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Interaction between excitons determines the non-linear response of nanocrystals |
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| Authors: | Mayrose R Salvador P Sreekumari Nair Minhaeng Cho Gregory D Scholes |
| Institution: | aLash Miller Chemical Laboratories, 80 St. George Street, Center for Quantum Information and Quantum Control, and Institute for Optical Sciences, University of Toronto, Toronto, Ontario, Canada M5S 3H6;bDepartment of Chemistry and Center for Multidimensional Spectroscopy, Korea University, Seoul 136-701, South Korea |
| Abstract: | The non-linear response of semiconductor quantum dots is investigated using three-pulse photon echo peak shift (3PEPS) experiments and simulations. The third-order non-linear response is modeled by a three-level system, utilizing Brownian oscillators to model the line-broadening functions. Our results show that biexciton formation and exciton–exciton scattering significantly influence the non-linear response of quantum dots. The exciton to biexciton excited state absorption pathways are also investigated for quantum dots with different crystal structures. Our calculations suggest that the probability of excited state absorption to the biexcitonic state is higher for zinc-blende structured nanocrystals. |
| Keywords: | Nanocrystal Quantum dot Photo echo Non-linear response Laser Ultrafast CdSe |
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