Cavity Manipulation\nof Attosecond Charge Migration\nin Conjugated Dendrimers

Dendrimers are branched polymers with wide applications\nto photosensitization,\nphotocatalysis, photodynamic therapy, photovoltaic conversion, and\nlight sensor amplification. The primary step of numerous photophysical\nand photochemical processes in many molecules involves ultrafast coherent\nelectronic dynamics and charge oscillations triggered by photoexcitation.\nThis electronic wavepacket motion at short times where the nuclei\nare frozen is known as attosecond charge migration. We show how charge\nmigration in a dendrimer can be manipulated by placing it in an optical\ncavity and monitored by time-resolved X-ray diffraction. Our simulations\ndemonstrate that the dendrimer charge migration modes and the character\nof photoexcited wave function can be significantly influenced by the\nstrong light-matter interaction in the cavity. This presents a new\navenue for modulating initial ultrafast charge dynamics and subsequently\ncontrolling coherent energy transfer in dendritic nanostructures.

Publication Details

Journal
Figshare
Published
2024-10-02
DOI
https://doi.org/10.1021/jacs.4c06727.s001
Primary Topic
Dendrimers and Hyperbranched Polymers
Type
article
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article

Cavity Manipulation\nof Attosecond Charge Migration\nin Conjugated Dendrimers

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Dendrimers and Hyperbranched Polymers
article

Cavity Manipulation\nof Attosecond Charge Migration\nin Conjugated Dendrimers

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Abstract

Dendrimers are branched polymers with wide applications\nto photosensitization,\nphotocatalysis, photodynamic therapy, photovoltaic conversion, and\nlight sensor amplification. The primary step of numerous photophysical\nand photochemical processes in many molecules involves ultrafast coherent\nelectronic dynamics and charge oscillations triggered by photoexcitation.\nThis electronic wavepacket motion at short times where the nuclei\nare frozen is known as attosecond charge migration. We show how charge\nmigration in a dendrimer can be manipulated by placing it in an optical\ncavity and monitored by time-resolved X-ray diffraction. Our simulations\ndemonstrate that the dendrimer charge migration modes and the character\nof photoexcited wave function can be significantly influenced by the\nstrong light-matter interaction in the cavity. This presents a new\navenue for modulating initial ultrafast charge dynamics and subsequently\ncontrolling coherent energy transfer in dendritic nanostructures.

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Dendrimers and Hyperbranched Polymers
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