Eur. Phys. J.

D 22, 401–415 (2003)

DOI: 10.1140/epjd/e2003-00017-9 THE EUROPEAN
PHYSICAL JOURNAL D

Nondispersive two-electron wave packets in driven helium

P. Schlagheck1 and A. Buchleitner2,a
1
Institut für Theoretische Physik, Universität Regensburg, 93040 Regensburg, Germany
2
Max-Planck-Institut für Physik komplexer Systeme, Nöthnitzer Str. 38, 01187 Dresden, Germany

Received 7 November 2002 / Received in final form 2 December 2002

Published online 28 January 2003 –

c EDP Sciences, Società Italiana di Fisica, Springer-Verlag 2003

Abstract. We provide a detailed quantum treatment of the spectral characteristics and of the dynamics of
nondispersive two-electron wave packets along the periodically driven, collinear frozen planet configuration
of helium. These highly correlated, long-lived wave packets arise as a quantum manifestation of regular
islands in a mixed classical phase space, which are induced by nonlinear resonances between the external
driving and the unperturbed dynamics of the frozen-planet configuration. Particular emphasis is given to
the dependence of the ionization rates of the wave packet states on the driving field parameters and on
the quantum mechanical phase space resolution, preceded by a comparison of 1D and 3D life times of
the unperturbed frozen planet. Furthermore, we study the effect of a superimposed static electric field
component, which, on the grounds of classical considerations, is expected to stabilize the real 3D dynamics
against large (and possibly ionizing) deviations from collinearity.

PACS. 32.80.Rm Multiphoton ionization and excitation to highly excited states (e.g., Rydberg states) –
05.45.Mt Semiclassical chaos (“quantum chaos”) – 31.25.Jf Electron correlation calculations for atoms
and ions: excited states

1 Introduction liptic polarization [11]. There, a Rydberg wave packet, ini-

tially launched along a Kepler orbit with principal quan-
As documented by an increasing amount of literature, tum number n, is exposed to a microwave field which
electronic wave packets represent an important object is resonant with the periodic classical motion. Then, for
of experimental studies in atomic and molecular physics appropriate field amplitudes (which must neither be too
(e.g., [1,2]). The possibility to localize the electronic pop- strong nor too weak, compared to the Coulomb force
ulation in phase space can be regarded as the crucial link on the electron) and for the appropriate relative phase
between a quantum wavefunction and a classical point between the microwave field and the Kepler oscillation,
particle [3], and has led to various applications in the con- the spreading of the wave packet (which usually occurs
text of quantum control (e.g., [4,5]). For a long time, it after approx. n/[3π(∆n)2 ] Kepler cycles, given a coher-
was common belief that the maximum evolution time un- ent superposition of ∆n unperturbed eigenstates centered
til which such a localized phase space distribution can be around n) is completely inhibited. While perfectly keeping
maintained is ultimately limited by the time scale corre- their shape, such nondispersive wave packets may well fol-
sponding to the anharmonicity of the underlying classical low the classical motion over time scales up to 106 Kepler
potential. After this time scale, any coherent superposition cycles [6,8,10,12] before appreciable ionization (induced
which was initially well localized in position and momen- by the driving field) sets in [6,8,13]. This stabilization
tum space would have spread out over the whole classical phenomenon is best understood from the underlying clas-
orbit due to dispersion, i.e., due to the fact that different sical dynamics. In classical phase space, the time-periodic
components of the superposition contribute with different perturbation of the microwave destroys the global integra-
classical frequencies. This is usually termed as the collapse bility of the Coulomb dynamics; local “islands” of regular
of the wave packet. motion, embedded into a “sea” of chaotic, ionizing dy-
A decade ago, however, it was found that this spread- namics, are created by the nonlinear resonance between
ing can actually be suppressed by means which are the driving field and the unperturbed Kepler motion. The
common in quantum control, namely by applying electro- nondispersive quantum wave packets are nothing but the
magnetic fields to the quantum configuration. This was time-periodic eigenstates (Floquet states) of the driven
explicitly demonstrated for one-electron atoms driven by atom, which arise from a local quantization within these
microwave fields with linear [6–8], circular [9,10], and el- resonance islands [14,15] (see [16] for a recent review on
a
the topic).
e-mail: [email protected]
402 The European Physical Journal D

The above interpretation in terms of nonlinear reso- the quantum dynamics along this axis. Indeed, nondisper-
nances in a mixed phase space suggests that the concept of sive two-electron wave packets associated with the classi-
nondispersive wave packets can be generalized to atomic cal resonances are found in quantum calculations on the
(or molecular) systems that are more complex than hy- collinear model atom, as we have already reported in a
drogen or hydrogen-like Rydberg atoms – such as, e.g., previous letter [24]. Here we shall give detailed account of
the correlated dynamics in doubly excited helium. How- our quantum treatment of these objects, identify them as
ever, such a generalization is not at all obvious, since most special eigenstates in the Floquet spectrum of the driven
doubly excited two-electron orbits of the bare three-body atomic system (alike their counterparts in driven hydrogen
Coulomb problem (as the classical version of the doubly atoms), and investigate their characteristic properties.
excited helium atom) are unstable and promote rapid au- To make the present contribution self-contained, we
toionization of the configuration. This prevents the con- start out in Section 2 with a review of the classical dy-
finement of an initially localized wave packet on longer namics of the driven frozen-planet configuration, which
time scales. was already described elsewhere [20,21]. Section 3 is de-
Nonetheless, extensive studies on the classical dynam- voted to the formulation of the quantum eigenvalue prob-
ics of helium [17] have identified local regions of regu- lem for the collinear model. As a first application thereof,
lar motion which are associated with configurations of we study the unperturbed collinear atom in Section 4,
particular symmetry of the two-electron atom. The most what provides a remarkable example of regular dynamics
prominent and surprising example is the “frozen planet” in an atomic two-electron system. In Section 5, we show
orbit [18,19], a highly polarized, nearly collinear con- how the nondispersive wave packets emerge in the spec-
figuration with asymmetric excitations of the electrons. trum of driven helium (Sect. 5.1) and discuss their life-
The frozen planet’s stability essentially relies on the non- times (Sect. 5.2), as well as their properties in presence of
negligible electron-electron interaction (the electrons are, an additional static electric field (Sect. 5.3).
contrary to intuition, located on the same side of the
nucleus). Stable eigenmodes sustain radial, vibration-like
oscillations of the outer electron, as well as coupled trans- 2 Classical dynamics of the driven
verse excursions of the outer and inner electron. Well- frozen-planet configuration
defined eigenfrequencies are associated with these eigen-
modes, what makes the configuration a good candidate 2.1 The frozen-planet configuration of helium
for inducing nonspreading wave packets in the correlated
two-electron dynamics, by near-resonant external driving. In atomic units, which are used throughout this paper,
In fact, our earlier analysis of the classical dynamics of the classical Hamiltonian of the electromagnetically driven
helium in a linearly polarized electromagnetic field already helium atom reads
provided strong support for nondispersive wave packets p21 p2 Z Z 1
along the frozen-planet orbit [20,21]. The external per- H= + 2 − − +
2 2 |r1 | |r2 | |r1 − r2 |
turbation induces regular islands within the phase space
of collinear motion (where electrons and nucleus are lined + F(t) (r1 + r2 ), (1)
up parallel to the driving field polarization axis), which
with ri = (xi , yi , zi ) and pi = (pix , piy , piz ) the position
are due to nonlinear resonances between the drive and
and the momentum of electron i = 1, 2, respectively, Z = 2
the oscillation of the outer electron. The dynamics within
the nuclear charge, and
these resonances is in general unstable with respect to
deviations from collinearity (in contrast to the analogous F = (F cos ωt + Fst ) ez (2)
scenario in atomic hydrogen, the resonantly driven one
dimensional Kepler orbit [22]). However, a static electric the external, linearly polarized driving at frequency ω
field applied parallel to the microwave polarization axis and amplitude F , possibly superimposed by an additional,
can be used to enforce stability of the driven configura- static component with field strength Fst (ez represents the
tion in all three spatial dimensions [20]. This suggests that unit vector along the z-axis). In analogy to driven hydro-
nondispersive two-electron wave packets can be built on gen [25] as well as to the unperturbed helium atom [26],
these stabilized resonances, and, on the basis of semiclas- the Hamiltonian (1) exhibits general scaling laws: the clas-
sical considerations, at experimentally accessible quantum sical dynamics generated by (1) remain invariant if all
numbers of doubly excited helium [21,23]. Yet, this con- variables and parameters of the system are transformed
jecture remains to be corroborated by an exact quantum according to
treatment.
With the presently available computational facilities, ri
−→ N 2 ri (i = 1, 2), (3)
full blown quantum ab initio calculations of highly cor- pi
−→ N −1 pi (i = 1, 2),
related two-electron wave packet states under electromag- t
−→ N 3 t,
netic driving are prohibitive. However, since the stabilizing
F
−→ N −4 F,
static field confines the wave packet to the near vicinity
of the field polarization axis, essential properties of these ω
−→ N −3 ω,
wave packets appear accessible through the restriction of H
−→ N −2 H,
 P. Schlagheck and A. Buchleitner: Nondispersive two-electron wave packets in driven helium 403

Fig. 2. Collinear trajectory of the frozen-planet configuration.

