Giant topological longitudinal circular photo-galvanic effect in the chiral multifold semimetal CoSi

The absence of mirror symmetry, or chirality, is behind striking natural phenomena found in systems as diverse as DNA and crystalline solids. A remarkable example occurs when chiral semimetals with topologically protected band degeneracies are illuminated with circularly polarized light. Under the right conditions, the part of the generated photocurrent that switches sign upon reversal of the light’s polarization, known as the circular photo-galvanic effect, is predicted to depend only on fundamental constants. The conditions to observe quantization are non-universal, and depend on material parameters and the incident frequency. In this work, we perform terahertz emission spectroscopy with tunable photon energy from 0.2 –1.1 eV in the chiral topological semimetal CoSi. We identify a large longitudinal photocurrent peaked at 0.4 eV reaching ~550 μ A/V2, which is much larger than the photocurrent in any chiral crystal reported in the literature. Using first-principles calculations we establish that the peak originates only from topological band crossings, reaching 3.3 ± 0.3 in units of the quantization constant. Our calculations indicate that the quantized circular photo-galvanic effect is within reach in CoSi upon doping and increase of the hot-carrier lifetime. The large photo-conductivity suggests that topological semimetals could potentially be used as novel mid-infrared detectors.

Linear and nonlinear optical responses in the chiral multifold semimetal RhSi

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.

Terahertz Emission Spectroscopy and Microscopy on Ultrawide Bandgap Semiconductor β-Ga2O3

Although gallium oxide Ga2O3 is attracting much attention as a next-generation ultrawide bandgap semiconductor for various applications, it needs further optical characterization to support its use in higher-performance devices. In the present study, terahertz (THz) emission spectroscopy (TES) and laser THz emission microscopy (LTEM) are applied to Sn-doped, unintentionally doped, and Fe-doped β-Ga2O3 wafers. Femtosecond (fs) laser illumination generated THz waves based on the time derivative of the photocurrent. TES probes the motion of ultrafast photocarriers that are excited into a conduction band, and LTEM visualizes their local spatiotemporal movement at a spatial and temporal resolution of laser beam diameter and a few hundred fs. In contrast, one observes neither photoluminescence nor distinguishable optical absorption for a band-to-band transition for Ga2O3. TES/LTEM thus provides complementary information on, for example, the local mobility, surface potential, defects, band bending, and anisotropic photo-response in a noncontact, nondestructive manner. The results indicated that the band bends downward at the surface of an Fe-doped wafer, unlike with an n-type wafer, and the THz emission intensity is qualitatively proportional to the product of local electron mobility and diffusion potential, and is inversely proportional to penetration depth, all of which have a strong correlation with the quality of the materials and defects/impurities in them.