Efficient open-air synthesis of Mg2+-doped CsPbI3 nanocrystals for high-performance red LEDs.

Inorganic CsPbI3 perovskite nanocrystals (NCs) exhibit remarkable optoelectronic properties for illumination. However, their poor stability has hindered the development of light-emitting diodes (LEDs) based on these materials. In this study, we propose a facile method to synthesize Mg2+-doped CsPbI3 NCs with enhanced stability and high photoluminescence (PL) intensity under ambient air conditions. Theoretical calculations confirm that doped NCs possess stronger formation energy compared to undoped NCs. The undoped CsPbI3 NCs emit red light at approximately 653 nm. We optimize the doping ratio to 1/30, which significantly enhances the photoluminescence of single-particle CsPbI3 NCs. Subsequently, we fabricate a red LED by combining the CsPbI3 NCs with a blue chip. The resulting LED, based on the doped CsPbI3 NCs, exhibits excellent performance with a high luminance of 4902.22 cd m-2 and stable color coordinates of (0.7, 0.27). This work not only presents a simple process for synthesizing perovskite NCs but also provides a design strategy for developing novel red LEDs for various applications.

Multiplexed immunosensing of cancer biomarkers on a split-float-gate graphene transistor microfluidic biochip.

This work reports the development of a novel microfluidic biosensor using a graphene field-effect transistor (GFET) design for the parallel label-free analysis of multiple biomarkers. Overcoming the persistent challenge of constructing µm2-sized FET sensitive interfaces that incorporate multiple receptors, we implement a split-float-gate structure that enables the manipulation of multiplexed biochemical functionalization using microfluidic channels. Immunoaffinity biosensing experiments are conducted using the mixture samples containing three liver cancer biomarkers, carcinoembryonic antigen (CEA), α-fetoprotein (AFP), and parathyroid hormone (PTH). The results demonstrate the capability of our label-free biochip to quantitatively detect multiple target biomarkers simultaneously by observing the kinetics in 10 minutes, with the detection limit levels in the nanomolar range. This microfluidic biosensor provides a valuable analytical tool for rapid multi-target biosensing, which can be potentially utilized for domiciliary tests of cancer screening and prognosis, obviating the need for sophisticated instruments and professional operations in hospitals.

Nonlocal Optical Response of Particle Plasmons in Single Gold Nanorods.

The investigation of particle plasmons in metal nanoparticles has predominantly relied on local optical response approximations. However, as the nanoparticle size approaches the average distance of electrons to the metal surface, mesoscopic effects such as size-dependent plasmon line width broadening and resonance energy blue shifts are expected to become observable. In this work, we compared the experimental spectral characteristics with simulated values obtained by using a generalized nonlocal optical response theory-based local analogue model. Our results show that the nonlocal plasmon damping effects in single nanoparticles are less pronounced than those observed in plasmon-coupled systems. Furthermore, our research demonstrates that single-particle dark-field spectroscopy is an effective tool for investigating the nonlocal optical response of particle plasmons in single nanoparticles. These results have important implications for the rational design of novel nanophotonic devices.

Multiple solution solving in plasmon sensing by deep learning: determination of layer refractive index and thickness in one experiment: comment.

In a recent Letter [Opt. Lett.46, 5667 (2021)10.1364/OL.444442], Du et al. proposed a deep learning method for determining the refractive index (n) and thickness (d) of the surface layer on nanoparticles in a single-particle plasmon sensing experiment. This comment highlights the methodological issues arising in that Letter.

Perivascular epithelioid cell tumors of the liver misdiagnosed as hepatocellular carcinoma: Three case reports.

