Observation of Type-II Topological Nodal-Line Fermions in ZrSiSe.

Recently, there has been significant interest in topological nodal-line semimetals due to their linear energy dispersion with one-dimensional nodal lines or loops. These materials exhibit fascinating physical properties, such as drumhead surface states and 3D anisotropic nodal-line structures. Similar to Weyl semimetals, type-II nodal-line semimetals have two crossing bands that are both electron-like or hole-like along a certain direction. However, the direct observation of type-II nodal-line Fermions has been challenging due to the lack of suitable material platforms and the low density of states. Here we present experimental evidence for the coexistence of both type-I and type-II nodal-line Fermions in ZrSiSe, which was obtained through magneto-optical and angle-resolved photoemission spectroscopy (ARPES) measurements. Our density functional theory calculations predict that the type-II nodal-line structure can be developed in the Z-R line of the first Brillouin zone based on the lattice constants of the grown single crystal. Indeed, ARPES measurements reveal the type-II nodal-line band structure. The extracted type-II Landau level transitions from magneto-optical measurements exhibit good agreement with the calculated type-II energy dispersion model based on the band structure. Our experimental results demonstrate that ZrSiSe possesses two types of nodal-line Fermions, distinguishing it from other ZrSiX (X = S, Te) materials and positioning it as an ideal platform for investigating type-II nodal-line semimetals.

Coercive Fields Exceeding 30 T in the Mixed-Valence Single-Molecule Magnet (CpiPr5)2Ho2I3.

Mixed-valence dilanthanide complexes of the type (CpiPr5)2Ln2I3 (CpiPr5 = pentaisopropylcyclopentadienyl; Ln = Gd, Tb, Dy) featuring a direct Ln-Ln σ-bonding interaction have been shown to exhibit well-isolated high-spin ground states and, in the case of the Tb and Dy variants, a strong axial magnetic anisotropy that gives rise to a large magnetic coercivity. Here, we report the synthesis and characterization of two new mixed-valence dilanthanide compounds in this series, (CpiPr5)2Ln2I3 (1-Ln; Ln = Ho, Er). Both compounds feature a Ln-Ln bonding interaction, the first such interaction in any molecular compounds of Ho or Er. Like the Tb and Dy congeners, both complexes exhibit high-spin ground states arising from strong spin-spin coupling between the lanthanide 4f electrons and a single σ-type lanthanide-lanthanide bonding electron. Beyond these similarities, however, the magnetic properties of the two compounds diverge. In particular, 1-Er does not exhibit observable magnetic blocking or slow magnetic relaxation, while 1-Ho exhibits magnetic blocking below 28 K, which is the highest temperature among Ho-based single-molecule magnets, and a spin reversal barrier of 556(4) cm-1. Additionally, variable-field magnetization data collected for 1-Ho reveal a coercive field of greater than 32 T below 8 K, more than 6-fold higher than observed for the bulk magnets SmCo5 and Nd2Fe14B, and the highest coercive field reported to date for any single-molecule magnet or molecule-based magnetic material. Multiconfigurational calculations, supported by far-infrared magnetospectroscopy data, reveal that the stark differences in magnetic properties of 1-Ho and 1-Er arise from differences in the local magnetic anisotropy of the lanthanide centers.

Cobalt(II) Single-Ion Magnet Coordinated by Double Deprotonation of 2,2'-Bipyridine-6,6'-diol Ligands.

In this study, we synthesized a new Co(II) complex, [NMe4]2[Co(bpyO2)2] (1), using deprotonated 2,2'-bipyridine-6,6'-diol ligands (bpyO2 2-). This compound exhibits a significant zero-field splitting (D) value. The far-infrared magneto spectroscopy and high-frequency and field electron paramagnetic resonance (HFEPR) measurements indicated that compound 1 possesses D = -54.8 cm-1 and E ∼ 0 cm-1. These findings were subsequently confirmed by other experimental data, including DC magnetic susceptibilities and variable temperature and variable magnetic field reduced magnetizations. Additionally, we conducted a series of AC magnetic susceptibility measurements to investigate the kinetics of magnetization relaxation. Below 6.6 K and under zero external magnetic field, fast quantum tunneling of magnetization (QTM) dominates (∼570 Hz), and temperature-independent out-of-phase signals are observed. Above 8.1 K, temperature-dependent behavior is observed. Furthermore, we examined the AC magnetic susceptibility behavior under external magnetic fields ranging from 300 to 4000 G. The effect of QTM is significantly reduced in the presence of an external magnetic field. Temperature-dependent behavior is primarily governed by Raman relaxation. Through structural analysis of compound 1 and a series of pure nitrogen-coordinated single-ion magnets (SIMs), we propose that the oxo substituents from the double-deprotonated form of the 2,2'-bipyridine-6,6'-diol ligands donate their negative charge to the pyridine ring, forming amido anion sites. This triggers a more pronounced out-of-phase signal than that observed in pure pyridine-coordinated compounds. Moreover, we observed intermolecular interactions, including intermolecular hydrogen bonding, which, to some extent, influenced the slow relaxation of molecules. Therefore, we speculate that the slow relaxation phenomenon of compound 1 may be attributed to the combination of oxo back-donating effects and intermolecular interactions.

