Extreme Thermal Insulation and Tradeoff of Thermal Transport Mechanisms between Graphene and WS2 Monolayers.

Controlling and understanding the heat flow at a nanometer scale are challenging, but important for fundamental science and applications. Two-dimensional (2D) layered materials provide perhaps the ultimate solution for meeting these challenges. While there have been reports of low thermal conductivities (several mW m-1 K-1 ) across the 2D heterostructures, phonon-dominant thermal transport remains strong due to the nearly-ideal contact between the layers. Here, this work experimentally explores the heat transport mechanisms by increasing the interlayer distance from perfect contact to a few nanometers and demonstrates that the phonon-dominated thermal conductivity across the WS2 /graphene interface decreases further with the increasing interlayer distance until the air-dominated thermal conductivity increases again. This work finds that the resulting tradeoff of the two heat conduction mechanisms leads to the existence of a minimum thermal conductivity at 2.11 nm of 1.41 × 10-5  W m-1 K-1 , which is two thousandths of the smallest value reported previously. This work provides an effective methodology for engineering thermal insulation structures and understanding heat transport at the ultimate small scales.

Self-optimized single-nanowire photoluminescence thermometry.

Nanomaterials-based photoluminescence thermometry (PLT) is a new contact-free photonic approach for temperature sensing, important for applications ranging from quantum technology to biomedical imaging and diagnostics. Even though numerous new materials have been explored, great challenges and deficiencies remain that hamper many applications. In contrast to most of the existing approaches that use large ensembles of rare-earth-doped nanomaterials with large volumes and unavoidable inhomogeneity, we demonstrate the ultimate size reduction and simplicity of PLT by using only a single erbium-chloride-silicate (ECS) nanowire. Importantly, we propose and demonstrate a novel strategy that contains a self-optimization or "smart" procedure to automatically identify the best PL intensity ratio for temperature sensing. The automated procedure is used to self-optimize key sensing metrics, such as sensitivity, precision, or resolution to achieve an all-around superior PLT including several record-setting metrics including the first sensitivity exceeding 100% K-1 (~138% K-1), the highest resolution of 0.01 K, and the largest range of sensible temperatures 4-500 K operating completely within 1500-1800 nm (an important biological window). The high-quality ECS nanowire enables the use of well-resolved Stark-sublevels to construct a series of PL intensity ratios for optimization in infrared, allowing the completely Boltzmann-based sensing at cryogenic temperature for the first time. Our single-nanowire PLT and the proposed optimization strategy overcome many existing challenges and could fundamentally impact PL nano-thermometry and related applications such as single-cell thermometry.

Strain-Induced Indirect-to-Direct Bandgap Transition, Photoluminescence Enhancement, and Linewidth Reduction in Bilayer MoTe2.

Two-dimensional (2D) layered materials provide an ideal platform for engineering electronic and optical properties through strain control because of their extremely high mechanical elasticity and sensitive dependence of material properties on mechanical strain. In this paper, a combined experimental and theoretical effort is made to investigate the effects of mechanical strain on various spectral features of bilayer MoTe2 photoluminescence (PL). We found that bilayer MoTe2 can be converted from an indirect to a direct bandgap material through strain engineering, resulting in a photoluminescence enhancement by a factor of 2.24. Over 90% of the PL comes from photons emitted by the direct excitons at the maximum strain applied. Importantly, we show that strain effects lead to a reduction of the overall linewidth of PL by as much as 36.6%. We attribute the dramatic decrease of linewidth to a strain-induced complex interplay among various excitonic varieties such as direct bright excitons, trions, and indirect excitons. Our experimental results on direct and indirect exciton emission features are explained by theoretical exciton energies that are based on first-principles electronic band structure calculations. The consistent theory-experimental trend shows that the enhancement of PL and the reduction of linewidth are the consequences of the increasing direct exciton contribution with the increase of strain. Our results demonstrate that strain engineering can lead to a PL quality of the bilayer MoTe2 comparable to that of the monolayer counterpart. The additional benefit of a longer emission wavelength makes the bilayer MoTe2 more suitable for silicon-photonics integration due to the reduced silicon absorption.

Extraction of silver losses at cryogenic temperatures through the optical characterization of silver-coated plasmonic nanolasers.

We report on the extraction of silver losses in the range 10 K-180 K by performing temperature-dependent micro-photoluminescence measurements in conjunction with numerical simulations on silver-coated nanolasers around near-infrared telecommunication wavelengths. By mapping changes in the quality factor of nanolasers into silver-loss variations, the imaginary part of silver permittivity is extracted at cryogenic temperatures. The latter is estimated to reach values an order of magnitude lower than room-temperature values. Temperature-dependent values for the thermo-optic coefficient of III-V semiconductors occupying the cavity are estimated as well. This data is missing from the literature and is crucial for precise device modeling. Our results can be useful for device designing, the theoretical validation of experimental observations as well as the evaluation of thermal effects in silver-coated nanophotonic structures.

