Uniaxial Strain Dependence on Angle-Resolved Optical Second Harmonic Generation from a Few Layers of Indium Selenide.

Indium selenide (InSe) is an emerging van der Waals material, which exhibits the potential to serve in excellent electronic and optoelectronic devices. One of the advantages of layered materials is their application to flexible devices. How strain alters the electronic and optical properties is, thus, an important issue. In this work, we experimentally measured the strain dependence on the angle-resolved second harmonic generation (SHG) pattern of a few layers of InSe. We used the exfoliation method to fabricate InSe flakes and measured the SHG images of the flakes with different azimuthal angles. We found the SHG intensity of InSe decreased, while the compressive strain increased. Through first-principles electronic structure calculations, we investigated the strain dependence on SHG susceptibilities and the corresponding angle-resolved SHG pattern. The experimental data could be fitted well by the calculated results using only a fitting parameter. The demonstrated method based on first-principles in this work can be used to quantitatively model the strain-induced angle-resolved SHG patterns in 2D materials. Our obtained results are very useful for the exploration of the physical properties of flexible devices based on 2D materials.

Anisotropic Excitons Reveal Local Spin Chain Directions in a van der Waals Antiferromagnet.

A long-standing pursuit in materials science is to identify suitable magnetic semiconductors for integrated information storage, processing, and transfer. Van der Waals magnets have brought forth new material candidates for this purpose. Recently, sharp exciton resonances in antiferromagnet NiPS3 have been reported to correlate with magnetic order, that is, the exciton photoluminescence intensity diminishes above the Néel temperature. Here, it is found that the polarization of maximal exciton emission rotates locally, revealing three possible spin chain directions. This discovery establishes a new understanding of the antiferromagnet order hidden in previous neutron scattering and optical experiments. Furthermore, defect-bound states are suggested as an alternative exciton formation mechanism that has yet to be explored in NiPS3 . The supporting evidence includes chemical analysis, excitation power, and thickness dependent photoluminescence and first-principles calculations. This mechanism for exciton formation is also consistent with the presence of strong phonon side bands. This study shows that anisotropic exciton photoluminescence can be used to read out local spin chain directions in antiferromagnets and realize multi-functional devices via spin-photon transduction.

Ultrafast carrier dynamics and layer-dependent carrier recombination rate in InSe.

InSe layered semiconductors with high mobility have advantages over transition-metal dichalcogenides in certain device applications. Understanding the dynamics of carriers, especially around the major bandgaps, is not only of fundamental interest but also important for improving the performance of devices. We investigated ultrafast carrier dynamics in exfoliated InSe near the bandgap and found that the presence of photocarriers led to shrinkage in the optical bandgap. In addition, we observed that the carrier recombination rate increased when the thickness of the InSe nanoflakes was reduced and the process was dominated by surface recombination. For the same flakes, the recombination rate became lower after the freshly exfoliated InSe was exposed to air and oxidized. Using a free carrier diffusion model, layer-dependent surface recombination velocities were obtained. Our investigation reveals that the surface condition and the thickness of few-layer InSe play important roles in carrier lifetimes.

Reliable preparation and regeneration of well-defined single-atom tips through laser annealing.

Single-atom tips (SATs) have crucial scientific and technological applications, such as in scanning probe microscopy and charged particle beam technology. We reported a reliable method of preparing and regenerating noble metal-covered W(111) SATs through laser annealing at approximately 1000 K under ultrahigh vacuum. The field emission patterns obtained during laser heating revealed the self-assembly process of a pyramidal tip. The SATs can be regenerated through laser annealing tens of times with little change in sharpness, indicating a long lifetime. Various pyramidal SATs can be generated and regenerated using visible-light, near-infrared, mode-locked, and continuous-wave lasers at different polarizations relative to the tip axis. The generation of well-defined pyramidal SATs through laser annealing can facilitate various applications of SATs.

Fabry-Perot interferometric calibration of van der Waals material-based nanomechanical resonators.

