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Thermal equilibrium in gas-discharge

plasma of low pressure mercury lamp

Gorbunkov, V., Solomonov, V.

V. I. Gorbunkov, V. I. Solomonov, "Thermal equilibrium in gas-discharge

plasma of low pressure mercury lamp," Proc. SPIE 9810, International
Conference on Atomic and Molecular Pulsed Lasers XII, 98101L (15
December 2015); doi: 10.1117/12.2225188

Event: XII International Conference on Atomic and Molecular Pulsed Lasers,

2015, Tomsk, Russian Federation

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 Thermal equilibrium in gas-discharge plasma of low pressure mercury
lamp
VI Gorbunkov1, VI Solomonov2
1
Omsk State Technical University, vigorbunkov@list.ru
2
Institute of Electrophysics of the Ural Branch of the Russian Academy of Sciences, Russia,
Ekaterinburg, plasma@iep.uran.ru

Abstract

A study was conducted emission spectra germicidal low pressure mercury lamp at currents 100-306 mA located in a
closed opaque cavity. It is shown that the lamps located in the cavity with perfectly reflecting and absorbing internal
surfaces, in the emission resonance line of mercury is dominant at λr = 253.65 nm. The same pattern is observed in the
tube placed in a cavity with diffusely reflecting surface at a low current of about 100 mA. However the picture of
spectrum changes at higher discharge current. The spectrum of the lamp with arc discharge at a current of 306 mA
contains the maxima of the spectral lines. Its intensities are approximately described by Planck's radiation law at the
temperature of 9270 ± 230 K. The mechanisms of establish thermal equilibrium are discussed.

Keywords: gas-discharge plasma emission spectrum, Planck emitter of the discrete spectrum, the mechanism of thermal
equilibrium

1. Introduction

The study of electrical discharges in a mixture of mercury vapor and inert gases of low pressure had beginning
in the XIX century. As a results of these studies are a set of powerful light sources in the form of fluorescent lamps of
visible light, and ultraviolet germicidal radiation. Structurally, they are glass or quartz tube filled with a buffer gas -
argon pressure 100-5000 Pa at a mercury vapor pressure of 1-100 Pa 1-3. Power lamps are AC and DC. The fluorescent
lamps of low pressure mercury vapor (less than 10 Pa) use glow discharge. The germicidal lamps at the same pressure
use abnormal glow or arc discharge. The nonequilibrium low-temperature plasma with an electron density ne <1013 cm-1
is generated in these discharges regardless of the supply voltage 2,4. Only kinetic velocities of the particles submit
satisfactorily to the Maxwell distribution, but with very different temperatures: electrons temperature is Te = 7500 ÷ 16
000 K, atoms temperature is Tg <1000 K 1,4. A good sign of a spectral nonequilibrium plasma is the domination at the
emission spectrum of the resonance line of mercury atom at λr = 253.65 nm. It concentrates to 80% of the radiated
energy in the range of the emission spectrum from 200 to 600 nm 1-4. The radiation at this line at λr = 253.65 nm is used
directly at the bactericidal lamps widely used in medicine for ultraviolet radiation 2. Below we will call these lamps as
outdoor lamps.
Mercury germicidal lamps are widely used in extracorporeal photohemotherapy 5-7. In that case the lamp is
placed in a cavity of the metal opaque to protect workers from the harmful effects of ultraviolet radiation from. The lamp
light outputs through the aperture - small radius hole at the center of the cavity. Below we will call these lamps as closed
lamps. In 8,9 it was found that the spectrum of the radiation emerging from the opening of the closed bactericidal mercury
lamp (aluminum cavity) was significantly different from the emission spectrum of outdoor lamps. Namely, the resonance
line of mercury atom at λr = 253.65 nm lose its dominant role in the range of 200-600 nm. The contours of the spectral

International Conference on Atomic and Molecular Pulsed Lasers XII, edited by Victor F. Tarasenko,
Andrey M. Kabanov, Proc. of SPIE Vol. 9810, 98101L · © 2015 SPIE
CCC code: 0277-786X/15/$18 · doi: 10.1117/12.2225188

Proc. of SPIE Vol. 9810 98101L-1

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 lines were strongly distorted by self-absorption and emission lines appear molecule Hg2. The intensities of the discrete
emission lines of excited mercury atoms are distributed of the Planck law at about Tp = 9200 K. These signs indicate that
thermal equilibrium is achieved in the arc plasma of the closed lamps. However, the physical meaning of the temperature
distribution is not quite clear. Firstly, it is much larger gas temperature which may not exceed the Tg = 700 K for the
power supply (20 W) used in 9. Secondly, the value Tp is less the electron temperature Te = 11 600 K measured in 3,10,11
probe method in the plasma of open fluorescent lamps with similar germicidal lamp parameters discharge and the
equivalent inner diameter Din = 14 mm flasks.
At this article the attention is paid to the dynamics establish thermal equilibrium plasma germicidal mercury low
pressure lamps placed in an aluminum closed cavity with different reflective properties of its inner surface, at different
currents supply. The studies were conducted by the spectral method.

