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Excitation mechanisms for hydrogen atoms in strong microwave fields
H. Breuer, M. Holthaus
To cite this version:
H. Breuer, M. Holthaus. Excitation mechanisms for hydrogen atoms in strong microwave fields.
Journal de Physique II, EDP Sciences, 1991, 1 (4), pp.437-449. �10.1051/jp2:1991178�. �jpa-00247528�
Classification
Physics
Abstracts42 50 32.80K 03 658
Excitation mechanisms for hydrogen atoms in strong
microwave fields
H. P Breuer and M. Holthaus
Physikahsches
Institut der Universitat Bonn, Nussallee 12, D-5300 Bonn I,Gerrnany
(Received
5September1990,
revised 27 December1990,accepted
ii January1991)
Abstract. We
analyse
the excitation mechanisms which determine thedynamics
ofhighly
excited
hydrogen
atoms traversing awavegulde.
Experimental measurements toverify predictions
denved from Floquet
theory
aresuggested.
1. Introduction.
Rydberg
atomsexposed
toshort,
strong microwavepulses [1-4] provide
aparticularly
attractive
possibility
tostudy
short-timephenomena
m quantum mechanics. In suchexpenments
theamplitude
of the microwave field can beadjusted
to be of the same order ofmagnitude
as the Coulomb fieldbinding
theelectron, therefore,
a major theoretical task is thedevelopment
of new,non-perturbative
methods On theexpenmental
side essential datarequired
for athorough
companson of theoreticalpredictions
andexpenmental
results suchas
length
andshape
of thepulse
can be determined withgreat
precision.Thus,
there is a uniqueopportunity
to unravel the mechanismsgoveming
thequantum dynamics
ofsystems
mstrong penodic
fields ;insights gained
from ananalysis
of the microwaveproblem
should also throwlight
on the s1mllarproblem
of atomsinteracting
with strong laserpulses
In a recent work
[5],
we haveapplied
theFloquet
picture to thedescription
of microwaveionization
expenments performed
athigh
scaledfrequencies n~
w m I_ using cavities[2]
: an atom expenences, whenentering
the cavity, aslowly nsing
field which leads to diabatic-adiabatic motion on
coarse-grained
quasienergy surfaces such that the state thatfinally
ends up m the cavity is asuperposition
ofFloquet
states. The results of the ionizationexpenments
performed
in thecavity
are determinedby
theamplitudes
of theseFloquet
stateswhich,
mturn, refldct both the structure of the
underlying
quasienergy spectrum and theshape
of thefringe
field[5].
The concept of adiabatic motion is, of course, of central
importance
m many areas ofphysics.
For instance, within the framework of theBorn-Oppenheimer theory
m molecularphysics
one encounters adiabatic evolution on energy surfaces at avoidedcrossings
of energy levels Landau-Zener transitions occur. Forpenodically time-dependint
quantum systemssuch as atoms in strong laser fields or
Rydberg
atoms m microwavefields,
there is adiabaticevolution of
Floquet
states onquasienergy
surfaces[5, 6].
Now animportant
new point appears : The quasienergy spectrum isorganized
m Bnllouin zones This fact leads to avoidedJOURNAL DE PHYSIQUE II T I,M 4, AVRIL (W( 20
crossings
ofquasienergies corresponding
to «distant» states, Landau-Zener transitions amongFloquet
states,therefore,
open thepossibility
ofexciting high lying
states withlarge probability. Thus,
in the case ofRydberg
atomsinteracting
with apulsed
microwave field there is avanety
of processes which are inducedby
thepulse shape,
I-e-by
theparameter
motion and the
resulting
adiabatic or diabatic evolution of the wave function.Obviously
such effects can not be understoodby
anapproach [7]
whichsimply
assumes atemporally
constantmicrowave
amplitude.
In the present paper we will discuss the
question
whichexperimental signatures
detectablem
present-day experiments
can beemployed
for anunambiguous
test ofpredictions
denved from theFloquet theory.
Wewill, therefore, analyse
aparadigmatic type
ofexperiment
: weassume a beam of
fast,
excitedhydrogen
atoms to traverse arectangular waveguide operated
m the
TEjo
modethus,
theenvelope
of the microwavepulse
«seen»by
the atoms is assumed to be half a sine wave, modifiedby
the presence of the entrance holes in thewaveguide.