Fig. 1. A typical (planar) trajectory of the frozen-planet The positions of the electrons are plotted as a function of time.
configuration. While the inner electron oscillates on eccentric We see that the dynamics is characterized by two almost sep-
Kepler trajectories around the nucleus, the outer electron is arable modes: (i) the Kepler mode of the inner electron, which
dynamically stabilized and remains nearly “frozen” around a also manifests in the motion of the outer electron, as shown in
given equilibrium distance. The configuration is stable against the magnification (b) of the latter’s trajectory; (ii) the slow os-
autoionization and represents a large regular region in the clas- cillation of the outer electron around the equilibrium distance,
sical phase space of helium. which induces a feeble (and, at this scale, hardly visible) mod-
ulation of the amplitude of the inner electron’s excursion.

where N represents an arbitrary, real positive quantity.

Since any classical action scales linearly with N (as does
the product of position and momentum), we shall iden-
tify N with the principal quantum number of the inner
-

electron, which corresponds to the action variable of its

Kepler orbit. Due to the above scale invariance, we can -

restrict our classical phase space analysis to a fixed quan-

tum number N = 1, and use (3) to deduce the actual
phase space structure of the energy range of interest.
Figure 1 shows a solution of the classical equations Fig. 3. Effective adiabatic potential describing the slow os-
of motion generated by (1), which illustrates the frozen cillation of the outer electron around its equilibrium position
planet configuration we shall focus on throughout this pa- (see [28]). Intrinsic scales for frequency and field strength can
per. Both electrons are located on the same side of the be inferred from the shape of the potential. The natural scale
nucleus, librating with respect to a common symmetry of the field strength, FI  0.03 N −4 , is given by the maximum
axis. While the inner electron oscillates on extremely ec- slope of the potential (at z1  3.7 N 2 ). The frequency scale,
centric Kepler trajectories around the nucleus, the outer ωI  0.3 N −3 , is given by the curvature of the potential at
electron is dynamically stabilized due to the rapid oscil- its minimum at z1  2.6 N 2 , i.e., by the frequency of small
lation of the inner, and remains nearly “frozen” in the oscillations around the equilibrium.
vicinity of an equilibrium distance where the attractive
and repulsive forces due to the other charged particles
cancel each other when averaged over one Kepler cycle of effective potential which describes the slow dynamics of
the inner electron. The configuration is classically stable the outer electron, in the combined field of the nucleus and
against autoionization and defines a relatively large region of the rapidly oscillating inner electron [28]. As we see in
of regular motion in the dominantly chaotic phase space of Figure 3, this potential is attractive Coulombic for large
helium. Exact quantum calculations on doubly excited he- distances (due to the attraction by the nucleus), strongly
lium [19] have indeed revealed the existence of long-lived repulsive for short distances (due to encounter with the
autoionizing states (of which the energetically lowest one inner electron) and exhibits a local minimum at the equi-
lies below the N = 3 threshold) which are localized along librium distance.
the frozen-planet orbit. From the shape of this potential, we can immedi-
For a suitable choice of initial conditions, the motion of ately infer intrinsic scales for the frequency and the field
the electrons remains confined to the z-axis, what defines strength, which depend only on the inner electron’s quan-
the subspace of collinear motion. In this simplest case, tum number N , and which completely determine the ef-
the regular frozen-planet dynamics is characterized by two fect of an external drive on the configuration. The nat-
modes which almost perfectly separate (Fig. 2): the fast ural scale for the field strength, FI  0.03 N −4 , is given
Kepler mode of the inner electron (which is also manifest by the maximum slope of the potential (at z1  3.7 N 2 ;
in the motion of the outer electron, see Fig. 2b) and the throughout the paper, subscript 1 denotes the outer, and
slow oscillation of the outer electron around the equilib- subscript 2 the inner electron), and indicates the maxi-
rium distance (which also affects the motion of the inner mum static field that can be applied to the configuration
electron, as a slow modulation of its maximal excursion). without ionizing it. The frequency scale ωI  0.3 N −3 is
This separation of time scales (the Kepler oscillation given by the curvature of the potential at its minimum,
is almost 15 times faster than the slow mode of the outer i.e., by the frequency of small oscillations around the equi-
electron) allows to treat the frozen-planet dynamics within librium position. In the following, we shall study the ef-
the formalism of adiabatic invariants [27]. This defines an fect of an electromagnetic field which resonantly drives
404 The European Physical Journal D

0.6
the outer electron’s slow oscillation, i.e., a field with am- a b c
plitude F < FI and frequency ω  ωI .

−1
pz1 / N
0

−0.6
0 5 0 5 0 5
2.2 Phase space of the collinear, driven configuration 2
z1 / N

In the presence of the time-periodic perturbation, the dy- Fig. 4. Phase space of the collinear, driven frozen-planet
namics of the collinear, driven frozen-planet evolves in a configuration, for variable field amplitudes, (a) F = 0,
five-dimensional phase space spanned by the positions and (b) 0.001 N −4 , (c) 0.005 N −4 , at fixed driving frequency ω =
momenta of the electrons, and by the phase ωt of the driv- 0.2 N −3 . The momentum pz1 of the outer electron is plotted
ing field. A complete visualization of the driven dynamics versus its position z1 at fixed action N = 1 of the Kepler
mode, fixed position z2 = 0 of the inner electron, and fixed
within a simple two-dimensional Poincaré surface of sec-
phase ωt = 0 (mod 2π) of the driving field [21, 23]. The regular
tion is therefore not possible. However, for ω  ωI , and for
phase space of the unperturbed atom (a) turns mixed regular-
field amplitudes F < FI which do not appreciably affect chaotic in presence of the external perturbation (b, c). The
the Kepler motion of the inner electron, the separation of nonlinear 1:1 resonance between the driving field and the un-
time scales allows to map the phase space structure onto a perturbed oscillation of the electron gives rise to a substructure
two-dimensional surface by means of a two-step Poincaré at F = 0.001 N −4 (b) (centered around z1  4.8 N 2 ), which
section method [21,23]. We begin with a simple Poincaré transforms into a separate regular island within the chaotic sea
section by plotting the outer electron’s phase space vari- at larger field amplitude F = 0.005 N −4 (c).
ables z1 , pz1 whenever the inner electron reaches the nu-
cleus (z2 = 0) – i.e., whenever the phase of the Kepler
oscillation assumes a fixed value. In the time domain, the
resonances between the external driving and the unper-
points obtained by this section are separated by the Kepler
turbed oscillation of the outer electron, emerge within
period which is much shorter than any other time scale in
the regular region. The prominent substructure located
the system. The dynamics generated by the slow modes
around z1  4.8 N 2 for F = 0.001 N −4 (Fig. 4b) corre-
– i.e., the outer electron’s oscillation within the effective
sponds to the 1:1 resonance where one oscillation cycle of
potential, as well as the external driving – is therefore very
the outer electron is completed after precisely one period
well monitored by this sequence of points.
of the driving field.
Neglecting the effect of resonances between fast and
slow dynamics, the intersection of the Lagrangian mani- At larger field amplitude (F  0.003 N −4 for the fre-
fold with the surface defined by z2 = 0 can now be very quency used in Fig. 4), the field-induced resonance even-
well approximated by a cubic interpolation between sub- tually disconnects from the rest of the regular domain.
sequent points in the above sequence. This yields a con- The phase space then exhibits two separate, large reg-
tinuous trajectory which can be used to perform a second ular islands embedded into the chaotic sea (see Fig. 4c
Poincaré section, by fixing the phase of the driving field at F = 0.005 N −4): the intrinsic island (centered around
ωt = φ0 (mod 2π). As a consequence, we effectively plot z1  2.5 N 2 in Fig. 4c) which is essentially due to the
the outer electron’s position and momentum for z2 = 0 intrinsic nonlinear frozen-planet dynamics with the ex-
and for fixed ωt. The reduction of the phase space to a ternal field acting only as a small perturbation, and the
two-dimensional surface is completed by restricting the field-induced 1:1 resonance island (centered around z1 
initial conditions to those with fixed value N = 1 of the 4.9 N 2 in Fig. 4c) which arises from the combination of two
inner electron’s action. This latter quantity represents an equally important nonlinear components: the coupling to
adiabatic invariant of the system and therefore remains the external driving field and the internal interactions be-
nearly constant as time evolves. tween the charged particles of the atom.
Figure 4 shows the Poincaré section that is obtained Figure 5 illustrates the effect of tuning the frequency
by the two-step method described above, for fixed fre- ω at fixed field amplitude F = 0.005 N −4. With increas-
quency ω = 0.2 N −3 < ωI , fixed driving phase ωt = 0, ing ω, the field-induced resonance shifts towards lower ex-
and for variable field amplitude F . In the unperturbed citations within the effective potential, i.e., towards un-
case (F = 0, Fig. 4a), we recognize a regular phase space perturbed orbits with higher frequencies. Consequently,
structure, with closed curves corresponding to the regu- the resonance island is located closer (as compared to
lar oscillation of the outer electron within the effective Fig. 4c) to the equilibrium distance for ω = 0.25 N −3
potential. If we switch on the driving field, phase space (Fig. 5a) and finally undergoes a smooth transition into
turns mixed regular-chaotic. The bounded frozen-planet the intrinsic island at ω = 0.3 N −3  ωI (Fig. 5b). Above
dynamics is now represented by a local regular region cen- the intrinsic frequency ωI – which corresponds to the max-
tered around the equilibrium point, outside which the dy- imum frequency of free oscillations within the effective po-
namics is chaotic and leads to ionization. This remaining tential – the electromagnetic field can no longer induce a
regular region is, due to the Kolmogorov-Arnold-Moser 1:1 resonance. Resonances of higher order, however, are
(KAM) theorem [27], still large for weak field amplitudes still possible (e.g., the 2:1 resonance, where one period of
(F = 0.001 N −4, Fig. 4b), but decreases in size with in- the outer electron is completed precisely after two field
creasing F . As a consequence of the Poincaré-Birkhoff cycles; the elliptic islands created by this resonance are
theorem [27], elliptic substructures, induced by nonlinear located at z1  4 N 2 and pz1  ±0.2 N −1 in Fig. 5c).
 P. Schlagheck and A. Buchleitner: Nondispersive two-electron wave packets in driven helium 405

