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Dynamic Emission Tuning of X-ray Radioluminescent Crystalline Colloidal Arrays: Coupling the Optical Stop Band with Sequential F?rster Resonance Energy Transfers
摘要： X-ray radiation exhibits diminished scattering and a greater penetration depth in tissue relative to the visible spectrum and has spawned new medical imaging techniques that exploit X-ray luminescence of nanoparticles. The majority of the nanoparticles finding applications in this field incorporate metals with high atomic numbers and pose potential toxicity effects. Here, a general strategy for the preparation of a fully organic X-ray radioluminescent colloidal platform that can be tailored to emit anywhere in the visible spectrum through a judicious choice in donor/acceptor pairing and multiple sequential F?rster resonance energy transfers (FRETs) is presented. This is demonstrated with three different types of ≈100 nm particles that are doped with anthracene as the scintillating molecule to “pump” subsequent FRET dye pairs that result in emissions from ≈400 nm out past 700 nm. The particles can be self-assembled in crystalline colloidal arrays, and the radioluminescence of the particles can be dynamically tuned by coupling the observed rejection wavelength with the dyes’ emission.
关键词： anthracene,F?rster resonance energy transfer,photonic crystals,X-ray radioluminescence,colloidal crystals
更新于2025-09-23 15:21:21
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The Unified Theory of Resonance Energy Transfer According to Molecular Quantum Electrodynamics
摘要： An overview is given of the molecular quantum electrodynamical (QED) theory of resonance energy transfer (RET). In this quantized radiation field description, RET arises from the exchange of a single virtual photon between excited donor and unexcited acceptor species. Diagrammatic time-dependent perturbation theory is employed to calculate the transfer matrix element, from which the migration rate is obtained via the Fermi golden rule. Rate formulae for oriented and isotropic systems hold for all pair separation distances, R, beyond wave function overlap. The two well-known mechanisms associated with migration of energy, namely the R?6 radiationless transfer rate due to F?rster and the R?2 radiative exchange, correspond to near- and far-zone asymptotes of the general result. Discriminatory pair transfer rates are also presented. The influence of an environment is accounted for by invoking the polariton, which mediates exchange and by introducing a complex refractive index to describe local field and screening effects. This macroscopic treatment is compared and contrasted with a microscopic analysis in which the role of a neutral, polarizable and passive third-particle in mediating transfer of energy is considered. Three possible coupling mechanisms arise, each requiring summation over 24 time-ordered diagrams at fourth-order of perturbation theory with the total rate being a sum of two- and various three-body terms.
关键词： molecular quantum electrodynamics,virtual photon exchange,resonance energy transfer,discriminatory transfer,F?rster transfer,medium effects,polariton mediated exchange,radiative exchange
更新于2025-09-23 15:21:01
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Dual-Emission and Two Charge Transfer States in Ytterbium-Doped Cesium Lead Halide Perovskite Solid Nanocrystals
摘要： Some unusual phenomena besides near-infrared emission of Yb3+ ions have been observed in ytterbium-doped perovskite solid nanocrystals. A systematic study on doping kinetic and energy transfer processes is presented. The observed unique dual-peak PL emission of perovskite nanocrystals in the visible region can be attributed to radiative recombination in the near-surface region and the interior region of perovskite nanocrystals respectively. Insight studies based on dual-peak PL emission clarify the kinetic process of doping in perovskite nanocrystals. After dopant concentration of rare earth ions in the near-surface region is more than a certain value, dopant ions are starting to be immersed into the interior region of host nanocrystals. The unusual excitation spectra of ytterbium-doped perovskite solid nanocrystals could be explained by the presences of two charge transfer (CT) states at ~24000 cm-1 (CT1) and ~21460 cm-1 (CT2), and both of them could be observed in the near-surface region of the perovskite host. Furthermore, the lifetime of near-infrared emission of Yb3+ ions through the CT2 state is three orders faster than that through CT1 state (in millisecond) which should be fixed on the surface of perovskite nanocrystals. The results provide essential insights into the dynamic carrier behaviors and surface effects of all inorganic perovskite nanocrystals doped with rare earth ions for expanded functionality.
