Article
Optics
Jianai Chen, Sijie Tan, Yue Yu, Shitong Zhang, Weijun Li, Qingbao Song, Yujie Dong, Cheng Zhang, Wai-Yeung Wong
Summary: This study provides clear evidence for the conversion between coplanar localized excited (LE) and twisted intramolecular charge transfer (TICT) excited states of D-A molecules in solid state. The research contributes to a deep understanding of the stimulus-response behavior of fluorescent D-A molecular solids from the perspective of excited state control.
JOURNAL OF LUMINESCENCE
(2021)
Article
Chemistry, Multidisciplinary
Yongtao Liu, Anton V. Ievlev, Nikolay Borodinov, Matthias Lorenz, Kai Xiao, Mahshid Ahmadi, Bin Hu, Sergei V. Kalinin, Olga S. Ovchinnikova
Summary: The study directly observes photoinduced ion migration in HOIPs, demonstrating that light illumination induces significant CH3NH3+ migration but not I-/Br- migration. Light effects on the migration of organic cation and halides in HOIPs are revealed to be distinct, offering insights for improving the performance and stability of HOIPs optoelectronics.
ADVANCED FUNCTIONAL MATERIALS
(2021)
Article
Chemistry, Physical
Cristian Guerra, Leandro Ayarde-Henriquez, Yeray A. Rodriguez-Nunez, Adolfo Ensuncho, Eduardo Chamorro
Summary: In this study, we investigated the role of chemical bonding in the photochemical process of generating nitrile imines from 2-phenyl tetrazole derivatives. Our findings show that the formation of imine nitrile involves two key bond events: heterolytic C-N breakage in the T-1 state and homolytic N-N rupture in the T-2 excited state. The delocalization of electron pairs in the C-C-N bonded structure plays a significant role in the conversion of the biradical imine nitrile into different forms.
Article
Chemistry, Physical
Kong Ooi Tan, Robert G. Griffin
Summary: This paper reports the first direct observation of the four-spin solid effect (4SSE) at a specific frequency, and provides a derivation of its effective Hamiltonian, matching conditions, and transition probabilities. The experimental results are consistent with numerical simulations and analytical theory.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Multidisciplinary Sciences
Dejian Yu, Fei Cao, Jinfeng Liao, Bingzhe Wang, Chenliang Su, Guichuan Xing
Summary: Mixed-dimensional 2D/3D halide perovskite solar cells suffer from poor efficiency due to the photoinduced carrier blocking effect at the 2D/3D perovskite interface, which jeopardizes device parameters.
NATURE COMMUNICATIONS
(2022)
Article
Physics, Multidisciplinary
Y. Jin, C. Y. Niu, K. W. Brown, Z. H. Li, H. Hua, A. K. Anthony, J. Barney, R. J. Charity, J. Crosby, D. Dell'Aquila, J. M. Elson, J. Estee, M. Ghazali, G. Jhang, J. G. Li, W. G. Lynch, N. Michel, L. G. Sobotka, S. Sweany, F. C. E. Teh, A. Thomas, C. Y. Tsang, M. B. Tsang, S. M. Wang, H. Y. Wu, C. X. Yuan, K. Zhu
Summary: In this study, Mg-18 was observed for the first time, providing evidence for the demise of the N = 8 shell closure in nuclei far from stability. The invariant-mass spectrum reveals signs of a potential excited state, possibly the first excited state.
PHYSICAL REVIEW LETTERS
(2021)
Article
Chemistry, Physical
Matthew Ward, Tom Regier, Johannes Vogt, Wei-Qiang Han, Tsun-Kong Sham
Summary: The study demonstrated that by using time gating techniques, it is possible to retrieve the UV emission from the BG of the GNZO system, revealing it consists of separate components attributed to ZnO and GaN.
JOURNAL OF PHYSICAL CHEMISTRY C
(2021)
Article
Chemistry, Physical
Le-Ping Miao, Ning Ding, Na Wang, Chao Shi, Heng-Yun Ye, Linglong Li, Ye-Feng Yao, Shuai Dong, Yi Zhang
Summary: Sliding ferroelectricity is a polarity observed in two-dimensional materials. We report the direct observation of sliding ferroelectricity in a single-crystal coordination polymer with a large bandgap. This finding provides important insights into low-dimensional ferroelectrics and their control.
