研究目的
Investigating the effects resulting from the size dispersion in the two dots that constitute a dimer is the main motivation of this paper.
研究成果
The study demonstrates that the interdot coherent excitonic dynamics in CdSe quantum dot dimers can be characterized by pump-probe transient absorption spectroscopy, despite the inherent size dispersion of colloidal QDs. The coherence of excitons in QD dimers, leading to interdot charge migration, can survive size disorder and could be observed experimentally. The findings open the way to applications in light harvesting and information processing devices.
研究不足
The study does not explicitly take into account the effect of the environment on the exciton energy distribution. Additionally, the coupling to the phonon and acoustic modes, which could affect the longer time scale interdot electronic coherences, is not included in the model.
1:Experimental Design and Method Selection:
The methodology involves electronic quantum dynamical simulations to characterize the interdot coherent response to ultrashort fs laser pulses using pump-probe transient absorption spectroscopy. The time-dependent Schrodinger equation is solved including the interaction with the oscillating electric field of the pulses for an ensemble of dimers that differ by their size.
2:Sample Selection and Data Sources:
The study focuses on ensembles of small (2 to 4 nm diameter) heterodimers and homodimers of CdSe QDs, taking into account the inherent size distribution of colloidal QDs.
3:List of Experimental Equipment and Materials:
The study uses a model excitonic Hamiltonian for dimers parameterized by the QD size and interdot distance, using an effective mass approximation. Local and charge transfer excitons are included in the dimer basis set.
4:Experimental Procedures and Operational Workflow:
The optical electronic response is computed by solving the time-dependent Schrodinger equation for an ensemble of dimers, with the excitonic Hamiltonian parameterized by QD size and interdot distance.
5:Data Analysis Methods:
The computed pump-probe transient absorption maps are averaged over the ensemble to show that the coherence of excitons in QD dimers can survive size disorder.
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