2. EXPERIMENTAL

We studied the emission spectrum germicidal low pressure mercury lamp type DRB 8 TU16-535.659-77 placed
inside a cylindrical cavity (Figure 1).
The cavity 2 is an aluminum cylinder with a diameter of 8.4 cm long 50 cm, closed by the both ends. We used three
cavities: with light-absorbing (covered with soot), a reflective mirror (polished) and diffuse reflective inner surface.

Figure1. Schematic design of the radiator

The aperture 4 with diameter of 0.9 cm was cut in the middle of the cylinder opposite the middle of the discharge lamp.
It is used to display and record the radiation outside the emission spectrum of the plasma 8. Hole 3 was used to set the
cell for the irradiation of the liquid. Flask germicidal mercury lamp 1 is a quartz tube with a wall thickness of 1 mm, a
diameter of 16 mm and a length of 280 mm. The interelectrode distance is 235 mm. The tube is filled with argon buffer
gas at a pressure of 400 ÷ 800 Pa. Mercury vapor pressure at operating temperature wall lamp 322 ÷ 350 K was 0,8 ÷ 0,9
Pa. The design of the lamp emitter provides a secure fit coaxial lamp position in the cavity.
We used the standard throttle system AC power; lamp current varied between (0,100 ÷ 0,306) ± 0,003A by
changing the external voltage from 180 to 220 V using an autotransformer. Thus the voltage drop across the lamp was
varied from 50 to 42 V. In some cases the lamp current was reduced to 90 mA. Registration spectrum in the range of
200-600 nm was carried out using a spectrograph ISP-30 equipped with a semiconductor type SKCCD multichannel
analyzer with spectral resolution better than 0.05 nm, as well as multi-channel fiber-optic spectrometer «AvaSpec - ULS
204L-5-RM» with a spectral resolution of up to 0.15 nm. The dynamic range of the measurement line intensity was
1.6×106.

3. RESULTS AND DISCUSSION

Studies have shown that the emission spectrum of the lamp depends on the quality of the inner surface of the cavity. If
the lamp is placed in the cavity with the light-absorbing and mirror reflective inner surface, that the resonance line of
mercury atom at λr = 253.65 nm (fig. 2) with a noticeable reabsorption (fig. 3) dominates at the emission spectrum
regardless of the current value which determines the type of discharge.

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 lu¿suzi¿

Figure 2. The emission spectrum of a mercury lamp placed in the cavity with light-absorbing wall in Il = current of 312 mA. For
clarity, the intensity of the resonance line of mercury atom 253.65 nm reduced by 10 times

Figure 3. The contour of the resonance line of mercury atoms at λ = 253.65 nm lamps in the cavity with light-absorbing inner surface.
Vertical line denotes the physical center of the Doppler contour width ΔλD≈0.22 nm (dashed line)

A different pattern is observed in the tube placed in a cavity with diffusely reflecting internal surface. Thus, the
resonance line of the mercury atom at λr = 253.65 nm dominate in emission spectrum of the lamp in a glow discharge at
a current of about 100 mA - minimum currents of the discharge only. With the increase of the discharge current
additional atomic mercury lines appear in the spectrum while the dominant role of the resonance line maintains.
However, under abnormal glow discharge at a current of 194 mA (fig. 4) the intensities of other atomic lines become
comparable with the intensity of the resonance line and at arc discharge (Il = 306 mA) the envelope of intensities of the
all atomic mercury lines is well described by the Planck curve, and the lines of the molecule of mercury Hg2 appear at
spectrum (fig. 4b).

