Asynchronous wide-field transient absorption microscopy.

We have developed a new, to the best of our knowledge, femtosecond laser spatiotemporal imaging technique, named asynchronous wide-field transient absorption microscopy (AWTAM), which does not require phase synchronization between an optical chopper and a complementary metal-oxide-semiconductor (CMOS) camera. By presenting a theoretical scheme, an image reconstruction algorithm, and experimentally imaging the photocarrier diffusion process in a 2D layered semiconductor, our technique has been comprehensively demonstrated. Our technique is widely applicable for fundamental photo-physical research and industrial applications, with the advantages of lower hardware cost as well as higher imaging speed.

Spatiotemporal evolution of ultrafast photocarrier dynamics across WS2-ReS2 lateral interface.

2D lateral heterostructures possess atomically sharp lateral interfaces, while understanding of their ultrafast photocarrier dynamics from a spatiotemporal viewpoint is rather elusive. In this study, we have investigated the spatiotemporal evolution of photocarrier dynamics across the 1D lateral interface of a WS2-ReS2 2D lateral heterostructure utilizing femtosecond laser pump-probe. The nontrivial band offset across the 1D lateral interface markedly mediates the spatiotemporal photocarrier transfer and transport processes. Subsequently, a hole accumulation region on the WS2 side and an electron accumulation region (1DEG) on the ReS2 side have been spatially identified by correlating ultrafast photocarrier signals. The measured width of the unilateral depletion region is 1360 ± 160 nm. Our work has provided substantial insights into mediated photocarrier dynamics in the 2D lateral heterostructure, which will benefit explorations in 2D interfacial physics and 2D lateral optoelectronic devices.

Thickness-dependent ultrafast charge-carrier dynamics and coherent acoustic phonon oscillations in mechanically exfoliated PdSe2 flakes.

Recently, palladium diselenide (PdSe2) has emerged as a promising material with potential applications in electronic and optoelectronic devices due to its intriguing electronic and optical properties. The performance of the device is strongly dependent on the charge-carrier dynamics and the related hot phonon behavior. Here, we investigate the photoexcited-carrier dynamics and coherent acoustic phonon (CAP) oscillations in mechanically exfoliated PdSe2 flakes with a thickness ranging from 10.6 nm to 54 nm using time-resolved non-degenerate pump-probe transient reflection (TR) spectroscopy. The results imply that the CAP frequency is thickness-dependent. Polarization-resolved transient reflection (PRTR) measurements reveal the isotropic charge-carrier relaxation dynamics and the CAP frequency in the 10.6 nm region. In addition, the deformation potential (DP) mechanism dominates the generation of the CAP. Moreover, a sound velocity of 6.78 × 103 m s-1 is extracted from the variation of the oscillation period with the flake thickness and the delay time of the acoustic echo. These results provide insight into the ultrafast optical coherent acoustic phonon and optoelectronic properties of PdSe2 and may open new possibilities for PdSe2 applications in THz-frequency mechanical resonators.

Plasmon-coupled microcavity aptasensors for visual and ultra-sensitive simultaneous detection of Staphylococcus aureus and Escherichia coli.

Septicemia and bacteremia are serious infections in the bloodstream. Thus, time-saving and ultra-sensitive pathogenic bacteria detection is highly required. Herein, we constructed gold nanoparticle-modified polystyrene microspheres (Au/PS) as plasmon-coupled microcavities to realize simultaneous detection of Staphylococcus aureus and Escherichia coli based on a fluorescence and surface-enhanced Raman spectroscopy (SERS) dual-mode method. Fluorescence imaging, serving as a means for assistant validation and rapid screening, was carried out to achieve qualitative and semi-quantitative determination, which gave us visual information of the existence and distribution of the target bacteria. Meanwhile, SERS test was conducted to realize ultra-sensitive quantitative detection. The evanescent wave aroused from total internal reflection in PS microcavities coupled with the localized electromagnetic field from surface plasmons of gold nanoparticles to improve light-matter interaction synergistically, leading to an enhancement factor of 2.25 × 1011 for SERS sensing. The whole measurement was carried out in a typical sandwich assay of "capture probe-target bacteria-signal probe." As a result, calibrated concentration response curves demonstrated the sensitive quantitative detection with the limit of detection (LOD) of 3 cfu/mL for S. aureus and 2 cfu/mL for E. coli. This rapid, ultra-sensitive, and visual sensing method was further developed for dual-bacteria detection in the whole blood samples.

Ultrafast Interlayer Electron Transfer in Incommensurate Transition Metal Dichalcogenide Homobilayers.

