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**in Laser Ablation with Application to
**

Nano{Technology

Diomar Cesar Lob~ao12 and Alex Povitsky12

1

2

**Concordia University, Montreal H3G 1M8, Quebec, Canada,
**

lobao@cerca.umontreal.ca,

WWW home page: http://www.cerca.umontreal.ca/~lobao

Centre de recherche en calcul applique{CERCA, 5160, boul. Decarie, bureau 400

H3X 2H9 Montreal, Quebec, Canada

**The aim of this study is to nd optimal conditions for the
**

formation of carbon nanotubes in a laser furnace. This paper will describe our mathematical model and numerical algorithm, and discuss

some of the
uid physics underlying this crucial technology. An axisymmetric unsteady computational gas dynamic model of plume expansion

into ambiance has been developed. In the present work the vapor gas

phase is modeled using the Relaxing TVD scheme in generalized coordinates. A numerical model of pulsed ablated gas is proposed based

on the mass, momentum, and energy conservation laws. The proposed

model implements a multi-species formulation for concentration of chemical components combined with the compressible Euler equations. To advance the solution in time, this set of equations is integrated numerically

by second-order Runge-Kutta scheme.

Abstract.

1

Introduction

**Known processes of production of carbon nanotubes-tubes include laser ablation
**

(LA), chemical vapor deposition (CVD), and decomposition of high-pressure

carbon oxide (HiPco). The practical choice of the process is a trade-o between

product quality and quantity. All processes are controlled by metal catalyst

particles that initialize synthesis of carbon nanotubes from feed-stock gas or

ejected plume. Similar to the HiPco modeling [7], the LA CFD model is based

on the combined Eulerian and Lagrangian approach applied to the tracking of the

trajectories of catalyst particles. The Lagrangian approach to track temperature

of the catalyst particles in the plume is implemented to evaluate the eÆciency of

the process. In the laser vaporization process, the feedstock plume loaded with

catalyst particles expands explosively into the background gas. The thermal

behavior of catalyst particles is critical for nanotubes synthesis.

Available experimental data [1],[2] include average plume temperature at a

given time moment and the plume geometric shape. Our computational results

are in good agreement with these computational and experimental results. There

is no available experimental data about temperature of individual catalyst particles. The present code perform very well in very low ambient pressure, pressure

of order of 10 6 atm as well as up to 1:0 atm has been tested.

Shock waves were formed in the ambient gas in the case of the explosive ablation. The propagation of incident and re
ected shock waves aects the plume

behind it. The plume mixing is caused by the Raleigh{Taylor instability at the

plume{to{gas interface and the baroclinic deposition of vorticity while the re
ected shock wave interacts with the plume [7]. For the assessment of the proposed mathematical model and numerical method, numerical results are compared with those obtained in the experiments found in [1],[2] where the ambient

gas was the inert Argon and the substrate target material was the Carbon Trimmer C3.

2

Governing Equations

**The compressible Euler equations written in general curvilinear coordinates ;
**

for unsteady
ows take the following form:

@ Q~ + @ F~

@ t~ @

@ G~

@

+

= S~

(1)

For generality all variables will be non{dimensionalized. Although the parameters used in the non{dimensionalization process are arbitrary, freestream quantities are usually used. Applying a non-dimensionalization to the Euler equations

leaves all equations in the same form as before, so they can be viewed as equations in the new non{dimensional variables. The conserved variable vector and

uxes are given as,

Q

2

3

66 u 7

Æ 6 v 777

= 6

J 66 E 77

4 C1 5

F

C

2

U 3

6

uU + xp 77

6

6

Æ vU + y p 77

= 6

J 66 (E + p)U 77

4 C1 U 5

C U

2

G

(2)

2

2

V 3

66 uV + x p 7

7

6 vV + y p 7

Æ

7

= 6

6

J 6 (E + p)V 77

4 C1 V 5

S

2 3

0

6

607

7

16

p 77

= 6

J 66 0 77

405

(3)

C V

0

T

Where is the density, m = (U; V; C ; C ) is mass, E is total energy

per unit volume, p pressure, and C ; C are mass fraction of two species being

considered respectively. U; V are the contravariant velocities [8] which are in directions normal to constant ; surfaces respectively, and J = 1 = [x y x y ]

is the Jacobian of transformation. Æ is the radial axisymmetrical coordinate in

2

1

1

2

2

**direction, for 2D full geometry Æ = 1 and S = 0. The quantities x and x
**

are the metrics of the transformation (x; y ) ! (; ). In the numerical scheme,

the metrics are approximated by second{order nite dierences where the indices i; j are related to the ; directions respectively. Second order three{point

backward nite dierence are used for the boundary points.

