Ab-initio molecular dynamics studies of laser- and collision-induced processes in multielectron diatomics, organic molecules and fullerenes [Elektronische Ressource] : ionization, isomerization, fragementation and fusion / vorgelegt von Jan Handt

Ab-initio molecular dynamics studies of laser- and collision-induced processes in multielectron diatomics, organic molecules and fullerenes [Elektronische Ressource] : ionization, isomerization, fragementation and fusion / vorgelegt von Jan Handt

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onErlangungLfürrerumTheoretisc1978heFPhhenysiknat.)ForenakultätbMathematikragmentationundDissertationNaturwissenscakhaftenDoT(Dr.ecorgelegthniscHandthe18.UnivLutherstadtersitätDresdenDresdenFAb-InitioandMoleculausionrzurDynamicsdesStudiesademiscOfGradesLaser-ctorAndnaturaliumCollision-Inducedrer.ProvcessesvInJanMultielectrongebDiatomics,amOrganicJuliMoleculesinAndWittenFergullerenes2010Ionization,InstitutIsomerization,GutacVDr.hEingereictter:amhael15.01.2010am1.2.GutachhProf.ter:Jan-MicProf.RostDr.erteidigtRüdiger18.10.2010SchmidtcollisionmoendenceThiselowerimenorkofpresenvtsloapplicationsandofleadingan(Nab-initioandmolecularIndynamicswholemethotransferd,found,thequanso-calledcalculationsnona-thediabaticAbstractquanoftumtomolecularupdynamicsexcitation(NA-QMD),(Cforfullerene-fullerenevrstariousanmolecularvibrationalsystemswwithcollisions,manwyreproelec-basictronicinandasnhighuclearexcitationdegreesThisoftationfreedom.theTherebultielectronicy,,thethemoleculesntationucleigianwillthebinemtreatedsecondclassicallyareandfortheinelectronsofwithimpacttime-depconcerningendenelectronictpdensitFyenergeticfunctionalistheorya(TD-DFT)(!

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Institut
f?r
Theoretisc
des
Jan
F
he
naturalium
Ph
in
ysik
usion
F
Grades
akult?t
v
Mathematik
am
und
erg
Naturwissensc
and
haften
zur
T
ademisc
ec
ctor
hnisc
rer.
he
v
Univ
geb
ersit?t
Juli
Dresden
Witten
Ab-Initio
2010
Molecula
ragmentation
r
F
Dynamics
Dissertation
Studies
Erlangung
Of
ak
Laserhen
And
Do
Collision-Induced
rerum
Pro
(Dr.
cesses
nat.)
In
orgelegt
Multielectron
on
Diatomics,
Handt
Organic
oren
Molecules
18.
And
1978
F
Lutherstadt
ullerenes
b
Ionization,
Dresden
Isomerization,
LEingereic
h
t
am
am
ter:
hael
15.01.2010
Gutac
1.
Dr.
Gutac
V
h
2.
ter:
h
Prof.
Prof.
Dr.
Jan-Mic
R?diger
Rost
Sc
erteidigt
hmidt
18.10.20102 2 2
2
60
applications
of
an
collisions
features
diatomics
ab-initio
er").
molecular
regimes
dynamics
of
metho
t
d,
o-dimensional
the
in
so-called
dep
nona-
isomerization
diabatic
presen
quan
time
tum
and
molecular
it
dynamics
duce
(NA-QMD),
the
for
energetic
v
up
arious
ionization
molecular
O
systems
(N
with
de
man
the
y
estigated,
elecrange
tronic
cities
and
("stopping
n
w
uclear
that
degrees
mo
of
titativ
freedom.
scattering
Thereb
as
y
t.
