- 125
- Spielman
- Lecture 04c - Shortcut Exchanger Design Procedure.ppt
- FM 3-5 NBC Decontamination (2000) WW
- Composite Dan Future IPR - 2010
- foam spray
- pcourseiitd
- EN 147
- AFT Titan 4 Data Sheet
- Deposition Velocity Estimation
- MDV3-VVUQ-v0.5
- Squat
- Clouds Particles
- 978-1-58503-716-2-1
- jammu university mechanical engineering syllabus
- Lecture Slides (3) - Copy.pptx
- Two Phase Flow
- SPE-20421-MS
- LaminarFlowPipes&Annuli Newtonian
- Fluidized Bed
- Effect of Surface Rough Ness on Diffusionlimited Charge Transfer
- Aerodyn Appl Veh 3 Basics
- Pressure Drop Along Pipe Length - Fluid Flow Hydraulic and Pneumatic, Engine
- Sonatrach's _well Performance
- M7l35
- Drop Let Evaporation
- IJETR032825
- out3
- s 0022112070220996
- 54.IJMPERDDEC201754
- 52442
- 52438
- 52209.pdf
- 52143.pdf
- 52376
- 52136.pdf
- 52175.pdf
- 52376.pdf
- 52074
- 52606
- 52356
- 52074.pdf
- 52433
- 52970
- 52310.pdf
- 50761
- 50714
- 52209
- 48951
- 50477
- 52143
- 52310
- 50108
- 50262
- 52136
- 52175
- 49153
- 51678
- 50822

**World's largest Science,
**

Technology & Medicine

Open Access book publisher

2,800+

OPEN ACCESS BOOKS

BOOKS

DELIVERED TO

151 COUNTRIES

97,000+

INTERNATIONAL

AUTHORS AND EDITORS

AUTHORS AMONG

TOP 1%

MOST CITED SCIENTIST

90+ MILLION

DOWNLOADS

12.2%

**AUTHORS AND EDITORS
**

FROM TOP 500 UNIVERSITIES

**Selection of our books indexed in the
**

Book Citation Index in Web of Science™

Core Collection (BKCI)

**Chapter from the book Aerosols - Science and Case Studies
**

Downloaded from: http://www.intechopen.com/books/aerosols-science-and-casestudies

**Interested in publishing with InTechOpen?
**

Contact us at book.department@intechopen.com

Provisional

chapter1

Chapter

Operator

Operator Splitting

Splitting Monte

Monte Carlo

Carlo Method

Method for

for Aerosol

Aerosol

Dynamics

Dynamics

Kun Zhou and Tat Leung Chan

Kun Zhou and Tat Leung Chan

Additional information is available at the end of the chapter

**Additional information is available at the end of the chapter
**

http://dx.doi.org/10.5772/65140

Abstract

Aerosol dynamics are described by the population balance equation (PBE). In principle,

three typical methods (i.e., direct discretization, method of moments, and stochastic

method) have been widely used to solve the PBE. Stochastic method is the most flexible

among the three methods. However, stochastic method is computationally expensive.

Recently, an operator splitting Monte Carlo (OSMC) method has been developed so as

to improve the numerical efficiency while preserving the flexibility of the stochastic

method. Within the OSMC, nucleation and surface growth are handled with determin‐

istic means, while coagulation is simulated with a stochastic method (the Marcus‐

Lushnikov stochastic process). The stochastic and deterministic treatments of various

aerosol dynamic processes are synthesized under the framework of operator splitting.

Here, the operator splitting errors of various schemes are analyzed rigorously, combined

with concrete numerical examples. The analyses not only provide sound theoretical

bases for selecting the most efficient operator splitting scheme for the usage of the

OSMC, but also shed lights on how to adopt operator splitting in other PBE solving

methods, i.e., direct discretization, method of moments, etc.

Keywords: Monte Carlo simulation, aerosol dynamics, operator splitting

1. Introduction

Aerosols are dispersed systems of solid or liquid particles suspended in air. Aerosols are

created during various natural processes and industrial operations [1], such as clouds, smoke

particles from forest fires, sand and dust storms, volcanic dust, spores and seeds from plant

life, fluidized catalysts, spray drying of fluids, atomization of liquid fuels, fly ash from stacks,

soot in combustion flames, etc. Aerosol evolution is very complex, involving various physical

© 2016 The Author(s). Licensee InTech. This chapter is distributed under the terms of the Creative Commons

© 2016 The Author(s). Licensee InTech. This chapter is distributed under the terms of the Creative Commons

Attribution License (http://creativecommons.org/licenses/by/3.0), which permits unrestricted use, distribution,

Attribution License (http://creativecommons.org/licenses/by/3.0), which permits unrestricted use,

and reproduction in any medium, provided the original work is properly cited.

distribution, and reproduction in any medium, provided the original work is properly cited.

2

Aerosols - Science and Case Studies

**and chemical processes. The most popular description of aerosol evolution is using the
**

population balance equation (PBE) [2], which is also called the general dynamic equation in

aerosol field [3]. The PBE is a convection‐diffusion type equation with source terms taking into

account the particle formation and depletion from various aerosol dynamics, mainly nuclea‐

tion, surface growth (condensation), and coagulation.

Analytical solutions to the PBE are available for only a few specific cases [4–7]. Mostly,

numerical means are resorted to solve the PBE. There are generally three typical methods for

solving the PBE, i.e., direct discretization, method of moments, and stochastic methods. Direct

discretization may be in the particle size space, such as discretization by sections [8] or finite

difference/finite element [9] and may also be in the functional space, such as those in the

collocation method [10], Galerkin method [11], and weighted residual method [12]. Among

the various discretizations, the sectional method pioneered by Gelbard et al. [8] is the most

popular. There are quite a few sectional methods developed aiming to alleviate the nonposi‐

tiveness and nonconservation problems found in earlier works [13], and to obtain better

efficiency and flexibility, such as the fixed/moving pivot method [14, 15] and cell average

method [16, 17].

Other than solving the discretized PBE, a widely used alternative approach is the method of

moments, which solves a group of moments equations derived from the PBE. These moments

(generally several low order moments) provide important information on the particle size

distribution (PSD) function, i.e., number density, volume fraction, polydispersity, etc. How‐

ever, owing to the nonlinearity of the PBE, the governing equations for lower order moments

generally contain higher order moments, which are not closed after cutting off at a certain

order of moment. Various closure methods have been developed, such as unimodal log‐normal

approximation [18], quadrature/direct quadrature [19, 20], interpolative closure [21], Taylor

expansion [22], etc. Although the method of moments is computationally highly efficient, the

complexity of the closure makes it difficult to accommodate complex physical models for

aerosol dynamics with high flexibility. Another issue closely tied to method of moments is the

realizability problem, when the moments sequence fails to find its corresponding distribution

function [23, 24]. Among all the drawbacks, the inability to provide the PSD is the most severe,

when the PSD is highly needed.

Stochastic simulation (or Monte Carlo simulation) does not solve the PBE, but to mimic the

evolution of aerosol particles through a stochastic particle system. Based on the Marcus‐

Lushnikov process modeling of coagulation [29], various stochastic methods have been

developed to simulate the general aerosol evolution. It is very difficult to categorize precisely

so many diversified methods. According to the evolution of time, there is time‐driven or event‐

driven Monte Carlo [30, 31]. According to the different ways to weight the numerical particles,

there are the mass flow algorithms [32, 33], differentially weighted algorithm [34], and the

more general weighted flow algorithms [35]. Also, there are various types of methods to

improve the simulation efficiency, such as the majorant kernel method [36] and the � leaping

method [37].

