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result(s) for
"Jin, Shengye"
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Tailoring vertical phase distribution of quasi-two-dimensional perovskite films via surface modification of hole-transporting layer
2019
Vertical phase distribution plays an important role in the quasi-two-dimensional perovskite solar cells. So far, the driving force and how to tailor the vertical distribution of layer numbers have been not discussed. In this work, we report that the vertical distribution of layer numbers in the quasi-two-dimensional perovskite films deposited on a hole-transporting layer is different from that on glass substrate. The vertical distribution could be explained by the sedimentation equilibrium because of the colloidal feature of the perovskite precursors. Acid addition will change the precursors from colloid to solution that therefore changes the vertical distribution. A self-assembly layer is used to modify the acidic surface property of the hole-transporting layer that induces the appearance of desired vertical distribution for charge transport. The quasi-two-dimensional perovskite cells with the surface modification display a higher open-circuit voltage and a higher efficiency comparing to reference quasi-two-dimensional cells.
Vertical phase distribution of quasi-two-dimensional perovskite plays vital roles in their optoelectronic properties. Here Liu et al. show that surface modification of the hole-transporting layer is an effective approach to control the vertical phase distribution and optimize the device efficiency.
Journal Article
Efficient and stable emission of warm-white light from lead-free halide double perovskites
2018
Lighting accounts for one-fifth of global electricity consumption
1
. Single materials with efficient and stable white-light emission are ideal for lighting applications, but photon emission covering the entire visible spectrum is difficult to achieve using a single material. Metal halide perovskites have outstanding emission properties
2
,
3
; however, the best-performing materials of this type contain lead and have unsatisfactory stability. Here we report a lead-free double perovskite that exhibits efficient and stable white-light emission via self-trapped excitons that originate from the Jahn–Teller distortion of the AgCl
6
octahedron in the excited state. By alloying sodium cations into Cs
2
AgInCl
6
, we break the dark transition (the inversion-symmetry-induced parity-forbidden transition) by manipulating the parity of the wavefunction of the self-trapped exciton and reduce the electronic dimensionality of the semiconductor
4
. This leads to an increase in photoluminescence efficiency by three orders of magnitude compared to pure Cs
2
AgInCl
6
. The optimally alloyed Cs
2
(Ag
0.60
Na
0.40
)InCl
6
with 0.04 per cent bismuth doping emits warm-white light with 86 ± 5 per cent quantum efficiency and works for over 1,000 hours. We anticipate that these results will stimulate research on single-emitter-based white-light-emitting phosphors and diodes for next-generation lighting and display technologies.
After alloying with metal cations, a lead-free halide double perovskite shows stable performance and remarkably efficient white-light emission, with possible applications in lighting and display technologies.
Journal Article
Visible-light-driven coproduction of diesel precursors and hydrogen from lignocellulose-derived methylfurans
by
Liu, Junxue
,
Fonda, Emiliano
,
Nie, Wei
in
639/4077/909/4053/906/4052
,
639/4077/909/4086/4087
,
639/638/77/887
2019
Photocatalytic hydrogen production from biomass is a promising alternative to water splitting thanks to the oxidation half-reaction being more facile and its ability to simultaneously produce solar fuels and value-added chemicals. Here, we demonstrate the coproduction of H
2
and diesel fuel precursors from lignocellulose-derived methylfurans via acceptorless dehydrogenative C−C coupling, using a Ru-doped ZnIn
2
S
4
catalyst and driven by visible light. With this chemistry, up to 1.04 g g
catalyst
−1
h
−1
of diesel fuel precursors (~41% of which are precursors of branched-chain alkanes) are produced with selectivity higher than 96%, together with 6.0 mmol g
catalyst
−1
h
−1
of H
2
. Subsequent hydrodeoxygenation reactions yield the desired diesel fuels comprising straight- and branched-chain alkanes. We suggest that Ru dopants, substituted in the position of indium ions in the ZnIn
2
S
4
matrix, improve charge separation efficiency, thereby accelerating C−H activation for the coproduction of H
2
and diesel fuel precursors.
