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Method and experiment
J.C. Garreau, M. Allegrini, L. Julien, F. Biraben
To cite this version:
J.C. Garreau, M. Allegrini, L. Julien, F. Biraben. High resolution spectroscopy of the hy- drogen atom. I. Method and experiment. Journal de Physique, 1990, 51 (20), pp.2263-2273.
�10.1051/jphys:0199000510200226300�. �jpa-00212527�
High resolution spectroscopy of the hydrogen
atom.I. Method and experiment
J.C. Garreau
(*),
M.Allegrini (**),
L. Julien and F. BirabenLaboratoire de Spectroscopie Hertzienne de
l’ENS(***),
Université Pierre et Marie Curie, 4 place Jussieu, Tour 12, E01 75252 Paris Cedex 05, France(Received 2 February 1990, revised 15 June 1990, accepted 27 June 1990)
Résumé.2014 Pour mesurer la constante de Rydberg R~ avec une très grande précision, nous avons
fait une expérience d’absorption à deux photons sans effet Doppler sur les atomes d’hydrogène et de
deutérium. Nous avons obtenu une nouvelle valeur de R~ qui est en excellent accord avec les autres mesures récentes, et la plus précise à ce jour. Nous décrivons ici en détail la méthode et l’appareillage
utilisés. Un jet d’atomes d’hydrogène métastables est excité vers les états de Rydberg nS et nD (n~8)
dans une transition à deux photons. La géométrie expérimentale a été choisie de façon à rendre co-
linéaires le jet atomique et les faisceaux laser. Avec ce montage, nous avons observé des résonances très étroites avec une largeur relative inférieure à 10-9. Parmi toutes les transitions observées, nous
avons sélectionné trois transitions (2S-8D, 2S-10D et 2S-12D) dans l’hydrogène et le deutérium pour déterminer R~.
Abstract. 2014 In order to determine the Rydberg constant R~ to a very high accuracy, we have
performed a Doppler-free two-photon absorption experiment on atomic hydrogen and deuterium. We have obtained a new value of R~ which is in excellent agreement with other recent measurements and the most precise one at the present time. Here we give a detailed report on the method and
apparatus we have used. A metastable beam of 2S H and D atoms has been prepared and laser
excited to Rydberg nS and nD levels (n~8) in a two-photon transition. The experimental geometry
has been carefully designed to make the atomic beam collinear with the two counterpropagating laser
beams. With this set-up we have observed very narrow resonances, with relative linewidths smaller than 10-9. Among all the transitions investigated we have selected three transitions (2S-8D, 2S-10D
and 2S-12D) in hydrogen and deuterium to determine R~.
Classification
Physics A bstracts
35.10 - 06.20J - 32.80K
Article published online by EDP Sciences and available at http://dx.doi.org/10.1051/jphys:0199000510200226300
1. Introduction.
In a recent paper
[1] ,
we havereported
thewavelength
measurement of the three transitions 2S-8D, 2S-10D and 2S-12D in atomic
hydrogen
and deuterium. These measurements lead to a newdetermination of the
Rydberg
constant which is at present the mostprecise
one. This paper is the first of a series of three, hereinafter referred to as paper I, II and IIIrespectively,
in which wegive
acomplete description
of the method used to obtain this result. In this paper(I),
we presentthe
principle
of our method and we describe theexperimental
set-up which allowed us to observe very narrowsignals. Paper
II will be devoted to thesignal analysis
withspecial regard
to thecomparison
of calculated lineprofiles
with theexperimental
curves.Paper
III willgive
the detailsof the absolute
wavelength
measurementprocedure
and theRydberg
constant determination.The
Rydberg
constant Roo is one of the fundamentalphysical
constants which isimportant
tomany areas of
physics
andchemistry [2,3].
It issimply
related to the other fundamentalquantities
m
(electron mass), e (electron charge),
h(Planck constant)
and c(velocity
oflight):
and it is one of the most
accurately
measured. There are several reasons for the continuous effort toimprove
itsprecision.
Indeed itplays
akey
role in all calculations of atomic and molecular levels and in theleast-squares
fit of the fundamental constant values where it is used as anauxiliary
constant
(i.e.
with a fixed value notsubjected
toadjustment) [4, 5].
