Stimulated emission depletion dynamics in push-push polyenes

Richard John Marsh; Nicholas D. Leonczek; Daven Aidan Armoogum; Laurent Porres; Olivier M. Mongin; Mireille H. Blanchard-Desce; Angus J. Bain

doi:10.1117/12.564433

14 October 2004 Stimulated emission depletion dynamics in push-push polyenes

Richard John Marsh, Nicholas D. Leonczek, Daven Aidan Armoogum, Laurent Porres, Olivier M. Mongin, Mireille H. Blanchard-Desce, Angus J. Bain

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Proceedings Volume 5510, Nanophotonic Materials; (2004) https://doi.org/10.1117/12.564433
Event: Optical Science and Technology, the SPIE 49th Annual Meeting, 2004, Denver, Colorado, United States

Abstract

Two-photon fluorescence polarisation and stimulated emission depletion dynamics are investigated in three high two-photon cross-section push-push polyenes: OM62, LP79 and OM77 and compared to the behaviour of a standard fluorophore (rhodamine 6G). Two-photon fluorescence anisotropy measurements (R(0) and Omega) were undertaken using picosecond time-correlated single photon counting (TCSPC). For OM62 and LP79 these are consistent with a diagonal two-dimensional transition tensor with S_XX>S_YY. For OM77 the contribution of off-diagonal elements (SXY & SYX) appears significant. Two-photon fluorescence anisotropy decay data is combined with streak camera measurements of excited state population depletion to determine stimulated emission cross-sections and ground state vibrational relaxation times. Cross-sections for STED in all three polyenes were found to be significantly higher than those for rhodamine 6G. The efficiency of STED is however dependent on the degree to which the S₁→S₀ transition is saturated by the DUMP pulse; this is mediated by fast ground state vibrational relaxation. Of the three polyenes, LP79 is seen to combine a large stimulated emission cross-section (c.a. 13σ(r6G)) with rapid ground state relaxation (τ_R=240fs).

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Richard John Marsh, Nicholas D. Leonczek, Daven Aidan Armoogum, Laurent Porres, Olivier M. Mongin, Mireille H. Blanchard-Desce, and Angus J. Bain "Stimulated emission depletion dynamics in push-push polyenes", Proc. SPIE 5510, Nanophotonic Materials, (14 October 2004); https://doi.org/10.1117/12.564433

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