Large-Scale, High-Yield Laser Fabrication of Bright and Pure Single-Photon Emitters at Room Temperature in Hexagonal Boron Nitride.

Single-photon emitters (SPEs) play an important role in many optical quantum technologies. However, an efficient large-scale approach to the generation of high-quality SPE arrays remains an elusive goal at room temperature. Here, we demonstrate a scalable method of generating SPE arrays in hexagonal boron nitride (hBN) with high yield, brightness, and purity using single-pulse irradiation by a femtosecond laser. Our use of a single pulse per defect pattern minimized heat-related damages and improved the purity of SPEs compared with the previous laser-based approaches. Under the optimized fabrication and post-treatment conditions, SPE arrays were successfully generated from the 3.0 µm defect patterns with 43% yield, the highest among the 2D-based top-down approaches. Importantly, we found that 100% of the bright defect patterns are SPEs with g2(0) < 0.5 under such conditions, with the lowest g2(0) = 0.06 ± 0.03. Our SPEs also exhibit the highest brightness with the saturation SPE rate at 7.15 million counts per second. We believe that our overall high-quality and large-scale approach will help a wide range of applications of SPEs in on-chip quantum technologies.

Prolonging valley polarization lifetime through gate-controlled exciton-to-trion conversion in monolayer molybdenum ditelluride.

Monolayer 2D semiconductors provide an attractive option for valleytronics due to valley-addressability. But the short valley-polarization lifetimes for excitons have hindered potential valleytronic applications. In this paper, we demonstrate a strategy for prolonging the valley-polarization lifetime by converting excitons to trions through efficient gate control and exploiting the much longer valley-polarization lifetimes for trions than for excitons. At charge neutrality, the valley lifetime of monolayer MoTe2 increases by a factor of 1000 to the order of nanoseconds from excitons to trions. The exciton-to-trion conversion changes the dominant depolarization mechanism from the fast electron-hole exchange for excitons to the slow spin-flip process for trions. Moreover, the degree of valley polarization increases to 38% for excitons and 33% for trions through electrical manipulation. Our results reveal the depolarization dynamics and the interplay of various depolarization channels for excitons and trions, providing an effective strategy for prolonging the valley polarization.

Ultrasensitive Detection of Biomarkers in a Color-Switchable Microcavity-Reactor Laser.

Early detection and diagnosis are vitally important in reducing the mortality rate of fatal diseases but require highly sensitive detection of biomarkers. Presently, detection methods with the highest sensitivity require in vitro processing, while in vivo compatible fluorescence detections require a much higher concentration of biomarkers or limit of detection (LOD). In this paper, a fundamentally new strategy for ultrasensitive detection based on color-switchable lasing with a cavity-enhanced reduction of LOD is demonstrated, down to 1.4 × 10-16  mg ml-1 for a quantitative detection, lower than both the fluorescence method and plasmonic enhanced method. For a qualitative or a yes/no type of detection, the LOD is as low as 10-17  mg ml-1 . The approach in this work is based on a dye-embedded, in vivo compatible, polystyrene-sphere cavity, penetrable by biomarkers. A polystyrene sphere serves the dual roles of a laser cavity and an in vivo bio-reactor, in which dye molecules react with a biomarker, reporting biomarker information through lasing signals. The cavity-enhanced emission and lasing with only a single biomarker molecule per cavity allow improved visual distinguishability via color changes. Furthermore, when combined with a narrow-band filter, the color-switchable lasers act as an "on-off" logic signal and can be integrated into multiplexing detection assay biochips.

Injection-free multiwavelength electroluminescence devices based on monolayer semiconductors driven by an alternating field.

Two-dimensional (2D) semiconductors have emerged as promising candidates for various optoelectronic devices especially electroluminescent (EL) devices. However, progress has been hampered by many challenges including metal contacts and injection, transport, and confinement of carriers due to small sizes of materials and the lack of proper double heterostructures. Here, we propose and demonstrate an alternative approach to conventional current injection devices. We take advantage of large exciton binding energies in 2D materials using impact generation of excitons through an alternating electric field, without requiring metal contacts to 2D materials. The conversion efficiency, defined as the ratio of the emitted photons to the preexisting carriers, can reach 16% at room temperature. In addition, we demonstrate the first multiwavelength 2D EL device, simultaneously operating at three wavelengths from red to near-infrared. Our approach provides an alternative to conventional current-based devices and could unleash the great potential of 2D materials for EL devices.