Among the three typical methods, stochastic simulation is the most flexible for accommodating

complex physical models for various aerosol dynamics, and is easy to implement without

� . stochastic simulation is not numerically efficient when pursuing a high precision solution.g. which can be volume. The source terms of Inuc. and �(� . �(� . The stochastic simulation and the deterministic integration in OSMC are synthesized under the framework of operator splitting. Governing equations Aerosol particles are generally described statistically in a mesoscopic scale through defining the PSD. The determination of the convection velocity � requires solving the 3 .� . it is assumed � to be the particle size (volume or diameter specified by the context). Here.5772/65140 special numerical issues. the current OSMC code treats the diameter..Operator Splitting Monte Carlo Method for Aerosol Dynamics http://dx. combined properties to describe particles. constituent. Stochastic simulation for coagulation is much more efficient than directly solving the Smoluchowski integro‐differential equation (the coagulation model equation) with traditional discretization [27]. Hence. The evolution of the PSD function satisfies the PBE (also called the general dynamic equation) [3] ¶n r + Ñ × nu = Ñ × DÑn + I nuc + Gcond + Ccoag . where � is the number of total numerical particles used.doi. and � is the diffusion coefficient. On the other hand.�)�� denotes the number density of aerosol particles at location � at time � with aerosol properties between � and � + �� . stochastic simulation generally has convergence rate propor‐ tional to �. and volume of an aerosol particle independently. Zhou et al. the impact of various operator splitting schemes on the accuracy and efficiency of the OSMC is addressed. which are often encountered in the other two methods. Recently. etc. which can easily model particles of various morphologies. Especially.org/10. For simplicity. which combines stochastic simulation for coagulation process and deterministic integration for nucleation and surface growth (condensation). and coagulation. In fact.1. the OSMC has been implemented with Message Passing Interface (MPI) to achieve very promising parallel simulation efficiency [26]. surface. Methodology 2.. Here. The accuracy and efficiency of the OSMC have been demon‐ strated through various testing cases [26]. However. The simulation cost (CPU time and memory) is usually proportional to �2 [25].e.�). It is worth pointing out that the OSMC method can also deal with the cases with a vector type � . � is usually called an internal variable. ¶t (1) where � is the gas flow velocity. i. nonpo‐ sitiveness and nonconservation problems in direct discretization. and Ccoag on the right hand side denote nucleation. deterministic integration for nucleation and surface growth processes is far more efficient than stochastic simulations. realizability problem in method of moments. such as particles with fractal dimensions. 2. respectively. Gcond . e. surface growth (condensation). [26] developed an operator splitting Monte Carlo (OSMC) method. surface.

�* is simply denoted as �. 28–30].g. where the flow field can be considered as steady and one‐dimensional. Here. The aerosol dynamic processes on the right hand side describe the interactions among molecules (or cluster of molecules) and particles. the PBE can be simplified as ¶n = I nuc + Gcond + Ccoag . using some techniques (often computational fluid dynamics). a spherical particle with a diameter of 10 nm has a Schmidt number equal to 290. So the model Eq. and the coupling of the fluid dynamics with the aerosol dynamics is another important research field. For general cases of aerosol evolution in three dimensional flows. under standard atmospheric conditions. With the assumptions that the gas velocity � is known and the mass diffusion term is negli‐ gible. and to iterate between these two dynamics to obtain a converged solution. (2) and the subsequent OSMC method may have very broad applications. Another simplification in this work is to neglect the diffusion term in the PBE. Then it is very easy to integrate Eq. (2).4 Aerosols ... e. For example. which can be described by the Schmidt number (i. 0 u( x') (3) The transformation converts the Eulerian point of view in Eq. (1) to the Lagrangian point of view in Eq.e. (2). the gas velocity � is assumed known. So it is legitimate to neglect the aerosol mass diffusion under very general conditions. Nucleation is the process that dozens or hundreds of molecules form a stable critical nucleus. Hence. the ratio of the viscous diffusion to the mass diffusion).e. For aerosol particles. burner stabilized flames and counter flow diffusion flames. it is possible to use the Lagrangian particle scheme to simulate the aerosol evolution along Lagrangian trajectories [31. the convection can be readily assimilated in the model Eq. It is worth pointing out that the coupling between the fluid dynamics and the aerosol dynamics is generally handled by the operator splitting method [11. Surface growth includes physical . to solve the fluid dynamics and the aerosol dynamics one by one with the feedback from the other dynamics temporarily freezing.Science and Case Studies fluid dynamics control equations. (3) to build up a one‐to‐one mapping between the time and the spatial coordinate. and a 100 nm particle has Schmidt number 2.2 × 104 [3]. There are many practically interested conditions. since the Lagrangian point of view is not explicitly referred any longer. with the help of the assumed known velocity field � . the mass diffusion due to the number concentration gradient (∇ ⋅ � ∇�) is usually very small compared to the air viscous diffusion. Later on. ¶t * (2) The convection term on the left hand side of the original PBE (1) has been implicitly solved with the introduction of the Lagrangian time �* r r x dx' r t * ( x) = ò r r . i.. 32].

which involves interactions between gas phase molecules and an aerosol particle.5772/65140 condensation and surface chemical reactions. such as the forward Euler method or Runge‐Kutta method.Operator Splitting Monte Carlo Method for Aerosol Dynamics http://dx. the time evolution of �(�) is still handled by the classical methods. Figure 1. Flowchart of the OSMC.2.org/10. Surface chemical reactions will not be discussed here due to their vastness. (2). Coagulation is the process that two particles coalesce to form a new one. More details about the aerosol dynamic processes are presented in Section 2. such as �nuc �cond 1 �coag or �nuc 2 �cond 1 � . operator splitting separates the integration into multiple fractional steps.doi. Operator splitting Monte Carlo method Operator splitting is an efficient and powerful method to solve such evolution equations [33] as Eq. where 1/2 denotes a 2 coag 5 . There are various ways to construct the multiple fractional steps. In an operator splitting method. Other than to integrate all aerosol dynamic processes together in one time step ��. Adapted from Reference [26].2. Filled blocks denote steps where stochasticity arises. 2.

and the error analyses for various operator splitting schemes are given in Section 3. (2) can be expressed with the help of the Dirac delta function as I nuc = òId (dp . According to the classical Becker‐Döring theory [3. �� is the vapor pressure. the nucleation rate (how many particles are nucleated per unit volume. and �� = �/�� is the molecular effective volume of the nucleation vapor. Hence. the nucleation term in Eq. In the classical nucleation theory.1. � = �� /�sat is the vapor saturation ratio. There are various nucleation models. which is the minimum size of nucleated particles with stable nucleus. the ratio between the air mean free path � and the particle . � is the surface tension. i.e. �� is the particle density. 2. Nucleation Nucleation is the gas‐to‐particle transition to generate nascent nanoparticle. kBT ln S (5) dp* = Here. 35]. �� is the mole fraction of the vapor. nucleation model is not limited to the classical nucleation theory.. Details of the various models for the aerosol dynamics are described in the following subsections. The flowchart (Figure 1) shows an example how the operator splitting scheme �nuc �cond �coag is carried out.2. � is the temperature. � is the molecular mass of the nucleation vapor. and the critical size. Surface growth (condensation) The functional form of the particle volume growth rate due to condensation depends on the Knudsen number Kn = 2�/��. i. 2. there are two key parameters for the nucleation modeling.dp* )ddp . unit time). Any other nucleation model can be readily included..e.2. largely based on the classical nucleation theory developed in the 1920– 1940s [34].Science and Case Studies half integration step. should only the nucleation rate and the critical size be provided. exp ç 3 2 2 ç 3( kBT ) r p (ln S) ÷ kBT p m è ø (4) 4s vm . the nucleation rate � and critical diameter �∗ are I= æ ö Pv xv 2s 16ps 3 m2 ÷. �� is the Boltzmann constant. Within the OSMC.2. (6) which means that only particles with the critical size are nucleated.6 Aerosols .

Within the OSMC. (Volume is conserved before and after coagulation. which is usually assumed to be the saturation pressure of the condensation vapor. For particles close to the critical size.v% )n( v% )n( v . except for simplified conditions.1 (7) 0. The expressions for volume growth rate �� and the condensation term �cond are [3] ì p dp2 ( Pv . In the transition regime (0. In the free molecular regime (Kn ≥ 10) and the continuum regime (Kn ≤ 0. �� is the equilibrium vapor pressure for particles of size ��. kBT ï ïharmonicmean. The first term on the right‐hand side denotes the formation rate of particles with volume � due to coagulation between particles � and � − �. Practically. interpolation formulas are usually used.3.1 < Kn < 10). ï 1/ 2 ï (2p mkBT ) ï 2p Dd ( P . Stochastic simulation of coagulation Coagulation is the process that two particles coalesce/aggregate to form a new particle. ¶v (8) Here. v% )n( v)n( v% )dv% .�) describes the rate at which particles of size � coagulate with particles of size �. � has the form [3] 7 .5772/65140 radius �� /2.1 < Kn < 10 ¶(nGv ) .Pp )vm . v . ï ïî Gcond = - Kn ³ 10 Kn £ 0. In the free molecule regime (Kn ≥ 10).P )v ï p v p m Gv = í .2.v% )dv% .ò b ( v . should only the particle volume growth rate be provided. The coagulation dynamics is modeled by the well‐known Smoluchowski's equation [3] Ccoag = ¥ 1 v b ( v .doi.org/10.Operator Splitting Monte Carlo Method for Aerosol Dynamics http://dx. such as the harmonic mean of the free molecular and continuum regimes.�) is very hard to find. any other surface growth model can also be accommodated.1). 0 2 ò0 (9) The coagulation kernel function �(�. The second term on the right‐hand side describes the depletion rate of particles with volume � due to their coagulation with any other particles. the Kelvin correction is also required [3]. 2. the condensational growth rates can be derived from the gas kinetic theory and the gradient diffusion model. the coagulation kernel function �(�. respectively.) The half factor (1/2) is to correct the double‐counting effect.

