Two-dimensional (2D) lead halide perovskite (LHP) nanoplatelets (NPLs) have recently emerged as promising materials for solar cells and light-emitting devices. The reduction of LHP dimensions introduces an abundance of surface defects, which can strongly influence the photophysical properties of these materials. However, an insightful understanding of the effect of surface defects on hot carrier (HC) relaxation, one of the important properties of LHP NPLs, is still inadequate.
View Article and Find Full Text PDFPreparing chiral plasmonic nanoparticles (NPs) with strong chiroptical responses is crucial in numerous fields including constructing optical materials, chiral sensing, and chiral-dependent biological processes. However, precise regulation over the chiral optical activity and chiral configuration of plasmonic NPs is still a challenge. In this work, we report Au helicoid NPs with different chiral structures and reversal chirality directed by the oligomeric structure of inducer glutathione (GSH).
View Article and Find Full Text PDFPhotoluminescence (PL) metal nanoclusters (NCs) have attracted extensive attention due to their excellent physicochemical properties, good biocompatibility, and broad application prospects. However, developing water-soluble PL metal NCs with a high quantum yield (QY) and high stability for visual drug delivery remains a great challenge. Herein, we have synthesized ultrabright l-Arg-ATT-Au/Ag NCs (Au/Ag NCs) with a PL QY as high as 73% and excellent photostability by heteroatom doping and surface rigidization in aqueous solution.
View Article and Find Full Text PDFUnderstanding the influence of the inner shell on fluorescence blinking and exciton dynamics is essential to promote the optical performances of InP-based quantum dots (QDs). Here, the fluorescence blinking, exciton dynamics, second-order correlation function (), and ultrafast carrier dynamics of InP/ZnSe/ZnS QDs regulated by the inner ZnSe shell thickness varying from 2 to 7 monolayers (MLs) were systematically investigated. With an inner ZnSe shell thickness of 5 MLs, the photoluminescence quantum yield (PL QY) can reach 98% due to the suppressed blinking and increased probability of multiphoton emission.
View Article and Find Full Text PDFTriplet energy transfer (TET) from semiconductor quantum dots (QDs) is an emerging strategy for sensitizing molecular triplets that have great potential in many applications. Here, CdSe QDs with varying sizes and 1-pyrenecarboxylic acid (PCA) are selected as the triplet donor and acceptor, respectively, to study the TET and charge transfer dynamics as well as enhanced singlet oxygen (O) generation properties. The results from static and transient spectroscopy measurements demonstrate that both the TET and hole transfer occur at the QDs-PCA interface.
View Article and Find Full Text PDFFemtosecond helicity-resolved pump-probe spectroscopy is performed to study the spin and valley dynamics in monolayer (ML) MoS. Both the bright to dark intravalley exciton transition (∼50 fs) and the reverse transition process (<50 fs) are directly monitored. It suggests that the bright exciton state of ML MoS is lower in energy than the dark one, which is also confirmed by observing the temperature-dependent co-polarized photobleaching dynamics of A and B excitons.
View Article and Find Full Text PDFTriplet energy transfer (TET) from semiconductor quantum dots (QDs) to molecular triplets has potential applications in photon up-conversion and singlet oxygen generation. Here, we have constructed a complex consisting of CdTe QDs as the donor and 9-anthracenecarboxylic acid (ACA) as the triplet acceptor, and studied the TET pathways and enhanced singlet oxygen generation properties. The results from steady-state and time-resolved spectroscopy demonstrate efficient TET with a total efficiency of over 80% from photoexcited CdTe QDs to ACA.
View Article and Find Full Text PDFCirculating microRNAs (miRNA) can serve as key biomarkers for early diagnose of cholangiocarcinoma. Herein, an assay that uses circulating miRNA to trigger strand displacement amplification (SDA) and a CRISPR-Cas14a system to report the SDA process has been developed. In the proposed method, SDA directly amplifies miRNAs without reverse transcription.