BACKGROUND: Hepatic perivascular epithelioid cell neoplasms (PEComas) are rare. Diagnostic and treatment experience with hepatic PEComa remains insufficient. CASE SUMMARY: Three hepatic PEComa cases are reported in this paper: One case of primary malignant hepatic PEComa, one case of benign hepatic PEComa, and one case of hepatic PEComa with an ovarian mature cystic teratoma. During preoperative imaging and pathological assessment of intraoperative frozen samples, patients were diagnosed with hepatocellular carcinoma (HCC), while postoperative pathology and immunohistochemistry subsequently revealed hepatic PEComa. Patients with hepatic PEComa which is misdiagnosed as HCC often require a wider surgical resection. It is easy to mistake them for distant metastases of hepatic PEComa and misdiagnosed as HCC, especially when it's combined with tumors in other organs. Three patients eventually underwent partial hepatectomy. After 1-4 years of follow-up, none of the patients experienced recurrence or metastases. CONCLUSION: A clear preoperative diagnosis of hepatic PEComa can reduce the scope of resection and prevent unnecessary injuries during surgery.

Impact of shift work on irritable bowel syndrome and functional dyspepsia: A meta-analysis.

BACKGROUND: The possible association between shift work with irritable bowel syndrome (IBS) and functional dyspepsia (FD) remains controversial. The purpose of the study is to conduct a meta-analysis to explore the potential association between shift work with IBS/FD. METHODS: We searched relevant observational studies on Medline (PubMed) and Embase until June 30, 2021. Two different investigators extracted data and assessed the quality of each study independently. The meta-analysis was used to evaluate the pooled odds risk (OR) between shift work and IBS/FD. RESULTS: Eight studies were included ultimately. Shift workers were more likely to suffer from IBS. The OR of shift work was 1.81 (95% confidence interval 1.42; 2.32) with low heterogeneity (P < .05, I2 = 0%) for IBS. However, no evidence of the association was observed between shift work and the risk of FD. The OR of shift work was 0.87 (95% confidence interval 0.62; 1.23) (P > .05) for FD. CONCLUSIONS: There was a positive association between shift work and IBS. The prevalence of IBS was 81% higher among shift workers than among non-shift workers. Shift work was probably a risk factor for IBS. The low heterogeneity supports the reliability of the results. However, there was no significant association between shift work and FD. The strength of the evidence was limited and further prospective cohort studies were needed.

Obeticholic Acid Induces Hepatoxicity Via FXR in the NAFLD Mice.

Objective: Obeticholic acid (OCA), a potent farnesoid X receptor (FXR) agonist, is a promising drug for nonalcoholic fatty liver disease (NAFLD); however, it can cause liver injury, especially at high doses. Here, we investigated the role of FXR in the high-dose OCA-induced hepatoxicity in the condition of the NAFLD mouse model. Methods: Wild-type (WT) mice and FXR-/- mice were administered with over-dose OCA (0.40%) and high-dose OCA (0.16%), in a high-fat diet. RNA-seq on liver samples of mice fed with high-dose OCA was performed to dig out the prominent biological events contributing to hepatic fibrosis. Results: Over-dose OCA induced liver injury and shortened survival in WT mice, but not FXR-/- mice. High-dose OCA caused hepatic stellate cell activation and liver fibrosis in the presence of FXR. Furthermore, high-dose OCA induced cholesterol accumulation in livers via the upregulation of genes involved in cholesterol acquisition and downregulation of genes regulating cholesterol degradation in liver, leading to the production of interleukin -1ß and an FXR-mediated inflammatory response. Conclusion: The high-dose OCA induced FXR-dependent hepatic injury via cholesterol accumulation and interleukin -1ß pathway in the NAFLD mice.

Obeticholic acid inhibits hepatic fatty acid uptake independent of FXR in mouse.

