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Exciton polaron is a hypothetical many-body quasiparticle that involves an exciton dressed with a polarized electron-hole cloud in the Fermi sea. It has been evoked to explain the excitonic spectra of charged monolayer transition metal dichalcogenides, but the studies were limited to the ground state. Here we measure the reflection and photoluminescence of monolayer MoSe2 and WSe2 gating devices encapsulated by boron nitride. We observe gate-tunable exciton polarons associated with the 1 s–3 s exciton Rydberg states. The ground and excited exciton polarons exhibit comparable energy redshift (15~30 meV) from their respective bare excitons. The robust excited states contradict the trion picture because the trions are expected to dissociate in the excited states. When the Fermi sea expands, we observe increasingly severe suppression and steep energy shift from low to high exciton-polaron Rydberg states. Their gate-dependent energy shifts go beyond the trion description but match our exciton-polaron theory. Our experiment and theory demonstrate the exciton-polaron nature of both the ground and excited excitonic states in charged monolayer MoSe2 and WSe2. An exciton polaron is a quasiparticle composed of an exciton dressed with an electron-hole cloud, and this concept has been used to explain the ground excitonic states in charged monolayer transition metal dichalcogenides. Here the authors present experimental and theoretical evidence of exciton-polaron Rydberg states in monolayer MoSe2 and WSe2. [ABSTRACT FROM AUTHOR]

Large separation of magnetic levels and slow relaxation in metal complexes are desirable properties of single‐molecule magnets (SMMs). Spin‐phonon coupling (interactions of magnetic levels with phonons) is ubiquitous, leading to magnetic relaxation and loss of memory in SMMs and quantum coherence in qubits. Direct observation of magnetic transitions and spin‐phonon coupling in molecules is challenging. We have found that far‐IR magnetic spectra (FIRMS) of Co(PPh3)2X2 (Co‐X; X=Cl, Br, I) reveal rarely observed spin‐phonon coupling as avoided crossings between magnetic and u‐symmetry phonon transitions. Inelastic neutron scattering (INS) gives phonon spectra. Calculations using VASP and phonopy programs gave phonon symmetries and movies. Magnetic transitions among zero‐field split (ZFS) levels of the S=3/2 electronic ground state were probed by INS, high‐frequency and ‐field EPR (HFEPR), FIRMS, and frequency‐domain FT terahertz EPR (FD‐FT THz‐EPR), giving magnetic excitation spectra and determining ZFS parameters (D, E) and g values. Ligand‐field theory (LFT) was used to analyze earlier electronic absorption spectra and give calculated ZFS parameters matching those from the experiments. DFT calculations also gave spin densities in Co‐X, showing that the larger Co(II) spin density in a molecule, the larger its ZFS magnitude. The current work reveals dynamics of magnetic and phonon excitations in SMMs. Studies of such couplings in the future would help to understand how spin‐phonon coupling may lead to magnetic relaxation and develop guidance to control such coupling. [ABSTRACT FROM AUTHOR]

Metal-organic frameworks based on metal-formates have emerged as a intriguing class of multiferroics with wide range of applications. In this work, we present magneto-Raman spectroscopic investigations on [(CH3)2NH2]Co(HCOO)3 belonging to this family. The spectroscopic studies were performed at magnetic fields up to 31 T at the temperature of 2.3 K. It was observed that the formate bending mode at around 798 cm−1 shifts to higher energies with increasing magnetic field. The magneto-response of the phonon also exhibits anomalies at magnetic fields of 14.5 T and 23.5 T corresponding to magnetic phase transitions. Based on our results, we conclude that the formate bending mode does play a role in facilitating the saturation of magnetic states similar to its Mn and Ni analogs. [ABSTRACT FROM AUTHOR]

Large separations between ground and excited magnetic states in single‐molecule magnets (SMMs) are desirable to reduce the likelihood of spin reversal in the molecules. Spin‐phonon coupling is a process leading to magnetic relaxation. Both the reversal and coupling, making SMMs lose magnetic moments, are undesirable. However, direct determination of large magnetic states separations (>45 cm−1) is challenging, and few detailed investigations of the spin‐phonon coupling have been conducted. The magnetic separation in [Co(12‐crown‐4)2](I3)2(12‐crown‐4) (1) is determined and its spin‐phonon coupling is probed by inelastic neutron scattering (INS) and far‐IR spectroscopy. INS, using oriented single crystals, shows a magnetic transition at 49.4(1.0) cm−1. Far‐IR reveals that the magnetic transition and nearby phonons are coupled, a rarely observed phenomenon, with spin‐phonon coupling constants of 1.7–2.5 cm−1. The current work spectroscopically determines the ground–excited magnetic states separation in an SMM and quantifies its spin‐phonon coupling, shedding light on the process causing magnetic relaxation. [ABSTRACT FROM AUTHOR]