A veryprecise
value of Tïoo isrequired
to test QED calculations ofsimple
systems; twoexamples
are the determination of the H 1Sground
state Lamb shift and thecomparison
between measured and calculatedfrequency
ofthe
positronium 13Si - 23Si
transition. Since Roi can inprinciple
be measured from thefrequency
of any of the atomic
hydrogen
transitions, itprovides
a severe test of the 1/rdependence
of theCoulomb
potential
which may prove the existence of the "fifth force"[6].
Measurements of .Roo withequal precision
in differentspectral regions
wouldpermit
the use of thehydrogen
atom as awavelength-frequency
standard in theoptical
domain[7, 8] .
During
the last ten years several measurements of Rea have beenperformed
on atomichy- drogen
and deuteriumusing
the refinedtechniques
ofhigh
resolution laser spectroscopy.Early discrepancies
are now settled and aff recent results are in excellent agreement[1, 9-13].
The ac-curacy of Roo has been
improved
from 3 parts in108,
achieved in the first laserexperiment
onhydrogen [14] ,
to a few parts in 101 °. The limit is nowgiven by
the accuracy of the presentwavelength-frequency
standard in the visible,namely
the I2-stabilized He-Ne laser[15].
2. Method.
The energy of the
hydrogen
atom levels isstrictly proportional
to theRydberg
constant; thusa direct measurement of the
wavelength
orfrequency
of an atomic H-transition is inprinciple equivalent
to a measurement of Roo. Transitionsinvolving
low values of theprincipal
quantumnumber n lie in the
optical
domain and Roe is in this respect the natural unit ofoptical frequencies.
It is evident that the accuracy of Roe
depends
upon the measurement of the absolutefrequency
of the
hydrogen spectral
line underinvestigation.
Both thelineshape
and linewidth of the atomic transition are therefore crucial for the finalprecision
of the Aoo value.Figure
1 is a schematicreprésentation
of the transitionsinvestigated
in ourexperiment
as well asin other recent
experiments performed
in theoptical
domain. The moststraightforward
way is tostudy
the 2S-3P and 2S-4P Balmer lines becausethey correspond
to directone-photon
transitions.Indeed
they
have beenthoroughly investigated
at Yale in a set of neat andelegant experiments [16,10,11]
which are theequivalent
to theearly
microwaveexperiments [17] designed
for theLamb shift measurements. The linewidths of these resonances reflect the natural width of the P-states involved
(30
MHz and 12 MHzrespectively)
which is the mainlimiting
factor on theprecision
of Roo measured in theseexperiments.
Fig. 1. - Schematic energy diagram of atomic hydrogen.
Of
special
nature-and interest is the 1S-2Stwo-photon
transition which has beenextensively investigated by
three different groups(Stanford-Münich, Southampton
andOxford).
This is oneof the
sharpest
lines available tospectroscopists;
due to the 1.3 Hz linewidth of the metastable 2Slevel, the relative width of the 1S-2S transition is 5 x
10-16 only.
However, the 1S-2S transition is not the ideal choice for aRydberg
constant measurement because it is affectedby
theuncertainty
in the 1S Lamb shift. Therefore the 1S-2S transition
wavelength
measurementprovides
a value ofthe
Rydberg
constant within theuncertainty
of thecomputed
Lamb shift, orequivalently
allows todetermine the 1S Lamb shift, the value of the
Rydberg
constantbeing
taken from other sources.The way we have chosen to get very
sharp
lines is toinvestigate
thetwo-photon
transitions from 2S to nS and nD states(n>8)
in atomichydrogen
and deuterium[18].
The natural width of these levels decreases as n-3 and for the 10D state forexample
is ~ 300 kHz. First-orderDoppler
ef-fect has been eliminated
by
thetwo-photon absorption technique [19],
based on the interaction of the atom with astanding
waveresulting
from thesuperposition
of twocounterpropagating
laserbeams of the same
frequency.
Thistechnique,
like other non-linear processes,requires high
laserpower
density
which isresponsible
forbroadening
and shift of the transitions. However, theseeffects can be corrected for very
precisely,
as will be described in paper II. In order to avoid colli- sionalbroadening
the metastable atoms areproduced
in a beam which is animportant
part of our apparatus. Moreover we have used a geometry which makes the metastable beam collinear with the two laser beams so that laser-atom interaction time islong
and theresulting
linebroadening
reduced.
An
advantage
ofworking
with the 2S-nS and 2S-nD transitions is that the Lamb shift of themetastable 2S state has been
already
measured veryprecisely [20, 21] .
For theRydberg
states itis very small and calculated to
high precision.