Control of the geometry and anisotropy driven by the combination of steric and anion coordination effects in CoII complexes with N6-tripodal ligands: the impact of the size of the ligand on the magnetization relaxation time.

Four mononuclear CoII complexes of formula [Co(L)(SCN)2(CH3OH)0.5(H2O)0.5]·1.5H2O·0.75CH3OH (1), [Co(L1)Cl2]·H2O·2CH3CN (2), [Co(L1)(SCN)2]·1.5H2O·CH3OH (3) and [Co(L1)]ClO4·2CH3OH (4) were prepared from the N6-tripodal Schiff base ligands (S)P[N(Me)NC(H)2-Q]3 (L) and (S)P[N(Me)NC(H)1-ISOQ]3 (L1), where Q and ISOQ represent quinolyl and isoquinolyl moieties, respectively. In 1, the L ligand does not coordinate to the CoII ion in a tripodal manner but using a new N,N,S tridentate mode, which is due to the fact that the N6-tripodal coordination promotes a strong steric hindrance between the quinolyl moieties. However, L1 can coordinate to the CoII ions either in a tripodal manner using CoII salts with poorly coordinating anions to give 4 or in a bisbidentate fashion using CoII salt-containing medium to strongly coordinating anions to afford 2 and 3. In the case of L1, there is no steric hindrance between ISOQ moieties after coordination to the CoII ion. The CoII ion exhibits a distorted octahedral geometry for compounds 1-3, with the anions in cis positions for the former and in trans positions for the two latter compounds. Compound 4 shows an intermediate geometry between an octahedral and trigonal prism but closer to the latter one. DC magnetic properties, HFEPR and FIRMS measurements and ab initio calculations demonstrate that distorted octahedral complexes 1-3 exhibit easy-plane magnetic anisotropy (D > 0), whereas compound 4 shows large easy-axis magnetic anisotropy (D < 0). Comparative analysis of the magneto-structural data underlines the important role that is played not only by the coordination geometry but also the electronic effects in determining the anisotropy of the CoII ions. Compounds 2-3 show a field-induced slow relaxation of magnetization. Despite its large easy-axis magnetic anisotropy, compound 4 does not show significant slow relaxation (SMR) above 2 K under zero applied magnetic fields, but its magnetic dilution with ZnII triggers SMR at zero field. Finally, it is worth remarking that compounds 2-4 show smaller relaxation times than the analogous complexes with the tripodal ligand bearing in its arms pyridine instead of isoquinoline moieties, which is most likely due to the increase of the molecular size in the former one.

Dipolar Coupling as a Mechanism for Fine Control of Magnetic States in ErCOT-Alkyl Molecular Magnets.

The design of molecular magnets has progressed greatly by taking advantage of the ability to impart successive perturbations and control vibronic transitions in 4fn systems through the careful manipulation of the crystal field. Herein, we control the orientation and rigidity of two dinuclear ErCOT-based molecular magnets: the inversion-symmetric bridged [ErCOT(µ-Me)(THF)]2 (2) and the nearly linear Li[(ErCOT)2(µ-Me)3] (3). The conserved anisotropy of the ErCOT synthetic unit facilitates the direction of the arrangement of its magnetic anisotropy for the purposes of generating controlled internal magnetic fields, improving control of the energetics and transition probabilities of the electronic angular momentum states with exchange biasing via dipolar coupling. This control is evidenced through the introduction of a second thermal barrier to relaxation operant at low temperatures that is twice as large in 3 as in 2. This barrier acts to suppress through-barrier relaxation by protecting the ground state from interacting with stray local fields while operating at an energy scale an order of magnitude smaller than the crystal field term. These properties are highlighted when contrasted against the mononuclear structure ErCOT(Bn)(THF)2 (1), in which quantum tunneling of the magnetization processes dominate, as demonstrated by magnetometry and ab initio computational methods. Furthermore, far-infrared magnetospectroscopy measurements reveal that the increased rigidity imparted by successive removal of solvent ligands when adding bridging methyl groups, along with the increased excited state purity, severely limits local spin-vibrational interactions that facilitate magnetic relaxation, manifesting as longer relaxation times in 3 relative to those in 2 as temperature is increased.