Whereas m
cavity expenments
thepulse shape
has a « flat top », in the situation consideredby
us theamplitude
vanesduring
the whole interaction time and it should be clearimmediately
thatexpenmental
results obtained with both types ofexperimental
set-up can differsignificantly
eventhough
the maximalamplitude
and thefrequency employed
may be the same.We will
proceed
in twosteps
: in thefollowing chapter
wepresent
model calculations which illustrate the excitation mechanisms for thetype
ofexperiment
under consideration. Seen in amore
general
context, these calculations serve to establish the fact that adiabatic motion on quasienergy surfaces is of central importance for thedynamics
ofpenodically
dnven quantum systems. We then turn to thequestion
ofexpenmental
consequences andsuggest
measure-ments which could serve as a test of the
viability
of theFloquet
picture.2. Excitation mechanisms for atoms in microwave fields.
For our
niodel
calculations we use the(I
+ I)-dimensional
Hamlltonlan H=
Ho
+ H,~~(2.1)
describing
a « I-dimensionalhydrogen
atom »~
-~,
x>0Ho "jP
+ ~(2.2)
~~' ~'°
interacting
with alinearly polanzed
microwave field H,~~ = A(t)
x sin w t,
(2.3)
where(t) deiotes
thetime-dependent amplitude
of the field and w= 2 w
IT
itsfrequency.
We denote
stationary eigenstates
ofHo by w~(x),
nbeing
theprincipal
quantumnumber,
and theFloquet
states of the full Hamiltonian(2.I) by u~(x, t)
with quasienergy e~.Actual
experiments
done withreal,
three-dimensionalhydrogen
atoms are oftenperformed
m the
jresence
of a static electric field. The effect of such a field is obvious : the quasienergy Hamlltonlan of the three-dimensionalhydrogen
atom m a microwave field of constantamplitude
is invariant withrespect
to thesymmetry operatioq
lx-
-xS
=
T
(2.4)
~
~2'
this
symmetry
is brokenby
an additional static field. As is wellknown, symmetry
is essentialm the
theory
of levelcrossing
; the static field thus notonly
leads to a distortion of thequasienergy
surfaces but also to the appearance of further avoided crossings ofquasienergles.
In the one-dimensional
model,
the situation is different : onecould,
of course, include a termsimulating
a static field ofstrength
A~ in the model(2.I)
and writeH~=Ho+Axsinwt-A~x. (2.5)
However,
the(I
+ I)-dimensional
quasienergy Hamiltonian islacking
the symmetry S evenwithout the term A~ x.
Therefore,
this term does now notgive
rise to newanticrossmgs
in thequasienergy
spectrum butonly
to a Stark-shift of the individual levels.Furthermore,
thebasic mechanisms we want to illustrate
effectively
adiabatic evolution on smoothquasienergy
surfaces,
Landau-Zener transitions at reactive avoidedcrossings
remain unaltered. In order tokeep
the model assimple
aspossible
we thereforedrop
the termA~ x end
employ
the the Hamiltonian(2,I)
for our numericalanalysis
All calculations are
performed
m a basis of101 bound states ofHo (n~~=40,
n~~~=140).
We firstcompute
thequasienergy spectra
for three differentfrequencies w/2
w =13,00 GHz(Fig,1),
15.51GHz(Fig. 2)
and 18.00 GHz(Fig. 3).
Whendisplaying
quasienergles
graphically,
a technicaldifficulty
occurs : aquasienergy
e~actually
is a class(e~:
=
e~+mw)meZ)
E/W
1'
,
,
', , l
j ' '
'
fl
/ f
/
/
,'
, '
71 ?
,
~i
i i ii
I iiliii
Fig
I.- Part of thequasienergy
spectrum forw/2
w =1300GHzQuasienergles
are labelledby
pnncipal quantum numberscorresponding
to the static Hamlltonian Ho-E/W
'
'
i i 11
[(Iii]
Fig
2. Part of the quasienergy spectrum for w/2 w=
15 51GHz
of
physically equivalent representatives
e~, the first Bnllouin zonee I
~i~w ~i'
hence,
contains onerepresentative
of every class. Anattempt
todisplay
all levels contained inone Brillouin zone would
obviously
result in a blackpicture,
no structures would berecognizable.