Two-dimensional materials, such as graphene, transition metal dichalcogenides, and phosphorene, can be used to construct van der Waals multilayer structures. This approach has shown potentials to produce new materials that combine novel properties of the participating individual layers. One key requirement for effectively harnessing emergent properties of these materials is electronic connection of the involved atomic layers through efficient interlayer charge or energy transfer. Recently, ultrafast charge transfer on a time scale shorter than 100 fs has been observed in several van der Waals bilayer heterostructures formed by two different materials. However, information on the transfer between two atomic layers of the same type is rare. Because these homobilayers are essential elements in constructing multilayer structures with desired optoelectronic properties, efficient interlayer transfer is highly desired. Here we show that electron transfer between two monolayers of MoSe2 occurs on a picosecond time scale. Even faster transfer was observed in homobilayers of WS2 and WSe2. The samples were fabricated by manually stacking two exfoliated monolayer flakes. By adding a graphene layer as a fast carrier recombination channel for one of the two monolayers, the transfer of the photoexcited carriers from the populated to the drained monolayers was time-resolved by femtosecond transient absorption measurements. The observed efficient interlayer carrier transfer indicates that such homobilayers can be used in van der Waals multilayers to enhance their optical absorption without significantly compromising the interlayer transport performance. Our results also provide valuable information for understanding interlayer charge transfer in heterostructures.

Transient Absorption Measurements on Anisotropic Monolayer ReS2.

Anisotropic optical and transport properties of monolayer ReS2 fabricated by mechanical exfoliation are reported. Transient absorption measurements with different polarization configurations and sample orientations reveal that the absorption coefficient and transient absorption are both anisotropic, with maximal and minimal values occurring when the light polarization is parallel and perpendicular to the Re atomic chains, respectively. The maximal values are about a factor of 2.5 of the minimal values. By resolving the spatiotemporal dynamics of excitons, it is found that the diffusion coefficient of excitons moving along Re atomic chains is about 16 cm(2) s(-1) at room temperature, which is about a factor of three larger than those moving perpendicular to that direction. An exciton lifetime of 40 ps is also extracted. These findings establish monolayer ReS2 as an anisotropic 2D transition metal dichalcogenide.

All-optical switching based on spatial self-phase modulation of Ag/violet phosphorus heterojunctions.

With the increasing demand for high-performance passive nonlinear photonic devices, significant progress has been made in spatial self-phase modulation (SSPM) based on 2D nanomaterials in all-optical switches, logic gates, and information converters in recent years. However, there are still challenges in improving the responsiveness of photonic devices. In this work, we prepared a heterojunction of Ag nanoparticles deposited on the surface of violet phosphorus nanosheets (VP Ns), investigated their SSPM, and demonstrated their performance in all-optical switches. The SSPM experimental results show that compared with pure VP Ns at the same light intensity, both the maximum number and the formation time of self-diffraction rings in Ag/VP heterojunctions increase, and the nonlinear refractive index is approximately doubled. The main reason for optical nonlinearity enhancement is that the internal electric field in the heterojunction strengthens the mobility of the photogenerated carrier, thereby enhancing its optical nonlinearity. In particular, we demonstrate the performance of all-optical switches based on SSPM by utilizing the superior optical nonlinearity of Ag/VP heterojunctions. It is shown that with the increase of low-dose Ag content in heterojunctions, the switching time in the all-optical switch becomes shorter and the maximum number of self-diffraction rings of the signal light increases, although the quality of self-diffraction rings slightly decreases due to the scattering of Ag particles. The results contribute to the design and implementation of high-performance nonlinear photonic devices, based on the use of heterojunctions with low-cost preparation and a high nonlinear refractive index.

Strong anisotropic third-harmonic generation in layered violet phosphorus.

We demonstrate that layered violet phosphorus, an emerging 2D semiconductor, undergoes strong anisotropic third-harmonic generation (THG). Polarization dependence of in-plane THG presents a cruciate-flower-shaped curve. Through theoretical modeling of the in-plane THG response, done by considering crystalline symmetry of violet phosphorus, we successfully quantify four non-zero third-order nonlinear optical susceptibility tensor elements. From control experiments, the magnitude of third-order nonlinear optical susceptibility |χ3| is calculated to be about 4.0 × 10-19 m2 V-2, which is comparable to those of conventional 2D layered semiconductors. These results indicate that the layered violet phosphorus can serve as an ideal building block for nonlinear optical applications.

Spatial transcriptomic profiling of isolated microregions in tissue sections utilizing laser-induced forward transfer.

