Heterogeneous singlet fission in a covalently linked pentacene dimer DOI Creative Commons
Woojae Kim, Naitik A. Panjwani,

K. C. Krishnapriya

et al.

Cell Reports Physical Science, Journal Year: 2024, Volume and Issue: 5(7), P. 102045 - 102045

Published: June 13, 2024

Molecular dimers are generally regarded as essential tools for probing structure-property relationships in condensed-phase systems, revealing complexities where structural tuning is challenging. Traditionally treated "static," with properties defined by their optimized geometry, we argue that "dynamic," exhibiting considerable conformational heterogeneity over time, which significantly influences interchromophore coupling strengths. Illustrating this, explore the singlet fission dynamics of a pentacene dimer linked phenyl-diketopyrrolopyrrole and acetylene bridges. The unrestricted rotations yield myriad rotational conformers, each altering processes, evident through excitation-energy-dependent transient absorption electron paramagnetic resonance spectroscopy. This necessitates considering not only broad distribution rate constants but also multidimensional potential-energy surfaces multiple sub-ensembles, leading to "heterogeneous fission." Consequently, these findings challenge prevailing static approach molecular photophysics, suggesting individual steps excited-state relaxation pathways cannot be delineated unique yields.

Language: Английский

The Rise and Current Status of Polaritonic Photochemistry and Photophysics DOI Creative Commons
Rahul Bhuyan, Jürgen Mony, Oleg V. Kotov

et al.

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(18), P. 10877 - 10919

Published: Sept. 8, 2023

The interaction between molecular electronic transitions and electromagnetic fields can be enlarged to the point where distinct hybrid light-matter states, polaritons, emerge. photonic contribution these states results in increased complexity as well an opening modify photophysics photochemistry beyond what normally seen organic molecules. It is today evident that polaritons offer opportunities for photophysics, which has caused ever-rising interest field. Focusing on experimental landmarks, this review takes its reader from advent of field polaritonic chemistry, over split into polariton chemistry photochemistry, present day status within photophysics. To introduce field, starts with a general description interactions, how enhance these, characterizes coupling strength. Then strongly coupled systems using Fabry-Perot plasmonic cavities are described. This followed by room-temperature Bose-Einstein condensation/polariton lasing systems. ends discussion benefits, limitations, future developments strong exciton-photon

Language: Английский

Citations

71
Triplet–triplet annihilation photon upconversion-mediated photochemical reactions DOI
Ling Huang, Gang Han

Nature Reviews Chemistry, Journal Year: 2024, Volume and Issue: 8(4), P. 238 - 255

Published: March 21, 2024

Language: Английский

Citations

35
The Golden Age of Thermally Activated Delayed Fluorescence Materials: Design and Exploitation DOI Creative Commons
John Marques dos Santos, David Hall, Biju Basumatary

et al.

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

Published: Dec. 12, 2024

Since the seminal report by Adachi and co-workers in 2012, there has been a veritable explosion of interest design thermally activated delayed fluorescence (TADF) compounds, particularly as emitters for organic light-emitting diodes (OLEDs). With rapid advancements innovation materials design, efficiencies TADF OLEDs each primary color points well white devices now rival those state-of-the-art phosphorescent emitters. Beyond electroluminescent devices, compounds have also found increasing utility applications numerous related fields, from photocatalysis, to sensing, imaging beyond. Following our previous review 2017 (

Language: Английский

Citations

30
Triplet-Triplet Annihilation Mediated Photon Upconversion Solar Energy Systems DOI Creative Commons
Lukas Naimovičius, Pankaj Bharmoria, Kasper Moth‐Poulsen

et al.

Materials Chemistry Frontiers, Journal Year: 2023, Volume and Issue: 7(12), P. 2297 - 2315

Published: Jan. 1, 2023

Triplet–triplet annihilation mediated solar energy harvesting systems for a global transition toward carbon-neutral technologies.

Language: Английский

Citations

37
Boosting exciton-based energy transfer for singlet oxygen generation in type-II heterojunction DOI Open Access
Zhenzhou Wang, Shan Hu, Fang Deng

et al.

Separation and Purification Technology, Journal Year: 2023, Volume and Issue: 330, P. 125287 - 125287

Published: Oct. 5, 2023

Language: Английский

Citations

33
Recent advances in bismuth oxyfluoride-based photocatalysts for energy and environmental remediation DOI
Vinoth Kumar Selvaraj, Alagarsamy Pandikumar

Materials Today Chemistry, Journal Year: 2024, Volume and Issue: 36, P. 101924 - 101924

Published: Jan. 24, 2024

Language: Английский

Citations

11
Automated Research Platform for Development of Triplet–Triplet Annihilation Photon Upconversion Systems DOI Creative Commons
Paulius Baronas, Justas Lekavičius, Maciej Majdecki

et al.