Nonvolatile electrical switching of optical and valleytronic properties of interlayer excitons.

Long-lived interlayer excitons (IXs) in van der Waals heterostructures (HSs) stacked by monolayer transition metal dichalcogenides (TMDs) carry valley-polarized information and thus could find promising applications in valleytronic devices. Current manipulation approaches for valley polarization of IXs are mainly limited in electrical field/doping, magnetic field or twist-angle engineering. Here, we demonstrate an electrochemical-doping method, which is efficient, in-situ and nonvolatile. We find the emission characteristics of IXs in WS2/WSe2 HSs exhibit a large excitonic/valley-polarized hysteresis upon cyclic-voltage sweeping, which is ascribed to the chemical-doping of O2/H2O redox couple trapped between WSe2 and substrate. Taking advantage of the large hysteresis, a nonvolatile valley-addressable memory is successfully demonstrated. The valley-polarized information can be non-volatilely switched by electrical gating with retention time exceeding 60 min. These findings open up an avenue for nonvolatile valley-addressable memory and could stimulate more investigations on valleytronic devices.

Room-Temperature Exciton-Based Optoelectronic Switch.

Excitons, bound pairs of electrons and holes, could act as an intermediary between electronic signal processing and optical transmission, thus speeding up the interconnection of photoelectric communication. However, up to date, exciton-based logic devices such as switches that work at room temperature are still lacking. This work presents a prototype of a room-temperature optoelectronic switch based on excitons in WSe2 monolayer. The emission intensity of WSe2 stacked on Au and SiO2 substrates exhibits completely opposite behaviors upon applying gate voltages. Such observation can be ascribed to different doping behaviors of WSe2 caused by charge-transfer and chemical-doping effect at WSe2 /Au and WSe2 /SiO2 interfaces, respectively, together with the charge-drift effect. These interesting features can be utilized for optoelectronic switching, confirmed by the cyclic PL switching test for a long time exceeding 4000 s. This study offers a universal and reliable approach for the fabrication of exciton-based optoelectronic switches, which would be essential in integrated nanophotonics.

Ten years of spasers and plasmonic nanolasers.

Ten years ago, three teams experimentally demonstrated the first spasers, or plasmonic nanolasers, after the spaser concept was first proposed theoretically in 2003. An overview of the significant progress achieved over the last 10 years is presented here, together with the original context of and motivations for this research. After a general introduction, we first summarize the fundamental properties of spasers and discuss the major motivations that led to the first demonstrations of spasers and nanolasers. This is followed by an overview of crucial technological progress, including lasing threshold reduction, dynamic modulation, room-temperature operation, electrical injection, the control and improvement of spasers, the array operation of spasers, and selected applications of single-particle spasers. Research prospects are presented in relation to several directions of development, including further miniaturization, the relationship with Bose-Einstein condensation, novel spaser-based interconnects, and other features of spasers and plasmonic lasers that have yet to be realized or challenges that are still to be overcome.

Reconstructing Local Profile of Exciton-Emission Wavelengths across a WS2 Bubble beyond the Diffraction Limit.

Air bubbles formed between layers of two-dimensional (2D) materials not only are unavoidable but also emerge as an important means of engineering their excitonic emission properties, especially as controllable quantum light sources. Measuring the actual spatially resolved optical properties across such bubbles is important for understanding excitonic physics and for device applications; however, such a measurement is challenging due to nanoscale features involved which require spatial resolution beyond the diffraction limit. Additional complexity is the involvement of multiple physical effects such as mechanical strain and dielectric environment that are difficult to disentangle. In this paper, we demonstrate an effective approach combining micro-photoluminescence measurement, atomic force microscope profile mapping, and a theoretical strain model. We succeeded in reconstructing the actual spatial profiles of the emission wavelengths beyond the diffraction limit for bubbles formed by a monolayer tungsten disulfide on boron nitride. The agreements and consistency among various approaches established the validity of our approach. In addition, our approach allows us to disentangle the effects of strain and dielectric environment and provides a general and reliable method to determine the true magnitude of wavelength changes due to the individual effects across bubbles. Importantly, we found that micro-optical measurement underestimates the red and blue shifts by almost 5 times. Our results provide important insights into strain and screening-dependent optical properties of 2D materials on the nanometer scale and contribute significantly to our understanding of excitonic emission physics as well as potential applications of bubbles in optoelectronic devices.

Excitonic complexes and optical gain in two-dimensional molybdenum ditelluride well below the Mott transition.