Profiling gene expression while preserving cell locations aids in the comprehensive understanding of cell fates in multicellular organisms. However, simple and flexible isolation of microregions of interest (mROIs) for spatial transcriptomics is still challenging. We present a laser-induced forward transfer (LIFT)-based method combined with a full-length mRNA-sequencing protocol (LIFT-seq) for profiling region-specific tissues. LIFT-seq demonstrated that mROIs from two adjacent sections could reliably and sensitively detect and display gene expression. In addition, LIFT-seq can identify region-specific mROIs in the mouse cortex and hippocampus. Finally, LIFT-seq identified marker genes in different layers of the cortex with very similar expression patterns. These genes were then validated using in situ hybridization (ISH) results. Therefore, LIFT-seq will be a valuable and efficient technique for profiling the spatial transcriptome in various tissues.

A 3D Biocompatible Plasmonic Tweezer for Single Cell Manipulation.

Plasmonic tweezers are an emerging research topic because of their low input power and wide operating range from homogeneous particles to complex biological objects. But it is still challenging for plasmonic tweezers to trap or manipulate objects of tens of microns, especially in biological science. This study introduces a new 3D biocompatible plasmonic tweezer for single living cell manipulation in solution. The key design is a tapered tip whose three-layer surface structure consists of nanoprobe, gold nanofilm, and thermosensitive hydrogel, thiolated poly(N-isopropylacrylamide). Incident light excites the surface plasmon polaritons on gold film and generates heat to induce thermally driven phase transition of the thermosensitive hydrogel, which enables reversible binding between functionalized surface and cell membrane and avoids both thermal and mechanical stresses in the meanwhile. The 3D biocompatible plasmonic tweezer realizes selective capture, 3D pathway free transport, and position-controlled release of target cells, and it displays excellent biocompatibility, low energy consumption, and high operational flexibility.

Camouflaged Nanoreactors Mediated Radiotherapy-Adjuvant Chemodynamic Synergistic Therapy.

Chemodynamic therapy based on the Fenton-like catalysis ability of Fe3O4 has the advantages of no involvement of chemical drugs and minimal adverse effects as well as the limitation of depletable efficacy. Radiotherapy based on high-energy radiation offers the convenience of treatment and cost-effectiveness but lacks precision and cellular adaptation of tumor cells. Approaching such dilemmas from a nanoscale materials perspective, we aim to bridge the weaknesses of both treatment methods by combining the principles of two therapeutics reciprocally. We have designed a camouflaged Fe3O4@HfO2 composite nanoreactor (FHCM), which combines a chemodynamic therapeutic agent Fe3O4 and a radiosensitizer HfO2 that both has passed clinical trials and was inspired by a cell membrane biomimetic technique. FHCM is employed as conceived radiotherapy-adjuvant chemodynamic synergistic therapy of malignant tumors, which has undergone dual scrutiny from both the physical and biological aspects. Experimental results obtained at different levels, including theory, material characterizations, and in vitro and in vivo verifications, suggest that FHCM effectively impaired tumor cells through physical and molecular biological mechanisms involving a HfO2-Fe3O4 photoelectron-electron transfer chain and DNA damage-ferroptosis-immunity chain. It is worth noting that compared to single therapies such as only chemodynamic therapy or radiotherapy, FHCM-mediated radiotherapy-adjuvant chemodynamic synergistic therapy exhibits stronger tumor inhibition efficacy. It significantly addresses the inherent limitations of chemodynamic therapy and radiotherapy and underscores the feasibility and importance of using existing clinical weapons, such as radiotherapy, as auxiliary strategies to overcome certain flaws of emerging antitumor therapeutics like chemodynamic therapy.

Hydrophilic polypyrrole and g-C3N4 co-decorated ZnO nanorod arrays for stable and efficient photoelectrochemical water splitting.

It is of practical significance to manufacture high-performance and durable semiconductor heterojunctions for photoelectrochemical (PEC) water splitting. Herein, hydrophilic polypyrrole and graphitic carbon nitride (g-C3N4) co-decorated ZnO nanorod arrays were synthesized as a photoanode by facile spin-coating and plasma-treatment methods. On the one hand, g-C3N4 nanosheets are modified on ZnO nanorod arrays to broaden the light-absorption range and suppress the recombination of photogenerated charges. On the other hand, the polypyrrole coating layer inhibits the dissolution and corrosion of ZnO nanorods and constructs a p-n heterojunction with ZnO to further promote the separation and transfer of photogenerated charge carriers. Furthermore, its hydrophilic surface provides a vast electrochemically active surface area for efficient charge/mass transfer. As a result, the as-prepared photoanode exhibits an enhanced PEC performance with a distinctly increased photocurrent and remarkably ameliorated stability in contrast to the ZnO photoanode. This research would provide an innovative perspective on the design of organic/inorganic semiconductor heterojunctions with excellent performance and stability for PEC water-splitting systems.

