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Cell Imaging Using Two-Photon Excited CdS Fluorescent Quantum Dots Working within the Biological Window
摘要: In recent years, two-photon excited semiconductor quantum dots (QDs) have been the subject of intense investigation due to their long excitation wavelength which helps to achieve deeper penetration and higher image resolution in optical bioimaging. In this paper, water-soluble CdS QDs were synthesized using a hydrothermal method and applied to human liver hepatocellular carcinoma (HepG2) cells. The first-principles calculation suggested that the S-rich defected structure contributes to a narrower band gap compared to the pristine structure. The resulting fluorescence wavelength was significantly red shifted, which was attributed to the deep defect states emission. The large Stokes shifts (> 200 nm) of the QDs can eliminate the possible cross-talk between the excitation light and the emission light. Two-photon induced red fluorescence emission can avoid overlapping with the autofluorescence emission of biological samples. The uptake and cell viability measurements of the HepG2 cells showed a good biocompatibility and a low toxicity of CdS QDs. Two-photon excited scanning microscopy images revealed that the HepG2 cells incubated with CdS QDs emitted bright red upconversion fluorescence and the fluorescence brightness was 38.2 times of that of the control group. These results support CdS QDs as a good candidate for application in cellular imaging.
关键词: two-photon absorption,CdS quantum dots,deep defect states,HePG2 cells,biological imaging
更新于2025-11-21 11:24:58
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dz2 Orbitals Mediated Bound Magnetic Polarons in Ferromagnetic Ce Doped BaTiO3 Nanoparticles and its Enriched Two Photon Absorption Cross Section
摘要: Enriched ferromagnetism and two photon absorption (TPA) cross section of perovskite BaTiO3 nanoparticles are indispensible for magnetic and optical data storage applications. In this work, the hydrothermally synthesized Ce doped BaTiO3 nanoparticles exhibit the maximum room temperature ferromagnetism (4.26×10-3 emu/g) at 4 mol% due to the increase of oxygen vacancies as evidenced by X-ray photoelectron, electron spin resonance spectroscopies and density functional theory (DFT) calculations. Hence, the oxygen vacancy constituted bound magnetic polaron (BMP) model has been invoked to explain the enhancement of ferromagnetism. BMP theoretical model indicates the increase of BMP magnetization (M0, 3.0 to 4.8×10-3 emu/g) and true spontaneous moment per BMP (meff, 4 to 9.88×10-4 emu) on Ce doping. DFT calculations show that BMPs mediate via Ti d orbitals leading to the ferromagnetism. Besides, it is understood that the magnetic moment induced by Ce at Ba site is higher than Ce at Ti site in the presence of oxygen vacancies. Open aperture Z-scan technique displays the highest TPA coefficient β (7.08×10-10 m/W) and TPA cross section σTPA (455×104 GM) at 4 mol% of Ce as a result of robust TPA induced excited state absorption. A large σTPA is attributed to the longer excited state lifetime τ (7.63 ns) of charge carriers created by oxygen vacancies and Ce ions which encounter several electronic transitions in the excited sub-states.
关键词: Ce doping,oxygen vacancies,bound magnetic polarons,two photon absorption,DFT calculations,Z-scan technique,BaTiO3 nanoparticles,ferromagnetism
更新于2025-11-19 16:56:35
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Photo-physical properties of substituted 2,3-distyryl indoles: Spectroscopic, computational and biological insights
摘要: The structural dependence of the photo-physical properties of substituted 2,3-distyryl (23DSI) indoles were studied using several spectroscopic techniques including steady-state UV-VIS spectroscopy, steady-state fluorescence spectroscopy, steady-state excitation spectroscopy, time correlated single photon counting (TCSPC) spectroscopy, and time-resolved fluorescence upconversion spectroscopy (TRFLS). Each of 23DSI derivatives investigated showed distinct fluorescence emission and UV-VIS spectra, indicating strong structural dependence of the emission and the excitation. The UV-VIS spectra of the 23DSI derivatives showed three main identical absorption bands with minor deviations in the absorbance caused by substituent groups on the distyryl rings. The time-resolved fluorescence up-conversion studies indicated that the fluorescence undergoes a mono-exponential decay whereas the calculated fluorescence lifetime showed relatively short fluorescence lifetimes of approximately 1 ns. All of the 23DSI derivatives showed two-photon absorption upon direct excitation of 1.6 W laser pulses at 800 nm. These studies suggest that the substituents, attached to distyryl core, are capable of boosting or hindering fluorescence intensities by distorting the π-conjugation of the 23DSI molecule. Our studies showed that 23DSI (p-F) has the highest fluorescence emission quantum yield. Theoretical calculations for the ground state of 23DSI derivatives confirmed differences in electron densities in 23DSI derivatives in the presence of different substituent attachments. The excellent fluorescence emission, high fluorescence quantum yield and two-photon absorption properties of these 23DSI molecules make them attractive candidates for potential applications in the fields of biological imaging, biomedicine, fluorescent probes, and photodynamic inactivation (PDI). B. subtilis samples, treated with micro molar solutions of 23DSI (p-OCH3) and 23DSI (p-CH3), showed very effective photodynamic inactivation (PDI) upon irradiation with white light.
