Ionisation of Carbon in Intense Laser Fields

Chris Calvert - MSci Project

Supervisor Prof. Ian Williams

Ionisation of Carbon in Intense Laser Fields

Chris Calvert - MSci Project
In collaboration with
Prof Ian Williams Dr B. Srigengan Mr M. Suresh Mr Jarlath McKenna Prof Roy Newell Dr Will Bryan Miss Elizabeth English Mr Joseph Wood Dr Andrew Langley Dr Edwin Divall Dr Chris Hooker Dr Edmund Turcu

Overview

Ionisation in Intense Laser fields

Motivation Theory

Experimental Investigation
Experimental Setup and Method Modelling the experiment

Previous work on C+ Ions - Motivation for current research Results and Analysis

Motivation
Why investigate Ionisation in Intense Laser fields?
Specific Ionisation dynamics. Multiple Ionisation, Rescattering. More details on these later

Why Carbon?
Spin Forbidden C+ C2+ transition? Multiple Ionisation/Rescattering? explain later

Ionisation in Laser Fields

Main processes
Single Photon Ionisation Multi Photon Ionisation (MPI) Field Ionisation
Increased Laser Intensity

Non sequential Ionisation

Rescattering Model

Single Photon Ionisation

Ionisation Energy

Low Intensity Process

hY

Ground State

X  hR p X

q 1

e

Multi Photon Ionisation

Ionisation Energy

For MPI to occur, successive photons must arrive within the lifetime of the preceding intermediate excited states. Higher Intensity Process

hY

Real Excited State

hY

Virtual Excited States Ground State

hY
hY

X  nhR p X

q 1

e

Field Ionisation
High Intensities > 1014 W/cm2
Electric field of the Laser tends towards the magnitude of the atomic field. Potential V(x) Quasi static model

Atomic potential well (no external field)

Potential experienced by the electron arises from the resultant of the Atomic potential well + instantaneous effect of Laser field.

e-

Range of Potential

Field Ionisation
Intensities > 1014 W/cm2

Potential V(x)

Laser field effectively lowers the potential barrier experienced by electron

Electric Field of Laser

e-

Range of Potential

Resultant Potential experienced by the electron = Atomic potential well+ instantaneous effect of Laser field

Field Ionisation
Intensities > 1014 W/cm2

Tunnelling Ionisation
-Barrier width becomes finite -Electron can escape by Quantum Mechanical tunnelling.

Electric Field of Laser

Potential V(x)

e-

Range of Potential

Resultant Potential experienced by the electron = Atomic potential well+ instantaneous effect of Laser field

Field Ionisation
Intensities > 1014 W/cm2

Over the Barrier Ionisation

-The resultant potential barrier Saturation Intensity (Is) corresponding to anelectron is experienced by the Ionisation potential Vip can be calculated lower than the energy of the classically to be electron state.

Electric Field of Laser

Potential V(x)

e-

4 Vbound) ( eV 9 -The electron is no longer ip v 10 2 I s the cm 2 ) ! 4effective potential (W by resultant Z ( a .u .) and is free to escape

Range of Potential

Resultant Potential experienced by the electron = Atomic potential well+ instantaneous effect of Laser field

Double Ionisation
Sequential Ionisation Two Succesive steps

XpX

1

e

X 1 p X 2  e 

Non Sequential Ionisation Simultaneous removal of two electrons

XpX

2

 2e

Can be explained by Re-collision or Re-scattering Theory (Corkum 1993)

Electron Re-Scattering Re-

Laser Field

This free electron is ejected from classically the free pulse. as it A primaryelectron is then regardedthe atom byas a laserparticleThis proceeds towards the continuum.. can be modelled quantum mechanically by tunnelling ionisation.

Electron Re-Scattering Re-

Laser Field

The electrons passes through the to it can collisionally core and Bothoscillating have enough energyion escape the atomic remove a As the electronnature of the laser field can cause the electron to be driven electron. doubleback towards the atomic secondionisation is observed core.

Electron Re-Scattering ReCorkum predicted As Ellipticity (e) of the incident radiation increases the probability of the first electron being driven back into the ion decreases probability of non sequential ionisation decreases

Therefore, for Linearly polarised light (e=0), there is a high probability of Non-sequential ionisation occurring. For Circularly Polarised light (e=1) this probability is small.