One of the challenges in integrating nanomechanical resonators made from van der Waals materials in optoelectromechanical technologies is characterizing their dynamic properties from vibrational displacement. Multiple calibration schemes using optical interferometry have tackled this challenge. However, these techniques are limited only to optically thin resonators with an optimal vacuum gap height and substrate for interferometric detection. Here, we address this limitation by implementing a modeling-based approach via multilayer thin-film interference for in situ, non-invasive determination of the resonator thickness, gap height, and motional amplitude. This method is demonstrated on niobium diselenide drumheads that are electromotively driven in their linear regime of motion. The laser scanning confocal configuration enables a resolution of hundreds of picometers in motional amplitude for circular and elliptical devices. The measured thickness and spacer height, determined to be in the order of tens and hundreds of nanometers, respectively, are in excellent agreement with profilometric measurements. Moreover, the transduction factor estimated from our method agrees with the result of other studies that resolved Brownian motion. This characterization method, which applies to both flexural and acoustic wave nanomechanical resonators, is robust because of its scalability to thickness and gap height, and any form of reflecting substrate.

Photothermal Responsivity of van der Waals Material-Based Nanomechanical Resonators.

Nanomechanical resonators made from van der Waals materials (vdW NMRs) provide a new tool for sensing absorbed laser power. The photothermal response of vdW NMRs, quantified from the resonant frequency shifts induced by optical absorption, is enhanced when incorporated in a Fabry-Pérot (FP) interferometer. Along with the enhancement comes the dependence of the photothermal response on NMR displacement, which lacks investigation. Here, we address the knowledge gap by studying electromotively driven niobium diselenide drumheads fabricated on highly reflective substrates. We use a FP-mediated absorptive heating model to explain the measured variations of the photothermal response. The model predicts a higher magnitude and tuning range of photothermal responses on few-layer and monolayer NbSe2 drumheads, which outperform other clamped vdW drum-type NMRs at a laser wavelength of 532 nm. Further analysis of the model shows that both the magnitude and tuning range of NbSe2 drumheads scale with thickness, establishing a displacement-based framework for building bolometers using FP-mediated vdW NMRs.

Imaging Off-Resonance Nanomechanical Motion as Modal Superposition.

Observation of resonance modes is the most straightforward way of studying mechanical oscillations because these modes have maximum response to stimuli. However, a deeper understanding of mechanical motion can be obtained by also looking at modal responses at frequencies in between resonances. Here, an imaging of the modal responses for a nanomechanical drum driven off resonance is presented. By using the frequency modal analysis, these shapes are described as a superposition of resonance modes. It is found that the spatial distribution of the oscillating component of the driving force, which is affected by both the shape of the actuating electrode and inherent device properties such as asymmetry and initial slack, greatly influences the modal weight or participation. This modal superposition analysis elucidates the dynamics of any nanomechanical system through modal weights. This aids in optimizing mode-specific designs for force sensing and integration with other systems.

Publisher Correction: Giant photothermal nonlinearity in a single silicon nanostructure.

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

Giant photothermal nonlinearity in a single silicon nanostructure.

Silicon photonics have attracted significant interest because of their potential in integrated photonics components and all-dielectric meta-optics elements. One major challenge is to achieve active control via strong photon-photon interactions, i.e. optical nonlinearity, which is intrinsically weak in silicon. To boost the nonlinear response, practical applications rely on resonant structures such as microring resonators or photonic crystals. Nevertheless, their typical footprints are larger than 10 µm. Here, we show that 100 nm silicon nano-resonators exhibit a giant photothermal nonlinearity, yielding 90% reversible and repeatable modulation from linear scattering response at low excitation intensities. The equivalent nonlinear index is five-orders larger compared with bulk, based on Mie resonance enhanced absorption and high-efficiency heating in thermally isolated nanostructures. Furthermore, the nanoscale thermal relaxation time reaches nanosecond. This large and fast nonlinearity leads to potential applications for GHz all-optical control at the nanoscale and super-resolution imaging of silicon.

Modulating Charge Separation with Hexagonal Boron Nitride Mediation in Vertical Van der Waals Heterostructures.