The total energy is dened by

E

p + (u 2+ v )

2

=

2

+

h

(4)

**where h = h(hi ) is the enthalpy per unit mass for each species. The equation of
**

state for multi-species
ow can be written as,

p=

2

X

i=1

pi =

2

X

i=1

2

X

Ci Ri T = ( CiRi )T = RT

i=1

where T is temperature and R is dened as, R =

3

(5)

P2

i=1 Ci Ri [9].

Numerical Scheme

The relaxing TVD scheme as described in [22] and [6] provides high order accuracy to approximate solutions of compressible Euler equations (Eq.(1)) written

in conservation form. Relaxation methods make use of the characteristic variables of the system and nite speed of propagation and do not need Riemann

solvers. Using the same idea the relaxing TVD is very similar to central schemes

as those described in [23] and [11]. The method used to solve Euler equations

is the monotone upwind scheme for conservation laws (MUSCL). The MUSCL

alone when applied to Euler equations meets diÆculties by the fact that the

momentum and energy
uxes depend on the pressure. In order to determine the

ow upwind direction it is needed to calculate the
ux Jacobian eigenvectors

matrices at each cell at each time step. This is straight for advection equation

since that the velocity can be used to dene the
ow upwind direction, however

it is not for the Euler equations. The relaxing TVD scheme oers an alternative

to circumvent the need for calculating the
ux Jacobian eigenvectors matrices

the for Euler equations, which for multi{species and or reactive chemical systems

is extremely economical and eÆcient. The MUSCL method is completed with a

second order explicit Runge{Kutta time integrator.

3.1

Relaxing TVD Scheme

**Let us consider a 1D system of conservation laws and illustrate the relaxing TVD
**

scheme, since the generalization to multi{dimensional cases is straightforward.

@q

@t

+

@F [q]

@x

=0

(6)

This system is replaced by the relaxing system as,

@q + @cv = 0

@t @cq

@x

@v

@t + @x = 0

(7)

**where c(x; t) is a free parameter called freezing speed [6]. The essence of the
**

method is to apply Strang [12] splitting on these two equations. A TVD
ux

slope limiter is applied to the linear advection equation, also called relaxation

system with v = F [q ]=c and it is used to calculate
uxes, while an explicit time

integration is implemented using second order Runge{Kutta method. In [6] is

shown that this scheme is TVD under the constraint that c is grater than the

characteristic speed u given by @F

@q . One way to satisfy this condition is to dene

c as: c = j u j + a, where a is the local speedq+ofv sound. To solve

the relaxed

system, it is decoupled using variables w1 = 2 and w2 = q 2 v . The linear

system of equations

@w

@t

+

@cw

@x

=0

(8)

**is discretized in space using MUSCL scheme as described in [6].
**

The conserved averaged quantities w are dened at integer grid cells xi .

It is needed to dene the
uxes at cell boundaries, F = cw where F =

F (w1 ) F (w2 ) at xi+1=2 . Then, @x cw = F (xi+1=2 ) F (xi 1=2 ). The remaining

step is to dene the
ux F at the half cells. The rst{order upwind denition

is F (xi+1=2 ) = cw(xi ), assuming
ow is to right. There are two second{order

choices: 1) (cw(xi ) + cw(xi+1 ))=2 and 2) (3=2)cw(xi (1=2)cw(xi 1 )). Generalizing these choices is possible to write F (xi+1=2 ) = cw(xi ) + w, where

w+ = cw(xi+12) cw(xi) and w = cw(xi) 2cw(xi 1) . Dene the limiter minmod

as minmod(a; b) = (sign(a) + sign(b))Min(j a j; j b j)=2. It chooses the argument with smaller absolute magnitude if the magnitudes have the same sign, and

returns zero otherwise. The w = minmod(w+ ; w ) limiter is the simplest

TVD MUSCL choice. At the extrema, minmod=0, and the second order scheme

reverts to a rst order upwind scheme. The mathematical justication for this

can be found in [13]. The time step is determined by satisfying the CFL condit

tion, cmax

x 1. Note that a new freezing speed is computed for each partial

time step in the Runge-Kutta scheme.

For more than one spatial dimension, the simplest generalization is to apply

the freezing advection to each dimension. In two dimensions, the system( 1) can

be split using Strang technique [12] into two separate 1D equations which are

solved in sequential way. Consider that the operator Li represent the updating

of q t to q t+t making use of the
ux in the i direction. The sweep has to be

symmetrical, rst the forward sweep is carried out as, q t+t = L L q t and them

the reverse sweep is carried out as, q t+2t = L L q t+t . Note that the same

time step t has to be used in order to keep the second order accuracy in time.

4

Experimental Setup and Computational Model

**Radiation of a laser beam is focused on Carbon C3 solid target. The diameter of
**

the focusing spot is 5mm, placed inside a chamber containing Argon at pressure

of 1atm and temperature of 1500K [1],[2]. The pulse ring duration is 20ns. Under these conditions, the laser delivers 100atm pressure at 5000K for the gaseous

plume. The axisymmetrical chamber is 5:0cm of diameter and 25cm long. The

physical domain is discretized in a computational domain using a structured

grid, having 250 50 nodes in the axial and radial directions, respectively. The

initial conditions at the grid points corresponding to the 5mm diameter laser

beam spot was kept on for approximately 20:0ns. At the end of this time, the

carbon mass fraction boundary conditions are turned o and replaced by a non{

penetrating solid wall boundary condition. Then, the numerical code solves this

ow eld as the time progress. The out
ow is set as adjustable sub/supersonic

boundary. The solid boundary is treated imposing the tangential velocity satisfying n V = 0, n is the normal surface unit vector. On the axisymmetrical

boundary, simple extrapolation boundary condition is adopted.

5

Modeling of plume dynamics

**In all simulations, a sequence of CFL numbers was used in order to integrate the
**

equations with the maximum time step and to avoid the blow up of the solution

due to the large pressure gradients, which may cause non-linear instability. For

the rst 180 steps CFL of 0:0001 is used and the time step is of the order of

10 11 sec. The CFL increases after any 180 of 0:001, and is respectively equal to:

0:01; 0:1; 0:3 and 0:5, which is the maximum CFL. The time step t is computed

at the beginning of each step and is given by the maximum
oweld characteristic

velocity ; as t = maxCFL

. The most severe test case for the present code

( + )

is when the ambient pressure is close to the vacuum, in such situation some codes

doesn't work well or even doesn't work at all for such low pressure. In recent

years, material science community expresses strong interest to carry out laser

ablation based synthesis of nanotubes with very low chamber gas pressure since

the higher ambient gas pressure may halt the production of carbon nanotubes

(see [18] for more details). As the Argon pressure had decreased to near to

vacuum conditions, the plume expansion tends to process in much higher rate

than that for standard ambient pressure conditions.

The following computational results are obtained for the ambient pressure of

Argon equal to 10 6 atm. The plume shape is depicted in Fig. 1 left at 2:6s. At

this time moment, the plume has not hit the wall and the plume expansion is

similar to that for Sedov{Taylor blast. At a later time moment, as for example,

at 10s as depicted in Fig. 1 right the plume reaches the wall of the chamber tube

and its shape substantially deviates from the original semi{spherical surface.

**Plume Mass Fraction Carbon C3 - Vacuum
**

Time= 2.6 microsec

0.1

0

0.1

0

0

0.1

Symmetrical axis

Fig. 1.

5.1

0.939867

0.877209

0.814551

0.751893

0.689236

0.626578

0.56392

0.501262

0.438605

0.375947

0.313289

0.250631

0.187973

0.125316

0.0626578

0.2

Radial axis

Radial axis

0.934721

0.869007

0.803293

0.737579

0.671865

0.606152

0.540438

0.474724

0.40901

0.343296

0.277582

0.211868

0.146155

0.0804407

0.0147268

**Plume Mass Fraction Carbon C3 - Vacuum
**

Time= 10.0 microsec

0.3

0.2

0.2

0

0.1

0.2

0.3

Symmetrical axis

Plume Expansion Carbon C3. Left, vacuum at 2:6s. Right, vacuum at 10:0s.

