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1.
ACS Nano ; 18(33): 22220-22232, 2024 Aug 20.
Artigo em Inglês | MEDLINE | ID: mdl-39107108

RESUMO

Chiral molecules, a cornerstone of chemical sciences with applications ranging from pharmaceuticals to molecular electronics, come in mirror-image pairs called enantiomers. However, their synthesis often requires complex control of their molecular geometry. We propose a strategy called "electromagnetic enantiomers" for inducing chirality in molecules located within engineered nanocavities using light, eliminating the need for intricate molecular design. This approach works by exploiting the strong coupling between a nonchiral molecule and a chiral mode within a nanocavity. We provide evidence for this strong coupling through angular emission patterns verified by numerical simulations and with complementary evidence provided by luminescence lifetime measurements. In simpler terms, our hypothesis suggests that chiral properties can be conveyed on to a molecule with a suitable chromophore by placing it within a specially designed chiral nanocavity that is significantly larger (hundreds of nanometers) than the molecule itself. To demonstrate this concept, we showcase an application in display technology, achieving efficient emission of circularly polarized light from a nonchiral molecule. The electromagnetic enantiomer concept offers a simpler approach to chiral control, potentially opening doors for asymmetric synthesis.

2.
ACS Appl Mater Interfaces ; 16(15): 19551-19562, 2024 Apr 17.
Artigo em Inglês | MEDLINE | ID: mdl-38567787

RESUMO

Highly conductive, transparent, and easily available materials are needed in a wide range of devices, such as sensors, solar cells, and touch screens, as alternatives to expensive and unsustainable materials such as indium tin oxide. Herein, electrospinning was employed to develop fibers of PEDOT:PSS/silver nanowire (AgNW) composites on various substrates, including poly(caprolactone) (PCL), cotton fabric, and Kapton. The influence of AgNWs, as well as the applied voltage of electrospinning on the conductivity of fibers, was thoroughly investigated. The developed fibers showed a sheet resistance of 7 Ω/sq, a conductivity of 354 S/cm, and a transmittance value of 77%, providing excellent optoelectrical properties. Further, the effect of bending on the fibers' electrical properties was analyzed. The sheet resistance of fibers on the PCL substrate increased slightly from 7 to 8 Ω/sq, after 1000 bending cycles. Subsequently, as a proof of concept, the nanofibers were evaluated as electrode material in a triboelectric nanogenerator (TENG)-based energy harvester, and they were observed to enhance the performance of the TENG device (78.83 V and 7 µA output voltage and current, respectively), as compared to the same device using copper electrodes. These experiments highlight the untapped potential of conductive electrospun fibers for flexible and transparent electronics.

3.
Beilstein J Org Chem ; 20: 672-674, 2024.
Artigo em Inglês | MEDLINE | ID: mdl-38590539
8.
Mater Horiz ; 10(11): 5087-5098, 2023 Oct 30.
Artigo em Inglês | MEDLINE | ID: mdl-37681478

RESUMO

Poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) is a material that has become ubiquitous in the field of organic electronics. It is most commonly used as a hole transport layer (HTL) in optoelectronic devices and can be purchased commercially in various formulations with different properties. Whilst it is a most convenient material to work with, there are stability issues associated with PEDOT:PSS that are detrimental to device stability and these are due to the acidic nature of the PSS component. In this paper, we present a molecular, non-acidic alternative to PEDOT:PSS. The parent structure is composed of a quater(3,4-ethylenedioxythiophene) unit capped either side of the short chain with two pyridine units. This compound, termed (BEDOTPy)2, can be prepared chemically and electrochemically to give doped materials with a choice of counteranions. Further functionalisation via quaternisation at the nitrogen atoms allows for modification of solubility and film-forming properties. The conductivity of the doped samples can reach up to 3.75 S cm-1. The materials are non-acidic and are therefore attractive alternatives to PEDOT:PSS for device applications. We demonstrate an OLED device using the compound (BEDOTPy-EtOH-I)2PF6 as an HTL, and compare the device performance to one made with PEDOT:PSS. Due to the non-acidic nature of the molecular material, the corresponding OLED device does not show a drop in luminance over time, whereas a loss of performance is observed for the device containing PEDOT:PSS over a short period. These results are presented to introduce the parent compound (BEDOTPy)2 as an attractive alternative to PEDOT:PSS, which can be easily modified chemically to provide a plethora of potential compounds with tunable properties.

9.
Nature ; 621(7980): 746-752, 2023 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-37758890

RESUMO

Organic semiconductors are carbon-based materials that combine optoelectronic properties with simple fabrication and the scope for tuning by changing their chemical structure1-3. They have been successfully used to make organic light-emitting diodes2,4,5 (OLEDs, now widely found in mobile phone displays and televisions), solar cells1, transistors6 and sensors7. However, making electrically driven organic semiconductor lasers is very challenging8,9. It is difficult because organic semiconductors typically support only low current densities, suffer substantial absorption from injected charges and triplets, and have additional losses due to contacts10,11. In short, injecting charges into the gain medium leads to intolerable losses. Here we take an alternative approach in which charge injection and lasing are spatially separated, thereby greatly reducing losses. We achieve this by developing an integrated device structure that efficiently couples an OLED, with exceptionally high internal-light generation, with a polymer distributed feedback laser. Under the electrical driving of the integrated structure, we observe a threshold in light output versus drive current, with a narrow emission spectrum and the formation of a beam above the threshold. These observations confirm lasing. Our results provide an organic electronic device that has not been previously demonstrated, and show that indirect electrical pumping by an OLED is a very effective way of realizing an electrically driven organic semiconductor laser. This provides an approach to visible lasers that could see applications in spectroscopy, metrology and sensing.

10.
Adv Mater ; : e2302259, 2023 Apr 22.
Artigo em Inglês | MEDLINE | ID: mdl-37086184

RESUMO

The field of synthetic metals is, and remains, highly influential for the development of organic semiconductor materials. Yet, with the passing of time and the rapid development of conjugated materials in recent years, the link between synthetic metals and organic semiconductors is at risk of being forgotten. This review reflects on one of the key concepts developed in synthetic metals - heteroatom interactions. The application of this strategy in recent organic semiconductor materials, small molecules and polymers, is highlighted, with analysis of X-ray crystal structures and comparisons with model systems used to determine the influence of these non-covalent short contacts. The case is made that the wide range of effective heteroatom interactions and the high performance that has been achieved in devices from organic solar cells to transistors is testament to the seeds sown by the synthetic metals research community.

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