View Article and Find Full Text PDFCarbon dots (CDs) have attracted extensive attention for their unique properties and promising applications in many fields. Many efforts have been made to improve the optical and physicochemical properties of CDs using an atomic doping strategy; however, the photoelectric properties of CD-based devices have been less studied and the photocurrent density is far from satisfactory for practical operation. Deep understanding of the doping effects on the electronic structure and photophysical properties of CDs is fundamental and essential for effectively improving the optical and photoelectrical performance of CD-based devices.
View Article and Find Full Text PDFFluorescent gold nanoclusters (Au NCs) with excellent one-photon and multiphoton properties have been demonstrated as promising candidates in many application fields. However, small multiphoton absorption (MPA) cross sections and weak multiphoton excitation (MPE) fluorescence impede their practical applications under near-infrared (NIR) excitation for biological imaging. Here, we report the regulated one-photon and multiphoton properties and mechanisms of arginine-stabilized 6-aza-2-thiothymine Au NCs (Arg/ATT-Au NCs) and the applications for MPE fluorescence imaging.
View Article and Find Full Text PDFMonolayer MoS is an emergent 2D semiconductor for next-generation miniaturized and flexible electronics. Although the high-quality monolayer MoS is already available at wafer scale, doping of it uniformly remains an unsolved problem. Such doping is of great importance in view of not only tailoring its properties but also facilitating many potential large-scale applications.
View Article and Find Full Text PDFUsing excitation-energy-scanning ultrafast infrared microspectroscopy, the excess energy-dependent hot carrier relaxation dynamics in atomically thin two-dimensional transition metal dichalcogenides (2D TMDs) after femtosecond photoexcitation was directly monitored. A good linear relationship between the carrier relaxation time and the excitation wavelength is observed for all measured monolayer (ML) and bilayer (BL) TMD samples, which allows us to determine their quasiparticle bandgaps as well as corresponding exciton binding energies. A carrier-optical-phonon scattering-mediated cascading-relaxation model is proposed, which can perfectly describe all the measured dynamics.
View Article and Find Full Text PDFPurpose: Insertion of radioactive strips through the biliary stent has been reported to offer longer survival and patency than an uncovered conventional self-expanding metal stent in patients with unresectable malignant biliary obstruction. The aim of this study was to investigate the safety and effectiveness of intraluminal brachytherapy combined with I seed implantation and transarterial infusion chemotherapy for the treatment of pancreatic head cancer with obstructive jaundice.
Method: From October 2012 to January 2018, 21 consecutive patients diagnosed with biliary obstruction caused by locally advanced, nonmetastatic pancreatic cancer with cytologically or histologically confirmed by biopsy were enrolled and receive treatment with intraluminal brachytherapy using I seed strand and CT-guided percutaneous radioactive seed implantation therapy.
A new class of white luminescent materials, white-light-emitting graphene quantum dots (WGQDs), have attracted increasing attention because of their unique features and potential applications. Herein, we designed and synthesized a novel WGQDs via a solvothermal molecular fusion strategy. The modulation of chlorine doping amount and reaction temperature gives the WGQDs a single-crystalline structure and bright white fluorescence properties.
View Article and Find Full Text PDFFemtosecond transient absorption measurements have been performed to study the pump wavelength- and fluence-dependent hot carrier relaxation dynamics in monolayer MoS. The relaxation process of the photoinduced carriers monitored within hundreds of femtoseconds after photoexcitation is demonstrated to be achieved through the carrier-phonon scattering mechanism. It is observed that an efficient hot-phonon effect can slow down the relaxation rate by around three times with the injected carrier density changing from 1 × 10 to 3 × 10 cm.
View Article and Find Full Text PDFBy using femtosecond pump-probe spectroscopy with broadband detection from near-infrared to midinfrared, the carrier and phonon dynamics in few-layer 2H-MoTe after ultrafast excitation have been investigated in detail. Immediately following the photoexcitation, an ultrafast relaxation of the generated hot carriers by releasing phonons is observed within hundreds of femtoseconds. The subsequent electron-hole recombination with a time constant of ∼1.