Semiconductors that can provide optical gain at extremely low carrier density levels are critically important for applications such as energy efficient nanolasers. However, all current semiconductor lasers are based on traditional semiconductor materials that require extremely high density levels above the so-called Mott transition to realize optical gain. The new emerging 2D materials provide unprecedented opportunities for studying new excitonic physics and exploring new optical gain mechanisms at much lower density levels due to the strong Coulomb interaction and co-existence and mutual conversion of excitonic complexes. Here, we report a new gain mechanism involving charged excitons or trions in electrically gated 2D molybdenum ditelluride well below the Mott density. Our combined experimental and modelling study not only reveals the complex interplay of excitonic complexes well below the Mott transition but also establishes 2D materials as a new class of gain materials at densities 4-5 orders of magnitude lower than those of conventional semiconductors and provides a foundation for lasing at ultralow injection levels for future energy efficient photonic devices. Additionally, our study could help reconcile recent conflicting results on 2D materials: While 2D material-based lasers have been demonstrated at extremely low densities with spectral features dominated by various excitonic complexes, optical gain was only observed in experiments at densities several orders of magnitude higher, beyond the Mott density. We believe that our results could lead to more systematic studies on the relationship between the mutual conversion of excitonic species and the existence of optical gain well below the Mott transition.

Nanowires for Photonics.

All-photonic integrated circuits are promising platforms for future systems beyond the limitation of Moore's law. Over the last several decades, one-dimensional (1D) nanowires have demonstrated great potential in photonic circuitry because of their unique 1D structure to effectively generate and tightly confine optical signals as well as easily tunable optical properties. In this Review, we categorize nanowires based on the optical properties (i.e., semiconducting, metallic, and dielectric nanowires) for their potential photonic applications (as light emitters or plasmonic and photonic waveguides). We further discuss the recent efforts in integration of nanowire-based photonic elements toward next-generation optical information processors. However, there are still several challenges remaining before the nanowires are fully utilized as photonic building blocks. The scientific and technical challenges and outlooks are provided to indicate the future directions.

A measurement method of the intrinsic optical absorption spectrum of 1D nanomaterials and its application to erbium chloride silicate nanowires.

Measurement of the absolute absorption coefficient of various nanomaterials over a wide spectral range is important for a variety of photonic applications but is very challenging due to strong scatterings from the intrinsically granular features of nanomaterials. We report in this paper a two-step method to determine the absorption spectrum on the absolute scale for an ensemble of nanowires: first, the relative absorption spectrum over a wide spectral range is measured from the nanowire ensemble in a carefully designed experiment using integrating sphere. Second, the absorption coefficient at a single wavelength is measured on a single nanowire to serve as the calibration of the relative spectrum. The combination of the two measurements allows the determination of the absolute absorption spectrum over a wide range. We then apply this measurement strategy to a relatively new class of nanowire materials, the erbium compound (erbium chloride silicate (ECS)) nanowires to determine its absorption spectrum. The absorption coefficient in a wide spectral range from near infrared to visible was determined for the first time for this unique erbium compound material. The measurement strategy is generally applicable to other 1D nanomaterials. The precise determination of the ECS absorption spectrum in such a wide spectral range is of vital importance to various applications of ECS nanowires including nanolasers, solar cells, and nanoscale amplifiers.

Composition-graded nanowire solar cells fabricated in a single process for spectrum-splitting photovoltaic systems.

Nanomaterials such as semiconductor nanowires have unique features that could enable novel optoelectronic applications such as novel solar cells. This paper aims to demonstrate one such recently proposed concept: Monolithically Integrated Laterally Arrayed Multiple Band gap (MILAMB) solar cells for spectrum-splitting photovoltaic systems. Two cells with different band gaps were fabricated simultaneously in the same process on a single substrate using spatially composition-graded CdSSe alloy nanowires grown by the Dual-Gradient Method in a chemical vapor deposition system. CdSSe nanowire ensemble devices tested under 1 sun AM1.5G illumination achieved open-circuit voltages up to 307 and 173 mV and short-circuit current densities as high as 0.091 and 0.974 mA/cm(2) for the CdS- and CdSe-rich cells, respectively. The open-circuit voltages were roughly three times those of similar CdSSe film cells fabricated for comparison due to the superior optical quality of the nanowires. I-V measurements were also performed using optical filters to simulate spectrum-splitting. The open-circuit voltages and fill factors of the CdS-rich subcells were uniformly larger than the corresponding CdSe-rich cells for similar photon flux, as expected. This suggests that if all wires can be contacted, the wide-gap cell is expected to have greater output power than the narrow-gap cell, which is the key to achieving high efficiencies with spectrum-splitting. This paper thus provides the first proof-of-concept demonstration of simultaneous fabrication of MILAMB solar cells. This approach to solar cell fabrication using single-crystal nanowires for spectrum-splitting photovoltaics could provide a future low-cost high-efficiency alternative to the conventional high-cost high-efficiency tandem cells.