0.6
a b c
−1
pz1 / N

−0.6
0 5 0 5 0 5
2
z1 / N

Fig. 5. Phase space of the collinear, driven frozen planet con-

figuration for variable driving frequency, (a) ω = 0.25 N −3 ,
(b) 0.3 N −3 , (c) 0.4 N −3 , at fixed amplitude F = 0.005 N −4 Fig. 7. Unstable trajectory of the driven frozen-planet con-
and phase ωt = 0 of the drive. With increasing ω, the 1:1 res- figuration in two-dimensional configuration space. The con-
onance island (centered around z1  3.9 N 2 in (a)) shifts to- figuration is initially launched at the center of the collinear
wards the equilibrium distance, and finally undergoes a smooth 1:1 resonance island for ω = 0.25 N −3 and F = 0.005 N −4 (see
transition into the intrinsic island at ω = ωI = 0.3 N −3 (b). Fig. 5a), except for a small transverse component y1 = 0.01 N 2
The two islands at z1  4 N 2 , pz1  ±0.2 N −1 for ω = 0.4 N −3 of the outer electron’s position. The resulting time evolution
(c) are induced by the 2:1 resonance where one period of the of the trajectory is depicted from 0 to 15 field cycles in (a),
outer electron’s motion matches two field cycles. from 15 to 30 field cycles in (b), and from 75 to 91 field cy-
cles in (c). We see that the initially small deviation of the
configuration from the z-axis increases with time, until, after
approx. 10 field cycles, both electrons flip over to the other
side of the nucleus (a). The configuration then performs sev-
eral chaotic rotations around the nucleus (b), before the cor-
relation between the electrons eventually breaks down and the
atom ionizes (here at about 90 field cycles) (c).
Fig. 6. Phase space of the collinear, driven configuration for
variable phases of the driving field, (a) ωt = 0, (b) π/2,
(c) π, at fixed frequency ω = 0.2 N −3 and field amplitude eral chaotic rotations around the center, until the correla-
F = 0.005. While the intrinsic island remains basically at rest tion between the electrons eventually breaks down and the
during time evolution, the field-induced 1:1 resonance island atom ionizes after a subsequent electron-electron collision.
faithfully traces the resonantly driven trajectory of the outer This transverse instability turns out to be characteristic
electron. not only for the 1:1 resonance, but also for the intrinsic
island, as well as for the 2:1 and for higher resonances (ex-
ceptions are tiny resonances of higher order, such as the
The crucial qualitative difference between the intrinsic 3:2 resonance, see [21,23]). To launch nondispersive wave
island and the field-induced resonances is best illustrated packets along the frozen-planet orbit of the real three-
by visualizing the phase space structure for different times, dimensional atom, an additional perturbation of the atom
i.e., by performing the above two-step Poincaré section for is therefore required, in order to stabilize the electronic
different phases ωt of the driving field. Figure 6 shows the motion with respect to deviations from collinearity.
phase space of the driven configuration at ω = 0.2 N −3 , In fact, such a stabilization can be achieved by adding
F = 0.005 N −4, for the field phases ωt = 0, π/2, and π. a static component Fst to the electromagnetic field (see
We see that the intrinsic island remains basically at rest Eq. (2)). In resonantly driven hydrogen, a static field, ap-
during the time evolution. The field-induced 1:1 resonance plied parallel to the microwave polarization axis and forc-
island, on the other hand, oscillates once around the in- ing the electron away from the nucleus, tends to confine
trinsic island within one field cycle. the electron to the immediate vicinity of the polarization
axis [16,22,30]. This confinement effect can now be im-
ported to stabilize the motion of the driven frozen-planet
2.3 Stabilization against deviations from collinearity – by preventing the configuration from chaotic rotations.
Indeed, for weak static fields, Fst  0.1F , and for not
In contrast to their counterparts in driven hydro- too strong driving amplitudes F (e.g., F = 0.005 N −4 at
gen [16,29], however, the resonance islands of the collinear, ω = 0.25 N −3, see Fig. 8), small deviations from collinear-
driven frozen-planet dynamics are not embedded in a regu- ity do not lead to ionization. Instead of drifting away to
lar phase space domain of the three-dimensional problem. the other side of the nucleus (as in the absence of the static
Figure 7 shows the evolution of the configuration launched field, Fig. 8a), the electrons are forced back towards the
at the center of the 1:1 resonance island of Figure 5a (i.e., field polarization axis (Fig. 8b), and the configuration per-
for ω = 0.25 N −3 and F = 0.005 N −4) if the outer electron forms stable, quasi-periodic oscillations around the funda-
is slightly displaced from collinearity by a small transverse mental orbit shown in Figure 8c.
component y1 = 0.01 N 2 of its position. Due to the effec- This stabilization mechanism permits to embed the
tive torque exerted by the driving field on the configura- nonlinear resonances into regular regions within the un-
tion, the initially small deviation from the field polariza- restricted phase space of three-dimensional motion, while
tion axis increases rapidly with time, until, after about the electronic dynamics within the collinear subspace is
ten field cycles, both electrons “flip over” to the other only marginally modified by the weak static field. We
side of the nucleus. The configuration then performs sev- find that this multidimensional phase space region is
406 The European Physical Journal D