The discovery of three-dimensional Van Hove singularity.

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.

Electronic Structure of Three-Coordinate FeII and CoII ß-Diketiminate Complexes.

The ß-diketiminate supporting group, [ArNCRCHCRNAr]-, stabilizes low coordination number complexes. Four such complexes, where R = tert-butyl, Ar = 2,6-diisopropylphenyl, are studied: (nacnactBu)ML, where M = FeII, CoII and L = Cl, CH3. These are denoted FeCl, FeCH3, CoCl, and CoCH3 and have been previously reported and structurally characterized. The two FeII complexes (S = 2) have also been previously characterized by Mössbauer spectroscopy, but only indirect assessment of the ligand-field splitting and zero-field splitting (zfs) parameters was available. Here, EPR spectroscopy is used, both conventional field-domain for the CoII complexes (with S = 3/2) and frequency-domain, far-infrared magnetic resonance spectroscopy (FIRMS) for all four complexes. The CoII complexes were also studied by magnetometry. These studies allow accurate determination of the zfs parameters. The two FeII complexes are similar with nearly axial zfs and large magnitude zfs given by D = -37 ± 1 cm-1 for both. The two CoII complexes likewise exhibit large and nearly axial zfs, but surprisingly, CoCl has positive D = +55 cm-1 while CoCH3 has negative D = -49 cm-1. Theoretical methods were used to probe the electronic structures of the four complexes, which explain the experimental spectra and the zfs parameters.

Large Magnetic Anisotropy in Mono- and Binuclear cobalt(II) Complexes: The Role of the Distortion of the Coordination Sphere in Validity of the Spin-Hamiltonian Formalism.

To get a better insight into understanding the factors affecting the enhancement of the magnetic anisotropy in single molecule (single ion) magnets, two cobalt(II) complexes based on a tridentate ligand 2,6-di(thiazol-2-yl)pyridine substituted at the 4-position with N-methyl-pyrrol-2-yl have been synthesized and studied by X-ray crystallography, AC and DC magnetic data, FIRMS and HFEPR spectra, and theoretical calculations. The change of the counteranion in starting Co(II) salts results in the formation of pentacoordinated mononuclear [Co(mpyr-dtpy)Cl2]·2MeCN (1) complex and binuclear [Co(mpyr-dtpy)2][Co(NCS)4] (2) compound. The observed marked distortion of trigonal bipyramid geometry in 1 and cationic octahedral and anionic tetrahedral units in 2 brings up a question about the validity of the spin-Hamiltonian formalism and the possibility of determining the value and sign of the zero-field splitting D parameter. Both complexes exhibit field-induced slow magnetic relaxation with two or three relaxation channels at BDC = 0.3 T. The high-frequency relaxation time in the reciprocal form τ(HF)-1 = CTn develops according to the Raman relaxation mechanism (for 2, n = 8.8) and the phonon-bottleneck-like mechanism (for 1, n = 2.3). The high-frequency relaxation time at T = 2.0 K and BDC = 0.30 T is τ(HF) = 96 and 47 µs for 1 and 2, respectively.

Disorder-Enriched Magnetic Excitations in a Heisenberg-Kitaev Quantum Magnet Na_{2}Co_{2}TeO_{6}.

Using optical magnetospectroscopy, we investigate the magnetic excitations of Na_{2}Co_{2}TeO_{6} in a broad magnetic field range (0 T≤B≤17.5 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 Na_{2}Co_{2}TeO_{6} plays a crucial role in generating these modes. Our Letter demonstrates the necessity to consider disorder in the spin environment in the search for Kitaev quantum spin liquid states in practicable materials.

Chirality selective magnon-phonon hybridization and magnon-induced chiral phonons in a layered zigzag antiferromagnet.

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) FePSe3. 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.

Chemical design of electronic and magnetic energy scales of tetravalent praseodymium materials.

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 tetravalent 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 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.

