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Investigations of a r.f. stored Ca+ ion cloud and observation of the S-D forbidden transitions
M. Knoop, M. Vedel, F. Vedel
To cite this version:
M. Knoop, M. Vedel, F. Vedel. Investigations of a r.f. stored Ca+ ion cloud and observation of the S-D forbidden transitions. Journal de Physique II, EDP Sciences, 1994, 4 (10), pp.1639-1650.
�10.1051/jp2:1994222�. �jpa-00248067�
/. Phi.v. II Fianie 4 II 994j 1639-1650 OCTOBER 1994, PAGE 1639
Classification Phj,.ucv Absn.a<i.v
32.70F 32.808 35.80
Investigations of
ar,f, stored Ca+ ion cloud and observation of the S-D forbidden transitions
M.
Knoop.
M. Vedel and F. VedelPhy~ique des interactions
loniques
et Moldculaires j~). Universitd de Provence. Ca,e C21.13397 Marseille Cedex 20, France
(Re<en,ed 3/ Ma» /994, ac.c.epted m final fr)iJii /3 ./u/y /994)
R4sum4, Afin
d'explorer
[es possibilitds d'un dtalon de frdquence dans le domaineoptique
(729 nm), un nuage d'ions Ca+ estpidg6
dans undisposittf
de Paul de dimension intermddiaire. De longues durdes d'observation ~ont obtenues en prdsence d'h61ium dan; un domaine depre;;ion
autour de 10~~-10~~mbar et dans un putts de pseudopotenttel de 62eV. Le; preniikre~
ob~ervations de la transition quadrupolaire
dlectrique
ont dt6 obtenue~ par le peuplement dtrect du niveau mdtastable correspondant (T = s). L'utilisation d'une diode la~er accordable en cavitddtendue permettant de ;onder [es deux niveaux, alor~ que seulement l'un de, deux dtait
initialement peupld a niontrd des intensitds des tluore~cences corre~pondante~ du mdnie ordre.
indiquant la
prd,ence,
h c6td de la relaxation collisionnelle, de trbs forts mdlange; de; niveaux fin,.Abstract. In order to exploit the capability of a
high-Q
tran~ition tor a frequency ;tandard in theoptical
domain (729 nm), a stored Ca+ ion cloud in a medium-size ion trap i~ investigated. Longconfinement time~ are obtained in the presence of heltum as a buffer gas in the range
10~"-10-~ mbar and at a pseudopotential well depth of 62 eV. First ob,ervations of the electric
quadrupole
line were achteved by direct excitation of one of the fir;t metastable doublet level~IT = ~). Utilisation of a grating-~tabili~ed diode laser in order to probe both level~ when only one level is initially populated allo~,~ us to ob,erve almost equal ftuore~cence inten,itie, of both forbidden lines that ~how the pre,ence of a strong fine ~tructure mtxing which exists tn addition to
quenching.
1. Introduction.
Radiofrequency
traps are efficient tools fordeveloping
newfrequency
standards[1, 2].
Suchdevices exceed, in the micrometric domain, the
long
termstability properties
of cesiumclocks
[3].
Indeed, the mostimportant
cause of linebroadening jfirst-order Doppler
effect) does not exist in ion traps whenwavelengths
are of the same order ofmagnitude
as the ion motionamplitude
(Lamb-Dickeregime)
[4]. Lasercooling
extends this property to theoptical region
as demonstrated in[5],
where an effective linequality
factor(Q
=
v/Av of lo' ~ was achieved on the electric
quadrupole
UV line ofHgII
at 281 nm. The verylong-lived
D levels of Ball (49 s for D~j~[6]
and 34.5 s forD,j~ [7]) provide
another candidate. Thecorresponding
(*) URA CNRS 773.
1640 JOURNAL DE PHYSIQUE II N° 10
~j2p
3/2
4~(~~
3~D
866.21nm
~ 5/2
~/2
729.
~2~
1/2
Fig.
I. First energy levels of Call.6~Sjj~-5~D~j~
I-r- transition at 1.76 ~Lm with a natural linewidth of 5 mHz wasinvestigated
on asingle
laser cooled ion where a linewidth of 13 kHz was observed[8],
while the absolutefrequency
of themagnetic dipolar
transition at 12.48 ~Lm was measured on asingle
laser- cooled ion with a linewidth of II kHz[9].