关键词： dual-emission,kinetic process,rare earth,charge transfer states,Perovskite solid nanocrystals,energy transfer
更新于2025-09-23 15:21:01
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Unified theory of plasmon-induced resonance energy transfer and hot electron injection processes for enhanced photocurrent efficiency
摘要： Plasmons in metal nanoparticles (MNPs) promise to enhance solar energy conversion in semiconductors. Two essential mechanisms of enhancement in the near-field regime are hot electron injection (HEI) and plasmon-induced resonance energy transfer (PIRET). Individual studies of both mechanisms indicate that the PIRET efficiency is limited by the short lifetime of the plasmon, whereas the hot electrons result from the plasmon decay. The development of a unified theory of the coupled HEI and PIRET processes is fundamentally interesting and necessary for making reliable predictions but is complicated by the multiple interactions between various components that participate in the enhancement process. In this paper, we use the model-Hamiltonian approach to develop a combined theoretical framework including both PIRET and HEI. The coupled dynamics as well as the time evolution of hot electron energy distribution are studied. The theory further predicts an interference-induced asymmetry in the spectral dependence of PIRET, which can be used to distinguish it from HEI. As the relative contributions of PIRET and HEI strongly depend on the size of the MNPs, this presents itself as a simple route to control the strength of their contributions. The results presented here can further guide future applications of plasmonic solar energy harvesting.
关键词： plasmon,metal nanoparticles,hot electron injection,solar energy conversion,plasmon-induced resonance energy transfer
更新于2025-09-23 15:21:01
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Role of CdSe and CdSe@ZnS quantum dots interlayers conjugated in inverted polymer solar cells
摘要： We demonstrate the use of CdSe quantum dots (QDs) as an interlayer for improving photovoltaic performance in the inverted polymer solar cells (iPSCs). The conjugation of CdSe and CdSe@ZnS core@shell QDs between polyethylenimine ethoxylated (PEIE) polymer and PTB7:PC71BM blended layer played an important role in increasing the short circuit current density by F€orster resonance energy transfer (FRET) and efficient charge transport. The drastic mutual photoluminescence quenching suggests that the photon energy absorbed by PTB7:PC71BM are effectively transferred to the QDs. The PTB7:PC71BM based iPSCs with the CdSe QDs interlayer exhibits higher power conversion efficiency of 8.13%, which is 13.4% higher than that of the control device. The iPSCs with CdSe@ZnS QDs interlayer showed relatively lower PCE of 7.31%, which could be due to an increase in carrier recombination inside QDs by relatively high energy level of ZnS shell. As a consequence, the enhanced photovoltaic performance of iPSCs with CdSe QDs interlayer can be attributed to an effective charge transport and an increase in the overall photocurrent by FRET.
关键词： Carrier transport,Resonance energy transfer,Quantum dots,Inverted polymer solar cells,CdSe,Energy level alignment
更新于2025-09-23 15:21:01
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Red-Emitting Thermally Activated Delayed Fluorescence Polymers with Poly(fluorene- <i>co</i> -3,3′-dimethyl diphenyl ether) as the Backbone
摘要： A series of red-emitting thermally activated delayed ?uorescence (TADF) polymers have been designed and synthesized based on poly(?uorene-co-3,3′-dimethyl diphenyl ether) (PFDMPE) as the backbone. Compared with poly?uorene (PF, 2.16 eV), the introduction of 3,3′-dimethyl diphenyl ether into the main chain of PFDMPE leads to the increased triplet energy of 2.58 eV, which is higher enough than the tethered red TADF guest (2.13 eV) to prevent the unwanted triplet energy back-transfer. Meanwhile, there is a good overlap between the absorption spectrum of the red guest and the photoluminescence (PL) spectrum of the polymeric host, ensuring the e?cient energy transfer from host to guest. Consequently, the resultant polymers PFDMPE-R01 to PFDMPE-R10 in solid states show obvious red TADF properties with delayed ?uorescence lifetimes of 126?191 μs and PL quantum yields of 0.18?0.55. Among them, PFDMPE-R05 obtains the best device performance, revealing a bright red electroluminescence peaked at 606 nm and a promising current e?ciency of 10.3 cd/A (EQE = 5.6%). The results compete well with those of red phosphorescent polymers and indicate that PFDMPE other than PF is a suitable polymeric host for the construction of e?cient red TADF polymers.