One therefore has to select from all the levels certaindynamically
relevantones. We do this
by plotting only
thosequasienergies
for which thecorresponding Floquet
states are concentrated m a certain
subspace
of the full Hilbert space. Forfigures
I and2,
thissubspace
isspanned by eigenfunctions (w~s,.., wgs)
of thetime-independent
system(2.2),
forfigure
3by (w~o,.., wgo). Thus,
avanishing
line in thequasienergy
spectrasimply
indicates that theFloquet
state ismainly
contained in a differentsubspace
of the Hilbert spaceThe approximation
actually implicit
m our calculation is that weneglect
theimaginary
part of thequasienergles
which determines thedecay properties
of theFloquet
states[5].
However,
since the aim of thepresent
paper is toinvestigate
excitationmechanisms,
we will in thefollowing part only
considerexamples
withparameters
well below the ionization border.For the
frequencies
considered infigures
1, 2 and3,
the levels closest to the main resonancen~
w = I are n=
80,
75 and-72, respectively.
In all three cases we observe the samestrong
e/w
i
i
I liii
ig
3
deformation of the group of levels
adjacent
to the resonant one, the resonant level itself exhibitslarge
avoidedcrossings only
forcomparatively high
fieldstrengths
and thus enablespurely
adiabatic motion even forrelatively large amplitudes.
This fact leads to aquantum
mechanicalexplanation [5]
of the localstability
atn~
w =
I observed in actual expenments 121.
In the
following
we will use thesespectra
toexplain
the behaviour of solutions of the time-dependent Schr6dmger equation
Hw(t)
=
I
ojw(t) (2.6)
In order to model the
pulse shape
seenby
atoms traversing awaveguiie
we choose(t)
= ~~~ sin
I
,
0 « t « t
~,
(2.7)
t~
where t~ denotes the interaction time. As initial states at t = 0 we take the
eigenstates
w~~ ofHo.
As our calculations
show, basically
three different mechanismsgoveming
the short-time behaviour have to bedistinguished
: adiabatic motion(a),
Landau-Zener transitions(b)
andtransitions due to near
degeneracies
atvanishing
fieldstrength (c).
a)
To give anexample
for adiabatic motion we choose no =72, w/2
w=13.00GHz,
t~ = 98T, A~~
= 3 44
V/cm (in
atomic units, the scaledparameters
are :n(A~~~
=
0.018,
n(
w =0.737).
Wedecompose
theSchr6dmger
wave functionevolving
from the initial state w~~ with respect to theeigenstates
w~ ofHo
#(X, t)
"
£ c~(t) q~~(x) (2.8)
at time t =
t~/2,
when the maximal fieldamplitude
is reached(Fig. 4),
and at t = t~, i-e- at the end of thepulse (Fig. 5). Although
several states w, are excited m the middle of thepulse,
after the
pulse practically
allprobability
is again concentrated on the initial state. Theexplanation
for this non-diffusive behaviour is obvious from the quasienergyspectrum
infigure
I : since the quasienergy surface e~~ is smooth in the relevant interval of fieldstrength,
i-e- does not show any reactive avoided crossing
[5],
we conclude that the time evolution isalmost adiabatic. This means that the wave function #iis descnbed
by
asingle Floquet
state u~~ at every instant of time.Thus,
from thepoint
of view ofFloquet theory only
asingle
state is excitedduring
the whole process ; this state «moves»adiabatically
on its quasienergysurface e~~ in response to the
continuously changing amplitude. However,
the naivedecomposition (2.8)
for t=
t~/2
obscures thissimple
behaviour.b)
We now take w~~ as 1nltial state,w/2w=15.51GHz, A~~~=4.0V/cm
[n( A~~
=
0.021, n(
w =
0.880
]. Again
wedecompose
the wave functionaccording
to(2.8)
after the
pulse,
this time,however,
weplot
the coefficients [c~ [~ as functions of thepulse
N N
ii ii i~ ~~
jrincqil juinluR
nuRlerjriniijil juinluR
nuRlerFig
4Fig
5Fig.