Article
Chemistry, Multidisciplinary
Bowen Liu, Naifang Hu, Chao Li, Jun Ma, Jianwei Zhang, Yuan Yang, Deye Sun, Bangxun Yin, Guanglei Cui
Summary: This study for the first time investigates the initial activation mechanism of Li-rich layered oxide materials, revealing the heterogeneous Li-ion transport and the severe constraint on the activation of Li2MnO3 due to nanoscale phase separation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Multidisciplinary Sciences
Thomas Hartke, Botond Oreg, Carter Turnbaugh, Ningyuan Jia, Martin Zwierlein
Summary: The Hubbard model of attractively interacting fermions is used to study fermion pairing. In this model, a crossover between tightly bound pairs and long-range Cooper pairs occurs, with a pseudo-gap region above the superfluid critical temperature. By directly observing a Hubbard lattice gas of fermionic potassium-40 atoms under a bilayer microscope, the nonlocal nature of fermion pairing is revealed. The study also provides insights into the pseudo-gap behavior in strongly correlated fermion systems.
Article
Cell Biology
Alireza Mashaghi, Fatemeh Moayed, Eline J. Koers, Yang Zheng, Katharina Till, Gunter Kramer, Matthias P. Mayer, Sander J. Tans
Summary: The chaperone heat shock protein 90 (Hsp90) plays a crucial role in promoting local intra-chain interactions and suppressing distant interactions to alter the conformations of unstable substrates, thereby protecting and cooperating with them.
Article
Chemistry, Organic
Ani Deepthi, Nivedita Acharjee, S. L. Sruthi, C. B. Meenakshy
Summary: Nitrile imines (NIs) are a special class of compounds with versatile generation and inherent reactivity, and they have wide applications in synthetic chemistry. Recent research focuses on the [3+2] cycloaddition reactions of NIs, which are of great significance in bioorthogonal and material chemistry.
Article
Energy & Fuels
Yeonhwa Cho, Sooyong Lee, Hwajeong Kim, Youngkyoo Kim
Summary: Polymeric solid-state electrolytes composed of lithium hydroxide (LiOH) and branched-poly(ethyleneimine) (bPEI) were used to fabricate lithium polymer supercapacitors (LPSCs) with stable charging/discharging characteristics. The highest energy density of LPSCs was obtained with LiOH = 90 mol% due to the highest ion conductivity. The optimized LPSCs with bPEI:LiOH solid-state electrolytes (LiOH = 90 mol%) retained approximately 85% of their capacity after 700 cycles.
JOURNAL OF ENERGY STORAGE
(2023)
Article
Chemistry, Multidisciplinary
Juncao Bian, Huimin Yuan, Muqing Li, Sifan Ling, Bei Deng, Wen Luo, Xuedan Chen, Lihong Yin, Shuai Li, Long Kong, Ruo Zhao, Haibin Lin, Wei Xia, Yusheng Zhao, Zhouguang Lu
Summary: A new method for preparing composite electrolyte films based on lithium-rich antiperovskites (LiRAPs) has been proposed, which can enhance Li ion conductivity and reduce activation energy by adding LiRAP and NBR. This provides a foundation for potential practical applications by advancing the LiRAP-family solid-state electrolytes.
FRONTIERS IN CHEMISTRY
(2021)
Article
Chemistry, Physical
Sharma S. R. K. C. Yamijala, Pengfei Huo
Summary: In this study, direct nonadiabatic dynamics simulations were used to investigate photoinduced charge transfer reactions. The approach combines quantum-classical methods to treat electron transfer and model the excited state as a transferring single-electron occupying the LUMO of the donor molecule. Results from simulations of well-characterized molecular systems showed excellent agreement with experimental measurements and high-level theoretical results.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Chemistry, Multidisciplinary
Gangam Srikanth Kumar, Stefano Racioppi, Eva Zurek, Qing Lin
Summary: This article reports the design of a super fast bioorthogonal ligation reactant pair, enabling rapid bioorthogonal labeling on live cells.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Organic
Xiaohu Zhao, Yuqiao Zhou, Bao-Lin Li, Guangxi Du, Zhipeng Yu
Summary: A highly efficient and catalyst-free method has been developed for the dearomatization of 3-(2-isocyanoethyl)indoles using in situ generated nitrile imines. This method involves a nucleophilic/Friedel-Crafts/aza-Mannich type cascade and 1,3-dipolar cycloaddition reaction, and allows for the rapid assembly of a wide range of polycyclic indoline scaffolds with moderate to excellent yields and diastereoselectivities.
