ,zm ]
                                                   ¯                                  (1)

  where
                T
  Seff =            dτ dx           ¯                              ¯
                                    zm (∂t zm − D∆zm − Jδm,1 ) + H[zm + 1, zm ]
            0                  m

  and
                             1
             ¯
           H[z , z] = −                              ¯         ¯ ¯
                                            λm1 ,m2 (zm1 +m2 − zm1 zm2 ) zm1 zm2 .
                             2     m1 ,m2

                                                                                     ./figures/warwickL



             http://www.slideshare.net/connaughtonc    Stochastic aggregation
Diffusive fluctuations in d ≤ 2

  Critical dimension for the theory is 2. Below 2-d diffusive
  fluctuations cause mean field theory to fail.
  Exact solution (Takayasu 1985)for size distribution in 1-d
  (constant kernel):
                                     1       4                                  3
                   Nm = c J 3 m − 3                cf MF: Nm ∼ m− 2 .

  Renormalisation of reaction rate within perturbative RG
  framework ( = 2 − d):




                                                   d          2d+2
                                   Nm ∼ J d+2 m− d+2
  Leading term in RG expansion is exact in d = 1 ( = 1)!                            ./figures/warwickL



          http://www.slideshare.net/connaughtonc       Stochastic aggregation
Multiscaling and intermittency

  For d ≤ 2 higher order mass correlation functions exhibit
  multi-scaling with m:

          Cn = Nm1 . . . Nmn ∼ m−γn                                           3
                                                                   MF: γn = n 2

                                                   γ0 = 0.
                                                          4
                                                   γ1 =   3   in 1-d (exact solution).
                                                   γ2 = 3 is exact (analogue of
                                                   4
                                                   5 -law!).
                                                   These are not on a straight line.
                                                   RG calculation gives:
                                                   γn = 2d+2 n + d+2 n(n−1) + O( 2 )
                                                         d+2            2
                                                   where = 2 − d.
                                                                                    ./figures/warwickL



          http://www.slideshare.net/connaughtonc    Stochastic aggregation
Origin of intermittency: anti-correlation between
clusters

  “Large particles are large because they have merged with all of
  their neighbours".
                                                   Due to recurrence of random
                                                   walks in d < 2 particles
                                                   encounter their neighbours
                                                   infinitely often.
                                                   Large particles surrounded by
                                                   voids (correlation hole) and are
                                                   thus spatially correlated.
  Spatial intermittency of the mass distribution in low dimensions
  is due to sites having atypically few or atypically many particles.
                                                                               ./figures/warwickL



          http://www.slideshare.net/connaughtonc    Stochastic aggregation
Rare events in stochastic aggregation

  Can we calculate probabilities of atypical configurations?
  Spatial problem is hard. Start with a simpler 0-d problem:
      Initial condition: M particles of size 1. No source.
      Particles aggregate at rate λ.
      What is annihilation time, τ , when 1 particle remains?

  Mean-field equation for total number of particles:
                    ˙    λ
                    N = − N2      N(0) = M.
                         2
  Solution: N(t) = 2M/(2 + Mλ t) ⇒ τMF = 2/λ for large M.

  Two types of rare events in limit M                     1:
      Fast annihilation: P(N(τ ) = 1) with τ                                τMF .
      Slow annihilation: P(N(τ ) > 1) with τ                                τMF .   ./figures/warwickL



          http://www.slideshare.net/connaughtonc   Stochastic aggregation
Path integral formula for probabilities
  Path integral formula for probabilities is similar to before but
  includes boundary terms:

                                                                              ¯
                       P(N(T ) = 1) =                 D[zm , zm ] e−Seff [zm ,zm ]
                                                             ¯                        (2)

  where
                   T
    Seff =             dt           ¯
                                    zm ∂t zm               ¯
                                                       + H[zm , zm ]
               0               m


