Enabling Ultrafast Intramolecular Singlet Fission in Perylene Diimide Tetramer with Saddle-Shaped Linker DOI
Yu Guo,

Lisi Yang,

Yixuan Gao

et al.

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: 15(51), P. 12561 - 12570

Published: Dec. 16, 2024

Intramolecular singlet fission (SF) in multichromophore systems is of high interest for photovoltaic application. As an attractive candidate SF-based devices, enabling efficient SF covalent oligomers perylene diimide (PDI) still remains challenging. In this work, inter-PDI with τSF = ∼150 ps and ∼150% triplet yield a tetramer COTh-FPDI was facilitated by employing saddle-shaped cyclooctatetrathiophene (COTh) core fused linking PDIs. comparison, ultrafast symmetry-breaking charge separation (τCS ∼100 fs) observed the COTh-αPDI flexible linking. Taking advantage rigid minimized excited-state structural relaxation, unique geometry can be fully defined topological characteristic COTh, which plays key role electronic coupling required SF. Our work provides new strategy intramolecular predefining interchromophore structure, might inspired future designing systems.

Language: Английский

Nonadiabatic Couplings Facilitate Excitation Wavelength–Dependent Fluorescence in a Cyclooctatetraene-Based Polymorph DOI

P. E. Swathi Krishna,

Vivek V. Dev,

Jayashree Nagesh

et al.

The Journal of Physical Chemistry C, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 21, 2024

Achieving wide-range tunable emission colors in the crystalline state of single fluorophores is a challenging task. Here, we report vibronic coupling hitherto unexplored class nonaromatic tetrabrominated dibenzocyclooctatetraene two distinct polymorphic forms. The thermodynamically stable polymorph (P1) revealed single-emission maximum upon excitation at different wavelengths adhering to Kasha's rule and lacks luminescence from triplet states. In contrast, kinetically form (P2) exhibited wavelength–dependent with range Δλemimax= 100 nm room temperature phosphorescence. Prominent nonadiabatic couplings between bright several lower singlet states dimeric elucidate emission. variable fluorescence behavior highlights possibility cyclooctatetraene derivatives as novel multicolor luminescent materials for future optoelectronic applications.

Language: Английский

Citations

0

Photoregulated Supramolecular Polymerization through Halogen Bonding DOI Open Access

Alejandro Martinez Manjarres,

Antonia Albers,

Gustavo Fernández

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 1, 2024

Abstract Supramolecular polymers are able to change their structure, morphology and function in response external stimuli. However, controlling the independence of stimuli‐responses these systems is challenging. Herein, we exploit halogen bonding (XB) as a reversible network element regulate photoresponsive adaptive behavior supramolecular polymers. To this end, have designed two‐component system comprising an amphiphilic XB acceptor with ability self‐assemble aqueous media ( OPE‐Py ) molecule dual donor [ E )‐Azo‐I ]. self‐assembles into polymers, which transform nanoparticle assemblies upon co‐assembly . Interestingly, third type assembly (2D sheets) obtained if treated exposed photoirradiation. At ambient conditions, both nanoparticles 2D sheets remain invariant over time. heating dissociates interactions present assemblies, resulting transformation original fiber‐like Thus, breaking communication between self‐assembly restores state system, drawing parallels feedback loops programming language. This work broadens still limited scope solution paves way for multifunctional systems.

Language: Английский

Citations

0

Charge-Transfer Mediated J-aggregation in Red Emitting Ultra-Small-Single-Benzenic Meta-Fluorophore Crystal DOI Creative Commons
Mrinal Mandal, Sukumar Mardanya, Arijit Saha

et al.

Chemical Science, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 27, 2024

Red emission in crystals has been observed with an ultra-small-single-benzenic

Language: Английский

Citations

0

Cross‐Transition‐Dipole Stacking of Conjugated Organic Molecules: Structure, Exciton Behavior and Optoelectronic Property DOI
Weicong Li, Zengqi Xie

Chemistry - A European Journal, Journal Year: 2024, Volume and Issue: 31(8)

Published: Dec. 9, 2024

Abstract Organic conjugated molecules have gained widespread application as organic semiconductors due to their unique optoelectronic properties. The rigidity of these large structures facilitates strong intermolecular interactions, which significantly influence properties in the solid state through various molecular arrangements. study relationship among arrangement, exciton behavior, and is an eternal research topic. Cross‐dipole stacking a specific arrangement that demonstrates characteristics has received continuous attention over past decades. This mini‐review will first discuss behaviors cross‐dipole based on models, including weak coupling suppression Förster resonance energy transfer. These behaviors, determined by arrangements, are fundamental systems. Next, we introduce well‐defined systems summarize design principles from structure perspective. Finally, present outstanding performance, such high solid‐state luminescence, good charge carrier mobility, significant CD/CPL. Through this mini‐review, hope enhance understanding stacking, contributing construction systems, exploration excited‐state discovery high‐performance materials.

Language: Английский

Citations

0

Enabling Ultrafast Intramolecular Singlet Fission in Perylene Diimide Tetramer with Saddle-Shaped Linker DOI
Yu Guo,

Lisi Yang,

Yixuan Gao

et al.

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: 15(51), P. 12561 - 12570

Published: Dec. 16, 2024

Intramolecular singlet fission (SF) in multichromophore systems is of high interest for photovoltaic application. As an attractive candidate SF-based devices, enabling efficient SF covalent oligomers perylene diimide (PDI) still remains challenging. In this work, inter-PDI with τSF = ∼150 ps and ∼150% triplet yield a tetramer COTh-FPDI was facilitated by employing saddle-shaped cyclooctatetrathiophene (COTh) core fused linking PDIs. comparison, ultrafast symmetry-breaking charge separation (τCS ∼100 fs) observed the COTh-αPDI flexible linking. Taking advantage rigid minimized excited-state structural relaxation, unique geometry can be fully defined topological characteristic COTh, which plays key role electronic coupling required SF. Our work provides new strategy intramolecular predefining interchromophore structure, might inspired future designing systems.

Language: Английский

Citations

0