A numerical model of non-equilibrium thermal plasmas, Part I: Transport properties Xiao-Ning Zhang,1,2 He-Ping Li,2,1) A. B. Murphy,3 and Wei-Dong Xia1 1 Department of Thermal Science and Energy Engineering, University of Science and Technology of China, Hefei, Anhui Province 230026, P. R. China 2 Department of Engineering Physics, Tsinghua University, Beijing 100084, P. R. China 3 CSIRO Materials Science and Engineering, PO Box 218, Lindfield NSW 2070, Australia Supplementary Materials: SOLUTION OF THE BOLTZMANN EQUATION A. Modified Chapman-Enskog perturbation method Using the perturbation technique of Chapman and Enskog,1,2 the distribution function f r , ci , t of species i can be given from the solution of the Boltzmann equation (S-1):2 N fi X ci fi i ci fi fi ' f j' fi f j g ij dΩdc j . t mi j 1 (S-1) For the sake of convenience, Eq. (S-1) can be re-expressed as Dfi N J ij fi , f j , Dt j 1 (S-2) Dfi fi X ci fi i ci fi , Dt t mi (S-3) J ij fi , f j fi ' f j' fi f j g ij dΩ dc j , (S-4) with 1) Author to whom correspondence should be addressed. Electronic mail: liheping@tsinghua.edu.cn. 1 where ci , X i and mi are the velocity, external force and mass of species i, r and t are the space vector and time, f i ' is the distribution function after collision of species i, g is the relative speed of the species i and j, ij is the differential collision cross section and is the solid angle. Enskog obtained a series solution by introducing a perturbation parameter to the Boltzmann equation as Dfi 1 N J ij . Dt j 1 (S-5) In fact, Eq. (S-5) corresponds to the Boltzmann equation for the distribution function 1 f , so is merely a scaling factor. Since we eventually return to the value of unity, all i the results are in formal agreement with the original Boltzmann equation (S-2). If the distribution function, fi, is expanded in a series of ε, i.e., fi fi 0 fi 1 (S-6) , where the superscripts indicate the degree of approximation, by substituting the series (S-6) into the modified Boltzmann equation (S-5) and equating the coefficients with the equal powers of , the following set of equations can be obtained N 0 J ij fi 0 , f j 0 , j 1 (S-7) N Dfi 0 J ij fi 0 , f j1 J ij f i 1 , f j 0 J ij f i 0 , f j 0 . Dt j 1 (S-8) Equations (S-7) and (S-8) are the zero-order and first-order approximation of the Boltzmann equation, respectively. These equations allow us to determine the distribution function uniquely. B. Zero-order and first-order solutions 2 In the following derivations, the subscripts “1” or “e” denotes the electrons, while “i (i ≥ 2)” or “h” denotes the heavy-species, and “i (∀i)” represents an arbitrary species for simplicity. For the zero-order solution, the electron–heavy-particle collision terms are expected to have little