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1.
Phys Rev Lett ; 128(4): 047402, 2022 Jan 28.
Article in English | MEDLINE | ID: mdl-35148132

ABSTRACT

We perform first-principles GW plus Bethe-Salpeter equation calculations to investigate the photophysics of monolayer hexagonal boron nitride (h-BN), revealing excitons with novel k-space characteristics. The excitonic states forming the first and third peaks in its absorption spectrum are s-like, but those of the second peak are notably p-like, a first finding of strong co-occurrence of bright s-like and bright p-like states in an intrinsic 2D material. Moreover, even though the k-space wave function of these excitonic states are centered at the K and K^{'} valleys as in monolayer transition metal dichalcogenides, the k-space envelope functions of the basis excitons at one valley have significant extents to the basin of the other valley. As a consequence, the optical response of monolayer h-BN exhibits a lack of circular dichroism, as well as a coupling that induces an intervalley mixing between s- and p-like states.

2.
ACS Appl Mater Interfaces ; 13(47): 56630-56637, 2021 Dec 01.
Article in English | MEDLINE | ID: mdl-34794311

ABSTRACT

Interfacial quality of functional layers plays an important role in the carrier transport of sandwich-structured devices. Although the suppression of interface states is crucial to the overall device performance, our understanding on their formation and annihilation mechanism via direct characterization is still quite limited. Here, we present a thorough study on the interface states present in the electron transport layer (ETL) of blue quantum dot (QD) light-emitting diodes (QLEDs). A ZnO/ZnMgO bilayer ETL is adopted to enhance the electron injection into blue QDs. By probing the ETL band structure with photoelectron spectroscopy, we discover that substantial band bending exists at the ZnO/ZnMgO interface, elucidating the presence of a high density of interface states which hinder electron transport. By inserting a ZnO@ZMO interlayer composed of mixed ZnO and ZnMgO nanoparticles, the band bending and thus the interface states are observed to reduce significantly. We attribute this to the hybrid surface properties of ZnO@ZMO, which can annihilate the surface states of both the ZnO and ZnMgO layers. The introduction of a bridging layer has led to ∼40% enhancement in the power efficiency of blue QLEDs and noticeable performance boosts in green and red QLEDs. The findings here demonstrate a direct observation of interface states via detailed band structure studies and outline a potential pathway for eliminating these states for better performances in sandwich-structured devices.

3.
ACS Appl Mater Interfaces ; 13(41): 49058-49065, 2021 Oct 20.
Article in English | MEDLINE | ID: mdl-34633792

ABSTRACT

With many advantages including superior color saturation and efficiency, quantum dot light-emitting diodes (QLEDs) are considered a promising candidate for the next-generation displays. Emission uniformity over the entire device area is a critical factor to the overall performance and reliability of QLEDs. In this work, we performed a thorough study on the origin of dark spots commonly observed in operating QLEDs and developed a strategy to eliminate these defects. Using advanced cross section fabrication and imaging techniques, we discovered the occurrence of voids in the organic hole transport layer and directly correlated them to the observed emission nonuniformity. Further investigations revealed that these voids are thermal damages induced during the subsequent thermal deposition of other functional layers and can act as leakage paths in the device. By inserting a thermo-tolerant 1,4,5,8,9,11-hexaazatriphenylene-hexacarbonitrile (HATCN) interlayer with an optimized thickness, the thermally induced dark spots can be completely suppressed, leading to a current efficiency increase by 18%. We further demonstrated that such a thermal passivation strategy can work universally for various types of organic layers with low thermal stability. Our findings here provide important guidance in enhancing the performances and reliability of QLEDs and also other sandwich-structured devices via the passivation of heat-sensitive layers.

4.
Small ; 17(43): e2101359, 2021 Oct.
Article in English | MEDLINE | ID: mdl-34121319

ABSTRACT

Colloidal all-inorganic perovskites nanocrystals (NCs) have emerged as a promising material for display and lighting due to their excellent optical properties. However, blue emissive NCs usually suffer from low photoluminescence quantum yields (PLQYs) and poor stability, rendering them the bottleneck for full-color all-perovskite optoelectronic applications. Herein, a facile approach is reported to enhance the emission efficiency and stability of blue emissive perovskite nano-structures via surface passivation with potassium bromide. By adding potassium oleate and excess PbBr2 to the perovskite precursor solutions, potassium bromide-passivated (KBr-passivated) blue-emitting (≈450 nm) CsPbBr3 nanoplatelets (NPLs) is successfully synthesized with a respectably high PLQY of 87%. In sharp contrast to most reported perovskite NPLs, no shifting in emission wavelength is observed in these passivated NPLs even after prolonged exposures to intense irradiations and elevated temperature, clearly revealing their excellent photo- and thermal-stabilities. The enhancements are attributed to the formation of K-Br bonding on the surface which suppresses ion migration and formation of Br-vacancies, thus improving both the PL emission and stability of CsPbBr3 NPLs. Furthermore, all-perovskite white light-emitting diodes (WLEDs) are successfully constructed, suggesting that the proposed KBr-passivated strategy can promote the development of the perovskite family for a wider range of optoelectronic applications.