,
electronic
the
to
n
orien
uclei
of
will
m
b
ork
e
),
treated
organic
classically
H
and
breathing
the
fullerenes
electrons
).
with
part,
time-dep
in
enden
the
t
the
densit
relev
y
v
functional
the
theory
energy
(TD-DFT)
o
in
or
basis
(adiabatic)
expansion.
surprisingly
Dep
t
ending
phenomenological
on
can
the
en
actual
the
system
fusion
and
ed
ph
microscopic
ysical
ell
pro
exp
cess,
or
w
collisions,
ell
vibrational
suited
predicted,
basis
ultifragmen
sets
complete
for
tation
the
endence
K
the
ohn-Sham
of
orbitals
ultielectronic
has
(N
to
,
b
w
e
the
ts
of
)
molecules
the
This
t
c
hosen.
and
F
gian
or
excitation
the
the
ionization
mo
pro
in
cess
(C
Abstract
a
no
In
v
second
el
fullerene-fullerene
absorb
are
er
v
acting
for
in
rst
the
in
energy
whole
space
of
as
an
w
impact
ell
elo
as
concerning
additional
vibrational
basis
electronic
functions
transfer
will
p
b
w
e
F
used
lo
dep
energetic
ending
collisions,
on
is
the
found,
laser
a
frequency
w
.
(!),
In
collision
the
del
rst
repro
part
(ev
of
quan
the
ely)
applications,
basic
a
of
large
and
v
observ
ariet
in
y
fully
of
calculations
dieren
w
t
as
laser
the
-induced
erimen
molecular
F
pro
high
cesses
(nonadiabatic)
will
the
b
and
e
excitation
in
are
v
leading
estigated.
m
This
tation
concerns,
to
the
atomization.2 2
2 2
60
60 60
60 60
70 70
60 60
.
.
.
.
higher
.
.
Dep
.
.
.
.
.
C
.
.
.
.
.
Laser
.
.
.
.
.
.
.
87
.
.
.
.
.
3.3
.
C
.
.
.
.
.
.
.
.
.
.
.
C
.
w
.
usion
.
.
.
.
.
.
.
5
.
.
.
.
.
.
.
fullerenes
.
53
.
.
.
Resonan
.
.
.
.
.
.
.
.
.
.
.
.
.
.
7
diabatic
2
.
Theo
.
ry:
scattering
Ab-initio
.
Molecula
.
r
.
dynamics
.
.
F
.
.
.
.
.
tation
.
.
.
94
.
.
.
.
.
.
.
.
.
.
.
e
.
.
.
.
.
e
.
.
.
.
.
state
.
.
.
.
.
.
.
t
.
.
.
.
.
de
.
.
.
.
.
3.3.4
.
.
.
.
.
.
.
4
.
.
.
.
.
.
.
.
11
.
2.1
.
Molecular
.
dynamics
.
metho
.
ds
C
.
F
.
.
.
.
.
70
.
jectory
.
.
.
.
.
.
.
for
.
.
.
C
.
scattering
.
.
.
.
.
of
.
.
.
92
.
duction
.
impact
.
.
.
.
.
Ion-F
.
.
.
.
.
.
.
.
11
.
2.2
.
A
.
diabatic
.
Quan
.
tum
.
Molecular
3.2.3
dynamics
tation
(QMD)
states
.
.
.
.
.
.
.
t
.
excitation
.
.
.
.
.
.
.
.
.
The
.
erties
.
.
.
.
.
.
.
.
.
.
16
54
2.3
and
Nonadiabatic
excitation
Quan
.
tum
.
Molecular
.
dynamics
59
(NA-QMD)
breathing
.
.
.
.
.
.
.
.
.
.
.
.
.
e
.
.
.
.
.
.
.
.
17
.
2.3.1
.
The
.
mixed
fullerene
classical-quan
.
tum
.
equations
.
of
.
motion
.
.
.
.
.
.
.
.
.
.
4.1
.
.
.
.
.
.
.
.
.
.
.
.
17
.
2.3.2
.
NA-QMD
69
and
.
ionization
.
.
v
.
.
.
.
.
.
.
.
.
.
.
A
.
classical
.
del
.
.
.
.
.
.
.
4.1.3
.
+
.
:
.
ersus
.
temp
.
.
.
83
.
.
.
.
.
v
.
.
.
.
.
.
20
.
2.3.3
.
Denition
Nonadiabatic
of
collisions
ph
.
ysical
.
prop
.
erties
F
in
in
the
92
NA-QMD
on
approac
.
h
.
.
.
.
.
.
.
.
Comparison
.
collisions
.
.
23
.
2.3.4
.
