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Since the last century, considerable efforts have been devoted to the study of valley-degenerate narrow gap semiconductors, such as the Pb$_{1-x}$Sn$_x$Se alloy. This material possesses band minima at the $L$-points of their Brillouin zone, yielding a valley degeneracy of four. However, in (111)-oriented films, it is still not fully understood how differences between the longitudinal valley, oriented along the growth axis, and the oblique valleys, oriented at an angle with respect to that axis, appear in magneto-optical infrared spectroscopy. In this work, we report a magnetooptical study on this family of alloys, focusing on an anomaly in the interband transition of the peak intensity ratio of longitudinal and oblique valleys under a magnetic field applied along the [111] direction. Based on the Mitchell-Wallis model, we provide a theoretical fit for the experimental transmission data, which quantitatively explains the spectral shape of the data at magnetic fields as high as 35T. In particular, we attribute this anomalous peak intensity variation to the carrier density difference between the two types of valleys as well as the field-dependent thin-film interference. Our analysis also allows for the extraction of the real and imaginary parts of the dielectric function., Comment: 11 pages, 9 figures. Comments are welcome

Probing the quantum geometry and topology in condensed matter systems has relied heavily on static electronic transport experiments in magnetic fields. Yet, contact-free optical measurements have rarely been explored. Magnetic dichroism (MCD), the nonreciprocal absorption of circular polarized light, was theoretically linked to the quantized anomalous Hall effect in magnetic insulators and can identify the bands and momenta responsible for the underlying Berry Curvature (BC). Detecting BC through MCD faces two challenges: First, the relevant inter-band transitions usually generate MCD in the infrared (IR) range, requiring large samples with high quality. Second, while most magnetic materials are metallic, the relation between MCD and BC in metals remains unclear. Here, we report the observation of MCD in the IR range along with the anomalous Hall effect in thin film MnBi2Te4. Both phenomena emerge with a field-driven phase transition from an antiferromagnet to a canted ferromagnet. By theoretically relating the MCD to the anomalous Hall effect via BC in a metal, we show that this transition accompanies an abrupt onset of BC, signaling a topological phase transition from a topological insulator to a doped Chern insulator. Our density functional theory calculation suggests the MCD signal mainly originates from an optical transition at the Brillouin zone edge, hinting at a potential new source of BC away from the commonly considered {\Gamma} point. Our findings demonstrate a novel experimental approach for detecting BC and identifying the responsible bands and momenta, generally applicable to magnetic materials.

The Mott-Ioffe-Regel limit sets the lower bound of carrier mean free path for coherent quasiparticle transport. Metallicity beyond this limit is of great interest because it is often closely related to quantum criticality and unconventional superconductivity. Progress along this direction mainly focuses on the strange-metal behaviors originating from the evolution of quasiparticle scattering rate such as linear-in-temperature resistivity, while the quasiparticle coherence phenomena in this regime are much less explored due to the short mean free path at the diffusive bound. Here we report the observation of quantum oscillations from Landau quantization near the Mott-Ioffe-Regel limit in CaAs3. Despite the insulator-like temperature dependence of resistivity, CaAs3 presents giant magnetoresistance and prominent Shubnikov-de Haas oscillations from Fermi surfaces, indicating highly coherent band transport. In contrast, the quantum oscillation is absent in the magnetic torque. The quasiparticle effective mass increases systematically with magnetic fields, manifesting a much larger value than the expectation given by magneto-infrared spectroscopy. It suggests a strong many-body renormalization effect near Fermi surface. We find that these unconventional behaviors may be explained by the interplay between the mobility edge and the van Hove singularity, which results in the formation of coherent cyclotron orbits emerging at the diffusive bound. Our results call for further study on the electron correlation effect of the van Hove singularity., Comment: 18 pages, 5 figures

Topological semimetals with massless Dirac and Weyl fermions represent the forefront of quantum materials research. In two dimensions, a peculiar class of fermions that are massless in one direction and massive in the perpendicular direction was predicted fifteen years ago. These highly exotic quasiparticles - the semi-Dirac fermions - ignited intense theoretical interest but remain undetected. Using magneto-optical spectroscopy, we demonstrate the defining feature of semi-Dirac fermions - B^(2/3) scaling of Landau levels - in a prototypical nodal-line metal ZrSiS. In topological metals, including ZrSiS, nodal-lines extend the band degeneracies from isolated points to lines, loops or even chains in the momentum space. With ab initio calculations and theoretical modeling, we pinpoint the observed semi-Dirac spectrum to the crossing points of nodal-lines in ZrSiS. Crossing nodal-lines exhibit a continuum absorption spectrum but with singularities that scale as B^(2/3) at the crossing. Our work sheds light on the hidden quasiparticles emerging from the intricate topology of crossing nodal-lines.

