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Fermi surface and Berry phase analysis for Dirac nodal line semimetals: Cautionary tale from SrGa 2 and BaGa 2

A Berry phase of odd multiples of 𝜋 inferred from quantum oscillations (QOs) has often been treated as evidence for nontrivial reciprocal space topology. However, disentangling the Berry phase values from the Zeeman effect and the orbital magnetic moment is often challenging. In centrosymmetric compounds, the case is simpler as the orbital magnetic moment contribution is negligible. Although the Zeeman effect can be significant, it is usually overlooked in most studies of QOs in centrosymmetric compounds. Here, we present a detailed study on the nonmagnetic centrosymmetric SrGa 2 and BaGa 2 , which are predicted to be Dirac nodal line semimetals based on density functional theory (DFT) calculations. Evidence of the nontrivial topology is found in magnetotransport measurements. The Fermi surface topology and band structure are carefully studied through a combination of angle-dependent QOs, angle-resolved photoemission spectroscopy (ARPES), and DFT calculations, where the nodal line is observed in the vicinity of the Fermi level. Strong de Haas–van Alphen fundamental oscillations associated with higher harmonics are observed in both compounds, which are well fitted by the Lifshitz-Kosevich (LK) formula. However, even with the inclusion of higher harmonics in the fitting, we found that the Berry phases cannot be unambiguously determined when the Zeeman effect is included. We revisit the LK formula and analyze the phenomena and outcomes that were associated with the Zeeman effect in previous studies. Our experimental results confirm that SrGa 2 and BaGa 2 are Dirac nodal line semimetals. Additionally, we highlight the often overlooked role of spin-damping terms in Berry phase analysis.

36 MATERIALS SCIENCE↗

Materials Data on SrGa by Materials Project

SrGa crystallizes in the cubic P2_13 space group. The structure is three-dimensional. there are four inequivalent Sr sites. In the first Sr site, Sr is bonded in a 6-coordinate geometry to six Ga atoms. There are a spread of Sr–Ga bond distances ranging from 3.28–3.68 Å. In the second Sr site, Sr is bonded in a 7-coordinate geometry to seven Ga atoms. There are a spread of Sr–Ga bond distances ranging from 3.31–3.58 Å. In the third Sr site, Sr is bonded in a 6-coordinate geometry to six Ga atoms. There are three shorter (3.38 Å) and three longer (3.42 Å) Sr–Ga bond lengths. In the fourth Sr site, Sr is bonded in a 1-coordinate geometry to seven Ga atoms. There are a spread of Sr–Ga bond distances ranging from 3.09–3.51 Å. There are four inequivalent Ga sites. In the first Ga site, Ga is bonded in a 9-coordinate geometry to six Sr and three Ga atoms. There are two shorter (2.72 Å) and one longer (2.76 Å) Ga–Ga bond lengths. In the second Ga site, Ga is bonded in a 9-coordinate geometry to seven Sr and two equivalent Ga atoms. Both Ga–Ga bond lengths are 2.82 Å. In the third Ga site, Ga is bonded in a 7-coordinate geometry to seven Sr atoms. In the fourth Ga site, Ga is bonded in a 9-coordinate geometry to six Sr and three equivalent Ga atoms.

36 MATERIALS SCIENCE↗

Origin of charge density wave in topological semimetals SrAl 4 and EuAl 4

Topological semimetals in BaAl 4 -type structure show many interesting behaviors, such as charge density wave (CDW) in SrAl 4 and EuAl 4 , but not the isostructural and isovalent BaAl 4 , SrGa 4 , and BaGa 4 . Here using Wannier functions based on density functional theory, we calculate the susceptibility functions with millions of k-points to reach the small q-vector and study the origin and driving force behind the CDW. Our comparative study reveals that the origin of the CDW in SrAl 4 and EuAl 4 is the strong electron-phonon coupling interaction for the transverse acoustic mode at small q-vector along the Γ-Z direction besides the maximum of the real part of the susceptibility function from the nested Fermi surfaces of the Dirac-like bands, which explains well the absence of CDW in the other closely related compounds in a good agreement with experiment. We also connect the different CDW behaviors in the Al compounds to the macroscopic elastic properties.

36 MATERIALS SCIENCE↗