Otherpossibilities
exist with alkaline-earth ions because of their similar A energy level scheme, for instance Yb+ at 411 nm[10],
which also has along-lived
metastable D-level (T(5D~j~
= 20 ms II).
Among
several candidates foroptical frequency
standardsusing
thetechnique
of ionstorage,
Ca+ appears to be one of the mostpromising [12, 13].
The forbidden line4~Sjj~-3~D~j~
at 729 nm(Fig,
I allows theprediction
of aQ
factorsuperior
to 10~~ Linewidthbroadening
due to the Zeeman effect can be avoided in~~Ca+
because of the existence of a transition which, due to its nuclearspin
of 7/2, isindependent (to
firstorder)
ofmagnetic
fields. Lasercooling
must be used to eliminate the first-orderDoppler
width. The resonance line4~Sjj~-4~Pjj~
is strongenough
to cool the ionsby
radiation pressure. However, thecorresponding branching
ratio to the (n I D level~ ~~~ ~~~'~~
=
17.6
[14], requires
jj
A(~P-~Dj)
~
recycling
of the3~Dj~-state
ionsby using
the 866 nm line. The fine structure transition of the D-levels at 1.89 THz can also be used as afrequency
standard in the far I.r.region
andfinally
the
hyperfine
structure of the fundamental level of~~Ca+
at 3.2 GHz. Animportant quality
of the Ca+ system is that all the transitions involved in theoptical
domain are accessibleby
diodelasers. D-P transitions can be
generated directly by using
commercial diodes. The clock transition can beprobed
with anitrogen-cooled
laser diode.Recently, doubling
of ahigh-
power diode laser was demonstrated to
produce
the UV lines[15]. Otherwise,
Ca+ is ofN° lo STORED Ca- AND S-D FORBIDDEN TRANSITIONS STUDY 1641
Table I.
Compilation of
data on thefii~st
metastable D-levels in Call. All theexperiments
were carried out with Paul traps.
Computed (s) Experiments
:(s)
Ref. 17 16 18 19 21 22 20
2D~/~ l.271 1.16 1.20
1.24(39)
1-113(45)
2D~/~ l.236 1,14 1,16
1.24(39) 0.77(7) 1.08(22) 1.054(61)
astrophysical
interest(intense
resonance line in the sun spectrum, E2-lines inSeyfert galaxies,
T Tauri stars and in Betapictoris
disk[16])
andprecise spectroscopic
data arerequired
to builddynamic
models forunderstanding
thesephenomena. Finally, knowledge
of Call oscillatorstrengths
contributes to theunderstanding
of the d orbitalcollapse
withincreasing
nuclearcharge.
The metastable
(n
I D-levels are now considered boththeoretically
andexperimentally.
Table I
gives
recentcomputations
of the natural lifetimesby using
relativisticmany-body
calculations with a third-order
perturbation [17],
amulticonfiguration
Hartree-Fock(MCHF)
method
taking
into account core-valence correlation[161,
animproved
MCHF methodincluding
a relativistic correction[18]
as well as theexperimental
values. The latter are obtained from ion clouds at 2 000 K[19],
at 8 000 K[20],
with lasercooling
on two to three ions at a temperature lower than I K[21],
and on asingle
ion at 130 mK[22].
In
spite
of the fact that ultimatequalities
for theoptical
transitions will be reachedonly
in the presence of a few ions(or only one)
with ahighly-stabilised laser,
we startedby confining
aCa+ ion cloud. The aim of this paper is to report on the interaction between the buffer gas and the atomic ions and to
give
our first resultsconcerning
thespectroscopic investigations.
We present first our apparatus,secondly
theproperties
of the stored ion cloud andfinally
wedescribe the
experiments
on the forbidden lines, which wereperformed
from direct excitation of the D-levels followedby
thepumping
of the P-level from the metastable states. Aqualitative study
of the D-level fine-structuremixing
ispresented.
