Bridging atomistic and surface integral approaches for the efficient modeling of the optical properties of soot
Abstract
The accurate optical modeling of carbonaceous soot nanoparticles is computationally challenging due to their complex morphologies and the multi-scale nature of their electromagnetic interactions. In this work, we bridge the gap between atomistic and continuum computational methods by coupling the semi-empirical dynamic atomic dipole interaction (DADI) model with the surface integral equation (SIE) method. By deriving effective complex refractive indices from atomistically defined primary soot nanoparticles via the DADI model, we parametrize equivalent continuous surface boundaries in the open-source SIE code HELIOS. The optical cross sections of isolated spherules and non-overlapping spherules are benchmarked against the T-matrix method, whereas interpenetrated spherules are assessed through a quantitative comparison between DADI and SIE. Both approaches demonstrate exceptional agreement for isolated and separated particles. For closely interacting and interpenetrated configurations, DADI and SIE effectively capture fundamental near-field dipole-dipole interactions, shifting the primary ultraviolet absorption peak and enhancing visible absorption, despite minor quantitative discrepancies inherent to atomic versus continuum representations. Finally, we demonstrate the scalability of this coupled approach by computing the absorption cross section of a realistic, highly complex soot aggregate reconstructed via 3D tomography, establishing a highly efficient pathway that bypasses the prohibitive computational costs of fully atomistic or volumetric methods.
Related
- Atomistic Modeling of Chemical Disorder in Materials: Bridging Conventional Methods and AI-Assisted Approaches
- PINNIES: An efficient physics-informed neural network framework for integral operator problems
- Impact of Chemical Clustering on the Structural, Topological, and Functional Properties of Ba(ZrxTi1−x)O3: An Atomistic Simulation Study
- Synthesis and properties of (FeSnPbSb)S quinary sulphides: Bridging mechanochemical and high-entropy concepts
- Structural, electronic, spectroscopic, and thermodynamic properties of gentisic acid: solvent and temperature effects using DFT and TD-DFT approaches
BibTeX
@article{brosseauhabert2026bridging,
title = {{Bridging atomistic and surface integral approaches for the efficient modeling of the optical properties of soot}},
author = {N. Brosseau-Habert and P. Mavrikakis and Sylvain Picaud and O.J.F. Martin and M. Devel},
journal = {Optics Communications},
year = {2026},
month = oct,
doi = {10.1016/j.optcom.2026.133843},
url = {https://hal.science/hal-05799624v1},
note = {CC BY-NC-ND 4.0},
}
RIS
TY - JOUR
TI - Bridging atomistic and surface integral approaches for the efficient modeling of the optical properties of soot
AU - N. Brosseau-Habert
AU - P. Mavrikakis
AU - Sylvain Picaud
AU - O.J.F. Martin
AU - M. Devel
PY - 2026
DA - 2026/10/10
JO - Optics Communications
DO - 10.1016/j.optcom.2026.133843
UR - https://hal.science/hal-05799624v1
AB - The accurate optical modeling of carbonaceous soot nanoparticles is computationally challenging due to their complex morphologies and the multi-scale nature of their electromagnetic interactions. In this work, we bridge the gap between atomistic and continuum computational methods by coupling the semi-empirical dynamic atomic dipole interaction (DADI) model with the surface integral equation (SIE) method. By deriving effective complex refractive indices from atomistically defined primary soot nanoparticles via the DADI model, we parametrize equivalent continuous surface boundaries in the open-source SIE code HELIOS. The optical cross sections of isolated spherules and non-overlapping spherules are benchmarked against the T-matrix method, whereas interpenetrated spherules are assessed through a quantitative comparison between DADI and SIE. Both approaches demonstrate exceptional agreement for isolated and separated particles. For closely interacting and interpenetrated configurations, DADI and SIE effectively capture fundamental near-field dipole-dipole interactions, shifting the primary ultraviolet absorption peak and enhancing visible absorption, despite minor quantitative discrepancies inherent to atomic versus continuum representations. Finally, we demonstrate the scalability of this coupled approach by computing the absorption cross section of a realistic, highly complex soot aggregate reconstructed via 3D tomography, establishing a highly efficient pathway that bypasses the prohibitive computational costs of fully atomistic or volumetric methods.
SN - 0030-4018
SN - 1873-0310
ER -