Multiscale Numerical Modelling and Structural Design of Bulk Heterojunction Nanocomposites for Organic Photovoltaics: From Molecular Interfaces to Device Optimization

Bulk heterojunction (BHJ) active layers in organic photovoltaics (OPVs) are nanostructured composites in which electron-donating and electron-accepting semiconductors form interpenetrating phases for exciton dissociation and charge transport. The power conversion efficiency (PCE) of these organic-organic nanocomposites is governed by structural features spanning multiple length scales: molecular packing and energy-level alignment at donor/acceptor (D/A) interfaces, phase-separation morphology and crystallite connectivity, and thin-film optical and charge-transport characteristics. Rational design of high-performance OPV nanocomposites requires multiscale numerical modelling that bridges quantum chemistry, mesoscale morphology simulation, and device-scale optoelectronic modelling. This review surveys and critically compares recent advances in the structural design and numerical simulation of OPV BHJ nanocomposites. At the molecular scale, we examine density functional theory and non-adiabatic molecular dynamics approaches for resolving charge-separation driving forces, interfacial energy-level alignment, and exciton dynamics. At the mesoscale, we discuss molecular dynamics, kinetic Monte Carlo, and electronic coarse-graining methods for describing phase separation, crystallization kinetics, morphology evolution, and charge transport. At the device scale, we review exciton-diffusion, optical transfer-matrix, and drift-diffusion models that quantitatively link morphology to photovoltaic performance metrics. The review also evaluates how machine learning, high-throughput screening, surrogate models, and generative design accelerate donor–acceptor selection and morphology optimization, while distinguishing benchmark predictions from experimentally validated design rules. Across these scales, we compare the strengths, assumptions, and validation limits of the principal modelling approaches. Finally, we highlight emerging multiscale integration frameworks, including sequential parameter-passing pipelines and differentiable digital-twin concepts. By framing OPV BHJ layers as nanocomposites whose performance bottlenecks map onto composite-design challenges such as interface integrity, phase connectivity, multiscale charge transfer, and degradation-aware design, this review connects OPV modelling with broader structural-composites thinking for next-generation organic solar cells.