Lead-free double-perovskite
nanocrystals (NCs), that is, Cs2AgIn
x
Bi1–x
Cl6 (x = 0, 0.25, 0.5, 0.75, and
0.9), that can be tuned from indirect band gap (x = 0, 0.25, and 0.5) to direct band gap (x = 0.75
and 0.9) are designed. Direct band gap NCs exhibit 3 times greater
absorption cross section, lower sub-band gap trap states, and >5
times
photoluminescence quantum efficiency (PLQE) compared to those observed
for indirect band gap NCs (Cs2AgBiCl6). A PLQE
of 36.6% for direct band gap NCs is comparable to those observed for
lead perovskite NCs in the violet region. Besides the band edge violet
emission, the direct band gap NCs exhibit bright orange (570 nm) emission.
Density functional theory calculations suggesting forbidden transition
is responsible for the orange emission, which is supported by time-resolved
PL and PL excitation spectra. The successful design of lead-free direct
band gap perovskite NCs with superior optical properties opens the
door for high-performance lead-free perovskite optoelectronic devices.
A series of lead‐free double perovskite nanocrystals (NCs) Cs2AgSb1−yBiyX6 (X: Br, Cl; 0≤y≤1) is synthesized. In particular, the Cs2AgSbBr6 NCs is a new double perovskite material that has not been reported for the bulk form. Mixed Ag–Sb/Bi NCs exhibit enhanced stability in colloidal solution compared to Ag–Bi or Ag–Sb NCs. Femtosecond transient absorption studies indicate the presence of two prominent fast trapping processes in the charge‐carrier relaxation. The two fast trapping processes are dominated by intrinsic self‐trapping (ca. 1–2 ps) arising from giant exciton–phonon coupling and surface‐defect trapping (ca. 50–100 ps). Slow hot‐carrier relaxation is observed at high pump fluence, and the possible mechanisms for the slow hot‐carrier relaxation are also discussed.
We developed a high-performance photodetector based on (CHNH)SbI (MASbI) microsingle crystals (MSCs). The MASbI single crystals exhibit a low-trap state density of ∼10 cm and a long carrier diffusion length reaching 3.0 μm, suggesting its great potential for optoelectronic applications. However, the centimeter single crystal (CSC)-based photodetector exhibits low responsivity (10 A/W under 1 sun illumination) due to low charge-carrier collection efficiency. By constructing the MSC photodetector with efficient charge-carrier collection, the responsivity can be improved by three orders of magnitude (under 1 sun illumination) and reach 40 A/W with monochromatic light (460 nm). Furthermore, the MSC photodetectors exhibit fast response speed of <1 ms, resulting in a high gain of 108 and a gain-bandwidth product of 10 Hz. These numbers are comparable to the lead-perovskite single-crystal-based photodetectors.
A series of lead‐free double perovskite nanocrystals (NCs) Cs2AgSb1−yBiyX6 (X: Br, Cl; 0≤y≤1) is synthesized. In particular, the Cs2AgSbBr6 NCs is a new double perovskite material that has not been reported for the bulk form. Mixed Ag–Sb/Bi NCs exhibit enhanced stability in colloidal solution compared to Ag–Bi or Ag–Sb NCs. Femtosecond transient absorption studies indicate the presence of two prominent fast trapping processes in the charge‐carrier relaxation. The two fast trapping processes are dominated by intrinsic self‐trapping (ca. 1–2 ps) arising from giant exciton–phonon coupling and surface‐defect trapping (ca. 50–100 ps). Slow hot‐carrier relaxation is observed at high pump fluence, and the possible mechanisms for the slow hot‐carrier relaxation are also discussed.
Phosphorylation of
glucose is the prime step in sugar metabolism
and energy storage. Two key glucose phosphates are involved, that
is, glucose 6-phosphate (G6P) and α-glucose 1-phosphate (αG1P).
The chiral conformation of glucose, G6P, and αG1P plays an essential
role in enzyme-mediated conversions. However, few techniques were
able to give a direct view of the conformational changes from glucose
to G6P and αG1P. Here, Raman optical activity (ROA) was used
to elucidate the stereochemical evolution of glucose upon phosphorylation.
ROA was found to be extremely sensitive to different phosphorylation
sites. A characteristic ROA marker of (+)980 cm–1, originated from the phosphate group symmetric stretching vibration,
is observed for αG1P with phosphorylation at chiral C1, while
no corresponding ROA signal for G6P with phosphorylation at achiral
C6 is observed. Phosphorylation-induced gauch–gauch (gg)/gauch–trans
(gt) rotamer distribution changes can be sensitively probed by the
sign of the ROA band around 1460 cm–1. A positive
ROA band at 1465 cm–1 of glucose corresponds to
a higher gt ratio, while a negative band at 1455 cm–1 of G6P suggests a dominant gg population, and the disappearance
of this ROA band for αG1P indicates a nearly balanced gg/gt
distribution. Meanwhile, the phosphorylation at C6 and C1 could cause
dramatic reduction of the conformational flexibility of the adjacent
C4–OH and C2–OH, respectively. These stereochemical
changes revealed by ROA spectra offer a structural basis on the understanding
of sugar phosphorylation from the perspective of chirality.
Sandfly feeding behaviour and destination of coloured sugar meals in the gut of Lutzomyia longipalpis were investigated with particular attention to the role of the crop. Sandflies were able to ingest sugar from liquid drops, microcapillaries, a slice of pear and even sugar powder. In most cases the flies adopted a 'sugar feeding mode' with raised palps. As the fruit dried, flies of both sexes fed by piercing the tissue with the proboscis. All sugar-fed flies had a full crop plus a small amount of sugary fluid in the thoracic mid-gut, i.e. past the stomodaeal valve. Dissections of flies interrupted during feeding showed that the very first trace of sugar passed through the stomodaeal valve, but that the rest of the meal was diverted into the crop. This suggests that closure of the stomodaeal valve is initiated only after a small volume of sugar solution has passed through it.
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