Spectroscopic and Magnetic Studies of Co(II) Scorpionate Complexes: Is There a Halide Effect on Magnetic Anisotropy?

The observation of single-molecule magnetism in transition-metal complexes relies on the phenomenon of zero-field splitting (ZFS), which arises from the interplay of spin-orbit coupling (SOC) with ligand-field-induced symmetry lowering. Previous studies have demonstrated that the magnitude of ZFS in complexes with 3d metal ions is sometimes enhanced through coordination with heavy halide ligands (Br and I) that possess large free-atom SOC constants. In this study, we systematically probe this "heavy-atom effect" in high-spin cobalt(II)-halide complexes supported by substituted hydrotris(pyrazol-1-yl)borate ligands (TptBu,Me and TpPh,Me). Two series of complexes were prepared: [CoIIX(TptBu,Me)] (1-X; X = F, Cl, Br, and I) and [CoIIX(TpPh,Me)(HpzPh,Me)] (2-X; X = Cl, Br, and I), where HpzPh,Me is a monodentate pyrazole ligand. Examination with dc magnetometry, high-frequency and -field electron paramagnetic resonance, and far-infrared magnetic spectroscopy yielded axial (D) and rhombic (E) ZFS parameters for each complex. With the exception of 1-F, complexes in the four-coordinate 1-X series exhibit positive D-values between 10 and 13 cm-1, with no dependence on halide size. The five-coordinate 2-X series exhibit large and negative D-values between -60 and -90 cm-1. Interpretation of the magnetic parameters with the aid of ligand-field theory and ab initio calculations elucidated the roles of molecular geometry, ligand-field effects, and metal-ligand covalency in controlling the magnitude of ZFS in cobalt-halide complexes.

Pushing up the easy-axis magnetic anisotropy and relaxation times in trigonal prismatic CoII mononuclear SMMs by molecular structure design.

The replacement of pyridine by 1-methyl-imidazol in the arms of a N6-tripodal ligand allows preparing two new CoII complexes with quasi-ideal triangular prismatic geometry, which behave as SIMs (Single Ion Magnets) at zero dc field with enhanced axial magnetic anisotropy, magnetic relaxation times and magnetic hysteresis.

Magnetic anisotropy and structural flexibility in the field-induced single ion magnets [Co{(OPPh2)(EPPh2)N}2], E = S, Se, explored by experimental and computational methods.

During the last few years, a large number of mononuclear Co(II) complexes of various coordination geometries have been explored as potential single ion magnets (SIMs). In the work presented herein, the Co(II) S = 3/2 tetrahedral [Co{(OPPh2)(EPPh2)N}2], E = S, Se, complexes (abbreviated as CoO2E2), bearing chalcogenated mixed donor-atom imidodiphosphinato ligands, were studied by both experimental and computational techniques. Specifically, direct current (DC) magnetometry provided estimations of their zero-field splitting (zfs) axial (D) and rhombic (E) parameter values, which were more accurately determined by a combination of far-infrared magnetic spectroscopy and high-frequency and -field EPR spectroscopy studies. The latter combination of techniques was also implemented for the S = 3/2 tetrahedral [Co{(EPiPr2)2N}2], E = S, Se, complexes, confirming the previously determined magnitude of their zfs parameters. For both pairs of complexes (E = S, Se), it is concluded that the identity of the E donor atom does not significantly affect their zfs parameters. High-resolution multifrequency EPR studies of CoO2E2 provided evidence of multiple conformations, which are more clearly observed for CoO2Se2, in agreement with the structural disorder previously established for this complex by X-ray crystallography. The CoO2E2 complexes were shown to be field-induced SIMs, i.e., they exhibit slow relaxation of magnetization in the presence of an external DC magnetic field. Advanced quantum-chemical calculations on CoO2E2 provided additional insight into their electronic and structural properties.

Topological Lifshitz transition and one-dimensional Weyl mode in HfTe5.

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 a one-dimensional Weyl mode with the 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 the 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.

Comprehensive Studies of Magnetic Transitions and Spin-Phonon Couplings in the Tetrahedral Cobalt Complex Co(AsPh3)2I2.