Scanning tunneling spectroscopy (STS) has yielded significant insight into the electronic structure of graphene and other two-dimensional (2D) materials. STS directly measures a fundamental and directly calculable quantity: single particle density of states (SPDOS). Due to experimental setup limitations, however, STS has been unable to explore 2D materials in ultrahigh magnetic fields where electron-electron interactions can drastically change the SPDOS. Recent developments in the assembly of heterostructures composed of graphene and hexagonal boron nitride have enabled a device-based alternative to potentially overcome these roadblocks. Thus far, however, these nascent efforts are incomplete in analyzing and understanding tunneling spectra and have yet to explore graphene at high magnetic fields. Here, we report an experiment at magnetic fields up to 18 T, which uses graphene tunneling field effect transistors (TFETs) to establish a clear benchmark for the measurement and analysis of graphene planar tunneling spectroscopy. We acquire gate tunable tunneling spectra of graphene and then use these data and electrostatic arguments to develop a systematic analysis scheme. This analysis reveals that TFET devices directly probe electronic structure features near and far from the Fermi level. In particular, our study yields identification of the Dirac point and numerous Landau levels as they fill and empty with charge via the application of a gate voltage. Our work demonstrates that TFET devices are a viable platform for directly probing the electronic structure of graphene and other 2D materials in high magnetic fields, where exotic electronic states emerge. [ABSTRACT FROM AUTHOR]

The observation of a previously unreported optoelectronic effect, namely, a light‐induced diode‐like response in multilayered MoSe2 field‐effect transistors is reported. It has a sense of current rectification that is controllable through a gate voltage. It is argued, using numerical simulations, that this behavior results from the difference in the size of the Schottky barriers between the drain and source metal contacts. Each barrier can be modeled as a Schottky diode but with opposite senses of current rectification between them, with the diode response resulting from the light induced promotion of photogenerated carriers across the smaller barrier. The back gate voltage controls the sense of current rectification by modulating the relative amplitude between them. This effect, which gives rise to a novel type of optoelectronic switch, also yields a photovoltaic response. Hence, it can provide an alternative to p–n junctions when harvesting photovoltaic currents from transition metal dichalcogenides. It is argued that the photovoltaic efficiency associated to this effect can be increased by just increasing the relative asymmetry between both Schottky barriers. It is also suggested that this new electro‐optical effect has potential for technological applications. [ABSTRACT FROM AUTHOR]

An amendment to this paper has been published and can be accessed via a link at the top of the paper. [ABSTRACT FROM AUTHOR]

Tungsten-based monolayer transition metal dichalcogenides host a long-lived "dark" exciton, an electron-hole pair in a spin-triplet configuration. The long lifetime and unique spin properties of the dark exciton provide exciting opportunities to explore light-matter interactions beyond electric dipole transitions. Here we demonstrate that the coupling of the dark exciton and an optically silent chiral phonon enables the intrinsic photoluminescence of the dark-exciton replica in monolayer WSe2. Gate and magnetic-field dependent PL measurements unveil a circularly-polarized replica peak located below the dark exciton by 21.6 meV, equal to E″ phonon energy from Se vibrations. First-principles calculations show that the exciton-phonon interaction selectively couples the spin-forbidden dark exciton to the intravalley spin-allowed bright exciton, permitting the simultaneous emission of a chiral phonon and a circularly-polarized photon. Our discovery and understanding of the phonon replica reveals a chirality dictated emission channel of the phonons and photons, unveiling a new route of manipulating valley-spin. The long lifetime and spin properties of dark excitons in atomically thin transition metal dichalcogenides offer opportunities to explore light-matter interactions beyond electric dipole transitions. Here, the authors demonstrate that the coupling of the dark exciton and an optically silent chiral phonon enables the intrinsic photoluminescence of the dark-exciton replica in monolayer WSe2 [ABSTRACT FROM AUTHOR]