(10) In the continuum regime (Kn ≤ 0. and give an intuitive introduction to the stochastic simulation of coagulation. u) = 2 kBT æ 1 1 ö 1/ 3 1/ 3 ç 1/ 3 + 1/ 3 ÷ ( v + u ). Any two particles may coalesce/aggregate to form a new one at a random time. The random coagulation time � satisfies a Poisson process (the exponential distribution). and it can be generated as . then it is found [25] é N -1 N ù P(t . the number of particles drops. i . u) = ç ÷ èp ø 2/3 æpk T ö ç B ÷ ç 2rp ÷ è ø 1/ 2 æ1 1ö ç + ÷ è v uø 1/ 2 ( v1/ 3 + u1/ 3 )2 .�)/�.�.1).�.. interpolation formula taking into account the former two regimes are generally used. the simulation is to randomly pick up two particles � and � to coalesce (forming a new particle) at the random time � according to the joint probability density function �(�. The well‐known review paper [5] provides a wide‐ ranging survey on the Marcus‐Lushnikov process and the Smoluchowski's equation. � takes the form [3] b ( v .�).�.8 Aerosols .� + ��) between � and � (� < �). Repeat the former process as time advances. The Marcus‐Lushnikov process is the natural stochastic analogue of the finite discrete Smoluchowski coagulation equation.1 < Kn < 10). no analytical solutions are known for the kernels discussed above. the coagulation process is simulated by the Marcus‐Lushnikov stochastic process in the OSMC. k =1 l = k + 1 ë û (12) In essence. and the particle number density drops also. In a virtual box of volume �. 3m è v u ø (11) where � is the dynamic viscosity of the gas‐phase. Let �(�. Analytical solutions known so far are only limited to the following three simple kernels (or their linear combination) [5]. (i) �(�. i. Here.�). During the simulation.�) = 1.�. Other than to solve the Smoluchowski's equation directly through various numerical means.�)�� denote the probability that the next coalescence will occur in the time interval (�. The propensity ��� of coalescence between two particles � and � is determined by the coagulation kernel ��� = �(�. Although the Smoluchowski's equation was developed one century ago.�) = ��. The key step in the simulation is to generate a random point (�. j ) = Cij exp ê .�) according to the density function �(�.�) = � + �.Science and Case Studies æ6ö b ( v . (ii) �(�.å å C klt ú . and (iii) �(�. In the transition regime (0. there are � “well‐mixed” particles. we follow the work of Gillespie [25].e. and it has received broad attention in diverse fields.

and check the random number landing on which corresponding part in the range. calculate the partial sum �� = ∑�� = � + 1 ���. 2.� (preferably the smallest upper bound). so that there is a better chance that � ≤ �(� ) so as to accept � as the required � without too often rejections and repetitions of the whole process. and then it is straightforward to build up a linear mapping between the range and the unit interval (0. Draw a random number from the uniform distribution. In the partial conditioning method. Gillespie [25] introduced two methods to choose � and �. In the acceptance‐rejection method [25] to generate � and � according to �2(�. �0 is the total coagulation probability between any two particles. C0 çè r1 ÷ø (13) −1 � where �0 = ∑� � = 1 ∑ � = � + 1 ���. it needs to choose a density function �(� ) and a constant � ≥ 1 such that ��(� ) ≥ �(� ). then set � = � . In a general acceptance‐rejection algorithm to generate a vector random variable � with density �(� ).Operator Splitting Monte Carlo Method for Aerosol Dynamics http://dx. it is actually an acceptance‐rejection method to generate a bivariate random number (�.…. the selection of � and � is accomplished in two steps. However. the next step is to randomly select two particles according to the probability function �2(�. Generate � from density �.1). Loosely speaking. and �2(�. The algorithm proceeds as follows [36]: 1. It is argued [25] that when the values of ��� are relatively comparable with each other (ideally 9 . and �1 is a random number picked from the uniform distribution in the unit interval. return to 1. Generate � from the uniform distribution on the interval (0. and then select particle � by the part index. the optimal choice is to make the interval in 2 as small as possible.�). �(� ) is chosen as a uniform function. During the first step. combine ���. (13) gives the classical way to generate a random variate from the exponential distribution with parameter �0. The density function �(� ) can be chosen freely.�). else. and � is an upper bound of all ��. then draw another random number to determine the particle � in a similar way as in the first step. During the second step.doi. the so‐called full conditioning and partial conditioning methods.�) in sequential to form another range.�) is the fraction of the coagulation probability ��� over �0. In the full conditioning method.�) = ��� /�0. Eq. If � ≤ �(� ). ��(� )).�). then combine the � partial sums in sequential to form a range with the index � from 1 to � denoting the part for each partial sum.org/10. and build up the linear mapping between the new range with the unit interval.5772/65140 t= 1 æ1ö ln ç ÷ . 3.�) from the function �2(�. (� = 1. After selecting the time at which two particles coagulate.…. (� = � + 1.

(13).3. the simulator size � is adjusted to reflect the change of particle number density due to nucleation.Science and Case Studies constant) the particle conditioning method should be more efficient than the full condition‐ ing method. If the total number of MC particles exceeds the maximum allowable threshold value (which is set beforehand to balance the stochastic error and numerical cost). (� = 1. In the particles nucleation step. and the number of MC particles decreases by one. and the simulator size is set to a huge value. And then every MC particle undergoes the surface growth process according to its growth rate (usually depends on its size). then down‐ sampling is performed.. and the initial PSD. number of Monte Carlo (MC) particles �. exceeding MC particles are randomly removed from the pool to satisfy the number constraint. The random coagulation time � is generated according to Eq. . � = � + 1. two particles are selected to perform coagula‐ tion.e. The subsequent up‐sampling step is to keep the number of MC particles above a given threshold to avoid severe stochastic error. The simulator size is determined as � = �/�0. � �)/�. simulator size �.�). although they are usually not necessary in Monte Carlo simulation of aerosol dynamics. say � = 1010. �0 = 0.e. If simulation starts from an empty case. If the comparison statement is true. Nascent nucleated particles are added to the pool of MC particles. If simulation starts from a case with a specific PSD. where �0 is the initial number density.e. Updating coagulation kernel is to calculate the pair coagulation rate ��� = �(��. The com‐ parison statement �sum + � < �� is to judge whether the time for two particles to coagulate is still admissible within the discrete time step ��.10 Aerosols . then the size of the � simulation particles is assigned by a stochastic process to satisfy the initial PSD. then the simulator is initialized with � particles of uniform size (the real value of the size is immaterial to the simulation results). the simulator is initialized with given parameters. since mostly the simulation starts from an empty case. i.…. i. which is initialized to zero before a coagulation step begins. i. 2. Only the first‐order operator splitting is sketched in the figure. which renders a tiny particle number density to approximate the condition �0 = 0. Here �sum is the accumulated coagula‐ tion time in the coagulation step..…. There are various convenient ways to generate random number to satisfy a given distribution [37].. The coagulation simulation process (those steps grouped in the dashed bounding box �� in Figure 1) shows how to implement the stochastic algorithm of Gillespie [25].� − 1. At time � = 0. Within the OSMC. both the full and particle conditioning methods have been implemented to choose from easily. Full algorithm for the OSMC Figure 1 shows the flowchart of OSMC including all aerosol dynamics.

