Attosecond electron dynamics in strong laser fields

Stefanie Grfe
Institut fr Theoretische Physik Technische Universitt Wien

Timescales
Age of the universe My age Age of this talk Atomic- & Molecularphysics 1 Attosecond

1018 s

1 year

1s

10-18 s

Femtochemistry
micro 10-6 nano 10-9 Radiative transitions Rotations pico 10-12 Vibrations H2 vibration H2 vibration ~ 16 fs ~ 16 fs

Attophysics
atto 10-18 sec

femto 10-15 Fast electronic dynamics World record: World record: shortest light shortest light pulse pulse ~ 80 as ~ 80 as

ElectronElectronorbit orbit in H-atom in H-atom ~ 25 as ~ 25 as

Krausz, Ivanov, 2009

Strong infrared laser pulse

Number of photons Electric field 1015 1000 MV/cm

E (t ) = F f (t ) cos(t + )

Extension in space 1-10 m Radiation pressure 1 Million Atmospheric pressure (106Bar)

Infrared laser pulse (IR)

Mariana trench: 1000 Bar

Physics in Strong Laser Fields and Attophysics

Ionization in Strong Fields I: Tunneling

Atom (without laser field) V(x)

IP

Ionization potential

Atom with strong, external field T = 2.7 fs

+ Strong IR field 800 nm, 5fs, 1014 W/cm2 V(x) + x.E cos t

Ionization II: Multiphoton Channel

Keldysh Theory
Tunneling or Multiphoton? (Keldysh, 1967)

IP = 2U P

vel = = F

2I P F
Tunneling time

<< 1
Ionization rates

>> 1
Multi-photon

tunnel

2(2 I P ) exp 3F

32

Tunnel

multi photon I

IP +1

Ponderomotive potential

E (t ) = F f (t ) cos(t + )

F2 UP = 4 2

After ionization?
Electron in the laser field can acquire in average 2 UP of energy

F2 UP = 4 2
Trajectories follow the vector potential of the laser field neglecting atomic potential (strong field approximation) Final momentum determined by the vector potential at the time of birth

Krausz, Ivanov, 2009

Re-scattering zoo

Krausz, Ivanov, 2009

Krausz, Ivanov, 2009

Quantum picture: re-scattering

3-Step Model

3. Recombination 2. Re-collision

1. Laser ionization

E cos t
1. 2. 3. Laser-ionization: A strong, infrared laser pulse induces tunnel ionization Propagation of the free electron in the laser field. As soon as the laser field changes its direction, the electron is accelerated back and re-collides with the parent ion. Recombination of the electron with the parent ion under emission of high energetic radiation. As this process is periodic, a train of high order harmonics of the laser frequency is produced. {Corkum, 1993}

Electron Re-Collision - Trajectories

Erec/Up , Up=E2/42

Recollision energy (Chirp of the electron wave-packet)

Krausz, Ivanov, 2009

Time-Frequency Analysis

Krausz, Ivanov, 2009

Electron Re-collision generates high-harmonics

Emission periodic in time Periodic in frequency

Emission of high energetic radiation at each halfcycle of the laser pulse

Only odd harmonics of the laser frequency

Attosecond pulses from High-Harmonics

Spectral Filtering make attosecond pulses

Krausz, Ivanov, 2009

Reminder: Emission times

Emission of high-harmonic radiation occurs after each laser half-cycle: After spectral filtering not one attosecond pulse is obtained but a train of attosecond pulses

Single attosecond pulses

To make one single attosecond pulse, the number of recollisions has to be reduced.

h max = 3.2 U P + I P I Laser 2

Laser pulses with only few cycles

Stabilization of the carrier-envelope phase

Krausz, Ivanov, 2009

Oscillating dipole

r d (t ) = r

Harmonic spectrum:

~ && S ( ) = F d (t )

[ ]

Harmonic spectrum contains full information about electronic wavefunction

Krausz, Ivanov, 2009

Orbital-Tomography

Measuring the harmonic spectrum (and phase), it is possible to obtain information about the electronic wavefunction

EXPERIMENT

THEORY

Itatani et al., 2004

Molecules in strong laser fields

Ionization in strong fields: molecules

Field-free molecule, z.B. H2

Molecule with intense external field

E cos t

V(x,R) + x.E cos t

Enhanced ionization

Molecule with intense external field

E cos t

Zuo, Bandrauk, 1995

Electrons in a double well potential

u g
+ + + R + R Orbitals with even (|g) und odd (|u) symmetry

Laser + +

+ left =

1 2

(g

+ u

+
1 2

right =

(g

Positive or negative superposition of the orbitals |g and |u means that the electron is localized in the right or left potential well.

Recent experiment in H2
H2+

H+ + H H+H H2

M.F. Kling et al., Science 2006, 312, 246-248.

Born-Oppenheimer picture
Barrier comes up around R = 5 , the electronic 2+ H2 states are degenerate and tunneling freezes out!

10

E F

1 R

1
V(R) [eV]

2 XUV(T)
-10

g
R
u

~ 2 + A u ~2 + X g

H2

-20

H2
-30 0 1

1 R 2

+ g

3 4 -10 R [10 m]

Grfe, Ivanov, PRL 2007

Model system

10

H (t ) = Tx + TR + V ( x, R ) + x E (t )
V ( x, R ) =
V(R) [eV]

H2
F
0

2+

1 R

(x R / 2)2 + ( R)

XUV(T)
-10

1 nuclear and 1 electronic coordinate

-20

~ 2 + A u ~2 + X g

H2

R []

Population dynamics
Efficient population transfer

Persson, Burgdrfer, Grfe, New J. Phys. 2009

Electron densities

Localization very efficiently

Persson, Burgdrfer, Grfe, New J. Phys. 2009

Experimental Realization?

Experimental realization
E = 5-24 V/cm E = 5-24 V/cm B = 6-20 G B = 6-20 G E || B E || B

jet dump
m ea rb e as l

mirror

ion detector electron detector supersonic gas jet

COLTRIMS

Outlook

Open questions

Transferring charge (electron or hole) along a chain: antenna-like systems?

Dynamics in multi-electron systems? Role of electron-correlation vs. controllability? Chain-like molecules can be e.g. conjugated hydrocarbons, where electron density is parallel above and below the molecular plane

C C C

Acknowledgement
Prof. Dr. Joachim Burgdrfer Dr. Emil Persson Markus Pichler Thomas Hisch Prof. Dr. Werner Jakubetz Prof. Dr. Andrius Baltuska Dr. Markus Kitzler Dr. Daniil Kartashov TU Wien, Experiment Universitt Wien TU Wien

Acknowledgement: Deutsche Akademie der Naturforscher Leopoldina (Nationale Akademie der Wissenschaften), sterr. Fond fr wissenschaftliche Forschung: SFB ADLIS and Lise-MeitnerProgramm