arXiv subjects

Roderick C. I. Mackenzie

Publications and source records attributed to Roderick C. I. Mackenzie.

4 recordsLinked to original sources

arXiv2026

Mobility-lifetime relation links photodegradation in spin-coated and gravure-printed organic solar cells

The degradation mechanisms of organic solar cells (OSCs) have been studied primarily in spin-coated, laboratory-scale devices, whereas scalable processing modifies the device architecture, active-layer morphology, and underlying charge-transport and recombination properties. Whether these changes also alter how solar cells degrade remains unclear. Here, we compare spin-coated and fully roll-to-roll-compatible gravure-printed PM6:Y12 solar cells during $\sim$1000 h of continuous illumination. Despite distinct initial properties and degradation signatures, the loss of power-conversion efficiency systematically follows the mobility-lifetime product $μτ$. Remarkably, ageing of the printed devices increases the recombination lifetime while strongly reducing charge-carrier mobility, showing that a longer lifetime alone does not imply improved device performance. The mobility reduction is accompanied by decreased PM6 lamellar order, whereas the additional open-circuit voltage loss originates predominantly from increased non-radiative recombination. Dark recovery further reveals a metastable contribution specific to the printed architecture. These results identify the mobility-lifetime product as a unifying physical descriptor for photodegradation, linking ageing-induced microscopic changes to macroscopic performance loss across spin-coated and scalable printed OSCs.

cond-mat.mtrl-sci↗

arXiv2026

Rethinking Charge Transport and Recombination in Donor-diluted Organic Solar Cells

We systematically investigate PM6:Y12 bulk-heterojunction solar cells with donor fractions ranging from 1% to 45%, linking morphology, charge transport, and recombination to device performance. Complementary structural and spectroscopic methods reveal that a percolating PM6 network forms even at below 5% donor content, with lamellar stacking and vertical composition gradients that do not hinder the charge extraction. The reduction of the effective active layer conductivity towards low donor fractions obeys a three-dimensional percolation model, indicating that charge transport is governed by network topology rather without a pronounced percolation threshold. A transition from nongeminate Langevin recombination to a dispersive Smoluchowski-type loss occurs below 5% donor fraction. The latter regime is also nongeminate, i.e., pertains to recombination of the total charge carrier density. Correspondingly, we observe that the Langevin reduction in the higher donor fractions - mostly dominated by redissociation of electron-hole pairs after encounter - changes towards low donor fractions: in these cases, the nongeminate loss rate exceeds the prediction of the Langevin model. This regime coincides with increasing transport resistance due to topology-limited hole conduction, leading to reduced fill factors despite a high retained charge-generation efficiency. Our results demonstrate that strong donor dilution preserves photogeneration if a continuous donor network is maintained, and unveil how topology-controlled transport and non-Langevin recombination jointly define the performance limits of donor-diluted organic solar blends.

cond-mat.mtrl-sci↗

arXiv2026

Bridging the lab-to-fab gap in non-fullerene organic solar cells via gravure printing

Organic solar cells have reached record efficiencies with non-fullerene acceptors, yet their translation to industrial printing remains a critical bottleneck. Here we report the highest efficiency achieved for a fully roll-to-roll-compatible gravure-printed non-fullerene organic solar cell. High-performance blends are typically optimised under laboratory coating conditions, while roll-to-roll manufacturing imposes fundamentally different constraints on ink stability, drying dynamics, and multilayer integration. Whether these constraints intrinsically limit device physics has remained unresolved. Here, we demonstrate a gravure-printed PM6:Y12 solar cell architecture using commercially available materials and establish a quantitative framework that disentangles optical, recombination, and transport losses in printed devices. We find that favourable bulk morphology and exciton harvesting can be preserved under gravure printing and non-halogenated solvents. The dominant efficiency penalties arise instead from optical interference within the printed layer stack and slow charge transport. Our results demonstrate that the performance gap between laboratory and printed solar cells is originating from device architecture rather than the intrinsic physics of modern non-fullerene systems, providing a mechanistic roadmap for roll-to-roll manufacturing of non-fullerene solar cells.

cond-mat.mtrl-sci↗

arXiv2025

A Framework to Pinpoint Bottlenecks in Emerging Solar Cells and Disordered Devices via Differential Machine Learning

A key challenge in the development of materials for the next generation of solar cells, sensors and transistors is linking macroscopic device performance to underlying microscopic properties. For years, fabrication of devices has been faster than our ability to characterize them. This has led to a random walk of material development, with new materials being proposed faster than our understanding. We present two neural network-based methods for extracting key material parameters, including charge carrier mobility and trap state density, in optoelectronic devices such as solar cells. Our methods require solely measured light current--voltage curve and modest computational resources, making our approach applicable in even minimally equipped laboratories. Unlike traditional machine learning models, our methods place the final material values in a non-Gaussian likelihood distribution, allowing confidence assessment of each predicted parameter. We demonstrate these techniques using fresh PM6:Y12 and degraded PM6:BTP-eC9 organic solar cells.

physics.app-ph↗