A combination of inelastic neutron scattering (INS), far-IR magneto-spectroscopy (FIRMS), and Raman magneto-spectroscopy (RaMS) has been used to comprehensively probe magnetic excitations in Co(AsPh3)2I2 (1), a reported single-molecule magnet (SMM). With applied field, the magnetic zero-field splitting (ZFS) peak (2D') shifts to higher energies in each spectroscopy. INS placed the ZFS peak at 54 cm-1, as revealed by both variable-temperature (VT) and variable-magnetic-field data, giving results that agree well with those from both far-IR and Raman studies. Both FIRMS and RaMS also reveal the presence of multiple spin-phonon couplings as avoided crossings with neighboring phonons. Here, phonons refer to both intramolecular and lattice vibrations. The results constitute a rare case in which the spin-phonon couplings are observed with both Raman-active (g modes) and far-IR-active phonons (u modes; space group P21/c, no. 14, Z = 4 for 1). These couplings are fit using a simple avoided crossing model with coupling constants of ca. 1-2 cm-1. The combined spectroscopies accurately determine the magnetic excited level and the interaction of the magnetic excitation with phonon modes. Density functional theory (DFT) phonon calculations compare well with INS, allowing for the assignment of the modes and their symmetries. Electronic calculations elucidate the nature of ZFS in the complex. Features of different techniques to determine ZFS and other spin-Hamiltonian parameters in transition-metal complexes are summarized.

Giant g-factors and fully spin-polarized states in metamorphic short-period InAsSb/InSb superlattices.

Realizing a large Landé 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 ≈ 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.

High-Field Magnetoelectric and Spin-Phonon Coupling in Multiferroic (NH4)2[FeCl5·(H2O)].

We combine high field polarization, magneto-infrared spectroscopy, and lattice dynamics calculations with prior magnetization to explore the properties of (NH4)2[FeCl5·(H2O)]─a type II molecular multiferroic in which the mixing between charge, structure, and magnetism is controlled by intermolecular hydrogen and halogen bonds. Electric polarization is sensitive to the series of field-induced spin reorientations, increasing linearly with the field and reaching a maximum before collapsing to zero across the quasi-collinear to collinear-sinusoidal reorientation due to the restoration of inversion symmetry. Magnetoelectric coupling is on the order of 1.2 ps/m for the P∥c, H∥c configuration between 5 and 25 T at 1.5 K. In this range, the coupling takes place via an orbital hybridization mechanism. Other forms of mixing are active in (NH4)2[FeCl5·(H2O)] as well. Magneto-infrared spectroscopy reveals that all of the vibrational modes below 600 cm-1 are sensitive to the field-induced transition to the fully saturated magnetic state at 30 T. We analyze these local lattice distortions and use frequency shifts to extract spin-phonon coupling constants for the Fe-O stretch, Fe-OH2 rock, and NH4+ libration. Inspection also reveals subtle symmetry breaking of the ammonium counterions across the ferroelectric transition. The coexistence of such varied mixing processes in a platform with intermolecular hydrogen- and halogen-bonding opens the door to greater understanding of multiferroics and magnetoelectrics governed by through-space interactions.

Analysis of vibronic coupling in a 4f molecular magnet with FIRMS.

Vibronic coupling, the interaction between molecular vibrations and electronic states, is a fundamental effect that profoundly affects chemical processes. In the case of molecular magnetic materials, vibronic, or spin-phonon, coupling leads to magnetic relaxation, which equates to loss of magnetic memory and loss of phase coherence in molecular magnets and qubits, respectively. The study of vibronic coupling is challenging, and most experimental evidence is indirect. Here we employ far-infrared magnetospectroscopy to directly probe vibronic transitions in [Yb(trensal)] (where H3trensal = 2,2,2-tris(salicylideneimino)trimethylamine). We find intense signals near electronic states, which we show arise due to an "envelope effect" in the vibronic coupling Hamiltonian, which we calculate fully ab initio to simulate the spectra. We subsequently show that vibronic coupling is strongest for vibrational modes that simultaneously distort the first coordination sphere and break the C3 symmetry of the molecule. With this knowledge, vibrational modes could be identified and engineered to shift their energy towards or away from particular electronic states to alter their impact. Hence, these findings provide new insights towards developing general guidelines for the control of vibronic coupling in molecules.

Weyl Fermion magneto-electrodynamics and ultralow field quantum limit in TaAs.

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 limit­the field required to reach the lowest LL­of 0.8 tesla­unprecedentedly low for Weyl Fermions. LL spectroscopy allows us to isolate these Weyl Fermions from all other carriers in TaAs, and our result provides a way for directly exploring the more exotic quantum phenomena in Weyl semimetals, such as the chiral anomaly.