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1.
ACS Appl Electron Mater ; 6(3): 1530-1541, 2024 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-38558951

RESUMO

Transition metal dichalcogenide (TMD) moiré superlattices have emerged as a significant area of study in condensed matter physics. Thanks to their superior optical properties, tunable electronic band structure, strong Coulomb interactions, and quenched electron kinetic energy, they offer exciting avenues to explore correlated quantum phenomena, topological properties, and light-matter interactions. In recent years, scanning tunneling microscopy (STM) has made significant impacts on the study of these fields by enabling intrinsic surface visualization and spectroscopic measurements with unprecedented atomic scale detail. Here, we spotlight the key findings and innovative developments in imaging and characterization of TMD heterostructures via STM, from its initial implementation on the in situ grown sample to the latest photocurrent tunneling microscopy. The evolution in sample design, progressing from a conductive to an insulating substrate, has not only expanded our control over TMD moiré superlattices but also promoted an understanding of their structures and strongly correlated properties, such as the structural reconstruction and formation of generalized two-dimensional Wigner crystal states. In addition to highlighting recent advancements, we outline upcoming challenges, suggest the direction of future research, and advocate for the versatile use of STM to further comprehend and manipulate the quantum dynamics in TMD moiré superlattices.

2.
J Phys Chem Lett ; 14(33): 7581-7590, 2023 Aug 24.
Artigo em Inglês | MEDLINE | ID: mdl-37590125

RESUMO

It is necessary to improve the action cross section (η × σn) of high-order multiphoton absorption (MPA) for fundamental research and practical applications. Herein, the core-shell FAPbBr3/CsPbBr3 nanocrystals (NCs) were constructed, and fluorescence induced by up to five-photon absorption was observed. The value of η × σ5 reaches 8.64 × 10-139 cm10 s4 photon-4 nm-3 at 2300 nm, which is nearly an order of magnitude bigger than that of the core-only NCs. It is found that the increased dielectric constant promotes modulation of MPA effects, addressing the electronic distortion in high-order nonlinear behaviors through the local field effect. Meanwhile, the quasi-type-II band alignment suppresses the biexciton Auger recombination, ensuring the stronger MPA induced fluorescence. In addition, the core-shell structure can not only reduce the defect density but also promote the nonradiative energy transfer though the antenna-like effect. This work provides a new avenue for the exploitation of high-performance multiphoton excited nanomaterials for future photonic integration.

3.
Nanomicro Lett ; 15(1): 156, 2023 Jun 19.
Artigo em Inglês | MEDLINE | ID: mdl-37337117

RESUMO

For the further improvement of the power conversion efficiency (PCE) and stability of perovskite solar cells (PSCs), the buried interface between the perovskite and the electron transport layer is crucial. However, it is challenging to effectively optimize this interface as it is buried beneath the perovskite film. Herein, we have designed and synthesized a series of multifunctional organic-inorganic (OI) complexes as buried interfacial material to promote electron extraction, as well as the crystal growth of the perovskite. The OI complex with BF4- group not only eliminates oxygen vacancies on the SnO2 surface but also balances energy level alignment between SnO2 and perovskite, providing a favorable environment for charge carrier extraction. Moreover, OI complex with amine (- NH2) functional group can regulate the crystallization of the perovskite film via interaction with PbI2, resulting in highly crystallized perovskite film with large grains and low defect density. Consequently, with rational molecular design, the PSCs with optimal OI complex buried interface layer which contains both BF4- and -NH2 functional groups yield a champion device efficiency of 23.69%. More importantly, the resulting unencapsulated device performs excellent ambient stability, maintaining over 90% of its initial efficiency after 2000 h storage, and excellent light stability of 91.5% remaining PCE in the maximum power point tracking measurement (under continuous 100 mW cm-2 light illumination in N2 atmosphere) after 500 h.

