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Vacuum 84 (2010) 980–985

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Vacuum
journal homepage: www.elsevier.com/locate/vacuum

Electrons emission from laser induced metallic plasmas


K.A. Bhatti*, M. Khaleeq-ur-Rahman, M.S. Rafique, K.T. Chaudhary, A. Latif
Physics Department, University of Engineering and Technology, Lahore, 54890, Pakistan

a r t i c l e i n f o a b s t r a c t

Article history: Localized behavior of laser induced metallic plasmas has been investigated using Langmuir probe as an
Received 16 April 2009 electrostatic diagnostic tool. A Q-switched Nd:YAG pulsed laser (1064 nm, 12 ns, 1.1 MW) is tightly
Received in revised form focused on metal targets (Cu, Zn, Cd, Ag, Pt and Au) having dimensions 2  2  0.2 cm3 under vacuum
27 October 2009
w103 torr. The varying biasing voltages are applied to Langmuir probe. The electric signals are recorded
Accepted 5 January 2010
on two channel 200 MHz digital storage oscilloscope (UNI T – UTT 2202). A comparison shows strong
dependence of electron parameters (temperature, density, Debye length, plasma frequency and number
Keywords:
of particles in Debye sphere) in plasmas on target materials’ properties (atomic number, surface binding
Nd:YAG laser
Laser induced plasma energy etc.). The maximum values for electron density (8.08502  1017 m3), Debye length (8.07066  10
Langmuir probe
4
m), plasma frequency (5.19627  1010 Hz) are found for silver and copper metals, respectively, where
Electron parameters and vacuum as the electron temperature shows variation in this trend i.e. maximum value (1.36581  106 K) for
cadmium and minimum value is for gold (1.0008  105 K). the maximum value of number of particles in
Debye length at þ15 V (1.47  1026) for Pt and that minimum for Ag (2.1355  107).
Ó 2010 Elsevier Ltd. All rights reserved.

1. Introduction parameters show that the number density of metal species is


separated in the axial direction from those along radial direction.
Laser matter interaction has explored many dimensions on the Temperature of laser induced plasma may be explained by the
basis of laser ablation in fundamental studies and technological expansion of the plasma. Plasma at its inner part has high and low
applications including thin film deposition, production of micro- varying ionization degree which decreases to low values near to
clusters, cutting, drilling, surface treatment, laser patterning, front due to collision process between the plasma constituents
fabrication of micro and nano-electronic devices and magneto [11]. Space-charge affects the photoelectron kinetic energy that
hydrodynamic generators, etc. [1–3]. leads to fast moving electrons. The prompt electrons are energetic
Laser solid interaction leads to the formation of laser induced enough to ionize the ambient gas molecules or atoms [12,13]. In
plasma after a number of energy conversions, provided that energy plasma the ionization degree and energy distribution of ejected
of incident laser exceeds the ablation threshold of the solid. Plasma material (in form of neutral and ionized) depends on metal
ejectants consist of a mixture of atoms, molecules, electrons, ions, species, laser fluence and binding energy of the target molecules
clusters, micron-sized particles, and molten globules [4–6]. Laser [14,15]. It is well established as electron temperature and density
induced plasma is transient in nature whose characteristics depend depends strongly upon laser wave length and distance form the
on laser parameters, target material and ambient conditions, which target surface [16–18].
may vary radically along axial and radial direction [4,7–9] During laser matter interaction, the velocities of atoms and ions
The laser energy transferred to target material through elec- vary as their kinetic energy is independent of mass number and the
trons involves different mechanisms, viz. electron–phonon laser fluence. This indicates that energy absorbed by the electrons is
coupling, multi-photon ionization and cascade ionization, etc. [10]. redistributed within the electron system before thermalization
Thus, it is imperative to study the behavior of electrons when laser with the lattice. The electron ion thermalization is followed by the
radiation falls on target material and ablation of material has formation of a mixture of atomized vapor and liquid nanoparticles
taken place. Plasma parameters may be characterized by behavior through a mechanism phase explosion [19].
of electrons, i.e. electron density, temperature, ionization degree, Although, an intensive experimental and theoretical study has
relative number densities of neutral metal atoms and ions. These already been carried out by many scientists to understand the
nature of plasma, yet it is still far beyond the understanding. For
this purpose different diagnostic techniques are used to reveal it
* Corresponding author. Tel.: þ924299029204, 923006634399 (mobile). viz. Langmuir probe, mass spectroscopy, optical emission spec-
E-mail address: kabhatti@uet.edu.pk (K.A. Bhatti). troscopy, laser absorption spectroscopy, microwave interferometry,

0042-207X/$ – see front matter Ó 2010 Elsevier Ltd. All rights reserved.
doi:10.1016/j.vacuum.2010.01.036
K.A. Bhatti et al. / Vacuum 84 (2010) 980–985 981

Table 1
Probe I–V-characteristics curve.

