Ultrafast Excited-State Isomerization Dynamics of 1,1‘-Diethyl-2,2‘-Cyanine Studied by Four-Wave Mixing Spectroscopy Benjamin Dietzek, Niklas hristensson,

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Presentation transcript:

Ultrafast Excited-State Isomerization Dynamics of 1,1‘-Diethyl-2,2‘-Cyanine Studied by Four-Wave Mixing Spectroscopy Benjamin Dietzek, Niklas hristensson, Torbjörn Pascher, Tõnu Pullerits, and Arkady Yartsev J. Phys. Chem. B, 2007, 111 (19), pp 5396–5404 Miyasaka Lab. Masayasu Muramatsu

Contents Introduction Experimental method Results ＆ Discussion Summary Photoinduced Isomerization 1122C　Excited-State bond-twisting motion 　Experimental method Transient Absorption TransientGrating Three-pulse photon echo peak-shift 　Results ＆ Discussion 　Summary

Photoinduced Isomerization Control 　pathway 　rate　.etc eye sight trans-stilbene cis-stilbene hn’ 254nm hn 313nm hn 11-cis retinal all-trans retinal 200fs model system　vs 　biological system 　　　→function of the protein matrix

Excited-State bond-twisting motion Methanol 538nm 523nm 500ps trans-1122C cis-1122C

DA = -log I I0 a → b a b DA A A a b a b Transient Absorption Probe Pump Transient species Sample hn a → b a b DA A A a b Reference a b

Pulse participation Hole spectrum time Excited State Absorption （ESA） Ground State Bleach （GSB） Stimulated Emission （SE） Hole spectrum time

Transient Grating （TG） 2pulse interference １）　Thermal change ２）　Volume change ３）　Spectrum change 3pulse interference n(t)：refracture index k(t)：absorbance

Three-pulse photon echo peak-shift τ≫0：decoherent　　　　　　　　 → 　no echo T≫0：vanish diffraction fringe　 → 　no echo

Three-pulse photon echo peak-shift Signal in k3+k2-k1 direction 100fs 1ps 10ps 100ps

Transient Absorption Stimulated emission ESA:excited-state population 4.9ps ESA:excited-state population 405nm 405nm(filled triangle) 573nm(open star) 700nm(open triangle) 850nm(open aquare) 1000nm(filled circle)

Transient Grating 548nm Rise:Stimulated Emission (dark state) Viscosity, large →Decay time, large Rise:Stimulated Emission (dark state) Decay:Internal Conversion

Transient Grating 530nm 495nm 495nm：no emission 　　→no rise

3PEPS 548nm Rise:Stimulated Emission (another state) viscosity 　large 　　↓ inhomogeneity Rise:Stimulated Emission (another state) The osillation pattern is insensitive to solvent 　 →　It is not related to torsion

3PEPS 5ps~ Rise: cis isomer formation ? methanol propanol Vibrational Relaxation 548nm(red), 530nm(green), 495nm(blue) 5ps~ Rise: cis isomer formation ? or Ultrafast Internal Conversion ?

Summary Transient Absorption Transient Grating 3PEPS ESA(405nm): ~1ps(flat),τ=4.9ps(decay) SE(548nm):~1ps(decay)→dark state Transient Grating wavelength dependent rise ← ESA solvent dependent decay ← internal conversion 3PEPS high viscosity →high inhomogeneity rise(495nm) →cis isomer? 1ps 4.9ps 500ps 538nm 523nm