2. The r,f, ion storage
technique
and theexperimental
set-up.Radiofrequency
ion traps arecapable
ofstoring,
in a smallregion
of space, thanks to thelarge potential
welldepth
available, small ion clouds in a well defined and well controlledenvironment, without a
magnetic field,
forlong periods enabling
accurate observations.Confinement
[23. 24]
is obtainedby creating
aquadrupole
electricfield,
inside the trap, whichresults of the
superposition
of a directvoltage,
V~c, and of analternating voltage,
V~~, at the
radiofrequency
fl/2 gr, in such a way that the motionamplitude
stays finite for a setof values
(V~~,
V~~,fl),
whichdepends
on the electroncharge
toion-species
mass ratio~ and the geometry of the device, i-o, co
(Fig. 2).
This set of values constitutes thestability
m
diagram.
The usual reduced parameters are(for singly charged ions)
:16
eV~~
a, =
~ ~ ~ ; a~ = a~ =
a-/2 mfl
(ij
+2z~)
8
eV~~
~° mfl
~(r(
+ 2z()
~~ ~~ ~~~~ ~~~according
to the electrical scheme infigure
2.1642 JOURNAL DE PHYSIQUE II N° lo
J~ I-Sa Laser -~ill(iiilfi~il
@ $t$itzlty
ro=jTz~
~f2 /
q ~
Electron/~~ ))) / Ion traP
~Photomultiplier
~ j,;,;,;,;,;,;,;,,,,,,,;,,,,j
' $i~~~~~~~~~~~~~~~~~~~~~~~~
~~
Electron
muifipier
Lens '
'
Oven
a) b)
Fig.
2. Experimental apparatus (a) and the r-f- ion trap (b).Trapped
ion motion isideally quasiperiodic.
For each component, with respect to thecylindrical
revolution, thefrequency
spectrum contains the so-called fundamentalfrequency
w~
(resp.
w-), which isalways
smaller than thedriving frequency,
fl.Higher
harmonics arepresent at
w~±nfl (resp.
w.±nfl). The most intense onescorrespond
to n=0,±1 and, less
important,
to n=
2. Therefore, the motion is
mainly
thesuperposition
of aSecular motion at w~
(resp.
w=) and a micromotion at fl. Secularfrequencies
w~(resp.
w=)
depend
on the a~ and q~(resp.
a. and q=)values,
andthey
are obtained from the r.f.frequency
flaccording
tow~ = p
fl/2,
w.=
p-
fl/2(with
0~ p
~,
p- ~
1) (2)
where
p~ (resp. p-),
can beapproximated by ja~
+ 2q(
resp.~
a- + 2q]
for smallMathieu parameters.
Computations
of more exact values must however use iterativemethods
[25].
The micromotion causes r-f-
heating
and is the main limitation for lasercooling
with more than a few ions. Anharmonicities in the system,responsible
forcouplings
between the secularand the micromotion or between the different
degrees
of freedom[26, 27] modify
thefrequency
spectrum of each component of the motion. Theinvestigation
of these spectra cantherefore
give
information on the iondynamics
and storageproperties [?6].
Ca~ ions are stored in a conventional
hyperbolic radiofrequency
trap(Fig. 2)
withi-o =
,,fi
=o =7.2 mm. The
ring
of the ion trap is made< of stainless steel and the end caps frommolybdenum
mesh ofhigh
transmission(83
fb). Theexperiment
isperformed
underultrahigh-
vacuum conditions with residual pressures less than
10~~
mbar. A needle valve allows theintroduction of a pure buffer gas, the pressure of which is measured
by
a linearquadrupole
mass spectrometer and a
Bayard-Alpert
gauge. Ca atoms areevaporated
into the trap from asmall oven, situated very close to the
ring (Fig.
2) and are ionised inside the trap with apulsed
N° lo STORED Ca+ AND S-D FORBIDDEN TRANSITIONS STUDY 1643
electron gun, which is biased at 40 V. The confinement
radiofrequency
fl isequal
toI MHz
x2gr,
the dcvoltage
V~~ varies between 0 and lo V and the acvoltage
V~~ between 90 and 15 V.
Working points
are therefore close to the best conditions of storage[28, 29].
Besidesoptical
detection(see below),
Ca+ ions can be detectedelectronically by
resonant detection
[30]
which monitors the ion energyabsorption
in a circuit tuned to one ofthe motional
frequencies,
andby
a resonantejection
method[3 Ii, by using
anelectronmultip-
lier. The latter can show the ion motion
properties
when ions are submitted to an additionaldipole
orquadrupole alternating voltage
at variablefrequency.
