Efficient Visible‐to‐UV Photon Upconversion Systems Based on CdS Nanocrystals Modified with Triplet Energy Mediators DOI Creative Commons
Lili Hou, Axel Olesund, Shameel Thurakkal

и другие.

Advanced Functional Materials, Год журнала: 2021, Номер 31(47)

Опубликована: Авг. 21, 2021

Abstract Developing high‐performance visible‐to‐UV photon upconversion systems based on triplet–triplet annihilation (TTA‐UC) is highly desired, as it provides a potential approach for UV light‐induced photosynthesis and photocatalysis. However, the quantum yield spectral range of TTA‐UC nanocrystals (NCs) are still far from satisfactory. Here, three different sized CdS NCs systematically investigated with triplet energy transfer to four mediators annihilators, thus substantially expanding available materials TTA‐UC. By improving quality NCs, introducing mediator via direct mixing fashion, matching levels, high 10.4% (out 50% maximum) achieved in one case, which represents record performance without doping. In another photons approaching 4 eV observed, par highest energies observed optimized organic systems. Importantly, in‐depth investigation reveals that introduce key factor leads close unity efficiencies transfer, ultimately governs NC‐based These findings provide guidelines design toward solar harvesting.

Язык: Английский

Photons or Electrons? A Critical Comparison of Electrochemistry and Photoredox Catalysis for Organic Synthesis DOI
Nicholas E. S. Tay, Dan Lehnherr, Tomislav Rovis

и другие.

Chemical Reviews, Год журнала: 2021, Номер 122(2), С. 2487 - 2649

Опубликована: Ноя. 9, 2021

Redox processes are at the heart of synthetic methods that rely on either electrochemistry or photoredox catalysis, but how do and catalysis compare? Both approaches provide access to high energy intermediates (e.g., radicals) enable bond formations not constrained by rules ionic 2 electron (e) mechanisms. Instead, they 1e mechanisms capable bypassing electronic steric limitations protecting group requirements, thus enabling chemists disconnect molecules in new different ways. However, while providing similar intermediates, differ several physical chemistry principles. Understanding those differences can be key designing transformations forging disconnections. This review aims highlight these similarities between comparing their underlying principles describing impact electrochemical photochemical methods.

Язык: Английский

Процитировано

361
Photon Upconversion for Photovoltaics and Photocatalysis: A Critical Review DOI
Bryce S. Richards, Damien Hudry, Dmitry Busko

и другие.

Chemical Reviews, Год журнала: 2021, Номер 121(15), С. 9165 - 9195

Опубликована: Июль 30, 2021

Opportunities for enhancing solar energy harvesting using photon upconversion are reviewed. The increasing prominence of bifacial cells is an enabling factor the implementation upconversion, however, when realistic constraints current best-performing silicon devices considered, many challenges remain before photovoltaics operating under nonconcentrated sunlight can be enhanced via lanthanide-based upconversion. A photophysical model reveals that >1–2 orders magnitude increase in intermediate state lifetime, transfer rate, or generation rate would needed such could start to become efficient. Methods as use cosensitizers expand absorption range and plasmonics photonic structures opportunities these approaches (or combinations thereof) achieve efficient discussed. opportunity performance technologies luminescent concentrators by combining together with micro-optics also Triplet–triplet annihilation-based progressing steadily toward being relevant lower-bandgap cells. Looking photocatalysis, modeling indicates blue-to-ultraviolet lanthanide systems very inefficient. However, hope remains this direction organic visible-light-active photocatalysts.

Язык: Английский

Процитировано

305
Photophysical Properties and Redox Potentials of Photosensitizers for Organic Photoredox Transformations DOI
Thomas S. Teets, Yanyu Wu, Dooyoung Kim

и другие.

Synlett, Год журнала: 2021, Номер 33(12), С. 1154 - 1179

Опубликована: Фев. 15, 2021

Abstract Photoredox catalysis has proven to be a powerful tool in synthetic organic chemistry. The rational design of photosensitizers with improved photocatalytic performance constitutes major advancement photoredox transformations. This review summarizes the fundamental ground-state and excited-state photophysical electrochemical attributes molecular photosensitizers, which are important determinants their reactivity.

Язык: Английский

Процитировано

118
Recent Development in Sensitizers for Lanthanide-Doped Upconversion Luminescence DOI
Xingwen Cheng, Jie Zhou,

Jingyi Yue

и другие.

Chemical Reviews, Год журнала: 2022, Номер 122(21), С. 15998 - 16050

Опубликована: Окт. 4, 2022

The attractive features of lanthanide-doped upconversion luminescence (UCL), such as high photostability, nonphotobleaching or photoblinking, and large anti-Stokes shift, have shown great potentials in life science, information technology, energy materials. Therefore, UCL modulation is highly demanded toward expected emission wavelength, lifetime, relative intensity order to satisfy stringent requirements raised from a wide variety areas. Unfortunately, the majority efforts been devoted either simple codoping multiple activators variation hosts, while very little attention has paid critical role that sensitizers playing. In fact, different possess excitation wavelengths transfer pathways (to activators), which will lead features. Thus, rational design shall provide extra opportunities for tuning, particularly side. this review, we specifically focus on advances sensitizers, including current status, working mechanisms, principles, well future challenges endeavor directions.

