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Atomic and Molecular Physics

Ultrafast Laser Physics and Laser Spectroscopy


Instrumentation seminar

Femtosecond spectroscopy
Ultrafast gas phase phenomena
Femtochemistry
Laser Spectroscopy
Laser physics on surfaces
PSP-investigations
Personnell Lars-Erik Berg
sa Larsson
Femtosecond spectroscopy Rene Andersson
Ultrafast gas phase Niklas Gador
Femtochemistry Ming Liu
Peter Saln
Mats Larsson SU
Bo Zhang
Tony Hansson Peter vd Meulen
Peder Royen Pia Johansson
Laser Spectroscopy Marica Sjdin
Laser physics Nils Tillmark M
Sonoluminiscence Timmy Sigfrids M
PSP-investigations Nathan Ross FOI
FastPhenomena
Fast Phenomena

-15 -14 -13 -12 -11


Time 10 10 10 10 10 s

scale fs ps
Wave 3 m 3 mm

train
100 nm 1 nm
Band
width
Interested visitor at the fs-lab

Bo
Gran
Pia Niklas
Femtosecond spectroscopy

Theadventofthelaserin1960andthedevelopmentofthe
femtosecondlaserwith t=100fsin1990ledto:

*hopethatthelaserscansteerchemicalreactions
*hopethatfinalproductscanbeselected
*thefslaserexcitesmoleculesandprobesthepot.surfaces
*thefslaserexitesmoleculesinstudiesofdecaychannels
*thefslasercanexcitequantumwellsemiconductor
surfacesgivinginformationaboutmesoscopicstructures
*fewexperimentsdonerevealrealtimeevolution

Vibration of small
molecules ..

V Oscillation period T~ 100 fs

t=0
r
t = T/2

t=T 0 T 2T t
r
Fragmentation of molecules

A*+B
A+B
r
1in50fs

r
Collisions atoms - atoms

Ar
r
10eV10keV
+
Ar Timescale 100 fs - 1 fs
Other Ultra-fast Phenomena

Electronholerecombinations
Timescale 30 fs - 200 fs
Interactiontimesinliquids
r
Timescale 1ps - 100 ps
Fastrelaxationsinlargemolecules
Timescale 30 fs - 200 fs
Femtosecond delay
1fs 0.3m

7fs 2m
Wave packets
Wave- packet splitting at a Curve- crossing

Diabatic states : Adiabatic states :


1 2
Energy

V Include V in
VNA
H0
r

TIME

Rb2, D system
TOF Crossed
heat- pipe oven
supersonic- effusive
Rb2, D;A system beams
Effusive beam He: cooling of Rb2
Ar,Kr: Rb2 clusters
Experimental
Photon counter
Mode-locked fiber laser

780 nm; 170 fs; 150 cm-1


PM computer
Topas 2, OPA Rb2
tube
Topas 1, OPA
/2 wave-
plate Acetone inlet

+ prism compressors
for both beams Rb, Rb2
Laser
delay-
mirror copper Fluorescence
shield
T2

Pump: 427nm, 5 J per pulse,1kHz Thermo-


Probe: 927nm, 2 J per pulse,1kHz couples T1
Molecular quantum dynamics (MQD),
Wavepacket (WP) and Delay stage

fs laser spectroscopy t

1. MQD nuclear vibration, rotation


& change of electronic configuration.

2. WP nonstationary superposition
of a set of wavefunctions with fixed
phase relationship.

3. Pump-probe technique pump


process, probe process, delay time
and time zero.
Femtosecond
Femtosecond laser:
laser:
Dynamics
Pump canEr-doped
Pump laser,
laser, be studied
Er-doped fiber
fiberlaser, by
laser, kHz
kHz 2
2
Non-linear setups
Femtosecond
Non-linear
YAG
YAG laser
laser
TOPAS:
TOPAS:270
spectroscopy
270 nm
setups
...33 m
nm ... m
..
WLC generator: White light
WLC generator: White light
continuum
continuum
Mirrors,
Mirrors, mirrors,
mirrors, ....
....
"3D Nozzle": Compressible
Flow with Shock, Transition,
Turbulence and
Unsteadiness
H Alfredsson, N Tillmark, T Sigfrids, L-E

p=?

Wind tunnel at KTH


Pressure Sensitive Paint
Method:
Laser excitation of pressure sensitive paint
in order to measure the gas pressure over
a surface.

1. Fluorescence measurements
2. Life-time measurements

Laser light Pressure sensitive paint


Fluorescence
Basic photophysics
SN Vibration
relaxations Photon transitions in
an energy diagram of
the condensed phase
S2 intersystem
crossingISC
S1
T1
f p
h
fosforescens
excitation

fluorescens
S0
Ruthenium based paint
tris(2,2bipyridil)rutheniumRu(bpy)
Absorption and emnission spectrum
4 YAG
3 YAG
Ar 488
Intensity

2 YAG

200300400500600700
wavelength(nm)
Binder:urethane,clear,ispermeabletooxygen
Pressure measurements
Decayrates
Quenching=kq[L*][O2]

I0 0
1 k q 0 [O2 ]
I
1/

SternVollmerplot

[O2]
Instrumentation

. Pressure measurements on a surface with a jet nozzle


. Measurements in the wind tunnel

requency tripled YAG, Ar ion laser chopped, blue diod laser


Mechelle+ICCD or ICCD+filter
ICCD-camera
ANDOR iStar
Digital delay generator
Propagation delay 40 ns
Optical gate width <2ns
CCD cooling -40oC
Monochromator
Resoving power
7500
R
1
Wavelength coverage

3 m optical fibre 190nm<< 1.1m


Mechelle
Mechelle
Optical system
Pressure Sensitive Paint
300PSP measurements
2000 shots averaged, filter K60, gain 700
Frequency doubled YAG laser excitation t = 5ns, = 532 nm
532 nm
200
Intensity

100

K60 transmission curve


0

500 520 540 560 580 600 620 640 660


nm

PSP1 decay Stern-Vollmer plot

0.0025
Invesre life-time (ms)

0.002
= 4.0 (0.2) s
0.0015 Series1

0.001
= 488 nm Ar ion
0.0005
0 200 400 600 800
Pressure /Torr)
Time-resolved spectrum

340 350
wavelength
Time-resolved spectra cont.
Sonoluminiscence Shocktubes
High pressure
Vacuum

Intense
Planck
Radiation

M Lesser, N Apazidis H Alfredsson,


N Tillmark, H Essn, Mechanics, L-E B
Experimental setup
Time-resolved spectra cont.

T=?

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