4Decomposition
with respect to static states (28)
of the wave function which evolves from the initial state p~~ under the influence of thepulse (2.3), (2.7)
for w/2 WI 13.00 GHz,A~~
=
3 44
V/cm,
t~ = 98 T,
the
decomposition
has beenperformed
at i = t~/2 when the maximalamplitude
was reached This wave function is an almost pureFloquet
stateFig.
5.Decompos1tlon
of the wavefunctionevolving
from p72 after thepulse
at t = t~, the parameters used are the same as infigure
4.e/tv
~
r
i.,_
~
-.~,-.r ,-,----.-~
j
II
_~ ~~~_
ii iii iii i i i 1
l~ii i tin&i
Fig
6Fig.
7.Fig.
6Occupatlon probabilities
of the bound states n= 72 (upper full line), 78 (lower full
line),
79(larger dashes)
and 84(short dashes)
after the pulse as a function of thepulse length
t~ in units of T= 2grim
The initial state was no = 72; final states other than the onesdisplayed
are of minorimportance The parameters are
w/2
w = 15 51 GHz, A~~ = 4 00V/cm
Fig
7 Part of the quasienergy spectrum relevant for thedynamics
of the initial state no =72 at
w/2
w = 15 51GHz(cf. Fig. 6),
thestraight
lines indicate Landau-Zener transitionslength
t~. Theresulting pattem (Fig. 6)
has a clearexplanation
from thequasienergy spectrum
infigure
7: the initial state no = 72 is shifted into the connectedFloquet
state u72 andundergoes
two Landau-Zener transitions to u~g and u~~during
the nse of thefield,
when theamplitude
decreases again interferences occurleading
toStfickelberg
oscillations visible m the excitationprobabilities
of the final states. In order to observe these oscillationsexpenmentally
one has to vary the interaction time t~, which up to now has not been done m a
systematic
manner.
c)
As anexample
for the third mechanism we take no=72, w/2w =18.00GHz,
A~~~ = 6.5V/cm [n(
A~~~ =
0.034, n(
w= 1.021 and
display
infigure 8a), o
theexcitation
probabilities [c~[~
of the final bound states as functions of t~ The intncate oscillationpattems
can be understood from theunderlying quasienergy spectrum (Fig. 3).
Now the initial state is very close to resonance, i-e- several quasienergles are
nearly degenerate
in the Brillouin-zone at A=
0 This near
degeneracy
israpidly
removed forincreasing amplitude. Thus, right
at thebeginning
of thepulse
the 1nltial state is distnbutedover several
Floquet
states which thendecouple
and evolve on their ownquasienergy
surface.At the end of the
pulse
theFloquet
statescouple
again when A =0 and theresulting
interference
pattem
is determinedby
thedynamical phases
eachFloquet
state hasaccumulated.
,
N N
i
u u
i i
iii iii i~~ iii
t~ii
iia)
)
Fig
8aOccupatlon probability
of the final bound state n = 69 after thepulse,
the initial state wasno = 72 Parameters w/2 w = 18.00 GHz, A~~~
= 6 5 V/cm
Fig 8b As
figure
8a for the final state n=
70.
m N
- N
~ ~
U
iii iii iii iii
ii
t~li
~) d)
Fig.
8c Asfigure
8a for the final state n=
71.
Fig
8d Asfigure
8a for the final state n = 72N N
I /
u u
i i
iii iii iii iii
t~li i~li
e)
o
Fig
8e. Asfigure
8a for the final state n= 73
Fig 8f As
figure
8a for the final state n = 74We finish this section with two remarks
conceming
theimportant
differences between mechanismb)
andc)
The transitions m
b)
are due to avoided crossings at A » 0 whichcouple
statesdiffering by
several units in
pnncipal
quantum number in ourexample
we had transitions 72=
78,
79corresponding
to an energy difference of 6.05 Am and 6.93Am, respectively.
In contrast, thenear
degeneracy
at= 0 m
c) perturbatively couples
states which are the nearestneighbours
of the initial one.