Band gap is known as an effective parameter for tuning the Lande $g$-factor in semiconductors and can be manipulated in a wide range through the bowing effect in ternary alloys. In this work, using the recently developed virtual substrate technique, high-quality InAsSb alloys throughout the whole Sb composition range are fabricated and a large $g$-factor of $g\approx -90$ at the minimum band gap of $\sim 0.1$ eV, which is almost twice that in bulk InSb is found. Further analysis to the zero gap limit reveals a possible gigantic $g$-factor of $g\approx -200$ with a peculiar relativistic Zeeman effect that disperses as the square root of magnetic field. Such a $g$-factor enhancement toward the narrow gap limit cannot be quantitatively described by the conventional Roth formula, as the orbital interaction effect between the nearly triply degenerated bands becomes the dominant source for the Zeeman splitting. These results may provide new insights into realizing large $g$-factors and spin polarized states in semiconductors and topological materials.

Using optical magneto-spectroscopy, we investigate the magnetic excitations of Na$_2$Co$_2$TeO$_6$ in a broad magnetic field range ($0\ \rm{T}\leq B\leq 17.5\ \rm{T}$) at low temperature. Our measurements reveal rich spectra of in-plane magnetic excitations with a surprisingly large number of modes, even in the high-field spin-polarized state. Theoretical calculations find that the Na-occupation disorder in \NCTO plays a crucial role in generating these modes. Our work demonstrates the necessity to consider disorder in the spin environment in the search for Kitaev quantum spin liquid states in practicable materials.

Arising from the extreme/saddle point in electronic bands, Van Hove singularity (VHS) manifests divergent density of states (DOS) and induces various new states of matter such as unconventional superconductivity. VHS is believed to exist in one and two dimensions, but rarely found in three dimension (3D). Here, we report the discovery of 3D VHS in a topological magnet EuCd2As2 by magneto-infrared spectroscopy. External magnetic fields effectively control the exchange interaction in EuCd2As2, and shift 3D Weyl bands continuously, leading to the modification of Fermi velocity and energy dispersion. Above the critical field, the 3D VHS forms and is evidenced by the abrupt emergence of inter-band transitions, which can be quantitatively described by the minimal model of Weyl semimetals. Three additional optical transitions are further predicted theoretically and verified in magneto-near-infrared spectra. Our results pave the way to exploring VHS in 3D systems and uncovering the coordination between electronic correlation and the topological phase.

Two-dimensional (2D) magnetic systems possess versatile magnetic order and can host tunable magnons carrying spin angular momenta. Recent advances show angular momentum can also be carried by lattice vibrations in the form of chiral phonons. However, the interplay between magnons and chiral phonons as well as the details of chiral phonon formation in a magnetic system are yet to be explored. Here, we report the observation of magnon-induced chiral phonons and chirality selective magnon-phonon hybridization in a layered zigzag antiferromagnet (AFM) FePSe$_3$. With a combination of magneto-infrared and magneto-Raman spectroscopy, we observe chiral magnon polarons (chiMP), the new hybridized quasiparticles, at zero magnetic field. The hybridization gap reaches 0.25~meV and survives down to the quadrilayer limit. Via first principle calculations, we uncover a coherent coupling between AFM magnons and chiral phonons with parallel angular momenta, which arises from the underlying phonon and space group symmetries. This coupling lifts the chiral phonon degeneracy and gives rise to an unusual Raman circular polarization of the chiMP branches. The observation of coherent chiral spin-lattice excitations at zero magnetic field paves the way for angular momentum-based hybrid phononic and magnonic devices.

