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.Keywords: epitaxial silver film; low threshold; plasmonic nanolaser; semiconductor nanolaser; surface plasmon polariton; telecom wavelength;

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 a rather unique electronic structure of WSe2: the existence of a dark state below the bright exciton state.Keywords: dark exciton; defect-bound exciton; Monolayer WSe2; photoluminescence; surface plasmon polaritons; transition metal dichalcogenide;

AbstractSemiconductor heterostructures have played a critical role as the enabler for new science and technology. The emergence of transition-metal dichalcogenides (TMDs) as atomically thin semiconductors has opened new frontiers in semiconductor heterostructures either by stacking different TMDs to form vertical heterojunctions or by stitching them laterally to form lateral heterojunctions via direct growth. In conventional semiconductor heterostructures, the design of multijunctions is critical to achieve carrier confinement. Analogously, successful synthesis of a monolayer WS2/WS2(1−x)Se2x/WS2 multijunction lateral heterostructure via direct growth by chemical vapor deposition is reported. The grown structures are characterized by Raman, photoluminescence, and annular dark-field scanning transmission electron microscopy to determine their lateral compositional profile. More importantly, using microwave impedance microscopy, it is demonstrated that the local photoconductivity in the alloy region can be tailored and enhanced by two orders of magnitude over pure WS2. Finite element analysis confirms that this effect is due to the carrier diffusion and confinement into the alloy region. This work exemplifies the technological potential of atomically thin lateral heterostructures in optoelectronic applications.

Aluminum (Al) provides an excellent material platform for plasmonic applications in the ultraviolet (UV) regime due to its low loss coefficient at UV wavelengths. To fully realize the potential of this material, it is imperative to create nanostructures with minimal defects in order to prevent light scattering and better support plasmonic resonances. In this work, we report the successful development of atomically smooth epitaxial Al films on silicon. These epitaxial Al thin films facilitate the creation of fine plasmonic nanostructures and demonstrate considerable loss reduction in the UV frequency range, in comparison to the polycrystalline Al films based on spectroscopic ellipsometry measurements. Remarkably, our measurements on the epitaxial Al film grown using the two-step method suggest that the intrinsic loss in Al is significantly lower, by up to a factor of 2 in the UV range, with respect to current widely quoted Palik’s values extracted from polycrystalline films. These high-quality epitaxial Al films provide an ideal platform for UV plasmonics. In addition, the availability of intrinsic optical constants will enable more accurate theoretical predictions to guide the device design.Keywords: ellipsometry; epitaxial growth; intrinsic optical constants; plasmonic resonances; single-crystalline aluminum

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.

By using a comprehensive form of scanning tunneling spectroscopy, we have revealed detailed quasi-particle electronic structures in transition metal dichalcogenides, including the quasi-particle gaps, critical point energy locations, and their origins in the Brillouin zones. We show that single layer WSe2 surprisingly has an indirect quasi-particle gap with the conduction band minimum located at the Q-point (instead of K), albeit the two states are nearly degenerate. We have further observed rich quasi-particle electronic structures of transition metal dichalcogenides as a function of atomic structures and spin–orbit couplings. Such a local probe for detailed electronic structures in conduction and valence bands will be ideal to investigate how electronic structures of transition metal dichalcogenides are influenced by variations of local environment.

•The thickness dependence of Au-Pb alloy formation on Pb quantum films is observed via in-situ STM/S.•DFT shows Au can get into either subsurface interstitial sites or surface-layer substitutional sites of Pb(111) surface.•2D islands with moiré pattern are observed on Pb films when sub-monolayer Au is deposited onto Pb films at 90 K.•2D islands with moiré pattern are transformed into various types of Au-Pb alloys after annealing at up to 250 K.•A STS study suggests that the formation of these Au-Pb alloys is directly related to the quantum well states of Pb films.The thickness dependence of Au–Pb alloy formation on Pb quantum films is studied via in-situ low-temperature scanning tunneling microscopy/spectroscopy (STM/S). 2D islands with moiré pattern are observed on top of Pb films when sub-monolayer Au is deposited onto Pb films at a substrate temperature of 90 K. After annealing at up to 250 K, various types of 2D islands, including Au–Pb alloys, are formed and show very different electronic structures. A detailed STS study suggests that the formation of these islands is directly related to the quantum well states (QWS) of Pb films, indicating quantum size effects (QSE) on the formation of Au–Pb alloys.

Using scanning tunneling microscopy and spectroscopy, we probe the electronic structures of single layer MoS2 on graphite. The apparent quasiparticle energy gap of single layer MoS2 is measured to be 2.15 ± 0.06 eV at 77 K, albeit a higher second conduction band threshold at 0.2 eV above the apparent conduction band minimum is also observed. Combining it with photoluminescence studies, we deduce an exciton binding energy of 0.22 ± 0.1 eV (or 0.42 eV if the second threshold is use), a value that is lower than current theoretical predictions. Consistent with theoretical predictions, we directly observe metallic edge states of single layer MoS2. In the bulk region of MoS2, the Fermi level is located at 1.8 eV above the valence band maximum, possibly due to the formation of a graphite/MoS2 heterojunction. At the edge, however, we observe an upward band bending of 0.6 eV within a short depletion length of about 5 nm, analogous to the phenomena of Fermi level pinning of a 3D semiconductor by metallic surface states.