Numerics
.
.
ok
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
47
.
Selectiv
.
fragmen
.
via
.
excited
.
.
.
.
.
.
.
.
.
.
.
.
.
51
.
Gian
.
collectiv
.
vibrational
.
in
.
.
25
.
3
.
Laser-induced
.
dynamics
.
.
.
.
.
.
.
.
3.3.1
.
ground
.
prop
.
of
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
3.3.2
.
t
.
nonresonan
.
laser
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
3.3.3
.
excited
.
mo
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
61
.
Pump-prob
.
scenario
.
.
.
.
29
.
3.1
.
Ionization
.
of
.
diatomics
.
.
.
.
.
.
.
.
.
.
.
.
.
.
63
.
Collision-induced
.
dynamics
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
69
.
A
.
dynamics
29
.
3.1.1
.
The
.
ground
.
state
.
prop
.
erties
.
of
.
N
.
1
.
and
.
O
.
ts
.
.
.
.
.
.
.
.
4.1.1
.
.
.
+
.
.
.
:
.
usion
.
ersus
.
.
.
.
.
.
.
.
.
.
31
.
3.1.2
.
W
.
a
.
v
.
elength
4.1.2
Dep
t
endence
o-dimensional
of
tra
the
mo
Ionization
.
.
.
.
.
.
.
.
.
.
.
.
.
.
75
.
C
.
.
.
C
.
.
.
F
.
v
.
scattering
.
nite
.
eratures
35
.
3.1.3
.
Orien
.
tation
4.1.4
Dep
.
endence
+
of
.
the
:
Ionization
usion
.
ersus
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
4.2
.
dynamics
.
fullerene-fullerene
.
.
.
.
.
.
+
.
.
.
collisions
.
.
.
.
4.2.1
.
ragmen
.
regimes
.
C
.
37
3.2
C
Intro
Isomerization
and
.
fragmen
.
tation
.
of
.
organic
.
molecules
.
.
.
.
4.2.2
.
endence
.
the
.
parameter
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
42
.
3.2.1
4.2.3
The
with
ground
ullerene
state
.
prop
.
erties
.
of
.
the
.
diimide
.
molecule
.
N
.
ten
95
.
Outlo
.
.
H
.
Con
.
.
.
.
.
.
.
.
.
.
.
.
.
43
.
3.2.2
.
Isomerization
.
via
.
the
.
1st
.
excited
.
state
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
972 2
60
60
A
.
.
.
.
des
.
.
.
.
.
.
.
jectory
.
.
.
.
.
.
.
.
.
.
.
.
.
fullerene-fullerene
.
.
.
.
.
.
.
107
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
de
.
.
.
.
.
.
endix
107
.
.
.
.
.
.
.
.
.
109
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
111
.
asymmetrical
.
Analytical
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
99
.
A.1
.
Num
.
b
.
er
.
of
Normal
excited
.
electrons
.
in
.
TD-DFT
.
.
.
.
.
.
.
.
.
.
Normal
.
C
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
endix
.
.
.
.
.
.
.
.
.
.
99
.
A.2
.
Visualization
.
of
.
the
.
electron
.
dynamics
.
.
.
.
.
.
.
.
Classical
.
del
.
collisions
.
111
.
for
.
.
.
.
.
Bibliography
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
101
.
A.2.1
.
The
.
electron
.
lo
.
calization
.
function
.
(ELF)
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
B.1
.
mo
.
analysis
.
.
.
.
101
.
A.2.2
.
The
.
dimers
.
N
.
ts
.
and
.
O
.
ten
.
.
.
.
.
.
.
.
.
.
B.2
.
mo
.
of
App
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
App
.
C
102
.
A.2.3
.
The
.
C
.
Con
.
.
.
.
.
6
.
molecule
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
C.1
.
tra
.
mo
.
for
.
fullerene-fullerene
.
.
104
.
App
C.2
endix
solution
B
symmetrical
.
collisions
.
.
.
.
.
.
.
113
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
.
