Perspectives in Dye Chemistry: A Rational Approach toward Functional Materials by Understanding the Aggregate State

Journal of the American Chemical Society, Год журнала: 2021, Номер 143(12), С. 4500 - 4518

Опубликована: Март 15, 2021

The past 20 years have witnessed a renaissance of dye chemistry, moving from traditional colorant research toward functional materials. Different research, the properties materials are governed extensively by intermolecular interactions, thereby entailing significant limitations to classical approach based on molecular structure–molecular property (color, emission, redox properties, etc.) relationships for respective molecules. However, as discussed in this Perspective, such an can be pursued aggregates, and many cases already well-tailored dimers sufficient understand influence supramolecular organization ground photoexcited states. Illustrative examples will given exciton coupling charge-transfer how these relate desirable functions fluorescence, symmetry-breaking charge separation, singlet fission aggregates. While progress so far mostly originated studies well-defined folded self-assembled structures composed only two molecules, future work advance larger oligomers specific size geometry. Furthermore, experimental should guided extent theoretical predictions that may supported machine learning algorithms new concepts artificial intelligence. Beyond calculations potential energy landscapes, we suggest development approaches identify most aggregate particular landscapes.

Язык: Английский

---

Luminescence in Crystalline Organic Materials: From Molecules to Molecular Solids

Advanced Optical Materials, Год журнала: 2021, Номер 9(13)

Опубликована: Апрель 30, 2021

Abstract Luminescent small, all‐organic molecules are of tremendous interest in materials and life science applications. Nevertheless, targeted design requires a basic understanding the excited state deactivation pathways themselves, modulations processes that occur solid state. This particularly concerns crystalline molecular solids, as here not only solid‐state rigidification contributes to these modulations, but specific intermolecular interactions well. Starting from properties, this work carefully disentangles all intramolecular factors radiative nonradiative solids provide guidelines for design.

Язык: Английский

---

In Situ Hypoxia-Induced Supramolecular Perylene Diimide Radical Anions in Tumors for Photothermal Therapy with Improved Specificity

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(5), С. 2360 - 2367

Опубликована: Янв. 20, 2022

Considering that hypoxia is closely associated with tumor proliferation, invasion, metastasis, and drug resistance, it of great significance to overcome in treatment. Herein, we report a hypoxia-induced specific photothermal therapy (PTT) based on the agent supramolecular perylene diimide radical anions. Hypoxic regions various tumors display strong reductive ability, such environments complex derivative cucurbit[7]uril could be reduced Benefiting from NIR absorption good conversion performance situ generated anions, PTT strategy exhibits excellent therapeutic efficiency as well specificity biological safety. Moreover, inducible factor expression decreases normal level after It anticipated opens new horizons for against hypoxic improved

Язык: Английский

---

Slip‐Stacked J‐Aggregate Materials for Organic Solar Cells and Photodetectors

Advanced Materials, Год журнала: 2021, Номер 34(22)

Опубликована: Окт. 19, 2021

Abstract Dye–dye interactions affect the optical and electronic properties in organic semiconductor films of light harvesting detecting optoelectronic applications. This review elaborates how to tailor these semiconductors for solar cells (OSCs) photodiodes (OPDs). While devices rely on similar materials, demands their are rather different, former requiring a broad absorption spectrum spanning from UV over visible up near‐infrared region latter an ultra‐narrow at specific, targeted wavelength. In order design satisfying demands, fundamental insights relationship provided depending molecular packing arrangement resultant coupling thereof. Based recent advancements theoretical understanding intermolecular between slip‐stacked dyes, distinguishing classical J‐aggregates with predominant long‐range Coulomb charge transfer (CT)‐mediated or ‐coupled J‐aggregates, whose red‐shifts primarily governed by short‐range orbital interactions, is suggested. Within this framework, aggregate structure functional representative classes dye aggregates analyzed most advanced OSCs wavelength‐selective OPDs, providing important into rational thin‐film materials.

