Demonstration of the snow-plow effect in laser-produced plasma

expansion in background gas using SPARTA

Rommil B. Emperado,1* Lean L. Dasallas,2 and Wilson O. Garcia1

1
National Instititute of Physics, University of the Philippines Diliman, Quezon City 1101
2
Materials Science and Engineering Program, University of the Philippines Diliman, Quezon City 1101
*
Corresponding author: remperado@nip.upd.edu.ph

Abstract
Here we demonstrate the snow-plow effect, which is the splitting of a laser-produced plasma into fast-
and slow-moving components as it expands in background gas. We modelled the expansion in two
dimensions using the direct simulation Monte Carlo method implemented via the open-source software
SPARTA. Density and kinetic energy maps confirmed the splitting of a copper plume as it expands
in argon gas. The effect of gas pressure on the plume expansion and splitting was also discussed.
Moreover, the energy exchange between the plume and background gas was further demonstrated
based on energy distributions.
Keywords: laser-produced plasma, plume-splitting, pulsed laser deposition, direct simulation Monte
Carlo method

1 Introduction
Pulsed laser deposition of thin films often requires a background gas environment to improve the prop-
erties of the deposited film. For instance, species ablated from a target using a high laser fluence have
large kinetic energies which lead to resputtering and subsequent defects on the deposited film [1]. The
background gas then acts as a buffer to lower the kinetic energy of the incoming particles [2, 3]. The
deposition gas also influences the angular distribution of ablated species within the plasma plume [4, 5].
Moreover, the background gas may also be used to supply additional atoms and improve the stoichiometry
of resulting films [4, 6].
Another effect of the background gas on the plasma plume expansion is the spatial splitting of the
plume into fast- and slow-moving components [7–9]. The origin of the splitting phenomenon is still an
open question [9] and one of the proposed theories include the ambipolar electric field generated by the
separation of electrons and ions within the plume [10]. Meanwhile, Volkov et al. recently demonstrated
using direct simulation Monte Carlo (DSMC) method [11] that the bimodal distribution of species may
not be caused by the ambipolar field, and the splitting could exist even in neutral plumes [9]. They
proposed the so-called snow-plow effect, which includes a shockwave that sweeps the background gas like
a plow. The hydrodynamic and kinetic modelling of the plume qualitatively agrees with experimental
demonstrations of plume-splitting [7, 9, 12].
We have previously performed similar DSMC simulations of laser-produced plasma expansion [13]
and demonstrated the flip-over effect [5] using the open-source software SPARTA (Stochastic PArallel
Rarefied-gas Time-accurate Analyzer [14]). SPARTA can be used to model plume expansion by intro-
ducing particles into the simulation space with a shifted Maxwellian velocity distribution. The code also
allows for time-resolved diagnostics of quantities such as plume density and gas kinetic energies. Thus,
we aim to simulate plume expansion in background gas and demonstrate the snow-plow effect in the
context of density and kinetic energy diagnostics in SPARTA.

2 Plasma plume expansion model

We modelled the 2D laser plume expansion in SPARTA using a 35 mm by 20 mm simulation space with
a grid size of 1 × 10−4 m, time step of 100 ps, and periodic boundary conditions. The periodic boundaries
ensure that the number of background gas particles and the pressure remain constant. To simulate laser
ablation from a monoatomic target, we setup a rectangular surface in SPARTA with a 1 mm-wide region
that introduces particles into the simulation space. Copper particles were used as the ablated species
with a shifted Maxwellian velocity distribution as it enters the simulation. The initial copper plume is
at 1000 K and a flow speed of 2500 m/s to match the expansion velocity of the plume recently modelled
by Volkov [9]. The initial plume density was 1 × 1018 cm−1 with a real-to-simulated particle number
ratio of 3.75 × 1011 . For every time step, around 1.33 × 104 particles enter the simulation space. The

Proceedings of the Samahang Pisika ng Pilipinas

40th Samahang Pisika ng Pilipinas Physics Conference
19–21 October 2022
SPP-2022-2C-02-1
Figure 1: Density maps of Cu plume during expansion in (a,b) vacuum and in Ar background gas at different
pressures: (c,d) 3 Pa; (e,f) 30 Pa; and (g,h) 100 Pa. Snapshots were taken at 3 µs and 5µs, respectively. The low
density maps at 5µs were multiplied by 1.5 to improve visibility.

plume expands in an argon background gas with a Maxwellian velocity distribution at 300 K. The plume
expansion was studied for different background gas pressures by setting the density of Ar particles in
SPARTA.
In DSMC modelling, the particles interact stochastically and the collision pairs per grid cell are chosen
with a probability distribution that depends on the collision cross-section using G. A. Bird’s No Time
Counter algorithm [11]. The particles then collide according to the variable hard sphere model and the
collision parameters were obtained from Ref. [15]. The resulting density and kinetic energy distribution
across the simulation grid was then obtained at different times to visualize the plume-gas interaction.
The per-particle kinetic energy was also obtained to monitor the energy distribution of the plume and
background gas particles during plume expansion.