11512 1510 −10
2
+
2
adv
ances
ha
enden
quan
use
v
b
e
short
b
and
een
p
made
2.1
in
a
the
desired
exp
prop
erimen
a
tal
parallel
study
only
of
[25].
nonadiabatic
atomic
pro
more
cesses
b
in
whic
atoms,
scale,
molecules
attosecond
and
ab
clusters,
n
e.g.
at
ab
e
o
the
v
with
e-threshold
Therefore,
ionization
n
(A
tem
TI)
of
[1]
e
resp.
the
ab
or
o
k
v
y
e-threshold
tuned
disso
system
ciation
On
(A
ecome
TD)
b
[2],
and
high
On
harmonic
the
generation
man
(HHG)
freedom
[3],
Up
c
v
harge
equation
resonan
only
t
b
enhanced
[21],
ionization
the
(CREI)
F
[4],
the
molecular
is
alignmen
treatmen
t
dynamics
[5],
the
selectiv
tough
e
v
b
enden
ond
ev
breaking
b
[6]
metho
or
k
Coulom
the
b
uclear
explosion
e
[7].
dynamics
Esp
manipulated
ecially
sequence
,
pulses
the
e
rapid
steer
progress
to
in
tum
the
attosecond
creation
has
and
ossible
manipulation
Harmonic
of
to
fem
pulses
tosecond
study
laser
[19,
pulses
other
with
calculations
high
of
in
systems
tensities
electronic
(
degrees
large
inheren
decades,
hallenging
o
no
w
um
t
time
last
Sc
the
can
During
n
duction
large
W
This
cm
done
tro
en
In
to
in
theory
has
single
fully
umerics
hanically
molecular
constrain
smallest
recen
)
has
laser
lead
een
to
tum
the
an
new
v
eld
[23,
of
vibrational
fem
appro
tosecond
a
ph
of
ysics
in
[8]
metho
or
coupling
fem
ultielectron
to
still
c
(see
hemistry
an
[9].
The
Ultrashort
time-
ligh
electronic
t
ho
pulses
can
can
mean
no
man
w
c
b
lik
e
o
used
ximation,
to
hemes,
follo
electronic
w
n
in
w
real-time
v
the
pac
primary
ets
ev
can
en
e
ts
b
of
a
man
of
y
laser
c
with
hemical
relativ
but
phases,
also
h
ph
the
ysical
in
or
the
biological
quan
pro
state.
cesses.
the
Pump-prob
time
e
it
exp
b
erimen
p
ts
to
allo
High
w
Generation,
for
oth
the
generate
study
XUV
the
[18]
vibrational
to
dynamics
molecular
in
erties
diatomics
20].
and
the
more
hand,
complex
initio
molecules
of
on
dynamics
the
atomic
fem
molecular
tosecond
with
scale
y
using
resp.
momen
uclear
tum
of
imag-
is
ing
tly
tec
c
hniques
task.
for
to
electrons,
w,
e.g.
maxim
time-resolv
the
ed
e-dimensional
photo
dep
electron
t
sp
hr?dinger
ectroscop
(TDSE)
y
b
(TRPES)
propagated
[10],
umerically
and
on
ion
scaled
fragmen
computers.
ts
has
[1113].
een
In
for
addition,
laser-driv
also
He-atom
the
e.g.
con
compare
trol
ertubation
of
for
atomic
N-photon
and
ionization
molecular
n
systems,
[22].
e.g.
or
c
systems,
hemical
the
reactions,
molecules,
is
D
1
the
sub
a
ject
eld,
of
b
recen
treated
t
quan
researc
mec
h.
without
In
y
optimal
t,
con
ery
trol
tly
exp
24].
erimen
the
ts
motion
the
usually
molecular
ximated
resp
y
onse
classical
is
t
manipulated
the
b
uclei
y
molecular
adaptiv
(MD)
e
ds
closed-lo
The
op
to
feedbac
m
k
sys-
sc
is
hemes
a
using
problem
phase-shap
Sec.
ed
for
laser
o
pulses
erview).
in
calculation
order
the
to
indep
optimize
t
c
and
hemical
structure,
reactions
w
[14,
er,
15].
b
In
done
Coheren
while
t
y
Con
y
trol
tum
[16]
hemical
resp.
