The physics of quantum materials is dictated by many-body interactions and mathematical concepts such as symmetry and topology that have transformed our understanding of matter. Angle-resolved ...photoemission spectroscopy (ARPES), which directly probes the electronic structure in momentum space, has played a central role in the discovery, characterization, and understanding of quantum materials ranging from strongly correlated states of matter to those exhibiting nontrivial topology. Over the past two decades, ARPES as a technique has matured dramatically with ever-improving resolution and continued expansion into the space, time, and spin domains. Simultaneously, the capability to synthesize new materials and apply nonthermal tuning parameters in situ has unlocked new dimensions in the study of all quantum materials. These developments are reviewed, and the scientific contributions they have enabled in contemporary quantum materials research are surveyed.
Strong electron correlation can induce Mott insulating behaviour and produce intriguing states of matter such as unconventional superconductivity and quantum spin liquids. Recent advances in van der ...Waals material synthesis enable the exploration of Mott systems in the two-dimensional limit. Here we report characterization of the local electronic properties of single- and few-layer 1T-TaSe2 via spatial- and momentum-resolved spectroscopy involving scanning tunnelling microscopy and angle-resolved photoemission. Our results indicate that electron correlation induces a robust Mott insulator state in single-layer 1T-TaSe2 that is accompanied by unusual orbital texture. Interlayer coupling weakens the insulating phase, as shown by reduction of the energy gap and quenching of the correlation-driven orbital texture in bilayer and trilayer 1T-TaSe2. This establishes single-layer 1T-TaSe2 as a useful platform for investigating strong correlation physics in two dimensions.The electrons that contribute to the Mott insulator state in single-layer 1T-TaSe2 are shown to also have a rich variation in their orbital occupation. As more layers are added, both the insulating state and orbital texture weaken.
Abstract
Almost a decade has passed since the serendipitous discovery of the iron-based high temperature superconductors (FeSCs) in 2008. The fact that, as in the copper oxide high temperature ...superconductors, long-range antiferromagnetism in the FeSCs arises in proximity to superconductivity immediately raised the question of the degree of similarity between the two. Despite the great resemblance in their phase diagrams, there exist important differences between the FeSCs and the cuprates that need to be considered in order to paint a full picture of these two families of high temperature superconductors. One of the key differences is the multi-orbital multi-band nature of the FeSCs, which contrasts with the effective single-band nature of the cuprates. Systematic studies of orbital related phenomena in FeSCs have been largely lacking. In this review, we summarize angle-resolved photoemission spectroscopy (ARPES) measurements across various FeSC families that have been reported in literature, focusing on the systematic trends of orbital dependent electron correlations and the role of different Fe 3d orbitals in driving the nematic transition, the spin-density-wave transition, and superconductivity.
Quantum emitters are an integral component for a broad range of quantum technologies, including quantum communication, quantum repeaters, and linear optical quantum computation. Solid-state color ...centers are promising candidates for scalable quantum optics due to their long coherence time and small inhomogeneous broadening. However, once excited, color centers often decay through phonon-assisted processes, limiting the efficiency of single-photon generation and photon-mediated entanglement generation. Herein, we demonstrate strong enhancement of spontaneous emission rate of a single silicon-vacancy center in diamond embedded within a monolithic optical cavity, reaching a regime in which the excited-state lifetime is dominated by spontaneous emission into the cavity mode. We observe 10-fold lifetime reduction and 42-fold enhancement in emission intensity when the cavity is tuned into resonance with the optical transition of a single silicon-vacancy center, corresponding to 90% of the excited-state energy decay occurring through spontaneous emission into the cavity mode. We also demonstrate the largest coupling strength (g/2π = 4.9 ± 0.3 GHz) and cooperativity (C = 1.4) to date for color-center-based cavity quantum electrodynamics systems, bringing the system closer to the strong coupling regime.
Magnetic domain walls are boundaries between regions with different configurations of the same magnetic order. In a magnetic insulator, where the magnetic order is tied to its bulk insulating ...property, it has been postulated that electrical properties are drastically different along the domain walls, where the order is inevitably disturbed. Here we report the discovery of highly conductive magnetic domain walls in a magnetic insulator, Nd₂Ir₂O₇, that has an unusual all-in-all-out magnetic order, via transport and spatially resolved microwave impedance microscopy. The domain walls have a virtually temperature-independent sheet resistance of ∼1 kilohm per square, show smooth morphology with no preferred orientation, are free from pinning by disorders, and have strong thermal and magnetic field responses that agree with expectations for all-in-all-out magnetic order.