Strong Coulomb interactions in single-layer transition metal dichalcogenides (TMDs) result in the emergence of strongly bound excitons, trions, and biexcitons. These excitonic complexes possess the valley degree of freedom, which can be exploited for quantum optoelectronics. However, in contrast to the good understanding of the exciton and trion properties, the binding energy of the biexciton remains elusive, with theoretical calculations and experimental studies reporting discrepant results. In this work, we resolve the conflict by employing low-temperature photoluminescence spectroscopy to identify the biexciton state in BN-encapsulated single-layer WSe2. The biexciton state only exists in charge-neutral WSe2, which is realized through the control of efficient electrostatic gating. In the lightly electron-doped WSe2, one free electron binds to a biexciton and forms the trion-exciton complex. Improved understanding of the biexciton and trion-exciton complexes paves the way for exploiting the many-body physics in TMDs for novel optoelectronics applications. Owing to strong Coulomb interactions, atomically thin transition metal dichalcogenides host strongly bound excitonic complexes. Here, the authors report charge-neutral biexciton and negatively charged trion-exciton complexes in hBN encapsulated monolayer WSe2 by employing low-temperature photoluminescence spectroscopy. [ABSTRACT FROM AUTHOR]

Higher-order correlated excitonic states arise from the mutual interactions of excitons, which generally requires a significant exciton density and therefore high excitation levels. Here, we report the emergence of two biexcitons species, one neutral and one charged, in monolayer tungsten diselenide under moderate continuous-wave excitation. The efficient formation of biexcitons is facilitated by the long lifetime of the dark exciton state associated with a spin-forbidden transition, as well as improved sample quality from encapsulation between hexagonal boron nitride layers. From studies of the polarization and magnetic field dependence of the neutral biexciton, we conclude that this species is composed of a bright and a dark excitons residing in opposite valleys in momentum space. Our observations demonstrate that the distinctive features associated with biexciton states can be accessed at low light intensities and excitation densities. [ABSTRACT FROM AUTHOR]

Strong Coulomb interactions in single-layer transition metal dichalcogenides (TMDs) result in the emergence of strongly bound excitons, trions, and biexcitons. These excitonic complexes possess the valley degree of freedom, which can be exploited for quantum optoelectronics. However, in contrast to the good understanding of the exciton and trion properties, the binding energy of the biexciton remains elusive, with theoretical calculations and experimental studies reporting discrepant results. In this work, we resolve the conflict by employing low-temperature photoluminescence spectroscopy to identify the biexciton state in BN-encapsulated single-layer WSe2. The biexciton state only exists in charge-neutral WSe2, which is realized through the control of efficient electrostatic gating. In the lightly electron-doped WSe2, one free electron binds to a biexciton and forms the trion-exciton complex. Improved understanding of the biexciton and trion-exciton complexes paves the way for exploiting the many-body physics in TMDs for novel optoelectronics applications. [ABSTRACT FROM AUTHOR]

Keywords: electro-optical effect; field-effect transistors; photovoltaic effect; Schottky barriers; Schottky diodes; transition metal-dichalcogenides EN electro-optical effect field-effect transistors photovoltaic effect Schottky barriers Schottky diodes transition metal-dichalcogenides 1 1 1 10/06/21 20151101 NES 151101 In article number 1500215, Nihar R. Pradhan, Luis Balicas, and co-workers demonstrate that the Schottky barriers between metallic interconnects and a van der Waals coupled semiconductor can lead to a light-induced, diode-like response with a sense of current rectification that can be controlled via a back gate voltage. Electro-optical effect, field-effect transistors, photovoltaic effect, Schottky barriers, Schottky diodes, transition metal-dichalcogenides Optoelectronic Switches: An Optoelectronic Switch Based on Intrinsic Dual Schottky Diodes in Ambipolar MoSe2 Field-Effect Transistors (Adv. [Extracted from the article]

The quantum anomalous Hall effect (QAHE) is a robust topological phenomenon that features quantized Hall resistance at zero magnetic field. We report the QAHE in a rhombohedral pentalayer graphene-monolayer tungsten disulfide (WS 2 ) heterostructure. Distinct from other experimentally confirmed QAHE systems, this system has neither magnetic element nor moiré superlattice effect. The QAH states emerge at charge neutrality and feature Chern numbers C = ±5 at temperatures of up to about 1.5 kelvin. This large QAHE arises from the synergy of the electron correlation in intrinsic flat bands of pentalayer graphene, the gate-tuning effect, and the proximity-induced Ising spin-orbit coupling. Our experiment demonstrates the potential of crystalline two-dimensional materials for intertwined electron correlation and band topology physics and may enable a route for engineering chiral Majorana edge states.

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(AsPh 3 ) 2 I 2 ( 1 ), a reported single-molecule magnet (SMM). With applied field, the magnetic zero-field splitting (ZFS) peak (2 D ') 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 P 2 1 / 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.