3 Results and Discussion

Figure 1 compares the density maps of the copper plume as it expands in vacuum and in argon background
gas at different pressures. When the plume expands in vacuum, the plume core remains intact and the
density decreases (Fig. 1a,b). Meanwhile, interaction with the background gas causes the formation of
a mixing layer at the plume front (Fig. 1c). The interaction of the plume front with the background
gas slows down the copper particles in this region while the rest of the plume still carries the same flow
velocity. As the plume expands, the shape of the mixing layer becomes more defined and a gas cloud
forms behind the plume front (Fig. 1d), which demonstrates the snow-plow effect [9] in the plume. As the

Figure 2: Kinetic energy maps of Cu plume during expansion in (a) vacuum and in Ar background gas at different
pressures: (b) 3 Pa; (c) 30 Pa; and (d) 100 Pa. Snapshots were taken at 5µs. The low kinetic energy maps for 30
Pa and 100 Pa were multiplied by 2 and 4, respectively to improve visibility.

Proceedings of the Samahang Pisika ng Pilipinas

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Figure 3: Energy distribution of Cu particles at different times during plume expansion in (a) vacuum and in Ar
background gas at different pressures: (b) 3 Pa; (c) 30 Pa; and (d) 100 Pa.

gas pressure increases, the mixing layer becomes more prominent, the plume is more spatially confined,
and the plume propagation seems to be slowed down by the background gas, which is consistent with
experimental observations [1, 2, 7].
The energy loss and slowing down of the plume particles due to their interaction with the background
gas is further demonstrated by the corresponding kinetic energy maps for the copper plume as shown
in Fig. 2. For the copper plume in vacuum, the kinetic energy distribution appears smooth with the
plume front having the highest energy owing to minimal collisions with other copper particles. Upon
background gas interaction, the high-energy particles in front of the plume may not be colliding with the
background gas as the collision probability depends on the speed of colliding particles [11]. Meanwhile,
a local kinetic energy minimum forms within the mixing layer. This minimum is slightly visible in 3 Pa
argon gas (approximately at x = 7 mm) and becomes more prominent at higher pressures (5 mm at 30
Pa and 3 mm at 100 Pa). This observation agrees with the recent results of Volkov et al. about how the
local minima in kinetic energy near the plume front corresponds to maxima in vapor density [12].
We also extracted the energy distribution of copper (Fig. 3) and argon particles (Fig. 4) to get insights
about the energy exchange between the plume and the background gas. As shown in Fig. 3a, copper
vapor expansion in vacuum does not affect the peak position while the width of the distribution slightly
increases due to interparticle collisions. At 3 Pa, the energy loss of the plume is apparent as the energy
peak consistently shifts to lower values. The energy decreases further as the background gas pressure
increases. Interestingly, not only does the peak position shifts, but the height of the low-energy tail of
the distribution also increases. This could be due to the interaction of the low-energy copper particles
with the background gas.
Figure 4 shows the energy distribution of argon atoms. The curves are sharp and peaks at around
0.013 eV (corresponding to 300 K). The y-axes were split to better emphasize the low- and high-energy
features of the curves. At 3 Pa, local maxima appear at positions corresponding to the peak positions of
copper vapor expanding at the same pressure (Fig. 3b). At 30 Pa and 100 Pa, the maxima are no longer
significant, and the distribution slightly narrows from 30 to 100 Pa. This could indicate that the plume
minimally affects the overall energy of background gas at high pressures.

4 Conclusions
We have demonstrated the snow-plow effect in a monoatomic plume expanding in background gas of
varying pressures using DSMC simulations in SPARTA. The mixing layer near the plume front was

Figure 4: Energy distribution of Ar particles at various times and pressures: (a) 3 Pa; (b) 30 Pa; and (c) 100 Pa.

Proceedings of the Samahang Pisika ng Pilipinas

40th Samahang Pisika ng Pilipinas Physics Conference
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SPP-2022-2C-02-3
observed from the density maps and the kinetic energy minima in this region was confirmed at varying
pressures. Aside from using grid data in SPARTA to extract 2D quantity maps, we also obtained particle
data and compared the energy distribution of interaction copper and argon atoms during plume expansion.
While the periodic boundaries have kept the pressure constant during simulations, the results could be
further improved by considering a wider padding around the simulation space to avoid unwanted particle
trajectories which could affect the simulation. Smaller grid sizes can also be used to ensure accuracy
of the collision calculations. The grid sizes and padding width in this study is currently limited by the
computational time. Moreover, 3D simulations could be employed in future research to account for the
anisotropy in the third dimension of the simulation space.
Our simulations support the hypothesis that the plume-splitting phenomenon is more likely caused
by the hydrodynamic snow-plow effect than the ambipolar field due to charge separation of electrons and
ions. Moreover, this study paves the way for more substantial and informative modelling of laser-produced
plasma expansion in background gas, such as simulating off-axis film deposition or multielemental plume
expansion to predict the angular distribution of ablated species.

Acknowledgments
L.D. acknowledges the Office of the Chancellor of the University of the Philippines Diliman, through
the Office of the Vice Chancellor for Research and Development, for funding support through the Ph.D.
Incentive Award.

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Proceedings of the Samahang Pisika ng Pilipinas

40th Samahang Pisika ng Pilipinas Physics Conference
19–21 October 2022
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