关键词: Two photon absorption,Time-resolved fluorescence upconversion laser spectroscopy,Photodynamic inactivation,Gaussian calculations,Photo-physical properties,Light-activation
更新于2025-11-14 15:26:12
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Effects of two-photon absorption on pseudo-random bit sequence operating at high speed
摘要: The effect of two-photon absorption (TPA) on all-optical logic operation in quantum-dot semiconductor optical amplifier (QD-SOA) has been carried out. We model the rate equation with the TPA effect for the logic XOR gate, AND gate, and, for pseudo-random bit sequence (PRBS) generation. The simulated results indicate that the TPA induced pumping increases the output Q-factor (quality). The results show that the quality of the output depends on the input pulse width and the speed of operation. The PRBS system can operate at 250 and 320 Gb/s but an increase in pulse width decreases the output Q-factor.
关键词: quantum-dot semiconductor optical amplifier,pseudorandom bit sequence,optical logic,Q factor,Two-photon absorption
更新于2025-09-23 15:23:52
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A turn-on two-photon fluorescent probe for detecting lysosomal hydroxyl radicals in living cells
摘要: The detection of reactive oxygen species (ROS) in biological systems and its imaging is of great importance. Among them, the hydroxyl radical (?OH) stands out as one of the most reactive, playing an important role in many physiological and pathological processes. Here we report a two-photon (TP) turn-on fluorescent probe with good selectivity and sensitivity towards ?OH. The molecular design of this naphthalene-indoline compound enables it to accurately target lysosomes in its non-fluorescent (“off”) state, where interaction with ?OH gives rise to the fluorescent (“on”) state and allows for the imaging of ?OH generation in living mouse embryonic fibroblast (MEF) cells. The present study provides an approach for improving our understanding of the role of ?OH in biological processes.
关键词: Lysosomes,Two-photon absorption,Biosensors,Fluorescent Probes,Reactive Oxygen Species
更新于2025-09-23 15:23:52
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Up-conversion Luminescence Properties of Er3+/Yb3+ Co-Doped Oxyfluoride Glass Ceramic
摘要: Er3+/Yb3+ co-doped glass ceramic samples were prepared by melt-quenching method utilizing nominal composition 52SiO2-8Na2CO3-16Al2O3-33NaF-3LuF3-0.15Yb2O3-0.03Er2O3 (in mol%). The spectral characteristic was studied based on Judd-Ofelt theory. Spectrum intensity parameters Ωλ(λ=2,4,6) were calculated on the basis of the absorption spectrum. The theoretical and experimental oscillator strengths were calculated according to the spectrum intensity parameters, and the root mean square deviation (δrms) of glass ceramic sample was 4.28x10-6. The parameters such as transition probability, decay branching ratios and level lifetime of Er3+ were obtained. Lifetimes of metastable level 4I13/2 and 4I11/2 in as-prepared samples are respectively 11.64 and 13.61ms which are suitable for up-conversion intermediate levels. Decay branching ratio of 4I13/2→4I15/2 is nearly 100% in Er3+/Yb3+ co-doped oxyfluoride glass ceramic samples which can be used to produce 1543nm laser. Under the excitation of 980 nm diode laser, up-conversion luminescence is observed at the wavelength of 549nm and (653, 664) nm, corresponding to the radiative transitions of Er3+: 4S3/2→4I15/2 and 4F9/2→4I15/2, respectively. The numbers of absorbed photons in the transition process of Er3+/Yb3+ co-doped oxyfluoride glass ceramic samples are estimated at 1.99 and 2.06 respectively according to the relationship between the up-conversion transmitting power and the 980 nm LD laser power. It is determined that the transition process of Er3+/Yb3+ co-doped oxyfluoride glass ceramic samples is two-photon absorption process.
关键词: Glass ceramic,Two-photon absorption,Up-conversion,Judd-Ofelt theory
更新于2025-09-23 15:23:52
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Transition from Two-photon Absorption to Saturable Absorption in Gold Patterned Ruby Thin Film
摘要: Nonlinear behaviour of gold micro disks patterned Ruby film has been investigated via Z-scan technique. Open Z-scan was performed for Ruby and Ruby/gold thin film using 532 nm Laser source. Two-photon absorption (TPA) and Saturable absorption (SA) have been observed in pure Ruby and Ruby/gold thin film respectively. The expression for normalized transmittance in open Z-scan was obtained by Gaussian decomposition method for fitting the open. The values for nonlinear absorption coefficient (β) for Ruby/gold (7.41 × 10?7??/??) was two orders of magnitude higher than that of Ruby (1.41 × 10?9??/??). Further, TPA and SA were confirmed by open Z-scan on these films, performed by 633 nm Laser source.