which are the two most important statistics of aerosol particles. 3. These processes have very different effects on the evolution of the total number density and volume fraction. and it does not change in the surface growth process (mainly condensation).uk ]b ( v . we introduce an integral transfor‐ mation of the Smoluchowski's equation (9). Error analyses for operator splitting Aerosol dynamics usually contain nucleation. dt 2 0 0 (15) Specifically. because nucleated particles are very small in size. dt 2 0 0 (16) One interesting but somewhat overlooked conclusion [1] is that the right hand side of Eq. and Eq. and coagulation processes. and nucleation has limited contribution to the volume fraction directly. u)n( v . it can be derived [1] dM(t ) 1 ¥ ¥ = ò ò [ F( v + u) . Nucleation is generally a function of the temperature and the nucleated vapor concentration. condensation and coagulation are usually loosely coupled through particle size and number density. Case of nucleation + coagulation Before discussing the case of nucleation and coagulation. (15) transforms to the dynamic equation for the moment ��(�) dM k (t ) 1 ¥ ¥ = ò ò [( v + u)k . 0 (14) then from the Smoluchowski's equation (9). Suppose �(�) is an arbitrary function of �.Operator Splitting Monte Carlo Method for Aerosol Dynamics http://dx. which determine the volume fraction.F( v) .5772/65140 3. surface growth. etc). For the volume fraction. and let ¥ M(t ) = ò F( v)n( v . However. Therefore.F(u)]b ( v . t )n(u. t )dv . The volume fraction is generally dominated by surface growth process.doi. particle size. which mean that �� will grow with time for 11 . On the other hand. it is conserved in the coagulation process.v k . t )n(u. (16) is negative if � < 1. which is very useful to understand the evolution of the moments of the PSD. and (ii) nucleation + condensation. (� ≥ 0). ��(�) is the �th order moment. t )dudv. which is largely determined by the nucleation process. and it does not depend on the aerosol status (number density. when �(�) = ��.org/10. it increases due to nucleation while decreases due to coagulation. t )dudv. and it is positive if � > 1. For the number density. which determine the number density. it is convenient and meaningful to consider two isolated cases: (i) nucleation + coagulation. both condensation and coagulation are closely related to the number density. u)n( v .1.

the model Eq. Hence. Mathematically. the number density (�0) satisfies the following simple model equation dM0 = J + KM02 . t )dudv. In fact. In the case of constant rate nucleation and constant kernel coagulation. ç JK ÷ ú K è øû ëê (19) . and � represents the nucleation rate (number of particles nucleated per unit volume 1 per unit time). and it will decrease with time for � < 1. t )dudv = ò ò 0 b ( v . and � = − �0. we 1 1 immediately have − �0�20 on the right‐hand side. (18) Of course. which does decay due to coagulation. dt (17) One the right‐hand side. t )n(u. The second term models the contribution from coagulation. it is possible to find a �0 that satisfies ¥ ¥ ¥ ¥ 0 0 b 0 M02 = b 0 ò ò 0 n( v . �1(�) is constant with time. Here. It is worth pointing out that although fractional moments (with � being a fraction number) do not possess obvious physical meaning. (16) if the coagulation kernel is the constant �0 and let � = 0 (to obtain the number density equation).Science and Case Studies � > 1. they are very useful in the method of moments with the interpolative closure [21] or with the Taylor expansion closure [22]. the right �0 depends not only on the specific � function. we assume that a good estimate of �0 is available and will not delve into this issue further. 2 where �0 is a constant coagulation kernel. On the other hand. �1 is the volume fraction.12 Aerosols . Given the initial condition �0(� = 0) = �0* . but also on the distribution �. in the moment dynamic Eq. u)n( v . Especially. Actually. The analyses focus on the local error in a generally small single time step. The assumption of a constant nucleation rate and a constant coagulation kernel does not severely limit the applicability of the following discussion on the operator splitting errors for the more general case of nucleation and coagulation. The notation � = − �0 (be aware of the 2 2 negative sign) is found to be able to greatly simplify the following analyses. the coagulation kernel � is a bivariate function of colliding particles sizes. �0 is the total number density. (17) has analytical solution M 0 (t ) = é æ M * K öù JK tan êt JK + arctan ç 0 ÷ ú . which is conserved during the pure coagulation process. the first term models the contribution to the number density from nucleation. even a time‐dependent nucleation rate �(�) can be readily assumed constant within the single time step. t )n(u.

and compare the obtained solutions with the true solution (19) to quantify the operator splitting errors. then Eq. (iii) 1 � 2 nuc �coag 1 1 � . i.org/10. the 2 form in Eq. 3 (21) On the other hand. we can try to use the operator splitting method to solve the same Eq. There are various operator splitting schemes. and (iv) �coag 2 nuc 2 �nuc 1 � . (i) �nuc �coag. (22b) is solved with the just obtained solution at � = �� as the initial condition.doi. dt (22a) dM0(2) = KM02 . (20) (with � replaced by − �0) is more natural.JK + arctanh ç 0 ÷ ú . (19) involves imaginary numbers. (19) at � = �� as Taylor series for later usage 1 M0 (d t ) = M0* + ( KM0* 2 + J )d t + K( KM0* 2 + J ) M0*d t 2 + K(3K 2 M0* 4 + 4 JKM0* 2 + J 2 )d t 3 + O (d t4 ). it is easy to show that Eqs. Although the solution Eq.e. Eq. (ii) �coag �nuc. (19) proves more handy in the following analyses. � = − �0 < 0 the solution Eq. we expand Eq.Operator Splitting Monte Carlo Method for Aerosol Dynamics http://dx. ç . (19) and (20) are actually 1 equivalent. Eq. we will focus on two first‐order Lie schemes and two second‐order Strang schemes. Here.JK ÷ ú K êë è øû (20) 1 Since. (22a) is solved first with the given initial condition at � = 0. (17) is found as [7] M 0 (t ) = é æ M * K öù . (17). a solution of the same Eq. 2 coag In the operator splitting method. the following two joint equations are solved (i) Lie scheme �nuc dM0(1) = J. Here. (22a) has solution: M0(1) (t ) = Jt + M0* .5772/65140 In fact.. dt (22b) �coag (Denoted as Lie1) To seek the solution at � = ��. (23) 13 . Using their relation 2 to the complex exponential function.JK tanh êt .

1 (24) Let � = �� in the above equation.M0* J b 0d t2 + O (d t3 ). (25) The operator splitting error can be found by comparing the two Taylor expansion series (25) and (21) 1 Er0i) = M0(OP) (d t ) . (28) Hence. and expand it into Taylor series M0(OP) (d t ) = M0* + ( KM02 + J )d t + K( KM0* 2 + 2 J ) M0*d t2 + O (d t3 ). 2 0 0 t 1 � (Denoted as Strang1) 2 nuc (29) .M0* JKd t2 + O (d t3 ) = 1 (iii) Strang scheme �nuc 2 �coag 1 * M J b d 2 + O (d t3 ). 2 (ii) Lie scheme �coag (26) �nuc (Denoted as Lie2) The analysis is quite similar to case (i).1 (27) and its Taylor expansion is M0(OP) (d t ) = M0* + ( KM02 + J )d t + K 2 M0* 3d t2 + O (d t3 ). the operator splitting error is Er0ii) = . (22b).Science and Case Studies (1) Hence. KM0*d t . Take �0 (��) as the initial condition and solve Eq. (22a) and (22b) is reversed. �(1) 0 (��) = ��� + �*0. JKd t t + KM0* t . then the final solution is found as M0(OP) (t ) = - Jd t + M0* . The final solution is M0(OP) (d t ) = Jd t - M0* .M0 (d t ) = M0* JKd t2 + O (d t3 ) = . except that the solution procedure for the two joint Eqs.14 Aerosols .

