Plasmonic resonances in metallic nanostructures can strongly enhance the emission from quantum emitters, as commonly used in surface-enhanced spectroscopy techniques. The extinction and scattering spectrum of these quantum emitter-metallic nanoantenna hybrid systems are often characterized by a sharp Fano resonance, which is usually expected to be symmetric when a plasmonic mode is resonant with an exciton of the quantum emitter. Here, motivated by recent experimental work showing an asymmetric Fano lineshape under resonant conditions, we study the Fano resonance found in a system composed of a single quantum emitter interacting resonantly with a single spherical silver nanoantenna or with a dimer nanoantenna composed of two gold spherical nanoparticles. To analyze in detail the origin of the resulting Fano asymmetry we develop numerical simulations, an analytical expression that relates the asymmetry of the Fano lineshape to the field enhancement and to the enhanced losses of the quantum emitter (Purcell effect), and a set of simple models. In this manner we identify the contributions to the asymmetry of different physical phenomena, such as retardation and the direct excitation and emission from the quantum emitter.
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http://dx.doi.org/10.1364/OE.477200 | DOI Listing |
J Phys Chem A
January 2025
Shandong Province Key Laboratory of Medical Physics and Image Processing Technology, School of Physics and Electronics, Shandong Normal University, Jinan 250014, China.
The strategy of designing efficient room-temperature phosphorescence (RTP) emitters based on hydrogen bond interactions has attracted great attention in recent years. However, the regulation mechanism of the hydrogen bond on the RTP property remains unclear, and corresponding theoretical investigations are highly desired. Herein, the structure-property relationship and the internal mechanism of the hydrogen bond effect in regulating the RTP property are studied through the combination of quantum mechanics and molecular mechanics methods (QM/MM) coupled with the thermal vibration correlation function method.
View Article and Find Full Text PDFAdv Mater
January 2025
Organic Semiconductor Centre, EaStCHEM School of Chemistry, University of St Andrews, St Andrews, Fife, KY16 9ST, UK.
The development of narrowband emissive, bright, and stable solution-processed organic light-emitting diodes (SP-OLEDs) remains a challenge. Here, a strategy is presented that merges within a single emitter a TADF sensitizer responsible for exciton harvesting and an MR-TADF motif that provides bright and narrowband emission. This emitter design also shows strong resistance to aggregate formation and aggregation-cause quenching.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
South China University of Technology School of Materials Science and Engineering, State Key Laboratory of Luminescent Materials and Devices and Institute of Polymer Optoelectronic Materials and Devices, 381 Wushan Road, 510640, Guangzhou, CHINA.
Chalcogen-containing carbonyls, specifically thioxanthone (TX), hold great potential in organic light-emitting diodes (OLEDs). While the development of narrowband OLEDs with chalcogen-containing carbonyls remains challenging due to difficulties in achieving both high device efficiency and narrow emission spectra. Herein, via a strategic incorporation of the TX moiety, two orange-red narrowband emitters, 2TXBN and BNTXBN, are designed and synthesized for the first time.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
University of Science and Technology of China, Chemistry and Material Science, No.96, JinZhai Road Baohe District, 230026, Hefei, CHINA.
Multi-resonance thermally activated delayed fluorescence (MR-TADF) materials have great potential for applications in ultrahigh-definition (UHD) organic light-emitting diode (OLED) displays, that benefit from their narrowband emission characteristic. However, key challenges such as aggregation-caused quenching (ACQ) effect and slow triplet-to-singlet spin-flip process, especially for blue MR-TADF materials, continue to impede their development due to planar skeletons and relatively large ΔESTs. Here, an effective strategy that incorporates multiple carbazole donors into the parent MR moieties is proposed, synergistically engineering their excited states and steric hindrances to enhance both the spin-flip process and quenching resistance.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2025
Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, State Key Laboratory of Polymer Physics and Chemistry, No.159 Renmin Street, 130022, Changchun, CHINA.
The multiple resonance thermally activated delayed fluorescence (MR-TADF) device has drawn great attention due to their outstanding efficiency and color purity. However, the efficiency of solution-processed MR-TADF devices is still far behind their vacuum-deposited counterparts, due to the uncontrollable horizontal emitting dipole orientation for emitters during solution process, resulting in low light out-coupling efficiency. Here, we proposed a new strategy namely electrostatic interaction between a dendritic host with high positive electrostatic potential (ESP) and dendritic emitter with multiple negative ESP sites, which could induce high horizontal dipole ratio (ΘII) up to 83.
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