Язык: Английский

Процитировано

114
Manipulating Exciton Dynamics toward Simultaneous High-Efficiency Narrowband Electroluminescence and Photon Upconversion by a Selenium-Incorporated Multiresonance Delayed Fluorescence Emitter DOI
Xiaosong Cao,

Ke Pan,

Jingsheng Miao

и другие.

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(50), С. 22976 - 22984

Опубликована: Дек. 7, 2022

Multiresonance thermal activated delayed fluorescence (MR-TADF) materials with an efficient spin-flip transition between singlet and triplet excited states remain demanding. Herein, we report MR-TADF compound (BN-Se) simultaneously possessing (reverse) intersystem crossing (ISC/RISC), fast radiative decay, close-to-unity quantum yield, narrowband emission by embedding a single selenium atom into common 4,4'-diazaborin framework. Benefitting from the high RISC efficiency accelerated heavy-atom effect, organic light-emitting diodes (OLEDs) based on BN-Se manifest excellent performance external of up to 32.6% ultralow roll-off 1.3% at 1000 cd m-2. Furthermore, ISC small inherent energy loss also render superior photosensitizer realize first example visible (λex > 450 nm)-to-UV (λem < 350 nm) triplet-triplet annihilation upconversion, (21.4%) extremely low threshold intensity (1.3 mW cm-2). This work not only aids in designing advanced pure molecules exciton dynamics but highlights value compounds beyond OLED applications.

Язык: Английский

Процитировано

96
Nanoengineering Triplet–Triplet Annihilation Upconversion: From Materials to Real-World Applications DOI
Tracy H. Schloemer, Pournima Narayanan, Qi Zhou

и другие.

ACS Nano, Год журнала: 2023, Номер 17(4), С. 3259 - 3288

Опубликована: Фев. 17, 2023

Using light to control matter has captured the imagination of scientists for generations, as there is an abundance photons at our disposal. Yet delivering beyond surface many photoresponsive systems proven challenging, particularly scale, due attenuation via absorption and scattering losses. Triplet–triplet annihilation upconversion (TTA-UC), a process which allows low energy be converted high photons, poised overcome these challenges by allowing precise spatial generation its nonlinear nature. With wide range sensitizer annihilator motifs available TTA-UC, researchers seek integrate materials in solution or solid-state applications. In this Review, we discuss nanoengineering deployment strategies highlight their uses recent state-of-the-art examples TTA-UC integrated both Considering implementation tactics application-specific requirements, identify critical needs push TTA-UC-based applications from academic curiosity scalable technology.

Язык: Английский

Процитировано

85
Recent advances in triplet–triplet annihilation upconversion and singlet fission, towards solar energy applications DOI Creative Commons
Andrew J. Carrod, Victor Gray, Karl Börjesson

и другие.

Energy & Environmental Science, Год журнала: 2022, Номер 15(12), С. 4982 - 5016

Опубликована: Янв. 1, 2022

Here we consolidate recent advances in the fields of triplet–triplet annihilation photon upconversion and singlet fission. We further describe their utility increasing efficiency photovoltaic devices.

Язык: Английский

Процитировано

75
Visible‐to‐UV Photon Upconversion: Recent Progress in New Materials and Applications DOI

Masanori Uji,

Till J. B. Zähringer, Christoph Kerzig

и другие.

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(25)

Опубликована: Март 8, 2023

Ultraviolet (UV, λ<400 nm) light is essential for various photochemical reactions, but its intensity in the solar spectrum very low, and sources that artificially generate high-energy UV are inefficient environmentally unfriendly. A solution to this problem photon upconversion (UC) from visible (vis, λ>400 light. Among several mechanisms, UC based on triplet-triplet annihilation (TTA-UC) particular has made remarkable progress recent years. The development of new chromophores enabled highly efficient conversion low-intensity into In review, we summarize visible-to-UV TTA-UC, their production films application processes such as catalysis, bond activation polymerization. Finally, challenges opportunities future material applications will be discussed.

Язык: Английский

Процитировано

54
Triplet–triplet annihilation photon upconversion-mediated photochemical reactions DOI
Ling Huang, Gang Han

Nature Reviews Chemistry, Год журнала: 2024, Номер 8(4), С. 238 - 255

Опубликована: Март 21, 2024

Язык: Английский

Процитировано

30
Factors that Impact Photochemical Cage Escape Yields DOI
Matthew Goodwin, John C. Dickenson, Alexia Ripak

и другие.

Chemical Reviews, Год журнала: 2024, Номер 124(11), С. 7379 - 7464

Опубликована: Май 14, 2024

The utilization of visible light to mediate chemical reactions in fluid solutions has applications that range from solar fuel production medicine and organic synthesis. These are typically initiated by electron transfer between a photoexcited dye molecule (a photosensitizer) redox-active quencher yield radical pairs intimately associated within solvent cage. Many these radicals undergo rapid thermodynamically favored "geminate" recombination do not diffuse out the cage surrounds them. Those escape useful reagents may subsequent important above-mentioned applications. process factors determine yields remain poorly understood despite decades research motivated their practical fundamental importance. Herein, state-of-the-art on light-induced appeared since seminal 1972 review J. P. Lorand entitled "The Cage Effect" is reviewed. This also provides some background for those new field discusses both homolytic bond photodissociation bimolecular induced reactions. concludes with key goals directions future promise elevate this very vibrant even greater heights.

Язык: Английский

Процитировано

18