**Lagrangian Approach to Model the Temperature of Catalyst
**

Particles

**The 10 uniformly{distributed initial positions for the streaklines are chosen at
**

the laser spot. The streakline is a line connecting particles released from the

same location. Since the catalyst particles are of sub{micron size, they follow

the streaklines and do not have their own inertia. A Runge{Kutta second order

explicit scheme is used to integrate in time the streaklines. The Langrange's

approach has an advantage over the Euler's approach since it gives the temperature of each catalyst particle as a function of time. Having the temperature of

catalyst particles as a function of time, it will be possible to model kinetics of

formation of carbon nanotubes.

The temperature along streaklines for the above mentioned 10 particles is

shown in Fig. 2 left. The smooth temperature drop is clearly observed for the

initial phase of plume expansion into the vacuum. In Fig. 2 right the instantaneous plume temperature distribution and velocity vector eld are shown. The

stagnation points in the
oweld appear as a result of interaction of plume with

the wall. The particles move upstream passing through regions of higher temperature. In the case of laser ablation into vacuum, the velocity eld is a quite

complex vector eld, that includes the contact lines, boundary curves dividing

vortices, and critical points.

For the laser ablation into vacuum, the temperature of catalyst particles is

quite dierent from the maximum temperature of the plume. While the latter

temperature tends to increase up to 28 second, the temperature of catalyst

particles increases until the particles become aected by the backward velocity.

The re
ected shock waves caused by the wall are relatively weak and do not

cause visible temperature jumps along trajectories of catalyst particles. In the

case of low ambient pressure, the major reason for particle temperature jumps

is a backward motion of particles upstream of the stagnation point.

16

**Temperature of Catalyst Particles
**

Moving along Streaklines

15

Temperature, T/300 K

14

13

12

11

10

9

8

7

6

5

0.00E+00

1.00E-05

2.00E-05

3.00E-05

Time, microsecond

**Fig. 2. Temperature Streaklines - Vacuum, Left. Right, Temperature Contour/Velocity
**

Field - Vacuum.

5.2

Injection Velocity

**All our previous simulations used a zero carbon injection velocity (iv ). Carbon
**

injection velocity simulates the rate of carbon mass ablation as it is injected into

the
oweld by the laser ring process [1]. To nd carbon injection velocity, one

should model melting and vaporization processes, that is out of scope of this

paper. In this paper, we consider the range of carbon injection velocities and

nd the features of temperature dynamics of catalyst particles as a function of

injection velocity. Gaseous carbon is released with a velocity rate that is non{

dimensionalized by the freestream sound speed. The carbon injection velocity

is kept on during the plume injection process. After the 20 ns plume injection

period, the injection velocity is turned o and replaced by the chamber boundary

condition.

For iv = 15:0, the carbon plume concentration is depicted in Fig. 3 left, the

temperature along streaklines is shown in Fig. 3 right, and the peak temperature

prole as a function of time is shown in Fig. 4 left. To show that temperature

oscillations of catalyst particles are caused by crossing the shock waves, the pressure along the streaklines is shown in Fig. 4 right. To summarize, the temperature

of particles substantially increases with the increase of injection velocity. However, the amplitude of temperature oscillations increases as well that may cause

problems of performance of particles as good catalysts.

6

Conclusion

**In the current research, the investigation has been carried out by numerical
**

simulation of the carbon plume expansion after the laser had red at the target.

The numerical modeling is based on unsteady multi{species formulation for Euler

**Fig. 3. Carbon C3 Plume for iv = 15:0, Left. Right, Temperature Streaklines for
**

iv = 15:0.

**equations using the TVD{based numerical discretization. The presented model
**

qualitatively ts the available experimental results for plume dynamics in carbon

nanotubes synthesis. Relaxing TVD scheme appears to have important numerical

features suitable for modeling of plume dynamics in laser ablation. In this work

we have discovered that:

{

{

{

{

**The high pressure initial conditions are similar to that of explosions. The
**

very strong shock and large gradients of conserved variables are correctly

presented by this numerical scheme.

The used relaxing TVD scheme does not show a problem to model low

ambiance pressure conditions close to vacuum.

The Lagrangian approach reveals important structures of shock interaction

with plume that are not explicitly observed in Eulerian pressure and concentration isolines.

Using dimensional splitting, it is a straightforward task to implement the

code in parallel environment of the Silicon Graphics F90 system.