ACS Central Science, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 21, 2025

Triplet-triplet annihilation photon upconversion (TTA-UC) systems hold great promise for applications in energy, 3D printing, and photopharmacology. However, their optimization remains challenging due to the need precise tuning of sensitizer annihilator concentrations under oxygen-free conditions. This study presents an automated, high-throughput platform discovery TTA-UC systems. Capable performing 100 concentration scans just two hours, generates comprehensive maps critical parameters, including quantum yield, triplet energy transfer efficiency, threshold intensity. Using this approach, we identify key loss mechanisms both established novel At high porphyrin-based concentrations, yield losses are attributed self-quenching via aggregation triplet-triplet (sensitizer-TTA). Additionally, reverse (RTET) at elevated levels increases excitation thresholds. Testing sensitizer-annihilator pairs confirms these mechanisms, highlighting opportunities molecular design improvements. automated offers a powerful tool advancing research other photochemical studies requiring low oxygen levels, intense laser excitation, minimal material use.

Language: Английский

Citations

2
Highly Effective Near-Infrared to Blue Triplet–Triplet Annihilation Upconversion Nanoparticles for Reversible Photobiocatalysis DOI
Yi Peng, Jiayao Li,

Fang Qi

et al.

Nano Letters, Journal Year: 2025, Volume and Issue: unknown

Published: March 21, 2025

Near-infrared (NIR) to blue triplet-triplet annihilation upconversion (TTA-UC) shows unique applications in optogenetics, photocaging, and stereoscopic three-dimensional printing, etc. Here, we disclose a strategy that narrowed the energy gap between triplet states of NIR photosensitizer annihilator, with aim maximally suppressing photoexcitation loss during TET. Hence, produced NIR-to-blue TTA-UC pair exhibited an exceptionally large anti-Stokes shift (0.76 eV) achieved record quantum yield (15.5%, out 50%). We further prepared for first time small, water-dispersed, oxygen-resistant nanoparticles up 1.8%. Such upconverted were successfully utilized as NIR-responsive photocatalysts reversible transformation enzyme cofactor NAD+/NADH photobiocatalytic system air-saturated aqueous solutions.

Language: Английский

Citations

2
Metal–Organic Bichromophore Lowers the Upconversion Excitation Power Threshold and Promotes UV Photoreactions DOI Creative Commons
Han Li, Cui Wang, Felix Glaser

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(20), P. 11402 - 11414

Published: May 15, 2023

Sensitized triplet–triplet annihilation upconversion is a promising strategy to use visible light for chemical reactions requiring the energy input of UV photons. This avoids unsafe ultraviolet sources and can mitigate photo-damage provide access reactions, which filter effects hamper direct excitation. Here, we report new approach make blue-to-UV more amenable photochemical applications. The tethering naphthalene unit cyclometalated iridium(III) complex yields bichromophore with high triplet (2.68 eV) naphthalene-based reservoir featuring lifetime 72.1 μs, roughly factor 20 longer than photoactive excited state parent complex. In combination three different annihilators, consistently lower thresholds crossover from quadratic into linear excitation power dependence regime were observed compared system composed 2,5-diphenyloxazole annihilator sufficiently robust under long-term blue irradiation continuously high-energy singlet-excited that drive normally light. Both photoredox transfer catalyses feasible using this concept, including reductive N–O bond cleavage Weinreb amides, C–C coupling reaction based on aryl debromination, two Paternò–Büchi [2 + 2] cycloaddition reactions. Our work seems relevant in context developing strategies driving energetically demanding photochemistry low-energy

Language: Английский

Citations

21
Exploring the Versatile Uses of Triplet States: Working Principles, Limitations, and Recent Progress in Phosphorescence, TADF, and TTA DOI Creative Commons
Larissa Gomes Franca, David G. Bossanyi, Jenny Clark

et al.

ACS Applied Optical Materials, Journal Year: 2024, Volume and Issue: 2(12), P. 2476 - 2500

Published: April 19, 2024

Triplet excited states in organic semiconductors are usually optically dark and long-lived as they have a spin-forbidden transition to the singlet ground state therefore hinder processes light-harvesting applications. Also, triplets often cause damage system can sensitize formation of reactive oxygen. Despite these unfavorable characteristics, there exist mechanisms through which we utilize triplet states, that constitutes scope this review. Commencing with an introductory short exploration problem, proceed elucidate principal underpinning utilization materials: 1. Phosphorescence (PH), 2. Thermally Activated Delayed Fluorescence (TADF), 3. Triplet-Triplet Annihilation (TTA). In each section unveil their working principles, highlight vast range applications, discuss limitations perspectives. We dedicate special attention use light-emitting diodes (OLEDs), given OLEDs represent most thriving commercial application semiconductors. This review aims provide readers insights opportunities engage contribute study photophysical properties device physics semiconductors, especially regarding harnessing potential states.

Language: Английский

Citations

9