Frequency-resolved multifold fermions in the chiral topological semimetal CoSi

We report the optical conductivity in the linear-response regime of the chiral topological semimetal CoSi, predicted to host elusive topological quasiparticles known as multifold fermions. We find that the optical response is separated into several distinct regions as a function of frequency, each dominated by different types of quasiparticles. The low-frequency response is captured by a narrow Drude peak that broadens strongly with increasing temperature from 10 K to 300 K and is dominated by a high-mobility electron pocket near a double Weyl fermion at the $R$ point. At high frequencies, we observe a sharp peak at 0.56 eV. Using tight-binding calculations, we link this peak to inter-band transitions around the $M$ point that are dominant due to the presence of a saddle point in the band structure. By subtracting the low-frequency sharp Drude and phonon peaks at low temperatures, we reveal two intermediate quasi-linear inter-band contributions separated by a kink at 0.2 eV. Using tight-binding models, we link the optical conductivity above and below 0.2 eV to inter-band transitions near the double Weyl fermion at the $R$ point and a three-fold fermion at $\Gamma$, respectively. To do so, we find the chemical potential to be slightly below the latter node, activating transitions between a linearly dispersing band and a flat band, for frequencies below 0.2 eV. More strikingly, below 0.1 eV our data are best explained if spin-orbit coupling is included, suggesting that at these energies the optical response is governed by transitions between a previously unobserved spin-3/2 node and a Weyl node. Our results highlight that different types of multifold fermions in CoSi are activated at different frequencies, providing a way to resolve them in energy. Our results provide the necessary basis to interpret the burgeoning set of optical and transport experiments in chiral multifold semimetals.