Both methods can increaseslightly
the ion kinetic energy.For
spectroscopic investigations,
the resonance radiations aregenerated by
a titanium-sapphire ring
laser(Coherent 899-05).
The first harmonic is doubledby
anintracavity LiIO~ crystal
whichprovides
up to 19 mW at 397 nm, with aspectral
width of i MHz. A laserdiode,
covered with an antireflectioncoating,
is mounted in an externalcavity (1
200 lines permm Jobin-Yvon
grating)
and can be tuned between 845 and 867 nm with aspectral
width ofapproximately
30 MHz. At 866 nm, theresulting
power is estimated to be 200 ~LW. The 729 and 732 nm lines are available from the fundamental of the Ti-Sa laser with power up to W.The laser beam traverses the trap
diagonally
between thering
and the caps. It is focussed at thecentre of the trap
giving
a beam waist diameter M,o of 70 ~Lm for the 397 nm and of 150 ~Lm forthe red radiation. The diode laser beams, due to their
divergence
andastigmatism,
are difficult to focus.They
have a minimal diameter of about 0.5 mm inside the trap andthey overlap
theTi-Sa laser beam. Emitted
photons
are collectedby
alarge
apertureaspherical
lens and are focused on a Hamamatsu H4730photo multiplier
which is run in thephotoncounting
mode. To discriminate thesignal
from thebackground
and the scatteredphotons,
an interference filtercan be
placed
in front of thephotomultiplier.
3. Electronic and
optical
ion-cloud studies.The
properties
of the ion cloud arefirstly investigated
with electronic methods. These methodsare more reliable for
long
measurementperiods
thanoptical
ones whichrequire
the laser power to be stableenough
toprecisely
measure relative ion number variation, as the ion cloud evolves. Moreover, all the ions aresubject
to the electrical excitation and thesignal
isgenerally independent
of thegeometrical shape
of the cloud.Introduction of a
light
buffer gas into the apparatus can, due to elastic collisions, reduce the ion kinetic energy. Thispartially
compensates the r-f-heating
and therefore increases the confinement times. In the presence of helium at 10~ ~ mbar, ions are stored for several hours.The storage time
depends
on the buffer gas pressure and, aspredicted,
isoptimised
for agiven
pressure
[32].
Other gases, such asnitrogen
or neon, make the ion-cloud storage time shorter,as their masses are
comparable
to that of calcium. These observations arerepresented
infigure
3.Resonant
ejection
[3Ii
with aquadrupolar
tickle of 0.01 Vduring
lo ms showspeaks
atw/2,
w,, w~, w~ +w/2,
2 w~ w,, w~ + w~, 2 w~(Fig. 4).
The measured secularfrequencies (contrary
to the theoretical values)depend
on thecoupling
parameters(space charge,
anharmonicities). The spacecharge
effects are related to the collisions with the buffer gas.Indeed, with
light
buffer gases, the collisions reduce the kinetic energy[30, 33]
and increase~
the F
coupling
factor[34] (F
=
~
,
where k is the Boltzmann constant, T the ion 4 gr ~o akT
temperature, defined below, and a is the mean distance between the ions such that 4 «no
a~
= I, with no the ion
density
at the center of thetrap).
The secularfrequencies
also are 3strongly
shifted to lower values[35].
These reductions can be seen as a reduction of the p1644 JOURNAL DE PHYSIQUE II N° lo
1000
~
. He Wo N~
+ CO
~
v Ne w
loo
_
w
£
u~
lo
~ (
~
~ ~ ~
~
~m
y
x
x
x wY
1E-8 lE-7 1E-6 0 o0001
p mbar
Fig.
3. Storage time as a function of buffer gas pressure.2000
E
~
a
d
it e
bS b
f
0 0
[kHz]
Fig.
4. Ion ejection signals in the presence of a quadrupolar excitation. The signal is observed with a delay after the electric excitation and when the confinement voltage is just interrupted in such a way that the spectrum is relevant from the axial and radial motion spectrum. al w,/2, b) w,, c) w~, d)w~ +
w/2,
el 2 w~ w,, fl w, + w~, g) 2 w~.parameters or a
displacement
in theStability diagram. Therefore,
if observations are made withthe resonant electronic detection (where the
signal
is obtainedby working
with a fixedresonance) the
dc-voltage
has to be decreased in order to compensate thedisplacement
of theworking point
in thestability diagram. Figure
5gives
agood
illustration of such an evolution of the cloud i,eisus thebuffer-gas
pressure, as well as the influence of the neutrallion mass ratio.Apparently,
collisions withnitrogen
molecules have almost no effect on the kineticN° lo STORED Ca" AND S-D FORBIDDEN TRANSITIONS STUDY 1645
. with He
+ vdth N~
@-~,w+, S,bw+
++ ++ i+ ~ ~ +
+ w~
*
,,.