View Article and Find Full Text PDFThe design of efficient and stable photocatalysts for robust CO reduction without sacrifice reagent or extra photosensitizer is still challenging. Herein, a single-atom catalyst of isolated single atom cobalt incorporated into BiOBr atomic layers is successfully prepared. The cobalt single atoms in the BiOBr favors the charge transition, carrier separation, CO adsorption and activation.
View Article and Find Full Text PDFTwo-dimensional (2D) material-controllable degradation under light radiation is crucial for their photonics and medical-related applications, which are yet to be investigated. In this paper, we first report the laser illumination method to regulate the degradation rate of TiCT nanosheets in aqueous solution. Comprehensive characterization of intermediates and final products confirmed that plasmonic laser promoting the oxidation was strikingly different from heating the aqueous solution homogeneously.
View Article and Find Full Text PDFSolar photocatalysis is a potential solution to satisfying energy demand and its resulting environmental impact. However, the low electron-hole separation efficiency in semiconductors has slowed the development of this technology. The effect of defects on electron-hole separation is not always clear.
View Article and Find Full Text PDFThe thylakoid membranes of plants play a critical role in electron transfer and energy fixation, and are highly dynamic. So far, studies on the thylakoid membranes have mainly focused on microalgae and higher plants, yet very little information is available on the macroalgal thylakoids. Here, we studied the structure and organization of the thylakoid membranes in Ulva prolifera, a representative species of the green macroalgae.
View Article and Find Full Text PDFAtomically thin two-dimensional materials have emerged as a promising system for optoelectronic applications; however, the low quantum yield, mainly caused by nonradiative energy dissipation, has greatly limited practical applications. To reveal the details for nonradiative energy channels, femtosecond pump-probe spectroscopy with a detection wavelength ranging from visible to near-infrared to mid-infrared is performed on few-layer MoS. With this method, the many-body effects, occupation effects, and phonon dynamics are clearly identified.
View Article and Find Full Text PDFSpectrochim Acta A Mol Biomol Spectrosc
January 2019
Photoisomerization provides a general means for photo-controlling molecular structure and function, and two-photon induced isomerization has some advantages over one-photon processes. Here, we report the two-photon absorption (TPA) induced optical properties and characteristics of an azobenzene derivative, namely N-(3,4,5-octanoxyphenyl)-N'-4-[(4-hydroxyphenyl)azophenyl]1,3,4-oxadiazole (AOB-t8). With the activation of red light, the photoproduct of cis-AOB-t8 isomers has been unambiguously identified, and the two-photon induced isomerization process of AOB-t8 in THF is characterized with the relevant rate constants of forward and backward reactions.
View Article and Find Full Text PDFHere, we present the investigations of photo-isomerization behavior and the nonlinear optical properties of azobenzene derivative LB films. The few-layer LB films of AOB-t4 and BNB-t4 exhibit positive nonlinear refraction and two-photon absorption properties as revealed by picosecond Z-scan. The increased conjugation by introducing an oxadiazole group improves the photo-isomerization rate and the nonlinear optical properties, due to a weaker intermolecular interaction and the formation of J-aggregates within AOB-t4 LB film.
View Article and Find Full Text PDFSpectrochim Acta A Mol Biomol Spectrosc
January 2017
Metal ion recognition is of great significance in biological and environmental detection. So far, there is very few research related to the ferric ion sensing based on photoresponsive azobenzene derivatives. In this work, we report a highly selective fluorescent "turn-off" sensor for Fe ions and the molecular sensing characteristics based on an azobenzene derivative, N-(3,4,5-octanoxyphenyl)-N'-4-[(4-hydroxyphenyl)azophenyl]1,3,4-oxadiazole (AOB-t8).
View Article and Find Full Text PDFDensity functional theory calculations and atoms in molecules theory were performed to investigate the mechanism of cellulose dissolution and regeneration in 1-ethyl-3-methylimidazolium acetate ([emim]Ac), and (1,4)-dimethoxy-β-D-glucose (Glc) was chosen as the model for cellulose. The theoretical results show that the interaction of [emim]Ac with Glc is stronger than that of Glc with Glc. Further studies indicate that the anion acetate of [emim]Ac forms strong H-bonds with hydroxyl groups of Glc.
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