Dynamical color-controllable lasing with extremely wide tuning range from red to green in a single alloy nanowire using nanoscale manipulation.

Multicolor lasing and dynamic color-tuning in a wide spectrum range are challenging to realize but critically important in many areas of technology and daily life, such as general lighting, display, multicolor detection, and multiband communication. By exploring nanoscale growth and manipulation, we have demonstrated the first active dynamical color control of multicolor lasing, continuously tunable between red and green colors separated by 107 nm in wavelength. This is achieved in a purposely engineered single CdSSe alloy nanowire with composition varied along the wire axis. By looping the wide-gap end of the alloy nanowire through nanoscale manipulation, two largely independent (only weakly coupled) laser cavities are formed respectively for the green and red color modes. Our approach simultaneously overcomes the two fundamental challenges for multicolor lasing in material growth and cavity design. Such multicolor lasing and continuous color tuning in a wide spectral range represents a new paradigm shift and would eventually enable color-by-design and white-color lasers for lighting, illumination, and many other applications.

Influence of supersaturation and spontaneous catalyst formation on the growth of PbS wires: toward a unified understanding of growth modes.

High quality stoichiometric lead sulfide (PbS) wires were synthesized by a simple chemical vapor deposition (CVD) process using pure PbS powder as the material source. Growth mechanisms were systematically investigated under various growth conditions, with three modes of growth identified: direct vapor-liquid-solid (VLS) wire growth nucleating from the substrate surface, bulk PbS crystallites by vapor-solid (VS) deposition, and subsequent VLS growth nucleating on top of the bulk deposition through spontaneously formed catalyst particles. Furthermore, we found that these growth modes can be organized in terms of different levels of supersaturation, with VS bulk deposition dominating at high supersaturation and VLS wire growth on the substrate dominating at low supersaturation. At intermediate supersaturation, the bulk VS deposition can form larger crystallites with domains of similarly oriented wires extending from the flat facets. Both predeposited catalysts and spontaneously formed Pb particles were observed as nucleation catalysts, and their interplay leads to various interesting growth scenarios such as reversely tapered growth with increasing diameter. The VLS growth mechanism was confirmed by the presence of Pb-rich caps revealed in an elaborate cross-sectional transmission electron microscopy (TEM) experiment after focused ion beam milling in a modified lift-out procedure. Temperature-dependent photoluminescence (PL) of PbS wires was performed in the mid-infrared wavelength range for the first time, demonstrating strong light emission from band edge, blue-shifted with increasing temperature. The high optical quality of PbS wires may lead to important applications in mid-infrared photonics. The substrate growth temperature as low as 400 °C allows for silicon-compatible processing for integrated optoelectronics applications.

In(x)Ga(1-x)As nanowires on silicon: one-dimensional heterogeneous epitaxy, bandgap engineering, and photovoltaics.

We report on the one-dimensional (1D) heteroepitaxial growth of In(x)Ga(1-x)As (x = 0.2-1) nanowires (NWs) on silicon (Si) substrates over almost the entire composition range using metalorganic chemical vapor deposition (MOCVD) without catalysts or masks. The epitaxial growth takes place spontaneously producing uniform, nontapered, high aspect ratio NW arrays with a density exceeding 1 × 10(8)/cm(2). NW diameter (∼30-250 nm) is inversely proportional to the lattice mismatch between In(x)Ga(1-x)As and Si (∼4-11%), and can be further tuned by MOCVD growth condition. Remarkably, no dislocations have been found in all composition In(x)Ga(1-x)As NWs, even though massive stacking faults and twin planes are present. Indium rich NWs show more zinc-blende and Ga-rich NWs exhibit dominantly wurtzite polytype, as confirmed by scanning transmission electron microscopy (STEM) and photoluminescence spectra. Solar cells fabricated using an n-type In(0.3)Ga(0.7)As NW array on a p-type Si(111) substrate with a ∼ 2.2% area coverage, operates at an open circuit voltage, V(oc), and a short circuit current density, J(sc), of 0.37 V and 12.9 mA/cm(2), respectively. This work represents the first systematic report on direct 1D heteroepitaxy of ternary In(x)Ga(1-x)As NWs on silicon substrate in a wide composition/bandgap range that can be used for wafer-scale monolithic heterogeneous integration for high performance photovoltaics.