Tuning the optical and electrical properties by stacking different layers of two-dimensional (2D) materials enables us to create unusual physical phenomena. Here, we demonstrate an alternative approach to enhance charge separation and alter physical properties in van der Waals heterojunctions with type-II band alignment by using thin dielectric spacers. To illustrate our working principle, we implement a hexagonal boron nitride (h-BN) sieve layer in between an InSe/GeS heterojunction. The optical transitions at the junctions studied by photoluminescence and the ultrafast pump-probe technique show quenching of emission without h-BN layers exhibiting an indirect recombination process. This quenching effect due to strong interlayer coupling was confirmed with Raman spectroscopic studies. In contrast, h-BN layers in between InSe and GeS show strong enhancement in emission, giving another degree of freedom to tune the heterojunction property. The two-terminal photoresponse study supports the argument by showing a large photocurrent density for an InSe/h-BN/GeS device by avoiding interlayer charge recombination. The enhanced charge separation with h-BN mediation manifests a photoresponsivity and detectivity of 9 × 102 A W-1 and 3.4 × 1014 Jones, respectively. Moreover, a photogain of 1.7 × 103 shows a high detection of electrons for the incident photons. Interestingly, the photovoltaic short-circuit current is switched from positive to negative, whereas the open-circuit voltage changes from negative to positive. Our proposed enhancement of charge separation with 2D-insulator mediation, therefore, provides a useful route to manipulate the physical properties of heterostructures and for the future development of high-performance optoelectronic devices.

Self-Sufficient and Highly Efficient Gold Sandwich Upconversion Nanocomposite Lasers for Stretchable and Bio-applications.

Multifunctional lanthanide-doped upconversion nanoparticles (UCNPs) have spread their wings in the fields of flexible optoelectronics and biomedical applications. One of the ongoing challenges lies in achieving UCNP-based nanocomposites, which enable a continuous-wave (CW) laser action at ultralow thresholds. Here, gold sandwich UCNP nanocomposites [gold (Au1)-UCNP-gold (Au2)] capable of exhibiting lasing at ultralow thresholds under CW excitation are demonstrated. The metastable energy-level characteristics of lanthanides are advantageous for creating population inversion. In particular, localized surface plasmon resonance-based electromagnetic hotspots in the nanocomposites and the huge enhancement of scattering coefficient for the formation of coherent closed loops due to multiple scattering facilitate the process of stimulated emissions as confirmed by theoretical simulations. The nanocomposites are subjected to stretchable systems for enhancing the lasing action (threshold ∼ 0.06 kW cm-2) via a light-trapping effect. The applications in bioimaging of HeLa cells and antibacterial activity (photothermal therapy) are demonstrated using the newly designed Au1-UCNP-Au2 nanocomposites.

Sn-Doping Enhanced Ultrahigh Mobility In1-xSnxSe Phototransistor.

Two-dimensional ternary materials are attracting widespread interest because of the additional degree of freedom available to tailor the material property for a specific application. An In1-xSnxSe phototransistor possessing tunable ultrahigh mobility by Sn-doping engineering is demonstrated in this study. A striking feature of In1-xSnxSe flakes is the reduction in the oxide phase compared to undoped InSe, which is validated by spectroscopic analyses. Moreover, first-principles density functional calculations performed for the In1-xSnxSe crystal system reveal the same effective mass when doped with Sn atoms. Hence, because of an increased lifetime owing to the enhanced crystal quality, the carriers in In1-xSnxSe have higher mobility than in InSe. The internally boosted electrical properties of In1-xSnxSe exhibit ultrahigh mobility of 2560 ± 240 cm2 V-1 s-1 by suppressing the interfacial traps with substrate modification and channel encapsulation. As a phototransistor, the ultrathin In1-xSnxSe flakes are highly sensitive with a detectivity of 1014 Jones. It possesses a large photoresponsivity and photogain (Vg = 40 V) as high as 3 × 105 A W-1 and 0.5 × 106, respectively. The obtained results outperform all previously reported performances of InSe-based devices. Thus, the doping-engineered In1-xSnxSe-layered semiconductor finds a potential application in optoelectronics and meets the demand for faster electronic technology.

Gold coated Cicada wings: Anti-reflective micro-environment for plasmonic enhancement of fluorescence from upconversion nanoparticles.