Label-Free Sensing of Biomolecular Adsorption and Desorption Dynamics by Interfacial Second Harmonic Generation.

Observing interfacial molecular adsorption and desorption dynamics in a label-free manner is fundamentally important for understanding spatiotemporal transports of matter and energy across interfaces. Here, we report a label-free real-time sensing technique utilizing strong optical second harmonic generation of monolayer 2D semiconductors. BSA molecule adsorption and desorption dynamics on the surface of monolayer MoS2 in liquid environments have been all-optically observed through time-resolved second harmonic generation (SHG) measurements. The proposed SHG detection scheme is not only interface specific but also expected to be widely applicable, which, in principle, undertakes a nanometer-scale spatial resolution across interfaces.

Time-Resolved Observation of Hole Tunneling in van der Waals Multilayer Heterostructures.

We reported a time-resolved study of quantum-mechanical tunneling of holes between two MoSe2 monolayers that are separated by a monolayer WS2 energy barrier. Four-layer heterostructures of MoSe2/WS2/MoSe2/graphene, as well as control samples, were fabricated by mechanical exfoliation and dry transfer techniques. To time-resolve the hole tunneling process, an ultrashort laser pulse was used to excite electrons and holes in both MoSe2 layers. By utilization of the graphene layer to eliminate carriers in the third MoSe2 layer, the first MoSe2 layer is selectively populated with the holes, which then tunnel to the third MoSe2 layer. By monitoring decay of the hole population with an ultrashort probe pulse, we measure a hole tunneling time of about 20 ps, which is found to slightly increase with the injected carrier density. Besides the fundamental interests of real-time observation of the quantum-mechanical tunneling effect across a nanometer barrier, these results provide quantitative understanding on tunneling mechanisms of charge transfer in van der Waals heterostructures, which is useful for designing sophisticated van der Waals multilayer heterostructures.

Inhomogeneous Trap-State-Mediated Ultrafast Photocarrier Dynamics in CsPbBr3 Microplates.

Quantitatively elucidating photocarrier dynamics mediated by trap states in perovskites is crucial for establishing a structure-performance relation and understanding the interfacial photocarrier transport mechanism. Here, trap-state-mediated photocarrier dynamics in defect-rich CsPbBr3 microplates are noninvasively investigated by ultrafast laser spectroscopy. Time-resolved photoluminescense (TRPL) measurements as a function of sample thickness indicate that trap densities of surface and bulk regions are inhomogeneous, leading to fast and slow decay components of TRPL, respectively. Fast and slow PL lifetimes present the same decreasing trend as the thickness is decreased from 5 to 0.1 µm, suggesting that both surface and bulk trap densities dramatically increase in sub-micrometer thick microplates. Furthermore, dynamical competition of ultrafast photocarrier energy relaxations between surface and bulk regions is studied in a 1.6 µm-thick sample by temporally correlating pump fluence-dependent TRPL with transient absorption signals. Strikingly, long-lived hot carriers (20 ps) are observed and complete filling of mid-gap trap states in the surface region can markedly enhance PL emission in the bulk region. By control measurements, we attribute these anomalous phenomena to the polaron-assisted ultrafast energy transfer process across the surface-bulk interface. Our results provide new insights into dynamical photocarrier energy relaxations and interfacial energy transport for inorganic perovskites.

Plasmon-exciton coupling dynamics and plasmonic lasing in a core-shell nanocavity.

Plasmonic nanolasers based on the spatial localization of surface plasmons (SPs) have attracted considerable interest in nanophotonics, particularly in the desired application of optoelectronic and photonic integration, even breaking the diffraction limit. Effectively confining the mode field is still a basic, critical and challenging approach to improve optical gain and reduce loss for achieving high performance of a nanolaser. Here, we designed and fabricated a semiconductor/metal (ZnO/Al) core-shell nanocavity without an insulator spacer by simple magnetron sputtering. Both theoretical and experimental investigations presented plasmonic lasing behavior and SP-exciton coupling dynamics. The simulation demonstrated the three-dimensional optical confinement of the light field in the core-shell nanocavity, while the experiments revealed a lower threshold of the optimized ZnO/Al core-shell nanolaser than the same-sized ZnO photonic nanolaser. More importantly, the blue shift of the lasing mode demonstrated the SP-exciton coupling in the ZnO/Al core-shell nanolaser, which was also confirmed by low-temperature photoluminescence (PL) spectra. The analysis of the Purcell factor and PL decay time revealed that SP-exciton coupling accelerated the exciton recombination rate and enhanced the conversion of spontaneous radiation into stimulated radiation. The results indicate an approach to design a real nanolaser for promising applications.

