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1.
Nanoscale Adv ; 5(23): 6724-6735, 2023 Nov 21.
Artículo en Inglés | MEDLINE | ID: mdl-38024291

RESUMEN

Low-temperature cracking and rutting are the most destructive problems of bitumen that hinder the application of high-performance bitumen engineering, which is dependent on its glass transition temperature (Tg). Through in silico studies, this work has systematically investigated the Tg of a bituminous binder with the addition of diamond nanothread (DNT) fillers with varying filler content, alignment, distribution, and functional groups. In general, the glass transition phenomenon of the bitumen is determined by the mobility of its constituent molecules. Tg is found to increase gradually with the increase in the weight percentage of DNT and then decreases when the weight percentage exceeds 5.05 wt%. The enhancement effect on Tg is weakened when DNTs are distributed vertically or functionalized with functional groups. Specifically, DNT fillers induce inhomogeneity, which promotes the motion of small molecules while hindering the motion of large molecules. The aggregation of DNTs and the molecular environment in the vicinity of DNTs directly affect Tg. In summary, aggregation and adhesion are the dominant mechanisms affecting the mobility of the constituent molecules in the DNT/bitumen system and thus its glass transition temperature. This work provides in-depth insights into the underlying mechanisms for the glass transition of a bituminous binder, which could serve as theoretical guidance for tuning the low-temperature performance of the bituminous binder.

2.
Sensors (Basel) ; 23(15)2023 Jul 28.
Artículo en Inglés | MEDLINE | ID: mdl-37571533

RESUMEN

Structural-response reconstruction is of great importance to enrich monitoring data for better understanding of the structural operation status. In this paper, a data-driven based structural-response reconstruction approach by generating response data via a convolutional process is proposed. A conditional generative adversarial network (cGAN) is employed to establish the spatial relationship between the global and local response in the form of a response nephogram. In this way, the reconstruction process will be independent of the physical modeling of the engineering problem. The validation via experiment of a steel frame in the lab and an in situ bridge test reveals that the reconstructed responses are of high accuracy. Theoretical analysis shows that as the sensor quantity increases, reconstruction accuracy rises and remains when the optimal sensor arrangement is reached.

3.
J Am Chem Soc ; 145(24): 13326-13334, 2023 Jun 21.
Artículo en Inglés | MEDLINE | ID: mdl-37279071

RESUMEN

Many optoelectronic processes in colloidal semiconductor nanocrystals (NCs) suffer an efficiency decline under high-intensity excitation. This issue is caused by Auger recombination of multiple excitons, which converts the NC energy into excess heat, reducing the efficiency and life span of NC-based devices, including photodetectors, X-ray scintillators, lasers, and high-brightness light-emitting diodes (LEDs). Recently, semiconductor quantum shells (QSs) have emerged as a promising NC geometry for the suppression of Auger decay; however, their optoelectronic performance has been hindered by surface-related carrier losses. Here, we address this issue by introducing quantum shells with a CdS-CdSe-CdS-ZnS core-shell-shell-shell multilayer structure. The ZnS barrier inhibits the surface carrier decay, which increases the photoluminescence (PL) quantum yield (QY) to 90% while retaining a high biexciton emission QY of 79%. The improved QS morphology allows demonstrating one of the longest Auger lifetimes reported for colloidal NCs to date. The reduction of nonradiative losses in QSs also leads to suppressed blinking in single nanoparticles and low-threshold amplified spontaneous emission. We expect that ZnS-encapsulated quantum shells will benefit many applications exploiting high-power optical or electrical excitation regimes.

4.
J Phys Chem Lett ; 13(39): 8987-8992, 2022 Oct 06.
Artículo en Inglés | MEDLINE | ID: mdl-36149015

RESUMEN

Using the cation-exchange method, colloidal PbS nanoribbons are converted completely into CdS nanoribbons. This process expands the emission spectrum of the nanoribbons from infrared to visible. The morphology of nanoribbons remains the same after cation exchange, but the crystal structure changes from rock salt to zincblende. CdS nanoribbons exhibit blue band-edge photoluminescence under ultraviolet-light excitation. Cathodoluminescence spectroscopy of the CdS nanoribbons shows multicolor (blue, green, and red) emissions. Further time-resolved photoluminescence spectroscopy studies show that the lifetime of the midgap states is more than 2 orders of magnitude longer than that of the band-edge states.