.;.,
'*%,
-
$
t
t~%
g
.
~
.~
~_
O
p
ig.5.
of
arametersersus
thepressure, ue to
charge,by
gases.
1646 JOURNAL DE PHYSIQUE II N° 10
long
lifetime of the metastable states, ions aretrapped
in the D-state.However,
observation ofa fluorescence
signal
ispossible by
the presence of a buffer gas which reduces the D-lifetimeby quenching.
The addition of a diode laser, which
empties
the D-level andpermits
all the ions to be involved in theabsorptionlemission cycle,
allows a drastic increase of thesignal-to-noise
ratioas seen in
figure
7.The Gaussian character of the ion
velocity
distribution is well establishedexperimentally [36]
as well astheoretically [33, 37].
The distribution for each component(with
respect to thecylindrical symmetry)
oscillates at theradiofrequency.
Its widthdepends
on theworking point (micromotion amplitude),
thepotential
welldepth
and, asalready
mentioned, on the neutral- to-ion mass ratio.Although already
used in thispresentation,
the notion of temperatureapplied
to a stored ion cloud must now be defined. The r,f.
time-average
of the mean kinetic energycommonly
allows definition of an a.<ial or radial temperature. This parameter can be checked either with electronic detection as intime-of-flight experiments [38-40]
or withoptical
measurements. In the case of
optical
measurements, the temperature can be deduced from theDoppler profile
obtainedby sweeping
the laserfrequency.
The temperature has to be deduced from the standard deviation whichcorresponds
to aprofile
of thevelocity
distribution i>ersusone
degree
of freedom. Since the laser crosses the ion trapdiagonally,
theprofile
is related to theprojection
of the three components of the ion motion. The standard deviation of theobserved Gaussian
profile
«~~, isgiven
from the standard deviations for each component3 kT/m
= « +
ml
+al
=
«j~,(2 sin~
~o +
cos~
#(3)
where ~ is the
angle
between the laser beam and the revolution axis of the ion trap. In ourexperiment,
~ isequal
to 38° and 3 kT/m= 1.4
«j~,.
Ion motions are
coupled together by
the anharmonicities of the fields and spacecharge,
which
permits
theassumption
that thevelocity
distribution isisotropic. Ideally (pure
quadrupole
field withoutparasitic coupling)
theanisotropic
property definedby
« -la does notexceed, for our
(a=, q=)
values, 1.3[41].
The
efficiency
of the collisionalcooling
was monitoredby
observation of theDoppler profile
and controlled
by
buffer gas pressure. The evolution of temperature can be seen infigure
8.j~#' ~ ~~~~~~ode
~ /
" '
fl
$
#
QI
X
~
lo 5 o 5 lo
Laser dewdng GIIz
Fig. 7. Detected resonance line at 397 nm (xl only with a buffer gas, (Al in double resonance.
N° 10 STORED Ca* AND S-D FORBIDDEN TRANSITIONS STUDY 1647
14000
12000
- »
v
j
- ~
~
jj
x_w
~
« w
~l*
x ~
10'~ 10'~ 10'~ 10"~
p mbar ]
Fig. 8. Temperature of the ion cloud as a function of helium buffer gas pressure at lower pressures.
the signal to noise ratio diminishes due to the decreasing ion density.
Here the
averaged
kinetic energy is therefore 0.2 to eV, for a totalpotential
welldepth (D,
+D~
of 62 eV. Similar values were obtained for Ca* stored in a shallowerpotential
well[19].
This confirms that thedependence
of the kinetic energy i>eisiis thepotential
welldepth
isnot
simple [37].
The variation of the kinetic energy ieisiis the pressure should be consideredfor rate constant studies.
4. Direct excitation of the E2-transitions.
Becau~e of the ~trong interest for the 729 nm line as a
frequency
standard, the forbidden transitions wereinvestigated.