4.
Adv Sci (Weinh) ; 9(29): e2203640, 2022 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-36057995

RESUMO

Perovskite solar cells (PSCs) via two-step sequential method have received great attention in recent years due to their high reproducibility and low processing costs. However, the relatively high trap-state density and poor charge carrier extraction efficiency pose challenges. Herein, highly efficient and stable PSCs via a two-step sequential method are fabricated using organic-inorganic (OI) complexes as multifunctional interlayers. In addition to reduce the under-coordinated Pb2+ ions related trap states by forming interactions with the functional groups, the complexes interlayer tends to form dipole moment which can enhance the built-in electric field, thus facilitating charge carrier extraction. Consequently, with rational molecular design, the resulting devices with a vertical dipole moment that parallels with the built-in electric field yield a champion efficiency of 23.55% with negligible hysteresis. More importantly, the hydrophobicity of the (OI) complexes contributes to an excellent ambient stability of the resulting device with 91% of initial efficiency maintained after 3000 h storage.

5.
Adv Sci (Weinh) ; 9(11): e2106054, 2022 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-35152567

RESUMO

All-inorganic CsPbIBr2 perovskite solar cells (PSCs) have recently gained growing attention as a promising template to solve the thermal instability of organic-inorganic PSCs. However, the relatively low device efficiency hinders its further development. Herein, highly efficient and stable CsPb0.7 Sn0.3 IBr2 compositional perovskite-based inorganic PSCs are fabricated by introducing appropriate amount of multifunctional zinc oxalate (ZnOX). In addition to offset Pb and Sn vacancies through Zn2+ ions incorporation, the oxalate group can strongly interact with undercoordinated metal ions to regulate film crystallization, delivering perovskite film with low defect density, high crystallinity, and superior electronic properties. Correspondingly, the resulting device delivers a champion efficiency of 14.1%, which presents the highest reported efficiency for bromine-rich inorganic PSCs thus far. More importantly, chemically reducing oxalate group can effectively suppress the notorious oxidation of Sn2+ , leading to significant enhancement on air stability.

6.
Adv Mater ; 33(21): e2100466, 2021 May.
Artigo em Inglês | MEDLINE | ID: mdl-33788315

RESUMO

Perovskite materials and their optoelectronic devices have attracted intensive attentions in recent years. However, it is difficult to further improve the performance of perovskite devices due to the poor stability and the intrinsic deep level trap states (DLTS), which are caused by surface dangling bonds and grain boundaries. Herein, the CH3 NH3 PbBr3 perovskite microcrystal is encapsulated by a dense Al2 O3 layer to form a microenvironment. Through optical measurement, it is found that the structure of perovskite can be healed by itself even under high temperature and long-time laser illumination. The DLTS density decreases nearly an order of magnitude, which results in 4-14 times enhancement of light emission. The observation is ascribed to the micron-level environment, which serves as a self-sufficient high-vacuum growth chamber, where the components of the perovskite are completely retained when sublimated and the decomposed atoms can re-arrange after thermal treatment. The modified structure showing high thermal stability is able to maintain excellent optical and lasing stability up to 2 years. This discovery provides a new idea and perspective for improving the stability of perovskite and can be of practical interest for perovskite device application.

7.
Nanoscale ; 12(25): 13360-13367, 2020 Jul 02.
Artigo em Inglês | MEDLINE | ID: mdl-32458915

RESUMO

Perovskite materials are very sensitive to the environment which is beneficial for humidity sensing. However, the existing illuminating humidity sensor has low luminous efficiency and sensitivity. Besides, the stability of perovskite materials remains a key issue to be resolved. Compared to luminescence, lasing is much more sensitive to the surrounding environmental situation. However, humidity sensing based on perovskite lasing has not been reported so far. In this work, all-inorganic halide perovskite CsPbBr3 nanorods with an optical gain coefficient as high as 954 cm-1 were designed and fabricated. Moreover, a microscale hydrophobic zeolite was introduced to modify perovskites for improved stability. It is interesting to note that the hydrophobic zeolite introduces strong scattering which is beneficial for three-dimensional random lasing with a quality (Q) factor of 2263. Through the strategy of using lasing instead of luminescence, optical stability and sensitive laser humidity sensing were demonstrated, and it exhibits high sensitivity and good reliability. This work provides a new idea of improved stability of perovskites, which will promote the practical application of perovskite materials and devices.

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