关键词： PFDMPE,electroluminescence,polymers,poly?uorene,triplet energy,PF,energy transfer,red-emitting,thermally activated delayed ?uorescence,poly(?uorene-co-3,3′-dimethyl diphenyl ether)
更新于2025-09-23 15:21:01
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~2????m emission properties and energy transfer processes in Tm3+ doped Bi2O3-GeO2-Na2O glass laser material
摘要： Tm3+ doped Bi2O3-GeO2-Na2O glass samples were synthesized by conventional melt-quenching method. The Raman spectra measurements showed the maximum phonon energy of prepared glass is 794 cm-1, which is considerably lower than silicate glasses. Based on the measured absorption spectra, Judd-Ofelt intensity parameters, spontaneous radiative transition probabilities and radiative lifetimes were calculated to elucidate the radiative properties of Tm3+ in the presented glass. Intense near infrared emission around ~2 μm was obtained under the pump of 808nm laser diode. A large stimulated emission cross section (5.51×10-21 cm2 at 1851 nm) of Tm3+: 3F4 → 3H6 was achieved in the prepared bismuth germanate glass doped with 1 mol% Tm2O3. Besides, the energy transfer processes among Tm3+ were analyzed using the extended overlap integral method. These results indicate that the presented glass is a promising candidate for ~2 μm laser applications.
关键词： Energy transfer,Thulium,Bismuth germanate glass,Emission properties
更新于2025-09-23 15:21:01
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Crystal growth and spectroscopic investigations of Dy:YAlO3 and Dy,Tm:YAlO3 crystals for a??3a?ˉ??m laser application
摘要： Dy3+:YAP and Dy3+,Tm3+:YAP single crystals have been successfully synthesized by Czochralski (CZ) method aiming for ~3 μm emission. The optical absorption and emission features of both crystals were studied in detail. A narrow and weak absorption band around 800 nm as well as an upconversion emission under the excitation of 802 nm in Dy3+:YAP crystal along with a weak ~3 μm emission were observed, indicating that Dy3+:YAP crystal is not suitable for direct pumping under 800 nm excitation. Tm3+ ion was introduced as a sensitizer for enhancing ~3 μm emission and found that co-doping with Tm3+ greatly improved the absorption capacity around 800 nm. An enhanced ~3 μm emission was observed in Dy3+,Tm3+:YAP crystal under 795 nm excitation. The energy transfer mechanisms between Dy3+ and Tm3+ ions and the energy transfer micro-parameters were discussed. Higher values of microscopic energy transfer constants between Dy3+ and Tm3+ ions were obtained, proving Tm3+ ion act as an effective sensitizer for Dy3+ ion in YAP crystal. Following the obtained optical results, Dy3+,Tm3+:YAP crystal could be a promising medium for 3 μm laser operation under 795 nm laser diode for practical applications.
关键词： optical absorption,energy transfer micro-parameters,3 μm emission,MIR laser,Dy3+,Tm3+:YAP crystal
更新于2025-09-23 15:21:01
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Rotation of electromagnetic energy initiated by azimuthal surface waves in coaxial metal waveguides entirely filled by plasma
摘要： Azimuthal surface waves are well-known to be eigenwaves of coaxial metal waveguides entirely ?lled by plasma. The present study of electro-magnetic energy transfer complements the investigation of the wave dispersion properties carried out earlier. The angular velocity of energy transfer is analyzed as a function of the coaxial-line parameters and compared with three limiting cases. One case is a metal waveguide entirely ?lled by plasma. The second case is a metal rod placed into in?nite plasma along an external static magnetic ?eld. Finally, the third one is a thin coaxial waveguide.
关键词： azimuthal surface waves,angular velocity,coaxial metal waveguides,electromagnetic energy transfer,plasma
更新于2025-09-23 15:21:01
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Excitation Transfer in Hybrid Nanostructures of Colloidal Ag2S/TGA Quantum Dots and Indocyanine Green J-Aggregates
摘要： The regularities of the electron excitations exchange in hybrid associates of colloidal Ag2S quantum dots, passivated with thioglycolic acid (Ag2S/TGA QDs) with an average size of 2.2 and 3.7 nm with Indocyanine Green J-aggregates (ICG) were studied in this work by methods of absorption and luminescence spectroscopy. It was shown that IR luminescence sensitization of Ag2S/TGA QDs with an average size of 3.7 nm in the region of 1040 nm is possible due to non-radiative resonance energy transfer from Ag2S/TGA QDs with an average size of 2.2 nm and luminescence peak at 900 nm using ICG J-aggregate as an exciton bridge. The sensitization efficiency is 0.33. This technique provides a transition from the first therapeutic window (NIR-I, 700-950 nm) to the second (NIR-II, 1000-1700 nm). It can allow high to increase the imaging in vivo resolution.
关键词： Non-radiative resonance energy transfer (FRET),Indocyanine green,Hybrid associate,Luminescence properties,Silver sulfide quantum dots,J-aggregates
更新于2025-09-23 15:21:01