Real-time spectroscopy to clarify the mechanism of ultrafast nonlinearity

Takayoshi Kobayashi; Mitsuhiro Ikuta

doi:10.1117/12.601403

4 April 2005 Real-time spectroscopy to clarify the mechanism of ultrafast nonlinearity

Takayoshi Kobayashi, Mitsuhiro Ikuta

Proceedings Volume 5724, Organic Photonic Materials and Devices VII; (2005) https://doi.org/10.1117/12.601403
Event: Integrated Optoelectronic Devices 2005, 2005, San Jose, California, United States

Abstract

In order to clarify the mechanism of ultrafast optical nonlinearity in polymer especially polydiacetylene real-time measurement of molecular vibration which can provide information of time-resolved structural changes associated with huge electronic spectral change was performed. Molecular vibration of several modes in blue-phase polydiacetylene-3-butoxycarbonylmethylurethane (PDA-3BCMU) was time resolved by 5-fs pump-probe measurement. The contributions of the vibrational wavepackets in the ground state and in the excited state in the signal were separated by multi-channel measurement. The C=C stretching mode in the ground state starts to oscillate π-out-of-phase with the C^≡C stretching mode. The structure of PDA-3BCMU in the geometrically relaxed state is not pure butatriene-type but more like acetylene-type. The frequencies of C=C and C^≡C stretching modes there were determined by singular value decomposition method to be 1472 ± 6 cm^-1 and 2092 ± 6 cm^-1, respectively. The double and triple bond stretching frequencies in the ground state which are 1463 ± 6 cm^-1 and 2083 ± 6 cm^-1, respectively. Frequencies of both modes are increased in the configuration after the geometrical relaxation after the generation in the excited state upon excitation.

Citation Download Citation

Takayoshi Kobayashi and Mitsuhiro Ikuta "Real-time spectroscopy to clarify the mechanism of ultrafast nonlinearity", Proc. SPIE 5724, Organic Photonic Materials and Devices VII, (4 April 2005); https://doi.org/10.1117/12.601403

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Signal processing

Transmittance

Absorption

Ultrafast laser spectroscopy

Spectroscopy

Modulation

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