        +               ¯            ¯
                       (zm zm − M ln zm ) δm,1 δ(t) − ln zm δm,M δ(t − T )
               m

  and
                             1
          ¯
        H[z , z] = −                               ¯         ¯ ¯
                                          λm1 ,m2 (zm1 +m2 − zm1 zm2 ) zm1 zm2 .
                             2   m1 ,m2                                              ./figures/warwickL



             http://www.slideshare.net/connaughtonc      Stochastic aggregation
Instanton equations for early annihilation
  If probability of the rare event of interest is concentrated on a
  single trajectory (“instanton") then Seff can be estimated using
  the Laplace method. Trajectory satisfies:
           δH    1
  ˙
  zm = −       =                                         ¯           ¯
                                    λm1 ,m2 (δm,m1 +m2 − zm1 δm,m2 − zm2 δm,m1 ) zm1 zm2
            ¯m
           δz    2m
                            1 ,m2

  ˙    δH     1
  ¯
  zm =     =−                                  ¯         ¯ ¯
                                      λm1 ,m2 (zm1 +m2 − zm1 zm2 )(zm1 δm,m2 + zm2 δm,m1 )
       δzm    2m                 m2
                            1,

  with boundary conditions:
                  ¯
           zm (0) zm (0) = M δm,1                           ¯
                                                    zm (T ) zm (T ) = 1 δm,M .
  Integrals of motion:
       E = H(z c , z c ) (’Instanton energy’)
                   ¯
                     c ¯c
       M = m mzm zm (Mass)
  Find that:
                                                                                 ./figures/warwickL
                    Seff = −E · t + boundary terms
           http://www.slideshare.net/connaughtonc    Stochastic aggregation
Solution of the instanton equations for constant kernel

  Task: find the value of E for which the boundary conditions are
                                                           ¯
  satisfied. For constant kernel, can solve for N = m zm (t)zm (t):

                      λ
              ∂t N = − N 2 + E,                     N(0) = M            N(T ) = 1.
                      2
  Solution:
      Know E < 0 so let E = − λ p2 .
                              2

                              λ                                          2      M
                N(t) = p tan p (t − t0 )                       t0 =        tan−1 .
                              2                                         λp      p
                                                                 π
      For M → ∞ and t → 0, we find p ∼                            λt .
  Obtain
                                          π2
           P(N(T ) = 1) ∼ e− 2 λ T                  for T       τMF and M            1.
                                                                                          ./figures/warwickL



           http://www.slideshare.net/connaughtonc    Stochastic aggregation
Late annihilation
  The opposite regime of late annihilation is not described by
  previous instanton equations. For T      τMF then
  P(N(T ) > 1) ≈ P(N(T ) = 2). Exact equation for ∂t N(t) :
                                 λ
                      ∂t N = − N (N − 1)
                                 2
  For late times N(t) = 1 + n(t) with n(t) ∈ {0, 1} and
                                λ
                      ∂t n = − ( n 2 + n )
                                2
                           = −λ n       since n2 = n
                            ⇒ n ∼ e−λt
             ⇒ P(n(t) = 1) ∼ e−λt


  Probability of late annihilation

                    P(N(T ) > 1) ∼ e−λt                  for T          τMF   ./figures/warwickL



          http://www.slideshare.net/connaughtonc   Stochastic aggregation
Statistics of mass flux fluctuations
  Analogue of the mass flux for toy model: J = M (τ is the
                                                τ
  annihilation time). JMF = τM = Mλ . Consider relative size of
                             MF   2
  fluctuations of J above and below JMF .

