Different time-scale relaxation dynamics in organic supramolecular ferroelectrics studied by linear and nonlinear spectroscopy

Tsugumi Umanodan, Se I.Ichi Tanaka, Suguru Naruse, Tadahiko Ishikawa, Ken Onda, Shin Ya Koshihara, Sachio Horiuchi, Yoichi Okimoto

Research output: Contribution to journalArticle

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Abstract

Time-resolved linear and nonlinear optical responses were investigated in an organic supramolecular ferroelectric material composed of protonated 2,3-di(2-pyridinyl)pyrazine (H-dppz) and deprotonated chloranilic acid (Hca). We irradiated nanosecond laser pulses (λ = 532 nm) on the crystal, pumped the intramolecular excitation of the Hca molecule, and observed a clear redshift of the molecular vibrational modes of C=O and C-O- just after the photoexcitation. Each softened mode gradually relaxed on different time scales, indicating that the electrons of the Hca molecules were redistributed after the photoexcitation. By the same excitation, a large suppression of the second-harmonic (SH) intensity was observed, driven by the macroscopic disordering of the transferred protons. The decay time of the SH intensity was longer than those of the vibrational modes, suggesting that the microscopic vibrations and macroscopic ferroelectricity have dynamics on different time scales.

Original languageEnglish
Article number073707
Journaljournal of the physical society of japan
Volume84
Issue number7
DOIs
Publication statusPublished - Jul 15 2015

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photoexcitation
spectroscopy
vibration mode
harmonics
ferroelectric materials
pyrazines
ferroelectricity
excitation
molecules
retarding
vibration
acids
protons
decay
pulses
crystals
lasers
electrons

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)

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Different time-scale relaxation dynamics in organic supramolecular ferroelectrics studied by linear and nonlinear spectroscopy. / Umanodan, Tsugumi; Tanaka, Se I.Ichi; Naruse, Suguru; Ishikawa, Tadahiko; Onda, Ken; Koshihara, Shin Ya; Horiuchi, Sachio; Okimoto, Yoichi.

In: journal of the physical society of japan, Vol. 84, No. 7, 073707, 15.07.2015.

Research output: Contribution to journalArticle

Umanodan, Tsugumi ; Tanaka, Se I.Ichi ; Naruse, Suguru ; Ishikawa, Tadahiko ; Onda, Ken ; Koshihara, Shin Ya ; Horiuchi, Sachio ; Okimoto, Yoichi. / Different time-scale relaxation dynamics in organic supramolecular ferroelectrics studied by linear and nonlinear spectroscopy. In: journal of the physical society of japan. 2015 ; Vol. 84, No. 7.
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AU - Umanodan, Tsugumi

AU - Tanaka, Se I.Ichi

AU - Naruse, Suguru

AU - Ishikawa, Tadahiko

AU - Onda, Ken

AU - Koshihara, Shin Ya

AU - Horiuchi, Sachio

AU - Okimoto, Yoichi

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