One of the D-levels wmpumped directly by
the first harmonic ofthe Ti-Sa laser.
Simultaneously,
thecorresponding
P-D transition was excitedusing
thegrating-stabilized
diode laser at a fixedfrequency.
Detection was made on the S-P fluorescenceat 397 nm, as discussed above. Thi~
pumping
scheme has theadvantage
ofeliminating
thescattered
photon background.
A
typical profile
of the 729 nm-line is shown infigure
9, with 700 mW of laser power (because of the smaller linewidth, lower power will berequired
for colder clouds). Inspite
of therelatively
weak count rate, thesignal/noise
ratio (close to10)
allows us to u~e directpumping
of the D-levels in order toinvestigate
them. For the excitation of the electricquadrupole transition,
the available laser power is much less than that needed for saturation, whereas for the D-P transition, the diode laser power far exceeds the saturation limit. In order to use this detection scheme for furtherexperiments,
itsefficiency
was tested over a broad range of helium pressures. It was observed that thesignal
growsrapidly
when the pressureincreases, with a
slight background
increase. This behaviour shows that collisions with the neutralparticles
concentrate the cloud and enhance theoptical signal. Moreover,
the width of the lines decreases due to thecooling
effect. The temperature, which is deduced from thi~profile
is very close to the valuesgiven
above.In the presence of helium (or other
gases),
the lifetime~ of the metastable levelsdepend
onthe
quenching
and fine-structuremixing
rates.Actually,
besides the collisional relaxation, astrong
mixing
rate exists due to the small energy difference between the D~/~ andD5n
levelsj648 JOURNAL DE PHYSIQUE II N° 10
'
~/
134 u '
m
li
#
$fl
i~
)
~~ '
~
aser
Fig. 9. - of
at
2
10~~ arN° 10 STORED Ca+ AND S-D FORBIDDEN TRANSITIONS STUDY j~49
(7.4 mev) [19].
Tostudy
this weprobed
the3~Djj~
levelby observing
the resonance line at 397 nm from the 4~Pj~~pumped
with the diode laser at 866 nm. Excitation was made either at 732 nm(4~S,j~-3~D~j~),
or at 729 nm(4~Sjj~-3~D5j~).
The normalized intensities of both lines(for
which the difference between the oscillatorstrengths
is verysmall)
arequite comparable
in the presence of helium at ratherhigh
pressures.Figure
10 shows the variation of thepopulation
differences i,ersus the helium pressure in a
large
domain. Itclearly
demonstrates thedependence
of thej-mixing
with the pressure. A maximum exists around10~~
mbar. Lower pressures reduce collisions and thej-mixing while,
forhigher
pressures, the collisions increase the observed D~j~ ion loss rate and shorten its lifetimeconsiderably
so thatmixing
can nolonger
takeplace.
5. Conclusion.
In order to
study
thepotential
of thehigh-Q
line of Call as afrequency
standard in theoptical domain,
webegan
aspectroscopic study
on stored Ca+ ions.We constructed an ion trap apparatus which can confine 10~ to 10~ Ca~ ions and obtained
experimental
conditions forlong
storage. The direct excitation of the electricquadrupole
transitions demonstrated a strong
j-mixing
which now must bequantitatively investigated.
We intend to thisby
measurements resolved in time in the presence of gases besides helium, suchas
N~,
Ne. Aquantitative study
of the D-level lifetime andcorresponding quenching
andmixing
ratesby
direct excitation of the metastable stages isunderway [42].
Thequenching
andmixing
rates shoulddepend
on the energyconditions,
which can bechanged by varying
theworking point.
Acknowledgments.
The authors would like to thank G.
Werth,
for encouragement andhelpful
discussions whenstarting
this research and for access to the mechanicalworkshop
in Mainz for the realisation of the ion trap.They
also want to thank R.Thompson,
for his efficientparticipation
in the firstoptical
measurements.This work was
supported by
Direction Gdndrale des Recherches et des EtudesTechniques.
M.
Knoop
isgrateful
to the EC(Human Capital
andMobility program)
for financial support.References
[1] Dehmelt H., Rev. Mod. Phys. 62 (1990) 525-530.
j2] Werth G., Jpn J. Appl. Ph_vs. 33 (1994) 1585-1589.
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