Modeling of Plume Dynamics in Laser Ablation with Application to Nanotubes Synthesis

D. Lobão1 and A. Povitsky2
Department of Mechanical and Industrial Engineering Concordia University, 1455 de Maisonneuve Blvd. West Montreal, Quebec, Canada H3G-1M8 CERCA, Centre de Recherche en Calcul Applique 5600, boul. Décarie, bureau 400 H3X 2H9 Montréal, Québec, Canada

Known processes of production of carbon nano-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-off between product quality and quantity. All processes are controlled by metal catalyst particles that initialize synthesis of carbon nanotubes from feedstock gas or ejected plume. This study is aiming at finding the optimal conditions of the formation of carbon nanotubes in laser furnace, proposing needed mathematical models and numerical algorithms, and discussing fluid physics features crucial for this technology. An axisymmetric unsteady computational gas dynamic model of plume expansion into ambience has been developed. In the present work the vapor gas phase is modeled using the Relaxing TVD scheme [6] in generalized coordinates [8]. In the present work, a numerical model of pulsed ablated gas is proposed based on the mass, momentum, and energy conservation laws. The proposed model implement 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 secondorder Runge-Kutta scheme. 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 efficiency 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 [2] include average plume temperature at a given time moment and the plume geometric shape. Our computational results that have been obtained at this stage of research are in good agreement with these experimental results. There is no available experimental data about temperature of individual catalyst particles.

Post-Doc Fellow at Concordia University, Dept. of Mechanical and Industrial Engineering and affiliated researcher CERCA 2 Associate Professor at Concordia University, Dept. of Mechanical and Industrial Engineering and affiliated researcher at CERCA

Analytical approach to the plume expansion into vacuum can be described as self-similar and adiabatic [3,4]. Our model is suitable for the wide range of surrounding gas pressure and the numerical results have been compared with above-mentioned analytical solution in the limit case of vacuum. In the situations with realistic ambient pressures the socalled point blast model [5] can be applied, however, in the more recent experiments low pressure is kept into the chamber containing Argon. The Sedov-Taylor self-similar solution [5] can be used as an approach to predict the shock wave expansion and plume formation behind it. For low ambient pressure, Anisimov [4] solution for plume expansion in vacuum has been used in our research to validate the code and to find the range of ambient pressures where this solution is adequate. Shock waves were formed in the ambient gas in the case of the explosive ablation. The propagation of incident and reflected shock waves affects 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 reflected shock wave interacts with the plume. An interface between fluids of different densities is unstable when subjected to an acceleration directed from the heavy fluid to the light fluid. Such acceleration is related to the density difference of the catalyst particles. The relative strength of different mixing mechanisms and validity of self-similar solution for plume expansion will be discussed in our presentation. For the validation of the proposed mathematical model and numerical method, numerical results are compared with those obtained in the experiments [1,2] where the ambient gas was the inert Argon and the substrate target material was the Carbon Trimmer C3. The plume injection velocity greatly affects the plume evolution (see Fig. 1a-h). We are performing the CFD parametric study to find the optimal laser furnace regime (light or heavy surrounding gas, gas pressure, and furnace temperature) to achieve uniform temperature profiles of catalyst particles. We are studying the effect of periodicity of plume emerging on the plume dynamics and thermal conditions of the catalyst particles subject to different carbon injection velocity (normalized by free stream sound speed).

fig. 1a

Injection Veloc=0

fig. 1b Injection Veloc=0

fig. 1c

Injection Veloc=15

fig. 1d Injection Veloc=15

fig. 1e

Injection Veloc=0

fig. 1f Injection Veloc=0

fig. 1g

Injection Veloc=15

fig. 1h

Injection Veloc=15

Figure 1. Effect of injection velocity on plume evolution : (a-d) t=10µs, (e-h) t=200µs.

[1] - Greendyke, R., Scott, C. and Swain, J., CFD Simulation of Laser Ablation Carbon Nanotube Production. 8Th AIAA/ASME Joint Thermophysics and Heat Transfer Conference. Paper AIAA 2002-3026, June 24-26, 2002, St. Louis, Missouri, U.S.A., 2002. [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, Vol. 65, 245425, 2002. [3] - Zeldovich, Y.B., Raizer, Y.P., Physics of Shock Waves and HighTemperature 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, 12076, 1993. [5] Sedov, L.I., Similarity and Dimensional Methods in Mechanics, Academics Press, London, 1959. [6] – Jin, S. and Xin, Z., The Relaxation Schemes for Systems of Conservation Laws in Arbitrary Space Dimensions”, Comm. Pure Appl. Math. 48, pp. 235-276, 1995. [7] – Povitsky, A. and Salas, M., Trajectory-based Approach to Jet Mixing and Optimization of the Reactor for Production of Carbon Nanotubes, accepted for publication in AIAA Journal, September 2002. [8] - Lobão, D.C., An Implicit Time Marching Procedure for High Speed Flow, AIAA Paper 93-3315-CP, presented at the 11th AIAA Computational Fluids Dynamics Conference, Orlando, FL, 1993.