The chemical potentials of excitons, defect states, electrons, and holes are important in charge and energy transport processes.  For a homogeneous ensemble, the standard chemical potential of an excited state appears in generalized Einstein relations connecting absorption and stimulated emission cross sections.  It is well known that absorptive two-dimensional Fourier transform spectra can separate inhomogeneous broadening along the 2D diagonal. When interferometrically calibrated 2D spectra are corrected for pulse propagation effects and spectral filtering, the fully relaxed 2D spectra can be fit to within the experimental error of 2% using only 5 parameters: inhomogeneity, bi-exciton shift, bi-exciton broadening, excited state emission strength, and excited state absorption strength. We describe use of broadband femtosecond two-dimensional Fourier transform spectroscopy to measure the standard chemical potential for creation of a 1S-1S exciton in an ensemble of colloidal lead sulfide quantum dots.  The role of excitonic fine structure and entropy changes in the standard chemical potential will be discussed.

Measuring the standard chemical potential for creation of an exciton

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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