5.
J Phys Chem Lett ; 13(33): 7756-7761, 2022 Aug 25.
Artículo en Inglés | MEDLINE | ID: mdl-35969488

RESUMEN

Two-dimensional colloidal PbS nanosheets exhibit more than one order of magnitude larger exciton binding energy than their bulk counterpart, making it possible to generate stable excitons at room temperature. It is experimentally revealed that the binding energy of the exciton increases from 26 to 68 meV as the thickness of the PbS nanosheet decreases from 4.7 to 1.2 nm. The dielectric confinement of the exciton plays a critical role in the binding-energy enhancement. The large binding energy results in a fast thickness-dependent exciton radiative recombination rate, confirmed experimentally.

6.
J Phys Chem Lett ; 12(1): 232-237, 2021 Jan 14.
Artículo en Inglés | MEDLINE | ID: mdl-33326246

RESUMEN

Charged facets of a nanocrystal can form an intrinsic nanometer-size electric dipole. When the spacing between these nano dipoles is adjusted, the dipolar interaction energy is tuned from a fraction to a multiple of the thermal energy. Consequently, the one-dimensional oriented attachment can be switched on or off, as is the growth of nanorods. This kinetically controlled growth is achieved at relatively low reaction temperatures while the thermodynamically controlled growth dominates at higher temperatures. The synthesized PbSe nanorods are branchless, exhibiting a single-exponential photoluminescence decay trace with an e-folding lifetime of 1.3 µs and a photoluminescence quantum yield of 35%.

7.
Adv Mater ; 29(10)2017 Mar.
Artículo en Inglés | MEDLINE | ID: mdl-28092130

RESUMEN

A PbS monolayer is demonstrated to be a novel platform for topological, valleytronic, and optical phenomena. Compressive strain can turn the trivial monolayer into a topological insulator. Optical pumping can facilitate charge, spin, and valley Hall effects tunable by external strain and light ellipticity. Similar results apply to other IV-VI semiconductors.

8.
Phys Chem Chem Phys ; 17(36): 23303-7, 2015 Sep 28.
Artículo en Inglés | MEDLINE | ID: mdl-26299359

RESUMEN

Dual photoluminescence peaks observed during the synthesis of colloidal PbS nanosheets reveal their growth mechanism - two-dimensional attachments of the quantum dots. Well-grown nanosheets show the photoluminescence linewidth of 95 meV at room temperature. Aged nanosheets in toluene have enhanced photoluminescence with intensity improved by an order of magnitude.

9.
Carbohydr Polym ; 118: 150-5, 2015 Mar 15.
Artículo en Inglés | MEDLINE | ID: mdl-25542120

RESUMEN

Regenerated cellulose fiber, fiber extrudate, and film were produced from cellulose solution prepared with raw pulp and ionic liquid solvent 1-butyl-3-methylimidazolium chloride ([BMIM]Cl). Spinning setting was based on a dry-jet and wet-spun approach including extrusion, coagulation, drawing, drying, and winding. Crystallization of the experimental fiber, fiber extrudate, and film was evaluated using a technique of wide angle X-ray diffraction (WAXD). Crystallinity index, crystallite size, and crystal orientation factor were calculated and compared among these samples. Influence of die shape, die dimension, and drawing speed on the regenerated cellulose crystallinity was discussed. The study indicated that the pulp cellulose was a Cellulose I type structure. The cellulose regeneration from the [BMIM]Cl solution completed a transformation from this intermediate phase to a final Cellulose II phase. The die shape and dimension and drawing speed were all important factors affecting the crystallinity of regenerated cellulose fiber and film.

10.
Nat Nanotechnol ; 7(6): 369-73, 2012 May 06.
Artículo en Inglés | MEDLINE | ID: mdl-22562037

RESUMEN

Infrared light-emitting diodes are currently fabricated from direct-gap semiconductors using epitaxy, which makes them expensive and difficult to integrate with other materials. Light-emitting diodes based on colloidal semiconductor quantum dots, on the other hand, can be solution-processed at low cost, and can be directly integrated with silicon. However, so far, exciton dissociation and recombination have not been well controlled in these devices, and this has limited their performance. Here, by tuning the distance between adjacent PbS quantum dots, we fabricate thin-film quantum-dot light-emitting diodes that operate at infrared wavelengths with radiances (6.4 W sr(-1) m(-2)) eight times higher and external quantum efficiencies (2.0%) two times higher than the highest values previously reported. The distance between adjacent dots is tuned over a range of 1.3 nm by varying the lengths of the linker molecules from three to eight CH(2) groups, which allows us to achieve the optimum balance between charge injection and radiative exciton recombination. The electroluminescent powers of the best devices are comparable to those produced by commercial InGaAsP light-emitting diodes. By varying the size of the quantum dots, we can tune the emission wavelengths between 800 and 1,850 nm.


Asunto(s)
Rayos Infrarrojos , Puntos Cuánticos , Semiconductores
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