Title:
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Pulsed laser ablation and laser-induced plasma diagnosis by optical emission spectroscopy
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Fundamental aspects of the laser ablation of solid targets using nanosecond pulses with
irradiances in the range ≈ 1-30 OW /cm2 have been investigated theoretically, modelled
using a simulation code, and explored experimentally by time-gated, spatially and
spectrally resolved imaging of the optical emission that accompanies the ablation plume.
During the earliest stages of the laser-target interaction, the target surface temperature
rises rapidly and electrons are ejected by both thermionic and photo-emission. These
electrons absorb energy from the · laser pulse by strong electron-photon coupling,
leading to formation of an embryonic plasma which continues to gain energy via
photoionization and, particularly, inverse bremsstrahlung (IB) absorption. The target is
further heated by the hot plasma and may reach temperatures of several thousand Kelvin,
approaching its critical point, and undergo an explosive phase transition to the
supercritical fluid. Such a super-hot target surface emits an abundance of electrons,
neutrals and ions.
The present work shows that the electron yield following 532 nm PLA of a Si target is
significantly higher than that produced using 1064 nm pulses of same irradiance. The
fastest electrons emerge at the leading edge of the plasma plume, creating an electric
field gradient with respect to the net positively charged body of the plume. This has the
effect of accelerating ions in the plume, to extents that ·depend on their charge state.
Emissions from any given charge state show identical spatial distributions in the time-gated
images. The most highly charged ions (e.g. SiIV ions in the case of PLA of Si in
vacuum) exhibit velocities of ~ 1 00 km/s. Experiment and simulation show that plasma
produced by 1064 nm excitation is hotter and expands faster than that formed by 532
nm PLA - a result that can be attributed to the stronger IB absorption of the longer
wavelength radiation.
A new and improved method for determining local electron densities (Ne) and
temperatures (Te) in laser induced plasmas is introduced. The model relies on fitting
Stark broadened line shapes but, in contrast to most rival approaches, makes no preassumption
regarding local thermodynamic equilibrium. The method is used to
determine temporally and spatially evolving Ne and Te distributions in plumes arising
from PLA of Si and SiC targets, as functions of irradiance, excitation wavelength and
ambient pressure. We also demonstrate how Ne and Te values determined by fitting lines
associated with one spectral carrier allow derivation of (hitherto unknown) Stark
parameters for transitions involving other carriers. A clear shock front is observed
following PLA of Si in background Ar pressures ~0.2 Torr, even as early as 40 ns.
Strong collisions between highly charged ions in the plume and the surround gas are
seen to introduce another level of complexity (e.g. ionization, recombination, charge
transfer, etc.) within and beyond the shock front in the plume.
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