Biomass can be used to scavenge photogenerated holes in photocatalytic hydrogen production, but the oxidized molecules that form are not always useful products. Here, the authors use Ru-ZnIn
2
S
4
to photocatalyse the dehydrogenative C−C coupling of lignocellulose-derived methylfurans, forming both hydrogen and diesel fuel precursors.
Journal Article
Photo-generated dinuclear {Eu(II)}2 active sites for selective CO2 reduction in a photosensitizing metal-organic framework
2018
Photocatalytic reduction of CO
2
is a promising approach to achieve solar-to-chemical energy conversion. However, traditional catalysts usually suffer from low efficiency, poor stability, and selectivity. Here we demonstrate that a large porous and stable metal-organic framework featuring dinuclear Eu(III)
2
clusters as connecting nodes and Ru(phen)
3
-derived ligands as linkers is constructed to catalyze visible-light-driven CO
2
reduction. Photo-excitation of the metalloligands initiates electron injection into the nodes to generate dinuclear {Eu(II)}
2
active sites, which can selectively reduce CO
2
to formate in a two-electron process with a remarkable rate of 321.9 μmol h
−1
mmol
MOF
−1
. The electron transfer from Ru metalloligands to Eu(III)
2
catalytic centers are studied via transient absorption and theoretical calculations, shedding light on the photocatalytic mechanism. This work highlights opportunities in photo-generation of highly active lanthanide clusters stabilized in MOFs, which not only enables efficient photocatalysis but also facilitates mechanistic investigation of photo-driven charge separation processes.
Solar-to-chemical CO
2
reduction provides a means to use light’s energy for CO
2
removal and upgrading to useful products, although this photochemical conversion is challenging. Here, authors construct a Europium-containing metal-organic framework that selectively converts CO
2
to formate with light.
Journal Article
Observation of triplet-assisted long-distance charge-transfer exciton transport in single organic cocrystal
by
Liu, Xuan
,
Xiao, Yejun
,
Yan, Xianchang
in
639/638/440/527/1819
,
639/638/440/948
,
Atomic energy levels
2025
Charge-transfer (CT) states with long transport distances are highly desired for promoting the performance of organic optoelectronic devices in photoconversion and electroluminescence. However, due to the limited lifetime and small diffusivity, only nanoscale CT transport has been observed so far. Herein, taking a binary CT cocrystal (
trans
−1,2-diphenylethylene-1,2,4,5-tetracyanobenzene, named as T
S
-T
C
) with efficient thermally activated delayed fluorescence (TADF) as a model material, we report the direct observation of long-distance CT exciton transport by using modified time-resolved and photoluminescence-scanned imaging microscopy, which reveals a triplet-assisted CT transport mechanism. We demonstrate that, enabled by the long-lived and high-yield triplet state and efficient TADF, the average transport distance of over 80% of CT excitons in T
S
-T
C
can be significantly enhanced from intrinsic nanoscale (≤58 nm) to ~11.2 μm. Our findings provide an effective strategy for greatly promoting short-lived CT exciton transport, which is of great significance for optoelectronic material design and device optimization.
Charge-transfer states with long transport distances in organic cocrystals have only been observed at nanoscale so far. Here, the authors report its direct observation at micron scale and reveal a triplet assisted transport mechanism to improve optoelectronic material design and device optimization.