                              M         π 2 J+
           P(J > J+ ) = P(τ <    ) ∼ e− 2λM     as M → ∞
                              J+
                              M       − λM
           P(J < J− ) = P(τ >    ) ∼ e J−      as M → ∞
                              J−

  Take J+ = LJMF , J− = JMF . Fluctuations are not symmetric with
                         L
  respect to L:
                     P(J > JMF L)        π2
                                    ∼ e−( 4 −1)L
                    P(J < JMF /L)
  Large fluxes are exponentially less probable than small ones.
  Reminiscent of Gallavotti-Cohen Fluctuation Relation for
  entropy production in dynamical systems.                   ./figures/warwickL



          http://www.slideshare.net/connaughtonc   Stochastic aggregation
Conclusions
     Cluster-cluster aggregation exhibits non-equilibrium
     statistical dynamics which are closely analogous to
     turbulence with a mass cascade playing the role of the
     energy cascade.
     CCA with diffusive transport has a critical dimension of 2.
     Unlike turbulence, the RG flow for this system has a stable
     perturbative fixed point in d < 2 of order = 2 − d.
     Mass distribution exhibits spatial intermittency due to
     anti-correlation between particles. Multi-scaling exponents
     can be calculated by RG.
     Probabilities of rare configurations can be calculated using
     “instanton" method (at least in 0-d). Instanton equations
     are very closely related to mean-field equations.
     Fluctuations of the mass flux exhibit a (geometric)
     asymmetry which is very reminiscent of various “fluctuation
                                                              ./figures/warwickL
     relations" in other non-equilibrium systems.
         http://www.slideshare.net/connaughtonc   Stochastic aggregation

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Fluctuations and rare events in stochastic aggregation