Secondly
we note that mechanismc) depends
verysensitively
on the way the field is tumedon and off. We have checked this
by smoothing
the sinusoidalamplitude (2.7)
at theedges
such that an
exponential
function is fittedcontinuously
differentiable at times ti and t~ti(ti
«t~)
of theoriginal pulse.
Twoexamples
for the influence of this modification aregiven m
figures
9 and lo(ti
=
3 T and ti = 5
T).
Thisdependence
on details of thepulse shape
is notsurpnsing
since thepulse
is modifiedexactly
when theFloquet
statesinteract,
I-e-near A
= 0. In contrast, as we have checked the same modification is of
negligible
influence fora)
andb).
3.
Experimental hnpficafions.
We saw m the previous
chapter
that theFloquet
representation offers a very convenient and efficient tool toanalyse
thedynamics
of atoms mpulsed
fields A process that appears to becomplicated
m theeigenbasis
ofHo
can be verysimple
whenanalysed
m theFloquet basis,
our mechanisma) being
aconvincing example
for this fact. As a measure of thecomplexity
of a processduring
the interaction we define the quantityS(t)
=£
p~ In p~(3.1)
N N
» »
u u
ii ii ii ii
jriniijil juiflluR
fluRlerjriniijil juifltuR
nuRlerFig
9Fig
loFig.
9.Occupation probabilities
of final bound states after apulse
whichslightly
differs from(2 7)
the
edges
of thepulse
have been smoothed such that at t = tr and t= t~ tr an
exponential
function has been fittedcontinuously
differentiable to theonglnal amplitude
For thisfigure,
tr= 3T and t~ = 135 T, the other parameters are as infigure
8.Fig
lo Asfigure
9, however tr = 5 Twhere
p, m
p,(t)
=
jut
(t)ipi 12, (3 2)
#i is the
Schrbdinger
wave function and the u~~~'~ denote theFloquet
statescorresponding
tothe instantaneous field
strength A(t). Compared
to the «Shannon entropy»recently
considered
by
Casati et al.[8]
to characterize localizationproperties
ofeigenfunctions,
thecomplexity (31)
is a measure of the dimension of the space of effectiveFloquet
states involved m thedynamics.
For apurely
adiabatic processS(t) stays
constant and increases when non-adiabaticphenomena
occur, e-g- when the wave functionsplits
» due to Landau- Zener transitions ifonly
asingle Floquet
state is excited in apurely
adiabatic process(mechanism a) S(t)
remainsidentically
zero. This factagain nicely
illustrates that thestationary Floquet
statesprovide
the appropnate basis for adescription
of thedynamics
:if in the definition
(3.2)
of theprobabilities p~(t)
theFloquet
states u~ werereplaced by
staticeigenstates
wi one would obtain themisleading
result that thecomplexity
of an adiabatic process growsduring
the rise of thepulse
and then decreases to itsonginal
value. As astnking example
for this we show mfigures I1,
12 a static statedecomposition
of the wave function for anadiabatic
process. Eventhough
the initial static state is almostcompletely depopulated
in the middle of thepulse
this process isadiabatic,
i-e- the above definedcomplexity
remainszero for the whole
pulse.
The
observables
m actual excitation expenmentsperformed
withwaveguides
are theoccupation probabilities
of the final static bound states wi after the interaction with theN N
/
i/
ii 11 ~~ ii i~ ii
jrifliipil juifltuR
hunterjriflcijil juifltun
fluRlerFig,
I IFig
12Fig I I.
Decomposition
of the wave function which has evolved from the initial state no =66 in the middle of the
pulse
,
w/2
v=
18.00 GHz, A
~~ =
60
V/cm,
t~=
136 T. Note that the initial static state seems to be
«
depopulated
Fig.