**The proposed mathematical model gives a physical insight into the plume
**

dynamics in laser ablation:

{

{

**The reasons for non{monotonic behavior of temperature of catalyst particles
**

are interaction of particles with re
ected shock waves and circular motion of

the particles caused by formation of vortical zones, stagnation points, and

sliplines. While the former reason is important for higher{pressure of the

ambient gas, the latter reason plays its role for near{vacuum condition.

The position of the front of the plume shows some discrepancies with experiments [2]. The position of the front of the plume primarily depends on the

injection velocity, which may be used as a tuning parameter to correspond

**Peak Temperature Prole for iv = 15:0, Left. Right, Pressure Streaklines for
**

iv = 15:0.

Fig. 4.

{

**numerical modeling with experiments. The plume propagation reveals to be
**

much slower than that of the leading shock wave especially for low injection

rate.

The self{similar solution for plume expansion revealed good agreement with

t4=5 power scale law rather than with Sedov{Taylor solution t2=5. This holds

even for very short duration of plume ejection.

Acknowledgments Authors were supported by the NSERC grant and by Con-

**cordia University Start{up Funds of Dr. Povitsky. The authors wish to thank
**

the Centre de Recherche en Calcul Applique{CERCA (Montreal) for the logistic

and computational facilities available during this work time. The rst author

thanks Dr. Ian Stewart, University of Bristol U.K., for his comments.

References

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Nanotube Production. 8Th AIAA/ASME Joint Thermophysics and Heat Transfer

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2. Puretzky, A.A., Chittenhelm, H., Fan, X., et al., Investigations of Single-Wall Carbon Nanotube Growth by Time{Restricted Laser Vaporization. Physical Review B,

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3. Zeldovich, Y.B., Raizer, Y.P., Physics of Shock Waves and High-Temperature Hydrodynamic Phenomena. Ed. by W.D. Hayes, R.F. Probstein, Academic Press, London, 1966.

4. Anisimov, S.I., Baverle, D. and Lukyanchuk, B.B., Physical Review B., Vol. 48,

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5. Sedov, L.I., Similarity and Dimensional Methods in Mechanics, Academics Press,

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Arbitrary Space Dimensions", Comm. Pure Appl. Math. 48, pp. 235-276, 1995.

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Conference, Orlando, FL, 1993.

9. Stall, D.R. and Prohet, H., JANAF Thermochemical Tables, National Standard

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10. Anderson, J.D., Hypersonic and High Temperature Gas Dynamics, McGraw-Hill,

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14. Yee, H.C. and Harten, A., Implicit TVD Schemes for Hyperbolic Conservation

Laws in Curvilinear Coordinates, AIAA Paper n. 85-1513, 1985.

15. Harten, A., On a Class of High Resolution Total Variation Stable Finite Dierence

Schemes, SIAM Journal Numerical Analysis, Vol.21, pp.1-23, 1984.

16. Aregba-Driollet, D., and Natalini, R., Discrete Kinetic Schemes for Multidimensional Systems of Conservation Laws. SIAM J. Numer. Anal. 37, pp. 1973-2004,

2000.

17. Valery, B., Rivie, K., and Israel, S., Converting Spatial to Pseudotempral Resolution in Laser Plasma Analysis by Simultaneous Multiber Spectroscopy, Anal.

Chem., 72, No. 13, pp. 2987-2994, 2000.

18. Chen, K.R., Leboeuf, J.N, and et al., Mechanisms Aecting Kinetic Energies of

Laser-Ablated Materials, J. VaC. Sci. Technol. A14(3), pp.1111-1114, 1996.

19. Kim, J.U., Clemens, N.T., and Varghese, P.L., Experimental Study of an Underexpanded Pulsed Laser-Jet, AIAA-99-0452, 37th Aerospace Sciences Meeting, Reno,

Jan., 1999.

20. Kim, K.J., and Wilson, D.E., Theoretical Analysis of a Plasma Jet impinging on a

Nonreacting Surface, AIAA-99-0455, 37th Aerospace Sciences Meeting, Reno, Jan.,

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21. Dabora, E.K., Variable Energy Blast Waves, AIAA J., vol. 10, no. 10, pp.13841386, 1972.

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Spectroscopy by Shock Wave Propagation. Spectrochimica Acta Part B 56, pp.609{

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