Second.2 M0* . (22b) to get the solution �0 (�). �0 ( ��) is used as M0(OP) (d t ) = Jd t + 2 M0* 1 . 12 48 (35) 15 .4 2 (33) and its Taylor expansion is 1 M0(OP) (d t ) = M0* + ( KM0* 2 + J )d t + K( KM0* 2 + J ) M0*d t 2 + K(4 K 2 M0* 4 + 5KJM0* 2 + 2 J 2 )d t 3 + O (d t4 ). �0 (��) is used as 1 the initial condition at � = �� to solve Eq.M0* 2 K + 2 J )d t3 + O (d t4 ) = . the operator splitting error is Jb JK (2 M0* 2 K . Finally.org/10. Eq.2 Jd t .2 (30) and its Taylor expansion is 1 M0(OP) (d t ) = M0* + ( KM0* 2 + J )d t + K( KM0* 2 + J ) M0*d t 2 + K(4 K 2 M0* 4 + 6 KJM0* 2 + J 2 )d t 3 + O (d t4 ).JK M0*d t 3 + 2 JKd t 2 + 4 KM0*d t .J )d t3 + O (d t4 ) = 0 ( M0* 2 b 0 + J )d t3 + O (d t4 ).Operator Splitting Monte Carlo Method for Aerosol Dynamics http://dx.0 ( M0* 2 b 0 + 4 J )d t3 + O (d t4 ). 12 24 Er0iii) = 1 (iv) Strang scheme �coag 2 �nuc (32) 1 � (Denoted as Strang2) 2 coag Similar to case (iii). First. (34) 4 Hence. the final solution is found as M0(OP) (d t ) = 2 JKM0*d t 2 . (22a) is solved 1 2 (2) (2) the initial condition to solve Eq.doi. the solution to the joint Eqs. 4 (31) Hence. Jd t 2 2 JKd t + 2 KM0*d t . (22a) again. The final solution at � = �� is found as 2 (1) with the initial condition �0(0) = �0* to get the solution �(1) 0 (�). the operator splitting error is Er0iv) = Jb JK ( . .5772/65140 Here. (22) is carried out in three steps.

when �0* 2�0 ≫ �. Since the total volume is conserved during coagulation. (32) and (35) 2( M0* 2 b 0 + J ) . the absolute splitting 2 0 0 1 error in Eq.. The Strang1 scheme is found to overestimate the number density. They are systematical ways to construct even higher order schemes. The magnitude of the absolute errors in these two schemes can be compared through investigating the coefficients of �3� in Eqs. (32) is smaller than that in Eq.2 J. On the other hand. (35). Hence. Here. When �0* 2�0 ≪ �. One interesting conclusion [38] is that the scheme 2 1 (Strang1 + Strang2) + (Lie1 + Lie2) is of third order. (6) and (16) as . The Lie1 scheme underestimates the number density. in the Strang schemes it is preferable to split the higher rate process into symmetric substeps to reduce the splitting error. Especially. and (29). while the Lie2 scheme overestimates that. i. (36) 1 �* 2� < �. (35). both are of second order in �� within a time step.Science and Case Studies To summarize. the error in Eq. the faster the coagulation rate.( M0* 2 b 0 + 4 J ) = M0* 2 b 0 . while the two Strang2 scheme to underestimate that. hence the number density would be underpredicted as in Lie1. then calculate the error in the third‐order scheme constructed as mentioned shortly before.e. Only the most common first and second‐order operator splitting schemes are discussed so far. and vice versa. which can be used to check the accuracy 3 4 of the above derivations. Following. the model equation for nucleation and coagulation can be easily derived from Eqs. it is found that only terms involving �4� and higher orders survive. This is an indirect proof that all the derivations of the error functions are correct. Hence. This is because coagulation rate closely depends on the number density. (32) 2 If nearly doubles that in Eq. the higher the number density. we will briefly discuss the splitting errors for higher order moments other than �0. there are no splitting errors for predicting �1 for �2. (29). The splitting errors in the two Strang schemes are of third order in �� within a time step.16 Aerosols . nucleation. a third‐order scheme [38] can be obtained through the combination of the two Lie and two Strang schemes. we are not interested to discuss the even higher order schemes other than the Lie and Strang schemes. Keep the third‐order term �3� in the error functions (26). (33) 2 1 approaches a half of that in Eq. which renders them a second‐order scheme globally. (36). (32). Coagulation rate would be overpredicted if nucleation is integrated before coagulation. the error in Eq. So the global integration error during time �all is of order ��. and coagulation are independent of each other with respect to �1 (volume fraction). since higher order schemes are complicate to implement and may not be worthy for the solving the aerosol dynamics. coagulation rate is smaller than nucleation rate. since the error will accumulate in �all /�� steps. the two Lie schemes have the same magnitude in splitting error.

0 0 dt 2 (37) and �1 is determined by nucleation only. �* is the critical volume of nucleated particle. Case of nucleation + condensation Here.Operator Splitting Monte Carlo Method for Aerosol Dynamics http://dx.5772/65140 ¥ ¥ dM 2 1 = Jv * 2 + b 0 ò ò (2 vu)n( v . (38) Here. The detailed 6 17 . The solution to Eq.b 0 Jv * ( Jv *d t + 3 M1* )d t2 . 3 (40b) Er2(i) = Er2(iii) = - 1 b J 2 v* 2d t3 . t )dudv = Jv * 2 + M12 . (37) can be readily obtained as 1 b Jv* (2 Jv*d t + 3 M1* )d t2 . the four splitting errors for solving Eq. 3 0 (40a) 1 Er2(ii) = . (37) is M 2 (t ) = 1 2 *2 3 J v b 0t + Jv * M1* b 0t 2 + ( Jv * 2 + b 0 M1* 2 )t + M 2* . and �1* is the initial value at � = 0. Eq. 3 (39) Similar to the above error analyses. t )n(u. a case with constant nucleation rate and constant condensation growth in diameter is considered.org/10. 3. The particle diameter growth rate � function can be obtained easily through the sphere volume formula � = �3�. A constant growth rate in diameter is not arbitrary at all. (7) gives the volume growth rate due to condensation as a piecewise function. which can be integrated as M1 (t ) = Jv * t + M1* . 6 0 (40d) The splitting errors for the two second‐order Strang schemes are independent of the initial conditions.2. 12 0 (40c) Er2(iv) = 1 b J 2 v* 2d t3 .doi.

In this subsection. the moments are defined with respect to the particle diameter �� other than the volume �� = ∫�(��)��� d��. the particle diameter growth rate in the free molecular regime is independent of its size. The dynamic equations for moments due to pure nucleation (to generate particles with diameter �*� at rate �) can be easily obtained with the help of the Delta function (6). the particle diameter growth rate is assumed as �. dt (41c) dM 3(1) = Jdp* 3 . No attempt is sought to distinguish the symbols for moments defined differently. which can be seen as a constant determined by environmental parameters (vapor pressure and temperature). =òdt ¶dp p p (42b) dM 2(2) ¶(nG) 2 d dd = 2G òndp ddp = 2GM1(2) . which are dM0(1) = J.Science and Case Studies function can also be found in reference [31]. dt (41b) dM 2(1) = Jdp* 2 . dt (41a) dM1(1) = Jdp* . dt (41d) The dynamic equations for moments due to condensation (at a constant diameter growth rate �) are dM0(2) ¶(nG) =òddp = 0. In the following discussion. with the hope to reduce new symbols and to bring no confusion. =òdt ¶dp p p (42c) . dt ¶dp (42a) dM1(2) ¶(nG) d dd = G ònddp = GM0(2) . In fact.18 Aerosols .

3 (44c) 1 3 4 3 JG t + ( Jdp* + GM0* )G 2t 3 + ( Jdp* 2 + 2GM1* )Gt 2 + ( Jdp* 3 + 3GM 2* )t + M 3* . 4 2 (44d) M1 ( t ) = M 2 (t ) = M 3 (t ) = (44a) On the other hand. (i) Lie scheme �nuc �cond (Denoted as Lie1) After solving Eqs. dt (43d) Assume the initial condition at � = 0 is [�0*.�*. then Eq. dt (43b) dM 2 = Jdp* 2 + 2GM1 .1. (41) and (42). Parallel to the analyses in Section 3. the final solution at � = �� is found as 19 . dt (43c) dM 3 = Jdp* 3 + 3GM 2 . the dynamic moments equations for nucleation and condensation are dM0 = J.Operator Splitting Monte Carlo Method for Aerosol Dynamics http://dx. 2 (44b) 1 2 3 JG t + ( Jdp* + GM0* )Gt 2 + ( Jdp* 2 + 2GM1* )t + M 2* . dt (43a) dM1 = Jdp* + GM0 .org/10. four splitting schemes are considered as follows.5772/65140 dM 3(2) ¶(nG) 3 =òd dd = 3G òndp2 ddp = 3GM 2(2) .� 2 *3]. 1 JGt 2 + ( Jdp* + GM0* )t + M1* .doi. dt ¶dp p p (42d) Hence. (43) has solution M0 (t ) = Jt + M0* . (41) and (42) sequentially. the operator splitting can be used to solve Eqs.�1*.