12Decomposition
of the wave function considered infigure
II after thepulse
microwave field and the
challenge
now is to detect clear evidence for the above descnbedexcitation mechanisms. Of course one faces several difficulties
expenmental
results may bemodified
by
the presence of noise[4]
and an accurate final bound stateanalysis
iscomplicated
because of thehigh degeneracy
in realhydrogen
atoms The latterproblem
couldpartially
becircumvented
by working
with helium[9]
or alkali[3, 4]
atoms m order to lift thef- degeneracy
or, as a differentpossibility, by superimposing
a static electnc field to achieve quasione-dimensionahty. Despite
thesecomplications,
we believe thatskilfully performed experiments
canunambigously identify
the basic mechanisms. To this end wesuggest
thefollowing
measurements :I)
The interaction time t~ can be variedby changing
thevelocity
of the atom beamLandau-Zener transition
probabilities during
thepulse
dodepend
on t~ and determine the final bound state distnbution.Thus,
measuring the [c~ [~ as functions of t~yields important
information about transitions occurnngduring
thepulse.
Inparticular, waveguide
exper-iments are
ideally
suited for a detection ofStfickelberg
oscillations : if thelength
of the wholepulse
isadjusted
to be of the order ofonly
loocycles
of the externalfield,
thedynamical
phases acquired by
theinterfering Floquet
states can beprevented
from growing toolarge
; m contrast, the flat top of thepulse
mcavity
expenments[2]
lastslonger
than 300cycles
and thus induceslarge phases
and acorrespondingly sharper
interference pattern which is harder to resolve. In order to resolveSt0ckelberg
oscillations asdepicted
mfigure
6 in suchwaveguide
expenments,
the necessary range of velocities translates into a variation of the proton accelerationvoltage
over a range of some 10 kev.448 JOURNAL DE
PHYSIQUE
II M 42)
The holesby
which the atoms enter and leave thewaveguide modify
thepulse shape
near t = 0 and t
= t~ such that the actual
envelope
obtainslong
tails. It is well known[10]
that smoothness conditions at theedges
of thepulse
are essential for adiabatic behaviour ;indeed,
as our calculations have
shown,
for near resonant 1nltial conditions(mechanism c)
the [c~ [~(t~)
can be influencedby shape
andmagnitude
of theholes,
whereas m casea)
andb)
properties of the holes haveonly
anegligible
effect.Hence, repeating
the expenmentsusing waveguides
withdifferently shaped
holeswill,
mgeneral, yield
identicalresults, however,
for certain initial states theexpenmental signal
will be charactenstic for themicroscopic
structure of the holes of theparticular apparatus employed.
3)
In order toinvestigate pulse-shape dependencies
it would be veryinteresting
tooperate
thewaveguide
mhigher modes,
e-g- m theTE~O-mode
which leads to a doublepulse
theFloquet
states involved thus interfere several timesduring
the interaction which maydrastically
alter the final bound state distribution.Of
particular importance
is anexpenmental
verification of mechanismb),
i-e- an excitation of bound statesconsiderably higher
than the initial one inducedby
Landau-Zener transitions at broad avoidedcrossings.
The very samephenomenon
occurnng for atoms irradiatedby
short
strong
laserpulses explains
trans1tlonsrequiring
an excitation energy of several Am.We would like to remark that m actual
expenments performed
in the presence of a static electric field there is an additionalpossibility
ofcontrolling
thesystem:
The «scaledfrequency (that
is, the ratio of the microwavefrequency
and theangular velocity
of thecorresponding
classical system forvanishing
microwaveamplitude)
is then nolonger given by n(
w but rather becomes a function of thestrength
of the static field ;furthermore,
thestructure of the Bnllouin zone at A
=
0 will be determined
by
theenergies
of the Stark states.Thus,
it is aninteresting
question whether it ispossible
to observedynamical
behavlourgovemed by
different mechanisms whenchanging
thestrength
of the static field.Summarizing,
we havetheoretically
discussed microwave excitation expenments onhighly
excited
hydrogen
atoms which are characterizedby
a continuouschange
of theamplitude during
the interaction time. As we havepointed
out, such atime-dependence
of the fieldstrength
makes the use of adiabatic methodsindispensable
for atransparent descnption.
We conclude thatwaveguide experiments
could serve as astnngent
test forFloquet dynamics
when the final bound state distribution is measured as a function of
pulse-shape parameters.
In this way, microwave expenments could
yield important insights
into short-timephenomena
m
strongly interacting
quantum systems.Acknowledgment.
Ii
is apleasure
to thank Professor K. Dietz for fruitfuldiscujsions
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