Lanthanides in the trivalent oxidation state are typically described using an ionic picture that leads to localized magnetic moments. The hierarchical energy scales associated with trivalent lanthanides produce desirable properties for e.g., molecular magnetism, quantum materials, and quantum transduction. Here, we show that this traditional ionic paradigm breaks down for praseodymium in the 4+ oxidation state. Synthetic, spectroscopic, and theoretical tools deployed on several solid-state Pr4+ oxides uncover the unusual participation of 4f orbitals in bonding and the anomalous hybridization of the 4f1 configuration with ligand valence electrons, analogous to transition metals. The resulting competition between crystal-field and spin-orbit-coupling interactions fundamentally transforms the spin-orbital magnetism of Pr4+, which departs from the Jeff =1/2 limit and resembles that of high-valent actinides. Our results show that Pr4+ ions are in a class on their own, where the hierarchy of single-ion energy scales can be tailored to explore new correlated phenomena in quantum materials., Comment: 9 pages, 4 figures, and SI (47 pages)

We report the temperature evolution of the Dirac band in semiconducting zirconium pentatelluride (ZrTe$_5$) using magneto-infrared spectroscopy. We find that the band gap is temperature independent at low temperatures and increases with temperature at elevated temperatures. Although such an observation seems to support a weak topological insulator phase at all temperatures and defy the previously reported topological phase transition (TPT) at an intermediate temperature in ZrTe$_5$, we show that it is also possible to explain the observation by considering the effect of conduction-valence band mixing and band inversion with a strong topological insulator phase at low temperatures. Our work provides an alternative picture of the band gap evolution across TPT.

Topological surface-states can acquire an energy gap when time-reversal symmetry is broken by interfacing with a magnetic insulator. This gap has yet to be measured. Such topological-magnetic insulator heterostructures can host a quantized anomalous Hall effect and can allow the control of the magnetic state of the insulator in a spintronic device. In this work, we observe the energy gap of topological surface-states in proximity to a magnetic insulator using magnetooptical Landau level spectroscopy. We measure Pb1-xSnxSe/EuSe heterostructures grown by molecular beam epitaxy exhibiting a record mobility and low Fermi energy. Through temperature dependent measurements and theoretical calculations, we show this gap is likely due to quantum confinement and conclude that the magnetic proximity effect is weak in this system. This weakness is disadvantageous for the realization of the quantum anomalous Hall effect, but favorable for spintronic devices which require the preservation of spin-momentum locking at the Fermi level., Comment: 10.1038/s42005-023-01327-5

Landau band crossings typically stem from the intra-band evolution of electronic states in magnetic fields and enhance the interaction effect in their vicinity. Here in the extreme quantum limit of topological insulator HfTe5, we report the observation of a topological Lifshitz transition from inter-band Landau level crossings using magneto-infrared spectroscopy. By tracking the Landau level transitions, we demonstrate that band inversion drives the zeroth Landau bands to cross with each other after 4.5 T and forms one-dimensional Weyl mode with fundamental gap persistently closed. The unusual reduction of the zeroth Landau level transition activity suggests a topological Lifshitz transition at 21 T which shifts the Weyl mode close to Fermi level. As a result, a broad and asymmetric absorption feature emerges due to the Pauli blocking effect in one dimension, along with a distinctive negative magneto-resistivity. Our results provide a strategy for realizing one-dimensional Weyl quasiparticles in bulk crystals.

Realizing a large Land\'{e} $g$-factor of electrons in solid-state materials has long been thought of as a rewarding task as it can trigger abundant immediate applications in spintronics and quantum computing. Here, by using metamorphic InAsSb/InSb superlattices (SLs), we demonstrate an unprecedented high value of $g\approx 104$, twice larger than that in bulk InSb, and fully spin-polarized states at low magnetic fields. In addition, we show that the $g$-factor can be tuned on demand from 20 to 110 via varying the SL period. The key ingredients of such a wide tunability are the wavefunction mixing and overlap between the electron and hole states, which have drawn little attention in prior studies. Our work not only establishes metamorphic InAsSb/InSb as a promising and competitive material platform for future quantum devices but also provides a new route toward $g$-factor engineering in semiconductor structures.

Topological semimetals are predicted to exhibit unconventional electrodynamics, but a central experimental challenge is singling out the contributions from the topological bands. TaAs is the prototypical example, where 24 Weyl points and 8 trivial Fermi surfaces make the interpretation of any experiment in terms of band topology ambiguous. We report magneto-infrared reflection spectroscopy measurements on TaAs. We observed sharp inter-Landau level transitions from a single pocket of Weyl Fermions in magnetic fields as low as 0.4 tesla. We determine the W2 Weyl point to be 8.3 meV below the Fermi energy, corresponding to a quantum limit - the field required to reach the lowest LL - of 0.8 Tesla - unprecedentedly low for Weyl Fermions. LL spectroscopy allows us to isolate these Weyl Fermions from all other carriers in TaAs and our result provides a new way for directly exploring the more exotic quantum phenomena in Weyl semimetals, such as the chiral anomaly.