(47c) M 3OP (t ) = G 3 M0* t 3 + 3G 2 M1* t 2 + ( Jdp* 3 + 3GM 2* )t + M 3* . (47d) . (45b) M 2OP (t ) = JG 2t 3 + (2 Jdp* + GM0* )Gt 2 + ( Jdp* 2 + 2GM1* )t + M 2* . 3 3 *2 2 3 Jd Gd t + 2 JG 2 dp*d t3 + JG 3d t4 . (42) and (41) sequentially. Er1(i) = 1 JGd t2 .20 Aerosols . the final solution at � = �� is found as M0OP (t ) = Jt + M0* . (47b) M 2OP (t ) = G 2 M0* t 2 + ( Jdp* 2 + 2GM1* )t + M 2* . (45d) The splitting error is found by comparing the splitting solution (45) with the exact solution (44) Er0(i) = 0. (45c) M 3OP (t ) = JG 3t 4 + (3 Jdp* + GM0* )G 2t 3 + (3 Jdp* 2 + 3GM1* )Gt 2 + ( Jdp* 3 + 3GM 2* )t + M 3* . (45a) M1OP (t ) = JGt 2 + ( Jdp* + GM0* )t + M1* . 2 p 4 (46a) (46b) (46c) (46d) �nuc (Denoted as Lie2) After solving Eqs. 2 Er2(i) = Jdp* Gd t2 + Er3(i) = (ii) Lie scheme �cond 2 2 3 JG d t .Science and Case Studies M0OP (t ) = Jt + M0* . (47a) M1OP (t ) = ( Jdp* + GM0* )t + M1* .

2 2 2 (49d) M1OP (t ) = M 2OP (t ) = M 3OP (t ) = The splitting error is found by comparing the splitting solution (49) with the exact solution (44) Er0(iii) = 0.JGd t2 . (42) with full time step. (41) with half step again.org/10. (49a) 1 JGt 2 + ( Jdp* + GM0* )t + M1* . (48a) 1 Er1(ii) = . the final solution at � = �� is found as M0OP (t ) = Jt + M0* . 6 (50c) 21 . 2 (48b) Er2(ii) = . 3 3 1 Er3(ii) = .doi. (50b) Er2(iii) = 1 2 3 JG d t .JG 3d t4 . and then Eq. 2 (49c) 1 3 4 3 * 3 JG t + ( Jdp + GM0* )G 2t 3 + ( Jdp* 2 + 3GM1* )Gt 2 + ( Jdp* 3 + 3GM 2* )t + M 3* .Jdp* 2Gd t2 . (50a) Er1(iii) = 0. (41) with half time step �� /2.2 Jdp* G 2d t3 . 2 4 1 (iii) Strang scheme �nuc 2 �cond (48c) (48d) 1 (Denoted as Strang1) � 2 nuc After sequentially solving Eq. 2 (49b) 1 2 3 JG t + ( Jdp* + GM0* )Gt 2 + ( Jdp* 2 + 2GM1* )t + M 2* . then Eq.5772/65140 The splitting error is found by comparing the splitting solution (47) with the exact solution (44) Er0(ii) = 0.Jdp* Gd t2 - 1 2 3 JG d t .Operator Splitting Monte Carlo Method for Aerosol Dynamics http://dx.

all Lie schemes are of first order (globally). (42) with half step again. (42) with half time step �� /2. 2 4 (50d) 1 � (Denoted as Strang2) 2 cond After sequentially solving Eq. 4 (51c) 1 3 4 3 * 3 JG t + ( Jdp + GM0* )G 2t 3 + ( Jdp* 2 + 3GM1* )Gt 2 + ( Jdp* 3 + 3GM 2* )t + M 3* . 12 1 1 Er3(iv) = . 8 4 2 (51d) M1OP (t ) = M 2OP (t ) = M 3OP (t ) = The splitting error is found by comparing the splitting solution (51) with the exact solution (44) Er0(iv) = 0. and the leading errors are of opposite sign between Lie1 and Lie2. (52a) Er1(iv) = 0.Science and Case Studies Er3(iii) = 1 (iv) Strang scheme �cond 2 �nuc 1 2 * 3 1 3 4 JG dpd t + JG d t . (41) with full time step.22 Aerosols . there is no splitting error for the number density (�0).JG 2 dp*d t3 . and the errors for �2 and �3 are of second order. 2 (51b) 1 2 3 JG t + ( Jdp* + GM0* )Gt 2 + ( Jdp* 2 + 2GM1* )t + M 2* . the splitting error for �1 is also zero. For �1 to �3. .JG 3d t4 . In Lie1 and Strang1 scheme. and then Eq. (52b) Er2(iv) = - 1 JG 2d t3 . which is solely deter‐ mined by nucleation. 4 8 (52c) (52d) To summarize. (51a) 1 JGt 2 + ( Jdp* + GM0* )t + M1* . then Eq. the final solution at � = �� is found as M0OP (t ) = Jt + M0* . For Strang schemes.

The OSMC results are averaged over dozens of independent simulations to eliminate the randomness.org/10. It is also found that Strang1 shows better precision than Strang2. Figure 2 shows the number density (�0) simulated by the four schemes.Operator Splitting Monte Carlo Method for Aerosol Dynamics http://dx. Strang2 slightly underpredicts the true solution. Case of nucleation + coagulation Corresponding to the error analyses in Section 3. Then only the time step �� matters when calculating the relative error. and the number density is �0* = 1.doi. In fact. while Lie2 to overpredict. almost independent of the nucleation rate and the condensational growth rate. 4. while Lie2 to underestimate.1. compared against the analytical solution (19). the relative errors due to the operator splitting are small. which seems strange at first glance. Nucleated particles also have unit volume size.e.1. The coagulation kernel and nucleation rate are set as unit �0 = 1.1. it is possible to construct higher order splitting scheme with zero splitting error for all moments. All these findings agree extremely well with the analyses in Section 3. with � = 2000 Monte Carlo particles. Strang1 gives result negligibly higher than the analytical solution. while the leading order in the analytical solution for �1 in Eq. All the simulations use fixed time step �� = 0. (58) also contains exactly the same factor ��. the case of constant nucleation and constant coagulation are simulated with the OSMC. and �3 * . the splitting errors are anchored to the moment's evolution. Generally speaking. that is because nucleation rate is higher than the coagulation rate 1 1 ( � = 1 > �0�0* = ). Lie1 scheme is found to systematically underpredict the number density. the error contains the factor ��. Figure 3 compares �2 among the four splitting schemes and the analytical solution (39). which renders the relative errors (splitting errors divided by the corresponding moments values) comparable among various moments. and � = 1. the leading order (with respect to ��) splitting errors for any two subsequent moments differ by a factor of �*�. The second‐order Strang 23 . On the other hand..5772/65140 the splitting solutions overpredict the high order moments.1 also. �1* . since nucleation in the prestep produces more than real particles to grow in condensation. Lie2 and Strang2 underpredict the high order moments.1. since two subse‐ quent moments also differ by a factor of the particles average diameter according to the moment definition. as explained 2 2 in Section 3. �2 * . Take the �1 splitting error in the Lie1 scheme as example. The splitting errors are independent of the initial conditions. Since the splitting errors are in closed form of the time step ��. Initially particles are mono dispersed with unit volume size. i. and the higher rate process nucleation is split in Strang1. Lie1 is found to overestimate �2 a little bit. Numerical examples 4. �0* . Furthermore.

Within the OSMC. The Strang1 scheme has much higher precision than the .Science and Case Studies schemes give result almost indistinguishable from the analytical solution. coagulation is the most computationally intensive part. and nucleation only makes a tiny fraction of the total time cost. Figure 3. Figure 2. Both the error analyses and the numerical examples above show that the second‐order Strang schemes have much higher precision than the first‐order Lie schemes. Although second‐ order Strang schemes give better results than the Lie schemes. Evolution of total particle number density (� � = 0.24 Aerosols . Evolution of moment �0 for constant kernel coagulation and constant rate nucleation �2 in case of constant kernel coagulation and constant rate nucleation (moment is defined with respect to the particle volume). the discrepancy is not so significant as that for �0 in Figure 2.1).