OBJECTIVE: Obeticholic acid (OCA), a farnesoid X receptor (FXR) agonist, is believed to alleviate nonalcoholic fatty liver disease (NAFLD) by decreasing hepatic lipogenesis in an FXR-dependent manner. Here, we revealed a novel mechanism by which OCA improves NAFLD by affecting hepatic long-chain fatty acids (LCFAs) uptake. METHODS: Stably transfected HEK-293 cells expressing fatty acid transport protein 5 (FATP5) were established to examine fatty acid uptake; FXR-/-, human (h) FATP5, and FXR-/-/hFATP5 mouse models were incorporated to explore the effects of OCA on FATP5 ex vivo and in vivo. RESULTS: OCA inhibited hFATP5 (IC50 =0.07 µM) more than murine (m) FATP5 (IC50 =1.04 µM) as measured by LCFAs uptake in FATP5 expressing HEK-293. OCA also inhibited LCFA uptake in primary hepatocytes from hFATP5 mice, FXR-/-/hFATP5 mice more than that from FXR-/- mice, ex vivo. Moreover, OCA inhibited LCFAs uptake by livers in hFATP5 mice and FXR-/-/hFATP5 mice, but not in FXR-/- mice, in vivo. Long-term administration of 0.04% OCA markedly reduced hepatic triglyceride (TG) accumulation in hFATP5 mice and FXR-/-/hFATP5 mice by 63% and 53%, respectively, but not in FXR-/- mice. CONCLUSIONS: OCA ameliorated high-fat diet-induced NAFLD independent of FXR by inhibiting hepatic hFATP5-mediated LCFAs uptake. This suggests that the therapeutic effects of OCA on NAFLD in vivo are mediated by a novel, hFATP5 dependent mechanism.

Steering the Pathway of Plasmon-Enhanced Photoelectrochemical CO2 Reduction by Bridging Si and Au Nanoparticles through a TiO2 Interlayer.

Photoelectrochemical (PEC) conversion of CO2 in an aqueous medium into high-energy fuels is a creative strategy for storing solar energy and closing the anthropogenic carbon cycle. However, the rational design of catalytic architectures to selectively and efficiently produce a target product such as CO has remained a grand challenge. Herein, an efficient and selective Si photocathode for CO production is reported by utilizing a TiO2 interlayer to bridge the Au nanoparticles and n+ p-Si. The TiO2 interlayer can not only effectively protect and passivate Si surface, but can also exhibit outstanding synergies with Au nanoparticles to greatly promote CO2 reduction kinetics for CO production through stabilizing the key reaction intermediates. Specifically, the TiO2 layer and Au nanoparticles work concertedly to enhance the separation of localized surface plasmon resonance generated hot carriers, contributing to the improved activity and selectivity for CO production by utilizing the hot electrons generated in Au nanoparticles during PEC CO2 reduction. The optimized Au/TiO2 /n+ p-Si photocathode exhibits a Faradaic efficiency of 86% and a partial current density of -5.52 mA cm-2 at -0.8 VRHE for CO production, which represent state-of-the-art performance in this field. Such a plasmon-enhanced strategy may pave the way for the development of high-performance PEC photocathodes for energy-efficient CO2 utilization.

Revisiting the plasmon radiation damping of gold nanorods.

Noble metal nanoparticles have been utilized for a vast amount of optical applications. For applications that use metal nanoparticles as nanosensors and for optical labeling, higher radiative efficiency is preferred. To get a deeper knowledge about the radiation damping of noble metal nanoparticles, we used gold nanorods with different geometry factors (aspect ratios) as the model system to study. We investigated theoretically how the radiation damping of a nanorod depends on the material, and shape of the particle. Surprisingly, a simple analytical equation describes radiation damping very accurately and allows the disentanglement of the maximal radiation damping parameter for gold nanorods with resonance energy Eres around 1.81 eV (685 nm). We found very good agreement with theoretical predictions and experimental data obtained by single-particle spectroscopy. Our results and approaches may pave the way for designing and optimizing gold nanostructures with higher optical signal and better sensing performance.

Single-particle spectroscopic investigation on the scattering spectrum of Au@MoS2 core-shell nanosphere heterostructure.

Owing to the uniform shape of the nanospheres, the Au@MoS2 core-shell nanosphere heterostructure enables us to design nano-optoelectronic devices and nanosensors with highly tunable and reproducible optical properties. However, until now, at the single-particle level, there is still uncertainty as to how much the scattering characteristics depend on the particle size and the local environment. In this letter, we performed an in situ single-particle study of the scattering spectrum of the Au@MoS2 core-shell nanosphere heterostructure before and after coating with the MoS2 layer. Single-particle characterization confirms that the classic quasi-static approximation (QSA) theory can be used to predict the scattering spectra of Au@MoS2 core-shell nanoparticles. Moreover, we have found that the A and B-exciton absorption peaks do not rely on the local refractive index change, while the position of the particle plasmon resonances does. Such features can be used as an internal reference for sensing applications against measurement errors, such as defocusing the imaging. Our results show that Au@MoS2 core-shell nanoparticles have the potential to become one of the promising nanosensors in the field of single-particle sensing.

