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Interaction of Zinc Oxide and Copper Oxide Nanoparticles with Chlorophyll: A Fluorescence Quenching Study
摘要： The present study aims to investigate the interactions of zinc oxide nanoparticles and copper oxide nanoparticles with the major photosynthetic pigment chlorophyll using ultraviolet-visible, steady state, and time resolved laser induced fluorescence spectroscopy. The steady state fluorescence measurements show that zinc oxide and copper oxide nanoparticles quench the fluorescence of chlorophyll in concentration-dependent manner. The Stern-Volmer plot for the chlorophyll-zinc oxide nanoparticles is linear, and the value of quenching constant has been observed to increase with temperature indicating the possibility of dynamic quenching. A decrease in the lifetime of chlorophyll with increase in the concentration of zinc oxide nanoparticles confirms the involvement of dynamic quenching in the chlorophyll–zinc oxide nanoparticle interaction. In the case of copper oxide nanoparticles, the Stern-Volmer plot deviates from linearity observed in the form of upward curvature depicting the presence of both static and dynamic quenching. In addition, the lifetime of chlorophyll decreases with increase in the concentration of copper oxide nanoparticles displaying the dominance of dynamic quenching in the chlorophyll-copper oxide nanoparticle interaction. The decrease observed in the value of binding constant with increasing temperature and negative values of change in enthalpy, entropy, and Gibb’s free energy indicates that van der Waal and hydrogen bonding are the prominent forces during the interaction of chlorophyll with both zinc oxide and copper oxide nanoparticles and that the process is spontaneous and exothermic. The interaction of zinc oxide and copper oxide nanoparticles with chlorophyll occurs through electron transfer mechanism. The obtained results are useful in understanding the sensitization processes involving chlorophyll and zinc oxide and copper oxide nanoparticles.
关键词： chlorophyll and nanoparticles,molecular interaction,ultraviolet-visible spectroscopy,laser-induced fluorescence spectroscopy,Attenuated total reflectance–Fourier transform infrared spectroscopy,steady state and time resolved fluorescence,X-ray diffraction
更新于2025-09-19 17:15:36
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Simultaneous detection of fumonisin B1 and ochratoxin A using dual-color, time-resolved luminescent nanoparticles (NaYF4: Ce, Tb and NH2-Eu/DPA@SiO2) as labels
摘要： A rapid and highly sensitive time-resolved fluorescence (TRF)-based aptasensor for simultaneous recognition of mycotoxins ochratoxin A (OTA) and fumonisin B1 (FB1) was developed using multi-color, Ln3+-doped time-resolved fluorescence nanoparticles (TRF-NPs) (NaYF4: Ce, Tb and NH2-Eu/DPA@SiO2 NPs) coupled with complementary strand DNA (cDNA) as luminescence probe and aptamers-conjugated amine-functionalized Fe3O4 magnetic nanoparticles (MNPs) act as a capture probe. Under the optimized conditions, the time-resolved fluorescence intensities at 544 and 618 nm corresponded with Tb3+ and Eu3+, respectively, were used to measure FB1 (Y = 19,177.1 + (? 12,054.4)x, R2 = 0.9917) and OTA (Y = 4138.8 + (? 11,182.6)x, R2 = 0.9924), respectively. The limits of detection (LODs) for FB1 and OTA were 0.019 pg mL?1 and 0.015 pg mL?1, respectively, which were much lower than previously described methods for simultaneous recognition of mycotoxins OTA and FB1 while detection range varied from 0.0001–0.5 ng mL?1. This aptasensor was effectively applied to quantity FB1 and OTA in maize samples and results were compared with ELISA method. This is the first reported time-resolved fluorescence (TRF)-based aptasensor to detect two agriculturally important toxins in the maize. The developed aptasensor has potential to be used for detection of toxins in food safety fields.
关键词： Simultaneous detection,Aptamer,Time-resolved fluorescence nanoparticles,Mycotoxins
更新于2025-09-19 17:15:36
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Dynamics of the photoinduced insulator-to-metal transition in a nickelate film
摘要： Material properties can be controlled via strain, pressure, chemical composition, or dimensionality. Nickelates are particularly susceptible due to their strong variations of the electronic and magnetic properties on such external stimuli. Here, we analyze the photoinduced dynamics in a single crystalline NdNiO3 film upon excitation across the electronic gap. Using time-resolved reflectivity and resonant x-ray diffraction, we show that the pump pulse induces an insulator-to-metal transition, accompanied by the melting of the charge order. Finally, we compare our results with similar studies in manganites and show that the same model can be used to describe the dynamics in nickelates, hinting towards a unified description of these photoinduced electronic ordering phase transitions.