We demonstrate that the upconversion nanoparticles (UCNPs) fluoresce 50 times more on a gold (Au) coated Cicada wing. UCNPs are attractive bioimaging, and therapeutic materials as it is excited in the infrared, limited only by the low fluorescence quantum yield. Here, a plasmonic effect, coupled with an anti-reflecting (AR) Cicada wing substrate coated with Au is demonstrated to enhance the fluorescence of the UCNPs. Silica (SiO2) coated Erbium doped green emitting core-shell UCNPs (NaYF4: Yb3+, Er3+@SiO2) show conventional metal enhanced fluorescence. The AR property of the Cicada wing (R ~0.2% @ 1000 nm) contributes >6-fold enhancement as compared to flat (silicon, and quartz) substrates (R~10-30% @ 1000 nm). Upon plasmon coupling, with an optimally sputtered Au coating, an unprecedented enhancement of >50-fold for the 520, and 655 nm emission was obtained on the Au coated Cicada wings, vis-à-vis planar uncoated (silicon, and quartz) substrates. The enhancement was also confirmed by direct fluorescence imaging of the photonic substrates used. The fluorescence lifetime of the core, and the core-shell UCNPs (~300 µs) decreased by ~30-40%, and 10-30%, respectively, when placed on Au coated substrates.

Optically coupled engineered upconversion nanoparticles and graphene for a high responsivity broadband photodetector.

A hybrid upconversion nanoparticle (UCNP)-graphene composite is demonstrated as a high-sensitivity and high-gain photodetector. The 980 nm multiphoton absorbing UCNPs are used as the photoabsorber, and optimized graphene is used as an efficient charge transporter. Although this device class is in its infancy, we show how critical engineering of the UCNPs, with a silica (SiO2) shell, helps to couple it optically with graphene to get a superior device. This initial report of UCNP-graphene optical coupling is expressed as fluorescence enhancement/quenching of the former in the presence of the latter. While the published literature relies mostly on fluorescence quenching in the UCNPs, our devices use both fluorescence quenching (using core UCNPs), and enhancement (using UCNP@SiO2) to significantly enhance the detector parameters. For example, the photoresponsivity of the core-UCNP device was ∼1.52 × 104 A W-1 which could be improved to ∼2.7 × 104 A W-1 (at 980 nm, power density of ∼31.84 µW cm-2, and under a 1.0 V bias) with the UCNP@SiO2 device. The responsivity, gain, and detectivity thus obtained are the highest reported so far for this class of composite photodetectors. The device could detect signals from domestic hand-held appliances such as laser pointers, cellphone flashlights, and air-conditioning remotes. This work will further the knowledge of device photophysics in this class of hybrids.

A Highly-Efficient Single Segment White Random Laser.

Production of multicolor or multiple wavelength lasers over the full visible-color spectrum from a single chip device has widespread applications, such as superbright solid-state lighting, color laser displays, light-based version of Wi-Fi (Li-Fi), and bioimaging, etc. However, designing such lasing devices remains a challenging issue owing to the material requirements for producing multicolor emissions and sophisticated design for producing laser action. Here we demonstrate a simple design and highly efficient single segment white random laser based on solution-processed NaYF4:Yb/Er/Tm@NaYF4:Eu core-shell nanoparticles assisted by Au/MoO3 multilayer hyperbolic meta-materials. The multicolor lasing emitted from core-shell nanoparticles covering the red, green, and blue, simultaneously, can be greatly enhanced by the high photonic density of states with a suitable design of hyperbolic meta-materials, which enables decreasing the energy consumption of photon propagation. As a result, the energy upconversion emission is enhanced by ∼50 times with a drastic reduction of the lasing threshold. The multiple scatterings arising from the inherent nature of the disordered nanoparticle matrix provide a convenient way for the formation of closed feedback loops, which is beneficial for the coherent laser action. The experimental results were supported by the electromagnetic simulations derived from the finite-difference time-domain (FDTD) method. The approach shown here can greatly simplify the design of laser structures with color-tunable emissions, which can be extended to many other material systems. Together with the characteristics of angle free laser action, our device provides a promising solution toward the realization of many laser-based practical applications.