effect on the distribution functions of heavy-species and electrons due to the small size of the ratio me/mh. Equation (S-7) can be re-written for the electrons f 0 ' 0 ' f 1 f1 0 f 0 g11 dΩ dc 0, (S-9) and for the heavy-species f f f f g N 0 ' i 0 ' 0 j i 0 j ij dΩ dc j 0, (S-10) j 2 where f 0 and c (without any subscript) in Equation (S-9) denote collision partner electrons. Thus, the Maxwellian distribution functions with Te for electrons and Th for heavy-species are obtained by solving the foregoing zero-order approximation equations (S-9) and (S-10) as 3 0 1 f m1 2 m1C12 n1 exp , 2 k BTe 2k BTe (S-11) 3 fi 0 mi 2 mi Ci2 ni exp 2 k BTh 2k BTh i 2 , (S-12) where the peculiar particle velocity of species i is defined as Ci ci v0 , and kB represents the Boltzmann constant. Consequently, the species number densities ( ni ), the mass-averaged velocity ( v0 ) and the temperatures (Te, Th) can be defined as ni f i dci , 0 (S-13) N N i 1 i 1 v0 mi ci f i 0 dci ni mi vi , (S-14) 3 1 n1k BTe m1 C12 f1 0 dc1 , 2 2 (S-15) 3 3 1 N nt n1 kBTh mi Ci2 fi 0dci , 2 2 i 2 N N i 1 i 1 (S-16) where nt ni is the total number density and ni mi is the total mass density. Because of the isotropy of the zero-order distribution function in velocity phase space, all the transport fluxes except for the momentum flux are zero. To obtain the non-zero transport fluxes, it is necessary to derive the first-order perturbation solution.2 The equation for the fi 1 may be written in terms of a perturbation function i , defined by fi 1 fi 0i r , ci , t . (S-17) It is worth noting that the definitions of Eqs. (S-13)-(S-16) have placed certain restrictions on i , namely, f 0 i dci 0 i N m c f dc 0 i i i i i (S-18) 0 (S-19) i 1 2 0 1 1 1 C f dc1 0 N m C (S-20) 2 0 i i i i f dci 0 (S-21) i 2 Thus, Eq. (S-8) may be re-written in terms of this function (S-17) to give Dfi 0 N 0 ' 0 ' ' ' fi f j i j fi 0 f j 0 i j g ij ddc j Dt j 1 N fi j 1 0 ' 0 ' fj 0 0 fi f j g ddc , ij (S-22) j The equations for electrons and heavy-species can then be written, respectively, as Df1 0 f1 0 f 0 1' ' 1 g 11 dΩ dc Dt f1 0 ' f j 0 ' 1' j' f1 0 f j 0 1 j g 1 j dΩ dc j N j 2 N f1 0 ' f j 0 ' f1 0 f j 0 g 1 j dΩ dc j , j 2 4 (S-23) Dfi 0 fi 0 ' f1 0 ' i' 1' fi 0 f1 0 i 1 g i1dΩ dc1 Dt fi 0 f j 0 i' j' i j g ij dΩ dc j N j 2 , ( i 2 ) (S-24) fi 0 ' f1 0 ' fi 0 f1 0 g i1dΩ dc1. Based on the form of Maxwellian f1 0 ' f j 0 ' f1 0 f j 0 1 O m1 m j relationship can distribution be given;3 functions, thus, the we have f1 0 ' f j 0 ' f10 f j 0 due to the fact m1 m j 1 . On the other hand, there exists the relationship i' i O m1 mi 1' 1 for the electron–heavy-particle collisions ( i 2 ); and therefore, the change in the first order perturbation function of heavy species may be neglected compared with that of electrons. According to the foregoing analysis, the zero-order approximation integral terms in Eqs. (S-23) and (S-24) are negligible. The validity of the simplifications can be verified by the very minor differences between the simplified theory and complete theory in comparisons presented in recent works.4-6 Equations (S-23) and (S-24) can be re-written as Df1 0 f1 0 f 0 1' ' 1 g 11dΩ dc Dt N f1 f j 0 0 j 2 ' 1 1 g 1 j dΩ dc j , Dfi 0 fi 0 f1 0 1' 1 g i1dΩ dc1 Dt N fi j 2 0 0 fj ' i ' j i j g ij dΩ dc j . (S-25) (S-26) It should be emphasized that the first integration term of Eq. (S-26), i.e., f 0 i f1 0 g ' 1 1 dΩ dc1 , is retained, unlike in the simplified theory of Devoto.3 i1 The left-hand sides of Eqs. (S-25) and (S-26) can be reduced using Enskog’s equation of change.1,2 We adopt the definition of the diffusion driving force ( di ) introduced by Rat et al.7 5 Df1 0 to take into account the coupling between electrons and heavy species. Thus, and Dt Dfi 0 ( i 2 ) become Dt Df1 0 C1 5 f1 0 W12 C1 ln Th 2W1 W1 : v0 d1 Dt 2 n1k BTe Q 0 2 5 C1 ln W12 C1 ln 1 W12 1 , n1k BTh 2 n1k BTe 3 1 Dfi 0 Ci 5 fi 0 Wi 2 Ci ln Th 2Wi Wi : v0 di Dt 2 ni k BTh Q1 0 2 2 Ci ln 1 W ni k BTh nt n1 kBTh 3 i i (S-27) (S-28) i 2 , where N 1 Q1 0 m1 C1'2 C12 f1 0 f j 0 g 1 j dΩ dc j dc1 , j 2 2 (S-29) represents the change of average kinetic energy of electrons via elastic collisions with the heavy particles, and d1 di i N n X j j 1 j x 1 N p n j X j n1 X 1 1 1 p 2 x1 , j 1 D D x ni X i i i D xi 1 p p x1 p xi D D2 where xi ni nt is the mass fraction of species i ( 1, (S-30) i 2 , (S-31) , N ) . The thermal non-equilibrium coefficient is defined as Te Th . For an arbitrary species i, the partial pressure is N pi ni k BTi , p pi represents the total pressure, Wi i 1 mi Ci corresponds to the 2kBTi 1 2 reduced velocity and Wi Wi is the symmetric traceless tensor WW i i Wi I , with I as the 3 6 unit tensor. In addition, D , 1 and i ( i 2 ) are given by D 1 x1 1 , 1 x1 p 1 x1 D2 and i xi x1 p D 2 , respectively. C. Expressions for the integral equations Comparing the form of Eq. (S-25) with that of Eq. (S-27), the perturbation function 1 for electrons can be expressed as N N j 1 j 1 1 A1 ln Th B1 : v0 C1j d j D1Q1 0 E1j j ln F1 ln . (S-32) It is important to note that the form of the third term on the right-hand side of Eq. (S-32), N C j 1 d j , is equivalent to taking into account the diffusion process between electrons and j 1 heavy-species, which makes the calculation of the complete set of diffusion coefficients available. This differs from the simplified theory presented in Refs. 3, 8-9. Similarly, the expression of i for heavy-species ( i 2 ) can be written as N N i Ai ln Th Bi : v0 Ci d j Di Q1 Ei j j ln Fi ln . (S-33) j