Figure 4. and the number density is �0* = 1. Both the nucleation rate and growth rate are set to unit � = 1 and � = 1. and Strang2 outperforms Strang1 in precision only if Strang1 is the optimal splitting scheme taking both the numerical precision and cost into account.2. The time step is �� = 0. the case of constant nucleation and constant condensational growth in diameter is simulated with the OSMC. Hence. which renders very small splitting errors for high order moments.doi.5772/65140 Lie schemes. Another general conclusion is that only �0 needs to be concerned when considering the operator splitting errors. and only needs to integrate nucleation twice often as in the Lie schemes. Operator splitting generally produces less errors for higher order moments.2. 4. and needs proper splitting scheme combined with small enough time step to satisfy the given error criteria.2. The �2 splitting errors for the Strang schemes contain the factor of the critical volume of nucleated particles. 25 . the splitting error for �0 may be still significant. which is generally very small.org/10. the critical volume �* is of order 10−27m3. Case of nucleation + condensation Corresponding to the error analysis in Section 3. However. Nucleated particles also have unit volume size. where the computational overhead is negligible. as Strang1. The best per‐ 2 0 0 formance of Strang2 over Strang1 is to nearly double the precision when �0�*02 ≫ �. Taking a more practical numerical example of dibutyl phthalate (DBP) aerosol nucleation and coagulation in a turbulent mixing layer [26]. Strang2 needs nearly double computational cost 1 � �* 2 > �. Initially particles are monodispersed with unit volume size.Operator Splitting Monte Carlo Method for Aerosol Dynamics http://dx. Evolution of moment �1 in case of constant nucleation and constant condensational growth in diameter (moment is defined with respect to particle diameter).

All the findings agree very well with the analyses in Section 3. since a relatively large time step �� = 0. Evolution of moment � (volume fraction missing a factor �/6) in case of constant nucleation and constant 3 condensational growth in diameter (moment is defined with respect to particle diameter).26 Aerosols . both the ODE integration error and splitting error are much smaller. Comparing Figures 4 and 5. According to the error analyses (49c) and (51c). Close scrutiny shows in Figure 4 that the numerical error is not actually zero. almost indistinguishable from the analytical solutions. Within the OSMC.2 is used. Lie1 is found to overpredict. Figure 5.Science and Case Studies Figures 4 and 5 show the evolution of moments �1 and �3. the relatively errors are comparable for both �1 and �3 here. The ultimate goal of the OSMC is to greatly improve the numerical efficiency and to . while Lie2 to underpredict. which actually arises from the ordinary differential equation (ODE) integration error. �1 do not have simple physical meaning. For both �1 and �3. Conclusions The operator splitting Monte Carlo (OSMC) method has been developed recently [26] for solving the population balance equation for aerosol dynamics. while coagulation is simulated with a stochastic method (the Marcus‐Lushnikov stochastic process). obtained by the four splitting schemes and the analytical solutions (44d). 5. the characteristics of splitting errors are quite similar. the splitting errors for �1 Strang schemes are zero. which may be used to define an average diameter through �1 /�0. The deterministic and stochastic approaches in the algorithm are synthesized under the framework of operator splitting. respectively. For a more appropriate smaller time step. While �3 directly represents the particle volume fraction (lacking a factor of �/6). nucleation and surface growth are handled with deterministic means.2. The splitting errors for the two Strang schemes are very small.

. but also shed lights on how to adopt operator splitting in other PBE solving methods. Strang2 1 1 1 1 ( �coag �nuc ) has better precision than Strang1 ( �nuc �coag � � ). Saudi Arabia. The OSMC has been validated through quite a few testing cases [26].5772/65140 preserve the extraordinary flexibility and applicability of a stochastic method for aerosol dynamics simulation. one of the most important statistics for aerosol particles. the splitting errors for four splitting schemes (two Lie schemes and two Strang schemes) are analyzed rigorously.doi. coagulation. KZ would like to thank Dr. Other‐ 2 2 2 coag 2 nuc wise. Research Grants Council of the Hong Kong SAR. The second‐order Strang schemes exhibit much better precision that the first‐ order Lie schemes. is found to be underestimated for the Lie1 scheme (�nuc �coag). If coagulation rate is higher than the nucleation rate. When a good scheme for splitting between nucleation and coagulation is constructed. and constant nucleation and con‐ densation. i. constant nucleation and coagulation.Operator Splitting Monte Carlo Method for Aerosol Dynamics http://dx. and vice versa. focused on two repre‐ sentative cases. Splitting between nucleation and condensation has marginal impact on accurately predicting the moments. while overestimated for the Lie2 scheme (�coag �nuc). 39]. splitting among other aerosol dynamic processes can be constructed at more freedom. The number density. Strang1 has better precision. where splitting between nucleation and coagulation has significant impact. The financial support from the General Research Fund. This is in great contrast to the prediction of �0.e. Strang1 is always the most preferable splitting scheme after taking the numerical cost and precision into account.. China (No. combined with concrete numerical examples. 27 . Bisetti at KAUST. direct discretization. hence the number density would be underpredicted as in Lie1. To construct a good operator splitting scheme for the general case of nucleation. and has also been used to simulate aerosol evolution under various conditions [32. i. and condensation the first priority is to consider the splitting error for �0. The analyses not only provide sound theoretical bases for selecting the most efficient operator splitting scheme for the usage of the OSMC. 11402179 and 11572274) is greatly acknowledged. Acknowledgements The financial support from the National Natural Science Foundation of China (No. method of moments etc.org/10.e. for his insightful discussion and valuable help. Here. for the OSMC. However. F. The overall splitting errors are pretty much determined by the splitting error for �0. This is because coagulation rate would be overpredicted if nucleation is integrated before coagulation. the operator splitting errors in the OSMC have not been systematically investigated. However. The operator splitting errors for the case of nucleation and condensation show that splitting errors for different moments (except for �0) are comparable with each other.

2000. T. Pergamon Press. Gelbard. 1980. China 2 Department of Mechanical Engineering. 1976. The Smoluchowski coagulation equations with continuous injection. 17:557–585. 201–376. Journal of Colloid and Interface Science. D. [5] D. M. Hong Kong References [1] R. W. Journal of Physics A: Mathematical and Theoretical. H. [2] D. pp. [9] S. . Davies. Aldous. AIChE Journal. Ramabhadran. Wattis. K. R. Seinfeld. and J. King. Rigopoulos and A. L.. In G. The Hong Kong Polytechnic University. [4] M. Hidy and J. 5:3–48. AIChE Journal. 760(2):541–556. 490(5):1127–1139. Finite‐element scheme for solution of the dynamic population balance equation. second edition. 2000. Ramkrishna. C.kun@wust. Jones. Dust. Smoke. Author details Kun Zhou1* and Tat Leung Chan2 *Address all correspondence to: zhou. Topics in Current Aerosol Research. and J. New York. 1999. 1916. G. 2003. [6] T. Academic Press. Population Balances: Theory and Applications to Particulate Systems in Engineering.cn 1 The State Key Laboratory of Refractories and Metallurgy. Bernoulli. New York. Dynamics of aerosol coagulation and condensation. A. Peterson. editors. 1972. Y. Brownsche Bewegung und Koagula‐ tion von Kolloidteilchen. Smoluchowski.28 Aerosols . J.Science and Case Studies PolyU 152663/16E) is also greatly appreciated for allowing the authors’ further development and extension of this OSCM foundation method. [3] S.edu. Tambour. Kowloon. R. Drei Vorträge über Diffusion. 220(5):840–851. Oxford University Press. Friedlander. 1999. San Diego. and Haze: Fundamentals of Aerosol Dynamics. Brock. and J. Drake. Seinfeld. [7] S. A general mathematical survey of the coagulation equation. Sectional representations for simulating aerosol dynamics. Wuhan University of Science and Technology. Physikalische Zeitschrift. H. [8] F. Wuhan. E. 32:7745– 7763. J. Deterministic and stochastic models for coalescence (aggregation and coagulation): a review of the mean‐field theory for probabilists.

