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Fifth-order two-quantum absorptive two-dimensional electronic spectroscopy of CdSe quantum dots

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Palato,  Samuel
Department of Chemistry, McGill University, Montreal;
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Seiler,  Helene
Department of Chemistry, McGill University, Montreal;
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Citation

Brosseau, P., Palato, S., Seiler, H., Baker, H., & Kambhampati, P. (2020). Fifth-order two-quantum absorptive two-dimensional electronic spectroscopy of CdSe quantum dots. The Journal of Chemical Physics, 153(23): 234703. doi:10.1063/5.0021381.


Cite as: http://hdl.handle.net/21.11116/0000-0007-A337-3
Abstract
Two-quantum variants of two-dimensional electronic spectroscopy (2DES) have previously been used to characterize multi-exciton interactions in molecules and semiconductor nanostructures though many implementations are limited by phasing procedures or non-resonant signals. We implement 2DES using phase-cycling to simultaneously measure one-quantum and two-quantum spectra in colloidal CdSe quantum dots. In the pump–probe geometry, fully absorptive spectra are automatically acquired by measuring the sum of the rephasing and nonrephasing signals. Fifth-order two-quantum spectroscopy allows for direct access to multi-exciton states that may be obscured in excited state absorption signals due to population relaxation or third-order two-quantum spectra due to the non-resonant response.