Strong-Field-Driven Non-Linear Electron Dynamics in Thiophene Oligomers
Abstract
The interaction between conjugated molecules and intense electric field pulses drives a plethora of intriguing nonlinear phenomena, including optical limiting. While excited-state absorption was recently identified as the primary mechanism for this effect in thiophene oligomers, open questions remain regarding field-dependent population dynamics under intense laser driving. Using real-time time-dependent density functional theory combined with a determinant-overlap population framework, we track the intensity-dependent nonlinear response of a single thiophene ring (1T) and quaterthiophene (4T) as prototypical members of the oligothiophene family with different length and symmetry. We demonstrate that extended π-conjugation in 4T lowers nonlinear excitation thresholds by orders of magnitude compared to 1T. State-resolved population dynamics reveal complete ground-state depletion accompanied by sequential excited-state absorption channels under intense driving. High-harmonic generation spectra explicitly reflect molecular symmetry constraints, while energy-resolved occupation densities confirm continuous orbital redistribution across the π*-manifold. This work provides dynamic physical insights for engineering organic materials with tailored nonlinear optical properties.
Related
- Silver-mediated fluorodestannylation of an electron-rich thieno[3,2- b ]thiophene diverts to oxygenation: an α-fluorothiophenone instead of an aryl fluoride
- Visualising redox-driven metal-oxide interface dynamics in Ni/GDC electrodes via in situ Auger-Meitner electron microscopy.
- Electron spectra from strong-field enhanced ionization in heavy water
- Chiral Dy(iii) single-molecule magnets supported by thiophene-substituted hexaazamacrocycles
- Electrochemical Proton-Coupled Electron Transfer Free Energy Surfaces from Ab Initio Molecular Dynamics
BibTeX
@misc{driouech2026strongfielddriven,
title = {{Strong-Field-Driven Non-Linear Electron Dynamics in Thiophene Oligomers}},
author = {Mustapha Driouech and Caterina Cocchi and Michele Guerrini},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2609.29284},
eprint = {2609.29284},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2609.29284},
note = {CC BY-NC-SA 4.0},
}
RIS
TY - UNPB
TI - Strong-Field-Driven Non-Linear Electron Dynamics in Thiophene Oligomers
AU - Mustapha Driouech
AU - Caterina Cocchi
AU - Michele Guerrini
PY - 2026
DA - 2026/09/24
PB - arXiv
DO - 10.48550/arxiv.2609.29284
UR - https://arxiv.org/abs/2609.29284
AB - The interaction between conjugated molecules and intense electric field pulses drives a plethora of intriguing nonlinear phenomena, including optical limiting. While excited-state absorption was recently identified as the primary mechanism for this effect in thiophene oligomers, open questions remain regarding field-dependent population dynamics under intense laser driving. Using real-time time-dependent density functional theory combined with a determinant-overlap population framework, we track the intensity-dependent nonlinear response of a single thiophene ring (1T) and quaterthiophene (4T) as prototypical members of the oligothiophene family with different length and symmetry. We demonstrate that extended π-conjugation in 4T lowers nonlinear excitation thresholds by orders of magnitude compared to 1T. State-resolved population dynamics reveal complete ground-state depletion accompanied by sequential excited-state absorption channels under intense driving. High-harmonic generation spectra explicitly reflect molecular symmetry constraints, while energy-resolved occupation densities confirm continuous orbital redistribution across the π^*-manifold. This work provides dynamic physical insights for engineering organic materials with tailored nonlinear optical properties.
ER -