Hybrid metal halides represent a novel type of semiconductor light emitters with intriguing excitonic emission properties, including free exciton emission and self-trapped exciton emission. Achieving precise control over these two excitonic emissions in hybrid metal halides is highly desired yet remains challenging. Here, the complete transformation from intrinsically broadband self-trapped exciton emission to distinctively sharp free exciton emission in a quasi-one-dimensional hybrid metal halide (CHN)[PbBr]·6Br with a ribbon width of n = 4, is successfully achieved based on high-pressure method. During compression, pressure-induced phonon hardening continuously reduces exciton-phonon coupling, therefore suppressing excitonic localization and quenching the original self-trapped exciton emission. Notably, further compression triggers excitonic delocalization to induce intense free exciton emission, accompanied with reduced carrier effective masses and improved charge distribution. Controlled high-pressure investigations indicate that the ribbon width of n > 2 is necessary to realize excitonic delocalization and generate free exciton emissions in similar quasi-one-dimensional hybrid metal halides. This work presents an important photophysical process of excitonic transitions from self-trapped exciton emission to free exciton emission in quasi-one-dimensional hybrid metal halides without chemical regulation, promoting the rational synthesis of hybrid metal halides with desired excitonic emissions.
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http://dx.doi.org/10.1038/s41467-024-51836-2 | DOI Listing |
Adv 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
Ningbo Institute of Materials Technology and Engineering CAS: Chinese Academy of Sciences Ningbo Institute of Materials Technology and Engineering, Key Laboratory of Advanced Marine Materials, Ningbo Institute of Materials Technology and Engineering, CHINA.
High-temperature phosphorescence (HTP) materials have attracted considerable attention owing to their expanded application prospects, whereas they still suffer from severe deactivation in polar media, limiting their reliability and utility. Here, we present an efficient multivalent assembly strategy to achieve high-temperature liquid-phase phosphorescence (HTLP). The supramolecular assembly of multivalent modules leads to extremely robust hydrogen-bonding networks, which firmly immobilize the organic phosphors and protect triplet excitons from annihilation in high-temperature polar media, resulting in excellent HTLP emission.
View Article and Find Full Text PDFJ 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.
Organic room-temperature phosphorescence (RTP) emitters with long lifetimes, high exciton utilizations, and tunable emission properties show promising applications in organic light-emitting diodes (OLEDs) and biomedical fields. Their excited-state properties are highly related to single molecular structure, aggregation morphology, and external stimulus (such as hydrostatic pressure effect). To gain a deeper understanding and effectively regulate the key factors of luminescent efficiency and lifetime for RTP emitters, we employ the thermal vibration correlation function (TVCF) theory coupled with quantum mechanics/molecular mechanics (QM/MM) calculations to investigate the photophysical properties of three reported RTP crystals (Bp-OEt, Xan-OEt, and Xan-OMe) with elastic/plastic deformation.
View Article and Find Full Text PDFNano Lett
January 2025
Department of Materials Science and Engineering, Centre for Functional Photonics, and Hong Kong Branch of National Precious Metals Material Engineering Research Centre, City University of Hong Kong, Hong Kong S.A.R., 999077, China.
The emission efficiency of interlayer excitons (IEs) in twisted 2D heterostructures has long suffered from momentum mismatch, limiting their applications in ultracompact excitonic devices. Here, we report strong room-temperature emission of momentum-forbidden IE in 30°-twisted MoS/WS heterobilayers. Utilizing a plasmonic nanocavity, the Purcell effect boosts the IE emission intensity in the cavity by over 2 orders of magnitude.
View Article and Find Full Text PDFACS Nano
January 2025
Department of Chemistry and the Smalley-Curl Institute, Rice University, Houston, Texas 77005, United States.
The reaction of aqueous suspensions of single-wall carbon nanotubes (SWCNTs) with UV-excited sodium hypochlorite has previously been reported to be an efficient route for doping nanotubes with oxygen atoms. We have investigated how this reaction system is affected by pH level, dissolved O content, and radical scavengers and traps. Products were characterized with near-IR fluorescence, Raman, and XPS spectroscopy.
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