Femtosecond Optical Kerr Effect Studies Water

J.Phys.Chem.1994,98,6308-6316
Femtosecond Optical Kerr Effect Studies Water
Jun, heesun
Experimental Section
ü Pump : linear polarization
Probe : 45o
D1,D2 : optical delay
(A) Ti:Sapphire detection sheme
(B) amplified CPM detection sheme
OVA : Optical variable attenuator
PD1,PD2 : photodiode
TIA1,TIA2 : matched transimpedance amplifiers
DA : differential amplifier
(B)
(A)
üAutocorrelation : KD*P crystal (100um)
Results and Discussion
(A)
ü Optical Kerr effect measurement of water utilizing
the synchronously pumped Ti:Sapphire system
V (t ) = C[ ò dtG0(2) (t - t ) R (t )]
X 30
(B)
ü Autocorrelation signal
OKE out-of-phase
OKE in phase
Polarization 45o
Polarization 45o
PUMP
PUMP
(Vertical+l+1o)
Vertical
PROBE
PROBE
pol1 φ˚
( Horizontal+1o )
é0 0ù écos 45o
ê0 1 ú ê sin 45o
ë
û ë
l
if
- sin 45o ù é e x
úê
cos 45o û êë 0
pol3
SAMPLE
pol3
pol1
Horizontal
4
0 ù é cos 45o
o
if ú ê
e y úû ë - sin 45
sin 45o ù é1 0ù
ú
cos 45o û êë0 i úû
écos j
ê sin j
ë
SAMPLE
4
- sin j ù é0 0ù é cos j
cos j úû êë0 1 úû êë - sin j
l
SAMPLE
l
pol3
pol3
φ˚
sin j ù
cos j úû
φ˚
4
écos j
ê sin j
ë
- sin j ù é1 0ù é cos j
cos j úû êë0 0úû êë - sin j
pol1
sin j ù é1 ù
1
= cos[j ]2 sin[ (2j + fx - f y )]2
ú
ê
ú
cos j û ë0û
2
φ˚
I =< E 2 >= j 2 + jDf +
écos 45o
ê
o
ë sin 45
if
- sin 45o ù é e x
úê
cos 45o û ëê 0
PROBE
Df
4
2
0 ù é cos 45o
o
if ú ê
e y ûú ë - sin 45
sin 45o ù
ú
cos 45o û
SAMPLE
é1 0ù é1 0ù é1 ù 1
ê0 i ú ê0 0ú ê0ú = 4 (2 - cos[2j + fx - f y ] - cos[2j - fx + f y ])
ë
û ë
û ë û
l
pol1
PROBE
4
I =< E 2 >=
1 1
- cos Df cos 2j
2 2
ü out-of-phase
Polarization 45o
Polarization 45o
PUMP
PUMP
PROBE
PROBE
jo
( Horizontal+1o )
J.Phys.Chem.1991,95,10395
ü in-phase
QUARTER
WAVEPLATE
I =< E 2 >= j 2 + jDf +
SAMPLE
Df 2
4
Vertical
Horizontal
QUARTER
WAVEPLATE
I =< E 2 >=
SAMPLE
jo
(Vertical+l+1o )
1 1
- cos Df cos 2j
2 2
üIn-phase heterodyne-detected results utilizing the amplified
CPM system
ü The absolute magnitude of the in-phase response was more
than 1 order of magnitude less than out-of-phase signal
under the same condition
Frequency domain OKE of water with an optimal t=0 position position obtained from the Fourier transform of the
out-of-phase heterodyne response from fig2
t=+1fs
(A) Imaginary part of χ(3)
F (VL (t )) = F (G0(2) (t )) F ( R (t ))
t=-1fs
(B) Real part of χ(3)
J.Chem.Phys.99,2410,1993