Abstract

Despite residing in an energetically and structurally disordered landscape, the spin degree of freedom remains a robust quantity in organic semiconductor materials due to the weak coupling of spin and orbital states. This enforces spin-selectivity in recombination processes which plays a crucial role in optoelectronic devices, for example, in the spin-dependent recombination of weakly bound electron-hole pairs, or charge-transfer states, which form in a photovoltaic blend. Here, we implement a detection scheme to probe the spin-selective recombination of these states through changes in their dielectric polarizability under magnetic resonance. Using this technique, we access a regime in which the usual mixing of spin-singlet and spin-triplet states due to hyperfine fields is suppressed by microwave driving. We present a quantitative model for this behaviour which allows us to estimate the spin-dependent recombination rate, and draw parallels with the Majorana–Brossel resonances observed in atomic physics experiments.

Highlights

  • Despite residing in an energetically and structurally disordered landscape, the spin degree of freedom remains a robust quantity in organic semiconductor materials due to the weak coupling of spin and orbital states

  • Organic photovoltaic devices (OPVs) are a particular example where the role of spin is of critical importance in determining solar cell performance[3]

  • Using this prototypical example of spin-dependent recombination, we highlight the parallels between our experiments conducted on disordered organic blends and the Majorana–Brossel resonances observed in atomic physics experiments on mercury vapour[24,25]

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Summary

Introduction

Despite residing in an energetically and structurally disordered landscape, the spin degree of freedom remains a robust quantity in organic semiconductor materials due to the weak coupling of spin and orbital states This enforces spin-selectivity in recombination processes which plays a crucial role in optoelectronic devices, for example, in the spin-dependent recombination of weakly bound electron-hole pairs, or charge-transfer states, which form in a photovoltaic blend. We develop a quantitative model to describe this behaviour, and use it to estimate the difference in recombination rate between spinsinglet and spin-triplet CT states Using this prototypical example of spin-dependent recombination, we highlight the parallels between our experiments conducted on disordered organic blends and the Majorana–Brossel resonances observed in atomic physics experiments on mercury vapour[24,25]

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