High quality WSe2 films have been grown on bilayer graphene (BLG) with layer-by-layer control of thickness using molecular beam epitaxy. The combination of angle-resolved photoemission, scanning ...tunneling microscopy/spectroscopy, and optical absorption measurements reveal the atomic and electronic structures evolution and optical response of WSe2/BLG. We observe that a bilayer of WSe2 is a direct bandgap semiconductor, when integrated in a BLG-based heterostructure, thus shifting the direct–indirect band gap crossover to trilayer WSe2. In the monolayer limit, WSe2 shows a spin-splitting of 475 meV in the valence band at the K point, the largest value observed among all the MX2 (M = Mo, W; X = S, Se) materials. The exciton binding energy of monolayer-WSe2/BLG is found to be 0.21 eV, a value that is orders of magnitude larger than that of conventional three-dimensional semiconductors, yet small as compared to other two-dimensional transition metal dichalcogennides (TMDCs) semiconductors. Finally, our finding regarding the overall modification of the electronic structure by an alkali metal surface electron doping opens a route to further control the electronic properties of TMDCs.
To date, effective control over the electrochemical reduction of CO2 to multicarbon products (C ≥ 2) has been very challenging. Here, we report a design principle for the creation of a selective yet ...robust catalytic interface for heterogeneous electrocatalysts in the reduction of CO2 to C2 oxygenates, demonstrated by rational tuning of an assembly of nitrogen-doped nanodiamonds and copper nanoparticles. The catalyst exhibits a Faradaic efficiency of ~63% towards C2 oxygenates at applied potentials of only −0.5 V versus reversible hydrogen electrode. Moreover, this catalyst shows an unprecedented persistent catalytic performance up to 120 h, with steady current and only 19% activity decay. Density functional theory calculations show that CO binding is strengthened at the copper/nanodiamond interface, suppressing CO desorption and promoting C2 production by lowering the apparent barrier for CO dimerization. The inherent compositional and electronic tunability of the catalyst assembly offers an unrivalled degree of control over the catalytic interface, and thereby the reaction energetics and kinetics.The interfacing of Cu with nitrogen-doped nanodiamond enables the electrocatalytic production of C2 oxygenates from CO2 with promising stability.
Two-dimensional (2D) transition metal dichalcogenides (TMDs) are emerging as a new platform for exploring 2D semiconductor physics. Reduced screening in two dimensions results in markedly enhanced ...electron-electron interactions, which have been predicted to generate giant bandgap renormalization and excitonic effects. Here we present a rigorous experimental observation of extraordinarily large exciton binding energy in a 2D semiconducting TMD. We determine the single-particle electronic bandgap of single-layer MoSe2 by means of scanning tunnelling spectroscopy (STS), as well as the two-particle exciton transition energy using photoluminescence (PL) spectroscopy. These yield an exciton binding energy of 0.55 eV for monolayer MoSe2 on graphene—orders of magnitude larger than what is seen in conventional 3D semiconductors and significantly higher than what we see for MoSe2 monolayers in more highly screening environments. This finding is corroborated by our ab initio GW and Bethe-Salpeter equation calculations which include electron correlation effects. The renormalized bandgap and large exciton binding observed here will have a profound impact on electronic and optoelectronic device technologies based on single-layer semiconducting TMDs.
In normal metals, macroscopic properties are understood using the concept of quasiparticles. In the cuprate high-temperature superconductors, the metallic state above the highest transition ...temperature is anomalous and is known as the "strange metal." We studied this state using angle-resolved photoemission spectroscopy. With increasing doping across a temperature-independent critical value
~ 0.19, we observed that near the Brillouin zone boundary, the strange metal, characterized by an incoherent spectral function, abruptly reconstructs into a more conventional metal with quasiparticles. Above the temperature of superconducting fluctuations, we found that the pseudogap also discontinuously collapses at the very same value of
These observations suggest that the incoherent strange metal is a distinct state and a prerequisite for the pseudogap; such findings are incompatible with existing pseudogap quantum critical point scenarios.
Establishing a minimal microscopic model for cuprates is a key step towards the elucidation of a high- Tc mechanism. By a quantitative comparison with a recent in situ angle-resolved photoemission ...spectroscopy measurement in doped 1D cuprate chains, our simulation identifies a crucial contribution from long-range electron-phonon coupling beyond standard Hubbard models. Using reasonable ranges of coupling strengths and phonon energies, we obtain a strong attractive interaction between neighboring electrons, whose strength is comparable to experimental observations. Nonlocal couplings play a significant role in the mediation of neighboring interactions. Considering the structural and chemical similarity between 1D and 2D cuprate materials, this minimal model with long-range electron-phonon coupling will provide important new insights on cuprate high- Tc superconductivity and related quantum phases.
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