5.
Nanomaterials (Basel) ; 9(7)2019 Jul 19.
Article in English | MEDLINE | ID: mdl-31331029

ABSTRACT

Here, we report the extraordinary electrochemical energy storage capability of NiMoO4@NiMoO4 homogeneous hierarchical nanosheet-on-nanowire arrays (SOWAs), synthesized on nickel substrate by a two-stage hydrothermal process. Comparatively speaking, the SOWAs electrode displays superior electrochemical performances over the pure NiMoO4 nanowire arrays. Such improvements can be ascribed to the characteristic homogeneous hierarchical structure, which not only effectively increases the active surface areas for fast charge transfer, but also reduces the electrode resistance significantly by eliminating the potential barrier at the nanowire/nanosheet junction, an issue usually seen in other reported heterogeneous architectures. We further evaluate the performances of the SOWAs by constructing an asymmetric hybrid supercapacitor (ASC) with the SOWAs and activated carbon (AC). The optimized ASC shows excellent electrochemical performances with 47.2 Wh/kg in energy density of 1.38 kW/kg at 0-1.2 V. Moreover, the specific capacity retention can be as high as 91.4% after 4000 cycles, illustrating the remarkable cycling stability of the NiMoO4@NiMoO4//AC ASC device. Our results show that this unique NiMoO4@NiMoO4 SOWA has great prospects for future energy storage applications.

7.
J Phys Chem B ; 110(39): 19285-90, 2006 Oct 05.
Article in English | MEDLINE | ID: mdl-17004781

ABSTRACT

Mass spectrometry and thermogravimetric analysis are used to explore the thermal decomposition of carbon precursors (primarily the tripropylammonium cations) occluded within AlPO(4)-5 (AFI) crystals prepared in various media (in the presence or absence of F(-) ions, Si(4+) substations of P(5+)), with the aim to fabricate high-density 0.4-nm single-walled carbon nanotubes (SWNTs). It has been found that the tripropylammonium precursors exist in the as-synthesized crystals in three different forms: tripropylammonium fluoride, hydroxide, and tripropylammonium cation compensating for the negative charge of the framework. The latter is bonded to the framework by strong chemical interaction and its decomposition takes place by a series of beta-elimination reactions to give propylene and ammonia, with the stepwise formation of dipropylammonium and n-propylammonium cations. The 0.4-nm SWNTs filling density was found to be higher than that resulting from the carbon precursor of tripropylammonium fluoride and hydroxide, because of the strong adsorption force of the channel walls to pyrolysate, as evidenced by the clear and strong radial breathing modes in Raman spectra.

8.
J Am Chem Soc ; 127(46): 16111-9, 2005 Nov 23.
Article in English | MEDLINE | ID: mdl-16287298

ABSTRACT

We report the fabrication process of isolated one-dimensional Se chains incorporated in the matrix of AlPO4-5 single crystals and the experimental investigation of the geometry, phase stability, electronic properties, and electron-phonon coupling effect of these Se chains. The structure of the helical Se chains inside the channels is discussed on the basis of X-ray scattering measurements. Thermal analysis and temperature-dependent micro-Raman measurements show that Se single chains are flexible and can convert from a weak distorted phase into another phase with strongly disordered structure ("melting" state) around 340 K. Since the electrons are confined in the one-dimensional channels, the absorption band of the Se chain is obviously blue shifted compared with that of trigonal Se. With increasing temperature, this band shifts linearly to the lower energy side, in sharp contrast to the nonlinear temperature coefficient of trigonal Se, which is attributed to the greatly diminished interchain interaction and the weakening of the electron-optical phonon coupling in a low-dimensional system. In the vicinity of the absorption band, both first-order and second-order Raman signals for the Se chain are enhanced, due to the strong electron-phonon coupling when the excitation laser energy matches the electronic transition in isolated Se chains.

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