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Using extremely nondegenerate photons in frequency (energy ratios >10/1), we measure 2–4 orders of magnitude enhancement of two-photon absorption in semiconductors compared to the degenerate case. We demonstrate sub-femtosecond gated detection directly on semiconductor diodes.
We report the two-photon absorption spectrum of single crystals of an asymmetric cyanine-like dye in comparison to its spectrum in solution. The 2PA peak magnitude is comparable to bulk semiconductors of similar absorption edge.
We performed frequency non-degenerate pump-probe experiments in several direct-gap semiconductors using femtosecond and picosecond pulses. Tuning the long wavelength photons in the IR region, we observed a 125-fold enhancement of the two-photon absorption coefficient.
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