关键词: Surface Plasmon Resonance,Ruby,Z-scan,Two-photon absorption,Saturable absorption
更新于2025-09-23 15:22:29
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Assessment of functionals for TDDFT calculations of one- and two-photon absorption properties of neutral and anionic fluorescent proteins chromophores
摘要: Performance of DFT functionals with different percentage of exact Hartree-Fock exchange energy (EX) is assessed for recovery of the CC2 reference one- (OPA) and two-photon absorption (TPA) spectra of fluorescent proteins chromophores in vacuo. The investigated DFT functionals, together with their EX contributions are: BLYP (0%), B3LYP (20%), B1LYP (25%), BHandHLYP (50%) and CAM-B3LYP (19% at short range and 65% at long range). Our test set consists of anionic and neutral chromophores as naturally occuring in the fluorescent proteins. For the first time, we compare TDDFT and CC2 methods for higher excited states, than the S1 state, exhibiting relatively large TPA intensity. Our TDDFT results for neutral chromophores reveal an increase of excitation energies as well as TPA and OPA intensities errors, compared to CC2-derived results, as the DFT functional contains less exact exchange. The long-range-corrected CAM-B3LYP functional performs the best, closely followed by BHandHLYP, while BLYP usually significantly underestimates all investigated spectral properties, hence being the worst in reproducing the reference CC2 results. The hybrid B3LYP and B1LYP functionals can be roughly placed in between. We propose that TDDFT may underestimate the TPA intensities for neutral chromophores of fluorescent proteins due to underestimated oscillator strengths between some excited states. In case of anionic chromophores, we find that B3LYP and B1LYP functionals overcome others in terms of reproducing CC2 excitation energies. On the other hand, however, TPA intensity is usually significantly underestimated and in this respect CAM-B3LYP functional seems to be again superior. In contrast to the case of neutral chromophores, it seems that large magnitude of excited-state dipole moment or change in dipole moment upon excitation may be the driving force behind high TPA transition moments.
关键词: fluorescent proteins chromophores,one-photon absorption,DFT functionals,two-photon absorption,TDDFT,CC2
更新于2025-09-23 15:21:21
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Robust Wavelength-Converting and Lasing Media from Wafer-Scale Inorganic Perovskites Enabled by a Protective Surface Layer
摘要: Despite that the inorganic halide perovskites show great promise in wavelength-conversion and lasing applications, the stability and scalability remain as the obstruction toward practical applications. Herein, we, for the first time, employ the wafer-scale inorganic perovskite single crystals to address the above issue. Our spectroscopic analysis reveals that the carrier trapping on the crystal surface is the most probable culprit to hinder the optical amplification for the weak-penetrating one-photon pumping, whilst, the interior of the crystal preserves intact and show low-threshold stimulated emission by two-photon absorption in the near infrared regime. Thanks to the effective protection from the surface layer, the stimulated emission maintains 90% of the initial intensity upon uninterrupted pumping of 4 hours and shows nearly constant threshold upon long-term storage without any encapsulation (> one year). By exploiting a parallel-mirror cavity, an optically pumped wavelength-converting and laser device featuring a spatially coherent output beam is constructed. Our finding greatly advances the development of practical coherent light sources based on halide perovskites.
关键词: wavelength-conversion,lasing,scalability,two-photon absorption,inorganic halide perovskites,stability,coherent light sources,stimulated emission
更新于2025-09-23 15:21:01
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Highly Conjugated, Fused-Ring, Quadrupolar Organic Chromophores with Large Two-Photon Absorption Cross-Sections in the Near-Infrared
摘要: The two-photon absorption (2PA) properties are investigated for two series of organic, π-conjugated, fused-ring, quadrupolar A-π-D-π-A chromophores of the type originally developed as non-fullerene acceptors for organic photovoltaics. These molecules are found to exhibit large nondegenerate two-photon absorption (ND2PA) cross-sections (ca. 6-27 × 103 GM) in the near infrared (NIR). In the first series, involving molecules of varying core size, ND2PA spectra and cross-sections characterized by femtosecond ND2PA spectroscopy in chloroform solutions reveal that increases in core size, and thus conjugation length, leads to substantially red-shifted and enhanced 2PA. In a second series, variation of the strength of the terminal acceptor (A) with constant core size (7 rings, indacene-based) led to less dramatic variation in the 2PA properties. Among the two core types studied, compounds in which the donor has a thieno[3,2-b]thiophene center demonstrate larger 2PA cross-sections than their indacene-centered counterparts, due to the greater electron-richness of their cores amplifying intramolecular charge transfer. Excited-state absorption (ESA) contributions to nonlinear absorption measured by open-aperture Z-scans are deduced for some of the compounds by analyzing the spectral overlap between 2PA bands and NIR ESA transitions obtained by ND2PA and transient absorption measurements, respectively. ESA cross-sections extracted from transient absorption and irradiance-dependent open-aperture Z-scans are in reasonable agreement and their moderate magnitudes (ca. 10-21 m2) suggest that, although ESA contributions are non-negligible, the effective response is predominantly instantaneous 2PA.
关键词: pump-probe spectroscopy,Nonlinear optics,Z-scan,organic optoelectronics,ultrafast spectroscopy,two-photon absorption
更新于2025-09-23 15:21:01