Journal Article
Heavy-atom functionalization promotes triplet-assisted charge-transfer exciton transport in organic cocrystals
2026
Charge-transfer (CT) states with long transport distance are highly desirable for boosting the performance of organic optoelectronic devices. Although micron-scale CT transport has been observed in cocrystals, effective strategies for enhancing the diffusivity of CT excitons remain a challenge. Herein, based on heavy atom effect (HAE), we successfully promote CT exciton transport in thermally activated delayed fluorescence (TADF) cocrystals through bromine-atom functionalization. In Br-functionalized cocrystal, the diffusivity of triplet CT excitons is enhanced by an order of magnitude, enabling a long-distance triplet-assisted CT transport exceeding 16 μm. By adjusting the Br content, the CT transport and TADF-related kinetics can be effectively modulated, thereby significantly enhancing the utilization of CT excitons and the photocurrent responses of cocrystals. Our findings provide compelling evidence that heavy-atom functionalization can serve as an effective strategy to promote CT transport, which is of great significance for the performance optimization of organic optoelectronic devices.
Charge-transfer states with long transport distance have potential in organic optoelectronic devices, but it can be challenging to improve this. Here, the authors report the promotion of exciton transport in thermally activated delayed fluorescence cocrystals by bromine-atom functionalisation.
Journal Article
An ultrastretchable seamlessly integrated contactless charging microsystem towards skin-attachable wireless microelectronics
2025
For electronics to be wearable, contactless charging and overall deformability are necessary pre-conditions. However, the current heterogeneous integration based on different active materials and separate manufacturing often leads to mechanical mismatch. Here, we report an ultrastretchable all-in-one integrated MXene-based microsystem comprising wireless coils, micro-supercapacitors (MSCs) and strain sensors. The seamless configuration without any connecting interface dramatically improves the structural integrity of the microsystem, and a pre-crumpled structure endows it with superior stretchability. Attributed to these, our MSCs can be wirelessly charged in ~20 s under various types of deformation and are capable of powering strain sensors, responding rapidly to body motion signals. Moreover, the MSCs display a high specific capacitance of 76.82 F cm
–3
, and superb mechanical stability with 98.5% capacitance retention after biaxial stretching 1000 cycles from 0% to 500% areal strain. Therefore, this work sheds new insights into design and implementation of skin-attachable wireless microelectronics.
The authors report a stretchable and integrated energy harvest-storage-application skin-adherent microsystem, by utilizing an all-in-one MXene film simultaneously as micro-supercapacitors, wireless receiver coils and strain sensors.
Journal Article
One-step rapid synthesis, crystal structure and 3.3 microseconds long excited-state lifetime of Pd1Ag28 nanocluster
by
Liu, Chao
,
Lin, Xinzhang
,
Wu, Ren’an
in
Absorption spectroscopy
,
Atomic/Molecular Structure and Spectra
,
Biomedicine
2020
Doping foreign atom(s) in metal nanoclusters is an effective strategy to engineer the properties and functionalities of metal nanoclusters. However, until now, to dope Pd atom into Ag nanoclusters remains a huge challenge. Here we develop a one-step rapid method to synthesize the Pd-doped Ag nanocluster with high yield. The prepared Pd
1
Ag
28
nanocluster was characterized by mass spectroscopy, X-ray photoelectron spectroscopy, X-ray crystallography, fluorescence spectroscopy, ultraviolet–visible absorption spectroscopy and transient absorption spectroscopy. The nanocluster exhibits a perfect face-centered cubic (FCC) kernel structure with a tetrahedron-like shell. Of note, Pd
1
Ag
28
nanocluster had an unexpectedly long excited-state lifetime of 3.3 microseconds, which is the longest excited-state lifetime for Ag-based nanoclusters so far. Meanwhile, the excellent near-infrared luminescence indicated the nanocluster has the potential in fluorescent bio-imaging. Besides, it was revealed that Pd
1
Ag
28
nanocluster could be transformed into Au
1
Ag
28
nanocluster via ion exchange reaction of AuPPh
3
Cl with Pd
1
Ag
28
nanocluster. This work provides an efficient synthetic protocol of alloy nanoclusters and will contribute to study the effect of foreign atom on the properties of metal nanoclusters.