Indeed our method to determine Roo , once wehave measured the
frequency
orwavelength
of the2S1/2 - 8Ds/2, 2Si/2 2013 lOD5/2
and2S1/2 - 12Ds/2
transitions of atomichydrogen,
takesadvantage
of the fact that the 2S Lamb shift is knownwith an accuracy of few kHz. We have used the Pal’chikov et al.
[20] experimental
value of the2Si/2 - 2Pi/2
energy interval and our measurement of the251/2 - nDs/2 (n
=8, 10, 12)
transitionwavelengths
to get thefrequencies
of thecorresponding 2Pl/2 - nD,5/2
transitions.By comparing
the theoretical and
experimental
values of this last energy interval, forwhich - Roo
is ascaling
factor, we determine Aoo Thetefore theprecision
of this measurement is not affectedby
the QED corrections on the 2S energy, butonly by
those on the 2P and nD levels(n
=8, 10, 12)
which areat least a factor 50 smaller. The overall effect of QED corrections, 2S Lamb shift
precision
andelectron-to-proton
mass ratiogives
at the present time an intrinsic limit(i.e.
not related to theexperiment)
of 1.9 x 10’ 11. For the determination of Roo we have also used three transitions of atomic deuterium for which the 2S Lamb shift has not been measured with suchhigh
accuracy as inhydrogen.
Nevertheless we have used the sameprocedure
except for the fact that we have been forced to use a theoretical value for the 2S Lamb shift(1057.229 MHz),
which we have calculatedusing
the formulagiven by
Erickson and Grotch[22] .
As we will see in paper III, the six values of Roo obtained from the threehydrogen
and the three deuterium transitions are consistent each with others. Thus this result is an indirect test of the agreement between calculated and measured values of the 2S Lamb shift.3. Apparatus.
The basic apparatus was
already
used in 1986 for a first measurement of Rooby two-photon
spec- troscopy ofhydrogen Rydberg
states[9].
For the presentexperiment
severalimprovements
havebeen made
designed
to reduce the linewidth and to measure the absolutewavelength
of the ob-served transitions with the
precision
of thewavelength
standard in the visibleregion.
The ap- paratus consists of four main parts sketched infigure
2 : the atomic beam, the laser source, theFig. 2. - Block diagram of the whole apparatus.
data
acquisition
system and thewavelength
measurement system. Theexperiment
is run in two steps :i)
determination of the atomic transitionpeak
relative to a fixed reference(blocks
a, b, c ofFig. 2)
andii)
measurement of the absolutedye
laserwavelength by comparison
with the standardHe-Ne laser
(blocks
b, c, d ofFig. 2).
The first step involves a carefulstudy
of the lineprofiles
which will be
given
in paper II; the secondstep
relies on the interferometrictechnique
for wave-length
calibration which is one of thesubjects
of paper III. The details of the lastportion
of the apparatus(d)
will also be in paper III. Thequality
of each component of the apparatus isimpor-
tant to the final
goal;
however, a crucial role iscertainly played
by the atomic beam apparatus forproduction
and detection of the metastable 2S-atoms ofhydrogen
and deuterium.3.1 ATOMIC BEAM. - 1èchnical details and
physical
characteristics of the beam which may be of interest in different types ofexperiments
aregiven
elsewhere[23].
Here we mentionschematically
the
working principles.
Atomichydrogen (or deuterium)
isproduced by
molecule dissociation ina
discharge
tube; then a thermal beam ofground
state atoms flows into a vacuum system which is divided in three chambers. In the first chamber, the atoms are excited to the 2S stateby
electronic bombardment; the deviation of ~ 20° due to the inelastic collisions with the electrons is used toget a metastable beam which is collinear with the two
counterpropagating
laser beams as shown infigure
3. The metastable atoms, with the propervelocity
direction, enter then a second chamberFig. 3. - Experimental geometry of laser and atom beams.
Fig. 4. - Interaction chamber and detection system.
with entrance and exit apertures
consisting
of two 7 mm diameterdiaphragms (see Fig. 4). This
region,
where the atoms interact with the laserlight,
is evacuatedby
twocryogenic
pumps andis
carefully
shieldedagainst
straymagnetic
and electric fields which affect the atomiclineshape
and line
position.