Experimental Investigation of Ionisation in Intense Laser Fields

Products of Interaction

Laser Ion Beam

The approach in this project is to focus Intense Femtosecond Laser pulses across an Ion Beam source and detect the resulting ionisation products.
Only two groups in the world use this Ion Beam approach method! Other groups use Gas targets

Experimental Investigation of Ionisation in Intense Laser Fields

Ion Beam Apparatus ASTRA Laser System

QUB Atomic and Molecular Division

Rutherford Appleton Laboratories (RAL), Oxfordshire

Ion Beam Apparatus

Analyser plates Selection Magnet

Discharge Ion source

Interaction Region

Needle Valve

Gas Source

Laser System
ASTRA (TA1)
Central Laser Facility, Rutherford Appleton Laboratories (RAL) Oxfordshire.

Interaction Region

Laser Path

Lens

Translation Stage

Ti:Sapphire, 50-55fs Pulses,800nm, 10Hz, Pulse Energies ~20mJ Peak Intensity ~ 5*1016 W/cm2

The Z-Scan Experiment Zor Intensity Selective Scan (ISS)

Ionisation Products

Laser Focal Point Ion Beam

z axis

The peak laser intensity (Io) occurs at the focal point. The intensity distribution changes along the z-axis. The z-dependence (and thus Intensity dependence) of the Ion yield can be found by varying the z-position of the Laser-Ion beam interaction.

The Z-Scan Experiment ZIonisation Products

Laser

Ion Beam

In practice the Laser Focus is moved with respect to the Ion beam by use of planar convex lens mounted on translation stage. This is carried out along the z-axis in steps of 0.25mm. 500 measurements (or shots) are taken at each z-position and the corresponding ion yields are recorded.

Z-Scan of
1.8

2+ C

Ion Yield

(Using Circularly Polarised Light)

Integrated Ion Yield (arb. units)

High intensity at focal point but small interaction volume

1.6 1.4 1.2 1.0 0.8 0.6 0.4 0.2 0.0 0 1 2 3 4 5 6

Good compromise between Intensity and Interaction Volume

Interaction Volume is large but Intensities are no longer high enough to cause Ionisation

z position (mm)

z axis

Modelling the Z-Scan

The Saturated Volume Model

The Intensity distribution of a focussed Laser beam is Lorentzian along the direction of beam travel, z, and Gaussian along the radial direction, r.

This can be modelled by the Isointensity Contour expression-

2 I0 2r Exp I (r , z ) ! 2 z 2 z 2 1 1 [ z0 0 z0

Io = Peak intensity of Laser, Beam waist radius

o

= 2f / d
o 2/

Rayleigh range zo= (

o

and zo are measurements of the focal point of the Laser)

Modelling the Z-Scan

The Saturated Volume Model

Expressing r as a function of I and z 2 [ rn ! s 0 2 2 1  z Ln z 0 In 2 I0 2 1  z z 0
1

The profile of the focussed laser can be plotted

In contour r

z
Laser Direction

The region contained in within each contour In has intensities > In The 3-D profile is generated by rotating these contours through 2

Modelling the Z-Scan

The Saturated Volume Model

4 Consider a 1+ to 2+ ionisation process. of the Ion beam is constant Assume that the current density Vip ( eV ) I s (W cm 2 ) ! 4 v109 2 Assume that this Ionisation process will occur for all I>Is Z ( a .u .)

Ion Yield at zi

Interaction Volume bounded by Ion w the number of 1+ ions bound by the ion beam and The 2+ Ion Yield at z =
i beam and the Is contour

the Is contour
r

Is shell
z Laser Direction

zi

Modelling the Z-Scan

The Saturated Volume Model

Original model (El-Zein 2001) used the interactionmodifications were Assuming Cylindrical Ion beam dimensions, new volume bounded made. A computer program was constructed to calculate the Interaction by a vertical slit and the laser contour. Volume at each z position.
Ion Beam direction into the screen Ion Beam Direction

0mm 0mm

7mm 7mm

10mm 10mm

Laser Direction

Hence a plot can be made to model the z-dependence of the Ion yield for a given Ionisation process.

