Orbital-resolved imaging of coherent femtosecond exciton dynamics in coupled molecules

Fuente: arXiv
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Main Authors: Luo, Yang, Sheng, Shaoxiang, Pisarra, Michele, Chen, Caiyun, Martin, Fernando, Kern, Klaus, Garg, Manish
Format: Preprint
Published: 2025
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author Luo, Yang
Sheng, Shaoxiang
Pisarra, Michele
Chen, Caiyun
Martin, Fernando
Kern, Klaus
Garg, Manish
author_facet Luo, Yang
Sheng, Shaoxiang
Pisarra, Michele
Chen, Caiyun
Martin, Fernando
Kern, Klaus
Garg, Manish
contents Optical excitation and control of excitonic wavepackets in organic molecules is the basis to energy conversion processes. To gain insights into such processes, it is essential to establish the relationship between the coherence timescales of excitons with the electronic inhomogeneity in the molecules, as well as the influence of intermolecular interactions on exciton dynamics. Here, we demonstrate orbital-resolved imaging of optically induced coherent exciton dynamics in single copper napthalocyanine (CuNc) molecules, and selective coherent excitation of dark and bright triplet excitons in coupled molecular dimers. Ultrafast photon-induced tunneling current enabled atomic-scale imaging and control of the excitons in resonantly excited molecules by employing excitonic wavepacket interferometry. Our results reveal an ultrafast exciton coherence time of ~ 70 fs in a single molecule, which decreases for the triplet excitons in interacting molecules.
format Preprint
id arxiv_https___arxiv_org_abs_2507_00830
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Orbital-resolved imaging of coherent femtosecond exciton dynamics in coupled molecules
Luo, Yang
Sheng, Shaoxiang
Pisarra, Michele
Chen, Caiyun
Martin, Fernando
Kern, Klaus
Garg, Manish
Optics
Quantum Physics
Optical excitation and control of excitonic wavepackets in organic molecules is the basis to energy conversion processes. To gain insights into such processes, it is essential to establish the relationship between the coherence timescales of excitons with the electronic inhomogeneity in the molecules, as well as the influence of intermolecular interactions on exciton dynamics. Here, we demonstrate orbital-resolved imaging of optically induced coherent exciton dynamics in single copper napthalocyanine (CuNc) molecules, and selective coherent excitation of dark and bright triplet excitons in coupled molecular dimers. Ultrafast photon-induced tunneling current enabled atomic-scale imaging and control of the excitons in resonantly excited molecules by employing excitonic wavepacket interferometry. Our results reveal an ultrafast exciton coherence time of ~ 70 fs in a single molecule, which decreases for the triplet excitons in interacting molecules.
title Orbital-resolved imaging of coherent femtosecond exciton dynamics in coupled molecules
topic Optics
Quantum Physics
url https://arxiv.org/abs/2507.00830