and coagulation in aerosol reactors. Chemical Engineering Science. 46(6):1447–1465. 2008. [12] J.Operator Splitting Monte Carlo Method for Aerosol Dynamics http://dx. Ramkrishna. Kumar. 51(8):1333– 1342. Ramkrishna. 149(2):425–449. Simultaneous nucleation. Seinfeld. G. 2008. Chemical Engineering Science. Chan. [18] S. [23] J. Tamarkin. M. and S. Alexopoulos. growth. [14] S. [17] J. 1988. breakage. Chemical Engineering Science. Heinrich. Pratsinis. 2008.5772/65140 [10] A. and T. 124(2):416–427. A new moment method for solving the coagulation equation for particles in Brownian motion. condensation. [22] M. The cell average technique for solving multi‐dimensional aggregation population balance equations. Evaluation of weighted residual methods for the solution of a population balance model describing bubbly flows: the least‐squares. Chemical Engineering Science. revised edition. Heinrich. ESAIM.doi. McGraw. M. The Problem of Moments. Aerosol Science and Technology. [15] S. Z. Marchisio and R. Description of aerosol dynamics by the quadrature method of moments. [19] R. [13] Y. Shohat and J. Computers and Chemical Engineering. Mathematical Modelling and Numerical Analysis. O. 1996. [11] S. tau. Solsvik and H. A fixed pivot technique. A. Ganesan. 59(24):5751–5769. Peglow. [21] M. Solution of population balance equations using the direct quadrature method of moments. Kumar. Kiparissides. 29 . 1970. Jakobsen. A. [16] J. Lin. Kim and J.org/10. Journal of Colloid and Interface Science. L. Simulation of multicomponent aerosol dynamics. 2005. and orthogonal collocation methods. On the solution of population balance equations by discretization‐II. [20] D. Industrial and Engineering Chemistry Research. J. 57(12):2229–2239. Providence. and S. D. Part I: Dynamic evolution of the particle size distribution in particulate processes undergoing combined particle growth and aggregation. and nucleation. An operator‐splitting Galerkin/SUPG finite element method for population balance equations : stability and convergence. 1991. 36(1):43–73. Journal of Colloid and Interface Science. 51(8):1311–1332. 52(45):15988–16013. I. P. 27(2):255–265. Method of moments with interpolative closure. H. Z. and C. Journal of Aerosol Science. Kumar and D. 2004. Roussos. E. 182(1):81–104. 32(8):1810–C1830. 2002. Galerkin. 2013. L. 1996. Fox. 42(9):705–713. A moving pivot technique. Warnecke. An efficient numerical technique for solving population balance equation involving aggregation. Frenklach. On the solution of population balance equations by discretization‐I. A. Powder Technology. Rhode Island. American Mathematical Society. 1997. G. Warnecke. 2012. Peglow. Kumar and D. Yu. H. Aerosol Science and Technology.

[31] K. Gillespie. 32(3):474–476. The Netherlands. and F . 2007. A third accurate operator splitting method. G. [27] K. Z. Physics of Fluids. Döring. Wei. T. 53(1–2):387–396. Matthies. M. Zhou. 12(2):1–7. Quispel. He. . G. Journal of Aerosol Science. Dordrecht. Pate. Bisetti. Schmeyer. 75:95–104. Ahmed. Acta Numerica.Science and Case Studies [24] Douglas L. K. 11:341–434. SIAM Review. Acceptance‐reject ion sampling made easy. International Journal of Chemical Reactor Engineering. Kinetische Behandlung der Keimbildung in übersättigten Dämpfern. 2014. and Applications. Monte Carlo: Concepts. Applied Numerical Mathematics. 2014. Fishman. [37] G. Springer‐Verlag. Alshaarawi. [28] N. Xiao. and F. Numerical advection of moments of the particle size distribution in Eulerian models. A. Parallel Monte Carlo simulation of aerosol dynamics. and E. D. Simulation of soot size distribution in a counterflow flame. T. 2013. R. and D. Splitting methods. W. 2013. and L. Algorithms. 2011. An exact method for numerically simulating the stochastic coalescence process in a cloud. He. 2014. Springer. 70(0):58–79. Becker and W. A. Nucleation Theory. and L. [25] D. 2011. Journal of Computational and Applied Mathe‐ matics. [36] B. A comparative study of a direct discretization and an operator‐splitting solver for population balance systems. [29] N. Ganesan. Zhou. Monte Carlo simulation of aerosol evolution in a planar mixing layer. Zhou and Z. 2014: 435936. Finite element methods of an operator splitting applied to population balance equations. 2015. Tobiska. Wright Jr. Flury. Computers and Chemical Engineering. 236(6):1604–1621. Anker. McLachlan and G. Attili. [38] H. Mathematical and Computer Modelling. Advances in Mechanical Engineering. and Z. Zhang. 2014. Stabilized finite element discretization applied to an operator‐splitting method of population balance equations. Kalikmanov. Tobiska. J. 24(8):719–752. International Journal of Numerical Methods for Heat & Fluid Flow. Kinneberg. 1975. Simulation of aerosol nucleation and growth in a turbulent mixing layer. Industrial and Engineering Chemistry Fundamentals. Rajamani. [30] F. 1996. Zhou. Xiao. 1990. I. 38:352–369. 26:065106. S. Annalen der Physik (Leipzig). [39] Z. W. Time‐driven and event‐driven Monte Carlo simulations of liquid‐liquid dispersions: a comparison. New York. 24(8):1769–1781. 32(10):1977–1989. Jia and K. Matthies. [35] R. Journal of the Atmospheric Sciences. [34] V.30 Aerosols . [33] R. 1935. Li. M. He. John. [26] K. 2002. [32] K. S. 1986. Ahmed. V. 25:746–752. I.

- 125Uploaded bysongjihyo16111994
- SpielmanUploaded byIrwan Januar
- Lecture 04c - Shortcut Exchanger Design Procedure.pptUploaded bysds
- FM 3-5 NBC Decontamination (2000) WWUploaded byapi-3708163
- Composite Dan Future IPR - 2010Uploaded byekokus
- foam sprayUploaded byShiny Sunil
- pcourseiitdUploaded byShanmugam Subramanyan
- EN 147Uploaded byMohan
- AFT Titan 4 Data SheetUploaded byerjainrachit
- Deposition Velocity EstimationUploaded byGlawenClattuc
- MDV3-VVUQ-v0.5Uploaded byDawei Wang
- SquatUploaded byutkarshgahtori
- Clouds ParticlesUploaded byluisrbarretop09
- 978-1-58503-716-2-1Uploaded byVikram Balaji
- jammu university mechanical engineering syllabusUploaded byAkshit Gupta
- Lecture Slides (3) - Copy.pptxUploaded byAyodeji Samuel Binuyo
- Two Phase FlowUploaded byAbderrahim Ouberri
- SPE-20421-MSUploaded byAsahel Nuñez
- LaminarFlowPipes&Annuli NewtonianUploaded bychem352
- Fluidized BedUploaded byRafique Ahmed Abro
- Effect of Surface Rough Ness on Diffusionlimited Charge TransferUploaded bysashankchappidigmail
- Aerodyn Appl Veh 3 BasicsUploaded byAsha Dash
- Pressure Drop Along Pipe Length - Fluid Flow Hydraulic and Pneumatic, EngineUploaded bybmsprague
- Sonatrach's _well PerformanceUploaded byadrien_ducaillou
- M7l35Uploaded byArun Yoga
- Drop Let EvaporationUploaded bymtsh
- IJETR032825Uploaded byerpublication
- out3Uploaded bymfmechanics
- s 0022112070220996Uploaded byDonVic
- 54.IJMPERDDEC201754Uploaded byTJPRC Publications

- 52442Uploaded bykj185
- 52438Uploaded bykj185
- 52209.pdfUploaded bykj185
- 52143.pdfUploaded bykj185
- 52376Uploaded bykj185
- 52136.pdfUploaded bykj185
- 52175.pdfUploaded bykj185
- 52376.pdfUploaded bykj185
- 52074Uploaded bykj185
- 52606Uploaded bykj185
- 52356Uploaded bykj185
- 52074.pdfUploaded bykj185
- 52433Uploaded bykj185
- 52970Uploaded bykj185
- 52310.pdfUploaded bykj185
- 50761Uploaded bykj185
- 50714Uploaded bykj185
- 52209Uploaded bykj185
- 48951Uploaded bykj185
- 50477Uploaded bykj185
- 52143Uploaded bykj185
- 52310Uploaded bykj185
- 50108Uploaded bykj185
- 50262Uploaded bykj185
- 52136Uploaded bykj185
- 52175Uploaded bykj185
- 49153Uploaded bykj185
- 51678Uploaded bykj185
- 50822Uploaded bykj185