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1.
Adv Sci (Weinh) ; 10(13): e2206560, 2023 May.
Article in English | MEDLINE | ID: mdl-36840658

ABSTRACT

Epitaxial heterostructures of colloidal lead halide perovskite nanocrystals (NCs) with other semiconductors, especially the technologically important metal chalcogenides, can offer an unprecedented level of control in wavefunction design and exciton/charge carrier engineering. These NC heterostructures are ideal material platforms for efficient optoelectronics and other applications. Existing methods, however, can only yield heterostructures with random connections and distributions of the two components. The lack of epitaxial relation and uniform geometry hinders the structure-function correlation and impedes the electronic coupling at the heterointerface. This work reports the synthesis of uniform, epitaxially grown CsPbBr3 /CdS Janus NC heterostructures with ultrafast charge separation across the electronically coupled interface. Each Janus NC contains a CdS domain that grows exclusively on a single {220} facet of CsPbBr3 NCs. Varying reaction parameters allows for precise control in the sizes of each domain and readily modulates the optical properties of Janus NCs. Transient absorption measurements and modeling results reveal a type II band alignment, where photoexcited electrons rapidly transfer (within ≈9 picoseconds) from CsPbBr3 to CdS. The promoted charge separation and extraction in epitaxial Janus NCs leads to photoconductors with drastically improved (approximately three orders of magnitude) responsivity and detectivity, which is promising for ultrasensitive photodetection.

2.
ACS Nano ; 16(9): 13674-13683, 2022 Sep 27.
Article in English | MEDLINE | ID: mdl-35867875

ABSTRACT

Precise patterning with microscale lateral resolution and widely tunable heights is critical for integrating colloidal nanocrystals into advanced optoelectronic and photonic platforms. However, patterning nanocrystal layers with thickness above 100 nm remains challenging for both conventional and emerging direct photopatterning methods, due to limited light penetration depths, complex mechanical and chemical incompatibilities, and others. Here, we introduce a direct patterning method based on a thermal mechanism, namely, the thermally activated ligand chemistry (or TALC) of nanocrystals. The ligand cross-linking or decomposition reactions readily occur under local thermal stimuli triggered by near-infrared lasers, affording high-resolution and nondestructive patterning of various nanocrystals under mild conditions. Patterned quantum dots fully preserve their structural and photoluminescent quantum yields. The thermal nature allows for TALC to pattern over 10 µm thick nanocrystal layers in a single step, far beyond those achievable in other direct patterning techniques, and also supports the concept of 2.5D patterning. The thermal chemistry-mediated TALC creates more possibilities in integrating nanocrystal layers in uniform arrays or complex hierarchical formats for advanced capabilities in light emission, conversion, and modulation.

3.
Sci Adv ; 8(11): eabm8433, 2022 Mar 18.
Article in English | MEDLINE | ID: mdl-35294230

ABSTRACT

Precise microscale patterning is a prerequisite to incorporate the emerging colloidal metal halide perovskite nanocrystals into advanced, integrated optoelectronic platforms for widespread technological applications. Current patterning methods suffer from some combination of limitations in patterning quality, versatility, and compatibility with the workflows of device fabrication. This work introduces the direct optical patterning of perovskite nanocrystals with ligand cross-linkers or DOPPLCER. The underlying, nonspecific cross-linking chemistry involved in DOPPLCER supports high-resolution, multicolored patterning of a broad scope of perovskite nanocrystals with their native ligands. Patterned nanocrystal films show photoluminescence (after postpatterning surface treatment), electroluminescence, and photoconductivity on par with those of conventional nonpatterned films. Prototype, pixelated light-emitting diodes show peak external quantum efficiency of 6.8% and luminance over 20,000 cd m-2. Both are among the highest for patterned perovskite nanocrystal devices. These results create new possibilities in the system-level integration of perovskite nanomaterials and advance their applications in various optoelectronic and photonic platforms.

4.
Anal Sci ; 34(12): 1385-1391, 2018 Dec 10.
Article in English | MEDLINE | ID: mdl-30175726

ABSTRACT

In this work, sodium dodecyl benzene sulfonate (SDBS) was used as a dispersing agent; a WO3 nanoparticle suspension was used as a sensing material. The SDBS-WO3 thin film/Sn-doped glass optical waveguide sensor element was prepared by spin coating. The sensing material was characterized by Fourier-transform infrared spectroscopy (FTIR), X-ray diffraction (XRD), and field-emission scanning electron microscopy (FESEM). The gas-sensing characteristics of the fabricated sensors were studied at room temperature for various gases. The experimental results indicate that the sensor exhibited a high selective response toward SO2 and H2S and a low detection limit of 10 ppb to SO2 and H2S. The response/recovery times for SO2 and H2S were 2/23 and 2/18 s. However, during an electrochemical gas-sensing performance test of the SDBS-WO3 film at room temperature, the results indicated that the trend of the variation in resistance was consistent with the variation in the output light.

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