Dual-Modal Nanoplasmonic Light Upconversion through Anti-Stokes Photoluminescence and Second-Harmonic Generation from Broadband Multiresonant Metal Nanocavities.

Metal nanocavities can generate plasmon-enhanced light upconversion signals under ultrashort pulse excitations through anti-Stokes photoluminescence (ASPL) or nonlinear harmonic generation processes, offering various applications in bioimaging, sensing, interfacial science, nanothermometry, and integrated photonics. However, achieving broadband multiresonant enhancement of both ASPL and harmonic generation processes within the same metal nanocavities remains challenging, impeding applications based on dual-modal or wavelength-multiplexed operations. Here, we report a combined experimental and theoretical study on dual-modal plasmon-enhanced light upconversion through both ASPL and second-harmonic generation (SHG) from broadband multiresonant metal nanocavities in two-tier Ag/SiO2/Ag nanolaminate plasmonic crystals (NLPCs) that can support multiple hybridized plasmons with high spatial mode overlaps. Our measurements reveal the distinctions and correlations between the plasmon-enhanced ASPL and SHG processes under different modal and ultrashort pulsed laser excitation conditions, including incident fluence, wavelength, and polarization. To analyze the observed effects of the excitation and modal conditions on the ASPL and SHG emissions, we developed a time-domain modeling framework that simultaneously captures the mode coupling-enhancement characteristics, quantum excitation-emission transitions, and hot carrier population statistical mechanics. Notably, ASPL and SHG from the same metal nanocavities exhibit distinct plasmon-enhanced emission behaviors due to the intrinsic differences between the incoherent hot carrier-mediated ASPL sources with temporally evolving energy and spatial distributions and instantaneous SHG emitters. Mechanistic understanding of ASPL and SHG emissions from broadband multiresonant plasmonic nanocavities marks a milestone toward creating multimodal or wavelength-multiplexed upconversion nanoplasmonic devices for bioimaging, sensing, interfacial monitoring, and integrated photonics applications.

Ambient-Air-Stable Lead-Free CsSnI3 Solar Cells with Greater than 7.5% Efficiency.

Black orthorhombic (B-γ) CsSnI3 with reduced biotoxicity and environmental impact and excellent optoelectronic properties is being considered as a promising eco-friendly candidate for high-performing perovskite solar cells (PSCs). A major challenge in a large-scale implementation of CsSnI3 PSCs includes the rapid transformation of Sn2+ to Sn4+ (within a few minutes) under an ambient-air condition. Here, we demonstrate that ambient-air stable B-γ CsSnI3 PSCs can be fabricated by incorporating N,N'-methylenebis(acrylamide) (MBAA) into the perovskite layer and by using poly(3-hexylthiophene) as the hole transporting material. The lone electron pairs of -NH and -CO units of MBAA are designed to form coordination bonding with Sn2+ in the B-γ CsSnI3, resulting in a reduced defect (Sn4+) density and better stability under multiple conditions for the perovskite light absorber. After a modification, the highest power conversion efficiency (PCE) of 7.50% is documented under an ambient-air condition for the unencapsulated CsSnI3-MBAA PSC. Furthermore, the MBAA-modified devices sustain 60.2%, 76.5%, and 58.4% of their initial PCEs after 1440 h of storage in an inert condition, after 120 h of storage in an ambient-air condition, and after 120 h of 1 Sun continuous illumination, respectively.

Nanoscale Texturing and Interfaces in Compositionally Modified Ca3Co4O9 with Enhanced Thermoelectric Performance.

Oxide thermoelectric materials are nontoxic, chemically and thermally stable in oxidizing environments, cost-effective, and comparatively simpler to synthesize. However, thermoelectric oxides exhibit comparatively lower figure of merit (ZT) than that of metallic alloy counterparts. In this study, nanoscale texturing and interface engineering were utilized for enhancing the thermoelectric performance of oxide polycrystalline Ca3Co4O9 materials, which were synthesized using conventional sintering and spark plasma sintering (SPS) techniques. Results demonstrated that nanoscale platelets (having layered structure with nanoscale spacing) and metallic inclusions provide effective scattering of phonons, resulting in lower thermal conductivity and higher ZT. Thermoelectric measurement direction was found to have a significant effect on the magnitude of ZT because of the strong anisotropy in the transport properties induced by the layered nanostructure. The peak ZT value for the Ca2.85Lu0.15Co3.95Ga0.05O9 specimen measured along both perpendicular and parallel directions with respect to the SPS pressure axis is found be 0.16 at 630 °C and 0.04 at 580 °C, respectively. The peak ZT of 0.25 at 670 °C was observed for the spark plasma-sintered Ca2.95Ag0.05Co4O9 sample. The estimated output power of 2.15 W was obtained for the full size model, showing high-temperature thermoelectric applicability of this nanostructured material without significant oxidation.

Optoperforation of single, intact Arabidopsis cells for uptake of extracellular dye-conjugated dextran.

A plant science research goal is to manipulate single cells in an intact organism in order to study their interactions with neighboring cells. Based on a technique previously demonstrated in isolated plant cells, mammalian cells and cyanobacteria, Arabidopsis epidermal cells were optoperforated to allow for uptake of external cascade blue-labeled dextrans. Adverse organelle responses were determined to be minimal and dye retention was demonstrated for at least 72 hours. This technique overcomes the physical challenges presented by the plant cell wall and demonstrates the feasibility of in situ optoperforation.

Near-infrared laser delivery of nanoparticles to developing embryos: a study of efficacy and viability.

Targeted delivery of materials to individual cells remains a challenge in nanoscience and nanomedicine. Near infrared (NIR) laser injection may be a promising alternative to manual injection (where the micropipet diameter limits targeting to small cells) or other laser techniques (such as picosecond green and UV lasers, which can be damaging to cells). However, the efficiency with which NIR pulses can deliver nanoparticles and any adverse effects on living cells needs thorough testing. Toward this end, we have determined the efficacy and toxicity of delivering quantum dots (QDs) into cells of Xenopus laevis embryos by NIR laser injection. Because this model system provides not only living cells but also a developing organism, we were able to assess relatively long-term effects of NIR pulses on embryonic development (through the tadpole stage). We developed parameters for NIR pulses that did not affect embryonic viability or morphology and delivered QDs as effectively as manual injection. Higher intensities of NIR pulses caused permanent damage to the targeted cells, and thus NIR pulses may also prove useful for ablation of specific cells within tissues.

Application of terahertz quantum-cascade lasers to semiconductor cyclotron resonance.

Quantum-cascade lasers operating at 4.7, 3.5, and 2.3 THz have been used to achieve cyclotron resonance in InAs and InSb quantum wells from liquid-helium temperatures to room temperature. This represents one of the first spectroscopic applications of terahertz quantum-cascade lasers. Results show that these compact lasers are convenient and reliable sources with adequate power and stability for this type of far-infrared magneto-optical study of solids. Their compactness promises interesting future applications in solid-state spectroscopy.