correlated states under external driving is still beyond

reach of the presently available computational facilities.
For unperturbed helium, where the total angular momen-
tum is conserved, autoionizing states can presently be cal-
culated for quantum numbers of the inner electron reach-
ing N  15 . . . 20 [19,37]. Therefore, in the near future
Fig. 8. Stabilization of the transverse frozen planet dynamics there is not much hope for an accurate treatment of the
at ω = 0.25 N −3 and F = 0.005 N −4 . As in Figure 7, the periodically driven problem, with a large number of angu-
configuration is initially launched at the center of the collinear lar momenta coupled by the field, at comparable or even
1:1 resonance island, except for a small transverse component higher excitations.
y1 = 0.01 N 2 of the outer electron’s position. Without the Nevertheless, essential qualitative information on the
static field (a), the electrons drift away from the z-axis and wave packets can be obtained by an approximate quan-
enter into chaotic rotations around the nucleus. A static electric tum description, which is motivated by the classical mo-
field, Fst = 0.1F , along the z-axis, directed such as to force tion of the electrons. As discussed in the previous section,
the electrons into the positive z-direction, counterbalances this the static field confines the electrons to the vicinity of the
drift mechanism (b); the electrons are driven back towards the
field polarization axis (Fig. 8), without major modifica-
z-axis, and the configuration performs stable, quasi-periodic
tions of the dynamics in the collinear subspace. Hence,
oscillations around the fundamental orbit shown in (c).
also a quantum state associated with the transversely sta-
bilized wave packet orbit should exhibit strong localiza-
particularly large for the 2:1 resonance (Fig. 5c): by means tion close to the z-axis. We therefore expect that essential
of the semiclassical Einstein-Brillouin-Keller (EBK) quan- properties of such a quantum state are reproduced by a
tization criterion [31] (which typically yields rather pes- collinear model which restricts the electrons to move along
simistic results, see [32]), we estimate that the minimum the field polarization axis. This, however, requires that the
principal quantum number of the inner electron needed to model takes into account the full Coulomb interaction be-
fully localize a quantum state on the stabilized 2:1 reso- tween the charged particles (i.e., that it really represents
nance island lies in the range N  50 . . . 100 [21,23]. Such the exact quantum analog of the classical, collinear config-
double excitations are clearly beyond reach in state-of- uration). A smoothing of the Coulomb singularity, which is
the-art experiments on helium, which currently can ex- frequently employed in one-dimensional models of driven
cite N  10 [33]. However, they should be accessible in atoms (e.g., [38]), may not be permitted, since it allows
earth alkaline atoms such as barium, where multi-step the electrons to penetrate to the other side of the nucleus,
isolated-core excitations [34] permit selective transitions what inevitably destroys the frozen-planet configuration.
up to states with quantum numbers N  100 of the in- Consequently, we write the Hamiltonian that generates
ner electron [35]. At N = 50, the field parameters that the quantum dynamics of the driven collinear configura-
are required to generate the 2:1 resonance islands of Fig- tion as
ure 5c are given by ω/(2π)  20 GHz and F  8 V/cm. 1 ∂2 1 ∂2 Z Z 1
Hence, by virtue of this semiclassical argument, nondisper- H=− − − − +
2 ∂z12 2 ∂z22 z1 z2 z1 − z2
sive two-electron wave packets appear realizable in earth

alkalines, at microwave frequencies and field amplitudes F 1 ∂ 1 ∂
− sin ωt + − Fst (z1 + z2 ), (4)
commonly used in state-of-the-art ionization experiments ω i ∂z1 i ∂z1
on one-electron atoms [36].
where the exact Coulomb interactions between the charged
particles are taken into account. Here, z1 and z2 represent
the Cartesian (not spherical) coordinates of the electrons
3 Formulation of the quantum eigenvalue along the field polarization axis, with 0 < z2 < z1 < ∞
problem – i.e., both electrons are located on the same side of the
nucleus, with electron 2 closer to it than electron 1. Note
3.1 The collinear Hamiltonian that the electrons effectively appear as distinguishable par-
ticles. This ansatz is consistent with the restriction to
The preceding classical analysis strongly suggests the exis- collinear motion, since in the classical collinear configu-
tence of nondispersive wave packets which propagate along ration the electrons are not able to pass each other and
the frozen-planet orbit, together with a rough estimate of to exchange their positions, nor do their quantum wave
the minimum required quantum number for their unam- functions appreciably overlap at the instant of closest
biguous identification in the spectrum of doubly excited approach (what can be deduced from the classical dy-
helium. Reliable information on the quantum properties namics sketched in Fig. 2, amended by Heisenberg’s un-
of the field-induced resonances, however, can only be ob- certainty). Furthermore, it represents quite good an ap-
tained by quantum calculations. In particular, classical proximation also for the three-dimensional frozen-planet
mechanics tells nothing about the lifetimes of the wave configuration, since the latter is characterized by a very
packets, since these are associated with a classically for- small overlap between the outer and the inner electron’s
bidden tunneling process. It is, on the other hand, also densities, and therefore by a very small splitting between
clear that a full-blown quantum treatment of such highly singlet and triplet states [19]. Precisely as for the classical
 P. Schlagheck and A. Buchleitner: Nondispersive two-electron wave packets in driven helium 407

Hamiltonian, the external electric field consists of an oscil- in triply excited lithium). In order to separate these res-
lating part F – which, in contrast to (1), is incorporated in onances from the flat background of the continuous spec-
the velocity gauge in order to ensure better convergence of trum, we use the method of complex scaling [45–47]. It
the numerical calculation [39] – and of a static component consists in the complexification of coordinates and mo-
Fst > 0 which forces the electrons away from the nucleus. menta (not of time!) according to1
In a last step, we introduce the coordinates
∂ ∂
ξ −→ ξeiθ −i −→ −i e−iθ
ξ = z1 − z2 , η = z2 , (5) ∂ξ ∂ξ
∂ ∂
which independently lie in the range 0 ≤ ξ, η ≤ ∞. η −→ ηeiθ −i −→ −i e−iθ , (10)
∂η ∂η
In these perimetric coordinates [40], the Hamiltonian is
rewritten as through application of the nonunitary complex scaling op-
(E)
erator R(θ) on ψt ,
∂2 1 ∂ ∂2 Z Z 1
H =− 2
− 2
+ − − + (E) (E) (E)
∂ξ 2 ∂η ∂ξ∂η ξ+η η ξ R(θ)ψt (ξ, η) = eiθ ψt (ξeiθ , ηeiθ ) =: ψθ,t (ξ, η) . (11)
F 1 ∂
− sin ωt − Fst (ξ + 2η), (6) Accordingly, the Hamiltonian is transformed as
ω i ∂η

what will turn out as a convenient form for our further H −→ Hθ = R(θ) H R(−θ), (12)
treatment.
what turns (8) into a complex symmetric rather than
hermitian eigenvalue problem, with eigenvalues in the
lower half of the complex plane. In particular, resonances
3.2 Floquet theory and complex scaling
of the “real” eigenvalue problem (i.e., at θ = 0) ap-
pear, for finite θ, as isolated, discrete complex eigenvalues
Due to the temporal periodicity of the Hamiltonian, the E = E − iΓ/2: their real and imaginary parts correspond
Schrödinger problem represented by (6) is conveniently to the energies E and to the half widths at half maximum
treated in the framework of Floquet theory [41,42]: any Γ/2 (HWHM) of the resonances, respectively.
solution of the Schrödinger equation can be expanded in
(E)
a set of 2π/ω-periodic quasienergy-eigenfunctions ψt ,
 3.3 Expansion in Sturmian basis functions
 (E)
ψt = dECE ψt e−iE t , The complex-scaled Floquet Hamiltonian is now expanded
(E) (E) in the product basis
with ψt+2π/ω = ψt , CE ∈ C (7)
{Sn(α) (ξ)Sm
(β)
(η): n, m ≥ 1} (13)
which satisfy the Floquet eigenvalue equation

 composed of the real-valued Sturmian functions [48]
∂ (E) (E)


H −i ψt = E ψt . (8) (−1)n 2ξ ξ 2ξ
∂t (α)
Sn (ξ) = √ exp −
(1)
Ln−1 , (14)
n α α α
(E)
A Fourier series expansion of ψt , (1)
where the Ln−1 denote the associated Laguerre polyno-
∞
 mials [49]. The real parameter α > 0 fixes the length
(E) (E)
ψt = ψ̂k ei k ω t , (9) scale of the Sturmians. As a consequence, the product ba-
k=−∞ sis (13) exhibits two independent scaling parameters, α
and β, which permit the optimal tuning of the basis with
yields a time-independent eigenvalue problem for the respect to the relative excitation of the electrons. Also
(E) (α)
Fourier components ψ̂k , where the effective Hamiltonian note that the Sturmians Sn scale at least linearly with
matrix contains the stationary part of the Hamiltonian ξ, for ξ → 0. This implies that the Coulomb singularities
shifted by kω as diagonal, and the Fourier components of of the Hamiltonian (6) do not lead to divergent matrix
the periodic driving as off-diagonal (block) elements. This elements in the product basis (13).
results in an ω-periodic spectrum of quasienergies E. Multiplication of (8) by ξη leaves 1/(ξ + η) as the only
For atomic systems, the Floquet spectrum is absolutely non-polynomial contribution in ξ and η, after inserting (6).
continuous: each bound state of the unperturbed atom is We factor out (ξ + η) from the eigenvectors of (8),
coupled to the atomic continuum via multiphoton transi-
tions, and therefore appears as a resonance structure in (E) (E)
ψt (ξ, η) =: (ξ + η) φt (ξ, η) , (15)
the spectrum – in analogy to autoionizing states in mul-
1
tiply excited atoms, which are coupled to the continuum Note that, due to (5), complexification of ξ, η and of z1 , z2
via configuration interaction [43] (see, e.g., [44] for a case is equivalent.
408 The European Physical Journal D