ds
Quan
e
tum
Hartree-F
Conc
trol
appro
[17]
or
sc
sophisticated
+
22
tro
duction
metho
the
v
t
ds
appro
lik
Densit
e
or
conguration-in
ha
teraction
a
(CI),
additional
m
een
ulticongurational
ionization,
self-consisten
[37
t
w
eld
the
theory
tial
(MCSCF),
NA-QMD
or
the
coupled-cluster
uclei.
theory
(LSD
(CC)
to
[26].
y-
Ho
the
w
et
ev
in
er,
arian
all
systems,
these
the
metho
[41,
ds
b
are
equations
dealing
The
with
(to
the
y
man
y
y
terms
electron
oten
w
ell
a
umerically
v
ionization
efunction
the
in
1
one
b
or
[31]
another
in
w
hanism
a
and
y
attempt
.
quan
Therefore,
[40].
their
NA-QMD
applications
as
are
classical
limited
een
due
ation,
to
uclear
the
it
large
non
computational
hange-correlation
eort,
enden
esp
appro
ecially
p
in
v
com
to
bination
laser
with
dev
molecular
hmidt
dynamics
motion
or
ariational
ev
y-dep
en
acting
explicitly
exc
time-dep
enden
enden
(LD
t
enden
situations.
e
There
whole
are,
e
ho
w
w
of
ev
restricted
In
systems
elds
er,
a
The
few
tosecond
metho
w
ds,
metallic
for
fullerenes
example
harge
the
collisions
time-dep
reaction
enden
collisions
t
een
m
or
ulticonguration
including
theory
tak
[27],
accoun
describing
eects
the
uclear
m
early
ultielectron
of
dynamics
,
of
er,
a
to
molecule
ecause
in
of
laser
e
elds.
ed
Muc
energy
h
done
more
of
ecien
vy-ion
t,
F
ho
as
w
e
ev
metho
er,
the
is
o-
the
the
use
K
of
b
a
b
theory
of
equiv
tials
alen
t
t
of
to
its
the
en
TDSE
e.g.

teractions)
the
b
time-dep
ed
enden
and
t
44].
densit
equations
y
obtained
functional
general
theory
leading
(TD-DFT)
elo
[28],
t)
whic
the
h
the
can
or
cop
correlation
e
the
with
Lo
the
Appro
man
as
y
the
electron
LD
systems
ha
b
een
y
Later,
reducing
has
the
to
problem
man
of
47].
the
er,
m
w,
ultidimen-
applications
sional
NA-QMD
man
one
yb
o
o
e
dy
or
w
strong
a
48,
v
of
efunction
in
to
pulses
the
treated
propagation
[50].
of
in
the
clusters
one-particle
and
densit
[32],
y
c
.
transfer
The
ion-cluster
rst
[3336],
com
the
bination
mec
of
in
TD-DFT
b
with
w
classical
ions
MD
molecules
has
clusters
b
39]
een
an
dev
to
elop
e
ed
to
and
t
realized
tum
b
in
y
n
Saalmann
motion
and
This
Sc
v
hmidt
t
[29].
the
This
theory
metho
ho
d
ev
w
w
as
restricted
named
closed
Non-A
b
diabatic
the
Quan
equations
tum
motion
Molecular
v
Dynamics
b
(NA-QMD).
deriv
With
from
this
total
theory
conserv
it
as
b
in
ecame
theory
p
n
ossible
hea
to
collisions
treat
42].
sim
urthermore,
ultaneously
w
and
an
self-
ximativ
consisten
(i.e.
tly
ab-initio)
(quan
d,
tum-mec
ecause
hanical)
exc
electronic
p
excitations
ten
and
in
(classical)
time-dep
n
t
uclear
ohn-Sham
motion
has
in
een
nite
ximated
atomic
y
man
sum
y-b
atomic
o
oten
dy
[29].
systems.
presen
F
ab-initio
rom
ersion
the
the
historical
and
p
extensions
oin
op
t
systems
of
include
view,
also
the
in
NA-QMD
ha
of
e
Saal-
een
mann
elop
and
b
Sc
Kunert
hmidt
Sc
represen
[43,
ted
Here,
the
classical
rst
of
attempt
are
to
b
generalize
the
the
v
till
principle
then
to
existing
(v
QMD-
cit
metho
enden
ds
correction
(lik
in
e
forces
the
on
Car-P
n
arrinello
F
Theory
the
[30])
hange
to
p
couple
tial
explicitely
time-dep
quan
t
tum-mec
cal
hanically
y
electronic
ximation
excitations
A)
and
w
transitions
as
(i.e.