Observing Mesoscopic Nucleic Acid Capacitance Effect and Mismatch Impact via Graphene Transistors.

This work reports a molecular-scale capacitance effect of the double helical nucleic acid duplex structure for the first time. By quantitatively conducting large sample measurements of the electrostatic field effect using a type of high-accuracy graphene transistor biosensor, an unusual charge-transport behavior is observed in which the end-immobilized nucleic acid duplexes can store a part of ionization electrons like molecular capacitors, other than electric conductors. To elucidate this discovery, a cascaded capacitive network model is proposed as a novel equivalent circuit of nucleic acid duplexes, expanding the point-charge approximation model, by which the partial charge-transport observation is reasonably attributed to an electron-redistribution behavior within the capacitive network. Furthermore, it is experimentally confirmed that base-pair mismatches hinder the charge transport in double helical duplexes, and lead to directly identifiable alterations in electrostatic field effects. The bioelectronic principle of mismatch impact is also self-consistently explained by the newly proposed capacitive network model. The mesoscopic nucleic acid capacitance effect may enable a new kind of label-free nucleic acid analysis tool based on electronic transistor devices. The in situ and real-time nucleic acid detections for virus biomarkers, somatic mutations, and genome editing off-target may thus be predictable.

Multiplexed detection of heavy metal ions by single plasmonic nanosensors.

Detection of multiple analytes simultaneously in small liquid samples with high efficiency and precision is highly important to the fields like water quality monitoring. In this letter, we present a multiplexed nanosensors with position-encoded aptamer functionalized gold nanorods for heavy metal ions detection. The individual gold nanorods respond specifically to two different heavy metal ions (Pb2+ and Hg2+) with a spectral shift in the scattering spectrum. We used a home-built spectral imaging dark-field microscope to measure the response of thousands of single plasmonic nanosensors with relatively high time resolution and precision. To explore the performance and limit of detection (LOD) of our nanosensor and setup, we recorded the concentration-dependent response of our position-encoded nanosensors with a series of mixture solutions that contain different concentrations of Hg2+ and Pb2+ ions. The LOD levels of our system are around 5 nM for Pb2+ ions and 1 nM for Hg2+ ions. Our method and results demostrate the nanomolar sensitivity and the potential to detect more different heavy metal ions.

4.9% Au stabilizes Ag in an atomically homogenous bimetallic alloy for anisotropic nanocrystals with enhanced stability under light irradiation.

Instability problems encountered by Ag nanocrystals largely limit their use in practical applications. In AuAg bimetallic alloys, the stability of Ag can be greatly enhanced, whereas doping a high fraction of Au to the alloy usually leads to the loss of the superior properties of Ag and undesirable degradation of the quality factor of the plasmonic resonance. Herein, we provide experimental evidence that the atomically homogenous AuAg alloy nanocrystals with Au fraction as low as 4.9% (at%) possess comparable stability to pure Au, while the superior plasmonic properties of Ag are largely reserved. The study is based on the synthetic strategy developed for the overgrowth on the Au nanorods of atomically homogenous AuAg alloy shells with a tunable Au/Ag ratio but constant size and anisotropic shape. The stability of over 800 individual alloy nanocrystals in the absence of surfactants is simultaneously characterized at the single-particle level for over 10 h under light irradiation. The stability transition is explained in correlation with the charge redistribution of Ag occurring at the same critical Au fraction. We note that such bimetallic alloy nanocrystals with a low Au fraction possessing both high stability and high quality of resonance are preferred in fundamental researches and practical applications.

Warhead Reactivity Limits the Speed of Inhibition of the Cysteine Protease Rhodesain.

