Effect of the dynamical disorder on the second-order nonlinear optical responses of helicity-encoded polymer strands

Raphaël Méreau, Frédéric Castet, Edith Botek, Benoît Champagne

Research output: Contribution to journalArticle

Abstract

By combining classical samplings with quantum chemistry semiempirical time-dependent Hartree-Fock calculations, the high impact of dynamic fluctuations on the NLO properties of helical strands has been evidenced. In particular, these fluctuations are responsible for relative variations of ∼20% in the hyperRayleigh responses in both pyridine - pyrimidine (py - pym) and hydrazone - pyrimidine (hy - pym) strands. Then, dynamical disorder has an even more important impact on the electric-field-induced second harmonic generation responses, whose variations can reach 2 (py - pym) or 5 (hy - pym) times their mean value. This work also highlights the relationships between the unit cell nature and helical conformation of foldamers and their second-order NLO responses. In particular, the octupolar symmetry of the hyper-Rayleigh depolarization ratios is related to the helix periodicity of three unit cells per turn in both compounds.

Original languageEnglish
Pages (from-to)6552-6554
Number of pages3
JournalJournal of physical chemistry A
Volume113
Issue number24
DOIs
Publication statusPublished - 18 Jun 2009

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pyrimidines
strands
Polymers
disorders
Hydrazones
hydrazones
polymers
pyridines
Quantum chemistry
Depolarization
quantum chemistry
Harmonic generation
cells
depolarization
helices
Conformations
periodic variations
harmonic generations
sampling
Electric fields

Cite this

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abstract = "By combining classical samplings with quantum chemistry semiempirical time-dependent Hartree-Fock calculations, the high impact of dynamic fluctuations on the NLO properties of helical strands has been evidenced. In particular, these fluctuations are responsible for relative variations of ∼20{\%} in the hyperRayleigh responses in both pyridine - pyrimidine (py - pym) and hydrazone - pyrimidine (hy - pym) strands. Then, dynamical disorder has an even more important impact on the electric-field-induced second harmonic generation responses, whose variations can reach 2 (py - pym) or 5 (hy - pym) times their mean value. This work also highlights the relationships between the unit cell nature and helical conformation of foldamers and their second-order NLO responses. In particular, the octupolar symmetry of the hyper-Rayleigh depolarization ratios is related to the helix periodicity of three unit cells per turn in both compounds.",
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Effect of the dynamical disorder on the second-order nonlinear optical responses of helicity-encoded polymer strands. / Méreau, Raphaël; Castet, Frédéric; Botek, Edith; Champagne, Benoît.

In: Journal of physical chemistry A, Vol. 113, No. 24, 18.06.2009, p. 6552-6554.

Research output: Contribution to journalArticle

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