We report on the first demonstration of broadband tunable, single-mode plasmonic nanolasers (spasers) emitting in the full visible spectrum. These nanolasers are based on a single metal–oxide–semiconductor nanostructure platform comprising of InGaN/GaN semiconductor nanorods supported on an Al2O3-capped epitaxial Ag film. In particular, all-color lasing in subdiffraction plasmonic resonators is achieved via a novel mechanism based on a property of weak size dependence inherent in spasers. Moreover, we have successfully reduced the continuous-wave (CW) lasing thresholds to ultrasmall values for all three primary colors and have clearly demonstrated the possibility of “thresholdless” lasing for the blue plasmonic nanolaser.

In this Letter we report a comparative study, in the infrared regime, of surface plasmon polariton (SPP) propagation in epitaxially grown Ag films and in polycrystalline Ag films, all grown on Si substrates. Plasmonic resonance features are analyzed using extraordinary optical transmission (EOT) measurements, and SPP band structures for the two dielectric/metal interfaces are investigated for both types of film. At the Si/Ag interface, EOT spectra show almost identical features for epitaxial and polycrystalline Ag films and are characterized by sharp Fano resonances. On the contrary, at the air/Ag interface, dramatic differences are observed: while the epitaxial film continues to exhibit sharp Fano resonances, the polycrystalline film shows only broad spectral features and much lower transmission intensities. In corroboration with theoretical simulations, we find that surface roughness plays a critical role in SPP propagation for this wavelength range.

Using scanning tunneling microscopy (STM), we demonstrate that oxidation on Pb films is greatly enhanced by atomic Cs catalysts. With only a minute concentration of isolated Cs substitutional atoms in the surface layer (0.004 ML coverage), surface oxidation rates are greatly enhanced. First-principles density functional theory (DFT) calculations reveal that a substitutional Cs atom strongly increases O2 binding on the surface. Then, with additional oxygen exposure this substitutional Cs-initiated oxidation process results in growth of PbO layers in an auto-catalytic manner. Furthermore, we investigate the role of temperature in the oxidation of the Pb films with and without Cs, and we explore the overall morphology of the resultant oxide layers.Highlights► Substitutional Cs atoms on Pb thin films as controllable atomic catalysts. ► Oxygen preferentially bonds to Cs atoms: very effective nucleation sites. ► Subsequent PbO growth follows auto-catalytic process with oxygen exposure. ► Cs functions as an effective nucleation site from 155 K to 290 K.

In this paper, we present the direct observation of quantum size effects (QSE) on the work function in ultrathin Pb films. By using scanning tunneling microscopy and spectroscopy, we show that the very existence of quantum well states (QWS) in these ultrathin films profoundly affects the measured tunneling decay constant κ, resulting in a very rich phenomenon of “quantum oscillations” in κ as a function of thickness, L, and bias voltage, Vs. More specifically, we find that the phase of the quantum oscillations in κ vs. L depends sensitively upon the bias voltage, which often results in a total phase reversal at different biases. On the other hand, at very low sample bias (|Vs| < 0.03 V) the measurement of κ vs. L accurately reflects the quantum size effect on the work function. In particular, the minima in the quantum oscillations of κ vs. L occur at the locations where QWS cross the Fermi energy, thus directly unraveling the QSE on the work function in ultrathin films, which was predicted more than three decades ago. This further clarifies several contradictions regarding the relationship between the QWS locations and the work function.

Single-quantum emitters emit only one photon at a time1, 2, but the properties of the photon depend on how the emitter is excited3. Incoherent excitation is simple and broadly used with solid-state emitters such as quantum dots, but does not allow direct manipulation of the quantum state. Coherent, resonant excitation on the other hand is used in pump–probe techniques to examine the quantum state of the emitter4, but does not permit collection of the single-photon emission. Coherent control with simultaneous generation of photons has been an elusive goal in solid-state approaches, where, because of strong laser scattering at the detection wavelength, measurement of resonant emission has been limited to cross-polarized detection5 or Stokes-shift techniques6, 7. Here we demonstrate that a semiconductor quantum dot in a microcavity can be resonantly driven and its single-photon emission extracted background free. Under strong continuous-wave excitation, the dot undergoes several Rabi oscillations before emitting, which are visible as oscillations in the second-order correlation function. The quantum-dot states are therefore ‘dressed’, resulting in a Mollow-triplet emission spectrum. Such coherent control will be necessary for future high-efficiency sources of indistinguishable single photons3, 8, which can be used for quantum key distribution9 or through post-selection10 to generate entangled photon pairs11, 12.

We investigated and compared the growth morphology of Ag films deposited on different Si surfaces at low temperatures and annealed at room temperature with scanning tunneling microscopy. Ag films on clean Si(1 1 1) 7×7 and Si(0 0 1) 2×1 surfaces exhibit with increasing film thickness: clusters (interconnected), islands with flat top terraces, flat films with voids extending down to the wetting layer, and flat films with no voids. The Ag films on Au-reconstructed Si(1 1 1) surfaces exhibit the same trend, with the exception that the initial islands exhibit no well defined heights. The growth morphology observed does not allow the identification of a single critical or minimum thickness of the Ag film as expected in the electronic growth model. Two different critical thicknesses are defined, which are higher for Si(0 0 1) 2×1 than for Si(1 1 1) 7×7 surfaces. The importance of surface states and pinning levels within the electronic growth model is discussed.

We investigate the interaction between propagating surface plasmons in silver nanowires and excitons generated in quantum dots. We show propagating surface plasmons can excite excitons, which results in quantum dot emission. In this process, the energy is directly transferred from the propagating surface plasmons to the excitons without converting to photons. Furthermore, we demonstrate the reverse process where the decay of excitons generates surface plasmons.