Biasing Probe current Ip (A)


voltage
Cu Zn Ag Cd Pt Au
(V)
30 4.48E7 4.48E7 2.71E8 1.21E8 – 1.7E7
25 4.74E7 4.58E7 2.27E8 7.84628E9 6.94E7 1.52E7
20 4.96E7 4.48E7 3.17E8 9.88744E9 7.04E7 1.24E7
15 5.22E7 4.6E7 2.27E8 7.84628E9 7.35E7 9.68E8
10 5.03E7 5.65E7 1.47E8 5.96887E9 7.88E7 6.93E12
5 5.03E7 5.67E7 1.26E6 7.66932E6 8.31E7 4.19E8
0 6.65E7 6.4E7 3.56E6 1.00816E5 8.93E7 9.94E7
5 1.03E6 9.2E7 6.55E6 7.66932E6 9.53E7 5.15E7
10 1.06E6 1.1E6 6.55E6 8.84801E6 1.09E6 2.49E6
15 1.08E6 1E6 6.55E6 8.84801E6 1.415E6 3.46E6
20 1.13E6 1.05E6 1.01E5 1.13768E5 1.57E6 4.75E6
25 1.16E6 1.11E6 1.01E5 1.13877E5 1.65E6 5.57E6
30 1.19E6 1.15E6 1.41E5 1.13777E5 –- 7.62E6
Fig. 1. Typical probes I–V characteristics curve [9,22].

laser interferometry, Thomson scattering, laser induced fluores- condition. Under wide range of conditions, the disturbance caused
cence, beam deflectometry, etc. [20,21]. Langmuir probe is one of by the probe is localized. Langmuir probe theory is based on the
the best techniques to study the local behavior of the electrons in assumption that the charge carriers in the space collisionless in the
the low temperature plasmas [21]. The measurements of plasma plasma sheath around the probe that forms a sheath that has
parameters using Langmuir probe as electrical diagnostic have a well-defined boundary and beyond which plasma is undisturbed
foundation on the current voltage (I–V) curve of a metallic elec- by the presence of the probe. Electric field produced by the
trode that is inserted in the plasma. Langmuir probe theory is based difference between the potential of probe and plasma potential is
on the assumption the charge carriers in the space collisionless in limited to the volume inside the boundary of probe sheath [21]. The
the plasma sheath around the probe that is formed sheath a well- probe current depends not only upon plasma parameters but also
defined boundary and beyond which plasma is undisturbed by the on the mechanism of plasma production. In spite of difficulties,
presence of the probe. Electric field produced by the difference Langmuir probe has an advantage on the other techniques that it
between the potential of probe and plasma potential is limited to can make local measurements whereas other diagnostics viz.
the volume inside the boundary of probe sheath [21,22]. The probe spectroscopy or microwaves propagation provides average
current density, probe current, electron temperature and electron measurements over a large volume of plasma. Biasing voltage is
density obey the Maxwellian distribution [9]. This study may be almost negligible as compared to plasma potential thus it is said
extended for further investigation on electrons. that the probe exhibits localized behavior. Fig. 1 shows typical
probe I–V-characteristics curve [9,22]. ‘Vs’ is called space potential
1.1. Langmuir probe theory or plasma potential. The negatively charged particles migrate to
probe due to lesser masses and are collected by probe. For positive
A Langmuir probe is employed to determine plasma parameters probe voltage of the plasma, electrons accelerate towards the probe
like electron temperature, electron density, and plasma potential at and ions are repelled. Thus a sheath formed, around tip of probe, is
constant or time-varying electric potential. Electromagnetic forces very thin, and very small electric field is formed to make the plasma
control dynamical behavior of plasma. The probe is biased for undisturbed. For negative probe potential ions accelerate that
various positive or negative voltages relative to plasma, and the causes the electron current to fall. At ‘Vf’ all the electrons, except
current collected by probe, provides the information about plasma whose flux is equal to the flux of approaching ions, are repelled. For

Fig. 2. (a) Biasing circuit for Langmuir probe; (b) schematic of experimental setup [9,21].
982 K.A. Bhatti et al. / Vacuum 84 (2010) 980–985