This is the first Ion beam Sat Vol Model

Previous Z-Scan of C2+ Yield (Feb 2002) Z-

4.5E-11 4.0E-11 3.5E-11 3.0E-11 2.5E-11 2.0E-11 1.5E-11 1.0E-11 5.0E-12 0.0E+00 0 2 4 6 8 10 12 14

Ion Yield (arbitrary units)

Shoulder
+ Yield at large z values (z > 4mm)

Z position (mm)

Previous Z-Scan of C2+ Yield (Feb 2002) Z-Modelled by Saturated Volume Fit-

V o u e ( r itr ry un it ) lm a b a s

C2+ Ground

configuration 1s2 2s2 spin orientation oq oq

)mm( noitisoP Z

oo

rescattering spin orientation oq o

31-e4

31-e2

forbidden! C2+ 1Sp C3+ 2S (47.8eV) +Check for + Metastable C configuration 1s2 Time to investigate this!2s 2p2

31-e8

31-e6

confirmation of Some C2+ to C3+ depletion But this transition is spinMetastable transition occurs at small z values

nacs-Z ATAD

21-e1

21-e1

4Pp C 1 C+C+ 2Pp 2+ 2+ 1S(19eV) C S Looking (24.4eV) In order to model thefor yield Ion

stif emuloV fo muS etatsdnuorG +3C tif loV elbatsateM +2C tif loV etatsdnuorG +2C tif loV

+2C fo nacS-Z rof tiF evruC emuloV

21-e2 21-e2 21-e2 21-e1

Aim z=1mm The Ion yieldfeature The Shoulder from to z=4mm is explained requires the metastable by Detailed experiment to the expected groundstate transition transition C2+ Z-scan. examine

Shoulder
+ Yield at large z values (z > 4mm)

Research at RAL
15th 19th November

2 Main Z-Scan Results Z C2+ Yield C3+ Yield

3+ C
0.25

Z-Scan
Linear Circular

Integrated Yield (arb. units)

0.2

0.15

If rescattering C+ to C3+ occurs, it is Saturatedeffect a very small Volume

0.1

Model can be Assume that 3+ yield arises from sequential process applied
C+ C2+ C3+

0.05

0 0 0.5 1 1.5 2 2.5 3 3.5

z position (mm)

Checking for Re-scattering C+ to C3+

3+ C

Z-Scan
Ion Yield (circ)
C2+ to C3+ fit (production) C3+ to C4+ fit (depletion)

0.25

Integrated Yield (arb. units)

0.2

0.15

0.1

0.05

0 0 0.5 1 1.5 2 2.5 3

z position (mm)

This saturated volume fit for C2+ to C3+ can now be used to give the depletion of C2+ ions when modelling C2+ Z-scan

3+ C
0.25

Z-Scan
Ion Yield (circ)
C2+ to C3+ fit (production) C3+ to C4+ fit (depletion) Saturated Volume Fit

Integrated Yield (arb. units)

0.2

0.15

0.1

Tunnelling and MPI occur at large values. Sat Vol only works for OTB ionisation.
0 0.5 1 1.5 2 2.5 3

0.05

z position (mm)

This saturated volume fit for C2+ to C3+ can now be used to give the depletion of C2+ ions when modelling C2+ Z-scan

C2+ Z-Scan
2

Linear Circular

Integrated yield (arb. units)

1.5

0.5

0 0 1 2 3 4 5 6

z position (mm)

Slight difference between Linear and circular signal around z=2mm Experimental factor As before assume little or no rescattering

C2+ Z-Scan
4.5E-11 4.0E-11 3.5E-11 3.0E-11 2.5E-11 2.0E-11 1.5E-11 1.0E-11 5.0E-12 0.0E+00

Ion Yield (arbitrary units)

Previous Z-Scan Linear Circular

Shoulder
Yield at z>4mm

Integrated yield (arb. units)

1.5

Z (mm)

10

15

! NO SHOULDER !
0.5

+ No Yield at large z values (z > 4mm)

0 0 1 2 3 4 5 6

z position (mm)

Shoulder not observed. Metastable transition absent? Applying the Saturated Volume Model to find out what transitions occur

C2+ Z-Scan
2

Ion Yield (circ)

C2+ to C3+ fit (depletion) C+ to C2+ ground state (production)

Integrated yield (arb.units)