The metastable atoms are detected in a third chamber where an electric field isapplied
to mix the 2S and 2P levels and theresulting Lyman-a
fluorescence is detectedby
apair
ofphotomultipliers symmetrically positioned
with respect to the atomic beam. Thequenching
volt-age is square-wave modulated at 830 Hz and a
phase
sensitive detection, at the samefrequency,
is used to monitor the
photomultiplier
outputs. Thevoltage applied
to eachphotomultiplier
isadjusted
in such a way that both deliverequal signals :
thesignal-to-noise
ratio of the sumsig-
nal is then maximized. From the
photomultiplier
efficiencies and the detection solidangle,
wecan deduce the value of the metastable atom flux : 2.6 x 106 s-1. The
velocity
distribution of the metastable atoms has been also studied : it has been deduced from theDoppler-shifted
2S-3P Balmer-a
absorption profile
recorded with adye
laser beam collinear with the metastable beam. The measured mostprobable
velocities in the beam are 3.05km/s
forhydrogen
atoms and1.97
km/s
for deuterium atoms.3.2 LASER souRCE. - The source used for the
optical
excitation is a home-made c.w.ring dye
laser described in reference[24] .
The radiation needed for the 2S-nD(n>8) two-photon
transition is in the 730-780 nm range, obtainable with LD700
dye pumped by
a Kr+ laser. Thedye
laser delivers power up to 1 W insingle
modeoperation
in thiswavelength
range.The
frequency
stabilisation is doneby locking
thedye
laser to an external 25 cmlong Fabry-
Perot
cavity, by monitoring
the reflected beampolarization according
to the method of Hânschand Couillaud
[25].
Anelectro-optic
device inserted in thedye
lasercavity
reduces the laserjitter
to about 50 kHz.
Th sweep and control the
dye laser-system
an additionaloptical
device has beenplaced
outsidethe
optical cavity
of theoriginal
laser, as shown infigure
5. Thefrequency
reference is a home- made I2-stabilized He-Ne laser at 633 nm. To check thestability
of this laser, the beatfrequency
with a second standard He-Ne laser, locked to a close 12 molecular line, is
continously
monitored.A reference
Fabry-Perot cavity (FPR)
is locked to this etalon laser so that itslength
is fixed. Thiscavity
is very stable : it consists of a 50 cmlong
zerodur rod, two silver coated mirrors, one flatand one
spherical (R
= 60cm),
and a PZT, all in an evacuated box. Thecavity
finesse is 100at 633 nm and 150 at 780 nm. To sweep the
dye
laserfrequency,
the laser beam issplit
and thesecondary
beam enters anacousto-optic
device. Thefrequency-shifted
beam is reflected back into theacousto-optic crystal
so that one of theemerging
beams is shifted twice. This beam then enters the referencecavity.
Itsfrequency
is locked to thecavity length using
aservo-loop acting
on the
dye
laser externalFabry-Perot cavity (for
thisservo-loop,
thelength
of the referencecavity
is modulated at 5.5
kHz). By changing
theacousto-optic
modulationfrequency,
which isprovided by
acomputer-controlled frequency synthesizer,
we can sweep thedye
laserfrequency
over arange of 250 MHz centered at any desired
frequency.
This whole set-up allows us to control veryprecisely
thedye
laserfrequency
with areproducibility
of about 10 - 11.lb induce the
two-photon
2S-nD transitions with agood efliciency,
we haveplaced
the wholemetastable beam apparatus inside a
I%bry-Perot cavity (see Fig. 4) having
itsoptical
axis in coin- cidence with the metastable beam. Thecavity
is 1.3 mlong
and the two mirrors have 4 m radii of curvature so that the beam waist wo inside thecavity
is about 600 um. The transmission of the en- try mirror Mi is 1.5% and the end mirror M2 is ahigh
reflector. The two mirrors are mounted onPZT and the
cavity length
is locked to the laserwavelength by monitoring
the reflected beam po- larization[25].
The total laser-atom interactionlength
is 956 mm, definedby
thepair
of aperturesplaced
at the entrance and the exit of the second vacuum chamber.Metastable atoms in the
cavity
are then submitted to an intenseoptical standing
wave result-ing
from thesuperposition
of twocounterpropagating
waves(power
up to 50 Weach).
Thelight
Fig. 5. - Scheme of the experimental set-up to control the dye laser frequency.
intensity
inside theoptical cavity
is controlledby monitoring
with aphotodiode
the smallportion
of the laser
light
which is transmittedby
thecavity
end mirror M2.3.3 DATA ACQUISITION SYSTEM. One
major improvement
to ouroriginal
apparatus used forthe 1986 measurement of Roo
[9]
is the use of amicrocomputer
for the control of several parts of theequipment,
and for the dataacquisition
andanalysis.
