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Updated: May 13, 2026

Excitonic Hamiltonians for Calculating Optical Absorption Spectra and Optoelectronic Properties of Molecular Aggregates and Solids

Excitonic Hamiltonians for Calculating Optical Absorption Spectra and Optoelectronic Properties of Molecular Aggregates and Solids

Published on: May 27, 2020

Exciton multiplication from first principles.

Heather M Jaeger¹, Kim Hyeon-Deuk, Oleg V Prezhdo

¹Department of Chemistry, University of Rochester , Rochester, New York 14627, United States.

Accounts of Chemical Research

|March 6, 2013

Summary

This summary is machine-generated.

Efficient exciton multiplication in semiconductor quantum dots boosts solar power. This study quantifies photoexcitation, dephasing, and impact ionization, key to generating multiple electron-hole pairs from single photons for advanced photovoltaics.

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Determination of the Excitation and Coupling Rates Between Light Emitters and Surface Plasmon Polaritons

Determination of the Excitation and Coupling Rates Between Light Emitters and Surface Plasmon Polaritons

Published on: July 21, 2018

Area of Science:

* Materials Science and Nanotechnology
* Physical Chemistry and Photophysics
* Renewable Energy Technologies

Background:

* Third-generation photovoltaics demand high cost-efficiency standards.
* Exciton multiplication, generating multiple electron-hole pairs per photon, is crucial for improving solar power conversion.
* Semiconductor quantum dots show promise for efficient exciton multiplication due to quantum confinement effects.

Purpose of the Study:

* To investigate the photophysics of nanocrystals concerning exciton multiplication.
* To analyze the roles of photoexcitation, phonon-induced dephasing, and impact ionization in this process.
* To computationally quantify the probability and dynamics of multiple exciton generation.

Main Methods:

* Utilized ab initio computation to analyze many-electron wave functions.
* Quantified the contribution of electron correlation to multiple exciton generation probability.
* Calculated exciton energies directly from excited state wave functions to determine generation thresholds.

Main Results:

* Multiple exciton generation probability correlates with electron correlation magnitude.
* Surface defects, dopants, and ionization significantly alter the multiple exciton generation threshold.
* Exciton multiplication dynamics, involving photoexcitation, dephasing, and impact ionization, complete within approximately 10 picoseconds.

Conclusions:

* Exciton multiplication in quantum dots is a collective quantum phenomenon driven by photoexcitation, dephasing, and nonadiabatic evolution.
* Computational methods without semiempirical parameters can accurately predict exciton multiplication probabilities.
* Findings from small model systems are extrapolatable to larger, practical quantum dots for solar energy applications.