  • 1. Fluctuations and rare events in stochastic aggregation Colm Connaughton Mathematics Institute and Centre for Complexity Science, University of Warwick, UK Collaborators: R. Rajesh (Chennai), R. Tribe (Warwick), O. Zaboronski (Warwick). IUTAM Syposium - Common aspects of extreme events in fluids University College Dublin July 2-6, 2012 ./figures/warwickL http://www.slideshare.net/connaughtonc Stochastic aggregation
  • 2. Introduction to cluster-cluster aggregation (CCA) Many particles of one material dispersed in another. Transport: diffusive, advective, ballistic... Particles stick together on contact. Applications: surface and colloid physics, atmospheric science, biology, cloud physics, astrophysics... ./figures/warwickL http://www.slideshare.net/connaughtonc Stochastic aggregation
  • 3. Mean-field model: Smoluchowski’s kinetic equation Cluster size distribution, Nm (t), satisfies the kinetic equation : Smoluchowski equation : m ∂Nm (t) 1 = dm1 dm2 K (m1 , m2 )Nm1 Nm2 δ(m − m1 − m2 ) ∂t 2 0 ∞ − dm1 dm2 K (m, m1 )Nm Nm1 δ(m2 − m − m1 ) 0 J + δ(m − m0 ) m0 Source of monomers: input mass flux J. Assumes no correlations. Very extensive literature on this equation. ./figures/warwickL http://www.slideshare.net/connaughtonc Stochastic aggregation
  • 4. Mass cascades in CCA with a source and sink Kernel is often homogeneous: K (am1 , am2 ) = aβ K (m1 , m2 ) Today we will mostly consider the con- stant kernel (β = 0): K (m1 , m2 ) = λ. K (m1 , m2 ) = 1. Stationary state for t → ∞, m m0 (White 1967): √ β+3 Nm = c J m− 2 . Describes a cascade of mass from source at m0 to sink at large m. Analogous to the Richardson cascade in turbulence. ./figures/warwickL http://www.slideshare.net/connaughtonc Stochastic aggregation
  • 5. Stochastic Particle System Model of Aggregation Consider a lattice in d dimensions with particles of integer masses. Nt (x, m)=number of particles of mass m on site x at time t. Diffusion: Nt (x, m) → Nt (x, m) − 1 Nt (x + n, m) → Nt (x + n, m) + 1 Rate: DNt (x, m)/2d Aggregation: Nt (x, m1 ) → Nt (x, m1 ) − 1 Nt (x, m2 ) → Nt (x, m2 ) − 1 Nt (x, m1 + m2 ) → Nt (x, m1 + m2 ) + 1 Rate: λNt (x, m1 )Nt (x, m2 ) Injection: Nt (x, m) → Nt (x, m) + 1 Rate: J ./figures/warwickL http://www.slideshare.net/connaughtonc Stochastic aggregation
  • 6. Path integral representation of correlation functions Stochastic particle system can be reformulated as a statistical field theory (Doi, Peliti, Zeldovich, Ovchinnikov, Cardy...) ¯ nm = D[zm , zm ] zm e−Seff [zm ,zm ] ¯ (1) where T Seff = dτ dx ¯ ¯ zm (∂t zm − D∆zm − Jδm,1 ) + H[zm + 1, zm ] 0 m and 1 ¯ H[z , z] = − ¯ ¯ ¯ λm1 ,m2 (zm1 +m2 − zm1 zm2 ) zm1 zm2 . 2 m1 ,m2 ./figures/warwickL http://www.slideshare.net/connaughtonc Stochastic aggregation
  • 7. Diffusive fluctuations in d ≤ 2 Critical dimension for the theory is 2. Below 2-d diffusive fluctuations cause mean field theory to fail. Exact solution (Takayasu 1985)for size distribution in 1-d (constant kernel): 1 4 3 Nm = c J 3 m − 3 cf MF: Nm ∼ m− 2 . Renormalisation of reaction rate within perturbative RG framework ( = 2 − d): d 2d+2 Nm ∼ J d+2 m− d+2 Leading term in RG expansion is exact in d = 1 ( = 1)! ./figures/warwickL http://www.slideshare.net/connaughtonc Stochastic aggregation
  • 8. Multiscaling and intermittency For d ≤ 2 higher order mass correlation functions exhibit multi-scaling with m: Cn = Nm1 . . . Nmn ∼ m−γn 3 MF: γn = n 2 γ0 = 0. 4 γ1 = 3 in 1-d (exact solution). γ2 = 3 is exact (analogue of 4 5 -law!). These are not on a straight line. RG calculation gives: γn = 2d+2 n + d+2 n(n−1) + O( 2 ) d+2 2 where = 2 − d. ./figures/warwickL http://www.slideshare.net/connaughtonc Stochastic aggregation
  • 9. Origin of intermittency: anti-correlation between clusters “Large particles are large because they have merged with all of their neighbours". Due to recurrence of random walks in d < 2 particles encounter their neighbours infinitely often. Large particles surrounded by voids (correlation hole) and are thus spatially correlated. Spatial intermittency of the mass distribution in low dimensions is due to sites having atypically few or atypically many particles. ./figures/warwickL http://www.slideshare.net/connaughtonc Stochastic aggregation