Correlated-electron systems have long been an important platform for various interesting phenomena and fundamental questions in condensed matter physics. As a pivotal process in these systems, d-d transitions have been suggested as a key factor toward realizing optical spin control in two-dimensional (2D) magnets. However, it remains unclear how d-d excitations behave in quasi-2D systems with strong electronic correlation and spin-charge coupling. Here, we present a systematic electronic Raman spectroscopy investigation on d-d transitions in a 2D antiferromagnet—NiPS 3 , from bulk to atomically thin samples. Two electronic Raman modes originating from the scattering of incident photons with d electrons in Ni 2+ ions are observed at ~1.0 eV. This electronic process persists down to trilayer flakes and exhibits insensitivity to the spin ordering of NiPS 3 . Our study demonstrates the utility of electronic Raman scattering in investigating the unique electronic structure and its coupling to magnetism in correlated 2D magnets.

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 way for directly exploring the more exotic quantum phenomena in Weyl semimetals, such as the chiral anomaly.

Large separation of magnetic levels and slow relaxation in metal complexes are desirable properties of single-molecule magnets (SMMs). Spin-phonon coupling (interactions of magnetic levels with phonons) is ubiquitous, leading to magnetic relaxation and loss of memory in SMMs and quantum coherence in qubits. Direct observation of magnetic transitions and spin-phonon coupling in molecules is challenging. We have found that far-IR magnetic spectra (FIRMS) of Co(PPh 3 ) 2 X 2 (Co-X; X=Cl, Br, I) reveal rarely observed spin-phonon coupling as avoided crossings between magnetic and u-symmetry phonon transitions. Inelastic neutron scattering (INS) gives phonon spectra. Calculations using VASP and phonopy programs gave phonon symmetries and movies. Magnetic transitions among zero-field split (ZFS) levels of the S=3/2 electronic ground state were probed by INS, high-frequency and -field EPR (HFEPR), FIRMS, and frequency-domain FT terahertz EPR (FD-FT THz-EPR), giving magnetic excitation spectra and determining ZFS parameters (D, E) and g values. Ligand-field theory (LFT) was used to analyze earlier electronic absorption spectra and give calculated ZFS parameters matching those from the experiments. DFT calculations also gave spin densities in Co-X, showing that the larger Co(II) spin density in a molecule, the larger its ZFS magnitude. The current work reveals dynamics of magnetic and phonon excitations in SMMs. Studies of such couplings in the future would help to understand how spin-phonon coupling may lead to magnetic relaxation and develop guidance to control such coupling., (© 2021 Wiley-VCH GmbH.)

A strong Coulomb interaction could lead to a strongly bound exciton with high-order excited states, similar to the Rydberg atom. The interaction of giant Rydberg excitons can be engineered for a correlated ordered exciton array with a Rydberg blockade, which is promising for realizing quantum simulation. Monolayer transition metal dichalcogenides, with their greatly enhanced Coulomb interaction, are an ideal platform to host the Rydberg excitons in two dimensions. Here, we employ helicity-resolved magneto-photocurrent spectroscopy to identify Rydberg exciton states up to 11s in monolayer WSe 2 . Notably, the radius of the Rydberg exciton at 11s can be as large as 214 nm, orders of magnitude larger than the 1s exciton. The giant valley-polarized Rydberg exciton not only provides an exciting platform to study the strong exciton-exciton interaction and nonlinear exciton response but also allows the investigation of the different interplay between the Coulomb interaction and Landau quantization, tunable from a low- to high-magnetic-field limit.

We used a combination of polarized Raman spectroscopy and spin wave calculations to study magnetic excitations in the strong spin-orbit-coupled bilayer perovskite antiferromagnet Sr_{3}Ir_{2}O_{7}. We observed two broad Raman features at ∼800 and ∼1400  cm^{-1} arising from magnetic excitations. Unconventionally, the ∼800  cm^{-1} feature is fully symmetric (A_{1g}) with respect to the underlying tetragonal (D_{4h}) crystal lattice which, together with its broad line shape, definitively rules out the possibility of a single magnon excitation as its origin. In contrast, the ∼1400  cm^{-1} feature shows up in both the A_{1g} and B_{2g} channels. From spin wave and two-magnon scattering cross-section calculations of a tetragonal bilayer antiferromagnet, we identified the ∼800  cm^{-1} (1400  cm^{-1}) feature as two-magnon excitations with pairs of magnons from the zone-center Γ point (zone-boundary van Hove singularity X point). We further found that this zone-center two-magnon scattering is unique to bilayer perovskite magnets which host an optical branch in addition to the acoustic branch, as compared to their single layer counterparts. This zone-center two-magnon mode is distinct in symmetry from the time-reversal symmetry broken "spin wave gap" and "phase mode" proposed to explain the ∼92  meV (742  cm^{-1}) gap in resonant inelastic x-ray spectroscopy magnetic excitation spectra of Sr_{3}Ir_{2}O_{7}.