ORGANIC CHEMISTRY FRONTIERS
(2022)
Article
Biochemistry & Molecular Biology
Yifang Yang, Candy Lee, Reddy Rajasekhar Reddy, David J. Huang, Weixia Zhong, Van T. B. Nguyen-Tran, Weijun Shen, Qing Lin
Summary: Recent trials have demonstrated that chimeric peptides activating GLP-1R and GIPR simultaneously are more effective in glycemic control and weight reduction than those activating GLP-1R alone. However, linear peptide-based dual agonists are not suitable for oral administration due to susceptibility to proteolytic cleavage. This study presents the design and synthesis of biaryl-stapled peptides with improved proteolytic stability. These stapled peptides showed strong dual agonist activities and exhibited excellent efficacy in an oral glucose tolerance test in mice.
ACS CHEMICAL BIOLOGY
(2022)
Article
Chemistry, Multidisciplinary
Yali Xu, Abdur Rahim, Qing Lin
Summary: In this study, we designed N-2-carboxy-4-aryl-1,2,3-triazole-lysines (CATKs) and incorporated them into proteins via genetic code expansion. CATKs allowed for spontaneous, site-selective crosslinking to generate covalent protein dimers in living cells. The resulting crosslinked proteins showed improved cellular uptake and enhanced stability.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Zheng Wang, Johnathan D. Rabb, Qing Lin
Summary: Compared to disulfide bonds, little attention has been given to naturally occurring intramolecular crosslinks, mainly due to their rarity in proteins. This article presents examples of natural non-disulfide crosslinks, known as orthogonal crosslinks, and highlights their impact on protein topology and function. Recent efforts to expand orthogonal crosslinks by utilizing protein circularization enzymes or the genetic code expansion strategy are summarized, including the advantages, disadvantages, and applications in generating novel protein topology and function. The spontaneous orthogonal crosslinking using a carbamate-based crosslink and its applications in designing topology-mimicking bacterial adhesins are specifically emphasized.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Tingting Zheng, Jielin Fu, Qin Xiong, Xin Shen, Baolin Li, Xiaohu Zhao, Zhipeng Yu
Summary: We present the genetic incorporation of DBDAA isomers into proteins using two evolved Methanosarcina mazei pyrrolysine tRNA synthetases, with the ability to tune enzymatic activity via cucurbit[7]uril host-guest recognition under either dark or 405 nm photo-stimulation.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Organic
Guangxi Du, Jielin Fu, Yuanqin Zheng, Fuqiang Hu, Xin Shen, Baolin Li, Xiaohu Zhao, Zhipeng Yu
Summary: We investigated the feasibility of using cyclic azobenzene/azobenzene-based photo-switchable drugs to fine-tune antibacterial activity against E. coli and S. aureus with light dependence. The light-controlled drug combination of these drugs could be reversibly controlled with different wavelength light to improve the antibiotic effect by reducing MICs. Importantly, their antimicrobial activity could be easily manipulated using light in bacterial patterning studies, allowing for localized activation of drugs and providing an alternative solution in photopharmacology.
ORGANIC & BIOMOLECULAR CHEMISTRY
(2023)
Article
Chemistry, Organic
Yuanqin Zheng, Yuqiao Zhou, Shichao Jiang, Xinyu Xie, Guangxi Du, Xin Shen, Xiaohu Zhao, Zhipeng Yu
Summary: A metal-free strategy for constructing deep-blue emissive bicyclic triazolines with high photoluminescent quantum yields has been developed. The resulting triazoline frameworks exhibit strong blue emissions in both solution and solid state, and have great potential for the development of new blue luminescent materials. Time-dependent density-functional theory calculations and crystallographic analysis reveal the factors affecting the fluorescence quantum yields of the triazolines. Additionally, the triazolines show excellent stability and low cytotoxicity, making them suitable for live-cell imaging.