Carrier dynamics of Mn-induced states in GaN thin films.

GaN-based materials are widely used for light emission devices, but the intrinsic property of wide bandgap makes it improper for photovoltaic applications. Recently, manganese was doped into GaN for absorption of visible light, and the conversion efficiency of GaN-based solar cells has been greatly improved. We conducted transient optical measurements to study the carrier dynamics of Mn-doped GaN. The lifetime of carriers in the Mn-related intermediate bands (at 1.5 eV above the valence band edge) is around 1.7 ns. The carrier relaxation within the Mn-induced bandtail states was on the order of a few hundred picoseconds. The relaxation times of different states are important parameters for optimization of conversion efficiency for intermediate-band solar cells.

THz Acoustic Spectroscopy by using Double Quantum Wells and Ultrafast Optical Spectroscopy.

GaN is a pivotal material for acoustic transducers and acoustic spectroscopy in the THz regime, but its THz phonon properties have not been experimentally and comprehensively studied. In this report, we demonstrate how to use double quantum wells as a THz acoustic transducer for measuring generated acoustic phonons and deriving a broadband acoustic spectrum with continuous frequencies. We experimentally investigated the sub-THz frequency dependence of acoustic attenuation (i.e., phonon mean-free paths) in GaN, in addition to its physical origins such as anharmonic scattering, defect scattering, and boundary scattering. A new upper limit of attenuation caused by anharmonic scattering, which is lower than previously reported values, was obtained. Our results should be noteworthy for THz acoustic spectroscopy and for gaining a fundamental understanding of heat conduction.

Ultrafast dynamics of quasiparticles and coherent acoustic phonons in slightly underdoped (BaK)Fe2As2.

We have utilized ultrafast optical spectroscopy to study carrier dynamics in slightly underdoped (BaK)Fe2As2 crystals without magnetic transition. The photoelastic signals due to coherent acoustic phonons have been quantitatively investigated. According to our temperature-dependent results, we found that the relaxation component of superconducting quasiparticles persisted from the superconducting state up to at least 70 K in the normal state. Our findings suggest that the pseudogaplike feature in the normal state is possibly the precursor of superconductivity. We also highlight that the pseudogap feature of K-doped BaFe2As2 is different from that of other iron-based superconductors, including Co-doped or P-doped BaFe2As2.

Ultrasmall all-optical plasmonic switch and its application to superresolution imaging.

Because of their exceptional local-field enhancement and ultrasmall mode volume, plasmonic components can integrate photonics and electronics at nanoscale, and active control of plasmons is the key. However, all-optical modulation of plasmonic response with nanometer mode volume and unity modulation depth is still lacking. Here we show that scattering from a plasmonic nanoparticle, whose volume is smaller than 0.001 µm(3), can be optically switched off with less than 100 µW power. Over 80% modulation depth is observed, and shows no degradation after repetitive switching. The spectral bandwidth approaches 100 nm. The underlying mechanism is suggested to be photothermal effects, and the effective single-particle nonlinearity reaches nearly 10(-9) m(2)/W, which is to our knowledge the largest record of metallic materials to date. As a novel application, the non-bleaching and unlimitedly switchable scattering is used to enhance optical resolution to λ/5 (λ/9 after deconvolution), with 100-fold less intensity requirement compared to similar superresolution techniques. Our work not only opens up a new field of ultrasmall all-optical control based on scattering from a single nanoparticle, but also facilitates superresolution imaging for long-term observation.

Tunable and stable UV-NIR photoluminescence from annealed SiOx with Si nanoparticles.

We demonstrate stable and tunable light emission in ultraviolet to near infrared regime by using annealed SiOx sample. By adjusting the ratio of Si and O of SiOx, different wavelengths such as ultraviolet, visible and near infrared photoluminescence can be tuned. From the results of transmission electron microscope, various sizes (1~4 nm) of the embedded Si nanoparticles were formed. Nanoparticles with smaller sizes were indeed formed for UV-blue emitting samples and the origin of light emission may be misattributed to the quantum confinement effects. However, we found the efficient and stable light emission in UV-blue regime, with lifetime on the order of nanoseconds, is dominantly from the defects.