Spin-dep
non-adiabatic
t
pro
A
cesses)
A)
with
v
classical
b
n
n
uclear
realized.
motion.
the
So
formalism
it
b
b
extended
ecame
describ
generally
also
p
y-electron
ossible
[45
to
Ho
in
ev
v
up
estigate
no
non-adiabatic
most
pro
the
cesses
of
in
ab-initio
atomic
are
man
to
y-b
or
o
w
dy
electron
systems
lik
on
H
8
a
fully
H
microscopic
in
basis,
laser
lik
[43,
e
49].
the
isomerization
electronic
eth
and
lene
n
fem
uclear
laser
"stophas
ping
een
p
as
o
ell
w
Multielectron
er"
large2 2 2 2
60
~ =e =m =
1e
b
een
examined
clusters
of
p
up
the
to
electron
no
application
w,
of
but,
excitation
represen
A-C.
t
to
the
the
main
discussed
topics
(ev
of
fully
the
high
presen
tation
t
ations
thesis.
structure
The
ear
outline
onds
of
formalism
the
ohn-Sham
thesis
ortan
is
w
as
del
follo
ely)
ws:
observ
In
w
Chapter
[54,
2,
the
rst
leading
a
plete
general
details
o
in
v
visualization
erview
the
of
(ELF)
dieren
a
t
y
(ab-initio)
A.2).
molecular
the
dynamics
appropriate
metho
whic
ds
Therefore,
is
the
presen
t
ted
in
(Sect.
(
2.1).
collision
The
repro
basic
quan
framew
basic
ork
and
of
in
QMD
calculations
and
as
NA-QMD
erimen
are
F
summarized
(nonadiabatic)
in
and
Sect.
are
2.2
m
and
to
2.3,
[56].
resp
tec
ectiv
analytical
ely
presen
.
App
In
them,
Chapter
the
3,
dynamics
a
of
large
calization
v
will
ariet
b
y
ery
of
to
dieren
hemical
t
(App
laser
k
-induced
t
molecular
or
pro
ts
cesses
hoice
will
[46]
b
the
e
are
in-
eac
v
ted
estigated.
this
This
p
concerns,
b
the
erately
orien
Throughout
tation
are
dep
strong
endence
phenomenological
of
mo
the
can
ionization
duce
of
en
m
titativ
ultielectronic
the
diatomics
features
(N
fusion
v
scattering
,
ed
O
the
ha
microscopic
)
as
[51],
ell
the
in
isomerization
exp
of
t
organic
55].
molecules
or
(N
energetic
collisions
collisions,
H
electronic
cluster
vibrational
)
regimes
[52]
predicted,
and
to
the
ultifragmen
gian
up
t
comexcitation
atomization
of
Most
the
the
breathing
hnical
mo
or
de
deriv
in
are
fullerenes
ted
(C
the
non-adiabatic
endices
or
Among
)
the
[53].
of
In
electronic
Chapter
and
4,
with
fullerene-fullerene
concept
collisions
the
are
lo
in
function
v
[57]
estigated,
app
for
to
the
e
rst
v
time
useful
in
ol
the
displa
whole
c
range
b
of
[58]
relev
endix
an
The
t
ey
impact
oin
v
of
elo
QMD
cities
NA-QMD
concerning
represen
the
the
vibrational
c
and
of
electronic
basis
energy
in
transfer
h
("stopping
K
p
orbitals
o
expanded.
w
for
er").
h
F
presen
or
in
lo
thesis
w
imp
energetic
t
(adiabatic)
oin
collisions,
will
it
e
is
sep
surprisingly
and
pulses,
detail.
not
this
atomic
ork
e
units
if
used
stated
laser
o-dimensional
in
(!),
found,
9
that
a
a.u.)
t
not
w
otherwise.