j 1 0 j 1 Substituting 1 and i into Eqs. (S-25) and (S-26), we obtain the expressions of the tensors 1 s ,k and i s ,k ( i 2 ) for the electrons and heavy species, respectively, as follows: R1 s ,k s ,k s ,k s ,k s ,k 0 0 1 1 f1 f g 11dΩdc ' ' N s ,k s ,k 0 0 1 1 f1 f j g 1 j dΩdc j , j 2 Ri s ,k ' (S-34) s ,k s ,k 0 0 1 1 fi f1 g i1dΩdc1 ' N s ,k s ,k s ,k s ,k 0 0 i j i j fi f j g ij dΩdc j . j 2 ' ' (S-35) The expressions for R1 s ,k , 1 s ,k , Ri s ,k and i s ,k are listed in Table I. The term Di (∀i) is, in fact, not taken into account in the following derivations of the transport 7 coefficients, since the corresponding integrals representing the transport fluxes vanish identically. Thus, Eqs. (S-34) and (S-35) and the auxiliary equation N miTi i s ,k Wi fi 0 dci 0, i 1 (S-36) which is equivalent to Eqs. (S-18)-(S-21), serve to specify i s ,k uniquely. Solutions to the integral equations (S-34) and (S-35) are obtained with a similar method to that presented in Refs. 1 and 2, in which the unknown quantity i s ,k are expanded in a series of Sonine polynomials s ,k i 1 i tip s ,k p 0 Sn p Wi 2 , (S-37) where is the so-called level of approximation to the transport coefficients. The value of the index n, the meaning of tensor i and the unknown coefficient tip s ,k are given in Table II. s ,k For simplicity, Rim is defined as Rim s ,k Ri s ,k : i Sn m Wi 2 dci , (S-38) Eventually, it is shown that tip ( ) can be obtained by solving the following equations: s ,k 1 R1m Q1mp t1 p s ,k s ,k , (S-39) p 0 and Rim s ,k 1 N Qijmp t jp s ,k p 0 j 2 1 * s ,k Qimp , 1 t1 p (i 2), (S-40) p 0 with Q1mp n1n j 1Sn m W12 ; 1Sn p W12 N 1j j 1 m n 1Sn 2 1 W ; S W , 2 1 8 p n 2 1 (S-41) when t jps ,k b jp Qijmp Qijmp mp n j m jT j mp Qii m 0 p 0 ( i 2, j 2 ) Qij ni miTi when t jps ,k a jp , c jps ,k , ejps ,k or f ip , (S-42) and * Qimp 1 * Qimp mp* n1 m1T1 mp 1 ( i 2) Qii m 0 p 0 Qi1 n m T i i i when t1 ps ,k b1 p when t1 ps ,k a1 p , c1 sp,k , ejps ,k or f1 p . (S-43) The second terms in the lower expressions of Eqs. (S-42) and (S-43) arise from the auxiliary equation (S-36), which can be written as N n miTi ti0s ,k 0, i (S-44) i 1 * and Qijmp and Qimp are defined as 1 Qijmp ni nk ij i Sn m Wi 2 ; i Sn p Wi 2 ik k 2 N W ; S W , n n S W ; S W m jk i Sn * Qimp 1 p 2 i k m i 1 The expressions for R1ms ,k and Rim s ,k i n n p 2 i 2 k 1 n (S-45) ik 2 1 i1 . (S-46) i 2 can then be obtained as listed in Table III. In Eqs. (S-45) and (S-46), the terms of form Gij ; Hij are the bracket integrals defined by ij Chapman and Cowling,8 which may be written as a linear combination of a set of collision * integrals defined. Expressions for some of the bracket integrals, Q1mp , Qijmp and Qimp in 1 terms of the collision integrals are given in Refs. 1-3, and 10. D. COEFFICIENTS OF THE SONINE POLYNOMIALS The coefficients tip s ,k listed in Table II can be derived from Eqs. (S-39) and (S-40) as follows. 