Cu -15
Zn -10
1.6x10-5
Ag 9.00E+017 -5
1.4x10-5 Cd +5
Pt 8.00E+017 +10
1.2x10-5 Au +15
7.00E+017

Electron Density (/m )


-5
1.0x10 6.00E+017

3
Probe Current Ip (A)

8.0x10 -6 5.00E+017

4.00E+017
6.0x10-6
3.00E+017
4.0x10-6
2.00E+017
2.0x10-6
1.00E+017
0.0
0.00E+000

-2.0x10-6 -1.00E+017
-30 -20 -10 0 10 20 30 30 40 50 60 70 80
Biasing Voltage (V) Atomic Number

Fig. 3. Probe I–V-characteristics curve. Fig. 5. Electron density vs atomic number for different biasing voltages.

-15 -15
-10 -10
1.6x10 6 6.00E+010
-5 -5
+5 +5
1.4x10 6 +10
+10 5.00E+010
+15 +15
6
1.2x10
Electron Temperature (K)

Plasma frequency (Hz)

4.00E+010
1.0x10 6

8.0x10 5 3.00E+010

5
6.0x10
2.00E+010
4.0x10 5

2.0x10 5 1.00E+010

0.0
0.00E+000
30 40 50 60 70 80
30 40 50 60 70 80
Atomic Number
Atomic Number
Fig. 6. Plasma frequency vs atomic number for different biasing voltages.
Fig. 4. Electron temperature vs atomic number for different biasing voltages.

ohmic) behavior, so Child–Langmuir law is used to calculate plasma


larger negative values, all electrons are repelled and only ion
current.
saturation current, similar to electron saturation region for large
Probe current is given by [9,21,22]:
positive values, reaches. The disparity in the absolute magnitude of
the currents arises due to difference in masses of electrons and ions
Ip ¼ P  AðVÞ3=2 =d2 (1)
that leads to a difference in ion and electron temperatures. This
forms a sheath for colder species and hotter species. Under the where Ip is the probe current; A, area of probe tip in plasma; d,
Maxwellian distribution the probe current density, probe current, diameter of tip; P, pervience; V, biasing voltage.
electron temperature and electron density has been discussed by The plasma parameters can be evaluated as under [9]:
many scientists [9,13,18,19]. As plasma shows nonlinear (non- Electron temperature is given by [9]

Table 2
Electron temperature vs atomic number for different biasing voltages.

Atomic number Biasing voltages (V)

15 10 5 þ5 þ10 þ15


29 736,251.7448 425,651.5464 212,825.7732 135,809.4114 254,892.9887 367,601.7867
30 539,789.1201 953,451.9281 490,635.3149 163,734.8866 219,426.1005 399,430.9235
47 35,263.21432 21,648.04366 57,209.22076 97,457.52145 194,915.0429 292,372.5644
48 24,902.24526 15,990.58829 217,272.8627 217,272.8627 910,536.7123 1.36581E6
78 915,491.2529 950,052.0691 825,777.4303 913,760.1481 596,151.1373 387,272.5513
79 76,536.69601 10,008.78021 18,765.57784 90,363.40193 129,413.5668 142,918.9256
K.A. Bhatti et al. / Vacuum 84 (2010) 980–985 983

Table 3
Electron density vs atomic number for different biasing voltages.

Atomic number Biasing voltages (V)

15 10 5 þ5 þ10 þ15


29 8.8339E15 6.64684E15 9.26585E15 1.60396E16 1.38554E16 1.02694E16
30 1.92253E17 2.45372E17 1.50939E17 1.15645E17 8.17734E16 6.67677E16
47 6.47879E17 8.08502E17 2.19336E17 2.19336E17 1.07143E17 8.7482E16
48 9.46475E15 9.291E15 9.96563E15 9.47371E15 1.17289E16 1.45522E16
78 3.64365E16 1.00758E17 7.35851E16 3.35332E16 2.80208E16 2.66641E16
79 8.8339E15 6.64684E15 9.26585E15 1.60396E16 1.38554E16 1.02694E16

Table 4
Frequency vs atomic number for different biasing voltages.