Язык: Английский

---

An Efficient Narrowband Near‐Infrared at 1040 nm Organic Photodetector Realized by Intermolecular Charge Transfer Mediated Coupling Based on a Squaraine Dye

Advanced Materials, Год журнала: 2021, Номер 33(26)

Опубликована: Май 31, 2021

A highly sensitive short-wave infrared (SWIR, λ > 1000 nm) organic photodiode (OPD) is described based on a well-organized nanocrystalline bulk-heterojunction (BHJ) active layer composed of dicyanovinyl-functionalized squaraine dye (SQ-H) donor material in combination with PC

Язык: Английский

---

There is still plenty of room for layer-by-layer assembly for constructing nanoarchitectonics-based materials and devices

Physical Chemistry Chemical Physics, Год журнала: 2021, Номер 24(7), С. 4097 - 4115

Опубликована: Дек. 2, 2021

While the layer-by-layer (LbL) assembly method has already reached a certain maturity, there is still plenty of room for expanding its usefulness fabrication nanoarchitectonics-based materials and devices.

Язык: Английский

---

Anti‐Quenching NIR‐II J‐Aggregates of Benzo[c]thiophene Fluorophore for Highly Efficient Bioimaging and Phototheranostics

Advanced Materials, Год журнала: 2023, Номер 35(20)

Опубликована: Март 3, 2023

Molecular fluorophores with the second near-infrared (NIR-II) emission hold great potential for deep-tissue bioimaging owing to their excellent biocompatibility and high resolution. Recently, J-aggregates are used construct long-wavelength NIR-II emitters as optical bands show remarkable red shifts upon forming water-dispersible nano-aggregates. However, wide applications in fluorescence imaging impeded by limited varieties of J-type backbone serious quenching. Herein, a bright benzo[c]thiophene (BT) J-aggregate fluorophore (BT6) anti-quenching effect is reported highly efficient phototheranostics. The BT manipulated have Stokes shift over 400 nm aggregation-induced (AIE) property conquering self-quenching issue fluorophores. Upon BT6 assemblies an aqueous environment, absorption 800 1000 boosted more than 41 26 folds, respectively. In vivo visualization whole-body blood vessel imaging-guided phototherapy results verify that NPs agent cancer This work develops strategy precisely properties biomedical applications.

Язык: Английский

---

Nitric‐Oxide‐Releasing aza‐BODIPY: A New Near‐Infrared J‐Aggregate with Multiple Antibacterial Modalities

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(32)

Опубликована: Июнь 3, 2022

The development of near-infrared (NIR) J-aggregates has received increasing attention due to their broad applications. Here, we report the nitrosation an amine-containing aza-BODIPY precursor (BDP-NH2 ), affording first nitric oxide (NO)-releasing NIR J-aggregate (BDP-NO). introduction N-nitrosamine moieties efficiently inhibits aromatic interactions BDP-NH2 , which instead promotes formation within micellar nanoparticles with a remarkable bathochromic shift ≈109 nm window (820 nm). Interestingly, NO release and photothermal conversion efficiency (PTCE) can be delicately tuned by loading contents BDP-NO nanoparticles, thereby enabling multiple antibacterial modalities exploring either release, therapy (PTT), or both. We demonstrate combination PTT elevate activity while attenuating PTT-associated inflammation for in vivo treatment MRSA infection.

Язык: Английский

---

Supramolecular polymers: Recent advances based on the types of underlying interactions

Progress in Polymer Science, Год журнала: 2022, Номер 137, С. 101635 - 101635

Опубликована: Дек. 14, 2022

Язык: Английский

---

J‐Aggregation Strategy toward Potentiated NIR‐II Fluorescence Bioimaging of Molecular Fluorophores

Advanced Materials, Год журнала: 2023, Номер 36(1)

Опубликована: Авг. 1, 2023

Molecular fluorophores emitting in the second near-infrared (NIR-II, 1000-1700 nm) window with strong optical harvesting and high quantum yields hold great potential for vivo deep-tissue bioimaging high-resolution biosensing. Recently, J-aggregates are harnessed to engineer long-wavelength NIR-II emitters show unique superiority tumor detection, vessel mapping, surgical navigation, phototheranostics due their bathochromic-shifted bands required slip-stacked arrangement aggregation state. However, despite preliminary progress of theoretical study structure-property relationships, further paradigms remain scarce lack on aggregated fashion. In this effort, how utilize specific molecular structure form packing motifs J-type exciton coupling is emphatically elucidated. First, several regulating strategies achieve containing intermolecular interactions external conditions positively summarized deeply analyzed. Then, recent reports theranostics systematically provide a clear reference direction promoting development organic fluorophores. Eventually, prospective efforts ameliorating clinical practices outlined.

Язык: Английский

---