9 c1 sp,k 4 Q100 Q101 Q102 Q103 Q110 Q120 Q130 Q111 Q112 Q121 Q122 Q131 Q132 Q113 Q123 Q133 p0 p1 p3 p2 k BTe 1s 1k 2me k BTe 3 0 0 0 0 Q100 Q110 Q120 Q130 Q101 Q102 Q111 Q112 Q121 Q122 Q131 Q132 3 , Q103 Q113 Q123 Q133 (S-47) k BTh ls lk 3 0 p* s ,k Ql1 c1 p 2ml k BTh p 0 Qlj00 Qlj01 Qlj02 Qlj03 Qlj10 Qlj11 Qlj12 Qlj13 Ql11p*c1 p Qlj20 Qlj21 Qlj22 Qlj23 Ql21 p*c1 sp,k Qlj30 Qlj31 Qlj32 Qlj33 Ql31p*c1 sp,k 0 0 3 s ,k p 0 3 p 0 3 ci0s ,k 4 ij 0 0 p 0 Qlj00 Qlj01 Qlj02 Qlj03 Qlj10 Qlj11 Qlj12 Qlj13 Qlj20 Qlj21 Qlj22 Qlj23 Qlj30 Qlj31 Qlj32 Qlj33 , (S-48) where Q22mp Q2mpN Qljmp , QNmp2 10 mp QNN (S-49) e1 sp,k 4 Q100 Q101 Q102 Q103 Q110 Q120 Q130 Q111 Q112 Q121 Q122 Q131 Q132 Q113 Q123 Q133 p0 p1 p3 p2 3 k BTe 1s 1k 2me k BTh 0 0 0 0 Q100 Q110 Q120 Q130 Q101 Q102 Q111 Q112 Q121 Q122 Q131 Q132 3 , Q103 Q113 Q123 Q133 (S-50) k BTh ls lk 3 0 p* s ,k Ql1 e1 p 2ml k BTh p 0 Qlj00 Qlj01 Qlj02 Qlj03 Qlj10 Qlj11 Qlj12 Qlj13 Ql11p*e1 p Qlj20 Qlj21 Qlj22 Qlj23 Ql21 p*e1 sp,k Qlj30 Qlj31 Qlj32 Qlj33 Ql31p*e1 sp,k 0 0 3 s ,k p 0 3 p 0 3 ei0s ,k 4 ij a1 p 4 0 0 p 0 Qlj00 Qlj01 Qlj02 Qlj03 Qlj10 Qlj11 Qlj12 Qlj13 Qlj20 Qlj21 Qlj22 Qlj23 Qlj30 Qlj31 Qlj32 Qlj33 Q100 Q101 Q102 Q103 Q110 Q111 Q112 Q113 Q120 Q130 Q121 Q122 Q131 Q132 Q123 Q133 0 0 p0 p1 p3 0 p2 0 kT 15 ne B e 2 2me Q100 Q110 Q101 Q102 Q111 Q112 Q103 Q113 Q120 Q130 Q121 Q122 Q131 Q132 Q123 Q133 11 , (S-51) , (S-52) 3 Ql01 p*a1 p Qlj00 Qlj01 Qlj02 Qlj03 Qlj10 Qlj11 Qlj12 Qlj13 Qlj20 Qlj21 Qlj22 Qlj23 Ql21 p*a1 p Qlj30 Qlj31 Qlj32 Qlj33 Ql31p*a1 p 0 0 p 0 3 kT 15 nl B h Ql11p*a1 p 2 2ml p 0 3 p 0 3 ai 0 4 ij 0 0 Qlj00 Qlj01 Qlj02 Qlj03 Qlj10 Qlj11 Qlj12 Qlj13 Qlj20 Qlj21 Qlj22 Qlj23 Qlj30 Qlj31 Qlj32 Qlj33 0 kT 15 ne B e 2 2me 0 0 f10 4 Q100 c11 s ,k 4 3 p 0 Q101 Q102 Q103 Q111 Q112 Q113 Q121 Q122 Q131 Q132 Q123 Q133 Q100 Q110 Q120 Q101 Q102 Q111 Q112 Q121 Q122 Q103 Q113 Q123 Q130 Q131 Q132 Q133 , , k BTe 1s 1k Q102 2me k BTe Q103 Q110 0 Q112 Q113 Q120 0 Q122 Q123 Q130 0 Q132 Q133 Q100 Q101 Q102 Q103 Q110 Q111 Q112 Q113 Q120 Q121 Q122 Q123 Q130 Q131 Q132 Q133 12 (S-53) (S-54) , (S-55) 3 k BTh ls lk 3 0 p* s ,k Ql1 c1 p 2ml k BTh p 0 Qlj00 Qlj01 Qlj02 Qlj03 Qlj10 Qlj11 Qlj12 Qlj13 Ql11p*c1 p Qlj20 Qlj21 Qlj22 Qlj23 Ql21 p*c1 sp,k Qlj30 Qlj31 Qlj32 Qlj33 Ql31p*c1 sp,k 0 0 3 s ,k p 0 3 p 0 3 ci1s ,k 4 0 ij 0 Q100 Q110 f11 4 Q100 e11 s ,k 4 p 0 Qlj00 Qlj01 Qlj02 Qlj03 Qlj10 Qlj11 Qlj12 Qlj13 Qlj20 Qlj21 Qlj22 Qlj23 Qlj30 Qlj31 Qlj32 Qlj33 0 Q102 Q103 kT 15 ne B e 2 2me Q112 Q113 0 0 Q122 Q132 Q123 Q133 Q120 Q130 Q100 Q110 Q120 Q101 Q102 Q111 Q112 Q121 Q122 Q103 Q113 Q123 Q130 Q131 Q132 Q133 3 , , k BTe 1s 1k Q102 2me kTh Q103 