Intensity, rel. units

100o 1000

a) 6)
750 750

500 500

250 25

0 II
253.7 296.7 365.0
I I
404.7 435.8
I
546.1 579.0
0
I
253.7 296.7 312.6 365.0 404.7 435.8 A, nm

Figure 4. The emission spectra of the lamp: a - abnormally glow discharge Il = 194 mA; in - arc at Il = 306 mA, it shows the line of
mercury molecules stroke, and the red line - the Planck curve at Tp = 9270 K

The dominant of the resonance mercury atom line in lamps placed in the cavity with the light-absorbing and mirror
reflective inner surfaces almost certainly indicates that the electric discharge plasma of these lamps is a non-equilibrium,

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 of course. This conclusion can apply to the glow discharge plasma of the lamps placed in a cavity with diffusely
reflecting internal surface with currents of about 100 mA, also. However, this conclusion can not apply to the abnormally
glow discharge plasma of this lamp already. At this discharge the intensities of all mercury atom lines in emission
spectrum are comparable (fig. 4). Moreover, the circuits of all lines are subject to absorption (fig. 5).

6,000
SKI

Figure 5. The contours of emission lines at λ = 546,07 nm: a - abnormally glow discharge Il = 100 mA, b - arc at Il = 276 mA

We analyze the behavior of the spectral emission lines intensities of the abnormally glow discharge plasma. Measured
intensity of the lines emitted on the optical transition from level k to level i writes as 12

J ki =
I ki
k ik
(
1 − e − k ik ⋅ d ) d4 Ωπ . (1)

Where d - the effective thickness of the plasma column; dΩ - the solid angle of observation; 4π - full solid angle of
radiation; Iki=NkAkihνki - the physical intensity of the spectral line at the frequency of the transition νki; Nk - population of
the upper emission level; h - Planck constant; Aki= ∫ a(ν) dν ≈ aki0 Δν - Einstein coefficient for spontaneous emission (the
integration is carried out along the contour lines); a(ν) and aki0 - spontaneous emission probability density inside the
contour line and the center thereof, respectively; Δν - circuit line width at half maximum; kik - the absorption coefficient
on the transition i→k, equal to

λ 2ki g ⎛ giN k ⎞
k ik = a k
N i ⎜⎜ 1 − ⎟⎟
ki 0
4 g gkN i ; (2)
i ⎝ ⎠
gi and gk - statistical weights of the levels i and k, Ni - population of the lower level of the optical transition.
Furthermore, it should be noted that the output aperture lying in the middle of the cavity, because emergent
from it rays are directly emitted portion located beneath the plasma and reflected from the inner surface of the cavity
which passed through the absorbent plasma extra. Such rays are absent in the cavity with a light-absorbing surface. Their
contribution can be neglected for a cavity with a mirror reflective surface. However, in the case of diffuse reflection from
the inner surface of the cavity the Lambert's law has a place with a reflection coefficient r. Measured intensity
substantially represents the superposition of the multiple reflection and passing through the plasma beam. Accordingly,
the expression (1) for measured intensity of spectral line from the lamp located in a cavity with diffusely reflecting
internal surface, is converted to
I ki 1 − e − k ik d θ d Ω
J =
k ik 1 − re − k ik d θ 4 π ,
ki (3)

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 where r - the diffuse reflection of the inner surface of the cavity, d0 = 4 d / π, π / 4 - the average cosine of the angle of the
diffuse reflection.
Using the expression (3) for the analysis of the plasma lamp located in the diffusely reflecting cavity. The
abnormally glow discharge (Il = 194 mA) is heated lamp bulb to a temperature 44°C that corresponds to the
concentration of mercury atoms NHg ≈ N0 ×2.8×1014 cm-3. The arc discharge (Il = 306 mA) rises bulb temperature to
50°C, which leads to a slight increase in the concentration of mercury atoms to N0 ≈ 3.4×1014cm-3. Evaluation of the
absorption coefficient (2) on the optical transition 63S0 → 63P1, corresponding to the resonance line at λr = 253.65 nm, at
these concentrations of mercury atoms gives a value of kr ≈ 0.8 and 1.0 cm-1 for the anomalous glow and arc discharge,
respectively. Pictures arc discharges removed through the aperture of the cavity using a blue filter shown that the
diameter of the positive column varies from 3 to 10 mm at discharge currents 194 and 306 mA, respectively. This
suggests that optical density of the plasma on the resonance transition (for abnormally glow discharge kik dθ ≈ 0.3 and arc
discharge kik dθ ≈ 1.2) is although quite high, but is not enough to neglect the exponential terms in (3).
It is easy to show that when the population of the levels of mercury atoms obey to Boltzmann low
gk N m ⎛ E − Ek ⎞
= exp⎜⎜ − m ⎟
gm N k ⎝ k BT ⎟⎠

equation (3) becomes

1 − e − k ik d θ d Ω
J = ρν ⋅ c ⋅ Δν
1 − re − k ik d θ 2
ki ki
, (4)

hν −1
ν 3 ⎛⎜ ⎞
ρν = 4h e k BT
− 1⎟
where c 3 ⎜⎝ ⎟
⎠
- the spectral density of the Planck distribution , Δνki - spectral line width.

