Control of Two-Photon Absorption in Organic Compounds by Pulse Shaping: Spectral Dependence

In this work, we investigate the control of the two-photon absorption process of a series of organic compounds via spectral phase modulation of the excitation pulse. We analyzed the effect of the pulse central wavelength on the control of the two-photon absorption process for each compound. Depending on the molecules` two-photon absorption position relative to the excitation pulse wavelength, different levels of coherent control were observed. By simulating the two-photon transition probability in molecular systems, taking into account the band structure and its positions, we could explain the experimental results trends. We observed that the intrapulse coherent interference plays an important role in the nonlinear process control besides just the pulse intensity modulation.

MEH-PPV photobleaching control by femtosecond pulse shaping

In the work reported here we were able to control the photobleaching of poly[2-methoxy-5-(2`-ethyl-hexyloxy)-1,4-phenylene vinylene] (MEH-PPV), excited by two-photon absorption, using femtosecond pulse shaping. By applying a cosine-like spectral phase mask, we observe a reduction of three times in the photobleaching rate, while the fluorescence intensity decreases by 20%, in comparison to the values obtained with a Fourier-transform-limited pulse. These results demonstrate an interesting trade-off between photobleaching rate and nonlinear fluorescence intensity. The possible mechanism behind this process is discussed in terms of the pulse spectral profile and the absorbance band of MEH-PPV. (C) 2009 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim