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2D materials have intriguing quantum phenomena that are distinctively different from their bulk counterparts. Recently, epitaxially synthesized wafer-scale 2D metals, composed of elemental atoms, are attracting attention not only for their potential applications but also for exotic quantum effects such as superconductivity. By mapping momentum-resolved electronic states using time-resolved and angle-resolved photoemission spectroscopy (ARPES), we reveal that monolayer Ag confined between bilayer graphene and SiC is a large gap (> 1 eV) 2D semiconductor, consistent with GW-corrected density functional theory. The measured valence band dispersion matches the DFT-GW quasiparticle band. However, the conduction band dispersion shows an anomalously large effective mass of 2.4 m0. Possible mechanisms for this large enhancement in the apparent mass are discussed.

Semiconductor moiré superlattices represent a rapidly developing area of engineered photonic materials and a new platform to explore correlated electron states and quantum simulation. In this Review, we briefly introduce early experiments that identified new exciton resonances in transition metal dichalcogenide heterobilayers and discuss several topics including two types of transition metal dichalcogenide moiré superlattice, new optical selection rules, early evidence of moiré excitons, and how the resonant energy, dynamics and diffusion properties of moiré excitons can be controlled via the twist angle. To interpret optical spectra, it is important to measure the energy modulation within a moiré supercell. In this context, we describe a few scanning tunnelling microscopy experiments that measure the moiré potential landscape directly. Finally, we review a few recent experiments that applied excitonic optical spectroscopy to probe correlated electron phenomena in transition metal dichalcogenide moiré superlattices.

Tailoring interlayer coupling has emerged as a powerful tool to tune the electronic structure of van der Waals (vdW) bilayers. One example is the usage of the moire pattern to create controllable two-dimensional electronic superlattices through the configurational dependence of interlayer electronic couplings. This approach has led to some remarkable discoveries in twisted graphene bilayers, and transition metal dichalcogenide (TMD) homo- and hetero-bilayers. However, a largely unexplored factor is the interlayer distance, d, which can impact the interlayer coupling strength exponentially. In this letter, we quantitatively determine the coupling strengths as a function of interlayer spacing at various critical points of the Brillouin zone in bilayer MoS2. The exponential dependence of the coupling parameter on the gap distance is demonstrated. Most significantly, we achieved a 280% enhancement of K-valley coupling strength with an 8% reduction of the vdW gap, pointing to a new strategy in designing a novel electronic system in vdW bilayers.

The electronic structure and dynamics of 2D transition metal dichalcogenide (TMD) monolayers provide important underpinnings both for understanding the many-body physics of electronic quasi-particles and for applications in advanced optoelectronic devices. However, extensive experimental investigations of semiconducting monolayer TMDs have yielded inconsistent results for a key parameter, the quasi-particle band gap (QBG), even for measurements carried out on the same layer and substrate combination. Here, we employ sensitive time- and angle-resolved photoelectron spectroscopy (trARPES) for a high-quality large-area MoS2 monolayer to capture its momentum-resolved equilibrium and excited-state electronic structure in the weak-excitation limit. For monolayer MoS2 on graphite, we obtain QBG values of ≈2.10 eV at 80 K and of ≈2.03 eV at 300 K, results well-corroborated by the scanning tunneling spectroscopy (STS) measurements on the same material.

Optical excitation serves as a powerful approach to control the electronic structure of layered Van der Waals materials via many-body screening effects, induced by photoexcited free carriers, or via light-driven coherence, such as optical Stark and Bloch-Siegert effects. Although theoretical work has also pointed to an exotic mechanism of renormalizing band structure via excitonic correlations in bound electron-hole pairs (excitons), experimental observation of such exciton-driven band renormalization and the full extent of their implications is still lacking, largely due to the limitations of optical probes and the impact of screening effects. Here, by using extreme-ultraviolet time-resolved angle-resolved photoemission spectroscopy together with excitonic many-body theoretical calculations, we directly unmask the band renormalization effects driven by excitonic correlations in a monolayer semiconductor. We revealed a surprising bandgap opening, increased by 40 meV, and a simultaneous enhancement of band effective mass. Our findings unmask the novel exciton-driven mechanism towards the band engineering in photoexcited semiconducting materials, opening a new playground to manipulate the transient energy states in layered quantum materials via optical controls of excitonic many-body correlations.

In moir\'e crystals formed by stacking van der Waals (vdW) materials, surprisingly diverse correlated electronic phases and optical properties can be realized by a subtle change in the twist angle. Here, we discover that phonon spectra are also renormalized in MoS$_2$ twisted bilayers, adding a new perspective to moir\'e physics. Over a range of small twist angles, the phonon spectra evolve rapidly due to ultra-strong coupling between different phonon modes and atomic reconstructions of the moir\'e pattern. We develop a new low-energy continuum model for phonons that overcomes the outstanding challenge of calculating properties of large moir\'e supercells and successfully captures essential experimental observations. Remarkably, simple optical spectroscopy experiments can provide information on strain and lattice distortions in moir\'e crystals with nanometer-size supercells. The newly developed theory promotes a comprehensive and unified understanding of structural, optical, and electronic properties of moir\'e superlattices., Comment: 21 pages, 4 figures

We present a strong coupling system realized by coupling the localized surface plasmon mode in individual silver nanogrooves and propagating surface plasmon modes launched by periodic nanogroove arrays with varied periodicities on a continuous silver medium. When the propagating modes are in resonance with the localized mode, we observe a √N scaling of Rabi splitting energy, where N is the number of propagating modes coupled to the localized mode. Here, we confirm a giant Rabi splitting on the order of 450-660 meV (N = 2) in the visible spectral range, and the corresponding coupling strength is 160-235 meV. In some of the strong coupling cases studied by us, the coupling strength is about 10% of the mode energy, reaching the ultrastrong coupling regime.

Aluminum has attracted a great deal of attention as an alternative plasmonic material to silver and gold because of its natural abundance on Earth, material stability, unique spectral capability in the ultraviolet spectral region, and complementary metal-oxide-semiconductor compatibility. Surprisingly, in some recent studies, aluminum has been reported to outperform silver in the visible range due to its superior surface and interface properties. Here, we demonstrate excellent structural and optical properties measured for aluminum epitaxial films grown on sapphire substrates by molecular-beam epitaxy under ultrahigh vacuum growth conditions. Using the epitaxial growth technique, distinct advantages can be achieved for plasmonic applications, including high-fidelity nanofabrication and wafer-scale system integration. Moreover, the aluminum film thickness is controllable down to a few atomic monolayers, allowing for plasmonic ultrathin layer devices. Two kinds of aluminum plasmonic applications are reported here, including precisely engineered plasmonic substrates for surface-enhanced Raman spectroscopy and high-quality-factor plasmonic surface lattices based on standing localized surface plasmons and propagating surface plasmon polaritons, respectively, in the entire visible spectrum (400–700 nm).

In intrinsic magnetic topological insulators, Dirac surface state gaps are prerequisites for quantum anomalous Hall and axion insulating states. Unambiguous experimental identification of these gaps has proved to be a challenge, however. Here we use molecular beam epitaxy to grow intrinsic MnBi2Te4 thin films. Using scanning tunneling microscopy/spectroscopy, we directly visualize the Dirac mass gap and its disappearance below and above the magnetic order temperature. We further reveal the interplay of Dirac mass gaps and local magnetic defects. We find that in high defect regions, the Dirac mass gap collapses. Ab initio and coupled Dirac cone model calculations provide insight into the microscopic origin of the correlation between defect density and spatial gap variations. This work provides unambiguous identification of the Dirac mass gap in MnBi2Te4, and by revealing the microscopic origin of its gap variation, establishes a material design principle for realizing exotic states in intrinsic magnetic topological insulators., Comment: Main and SI

We report an ultrafast increase of the quasi-particle bandgap and effective mass in photoexcited monolayer MoS2 on HOPG, utilizing extreme-ultraviolet time- and angle-resolved photoemission spectroscopy (XUV-trARPES). Combined with theoretical models, we attribute these compelling band renormalizations to the excitonic effects from bound electron-hole pairs.

By using extreme-ultraviolet time- and angle-resolved photoemission spectroscopy (XUV-trARPES), we visualized the photoemission signature and ultrafast inter-state transitions for the electron-hole plasma and exciton states in monolayer MoS2 with full visions of energy and momentum.

The hybridization of magnetism and superconductivity has been an intriguing playground for correlated electron systems, hosting various novel physical phenomena. Usually, localized d- or f-electrons are central to magnetism. In this study, by placing a PTCDA (3,4,9,10-perylene tetracarboxylic dianhydride) molecular monolayer on ultra-thin Pb films, we built a hybrid magnetism/superconductivity (M/SC) system consisting of only sp electronic levels. The magnetic moments reside in the unpaired molecular orbital originating from interfacial charge-transfers. We reported distinctive tunneling spectroscopic features of such a Kondo screened pi-electron impurity lattice on a superconductor in the regime of TK>>delta suggesting the formation of a two-dimensional bound states band. Moreover, moir\'e superlattices with tunable twist angle and the quantum confinement in the ultra-thin Pb films provide easy and flexible implementations to tune the interplay between the Kondo physics and the superconductivity, which are rarely present in M/SC hybrid systems., Comment: 4 figures

The electronic structure and dynamics of 2D transition metal dichalcogenide (TMD) monolayers provide important underpinnings both for understanding the many-body physics of electronic quasi-particles and for applications in advanced optoelectronic devices. However, extensive experimental investigations of semiconducting monolayer TMDs have yielded inconsistent results for a key parameter, the quasi-particle band gap (QBG), even for measurements carried out on the same layer and substrate combination. Here, we employ sensitive time- and angle-resolved photoelectron spectroscopy (trARPES) for a high-quality large-area MoS

One of the most important challenges in the field of topological insulators (TI) is to find materials with nontrivial topological surface state (TSS) while keeping the bulk intrinsic (insulating). In this letter, we report microscopic investigations of BiSbTeSe 2 (1112) and Bi 2 Te 2 Se (221) alloys which have been proposed as candidates to achieve an intrinsic bulk. Scanning tunneling microscopy (STM) confirms previous macroscopic experiments that 221 is an ordered alloy with a Te-Bi-Se-Bi-Te sequence. Nevertheless, it also reveals that the ordering is not perfect with the surface chalcogen layer containing 85% Te and 15% Se. On the other hand, STM shows that 1112 is a random alloy with a fine mixture of (Bi, Sb) in the pnictogen layers and (Te, Se) in the top/bottom chalcogen layers. A freshly cleaved 221 sample surface shows an intrinsic bulk with the Fermi energy, E F , in the gap, but quickly becomes n-type with aging, similar to the aging effect reported by others [27,32]. By contrast, the random alloy 1112 show remarkable robustness against aging and the E F remains within the gap even after aging for 7 days. We attribute this result to the nanoscale fine mixture of the random alloy which provides an effective doping compensation in very fine length scale, thus enabling its bulk to remain intrinsic against aging.

Excitons in monolayer transition metal dichalcogenides are formed at K and K′ points at the boundary of the Brillouin zone. They acquire a valley degree of freedom, which has been explored as an alternative information carrier, analogous to charge or spin. Two opposite valleys in transition metal dichalcogenides can be optically addressed using light with different helicity. Here, we demonstrate that valley-polarized excitons can be sorted and spatially separated at room temperature by coupling a MoS2 monolayer to a subwavelength asymmetric groove array. In addition to separation of valley excitons in real space, emission from valley excitons is also separated in photon momentum-space; that is, the helicity of photons determines a preferential emission direction. Our work demonstrates that metasurfaces can facilitate valley transport and establish an interface between valleytronic and photonic devices, thus addressing outstanding challenges in the field of valleytronics. Helicity of photons is exploited for preferential emission direction and sorting of valley-polarized excitons is achieved at room temperature.

Single crystalline Ag films on dielectric substrates have received tremendous attention recently due to their technological potentials as low loss plasmonic materials. Two different growth approaches have been used to produce single crystalline Ag films previously. One approach is based on repetitive cycles of a two-step process (low temperature deposition followed by RT annealing) using molecular beam epitaxy (MBE), which is extremely time-consuming due to the need for repeat growth cycles. Another approach is based on rapid e-beam deposition which is capable of growing thick single crystalline Ag films (300 nm) but lacks the precision in thickness control of thin epitaxial films. Here, we report a universal approach to grow atomically smooth epitaxial Ag films by eliminating the repetitive cycles used in the previous two-step MBE method while maintaining the precise thickness control from a few monolayers to the optically thick regime, thus overcoming the limitations of the two aforementioned methods. In addition, we develop an in situ growth of aluminum oxide as the capping layer to protect the epitaxial Ag films. The quality of the epitaxial Ag films was evaluated using a variety of techniques, and the superior optical performance of the films is demonstrated by measuring the propagation length of surface plasmon polaritons (∼80 μm at 632 nm) as well as their capability to support a plasmonic nanolaser in infrared incorporating an InGaAsP quantum well as the gain media.

Non-Hermitian photonic systems with gains and/or losses have recently emerged as a powerful approach for topology-protected optical transport and novel device applications. To date, most of these systems employ coupled optical systems of diffraction-limited dielectric waveguides or microcavities, which exchange energy spatially or temporally. Here, we introduce a diffraction-unlimited approach using a plasmon-exciton coupling (polariton) system with tunable plasmonic resonance (energy and line width) and coupling strength. By designing a chirped silver nanogroove cavity array and coupling a single tungsten disulfide monolayer with a large contrast in resonance line width, we show the tuning capability through energy level anticrossing and plasmon-exciton hybridization (line width crossover), as well as spontaneous symmetry breaking across the exceptional point at zero detuning. This two-dimensional hybrid material system can be applied as a scalable and integratable platform for non-Hermitian photonics, featuring seamless integration of two-dimensional materials, broadband tuning, and operation at room temperature.

Using Indium $\sqrt{7}\ifmmode\times\else\texttimes\fi{}\sqrt{3}$ on Si(111) as an atomically thin superconductor platform, and by systematically controlling the density of nanohole defects (nanometer size voids), we reveal the impacts of defect density and defect geometric arrangements on superconductivity at macroscopic and microscopic length scales. When nanohole defects are uniformly dispersed in the atomic layer, the superfluid density monotonically decreases as a function of defect density (from 0.7% to 5% of the surface area) with minor change in the transition temperature ${T}_{C}$, measured both microscopically and macroscopically. With a slight increase in the defect density from 5% to 6%, these point defects are organized into defect chains that enclose individual two-dimensional patches. This new geometric arrangement of defects dramatically impacts the superconductivity, leading to the total disappearance of macroscopic superfluid density and the collapse of the microscopic superconducting gap. This study sheds new light on the understanding of how local defects and their geometric arrangements impact superconductivity in the two-dimensional limit.

Description, 1T-NbSe2 is a correlated insulator with localized magnetic moments exhibiting Kondo resonances when exchange-coupled to 2H-NbSe2., Monolayer group V transition metal dichalcogenides in their 1T phase have recently emerged as a platform to investigate rich phases of matter, such as spin liquid and ferromagnetism, resulting from strong electron correlations. Newly emerging 1T-NbSe2 has inspired theoretical investigations predicting collective phenomena such as charge transfer gap and ferromagnetism in two dimensions; however, the experimental evidence is still lacking. Here, by controlling the molecular beam epitaxy growth parameters, we demonstrate the successful growth of high-quality single-phase 1T-NbSe2. By combining scanning tunneling microscopy/spectroscopy and ab initio calculations, we show that this system is a charge transfer insulator with the upper Hubbard band located above the valence band maximum. To demonstrate the electron correlation resulted magnetic property, we create a vertical 1T/2H NbSe2 heterostructure, and we find unambiguous evidence of exchange interactions between the localized magnetic moments in 1T phase and the metallic/superconducting phase exemplified by Kondo resonances and Yu-Shiba-Rusinov–like bound states.

It has been well established that the presence of quantum-well states in metal thin films plays an essential role in determining the thickness dependence of many physical properties. Oscillatory features in these properties are often observed and attributed to the energy variations of these quantum-well states near the Fermi level. Modern film growth capability has made it possible to create composite metal thin films in which one metal thin film is stacked on top of a dissimilar one with precise control of individual thickness. How the original quantum-well states evolve in the composite film becomes a critical issue in understanding the electronic structure of these new complex thin-film systems. In this paper we present first-principles calculations and measurements by angle-resolved photoemission spectroscopy for electronic states in a bimetallic film composed of ten layers of Pb and nine layers of Ag in the [111] direction on a Si substrate. It is found that the original quantum-well states in individual Pb and Ag films evolve into a new set of states in the bimetallic film by extending into the additional space, instead of directly coupling with each other as one would have expected. The new set of quantum-well states therefore has modified effective masses and energy values compared with the parent ones. Even though the Pb/Ag interface is incommensurate, the coherently coupled electronic states across the whole bimetallic film are verified by supercell configurations with different rotational arrangements in the calculation. The excellent agreement between theory and experiment in the energy dispersion of the quantum-well states in this bimetallic film confirms the physical picture proposed in this work, which could form the basis for exploring the electronic structure in multiple stacked thin films with more complicated designs.

In moiré crystals formed by stacking van der Waals materials, surprisingly diverse correlated electronic phases and optical properties can be realized by a subtle change in the twist angle. Here, we discover that phonon spectra are also renormalized in MoS

The optoelectronic properties of atomically thin transition-metal dichalcogenides are strongly correlated with the presence of defects in the materials, which are not necessarily detrimental for certain applications. For instance, defects can lead to an enhanced photoconduction, a complicated process involving charge generation and recombination in the time domain and carrier transport in the spatial domain. Here, we report the simultaneous spatial and temporal photoconductivity imaging in two types of WS2 monolayers by laser-illuminated microwave impedance microscopy. The diffusion length and carrier lifetime were directly extracted from the spatial profile and temporal relaxation of microwave signals respectively. Time-resolved experiments indicate that the critical process for photo-excited carriers is the escape of holes from trap states, which prolongs the apparent lifetime of mobile electrons in the conduction band. As a result, counterintuitively, the photoconductivity is stronger in CVD samples than exfoliated monolayers with a lower defect density. Our work reveals the intrinsic time and length scales of electrical response to photo-excitation in van der Waals materials, which is essential for their applications in novel optoelectronic devices., 21 pages, 4 figures

The emergence of two-dimensional (2D) materials launched a fascinating frontier of flatland electronics. Most crystalline atomic layer materials are based on layered van der Waals materials with weak interlayer bonding, which naturally leads to thermodynamically stable monolayers. We report the synthesis of a 2D insulator comprised of a single atomic sheet of honeycomb structure BeO (h-BeO), although its bulk counterpart has a wurtzite structure. The h-BeO is grown by molecular beam epitaxy (MBE) on Ag(111) thin films that are conveniently grown on Si(111) wafers. Using scanning tunneling microscopy and spectroscopy (STM/S), the honeycomb BeO lattice constant is determined to be 2.65 angstrom with an insulating band gap of 6 eV. Our low energy electron diffraction (LEED) measurements indicate that the h-BeO forms a continuous layer with good crystallinity at the millimeter scale. Moir\'e pattern analysis shows the BeO honeycomb structure maintains long range phase coherence in atomic registry even across Ag steps. We find that the interaction between the h-BeO layer and the Ag(111) substrate is weak by using STS and complimentary density functional theory calculations. We not only demonstrate the feasibility of growing h-BeO monolayers by MBE, but also illustrate that the large-scale growth, weak substrate interactions, and long-range crystallinity make h-BeO an attractive candidate for future technological applications. More significantly, the ability to create a stable single crystalline atomic sheet without a bulk layered counterpart is an intriguing approach to tailoring novel 2D electronic materials., Comment: 25 pages, 7 figures, submitted to ACS Nano, equal contribution by Hui Zhang and Madisen Holbrook

The emergence of transition metal dichalcogenides (TMD) as crystalline atomically thin semiconductors has created a tremendous amount of scientific and technological interest. Many novel device concepts have been proposed and realized (1-3). Nonetheless, progress in k-space investigations of ground/excited state electronic structures has been slow due to the challenge to create large scale, laterally homogeneous samples. Taking advantage of recent advancements in chemical vapor deposition, here we create a wafer-size MoS2 monolayer with well-aligned lateral orientation for advanced electron spectroscopy studies (4-6). Low energy electron diffraction and scanning tunneling microscopy (STM) demonstrate atomically clean surfaces with in-plane crystalline orientation. The ground state and excited state electronic structures are probed using scanning tunneling spectroscopy (STS), angle-resolved photoemission (ARPES) and time-resolved (tr-)ARPES. In addition to mapping out the momentum-space quasiparticle band structure in the valence and conduction bands, we unveil ultrafast excited state dynamics, including inter- and intra-valley carrier scattering and a rapid downward energy shift by ~ 0.2eV lower than the initial free carrier state at Sigma point.

Interlayer exciton diffusion in transition metal dichalcogenide heterostructures is controlled by the moiré potential., The properties of van der Waals heterostructures are drastically altered by a tunable moiré superlattice arising from periodically varying atomic alignment between the layers. Exciton diffusion represents an important channel of energy transport in transition metal dichalcogenides (TMDs). While early studies performed on TMD heterobilayers suggested that carriers and excitons exhibit long diffusion, a rich variety of scenarios can exist. In a moiré crystal with a large supercell and deep potential, interlayer excitons may be completely localized. As the moiré period reduces at a larger twist angle, excitons can tunnel between supercells and diffuse over a longer lifetime. The diffusion should be the longest in commensurate heterostructures where the moiré superlattice is completely absent. Here, we experimentally demonstrate the rich phenomena of interlayer exciton diffusion in WSe2/MoSe2 heterostructures by comparing several samples prepared with chemical vapor deposition and mechanical stacking with accurately controlled twist angles.

We report the layer-hybridized valley excitons in 2D hetero- and homobilayers manifested by band alignment and valley spin., Excitons in monolayer semiconductors have a large optical transition dipole for strong coupling with light. Interlayer excitons in heterobilayers feature a large electric dipole that enables strong coupling with an electric field and exciton-exciton interaction at the cost of a small optical dipole. We demonstrate the ability to create a new class of excitons in hetero- and homobilayers that combines advantages of monolayer and interlayer excitons, i.e., featuring both large optical and electric dipoles. These excitons consist of an electron confined in an individual layer, and a hole extended in both layers, where the carrier-species–dependent layer hybridization can be controlled through rotational, translational, band offset, and valley-spin degrees of freedom. We observe different species of layer-hybridized valley excitons, which can be used for realizing strongly interacting polaritonic gases and optical quantum controls of bidirectional interlayer carrier transfer.

Quantum dots (QDs) are steadily being implemented as down-conversion phosphors in market-ready display products to enhance color rendering, brightness, and energy efficiency. However, for adequate longevity, QDs must be encased in a protective barrier that separates them from ambient oxygen and humidity, and device architectures are designed to avoid significant heating of the QDs as well as direct contact between the QDs and the excitation source. In order to increase the utility of QDs in display technologies and to extend their usefulness to more demanding applications as, for example, alternative phosphors for solid-state lighting (SSL), QDs must retain their photoluminescence emission properties over extended periods of time under conditions of high temperature and high light flux. Doing so would simplify the fabrication costs for QD display technologies and enable QDs to be used as down-conversion materials in light-emitting diodes for SSL, where direct-on-chip configurations expose the emitters to temperatures approaching 100 °C and to photon fluxes from 0.1 W/mm

We have investigated how the photoluminescence (PL) of WSe2 is modified when coupled to Ag plasmonic structures at low temperature. Chemical vapor deposition (CVD) grown monolayer WSe2 flakes were transferred onto a Ag film and a Ag nanotriangle array that had a 1.5 nm Al2O3 capping layer. Using low-temperature (7.5 K) micro-PL mapping, we simultaneously observed enhancement of the defect-bound exciton emission and quenching of the band edge exciton emission when the WSe2 was on a plasmonic structure. The enhancement of the defect-bound exciton emission was significant with enhancement factors of up to ∼200 for WSe2 on the nanotriangle array when compared to WSe2 on a 1.5 nm Al2O3 capped Si substrate with a 300 nm SiO2 layer. The giant enhancement of the luminescence from the defect-bound excitons is understood in terms of the Purcell effect and increased light absorption. In contrast, the surprising result of luminescence quenching of the bright exciton state on the same plasmonic nanostructure is due to...

We report on the first demonstration of metal–insulator–semiconductor-type plasmonic lasers at the telecom wavelength (∼1.3 μm) using top-down fabricated semiconductor waveguides on single-crystalline metallic platforms formed using epitaxially grown Ag films. The critical role of the Ag film thickness in sustaining plasmonic lasing at the telecom wavelength is investigated systematically. Low-threshold (0.2 MW/cm2) and continuous-wave operation of plasmonic lasing at cryogenic temperatures can be achieved on a 150 nm Ag platform with minimum radiation leakage into the substrate. Plasmonic lasing occurs preferentially through higher-order surface-plasmon-polariton modes, which exhibit a higher mode confinement factor, lower propagation loss, and better field–gain coupling. We observed plasmonic lasing up to ∼200 K under pulsed excitations. The plasmonic lasers on large-area epitaxial Ag films open up a scalable platform for on-chip integrations of plasmonics and optoelectronics at the telecom wavelength.

Monolayer transition metal dichalcogenides (TMDCs), due to their structural similarity to graphene, emerge as a promising alternative material of integrated optoelectronic devices. Recently, intense research efforts have been devoted to the combination of atomically thin TMDCs with metallic nanostructures to enhance the light–matter interaction in TMDCs. One crucial parameter for semiconductor–metallic nanostructure hybrids is the spacer thickness between the gain media and the plasmonic resonator, which needs to be optimized to balance radiation enhancement and radiation quenching. In current investigations of TMDCs–plamonic coupling, one often adopts a spacer thickness of ∼5 nm or larger, a typical value for transitional gain media–plasmonic composites. However, it is unclear whether this typical spacer thickness represents the optimal value for TMDCs–plasmonic hybrids. Here we address this critical issue by studying the spacer thickness dependence of the luminescent efficiency in the monolayer tungsten...

Realization of half-metallicity with a sizable minority-spin gap and ferromagnetic ordering has been a central research emphasis in the development of next-generation spintronic devices. To date, only three-dimensional half-metals have been achieved experimentally, while their counterparts based on two-dimensional (2D) materials remain to be materialized despite extensive efforts based on various predictive designs. This standing challenge is largely due to stringent requirements to establish ferromagnetic order in low-dimensional systems. Here we use first-principles approaches to show that atomically thin zigzag tungsten dichalcogenide $\mathrm{W}{X}_{2}$ ($X=\mathrm{S}$, Se) nanoribbons preserving the stoichiometry of $\mathrm{W}:X=1:2$ stand as highly appealing intrinsic half-metallic systems, without invoking the prevailing approaches of applying an external electric field, chemical modification, or carrier doping. The readily accessible half-metallicity is attributed to distinctly different edge reconstructions, insulating along the X-terminated edges and metallic along the self-passivated W-terminated edges; the latter are further characterized by a robust spin-polarized electron transmission channel. These findings are expected to provide indispensable elemental building blocks for spintronic applications purely based on 2D materials.