Equation (4) shows that the diffuse reflectance of the inner surface of the cavity, close to unity, the curve, the
envelope peaks intensities of the spectral lines should be close in shape to the Planck curve. However, the emission
spectrum of the abnormally glow discharge plasma at Il = 194 mA (fig. 4) indicates that a distribution of intensities of the
spectral lines is significantly different from the Planck curve. This is due to the fact that in such a plasma population of
the energy levels of atoms of mercury are not subject to the Boltzmann law.
To establish the Boltzmann distribution of the populations of excited levels due to inelastic collisions with
electrons is necessary to the characteristic time of the collision τeHg≈ [neσeHgVe]-1 was less effective decay time of the
excited levels by other mechanisms. There σeHg≈10-16 cm2 - the cross section of inelastic collisions of electrons with
atoms of mercury, Ve ≈ 108 cm / s - the average velocity of the electrons, ne ≤ 2×1012 cm 3 - concentration of electrons in
a plasma arc at a current 306 mA and fall voltage 42.5 V. A decay of excited states of atoms in Ar-Hg low-pressure
plasma is carried out mainly in the emitting processes 4 with the characteristic times τr = (Aul) -1 ≈10-8 c 13. This size is
considerably smaller than the characteristic time τeHg ≥3×10-5 c when ne ≤ 2×1012 cm-3. Therefore, Boltzmann distribution
of the populations of the excited levels of the mercury atom is not installed in the arc plasma of open low-pressure
mercury lamp. The same applies to lamps placed in the cavity with the light-absorbing and mirror reflective inner
surface. However, the situation changes significantly when arc lamp placed into the cavity with diffusely reflecting
walls. The essential feature of such a lamp is strongly absorbed (capture) of all spectral lines (fig. 5b). It leads to an
increase in the effective emitting lifetime of levels τr eff -1, which becomes shorter than the time of their decay as a result
of electron-atom collisions. The result of this phenomena is an increase in population of 3P0,1,2 lower levels of mercury
atoms, which promotes the formation of excited molecules in the reactions of mercury Hg (3P0,1,2) + Hg (1S0) →Hg2.
Spectral bands of these molecules appear in the spectrum of the arc (fig. 4b). Thus, the Boltzmann distribution of the
populations of levels could enable set in the arc plasma at Il = 306 mA of the lamp placed into diffusely reflecting cavity.

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 In this arc discharge lamp curve, the envelope of the measured intensities of the mercury atoms spectral
emission lines, is in good agreement with the Planck curve with the temperature distribution T = 9270 ± 230 K (fig.4b).
Deviations from the Planck curve of individual spectral lines do not exceed 10%. According to formula (4) these
deviations can be a result of different widths of the emission lines Δνki and honors from one of the reflection coefficient
r. Since the formula (4) is valid when the Boltzmann law for the populations of the atomic levels of mercury, it can be
argued that this Boltzmann distribution is established in arc discharge plasma T = Te = 9270 ± 230 K.
The resulting temperature of distribution close to, but below the value of the electron temperatureTe =
11600K3,4,10,11 and Te = 12 765 K 14, which were measured by the probe method in glow discharge plasma of mercury
fluorescent lamps with diameter of the bulb neighbour to the our germicidal lamps. Decrease the electron temperature in
our arc discharge lamp is fully explained by increase of losses on the excitation of vibrational levels of the molecules
Hg2.

5. CONCLUSIONS
Arc low pressure mercury lamp placed in a cavity with diffusely reflective inner surface is qualitatively new
transmitter, in which the maxima of the spectral lines of mercury atoms are distributed according to Planck's radiation
law with the electron temperature of distribution, the contours of all the lines of heavily are distorted reabsorption, and
the mercury molecules lines appear at the emission spectra. These indicate that thermal equilibrium of discrete radiation
with excited mercury atoms is achieved in such plasma.

The work was performed as part of the project RFBR number 15-08-00726a.

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