Atomic number Biasing voltages (V)

15 10 5 þ5 þ10 þ15


29 5.4316E9 4.7115E9 5.56281E9 7.31895E9 6.80239E9 5.8563E9
30 2.53389E10 2.86262E10 2.24519E10 1.96524E10 1.65256E10 1.49326E10
47 4.65156E10 5.19627E10 2.70649E10 2.70649E10 1.89162E10 1.70927E10
48 5.6222E9 5.57035E9 5.76904E9 5.62486E9 6.25865E9 6.97133E9
78 1.10311E10 1.83439E10 1.56764E10 1.05825E10 9.67369E9 9.43658E9
79 5.4316E9 4.7115E9 5.56281E9 7.31895E9 6.80239E9 5.8563E9

h i1=2
  lD ¼ 30 kTe =e2 ne (5)
Te ¼ ½eVa =kT=ln Ip =I0 (2)

where Te is electron temperature; e, charge on electron; Va, applied where lD is the Debye length [9,21].
voltage; k, is Boltzmann constant; Ip, probe current. 3
The electron density is given by the following relation [21]: ND ¼ ne 4=3plD (6)
The present paper reports an investigation plasma electron
ne ¼ I0 =Ae½me =230 kTe  (3)
behavior emitted from different metal targets (Cu, Zn, Cd, Ag, Pt &
where ‘ne’ is the electron density; A, area of the probe; me, mass of Au) irradiated by Nd:YAG laser using self fabricated Langmuir probe
electron; 3o, permittivity of free space; and Te, the electron as electrostatic diagnostic to study the local behavior of electrons at
temperature. a distance 1 mm from target surface.
Plasma frequency is given by [9]:
2. Experimental setup
h i1=2
up ¼ ne e2 =30 me (4)
4 N pure transition metal targets (Cu, Zn, Cd, Ag, Pt & Au) are
where up is the plasma frequency. irradiated by Nd:YAG laser (1064 nm, 10 mJ, 1.1 MW) in eight ports
The Debys length is given by the following equation [21]: stainless steel vacuum chamber under vacuum w103 torr. Laser
(of spot size and power density at the focus are 12 mm and
3  1015 W/m2, respectively) is tightly focused at an angle 45 on
target materials by using IR Plano convex lens of focal length 10 cm
to produce plasma. The self fabricated Langmuir probe made up of
-15
copper and tungsten was used. The time resolved voltage signals
-10
9.0x10 -4 -5 -15V
+5 1.70E+026 -10V
8.0x10 -4 +10 1.60E+026 -5V
+15 1.50E+026 +5V
-4
7.0x10 1.40E+026 +10V
No. of particles in Debye's length

1.30E+026 +15V
-4
6.0x10 1.20E+026
Debye's length (m)

1.10E+026
5.0x10 -4 1.00E+026
9.00E+025
4.0x10 -4 8.00E+025
7.00E+025
3.0x10 -4 6.00E+025
5.00E+025
2.0x10 -4 4.00E+025
3.00E+025
1.0x10 -4 2.00E+025
1.00E+025
0.0 0.00E+000
-1.00E+025
-1.0x10-4 30 40 50 60 70 80
30 40 50 60 70 80 Atomic Number
Atomic Number
Fig. 8. Number of particles in Debye length vs atomic number for different biasing
Fig. 7. Debye length vs atomic number for different biasing voltages. voltages.
984 K.A. Bhatti et al. / Vacuum 84 (2010) 980–985

Table 5
Debye length vs atomic number for different biasing voltages.

Atomic number Biasing voltages (V)

15 10 5 þ5 þ10 þ15


29 5.26748E4 8.07066E4 4.90348E4 2.15298E4 2.68164E4 4.20258E4
30 2.88597E5 2.00154E5 4.14858E5 6.18602E5 1.04036E4 1.41011E4
47 1.32111E5 9.47674E6 6.70679E5 6.70679E5 1.96442E4 2.66258E4
48 6.62735E4 6.81412E4 6.13404E4 6.61795E4 4.80415E4 3.47626E4
78 9.76639E5 2.12382E5 3.40293E5 1.10618E4 1.44816E4 1.56009E4
79 5.26748E4 8.07066E4 4.90348E4 2.15298E4 2.68164E4 4.20258E4

