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note
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The microscope slides were carefully cleaned with acetone, ethanol, and ultrapure water. We verified that the undopped polymer sample did not exhibit any measurable signal under two-photon excitation.
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26
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0345185078
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note
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The wavelength distribution in the femtosecond pulses is neglegted in this model and only one ω fundamental pulsation is considered.
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28
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0344322660
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note
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The Gouy phase shift factor contribution has been shown to be of crucial importance in the case of SHG transmitted signals with distances along Z longer than the coherence length of the nonlinear process. In our reflection configuration, the nonlinear interaction takes place in the sample plane and the propagation length is lower than the coherence length; therefore a possible Z contribution factor does not affect the propagation of the SHG signal. This factor only brings a constant contribution to the SHG polarized signal level, which has been quantified accounting for our 1.4 numerical aperture, and seen to be negligible compared with the other in-plane contributions.
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31
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0345617273
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note
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The angle between the two dipoles of absorption and emission for DCM has been estimated separately using static fluorescence anisotropy measurements in solution. The measured value is around 25°, which does not significantly influence the results in the model, compared with the other effects described in this work.
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0344322659
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note
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Note that other SHG emission processes such as surface-SHG and incoherent Hyper-Rayleigh emission can be ruled out in the present work by the observation of the polarization responses of Figure 6. Indeed, these effects would lead to very different polarization response with an (X,Y) symmetry that would not depend on the electric field orientation.
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