关键词： resonant x-ray diffraction,nickelate,insulator-to-metal transition,charge order,photoinduced dynamics,time-resolved reflectivity
更新于2025-09-19 17:15:36
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Temperature dependence of inter-dot electron-spin transfer among laterally coupled excited states in high-density InGaAs quantum dots
摘要： The temperature dependence of interdot spin-transfer dynamics at laterally coupled excited states (ESs) in high-density InGaAs quantum dots (QDs) was studied using spin- and time-resolved photoluminescence spectroscopy. At low temperatures below 100 K, temporary suppression of electron-spin polarization decay due to selective relaxation of minority spins from emissive ESs to lower-energy states in neighboring QDs was observed. In the temperature range from 20 K to 140 K, thermal activation of electron spins from lower-energy QD states to higher-energy states via interdot transfer prevents the aforementioned selective relaxation of minority spins, leading to a faster decay of electron-spin polarization during light emission. At high temperatures above 140 K, reinjection of depolarized electron spins from barriers after thermal escape from QD ESs accelerates the further decay of the electron-spin polarization, wherein the electron spins can be activated via ladderlike interdot transfer. These findings indicate that the suppression of reinjection of electron spins from barriers in a high-density QD system is crucial for maintaining high electron-spin polarization during light emission at high temperatures.
关键词： electron-spin polarization,InGaAs quantum dots,interdot spin-transfer dynamics,spin- and time-resolved photoluminescence spectroscopy,temperature dependence
更新于2025-09-19 17:13:59
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Time-dependent optimization of laser-produced molecular plasmas through high-order harmonic generation
摘要： Analysis and characterization of laser-produced plasmas (LPPs) require the advanced methods for determination of different multiparticle component formation and spreading. Time-resolved high-order harmonic generation (HHG) in spreading LPPs allows determining optimal conditions for this process. One of the most important parameters of HHG in LPP is the delay between the heating and driving pulses. We demonstrate that the optimization of delays allows achieving the maximal harmonic yields in LPP created on the surfaces of the solid targets possessing different molar masses (m). The optimal delays (t) for B4C, ZnO, GaP, GaAs, and Ag2S plasmas were determined to be approximately 200, 300, 350, 500, and 700 ns, respectively. These variations of delays correspond to the t1(m)0.5 dependence for different materials. We demonstrate the applicability of the proposed method for analysis of the resonance-enhanced harmonics in atomic and molecular plasmas (Mo and MoS2) and for studies of large perovskite aggregates as potential emitters of harmonics. This diagnostic technique can also be applied to the analysis of the presence of different nanostructures in LPPs through HHG with a high spatiotemporal resolution.
关键词： perovskite aggregates,laser-produced plasmas,molar masses,time-resolved,high-order harmonic generation,optimization,nanostructures,resonance-enhanced harmonics
更新于2025-09-19 17:13:59
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Study of Interfacial Charge Transfer from an Electron Rich Organic Molecule to CdTe Quantum Dot by using Sterna??Volmer and Stochastic Kinetic Models
摘要： Photoinduced electron transfer from N-methylaniline (NMA) to a photoexcited CdTe quantum dot (QD*) is studied in toluene. The PET mechanism at low to moderate quencher (NMA) concentrations (< 0.08 M) remains mostly collisional with some contributions from QD-NMA complex formation. However, at high quencher concentrations (> 0.10 M), QDs form larger numbers of static complexes with NMA molecules leading to a steep positive deviation in the steady-state Stern–Volmer curves. An isothermal titration calorimetry (ITC) study confirms the formation of QD-NMA complexes (K ~ 150 M?1) at high quencher concentrations. Fitting our experimental data using a stochastic kinetic model indicates that the number of NMA molecules attached per QD at highest NMA concentration (~ 0.16 M) used in this study decreases from ~ 0.76 to ~ 0.47 with reducing the QD size from ~ 5.2 nm to ~ 3.2 nm. However, the PET rate increases with decreasing QD size, which is commensurate with the observation that the chemical driving force (ΔG) increases with decreasing the QD particle size. We have analyzed the PET kinetics mainly by using Stern-Volmer fittings. However, in some cases Tachiya’s stochastic kinetic model is used for stoichiometric analysis, which seems to be useful only at high quencher concentrations. The measured PET rate coefficients in all the cases are found to be at least an order of magnitude lower when compared to the diffusion-controlled rate of the reaction medium.
关键词： quantum dot,time-resolved fluorescence,photoinduced electron transfer,Stern–Volmer analysis,bimolecular quenching
更新于2025-09-19 17:13:59
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Microsecond Resolved Infrared Spectroelectrochemistry Using Dual Frequency Comb IR Lasers
摘要： A dual infrared frequency comb spectrometer with heterodyne detection has been used to perform time resolved electrochemical attenuated total reflectance surface enhanced infrared absorption spectroscopy (ATR-SEIRAS). The measurement of the potential dependent desorption of a monolayer of a pyridine derivative (4-dimethylaminopyridine, DMAP) with time resolution as high as 4 μs was achieved without the use of step-scan interferometry. An analysis of the detection limit of the method as a function of both time resolution and measurement co-additions is provided and compared to step-scan experiments of an equivalent system. Dual frequency comb spectroscopy is shown to be highly amenable to time-resolved ATR-SEIRAS. Microsecond resolved spectra can be obtained with high spectral resolution and fractional monolayer detection limits in a total experimental duration that is two orders of magnitude less than the equivalent step-scan experiment.
