Towards the preparation of two-.........

electron nondispersive wavepackets

...................................... in helium
.

Alejandro Gonzalez M.
Physics Department
Universidad del Valle
October 28, 2015

Outline

Introduction

Unperturbed 2D helium

Driven 2D helium atom

Unperturbed 3D description

Introduction

Three body problem

I
I
I

Highly complicated dynamics Chaotic dynamics

Perturbative methods
Numerical techniques

Helium atom
I

I
I

Microscopic realization of the three body problem of celestial

mechanics.
The two-electron dynamics is in general irregular or chaotic.
Failure of first quantization attempts on the basis of Bohrs quantum
postulates.
The non-integrability of the quantum system is understood as the
direct counterpart of the corresponding classical mixed
regular-chaotic dynamics.

[R. P. Madden and K. Codling, Phys. Rev. Lett. 10 (1963) : 516]

The doubly excited states

of two-electron atoms are
highly correlated states.

They cannot be in general described by

a simple model based on independentparticle quantum numbers.

Frozen Planet Configuration

Both electrons are located on the same side of the nucleus.

Classically stable under small transverse perturbation.

The inner electron precesses on highly eccentric ellipses. The outer

electron is locked upon the precessing motion of the inner electron.
[K. Richter and D. Wintgen, Phys. Rev. Lett. 65 (1990) : 1965]
4

Frozen Planet States

0.6

p1

Classical phase space of the collinear frozen planet (top left). Husimi distributions of the ground
(top right), first excited (bottom
left) and second excited (bottom
right) FPS under the N = 6 ionization threshold.

0.0

0.6
0.6

p1

0.0

0.6
0

x1

x1

Periodic driving field

0.11

p1

0.00

0.11
0.11

p1

0.00

0.11
0

200 0

200 0

200

The Husimi distribution of a Floquet

state associated with a frozen planet state for different phases of the
driving field (top). Classical phase
space structure of the restricted collinear problem (bottom).

x1

[J. Madroero et al., Adv. At. Mol. Opt. Phys. 53 (2006) : 33]
5

2D Theoretical Model (unperturbed system)

Hamiltonian for the helium atom
H=

p~12
p~ 2
2
2
1
+ 2

+
2
2
r1
r2
r12

Coordinate transformations
(
(xi , yi )

i = ri + xi

i = ri xi

=
=

1
2
2
1
2
2

x = r +

y = r

Creation and annihilation operators

x + ipx

,
2
y + ipy

=
,
2

ax =
ay

x ipx

2
y ipy

=
2

ax =
ay

We introduce the operators

ax+ iay+

,
2
ax iay

a3 =
,
2
a1 =

ax+ + iay+

2
ax + iay

a4 =
2
a2 =

[J. Madroero and A. Buchleitner, Phys. Rev. A 77 (2008) : 053402]

6

which satisfy
[ai , aj ] = 0,

[ai , aj ] = 0,

[ai , aj ] = ij ,

i, j = 1, 2, 3, 4

Basis set
|n1 n2 n3 n4 i = |n1 i |n2 i |n3 i |n4 i,

ni = ai ai

Generalized eigenvalue problem :

H|i = EJ|i
Introducing a shift parameter , so that
(H J) |i = (E ) J|i
we apply the Lanczos algorithm to calculate states for which E .

Complex rotation
To extract resonance states and their decay rates we use complex
rotation.

R()

==

E = i 2 ,

The bound states remain unchanged under the transformation.

The continuous spectra are rotated an angle of 2 with the real axis.

The resonances are exposed once the angle c and then

becomes independent of the angle .

[Ho, Phys. Rep. 99 (1983) : 1]

8

Numerical results
Spectrum of the 2D helium

Complex energy spectrum of the rotated 2D helium Hamiltonian for

states with l = 0, obtained by several runs of the Lanczos algorithm.
The basis is truncated according to the rule : n1 + n2 + n3 + n4 nbase
9

Identification of the FPS

Expectation value of cos 12 :

hcos 12 i ' 1

[T. Wei, Undergraduate thesis, Technische Universitt Mnchen, 2012.]

Projections of the electronic

density in configuration space :

Electronic density of a frozen planet

state of the N = 6 series, in 2D configuration space.
10

Coupling between the FPS and the bound states

Frozen planet states are not coupled to helium ground state through one
photon processes. However, they are coupled to single excited states.

Photoionization cross sections for the N = 4, n = 1 FPS state with

different bound states.
[I. Guzman, Undergraduate thesis, Universidad del Valle, 2015.]
11

Driven 2D helium atom

(
H=

H0 + F (x
1 + x2 ) cos(t)

H0

F
i

x1

x2

H(t + T ) = H(t),
=

|(t)i =

position gauge

sin(t)

velocity gauge

T = 2/

cj eij t |j (t)i

Floquet theorem

where
HF |j (t)i = j |j (t)i,
|j (t + T )i = |j (t)i

HF = H i

|j (t)i =

eikt |kj i

k=

(
(H0 + k)|kj i +
(H0 + k)|kj i +

k1
k
F
(x1 + x2 )(|k+1
j i + |j i) = j |j i
2
k1
k
F
( + x 2 )(|k+1
j i |j i) = j |j i
2 x1

[M.G. Floquet, Annales de lcole Normale Suprieure 12 (1883) : 47]

12

By applying the regularization and complex rotation we obtain :

k1
k
H(k) ()|kj i + F()(|k+1
j i + |j i) = j J|j i

GEVP :