were stored on 200 MHz (UNI T UTT 2202) digital storage oscillo- higher ionization energy and has small number of electron in
scope. The biasing circuit and schematic of experimental setup of plasma plume as compared to Cd and Ag. Although, the Cu metal
Langmuir probe is shown Fig. 2(a, b). has small ionization energy yet it has 3d10, 4s1 electronic configu-
ration, it has smaller number of electrons for conduction as
3. Results and discussion compared to Cd and Ag. Pt and Au have little higher ionization
energy as compared to Cd and Ag but large surface binding energy
Characteristics of the laser induced plasma strongly depend on [33]. The large probe current of Au may also due to having electric
irradiation conditions and emitted electrons [2,9,21]. Plasma configuration 5d10, 6s1. So, it can lose electrons more easily than Pt
expansion obeys fluid dynamics and forward-peaking phenomena which has configuration 5d9, 6s1. This shows metals with inter-
[23]. mediate atomic number (Cd, Ag) and possessing less surface
The plasma produced, in the region of electron emission beam binding energy have more electrons than metals with smaller (as
relaxation is subsonic in ambient gas at higher pressure, whereas in Cu, Zn) and larger (as Pt, Au) atomic number. The floating potential
vacuum, it behaves like supersonic due to the absence of collisions is negative for all the targets. In general the over all trend of all the
between plasma ejectants and ambient gas molecules. The hydro- curves is sigmoid.
dynamic propagation of ionization is due to production of elastic According to Eq. (2) electron temperature depends on the probe
waves in vacuum [4,24–28]. current. Fig. 4 illustrates the electron temperature verses atomic
Different plasma parameters may be calculated by varying number (z) of target metals for various applied voltages corre-
electrical biasing [29–31]. sponding to values given in Table 2 by using relation (2). Curves in
Child’s Langmuir law is used for calculation of nonlinear probe Fig. 4 show that electron temperature is higher for metals having
current (Eq. (1)). Probe current for metal targets (Cu, Zn, Cd, Ag and large surface binding energies and also has large temperature
Au) has been calculated for different biasing voltages by using values for negative applied potential. This is because only higher
relation (1) are given in Table 1. energetic electrons are able to reach probe [33]. It is obtained form
Generally, probe potential decreases with the decrease in the figure that for metals having low value of surface binding
biasing potential [9]. This could be due to the reduction in positive energy the electron temperature is less and almost same for all
sheath of ions as more electrons reach the probe tip, thus biasing voltages. Only cadmium metal has large value of electron
neutralizing the ions. The electronic peak increases because new temperature at þ15 V biasing voltage.
primary electrons are further produce electrons. Thus multiplica- The electron temperature for metals Cd, Ag and Au rises with
tion of electrons occurs. An increase in the biasing potential causes increase in biasing voltage form 5 V to þ15 V, while for metals Cu, Zn
an increase in the number of electrons collected by the probe tip and Pt there is a fall in electron temperature with increase in biasing
[21,30]. voltage. The metals having small value of surface binding energy is
Fig. 3 shows a comparison of I–V-curves for all target metals higher as compared to metals with larger surface binding energy [33].
corresponding to data given in Table 1. All the I–V-curves for metals Figs. 5 and 6 show the curves of electron density and plasma
have some trend with floating potential in the same region. The frequency respectively corresponding to values given in Tables 3
probe electronic current is maximum for Cd metal followed by that and 4, respectively for different biasing voltages. The values of
of silver and gold metals. Whereas the probe current for metals Cu, electron density and temperature have been evaluated by using
Zn and Pt is small and lay in same region. This higher electronic relations (3) and (4), respectively. Curves in both graphs show
probe current for metals Cd, Ag and Au is due to small surface monotonically decreasing and then increasing trend, the metals
binding energy in comparison with metals Cu, Zn and Pt [17,32,33]. with large value of temperature have small values of electron
The values of floating potential are positive which is in agreement density and plasma frequency in particular region and metals with
with the theoretical prediction of positive floating potential [32,33]. small values of electron temperature have high density which is in
The curves from 10 V to þ30 V shows the probe electronic agreement with previous result [9]. Eq. (3) shows that electron
current. There is a little variation in the values of probe current for density is inversely proportional to the square root of electron
applied voltage for all the target metals. Also other metal like Zn has temperature [31–35].

Table 6
Number of particles in Debye length vs atomic number for different biasing voltages.

Atomic number Biasing voltages (V)

15 10 5 þ5 þ10 þ15


29 998,254.2659 2.27091E6 6.4231E6 1.26004E7 4.90054E6 1.30564E13
30 1.53039E6 651914.7494 1.76604E6 9.16067E6 5.90482E6 2.40423E6
47 5.09831E8 1.05994E9 2.46723E8 1.10965E8 3.9232E7 2.13552E7
48 2.43293E9 4.72815E9 9.44016E7 9.44016E7 1.10038E7 5.98969E6
78 1.3807E25 1.24693E25 1.83347E25 1.3879E25 4.49177E25 1.47096E26
79 4.45185E7 9.41399E8 3.66693E8 2.02477E7 1.74466E7
K.A. Bhatti et al. / Vacuum 84 (2010) 980–985 985

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