1.5

0.5

0 0 1 2 3 4 5

z position (mm)

C2+ Z-Scan
2

Ion Yield (circ)

C2+ to C3+ fit (depletion) C+ to C2+ fit (production)

Integrated yield (arb.units)

1.5

Saturated Volume fit

0.5

0 0 1 2 3 4 5

z position (mm)

C2+ Z-Scan
2

Ion Yield (circ)

C2+ to C3+ fit (depletion) C+ to C2+ fit (production)

Integrated yield (arb.units)

1.5

Saturated Volume fit

1 Metastable transition (10% pop) 0.5

0 0 1 2 3 4 5

z position (mm)

Metastable transition is clearly not viable in this model

Best fit is
2

C2+ Z-Scan
Ion Yield (circ)
C2+ to C3+ fit (depletion) C+ to C2+ ground (production)

Integrated yield (arb.units)

1.5

Saturated Volume Fit

1

0.5

0 0 1 2 3 4 5

z position (mm)

No metastable, spin flip transition !

No Metastable transition Why?

Experimental Artefact in previous Carbon data? Uncertainties. In Applying Sat Vol fits. Peak Intensity, pulse length, relating Vip to Is. Tunnelling, MPI? Metastables absent from source? Contradicts previous evidence. Meta-Meta transition cant be distinguished from ground ground Shouldnt be surprised Dipole selection rules ( s=0) forbid the transition!

Conclusion
Ionisation in Intense Laser Fields researched Ion Beam Modifications made to Saturated Volume Model
-Useful applications for future research

Ionisation of Carbon in Intense Laser fields investigated

-Metastable Transition not observed. -Data successfully modelled by expected transitions - Multiple Ionisation from C+ investigated for the 1st time Mainly sequential suggest negligible contribution from rescattering - First successful modelling of C3+ z-scan.

Very Interesting and enjoyable project.

Future Work
Sat Vol Improvements - Ion beam current density

Deconvolution Allow for Tunnelling and MPI

Shorter Pulse times ~10fs allows probing of stationary molecule.

(Pulse time lower than Vibrational period of molecule e.g. H2 ~20fs.)

Acknowledgements
Many thanks to
Prof Ian Williams Dr B Srigengan Mr M Suresh Mr J McKenna

+ UCL and RAL Collaboration

Thank you for listening

Questions?

Polarisation of Light

Half-Wave Plate
Rotation of plate

U 2

Laser Polaroid
P 2

Plate

Through Polaroid I=Iocos2

Linear / Circular matching

-The 0.65 Factor[ circ 3 I ! [ lin T I 0
1 2

TZ ! 3 I n *3
3

>> 1

ADK theoretical fits show that; Linear yield at Intensity 1.3*I matches the Circular yield at I .

Linear at Io
Fig /4 Plate Linear transmission

Optical Axis

Measured Beam
Linearly polarised
Angle to optical axis = 0

Interaction Beam
Linearly polarised Intensity Io Electric Vector Eo

Electric Vector Eo Intensity Io P Plate 4

Interaction beam is at Io

Circular at Io
Optical Axis
Fig /4 Plate Linear to Circular

Interaction Beam Measured Beam

Linearly polarised
Angle to optical axis = 45o
45
o

Circularly polarised Electric Vector Eo 2 Intensity I 0 2

Electric Vector Eo Intensity Io P Plate 4

Interaction beam is actually 0.5Io

So Linear matches at 1.3(0.5I0) = 0.65Io

When matching to Circular Io

C+ Metastable

configuration 1s2 2s 2p2 spin orientation oq o o o

C2+ Ground

configuration 1s2 2s2 spin orientation oq oq

Electron Re-scattering

Laser Field

Summary

Laser System
Interaction region

Translation stage

ASTRA (TA1)

Laser source

Compressor

Central Laser Facility, Beam expander Rutherford Appleton Laboratories (RAL) Oxfordshire. Ti:Sapphire, 50-55fs Pulses,800nm, 10Hz Pulse Energies ~20mJ Peak Intensity ~ 5*1016 W/cm2

Auto correlator

C+ transitions
Ground state

Metastable

Ground state

Metastable Ground state

tunnelling
Can occur as long as the time taken for the electronic wavefunction to tunnel through the barrier is shorter than half the optical period of the incident light.