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 nonlinear 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 μA/V² 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 photogalvanic 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.

Significance: We present a comprehensive combined experimental and theoretical study of optical conductivity in the chiral topological semimetal CoSi based on the development of high-quality crystals. We reveal the presence and the energy range of various exotic multifold quasiparticles in the optical responses and provide experimental evidence for the realization of fourfold spin-3/2 fermions, which were not directly observed previously. Our work is critical to interpreting future optical and transport responses of multifold fermion materials. We believe the methods used in this work will not only stimulate future research in this class of materials but will also provide a strategy for addressing optical signatures of chiral topological fermions in solids.

Chiral multifold fermions are quasiparticles described by higher spin generalizations of the Weyl equation and are realized as low energy excitations near symmetry protected band crossings in certain chiral crystals. In this work we calculate the linear optical conductivity of all chiral multifold fermions. We show that it is enhanced with respect to that of Weyl fermions with the same Fermi velocity and features characteristic activation frequencies for each multifold fermion class, providing an experimental fingerprint to detect them. We calculate the conductivity for realistic chiral multifold semimetals by using lattice tight-binding Hamiltonians that match the effective models of multifold fermions at low energies, for space groups 199 and 198. The latter includes RhSi, for which we give quantitative predictions, and also CoSi and AlPt. Our predictions can be tested in absorption or penetration depth measurements and are necessary to extract the recently proposed quantized photocurrents from experiments.

Recent experiments in the topological Weyl semimetal TaAs have observed record-breaking second-harmonic generation (SHG), a nonlinear optical response at $2\omega$ generated by an incoming light source at $\omega$. However, whether SHG is enhanced in topological semimetals in general is a challenging open question because their band structure entangles the contributions arising from trivial bands and topological band crossings. In this work, we circumvent this problem by studying RhSi, a chiral topological semimetal with a simple band structure with topological multifold fermions close to the Fermi energy. We measure SHG in a wide frequency window, $\omega \in [0.27,1.5]\mathrm{eV}$ and, using first-principles calculations, we establish that, due to their linear dispersion, the contribution of multifold fermions to SHG is subdominant as compared with other regions in the Brillouin zone. Our calculations suggest that parts of the bands where the dispersion is relatively flat contribute significantly to SHG. As a whole, our results suggest avenues to enhance SHG responses.

In this work we study the electronic structure of Ag 3 AuSe 2 and Ag 3 AuTe 2 , two chiral insulators whose gap can be tuned through small changes in the lattice parameter by applying hydrostatic pressure or choosing different growth protocols. Based on first principles calculations we compute their band structure for different values of the lattice parameters and show that while Ag 3 AuSe 2 retains its direct narrow gap at the Γ point, Ag 3 AuTe 2 can turn into a metal. Focusing on Ag 3 AuSe 2 we derive a low energy model around Γ using group theory, which we use to calculate the optical conductivity for different values of the lattice constant. We discuss our results in the context of detection of light dark matter particles, which have masses of the order of a keV, and conclude that Ag 3 AuSe 2 satisfies three important requirements for a suitable detector: small Fermi velocities, meV band gap, and low photon screening. Our work motivates the growth of high-quality and large samples of Ag 3 AuSe 2 to be used as target materials in dark matter detectors.

The understanding of the mean free path (MFP) distribution of the energy carriers in materials (e.g., electrons, phonons, magnons, etc.) provides a key physical insight into their transport properties. In this context, MFP spectroscopy has become an important tool to describe the contribution of carriers with different MFP to the total transport phenomenon. In this work, we revise the MFP reconstruction technique and present a study on the impact of the regularization parameter on the MFP distribution of the energy carriers. By using the L-curve criterion, we calculate the optimal mathematical value of the regularization parameter. The effect of the change from the optimal value in the MFP distribution is analyzed in three case studies of heat transport by phonons. These results demonstrate that the choice of the regularization parameter has a large impact on the physical information obtained from the reconstructed accumulation function, and thus cannot be chosen arbitrarily. The approach can be applied to various transport phenomena at the nanoscale involving carriers of different physical nature and behavior.