(E) (α) (β)

and expand φt (ξ, η) in the Sturmian product basis. This the basis functions Sn (ξ), Sm (η) to be retained in the
factorization is justified since the triple collision between diagonalization, as well as by variation of the complex
the electrons and the nucleus – i.e., the event that cor- scaling angle θ, and of the length scale parameters α and
responds to ξ = η = 0 – is classically suppressed in the β which specify the (truncated) basis set (14) used in the
collinear frozen-planet dynamics (in contrast to the eZe calculation. Typical matrix dimensions are 64 000 (size)
configuration with the electrons on opposite sides of the × 1 300 (bandwidth) for Floquet spectra in the vicinity of
nucleus); hence, the quantum probability near ξ = η = 0 N  8, with n  1 . . . 150, m  1 . . . 25, and k  −8 . . . 8,
is very small. Note that, due to normalization, (15) entails for2 ω  0.2N −3 . Real and complex scaling parameters
(E)
a different transformation law for φt (ξ, η) as compared are fixed at θ = 0.1, α = 6, β = 2 in the above energy
(E) range. With these choices (and similar choices for other
to ψt (ξ, η), under the action of R(θ):
values of N ), all numerical results presented hereafter are
(E) (E) (E) converged to an absolute accuracy of 10−15 . . . 10−13 a.u.
R(θ)φt (ξ, η) = e2iθ φt (ξeiθ , ηeiθ ) =: φθ,t (ξ, η) . (16)

All together, the generalized Floquet eigenvalue equations 3.4 Visualization of the wavefunction
finally reads
The energies E and widths Γ extracted from the complex
(E)
(ξ + η)ξη(H0θ + kω − E)(ξ + η)φ̂θ,k (ξ, η) + (ξ + η) eigenvalues E allow to classify the Floquet states in se-
(E) (E) ries and to determine their stability; in general, however,
× ξηVθ (ξ + η)(φ̂θ,k−1 (ξ, η) − φ̂θ,k+1 (ξ, η)) = 0 , (17) they do not provide any direct information about the lo-
calization properties of these states in configuration or
with the complex scaled operators H0θ , Vθ given by in phase space, which in themselves can carry important

 physical information. To extract the latter from the eigen-
∂ 1 ∂ ∂2
H0θ = − 2 − + e−2iθ states of the complex symmetric eigenvalue problem (17),
∂ξ 2 ∂η 2 ∂ξ∂η some care has to be taken, due to the non-unitarity of the


Z Z 1 −iθ dilation operator R(θ). The technical and computational
+ − − + e
ξ+η η ξ details of this procedure are described in detail in [23,51],
and we only import here those results of immediate rele-
−Fst (ξ + 2η) eiθ , (18)
vance for our specific purpose.
F ∂ −iθ We first need the density of the physical wave function
Vθ = e , (19)
2ω ∂η (E)
(at real energy E) ψt (z1 , z2 ), which is obtained (up to
(E) a normalization constant), for a well-isolated resonance
and the φ̂θ,k (ξ, η) the Fourier components (see (9)) of the energy E = E−iΓ/2 (i.e., |Ej −E|  Γ , ∀Ej = E), from the
(E) (E)
wavefunction φθ,t (ξ, η). Introducing the scalar product image of ψθ,t under the inverse dilation operator R(−θ),
 ∞ ∞ ∞

1 
f |g
≡ f (ξ, η) g(ξ, η) dξ dη , (20) (E)
R(−θ)ψθ,t = R(−θ)
(E)
z1 φ̂θ,k (z1 − z2 , z2 ) eikωt ,
0 0 ξ η
k=−∞
with respect to which the Sturmians are orthogonal, we (22)
obtain a complex symmetric eigenvalue problem.
(E) together with the image of the corresponding left eigen-
All the opertor-valued terms acting on the φ̂θ,k and (E)
(E) vector ψθ,−t [23,51]3 :
φ̂θ,k±1 in (17) can now be expressed as polynomials of the
elementary ladder operators of the Sturmian basis (14) (E) (E)
|ψt (z1 , z2 )|2  Re z1 , z2 |R(−θ)|ψθ,t

(see [23,49]). Hence, upon expansion of the Fourier com-  

(E) (E)
ponents φ̂θ,k in the Sturmian product basis (13), × z1 , z2 |R(−θ)|ψθ,−t . (23)
∞
 Correspondingly, the Husimi representation Q(z1 , p1 ) [23,51]
(E) (k)
φ̂θ,k (ξ, η) = Cn,m Sn(α) (ξ) Sm
(β)
(η) , (21) in the classical phase space coordinates of the outer elec-
m,n=1 tron (subscript 1) is obtained by projection on Gaussian
2
we obtain strict selection rules which permit nonzero cou- Note that a nonvanishing static field component does only
(k) (k
) increase the bandwidth of the Floquet matrix (|n − n
| ≤ 4
plings between the coefficients Cn,m and Cn
,m
only if
instead of |n − n
| ≤ 3 [23]) but not its dimension, which is a
|n − n | ≤ 4, |m − m | ≤ 4, and |k − k  | ≤ 1. The eigen- peculiarity of the absence of the angular momentum degree of
value problem thus becomes a sparse, complex symmetric freedom in our collinear model.
matrix equation with rather narrow bandwidth, what al- 3
Only the time-dependent part of the wave function is com-
lows to apply efficient diagonalization methods based on plex conjugated to transform right into left eigenvectors, since
the Lanczos algorithm with inverse iteration [50]. Con- (E)
the Fourier components ψ̂θ,k of the eigenvectors obey the nor-
vergence of the complex eigenvalues is controlled by in- malization condition for complex symmetric rather than Her-
(E)
creasing the number of Fourier components φ̂θ,k and of mitian matrices [6, 23]!
 P. Schlagheck and A. Buchleitner: Nondispersive two-electron wave packets in driven helium 409

wave packets χp1 (z1 ) which are centered at position z1

and propagate with average momentum p1 :
 
(E)
Q(z1 , p1 )  Re χp1 (z1 )|R(−θ)|ψθ,t
 
(E)
× χp1 (z1 )|R(−θ)|ψθ,−t , (24)

where the bar denotes complex conjugation.

In order to establish a precise analogy with our above Fig. 9. Energies and ionization rates Γ/2 (HWHM) of the
construction of the two-step Poincaré section of the classi- autoionizing states of collinear helium belonging to the series
cal dynamics (see Sect. 2.2), we define the overlap matrix labeled by the inner electron’s quantum number N = 8. Note
element in (24) as the relatively small widths of the lowest members of the series,
which we attribute to the fact that these states are fully local-
 ∞ ized within a regular, bound domain in phase space. The cou-
(E) (0) (E)
χp1 (z1 )|R(−θ)|ψθ,t
= dz1 z1 , z2 |R(−θ)|ψθ,t
pling mediated by a driving field with frequency ω = 0.2 N −3
0 is sketched by the arrows of length ω. The particularly strong,