We report results of terahertz Faraday and Kerr rotation spectroscopy measurements on thin films of ${\text{Bi}}_{1\ensuremath{-}x}{\text{Sb}}_{x}$, an alloy system that exhibits a semimetal-to-topological-insulator transition as the Sb composition $x$ increases. By using a single-shot time-domain terahertz spectroscopy setup combined with a table-top pulsed minicoil magnet, we conducted measurements in magnetic fields up to 30 T, observing distinctly different behaviors between semimetallic ($xl0.07$) and topological insulator ($xg0.07$) samples. Faraday and Kerr rotation spectra for the semimetallic films showed a pronounced dip that blueshifted with the magnetic field, whereas spectra for the topological insulator films were positive and featureless, increasing in amplitude with increasing magnetic field and eventually saturating at high fields ($g20$ T). Ellipticity spectra for the semimetallic films showed resonances, whereas the topological insulator films showed no detectable ellipticity. To explain these observations, we developed a theoretical model based on realistic band parameters and the Kubo formula for calculating the optical conductivity of Landau-quantized charge carriers. Our calculations quantitatively reproduced all experimental features, establishing that the Faraday and Kerr signals in the semimetallic films predominantly arise from bulk hole cyclotron resonances while the signals in the topological insulator films represent combined effects of surface carriers originating from multiple electron and hole pockets. These results demonstrate that the use of high magnetic fields in terahertz magnetopolarimetry, combined with detailed electronic structure and conductivity calculations, allows us to unambiguously identify and quantitatively determine unique contributions from different species of carriers of topological and nontopological nature in ${\mathrm{Bi}}_{1\ensuremath{-}x}{\mathrm{Sb}}_{x}$.

The superconducting proximity effect is a long-standing topic of great importance in condensed matter physics. A crucial but unresolved issue is which interfacial and material details determine the efficiency of the proximity effect. In this paper, we study an epitaxially grown superconductor/normal metal (SC-NM) heterostructure (Pb/Ag) and find a spatially constant superconducting gap determined by local tunneling spectroscopy and magnetoresponse measurements, despite the highly mismatched Fermi surfaces between individual Pb and Ag epitaxial layers and the large differences in the lattice constants and electronic densities of states in the separate components. The uniform superconducting gap is in contrast to the spatially varying pair potential with a discontinuity at the interface theoretically predicted for an ideal SC-NM junction and experimentally observed previously in several lateral SC-NM junctions. We experimentally verify that the transmission of electrons across the interface in the vertical Pb/Ag heterostructure is high enough that a new band structure emerges even at the single-particle level. Our experimental results call for further theoretical work in order to develop predictive power for the proximity effect starting from realistic, materially relevant microscopic models.

Defect engineering is a key approach for tailoring the properties of the emerging two-dimensional semiconductors. Here, we report an atomic engineering of the W vacancy in monolayer WSe2 by single potassium atom decoration. The K decoration alters the energy states and reshapes the wave function such that previously hidden midgap states become visible with well-resolved multiplets in scanning tunneling spectroscopy. Their energy levels are in good agreement with first-principle calculations. More interestingly, the calculations show that an unpaired electron donated by the K atom can lead to a local magnetic moment, exhibiting an on-off switching by the odd-even number of electron filling. Experimentally the Fermi level is pinned above all defect states due to the graphite substrate, corresponding to an off state. The close agreement between theory and experiment in the off state, on the other hand, suggests the possibility of gate-programmable magnetic moments at the defects.

Defect engineering is a key approach for tailoring the properties of the emerging two-dimensional semiconductors. Here, we report an atomic engineering of the W vacancy in monolayer WSe

In a superconductor Cooper pairs condense into a single state and in so doing support dissipation free charge flow and perfect diamagnetism. In a magnetic field the minimum kinetic energy of the Cooper pairs increases, producing an orbital pair breaking effect. We show that it is possible to significantly quench the orbital pair breaking effect for both parallel and perpendicular magnetic fields in a thin film superconductor with lateral nanostructure on a length scale smaller than the magnetic length. By growing an ultra-thin (2 nm thick) single crystalline Pb nanowire network, we establish nm scale lateral structure without introducing weak links. Our network suppresses orbital pair breaking for both perpendicular and in-plane fields with a negligible reduction in zero-field resistive critical temperatures. Our study opens a frontier in nanoscale superconductivity by providing a strategy for maintaining pairing in strong field environments in all directions with important technological implications., It is highly desired to maintain superconductivity in presence of magnetic fields but it is by far difficult. Here, Nam et al. create a single crystalline superconducting Pb nanowire network, where critical temperatures are maintained and critical fields are enhanced in either parallel or perpendicular fields.