ORGANIC CHEMISTRY FRONTIERS
(2023)
Article
Chemistry, Multidisciplinary
Xinyu Xie, Fuqiang Hu, Yuqiao Zhou, Zhihao Liu, Xin Shen, Jielin Fu, Xiaohu Zhao, Zhipeng Yu
Summary: We present a novel photoclick reaction between 2,3-diaryl indenone epoxide (DIO) and ring-strained dipolarophiles, in which DIO acts as a P-type photoswitch to generate mesoionic oxidopyrylium ylide (PY) and initiate an ultra-fast [5+2] cycloaddition. The photoisomerization between DIO and PY can be tightly controlled by 365 or 520 nm photo-stimulation, enabling reversion or regeneration of the reactive PY dipole on demand. This reversible photoactivation is exploited to enhance chemoselectivity of the [5+2] cycloaddition in complex environments and to recycle DIO reagent for batch-wise protein conjugation. Additionally, a dynamic photoswitching strategy is proposed to improve spatial resolution of lithographic surface decoration and bioorthogonal labeling on living cells through spatiotemporal dual-lambda photo-modulation.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Biochemistry & Molecular Biology
Ming Fang, Gangam Srikanth Kumar, Qing Lin
Summary: This study reports the synthesis of hydrazonyl sultones (HS) with an ortho-CF3 group and different N-aryl substituents, and investigates their stability and reactivity towards BCN in a 1,3-dipolar cycloaddition reaction. The HS show good aqueous stability due to the electrostatic shielding effect of the CF3 group. The N-aryl substituents further influence the reactivity and stability of the HS, with electron-rich six-membered HS demonstrating excellent stability and increased cycloaddition reactivity. These improved HS reagents enable fast and selective modification of BCNK-encoded nanobodies.
Article
Chemistry, Multidisciplinary
Ming Fang, Gangam Srikanth Kumar, Stefano Racioppi, Heyang Zhang, Johnathan D. Rabb, Eva Zurek, Qing Lin
Summary: In this study, a new class of bioorthogonal reagents called hydrazonyl sultones (HS) were designed and synthesized as stable tautomers of highly reactive nitrile imines (NI). The HS demonstrated broad aqueous stability and tunable reactivity in a 1,3-dipolar cycloaddition reaction, depending on substituents, sultone ring structure, and solvent conditions. DFT calculations provided insights into the HS -> NI tautomerism and comparative kinetic analysis revealed the extraordinary stability of HS. The utility of HS was demonstrated in selective modification of nanobodies and fluorescent labeling of a transmembrane glucagon receptor.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Jielin Fu, Sitong Li, Lijun Deng, Xiaohu Zhao, Zhipeng Yu
Summary: We describe a genetically encoded m-trifluoromethylaniline modified l-lysine (m-TFMAK) that undergoes defluorination upon light activation and forms covalent conjugates with native residues via acyl fluoride exchange. The encoded m-TFMAK enables photo-crosslinking with temporal control, residue selectivity, and fluorogenic tracking, providing a useful tool for identifying protein interactions in living systems.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Lijun Deng, Cefei Zhang, Baolin Li, Jielin Fu, Zhong Zhang, Sitong Li, Xiaohu Zhao, Zhishan Su, Changwei Hu, Zhipeng Yu
Summary: Photo-click chemistry is a powerful tool for advancing bioconjugation technologies. In this study, researchers developed a novel photo-induced defluorination acyl fluoride exchange (photo-DAFEx) reaction that allows covalent conjugation in an aqueous environment. This strategy enables spatiotemporal control and has potential applications in small molecule decoration, peptide cyclization, protein functionalization, and designing photo-affinity probes for living cells.
Article
Biochemistry & Molecular Biology
Tracey M. Lewandowski, Peng An, Carlo P. Ramil, Ming Fang, Qing Lin
Summary: This study presents an integrated approach combining enzymatic SNAP-tagging and bioorthogonal chemistry for dual fluorescent labeling of GLP-1R. The resulting GLP-1R conformational biosensors enable FRET-based analysis of the receptor subdomain movement in response to ligand stimulation in live cells.
RSC CHEMICAL BIOLOGY
(2022)
Article
Chemistry, Multidisciplinary
Qin Xiong, Tingting Zheng, Xin Shen, Baolin Li, Jielin Fu, Xiaohu Zhao, Chunxia Wang, Zhipeng Yu
Summary: This study presents a method for genetically encoding proteins with novel noncanonical amino acids, enabling site-specific functionalization of proteins in living cells through photo-click reactions. By designing and synthesizing a photo-switchable amino acid and using directed evolution to encode it into recombinant proteins, a genetically encodable reporter for photo-click bioconjugation with spatiotemporal controllability is developed. The photo-isomerization of the amino acid can be used as a tool to convert photon energy into ring-strain energy, oscillating the conformational changes of the parent proteins. The photo-switching of the amino acid on proteins enables efficient and selective photo-click ligation with specific probes. This genetic code expansion method allows for further functional diversity of artificial proteins in living systems.