1 near-resonant coupling between the second and the third state
× exp − ωs (z1 − z1 )2 − ip1 z1 · (25)
2 (at E = −0.034 and E = −0.0336, respectively) gives rise to
the nondispersive two-electron wave packet associated with the
Thus, the quantum phase space probability density is eval- classical 1:1 resonance (see Fig. 13).
uated at fixed time t (corresponding to a fixed phase ωt of
(0)
the driving field), and at fixed position z2  0 of the in-
ner electron. The squeezing parameter ωs in this definition dynamics. In particular, each autoionizing state can be
determines the resolution of the Husimi distribution in classified by two quantum numbers which are associated
position and momentum, respectively. Large values of ωs with the two separating modes of the classical dynamics,
yield good resolution in position space and bad resolution as discussed in Section 2.1 (in contrast to the chaotic eZe
in momentum space, and vice versa for small values of ωs . configuration [52], where such a classification breaks down
For quantum states associated with the frozen-planet con- already for moderate double excitations). The quantiza-
figuration, the most appropriate choice for ωs is given by tion of the inner electron’s Kepler mode gives rise to the
the intrinsic frequency scale ωI of the configuration (see quantum number N ≥ 1. For each N , we obtain a series of
Sect. 2.1) – this is the value at which the Gaussian wave autoionizing states (or bound states, for N = 1) which are
packet χp (q) optimally fits the ground state of the effective labeled by the quantum number n. This quantum num-
potential experienced by the outer electron. We therefore ber arises from the quantization of the outer electron’s
choose ωs = 0.3 N −3 (see Fig. 3), with N the inner elec- oscillation within the effective potential, which, as in one-
tron’s principal quantum number of the state to be visual- electron atoms, gives rise to Rydberg series and continua,
ized (note that N remains approximately a good quantum due to its asymptotic 1/r dependence.
number in the presence of the external field, if the latter As an example, we show the energies and widths of
is not too strong). the autoionizing states of the series labeled by N = 8 in
Figure 9. We clearly recognize a regular Rydberg progres-
sion towards the N = 8 threshold at E = −0.3125 a.u.
4 The unperturbed collinear atom States belonging to different series are energetically well
separated: the lowest quantum state with N = 9 lies at
With the above theoretical machinery for our quantum E  −0.027 a.u., and the Rydberg series of N = 7 termi-
treatment of the driven, collinear frozen planet configu- nates at E  −0.04 a.u. As was verified numerically, an
ration at hand, we can now study in detail its physical energetic overlap of series belonging to different quantum
properties. As a “warm-up”, and equally so as a first as- numbers N occurs only above N = 20.
sessment of the physical implications of the restricted di- The near-separability of the two modes associated with
mensionality of our problem, we start out with the spectral the electrons is furthermore reflected by the probability
properties of the unperturbed (F = Fst = 0) frozen planet density (23) of the eigenstates (with k = 0 in (22), due
configuration confined to a single dimension of configura- to the time-independence of the problem). In the coordi-
tion space. nate z2 of the inner electron, the wavefunctions are essen-
tially given by the N th hydrogenic eigenstate of the one-
dimensional atom (most reminiscent of extremal parabolic
4.1 Energies and phase space distributions states of three-dimensional atomic hydrogen), whereas
in z1 they display distinct excitations within the effec-
Corresponding to the fact that its classical counterpart tive potential governing the outer electron’s motion. In
is almost completely integrable (Fig. 4a), the quantum Figure 10, the fundamental (a1), the first excited (a2),
spectrum of the unperturbed collinear frozen-planet con- and the second excited state (a3) of the effective poten-
figuration is characterized by typical signatures of regular tial (for N = 8), labeled by the outer electron’s quantum
410 The European Physical Journal D

- -

- -

- -

- -

- -

- -

- -

Fig. 10. Wavefunctions of the first three eigenstates of the - -

N = 8 series: (a1, b1) lowest (n = 1), (a2, b2) second (n = 2),

(a3, b3) third state (n = 3) of the series. (a1–a3) Probabil-
ity densities as a function of the coordinates of the outer (z1 ) Fig. 11. Energies (a) and ionization widths (c) of the lowest
and of the inner (z2 ) electron; (b1–b3) Husimi densities as a autoionizing eigenstate n = 1 (with the outer electron local-
function of position and momentum of the outer electron (the ized at the minimum of the effective potential of Fig. 3), plot-
contour lines are plotted on a linear scale). In the coordinate ted as a function of the inner electron’s quantum number N .
of the inner electron, the wavefunctions are essentially given We see that the ionization rates decrease near-exponentially
by the N th hydrogenic eigenstate of the unperturbed, one- for N > 4, what suggests that the associated eigenstates are
dimensional atom, whereas in z1 they display different excita- fully localized in the bound part of phase space, and only de-
tions within the effective potential (see Fig. 3). Their Husimi cay via tunneling through the classical phase space barriers
distributions clearly show that they are well localized along reg- that protect the frozen-planet configuration against classical
ular tori in the underlying classical phase space (see Fig. 4a). autoionization. These rates of the collinear model are com-
pared to the energies (b) and decay rates (d) of the analogous
frozen-planet eigenstates in three-dimensional helium, pub-
lished in reference [19], for singlet (+) and triplet (◦) symmetry.
While the energies agree quite well with their collinear coun-
numbers n = 1, n = 2, and n = 3, respectively, are plot- terparts (a, b), the ionization rates of the three-dimensional
ted in configuration space. The intimate correspondence frozen-planet states (d) lie by several orders of magnitude
of these eigenstates with regular structures of the under- above the widths of the corresponding eigenstates of the one-
lying classical phase space is highlighted by their Husimi dimensional model (c) (note the different scales of the vertical
distribution (24) shown in Figures 10b1–10b3. Comparing axes in (c) and (d)). This indicates that the autoionization of
these phase space projections of the quantum eigenfunc- the three-dimensional frozen-planet states is mediated by the
tions with the corresponding Poincaré surface of section transverse degrees of freedom of the configuration.
(Fig. 4a) unambiguously illustrates the neat localization
of the eigenfunctions along invariant tori of the classical
dynamics.

4.2 Ionization rates exponential law represents a clear signature of quantum

tunneling: the rate associated with such a process gener-
The “regular” character of the wavefunctions is also man- ally decreases exponentially with the semiclassical action
ifest in the ionization rates Γ/2 (HWHM) of the associ- SN across the tunneling barrier, and this latter quantity
ated spectral resonances. We see in Figure 9 that for the scales, as any other action variable, linearly with N , due
N = 8 series these widths first increase with n, and then to the general scaling laws (3) – i.e., SN = N S1 , with
decrease again towards the ionization threshold. While S1  0.8 directly extracted from Figure 11c.
this latter decrease is attributed to general scaling laws
of Γ in the Rydberg regime of atomic one-electron excita- For comparison, we plot in Figure 11d the ioniza-
tions [53], the extraordinary stability of low n states is a tion rates of the near-collinear frozen-planet states in
consequence of their full localization in the bound part of three-dimensional helium (with minimal excitations in
phase space. A coupling to the unbound, ionizing domain the transverse degrees of freedom), as reported in [19].
is then only possible via a classically forbidden process – Also these widths decrease on average exponentially in N ,
tunneling through the phase space barriers that confine with a scaled action S1 not too different from our one-
the frozen-planet configuration. dimensional model (fluctuations with respect to this ex-
This latter mechanism is beautifully illustrated in a ponential decrease arise from the mixed regular-chaotic
plot of the ionization rate of the lowest state (n = 1) as phase space structure of three-dimensional helium, see
a function of the inner electron’s quantum number N . In also the discussion in Sect. 5.2). However, the three-
Figure 11c, we observe that the width of this lowest eigen- dimensional rates are systematically enhanced by several
state in the effective potential of Figure 3 first increases orders of magnitude as compared to the one-dimensional
for N ≤ 4 (due to imperfect localization of the eigenstate model! This suggests that the three-dimensional helium
on classical phase space structures in the deep quantum dynamics provides efficient decay channels associated
regime) and then decreases exponentially with N . This with the transverse degrees of freedom, which are not
 P. Schlagheck and A. Buchleitner: Nondispersive two-electron wave packets in driven helium 411