We use angle resolved photoemission spectroscopy (ARPES) to investigate the coupling of electron quantum well states (QWS) in epitaxial thin Pb and Ag films. More specifically, we investigate the Ag/Si, Pb/Si, and Pb/Ag/Si systems. We found that the parallel momentum plays a very profound role determining how two adjacent quantum wells are coupled electronically across the interface. We revealed that in the Pb/Ag bimetallic system, there exist two distinctly different regimes in the energy versus momentum (E vs. k) space. In one regime the electronic states in Ag and Pb are strongly coupled resulting in a new set of quantum well states for the bi-metallic system. In the other regime the electronic states in individual metallic layers are retained in their respective regions, as if they are totally decoupled. This result is corroborated by calculations using density functional theory. We further unravel the underlying mechanism associated with the electron refraction and total internal reflection across the interface.

We report on a study of epitaxially grown ultrathin Pb films that are only a few atoms thick and have parallel critical magnetic fields much higher than the expected limit set by the interaction of electron spins with a magnetic field, that is, the Clogston-Chandrasekhar limit. The epitaxial thin films are classified as dirty-limit superconductors because their mean-free paths, which are limited by surface scattering, are smaller than their superconducting coherence lengths. The uniformity of superconductivity in these thin films is established by comparing scanning tunneling spectroscopy, scanning superconducting quantum interference device (SQUID) magnetometry, double-coil mutual inductance, and magneto-transport, data that provide average superfluid rigidity on length scales covering the range from microscopic to macroscopic. We argue that the survival of superconductivity at Zeeman energies much larger than the superconducting gap can be understood only as the consequence of strong spin-orbit coupling that, together with substrate-induced inversion-symmetry breaking, produces spin splitting in the normal-state energy bands that is much larger than the superconductor's energy gap.

Optical dielectric constants are critical to modeling the electronic and optical properties of materials. Silver, as a noble metal with low loss, has been extensively investigated. The recently developed epitaxial growths of single crystalline Ag on dielectric substrates have prompted efforts to characterize their intrinsic optical dielectric function. In this paper, we report spectral ellipsometry measurements and analysis of a thick, epitaxially-grown, single-crystalline Ag film. We focus on the range of 0.18 – 1.0 eV or 1.24 – 7 µm, an energy and wavelength range that has not been examined previously using epitaxial films. We compare the extracted dielectric constants and the predicted optical performances with previous measurements. The loss is appreciably lower than the widely quoted Palik’s optical constants (i.e., up to a factor of 2) in the infrared frequency range. The improved knowledge of fundamental optical properties of the high-quality epitaxial Ag film will have a broad impact on simulations and practical applications based on Ag in the long wavelength range.

Following the discovery of topological insulators, there has been a renewed interest in superconducting systems that have strong spin-orbit (SO) coupling. Here we address the fundamental question of how the spin properties of a otherwise spin-singlet superconducting ground state evolve with increasing SO impurity density. We have mapped out the Zeeman critical field phase diagram of superconducting Al films that were deposited over random Pb cluster arrays of varying density. These phase diagrams give a direct measure of the Fermi liquid spin renormalization, as well as the spin orbit scattering rate. We find that the spin renormalization is a linear function of the average Pb cluster-to-cluster separation and that this dependency can be used to tune the spin susceptibility of the Al over a surprisingly wide range from 0.8$\chi_0$ to 4.0$\chi_0$, where $\chi_0$ is the non-interacting Pauli susceptibility., Comment: 5 pages, 4 figures

The moire pattern formed between a two-dimensional (2D) material and the substrate has played a crucial role in tuning the electronic structure of the 2D material. Here, by using scanning tunneling microscopy and spectroscopy, we found a moire-pattern-dependent band gap and work function modulation in hexagonal boron nitride (hBN)/Cu(111) heterostructures, whose amplitudes increase with the moire pattern wavelength. Moreover, the work function modulation shifts agree well with the conduction band edge shifts, indicating a spatially constant electron affinity for the hBN layer. Density functional theory calculations showed that these observations in hBN/Cu(111) heterostructures mainly originated from the hybridization of the N 3pz orbital and Cu 4s orbital in different atomic configurations. Our results show that the twist-angle dependence of moire patterns in hBN/Cu(111) heterostructures can be used to tailor the electronic properties including band gap and work function.

Valley degree of freedom in monolayer transition metal dichalcogenides have been explored as an information carrier. In a different context, metasurfaces consisting of engineered components have enabled the manipulation of light in unprecedented ways. Here, we demonstrate that by placing a MoS2 monolayer onto a metasurface consisting of asymmetric grooves, valley polarized excitons can be spatially separated even at room temperature.