AX i = i J X i
Dimension of the matrix A
For instance :

nbase = 200
k = 0, 1, 2, 3

l = 0, 1, 2

a = 220804
b = 21481

memory = 76GB
whereas for the unperturbed
system :
a = 110402,

b = 4280

memory = 7.6GB
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Driven 2D frozen planet states

Projection of the electronic density of the outer electron of the Floquet

state associated with the N = 6, n = 3 FPS on the classical phase space.
Driving field amplitud F = 5.5 10 6 a.u.
Frequency = 0.0012 a.u.
E = 0.0731723 a.u.
life time 100 2

Matrix size :
nbase = 200
a = 527538
b = 51004
memory=430GB

[J. Madroero et al., Adv. At. Mol. Opt. Phys. 53 (2006) : 33]
14

How we proceed
We need to solve
H|i = E|i,

H = H0 + F

First we solve the unperturbed system :

H0 |l i = l |l i,
X l
|l i =
n |n, li,

l = lmin , . . . , lmax
|n, li = |n1 , n2 , n3 , n4 , li

The solution for the driven problem is expanded as

XX
|i =
li |li i
i

Matrix elements for the Hamiltonian

0

hli |H|lj i = hli |H0 |lj i + hli |F |lj i

0

hli |H0 |lj i

0

hli |F |lj i

li i,j l,l0

hli |m, lihm, l|F |n, l0 ihn, l0 |lj i

m,n

X
m,n

l
0
l
i,m j,n hm, l|F |n, l i

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For instance :

nbase = 200
k = 0, 1, 2, 3

l = 0, 1, 2

a = 220804
b = 21481

memory = 76GB

a = 820
b0 = 410

memory = 5.4MB
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Partial results
I

Complete system
Field-induced resonance state
for N = 3 :
E = 0.3425432 a.u.
/2 = 3.77 106

Field-induced resonance state

for N = 6 :
E = 0.0731723 a.u.
/2 < 106

Matrix :

Matrix :

a = 131588
b = 17055
memory=36GB

a = 527538
b = 51004
memory=430GB

[J. Madroero, Dissertation, Ludwig-Maximilians-Universitt Mnchen, 2004.]

I

Reduced system
Field-induced resonance state
for N = 3 :
E = 0.34253 a.u.
/2 = 3 106

Field-induced resonance state

for N = 6 :
E = 0.0731 a.u.
/2 106

Matrix :

Matrix :

a = 3205
b = 700
memory=36MB

a = 7948
b = 1729
memory=220MB
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3D description (unperturbed system)

The solution of the Schrodinger equation
H(~r1 , ~r2 ) = E(~r1 , ~r2 )
is expanded in a configuration interaction basis,
XX X
L,M (~r1 , ~r2 ) =
kl11sl2kLM
2s n1 n2
l1 ,l2

n1 ,n2

Snk1s
(r1 )
1 l1
r1

Snk2s
(r2 ) LM
2 l2
l1 l2 (
r1 , r2 )
r2

where
A=

1 + 12 P12

,
2

12 = 1

projects onto singlet or tripet states.

[J. Eiglsperger, Dissertation, Technische Universitt Mnchen, 2010.]
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k
The radial functions Sn,l
(r) are Sturmian functions defined by
k
Sn,l
(r)

k
= Nn,l
rl+1 ekr L2l+1
nl1 (2kr)

The approach uses distinct dilation parameters kns for the Sturmian
functions of the inner and outer electron.
Angular part
LM
r1 , r2 )
l1 ,l2 (

hl1 m1 l2 m2 |LM iYl1 ,m1 (

r1 )Yl2 ,m2 (
r2 )

m1 ,m2

After using the complex rotation we obtain :

GEVP :

H = E S

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Some results for the 3D unperturbed helium

Doubly excited 1P e states in helium sequence (Z = 3, 4).
Z=3

N=3

N=4

Z=4

This work
E(a.u.)
-0.831 281 25
-0.755 785 7
-0.661 038 52
-0.625 089
-0.598 310 3
-0.579 630 3

Ho and Bhatia
E(a.u.)
-0.831 281 4
-0.755 788 8
-0.661 038 6
-0.625 090 4
-0.598 310
-0.579 631

-0.476 220
-0.448 152 7
-0.409 147
-0.392 434 4
-0.374 205 21
-0.355 145 11

-0.476 219
-0.493 152
-0.409 139
-0.392 434
-0.374 205 1
-0.355 145 1

This work
E(a.u.)
-1.548 700 4
-1.442 538
-1.224 129 1
-1.170 311 9
-1.096 902 4
-1.068 836 7

Ho and Bhatia
E(a.u.)
-1.548 700
-1.442 543 02
-1.224 129
-1.170 313 3
-1.096 902
-1.068 837

-0.8431015
-0.788082
-0.72671
-0.6992265
-0.6700796
-0.6525476

-0.843 102
-0.788 071
-0.726 131
-0.699 226
-0.670 078 7
-0.652 547

[Y. K. Ho and A. K. Bhatia, Phys. Rev. A 47 (1993), 2628.]

Driven 3D helium...
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Summary
What we have :
2D :
I

Full code for the driven system, non appropriate for highly
excited states.

Code for the reduced driven system (in testing period).

3D :
I

Code for the unperturbed system.

Whats next :
I

Finish testing the 2D code.

-How to improve the convergence ?
-How to identify the relevant states ?

Implement the code for the driven 3D system.

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Thank you !

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