incorporated in the restricted one-dimensional dynamics

of our model Hamiltonian (4)4 .
On the other hand, the energies of the autoioniz-
ing states of three-dimensional helium agree quite well
with their collinear counterparts, as apparent from Fig-
ures 11a and 11b (apart from a small shift due to the ad-
ditional quantization of the transverse modes in the 3D
configuration [19]). This supports our expectation that
essential localization properties of the eigenstates of the
three-dimensional frozen-planet configuration are well re-
produced by the collinear model.
Fig. 12. (a) Evolution of the first three states of the N = 8 se-
ries in the Floquet spectrum, for driving frequency ω =
5 The collinear atom under periodic driving 0.2 N −3 . The quasienergies E are plotted as a function of the
field amplitude F . The diabatic continuation of the second
5.1 Nondispersive wave packets in the Floquet state (n = 2, upmost circles) undergoes a particularly pro-
spectrum nounced, almost linear shift with F . This is consistent with
the wave packet character of the Floquet state into which the
unperturbed n = 2 state evolves (see Fig. 13). (b–d) Ionization
For our investigation of the collinear frozen planet con- rates Γ of the diabatic continuations of the n = 1 (d), n = 2
figuration under external driving, we employ the field pa- (b), and n = 3 state (c). We see that the rates globally increase
rameters ω = 0.2 N −3 and F = 0.005 N −4 which induce with increasing F . Local, pronounced maxima occur at avoided
the classical phase space structure shown in Figure 6, crossings between these states and energetically higher-lying
where both the intrinsic island and the 1:1 resonance are eigenstates of the N = 8 series in the Floquet spectrum, as ap-
very well pronounced. The coupling induced by this driv- parent from a comparison with (a) (with the diabatic continu-
ing field is illustrated by the arrows in Figure 9 for the ations of n = 1 and n = 3 marked by the encircled eigenvalues
N = 8 series. We see that a particularly strong interac- in the lower and the middle part of (a), respectively).
tion is induced between the second (n = 2) and the third
(n = 3) state, since the energetic spacing between these
states is very close to the driving frequency. Provided the n = 15 . Its quasienergy exhibits a pronounced shift at al-
phase space volume of the 1:1 resonance island is large most constant, positive slope. This already indicates the
enough to support a fully localized quantum state (which wave-packet character of the associated eigenfunction in
is indeed the case for N = 8, as can be semiclassically configuration space, since it reflects a large dynamic dipole
estimated by the EBK quantization criterion), this near- moment of the electronic density (proportional to the ex-
resonant one-photon coupling gives rise to the nondisper- pectation value of the electronic dipole z1 , averaged over
sive wave packet associated with the classical nonlinear one cycle of the drive).
resonance. The wave packet character of this latter state is ulti-
Figure 12a shows the evolution of the quasienergies mately confirmed by its Husimi density, which is plotted in
associated with the first three Floquet eigenstates of the Figures 13b1–13b3 for F = 0.005 N −4, at driving phases
N = 8 series, as a function of the field amplitude F (for ωt = 0, π/2, and π. We see that the Floquet eigenfunc-
fixed driving frequency ω = 0.2 N −3 , and Fst = 0). In the tion is fully localized on the 1:1 resonance island in phase
limit F = 0, the energies E correspond to the unperturbed space, and that it precisely follows the classical time evo-
autoionizing levels folded into the Floquet zone due to the lution. The wave packet dynamics in configuration space
ω-periodicity of the Floquet spectrum. Switching on the is visualized in Figures 13a1–13a3 where we plot the prob-
driving field causes level shifts due to the repulsion be- ability density of the state n = 2 as a function of z1 and z2 .
tween strongly coupled, near-resonant Floquet states. A Comparison with Figures 10a1–10a3 show that the eigen-
particularly significant case is encountered for the state function is essentially composed of a time-periodic super-
n = 2, near-resonantly coupled to the states n = 3 and position of the low-lying eigenstates of the N = 8 series.
4
As a side remark, this observation also bears a caveat as While nearly stationary in the coordinate z2 of the in-
oversimplified models of the three body Coulomb problem are ner electron, the wave packet oscillates back and forth
concerned: often the Coulomb singularities in such 1D model in z1 , between the turning points of the effective potential
systems are smoothed such as to prevent the electrons (and (Fig. 3).
possibly the nucleus) from head-on collisions [54, 55], which,
5
on a first glance, could be most disastrous for the stability of Note that the field induced level dynamics which we ob-
the 1D dynamics and, hence, enhance its decay probability. serve here is somewhat reminiscent to the level shift of the
The present comparison of exact (no approximations beyond lowest three energy levels of a symmetric one dimensional dou-
dimensionality) 1D and 3D quantum calculations shows that ble well, under resonant driving of the transition between the
this is too simplistic an argument and completely neglects dy- first and second excited state [56]. A more general investigation
namical stabilization effects which result in such impressively of Floquet level dynamics in complex, non-decaying systems
stable quantum objects as the frozen planet. can be found, e.g., in [57].
412 The European Physical Journal D

Fig. 15. Energies and widths of the nondispersive wave packet

at ω = 0.2 N −3 for N = 9 (a1, a2) and N = 10 (b1, b2), as
a function of the scaled field amplitude F/N −4 . (a1, b1) Evo-
Fig. 13. Nondispersive two-electron wave packet of the lution of the quasienergies E in the Floquet spectrum. The
N = 8 series, for ω = 0.2 N −3 and F = 0.005 N −4 . We plot 1:1 resonance state (marked by circles) diabatically originates
the probability density in configuration space (a1–a3), and the from the unperturbed state n = 2 at N = 9, and from the
Husimi density in phase space (b1–b3), of the diabatic con- state n = 3 at N = 10. As for N = 8 (see Fig. 12a), its
tinuation of the state n = 2 (see Fig. 12), at driving field quasienergy undergoes a significant shift towards higher val-
phases (a1–c1) ωt = 0, (a2–c2) π/2, (a3–c3) π. The correspond- ues of E with almost constant slope, what indicates the pro-
ing Poincaré sections of the classical phase space are plotted nounced wave packet character of this eigenstate in configu-
in (c1–c3). We see that the Floquet wavefunction is well lo- ration space. (a2, b2) Ionization widths of the wave packet
calized on the 1:1 resonance island, and faithfully tracks its states. As in Figure 12c, local, sharp enhancements of Γ oc-
classical time evolution. cur near avoided crossings with higher-lying states of the same
series, which are associated with the chaotic phase space do-
main. Notice that the precise positions and strengths of the
avoided crossings and, consequently, their influence on the wave
packet’s lifetime at a given scaled field amplitude F/N −4 , can
be completely different for N (a1, a2) and N + 1 (b1, b2).

more, Floquet states corresponding to higher quantum

numbers n > 2 of the unperturbed system are entirely
associated with the chaotic phase space domain. As an
example, Figures 14b1–14b3 show the Husimi density of
the diabatic continuation of the state n = 3, which is
dominantly localized on the unstable fixed point of the
1:1 resonance (compare Figs. 14b3 and 14c3), and along
the associated separatrix layer.
Fig. 14. Husimi distribution of the states n = 1 (a1–a3) A similar scenario is encountered for different quantum
and n = 3 (b1–b3) of the N = 8 series, for ω = 0.2 N −3 numbers N of the inner electron (with adjusted field pa-
and F = 0.005 N −4 , at driving phases ωt = 0 (a1, b1), π/2 rameters ω = 0.2 N −3 and F = 0.005 N −4). Starting from
(a2, c2), π (a3, b3), compared to the corresponding classical N = 5, we find, for each N , one Floquet state that is lo-
Poincaré sections (c1–c3). We see that the diabatic continua- calized on the intrinsic island (the diabatic continuation of
tion of the lowest state of the N = 8 series is fully localized on
the island’s ground state in the unperturbed spectrum),
the intrinsic island and remains essentially stationary over one
as well as one nondispersive wave packet state localized
field cycle. The diabatic continuation of the third state, on the
on the 1:1 resonance island, represented by the diabatic
other hand, is associated with the chaotic phase space domain.
More precisely, it is anchored to the unstable fixed point of
continuation of the second unperturbed state for N < 10,
the 1:1 resonance and stretches out along the associated sepa- and by the continuation of the third or a higher state for
ratrix structure (see also [8, 16] for analogous states in driven N ≥ 10. As for N = 8, these wave packet states are char-
hydrogen atoms). acterized by a pronounced, almost linear level shift with
increasing F towards higher quasienergies (Fig. 15).
Figure 16 compares the Husimi distributions of the
Quite naturally, for the same field amplitude and fre- wave packet states for N = 5 and N = 15. Since the
quency as above, the diabatic continuation of the low- phase space area of the island increases linearly with N
est state n = 1 of the N = 8 series represents the while  remains constant, the electronic density is, with
Floquet state that is anchored to the remainder of the increasing N , more and more localized around the center
unperturbed regular structure of the frozen-planet con- of the 1:1 resonance island. At N = 15, the contour lines
figuration. Figures 14a1–14a3 show its Husimi distribu- of the Husimi density reproduce the classical island struc-
tion which is fully localized on the intrinsic island and ture in the Poincaré section already very well. In fact, at
remains nearly stationary over one field period. Further- such high values of N , the island is already large enough
 P. Schlagheck and A. Buchleitner: Nondispersive two-electron wave packets in driven helium 413

Fig. 17. Ionization rates (HWHM) of the wave packet state

localized on the 1:1 resonance island, as a function of the in-
ner electron’s quantum number N (ω = 0.2 N −3 and F =
0.005 N −4 ), for different strengths Fst of the static field. Cir-
cles connected by thick solid lines: Fst = 0; squares connected
by thin solid lines: Fst = 0.001 N −4 ; diamonds connected by
dotted lines: Fst = 0.002 N −4 . The strong fluctuations of the
rates are attributed to the coupling to Floquet states that are
associated with the chaotic domain of phase space.