  • 10. Rare events in stochastic aggregation Can we calculate probabilities of atypical configurations? Spatial problem is hard. Start with a simpler 0-d problem: Initial condition: M particles of size 1. No source. Particles aggregate at rate λ. What is annihilation time, τ , when 1 particle remains? Mean-field equation for total number of particles: ˙ λ N = − N2 N(0) = M. 2 Solution: N(t) = 2M/(2 + Mλ t) ⇒ τMF = 2/λ for large M. Two types of rare events in limit M 1: Fast annihilation: P(N(τ ) = 1) with τ τMF . Slow annihilation: P(N(τ ) > 1) with τ τMF . ./figures/warwickL http://www.slideshare.net/connaughtonc Stochastic aggregation
  • 11. Path integral formula for probabilities Path integral formula for probabilities is similar to before but includes boundary terms: ¯ P(N(T ) = 1) = D[zm , zm ] e−Seff [zm ,zm ] ¯ (2) where T Seff = dt ¯ zm ∂t zm ¯ + H[zm , zm ] 0 m + ¯ ¯ (zm zm − M ln zm ) δm,1 δ(t) − ln zm δm,M δ(t − T ) m and 1 ¯ H[z , z] = − ¯ ¯ ¯ λm1 ,m2 (zm1 +m2 − zm1 zm2 ) zm1 zm2 . 2 m1 ,m2 ./figures/warwickL http://www.slideshare.net/connaughtonc Stochastic aggregation
  • 12. Instanton equations for early annihilation If probability of the rare event of interest is concentrated on a single trajectory (“instanton") then Seff can be estimated using the Laplace method. Trajectory satisfies: δH 1 ˙ zm = − = ¯ ¯ λm1 ,m2 (δm,m1 +m2 − zm1 δm,m2 − zm2 δm,m1 ) zm1 zm2 ¯m δz 2m 1 ,m2 ˙ δH 1 ¯ zm = =− ¯ ¯ ¯ λm1 ,m2 (zm1 +m2 − zm1 zm2 )(zm1 δm,m2 + zm2 δm,m1 ) δzm 2m m2 1, with boundary conditions: ¯ zm (0) zm (0) = M δm,1 ¯ zm (T ) zm (T ) = 1 δm,M . Integrals of motion: E = H(z c , z c ) (’Instanton energy’) ¯ c ¯c M = m mzm zm (Mass) Find that: ./figures/warwickL Seff = −E · t + boundary terms http://www.slideshare.net/connaughtonc Stochastic aggregation
  • 13. Solution of the instanton equations for constant kernel Task: find the value of E for which the boundary conditions are ¯ satisfied. For constant kernel, can solve for N = m zm (t)zm (t): λ ∂t N = − N 2 + E, N(0) = M N(T ) = 1. 2 Solution: Know E < 0 so let E = − λ p2 . 2 λ 2 M N(t) = p tan p (t − t0 ) t0 = tan−1 . 2 λp p π For M → ∞ and t → 0, we find p ∼ λt . Obtain π2 P(N(T ) = 1) ∼ e− 2 λ T for T τMF and M 1. ./figures/warwickL http://www.slideshare.net/connaughtonc Stochastic aggregation
  • 14. Late annihilation The opposite regime of late annihilation is not described by previous instanton equations. For T τMF then P(N(T ) > 1) ≈ P(N(T ) = 2). Exact equation for ∂t N(t) : λ ∂t N = − N (N − 1) 2 For late times N(t) = 1 + n(t) with n(t) ∈ {0, 1} and λ ∂t n = − ( n 2 + n ) 2 = −λ n since n2 = n ⇒ n ∼ e−λt ⇒ P(n(t) = 1) ∼ e−λt Probability of late annihilation P(N(T ) > 1) ∼ e−λt for T τMF ./figures/warwickL http://www.slideshare.net/connaughtonc Stochastic aggregation
  • 15. Statistics of mass flux fluctuations Analogue of the mass flux for toy model: J = M (τ is the τ annihilation time). JMF = τM = Mλ . Consider relative size of MF 2 fluctuations of J above and below JMF . M π 2 J+ P(J > J+ ) = P(τ < ) ∼ e− 2λM as M → ∞ J+ M − λM P(J < J− ) = P(τ > ) ∼ e J− as M → ∞ J− Take J+ = LJMF , J− = JMF . Fluctuations are not symmetric with L respect to L: P(J > JMF L) π2 ∼ e−( 4 −1)L P(J < JMF /L) Large fluxes are exponentially less probable than small ones. Reminiscent of Gallavotti-Cohen Fluctuation Relation for entropy production in dynamical systems. ./figures/warwickL http://www.slideshare.net/connaughtonc Stochastic aggregation
  • 16. Conclusions Cluster-cluster aggregation exhibits non-equilibrium statistical dynamics which are closely analogous to turbulence with a mass cascade playing the role of the energy cascade. CCA with diffusive transport has a critical dimension of 2. Unlike turbulence, the RG flow for this system has a stable perturbative fixed point in d < 2 of order = 2 − d. Mass distribution exhibits spatial intermittency due to anti-correlation between particles. Multi-scaling exponents can be calculated by RG. Probabilities of rare configurations can be calculated using “instanton" method (at least in 0-d). Instanton equations are very closely related to mean-field equations. Fluctuations of the mass flux exhibit a (geometric) asymmetry which is very reminiscent of various “fluctuation ./figures/warwickL relations" in other non-equilibrium systems. http://www.slideshare.net/connaughtonc Stochastic aggregation