CdS quantum dots/Au nanoparticles/ZnO nanowire array for self-powered photoelectrochemical detection of Escherichia coli O157:H7.

In this paper, the hydrothermally grown ZnO nanowire array (NWs) was modified by Au nanoparticles (NPs) and CdS quantum dots (QDs) to construct a high-performance photoelectrochemical (PEC) electrode. The aligned ZnO NWs, which decorated Au NPs and CdS QDs have the effective light absorption range from UV to visible region. This hybrid structure provided a self-powered PEC electrode with a favorable energy-band configuration for fast charge separation and transportation. Meanwhile, the Au NPs and CdS QDs also made increase of the surface area to improve the immobilization of the analytes. After assembling aptamer as recognition element, this composite nanoarray was further developed as a self-powered PEC biosensor by synergizing above multiple enhancement factors. The PEC aptasensor exhibited a rapid response in a wide linear range of 10-107 CFU/mL with the detection limit as low as 1.125 CFU/mL to Escherichia coli O157:H7 (E. coli O157:H7). This approach would offer an alternative PEC transduction for fast environment monitoring and clinical diagnosis related to pathogenic bacteria.

Whispering-Gallery Mode Lasing in a Floating GaN Microdisk with a Vertical Slit.

Controlling the lasing mode, emission direction, threshold, and quality factor of whispering-gallery mode lasing is important for practical applications such as optical interconnections, on-chip communications, trace detection, high-density storage, etc. In order to simultaneously control the mode and emission direction and to achieve a high-quality factor in a low-threshold whisper-gallery mode laser, such as a GaN floating microdisk, a novel fabrication design of a microdisk with a vertical slit is proposed. To demonstrate proof of concept, we experimentally measure whispering-gallery mode lasing spectra of microdisks with and without a slit. Our findings suggest that the disks can indeed operate in whispering-gallery mode, and the slit is able to change the optical path in the microcavity without breaking lasing resonance. The slit in the microdisk can also influence the lasing mode, quality factor, and directional emission. Therefore, our study provides a feasible way to control whispering-gallery mode lasing properties.

Full-Spectrum Analysis of Perovskite-Based Surface Plasmon Nanolasers.

We systematically studied the characteristics of hybrid perovskite-based surface plasmon nanolasers. If one changes the anion composition of perovskites, the emission wavelength can be easily tuned. We conducted in full-spectrum modeling that featured hybrid perovskite nanowires placed on different SiO2-coated metallic (Au, Ag, and Al) plates. The proposed nanocavities that supported plasmonic gap modes exhibited distinguished properties of nanolasers, such as low-transparency threshold-gain and low lasing threshold. The corresponding experimental results for the MAPbBr3 nanolaser on Ag revealed the low-threshold operation. These superior features were attributed to enhanced light-matter interaction with strong coupling. Therefore, the proposed scheme, integrated with hybrid perovskite as gain material, provides an excellent platform for nanoscale plasmon lasing in the visible to near-infrared spectra.

Bilinear Staphylococcus aureus detection based on suspension immunoassay.

A novelty bilinear suspension immunoassay biosensor is developed for Staphylococcus aureus specific detection. In the present study, a dual-color-based sandwich immunosensor was constructed for sensitive and selective detection of this bacterium. In this bioassay system, the monoclonal antibodies of Staphylococcus aureus were immobilized on carboxyl-modified fluorescent microspheres (PSA-R6G) which acted as a capture probe. A secondary fluorescein isothiocyanate (FITC)-labelled antibody of Staphylococcus aureus acted as a sensitive reporter antibody. After dual-labelling with R6G and FITC, the enriched Staphylococcus aureus bacteria were observed by using the multiparameter flow cytometry analysis. In this method, two regression equations were obtained with IFITC = 1.56lgC + 4.50 and IR6G = 1.54lgC + 2.78, respectively. It can be noted that the two slopes were very similar, which indicated the false positives decrease significantly. For general applications, the quantificational measurements of Staphylococcus aureus in milk and water samples were also carried out. The suspension immunoassay exhibited an excellent specificity to Staphylococcus aureus in contrast to conventional culture-based method.