Journal Article
Regulating Exciton–Phonon Coupling to Achieve a Near‐Unity Photoluminescence Quantum Yield in One‐Dimensional Hybrid Metal Halides
by
Lin, Haoran
,
Ma, Biwu
,
Zhang, Wenqing
in
1D hybrid metal halides
,
exciton–phonon coupling
,
Huang–Rhys factor
2021
Low‐dimensional hybrid metal halides are emerging as a highly promising class of single‐component white‐emitting materials for their unique broadband emission from self‐trapped excitons (STEs). Despite substantial progress in the development of these metal halides, many challenges remain to be addressed to obtain a better fundamental understanding of the structure–property relationship and realize the full potentials of this class of materials. Here, via pressure regulation, a near 100% photoluminescence quantum yield (PLQY) of broadband emission is achieved in a corrugated 1D hybrid metal halide C5N2H16Pb2Br6, which possesses a highly distorted structure with an initial PLQY of 10%. Compression reduces the overlap between STE states and ground state, leading to a suppressed phonon‐assisted non‐radiative decay. The PL evolution is systematically demonstrated to be controlled by the pressure‐regulated exciton–phonon coupling which can be quantified using Huang–Rhys factor S. Detailed studies of the S‐PLQY relation for a series of 1D hybrid metal halides (C5N2H16Pb2Br6, C4N2H14PbBr4, C6N2H16PbBr4, and (C6N2H16)3Pb2Br10) reveal a quantitative structure–property relationship that regulating S factor toward 28 leads to the maximum emission. This work demonstrates a quantitative relationship between photoluminescence quantum yield (PLQY) and exciton–phonon coupling in a series of 1D hybrid metal halides. Using pressure to regulate the exciton–phonon interaction, a near 100% PLQY of broadband emission from self‐trapped excitons is achieved in a corrugated 1D compound C5N2H16Pb2Br6 whose initial PLQY is 10%.
Journal Article
H4K79 and H4K91 histone lactylation, newly identified lactylation sites enriched in breast cancer
2025
Metabolic reprogramming and epigenetic modification are two hallmarks of cancer. Protein lysine lactylation (Kla) is a novel type of glycolysis lactate-triggered posttranslational modification. However, the role of Kla in breast cancer (BC) remains largely unknown. Here, western blot, and immunohistochemical (IHC) staining of BC tissues revealed that global Kla levels were upregulated in BC tissues, and high levels of Kla were correlated with poor prognosis of patients with BC. A series of in vitro and in vivo assays demonstrated that interruption of glycolysis by lactate dehydrogenase (LDH) inhibitor or silencing LDHA and LDHB repressed the malignant behaviors of BC cells. Moreover, 4D label-free quantitative lactylproteomics analysis of BC tissues and cells revealed that lactylated proteins widely existed in several subcellular compartments and were closely associated with various cancer-related biological processes. Notably, two previously unresearched sites of histone lactylation, H4K79 lactylation (H4K79la) and H4K91 lactylation (H4K91la), were identified to be hyperlactylated in cancer tissues and cells. Glycolytic genes, such as lactate dehydrogenase A (LDHA), phosphoglycerate kinase 1 (PGK1), and hexokinase 1 (HK1) were identified to be the potential candidate genes epigenetically regulated by H4K79la and H4K91la by intersecting through chromatin immunoprecipitation sequencing (ChIP-seq), RNA sequencing (RNA-seq), and TCGA-BRCA database. Pharmacological inhibition of glycolysis downregulated H4K79 and H4K91 lactylation and suppressed the expression of glycolytic genes, whereas treatment with sodium lactate exhibited the opposite effects. Additionally, E1A-binding protein p300 (P300) acted as lysine lactyltransferase to regulate H4K79la and H4K91la, and control the transcription and expression of downstream glycolytic genes in BC cells. The results revealed an intriguing positive feedback loop formed by glycolysis/H4K79la/H4K91la/glycolytic genes in BC, highlighting the relationship between metabolic reprogramming and epigenetic regulation. These findings provide new therapeutic targets for patients with BC.
Journal Article