In the dataacquisition
we have todistinguish
between the detection of thetwo-photon
atomic transitions and therecording
of allother parameters necessary to get the final result.
After
optical
excitation of the atomic transition, there are several methods that can be used for detection : fluorescence measurements(for example
on the nD-2Ptransition),
field ionization(quite
efficient forn >25), quenching
of the 2S metastable atoms. In the present work we havechosen this third method,
detecting
the decrease of .the metastable beamintensity.
When theatoms are
optically
excited from the 2S metastable state to a nDRydberg
level, 95%decay
tothe 1S
ground
statethrough
a radiative cascade, and theoptical
transition can be detected as adecrease of the 2S
population.
Theadvantage
of this method is that alloptically
excited atomscontribute to the observed
signal, independently
of theirposition
in the beam. Indeed,figure
4shows that the metastable atoms are
produced just
beforeentering
theregion
of interaction with the laser and detectedjust
afterleaving
it. Ibedisadvantage
is that thesignal
is detected over thelarge
metastablepopulation background
which is not favourable to thesignal-to-noise
ratio. Forthe
Rydberg
constant determination we have usedonly
the2S1/2(F
=1) - nDs/2 (n
=8, 10, 12)
transitions because
they give
the more intensesignals.
We have
already explained
how thedye
laser is drivenby
acomputer-controlled synthesizer
which determines the absolute laser
frequency
with respect to apeak
of the referenceFabry-Perot cavity. By sweeping
thefrequency
of thesynthesizer we
can scan thedye
laser over the atomic tran- sition and detect theresulting signal
on the metastable atompopulation.
Inpractice,
for atypical signal recording
which lasts about 20 minutes(one "run"),
the laserfrequency
is scanned ten timesacross the atomic resonance,
alternately upwards
and downwards.Simultaneously,
the computerrecords the
signal provided by
the lock-inamplifier
which measures the number of metastable atoms at the end of the atomic beam. Other useful data such as the beatfrequency
between thetwo etalon lasers and the
light intensity
transmittedby
the excitationoptical cavity
are also col-lected. These data are useful to eliminate from the run the
signal acquired during
bad conditions ofoperation.
Afterwards thesignal
isaveraged
over the ten scans. Thisprocedure
is illustratedFig. 6. - Example of an experimental run
(281/2 -1081/2
transition in deuterium): signal recorded by thelock-in amplifier (a) and laser frequency scans (b) during a run of 20 minutes; two-photon signal averaged
over 10 scans versus the atomic frequency (c).
in
figure
6 in the case of the2Si/2 - 10Si/2
transition in deuterium.Figure
6a shows the metastablebeam
intensity
andfigure
6b the variation of the laserfrequency during
the run; after the averageover ten scans, the
two-photon signal clearly
appears, as shown infigure
6c.3.4 WAVELENGTH MEASUREMENT SYSTEM. Since this
portion
of the apparatus(block
d ofFig. 2)
will be described in detail in paper III, wesimply
report here the basic idea of the mea-surement. The absolute
frequency
of thedye
laser(and consequently
the measuredwavelength
of the atomic
transition)
is determinedby
an interferometriccomparison
with thefrequency
ofour reference 12-stabilized He-Ne laser. This laser has been
compared
with one of the "Institut National deMétrologie"
which has beenpreviously compared
with the standard He-Ne lasers of the "Bureau International des Poids et Mesures". Thekey
of thewavelength comparison
is anetalon
Fabry-Perot cavity
which has beenspecially designed
and built to match therequirements
of the present
experiment.
4. Observed signals.
Using
the method and theexperimental
set-up described so far, we have recorded lines corre-sponding
to the atomic transitions listed in table 1together
with theiramplitude.
The list of table 1 is not exhaustive; inprinciple
all the transitions coveredby
our laser source could be monitored.We have selected some of them for the determination of Roo
(namely
those which present thelargest amplitude),
some others to check the limit of theexpérimental
linewidth we can observewith this apparatus and
finally
some transitions with n = 20. Thesehigh
n transitions, which werenot accessible in our
previous experiment [9],
have been now observed because in the new beam apparatus the residual stray fields have beendrastically
reduced. We have in fact used the n = 20transitions to estimate an upper limit for the Stark effect due to
parasitic
electric fields.7table I. - Observed transitions and
signal amplitudes (percentage
decreaseof the
metastablebeam).
Fig. 7. - Typical two-photon transition signal, recorded as a decrease of the metastable beam intensity (example of the