Emergent cooperative motions of individual degrees of freedom, i.e. collective excitations, govern the low-energy response of system ground states under external stimulations and play essential roles for understanding many-body phenomena in low-dimensional materials. The hybridization of distinct collective modes provides a route towards coherent manipulation of coupled degrees of freedom and quantum phases. In magnets, strong coupling between collective spin and lattice excitations, i.e., magnons and phonons, can lead to coherent quasi-particle magnon polarons. Here, we report the direct observation of a series of terahertz magnon polarons in a layered zigzag antiferromagnet FePS3 via far-infrared (FIR) transmission measurements. The characteristic avoided-crossing behavior is clearly seen as the magnon-phonon detuning is continuously changed via Zeeman shift of the magnon mode. The coupling strength g is giant, achieving 120 GHz (0.5 meV), the largest value reported so far. Such a strong coupling leads to a large ratio of g to the resonance frequency (g/{\omega}) of 4.5%, and a value of 29 in cooperativity (g^2/{\gamma}_{ph}{\gamma}_{mag}). Experimental results are well reproduced by first-principle calculations, where the strong coupling is identified to arise from phonon-modulated anisotropic magnetic interactions due to spin-orbit coupling. These findings establish FePS3 as an ideal testbed for exploring hybridization-induced topological magnonics in two dimensions and the coherent control of spin and lattice degrees of freedom in the terahertz regime.

Low temperature optical spectroscopy in applied magnetic fields provides clear evidence of magnetoelastic coupling in the spin ice material Ho$_2$Ti$_2$O$_7$. In far-IR reflectometry measurements, we observe field dependent features around 30, 61, 72 and 78~meV, energies corresponding to crystal electronic field (CEF) doublets. The calculations of the crystal-field Hamiltonian model confirm that the observed features in IR spectra are consistent with magnetic-dipole-allowed excitations from the ground state to higher $^5$I$_8$ CEF levels. We present the CEF parameters that best describe our field-dependent IR reflectivity measurements. Additionally, we identify a weak field-dependent shoulder near one of the CEF doublets. This indicates that this level is split even in zero-field, which we associate with a vibronic bound state. Modeling of the observed splitting shows that the phonon resides at slightly lower energy compared to the CEF level that it couples to, which is in contrast with previously published inelastic neutron measurements. The magnetic field dependence of the vibronic state shows a gradual decoupling of the phonon with the CEF level as it shifts. This approach should work in pyrochlores and other systems that have magnetic dipole transitions in the IR spectroscopic range, which can elucidate the presence and the ability to tune the nature of vibronic states in a wide variety of materials.

Molecular vibrations play a key role in magnetic relaxation processes of molecular spin qubits as they couple to spin states, leading to the loss of quantum information. Direct experimental determination of vibronic coupling is crucial to understand and control the spin dynamics of these nano-objects, which represent the limit of miniaturization for quantum devices. Herein, we measure the vibrational properties of the molecular spin qubit $[$Ho(W$_5$O$_{18}$)$_2]^{9-}$ by means of magneto-infrared spectroscopy. Our results allow us to unravel the vibrational decoherence pathways in combination with $ab$ $initio$ calculations including vibronic coupling. We observe field-induced spectral changes near 63 and 370 cm$^{-1}$ that are modeled in terms of $f$-manifold crystal field excitations activated by odd-symmetry vibrations. The overall extent of vibronic coupling in this system is limited by a transparency window in the phonon density of states that acts to keep the intramolecular vibrations and $M_J$ levels apart. These findings advance the understanding of vibronic coupling in molecular magnets, place significant constraints on the pattern of crystal field levels in these systems, and provide a strategy for designing molecular spin qubits with improved coherence lifetimes., Comment: 22 pages

A Dirac-type energy spectrum was demonstrated in gapless ultra-short-period metamorphic InAsSb/InSb superlattices by angle-resolved photoemission spectroscopy (ARPES_ measurements. The Fermi velocity value 7.4x10^5 m/s in a gapless superlattice with a period of 6.2nm is in a good agreement with the results of magneto-absorption experiments. An "inverted" bandgap opens in the center of the Brillouin zone at higher temperatures and in the SL with a larger period. The ARPES data indicate the presence of a surface electron accumulation layer