Fig. 16. Nondispersive two-electron wave packet for N = 5

(a1–a3) and N = 15 (b1–b3), as well as the first excited
mode of the nondispersive wave packet for N = 15 (c1–c3), at
tial decrease is not observed in our calculations. As we
ω = 0.2 N −3 and F = 0.005 N −4 . The Husimi density of the see in Figure 17, the ionization rates exhibit, in the range
Floquet states is plotted for the phases (a1–d1) ωt = 0, (a2–d2) N = 5 . . . 15, strong, quasi-erratic fluctuations between
π/2, (a3–d3) π, and compared to the corresponding classical Γ/2 ∼ 10−12 a.u. and Γ/2 ∼ 10−8 a.u., corresponding to
Poincaré sections (d1–d3). With increasing N , the wave packet lifetimes between 104 and 107 field cycles. No significant
is more and more localized on the center of the 1:1 resonance, tendency towards lower values for increasing N can be
due to the decreasing relative size of 2π
(as compared to the unambiguously identified.
typical atomic scales, see Eqs. (3)) indicated by the dashed The observed fluctuations of Γ represent a clear sig-
rectangles in (a1) and (b1). At N = 15, the contour lines of nature of the mixed regular-chaotic structure of the clas-
the Husimi density reproduce the structure of the island in the sical phase space (see, e.g., Figs. 16d1–16d3). In contrast
classical Poincaré section rather well. to globally regular systems such as the unperturbed Zee
configuration (see Sect. 4.2), the coupling from the locally
to trap an additional wave packet state, giving rise to a bound domain to the ionization continuum is not given by
first excited mode of the nondispersive wave packet (see a single tunneling rate. Instead, it is mediated by a two-
Figs. 16c1–16c3, and reference [10] for an analogous case step process which, besides tunneling through the barri-
in driven hydrogen). ers of the regular island, involves also chaotic transport
through irregular phase space outside the island towards
the continuum. It is in fact this latter, chaotic component
5.2 Lifetimes of the wave packet states of the coupling process that generates the fluctuations of
the decay rates, on top of their on average exponential
As already mentioned in the introduction, the time scale decrease with N . This chaos-assisted tunneling mecha-
over which the nondispersive wave packet follows the res- nism, originally formulated for tunneling transitions be-
onantly driven classical orbit without spreading is only tween symmetric regular islands in bounded systems [58],
limited by the finite ionization rate of the correspond- was indeed proven to govern the decay of nondispersive
ing Floquet state. Since this ionization proceeds via a wave packets in driven one-electron atoms [12], the lat-
classically forbidden tunneling process, the associated de- ter exhibiting similar quasi-erratic deviations of Γ from a
cay rate is, as in driven hydrogen [6,8,10], very small. purely exponential law (see also [59]).
For the wave packet state of the N = 8 series (ω = In the Floquet spectrum, the chaos-induced modifi-
0.2 N −3 and F = 0.005 N −4) for instance, we obtain cation of the tunneling process can essentially be under-
Γ/2  1.77 × 10−11 a.u., which corresponds to a lifetime stood via the influence of near-resonant chaotic states on
of τ  1.8 × 106 field cycles before the wave packet popu- the ionization rate of the wave packet state. As we see
lation is appreciably redistributed over the ionization con- in Figures 12b–12d, the widths of the energetically low-
tinuum. lying members of the N = 8 series generally increase with
In general, one expects the ionization rate of the wave increasing F . Local, pronounced enhancements of Γ , how-
packets to decrease on average exponentially ∼ exp(−SN ) ever, occur near avoided crossings (corresponding to mul-
with N , where S is the semiclassical action across the tun- tiphoton resonances) with higher-lying states of the same
neling barrier that confines the resonance island at N = 1. series, which are associated with the chaotic phase space
In contrast to the unperturbed collinear configuration dis- domain (compare Figs. 12b–12d with Fig. 12a). Hence,
cussed in Section 4 (Fig. 11c), however, such an exponen- at a given scaled field amplitude, e.g. F = 0.005N −4,
414 The European Physical Journal D

the decay rate of the wave packet state depends sensitively

on the effective interaction with nearby chaotic states in
the spectrum, the latter being essentially determined by
the energetic distance to those states, as well as by the
corresponding coupling matrix elements. Since these in-
gredients vary in a random-like way with the quantum
number N of the inner electron (at fixed F/N −4 ), the re-
sulting effect on the wave packet’s ionization rate may turn
completely different when changing N to N + 1 (compare
here Figs. 12a, 12b to Figs. 15a1, 15a2 and 15b1, 15b2),
and therefore cannot be predicted by simple semiclassical Fig. 18. (a1–a3) Poincaré section of the classical dynamics
considerations. at ω = 0.2 and F = 0.005, with a static field Fst = 0 (a1),
The average exponential decrease of the ionization 0.001 (a2), 0.002 (a3). (b1–b3) Husimi density of the wave
rate, on the other hand, should in principle be amenable packet state localized on the 1:1 resonance island for N = 8,
to semiclassical estimations, as it is essentially determined at ω = 0.2 N −3 and F = 0.005 N −4 , calculated in presence of
by the height of the tunneling barrier that confines the a static field Fst = 0 (b1), 0.001 N −4 (b2), 0.002 N −4 (b3) (at
resonance island in phase space. Semiclassical approaches driving phase ωt = 0). The phase space projection of the wave
to quantitatively evaluate the associated tunneling rates packet remains almost invariant when increasing the static field
for nonintegrable systems are presently under construc- from Fst = 0 to 0.002 N −4 , in agreement with the observation
tion (see [60])6 . that also the classical 1:1 resonance island is largely unaffected
by the additional perturbation.

5.3 Influence of an additional, static electric field

to a decrease of the wave packet’s lifetime from 1.8×106 to
1.0 × 104 field cycles. Since the static field notably affects
Let us finally discuss to which extent the wave packet the asymptotic part of the effective potential experienced
dynamics of the collinear atom is modified by the applica- by the outer electron (see Fig. 3), and thereby modifies
tion of an additional, static electric field with a strength the transport towards the continuum, such an enhance-
of up to 20 percent of the driving field amplitude. As al- ment of Γ with Fst is not unexpected. However, Figure 17
ready pointed out in Section 2.3, such a static field is shows that the ionization rates do not always increase with
required to stabilize the driving-induced nonlinear reso- increasing Fst . Instead, a rather erratic dependence of Γ
nances in the classical dynamics of the three-dimensional on Fst and N is encountered, what calls for a more quan-
atom. While the transverse dynamics of the driven con- titative (and possibly statistical) analysis of the problem.
figuration is therefore substantially modified by the static
field, the structure of the collinear phase space remains
nearly unaffected. This is seen in Figures 18a1–18a3 which 6 Conclusion
show Poincaré sections of the collinear phase space at
ω = 0.2 and F = 0.005, for gradually increasing static Our present study provides abundant evidence for the
field components Fst = 0 . . . 0.002. Except for a slight re- stabilizing effect of classical nonlinear resonances on pe-
duction of their size, the two dominant regular islands are riodically driven quantum systems, in the presence of
not significantly affected by the static perturbation. strong electron-electron interactions. We have seen that
Accordingly, we find that the phase space projec- such nonlinear resonances, which actually reflect a phase
tions of the Floquet states localized on these islands re- locking phenomenon [16] between the unperturbed quan-
main essentially unmodified, too, in presence of the static tum dynamics and the driving field, allow to launch non-
field. This is illustrated in Figures 18b1–18b3 which show dispersive two-electron wave packets along the highly cor-
the resulting Husimi density of the nondispersive wave related frozen planet orbit of collinear helium, with tiny,
packet state of the N = 8 series at ω = 0.2 N −3 and tunneling induced leakage towards the atomic continuum.
F = 0.005 N −4. However, while no visible change oc- As already observed in simpler one electron systems un-
curs in the phase space localization properties, the ion- der external driving, these wave packets can be identified
ization rate is significantly affected by the static field: it by the characteristic parameter dependence of their en-
increases from Γ/2  1.77 × 10−11 a.u. at Fst = 0, to ergies and decay rates, with strong signatures of chaos
Γ/2  3.05 × 10−9 a.u. at Fst = 0.002 N −4, corresponding assisted ionization. Our 1D quantum calculations corrob-
6
Also note, that the critical field amplitude needed to induce orate an intimate quantum-classical correspondence, al-
an appreciable increase of the decay rates beyond their mini- ready at rather weak excitations (N ≥ 5) of the inner
mum value at small field amplitudes coincides remarkably well electron, even in the presence of a static electric field
for N = 8, 9, 10, as equally observable in Figures 12 and 15. component added to the periodic drive (which confines
This is a signature of the transition from globally regular to the real 3D dynamics to the vicinity of the field polariza-
dominantly chaotic dynamics in the classical phase space, and tion axis, in classical 3D calculations). This strongly sug-
highlights the relevance of the classical scaling laws (3), also gests that nondispersive two-electron wave packets exist
for the quantum mechanical ionization process. also in driven 3D helium (for which, so far, only classical
 P. Schlagheck and A. Buchleitner: Nondispersive two-electron wave packets in driven helium 415

simulations are feasible), and that similar stabilization 23. P. Schlagheck, Das Drei-Körper-Coulombproblem unter pe-
phenomena are possible also in other, high dimensional riodischem Antrieb, Ph.D. thesis, Technische Universität
atomic or molecular systems under external forcing. How- München, Herbert Utz Verlag, München, 1999
ever, our comparison of the life times of 1D and 3D 24. P. Schlagheck, A. Buchleitner, Europhys. Lett. 46, 24
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