Q110 0 Q112 Q113 Q120 0 Q122 Q123 Q130 0 Q132 Q133 Q100 Q101 Q102 Q103 Q110 Q111 Q112 Q113 Q120 Q121 Q122 Q123 Q130 Q131 Q132 Q133 13 (S-56) (S-57) , (S-58) k BTh ls lk 3 0 p* s ,k Ql1 e1 p 2ml k BTh p 0 3 Qlj00 Qlj01 Qlj02 Qlj03 Qlj10 Qlj11 Qlj12 Qlj13 Ql11p*e1 p Qlj20 Qlj21 Ql22 j Qlj23 Ql21 p*e1 sp,k Qlj30 Qlj31 Qlj32 Qlj33 Ql31p*e1 sp,k 0 0 3 s ,k p 0 3 p 0 3 ei1s ,k 4 ij 0 0 p 0 Qlj00 Qlj01 Qlj02 Qlj03 Qlj10 Qlj11 Qlj12 Qlj13 Qlj20 Qlj21 Qlj22 Qlj23 Qlj30 Qlj31 Qlj32 Qlj33 Q100 Q110 a11 4 0 Q102 Q103 kT 15 ne B e 2 2me Q112 Q113 0 0 Q122 Q132 Q123 Q133 Q120 Q130 Q100 Q110 Q120 Q101 Q102 Q111 Q112 Q121 Q122 Q103 Q113 Q123 Q130 Q131 Q132 Q133 , (S-59) , (S-60) 3 Ql01 p*a1 p Qlj00 Qlj01 Qlj02 Qlj03 Qlj10 Qlj11 Qlj12 Qlj13 Qlj20 Qlj21 Qlj22 Qlj23 Ql21 p*a1 p Qlj30 Qlj31 Qlj32 Qlj33 Ql31p*a1 p p 0 3 kT 15 nl B h Ql11p*a1 p 2 2ml p 0 3 p 0 3 ai1 4 0 ij 0 p 0 0 00 lj 10 lj 20 lj 30 lj 0 01 lj 11 lj 21 lj 31 lj 02 lj 12 lj 22 lj 32 lj 03 lj 13 lj 23 lj 33 lj Q Q Q Q Q Q Q Q Q Q Q Q Q Q Q Q 14 . (S-61) REFERENCES 1 J. O. Hirschfelder, C. F. Curtis, and R. B. Bird, Molecular Theory of Gases and Liquids, 2nd ed. (Wiley, New York, 1964). 2 S. Chapman and T. G. Cowling, The Mathematical Theory of Non-Uniform Gases, 3rd ed. (Cambridge University Press, Cambridge, England, 1970). 3 R. S. Devoto, Ph. D. Thesis, Stanford University (1965). 4 V. Colombo, E. Ghedini, and P. Sanibondi, Prog. Nucl. Energy 50, 921 (2008). 5 V. Colombo, E. Ghedini, and P. Sanibondi, J. Phys. D: Appl. Phys. 42, 055213 (2009). 6 V. Colombo, E. Ghedini, and P. Sanibondi, Plasma Sources Sci. Technol. 20, 035003 (2011). 7 V. Rat, P. Andre, J. Aubreton, M. F. Elchinger, P. Fauchais, and A. Lefort, Phys. Rev. E 64, 026409 (2001). 8 C. Bonnefoi, Ph. D. Thesis, University of Limoges, France (1983). 9 J. Aubreton, C. Bonnefoi, and J. M. Mexmain, Rev. Phys. Appl. 21, 365 (1986). 10 R. S. Devoto, Phys. Fluids 10, 2105 (1967). 15 TABLE I. Expressions of R1 s ,k , 1 s ,k , Ri s ,k and i s ,k . R1 s ,k 1 s ,k Ri s ,k ( i 2 ) i s ,k ( i 2 ) 5 f1 0 W12 C1 2 A1 5 fi 0 Wi 2 Ci 2 Ai 2 f1 0W1 W1 B1 2 fi 0Wi Wi Bi f1 0 C1 1s 1k n1k BTe C1s C1k fi 0 f1 0 C1 1s 1k n1k BTh E1s E1k fi 0 5 f1 0 W12 C1 2 Ci is ik ni k BTh Ci ni k BTh is ik Fi 0 F1 Here, ij is Kronecker delta. ij 1 if i j ; otherwise ij 0 . 16 Cis Cik Eis Eik 0 TABLE II. Expressions of i , tip s ,k and n. i s ,k n tip s ,k i Ai 3 2 aip Wi Bi 5 2 bip Wi Wi Cis Cik 3 2 cip s ,k Wi Eis Eik 3 2 eip s ,k Wi Fi 3 2 f ip Wi 17 s ,k TABLE III. Expressions of R1ms ,k and Rim . tip s ,k R1ms ,k s ,k (i 2 ) Rim aip k T 15 n1 B 1 m1 2 2m1 kT 15 ni B i m1 2 2mi bip 5n1 m0 5ni m0 cip s ,k 3 kBT1 1s 1k m0 2m1 kBT1 eip s ,k 3 kBT1 1s 1k m0 2m1 kBTh f ip k T 15 n1 B 1 m1 2 2m1 18 3 3 kBTi is ik m0 2mi kBTi kBTi is ik m0 2mi kBTh 0