关键词： 4-dimethyamino pyridine (DMAP),noise analysis,Dual frequency comb spectroscopy,time resolved spectroelectrochemistry,RC constant,attenuated total reflectance surface enhanced infrared absorption spectroscopy (ATR-SEIRAS),detection limit
更新于2025-09-19 17:13:59
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Express: Time-Gated Single-Shot Picosecond Laser-Induced Breakdown Spectroscopy (ps-LIBS) for Equivalence-Ratio Measurements
摘要： Time-gated picosecond laser-induced breakdown spectroscopy (ps-LIBS) for the determination of local equivalence ratios in atmospheric-pressure adiabatic methane–air flames is demonstrated. Traditional LIBS for equivalence-ratio measurements employ nanosecond (ns)-laser pulses, which generate excessive amounts of continuum, reducing measurement accuracy and precision. Shorter pulse durations reduce the continuum emission by limiting avalanche ionization. Furthermore, by contrast the use of femtosecond lasers, plasma emission via picosecond-laser excitation has high signal-to-noise ratio (S/N), allowing single-shot measurements suitable for equivalence-ratio determination in turbulent reacting flows. We carried out an analysis of the dependence of the plasma emission ratio Hα (656 nm)/NII (568 nm) on laser energy and time-delay for optimization of S/N and minimization of measurement uncertainties in the equivalence ratios. Our finding shows that higher laser energy and shorter time delay reduces measurement uncertainty while maintaining high S/N. In addition to atmospheric-pressure flame studies, we also examine the stability of the ps-LIBS signal in a high-pressure nitrogen cell. The results indicate that the plasma emission and spatial position could be stable, shot-to-shot, at elevated pressure (up to 40 bar) using a lower excitation energy. Our work shows the potential of using ps-duration pulses to improve LIBS-based equivalence-ratio measurements, both in atmospheric and high-pressure combustion environments.
关键词： time-resolved spectroscopy,combustion diagnostics,Laser-induced breakdown spectroscopy,picosecond phenomena,LIBS
更新于2025-09-19 17:13:59
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Ultrafast pump-probe ellipsometry and microscopy reveal the surface dynamics of femtosecond laser ablation of aluminium and stainless steel
摘要： An ultra-short laser pulse irradiated surface passes through a sequence of physical processes that occur over a wide temporal range, from femtoseconds to microseconds. In this paper for the first time, the complete laser ablation process for industrially relevant metals, aluminium (Al) and stainless steel (AISI 304) is tracked from the initial pulse impact to the final state. Time-resolved surface analytical techniques provide a complementary description of the surface dynamics. The pump-probe ellipsometry reveals changes of the complex refractive index for the first tens of picoseconds and time-resolved microscopy of the irradiated surface gives access to changes of the relative reflectivity from the initial femtosecond pulse impact to the final state at 10 μs. The changes in optical indices are affected by an ultrafast decrease in the density of the surface within the pressure unloading process in the first picoseconds and reveal spallation as the dominant mechanism for laser ablation in Al and stainless steel. The study also implies that the ablation volume is kept at an optimum when the ablation is initiated with ultrafast pulses within the pressure unloading process and is able to evolve over eight orders of magnitude without external perturbations.
关键词： Time-resolved ellipsometry,Spallation,Laser ablation,Nanostructure,Pump-probe reflectometry
更新于2025-09-19 17:13:59
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Photoswitching mechanism of a fluorescent protein revealed by time-resolved crystallography and transient absorption spectroscopy
摘要： Reversibly switchable fluorescent proteins (RSFPs) serve as markers in advanced fluorescence imaging. Photoswitching from a non-fluorescent off-state to a fluorescent on-state involves trans-to-cis chromophore isomerization and proton transfer. Whereas excited-state events on the ps timescale have been structurally characterized, conformational changes on slower timescales remain elusive. Here we describe the off-to-on photoswitching mechanism in the RSFP rsEGFP2 by using a combination of time-resolved serial crystallography at an X-ray free-electron laser and ns-resolved pump–probe UV-visible spectroscopy. Ten ns after photoexcitation, the crystal structure features a chromophore that isomerized from trans to cis but the surrounding pocket features conformational differences compared to the final on-state. Spectroscopy identifies the chromophore in this ground-state photo-intermediate as being protonated. Deprotonation then occurs on the μs timescale and correlates with a conformational change of the conserved neighbouring histidine. Together with a previous excited-state study, our data allow establishing a detailed mechanism of off-to-on photoswitching in rsEGFP2.
关键词： time-resolved crystallography,fluorescent proteins,transient absorption spectroscopy,photoswitching,rsEGFP2
更新于2025-09-19 17:13:59