  Chiral topological semimetals are materials that break both inversion and
mirror symmetries. They host interesting phenomena such as the quantized
circular photogalvanic effect (CPGE) and the chiral magnetic effect. In this
work, we report a comprehensive theoretical and experimental analysis of the
linear and non-linear optical responses of the chiral topological semimetal
RhSi, which is known to host multifold fermions. We show that the
characteristic features of the optical conductivity, which display two distinct
quasi-linear regimes above and below 0.4 eV, can be linked to excitations of
different kinds of multifold fermions. The characteristic features of the CPGE,
which displays a sign change at 0.4 eV and a large non-quantized response peak
of around 160 $\mu \textrm{A V}^{-2}$ at 0.7 eV, are explained by assuming that
the chemical potential crosses a flat hole band at the Brillouin zone center.
Our theory predicts that, in order to observe a quantized CPGE in RhSi, it is
necessary to increase the chemical potential as well as the quasiparticle
lifetime. More broadly our methodology, especially the development of the
broadband terahertz emission spectroscopy, could be widely applied to study
photo-galvanic effects in noncentrosymmetric materials and in topological
insulators in a contact-less way and accelerate the technological development
of efficient infrared detectors based on topological semimetals.