Viral and parasitic pathogens rely critically on cysteine proteases for host invasion, replication, and infectivity. Their inhibition by synthetic inhibitors, such as vinyl sulfone compounds, has emerged as a promising treatment strategy. However, the individual reaction steps of protease inhibition are not fully understood. Using the trypanosomal cysteine protease rhodesain as a medically relevant target, we design photoinduced electron transfer (PET) fluorescence probes to detect kinetics of binding of reversible and irreversible vinyl sulfones directly in solution. Intriguingly, the irreversible inhibitor, apart from its unlimited residence time in the enzyme, reacts 5 times faster than the reversible one. Results show that the reactivity of the warhead, and not binding of the peptidic recognition unit, limits the rate constant of protease inhibition. The use of a reversible inhibitor decreases the risk of off-target side effects not only by allowing its release from an off-target but also by reducing the rate constant of binding.

Single Out-of-Resonance Dielectric Nanoparticles as Molecular Sensors.

Light scattering from single nanoparticles and nanostructures is a commonly used readout method for nanosensors. Increasing the spectral sensitivity of resonant nanosensors to changes in their local surrounding has been the focus of many studies. Switching from spectral to intensity monitoring allows one to investigate nonresonant or out-of-resonance dielectric nanoparticles. Here, we systematically compared such dielectric silica nanoparticles with plasmonic gold nanorods by deriving analytical expressions and by performing experiments. The experiments show a similar sensitivity for the detection of an adsorbate layer for both particle types, which is in good agreement with theory. The flat spectral response of dielectric silica nanoparticles simplifies the choice of illumination wavelength. Furthermore, such dielectric nanoparticles can be made from many oxides, polymers, and even biological assemblies, broadening the choice of materials for the nanosensor.

Intensity-Based Single Particle Plasmon Sensing.

Plasmon sensors respond to local changes of their surrounding environment with a shift in their resonance wavelength. This response is usually detected by measuring light scattering spectra to determine the resonance wavelength. However, single wavelength detection has become increasingly important because it simplifies the setup, increases speed, and improves statistics. Therefore, we investigated theoretically how the sensitivity toward such single wavelength scattering intensity changes depend on the material and shape of the plasmonic sensor. Surprisingly, simple equations describe this intensity sensitivity very accurately and allow us to distinguish the various contributions: Rayleigh scattering, dielectric contrast, plasmon shift, and frequency-dependent plasmon bulk damping. We find very good agreement of theoretical predictions and experimental data obtained by single particle spectroscopy.

Plasmonic Nanosensors for the Label-Free Imaging of Dynamic Protein Patterns.

We introduce a new approach to monitor the dynamics and spatial patterns of biological molecular assemblies. Our molecular imaging method relies on plasmonic gold nanoparticles as point-like detectors and requires no labeling of the molecules. We show spatial resolution of up to 5 µm and 30 ms temporal resolution, which is comparable to wide-field fluorescence microscopy, while requiring only readily available gold nanoparticles and a dark-field optical microscope. We demonstrate the method on MinDE proteins attaching to and detaching from lipid membranes of different composition for 24 h. We foresee our new imaging method as an indispensable tool in advanced molecular biology and biophysics laboratories around the world.

Mapping Hot Electron Response of Individual Gold Nanocrystals on a TiO2 Photoanode.

Incorporating metal nanocrystals with semiconductor photoanodes significantly enhances the efficiency of the energy conversion in the visible range during water splitting due to the excitation of hot electrons. While extensively studied on ensemble samples, hot electron response of metal nanocrystals in a photoelectrochemical cell remains unexploited at the single-particle level. Herein, we systematically investigate hot electron response of individual single-crystalline gold nanocrystals (AuNCs) on a TiO2 photoanode during water splitting. We directly correlate the morphology of the AuNC and its plasmonic property to the efficiencies involving hot electrons with the help of single-particle dark-field microscopy and photocurrent mapping. Our results show that the efficiencies of individual AuNCs are dependent on a variety of factors including interface condition, applied bias, excitation power, incident angle, and AuNC size. Our research may shed light on optimizing the light-harvesting capability of metal/semiconductor photoanodes by providing insights into the photocatalytic processes.