Article
Chemistry, Physical
Lars H. Andersen, Anne P. Rasmussen, Henrik B. Pedersen, Oleg B. Beletsan, Anastasia V. Bochenkova
Summary: By using time-resolved action spectroscopy of cryogenically cooled molecular ions, we have achieved high vibrational resolution in the photoresponse of the deprotonated GFP chromophore. We have identified four characteristic spectral regions and determined the energy barrier towards internal conversion. The red-shifted origin of the S-0-S-1 band suggests similar photophysics between the protein and its chromophore.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Multidisciplinary Sciences
Omri Tau, Alice Henley, Anton N. Boichenko, Nadezhda N. Kleshchina, River Riley, Bingxing Wang, Danielle Winning, Ross Lewin, Ivan P. Parkin, John M. Ward, Helen C. Hailes, Anastasia Bochenkova, Helen H. Fielding
Summary: This study determines the electron detachment energy of the green fluorescent protein chromophore in aqueous solution using UV liquid-microjet photoelectron spectroscopy and quantum chemistry calculations. The research highlights the importance of electronically excited states of the chromophore in photo-induced electron transfer processes in the condensed phase.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Analytical
Attila Csomos, Ervin Kovacs, Miklos Madarasz, Flora Zsofia Fedor, Anna Fulop, Gergely Katona, Balazs Rozsa, Zoltan Mucsi
Summary: A library of fluorescent GFP chromophore based chemosensors (GFZnPs) was prepared for the detection of Zn2+ using two-photon microscopy. These sensors exhibit high selectivity, excellent water solubility, and wide pH-range usability, making them one of the best two-photon probes for Zn2+.
SENSORS AND ACTUATORS B-CHEMICAL
(2024)
Article
Chemistry, Physical
Cheng Chen, Hao Zhang, Jing Zhang, Hui-wang Ai, Chong Fang
Summary: The incorporation of ncAAs into fluorescent proteins has the potential to red-shift their fluorescence and improve tissue imaging. However, ncAA-based RFPs are rare. The recent advance of 3-aminotyrosine modified sfGFP has provided insights into the molecular mechanism of red-shifted fluorescence, but its dim fluorescence limits its applications.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Basanta Kumar Rajbongshi, Shahnawaz Rafiq, Suman Bhowmik, Pratik Sen
Summary: In this study, the excited state dynamics of a GFP chromophore analogue, DPI, was investigated using femtosecond spectroscopy and quantum chemical calculations. It was found that the dynamics of DPI involves the formation of an intramolecular charge transfer state mediated by a twisting motion. Quantum chemical computations further predicted the formation of a conical intersection between the S1 and S0 states, which is the main nonradiative deactivation pathway. This study highlights the importance of restricting twisting motion for GFP analogues to exhibit GFP-like excited state properties.
JOURNAL OF MOLECULAR STRUCTURE
(2023)
Article
Chemistry, Organic
Steven Frippiat, Camille Sarre, Christine Baudequin, Christophe Hoarau, Laurent Bischoff
Summary: In this study, alpha-isocyanoacetamide derivatives were successfully converted into oxazolines under newly developed conditions. These oxazolines served as precursors for alpha-isocyanoacrylamides, which could further lead to diverse 2-arylated imidazolones. Furthermore, it was demonstrated that both oxazolines and their precursors could rapidly and efficiently generate imidazolones unsubstituted at C2, offering unprecedented routes for the synthesis of imidazolones with good tolerance to different substitution patterns.
JOURNAL OF ORGANIC CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Xiaoqin Wei, Yiming Zhu, Xiang Yu, Lei Cai, Nanan Ruan, Luling Wu, Nengqin Jia, Tony D. James, Chusen Huang
Summary: The presence of ER stress is a significant factor in various biological processes associated with numerous diseases. By creating a new ER-targeting fluorescent probe, researchers have been able to measure changes in intracellular ER viscosity caused by ER stress. Their findings indicate an increase in ER viscosity during autophagy.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Physical
Yun-Hua Zhu, Xin-Xin Liu, Qiu Fang, Xiang-Yang Liu, Wei-Hai Fang, Ganglong Cui
Summary: In this study, a combined CASPT2//CASSCF approach within the QM/MM framework was used to investigate the early time photoisomerization of rsEGFP2 starting from its two OFF trans states, Trans1 and Trans2. The results showed similar vertical excitation energies in the Franck-Condon regions. By considering rotations of the C11-C9 bond, four pairs of excited-state minima and low-lying conical intersections were optimized, leading to the determination of four barrierless photoisomerization paths to efficient excited state deactivation. This work identified multiple photoisomerization and excited-state decay paths, providing significant insights for the understanding of GFP-like RSFPs and the design of novel GFP-like fluorescent proteins.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2023)
Article
Multidisciplinary Sciences
Nguyen Thuan Dao, Reinhard Haselsberger, Mai Thu Khuc, Anh Tuan Phan, Alexander A. Voityuk, Maria-Elisabeth Michel-Beyerle
Summary: The study focused on Baby Spinach, a truncated version of the Spinach RNA aptamer, and found that its fluorescence and excitation spectra were similar to those of the full Spinach aptamer. The unexpected discrepancy between absorption and fluorescence excitation spectra in the DFHBI/RNA complex could be explained by competing dark and fluorescent binding sites. This abnormal absorption spectrum might be caused by trans-isomers formed within the cis-bound DFHBI/RNA complex, providing valuable insight into the efficiency of a fluorogenic dye/RNA system.
SCIENTIFIC REPORTS
(2021)
Review
Biochemistry & Molecular Biology
Alexander W. Schuppe, Yannan Liu, Timothy R. Newhouse
Summary: This article discusses the use of cationic rearrangement reactions in natural product total synthesis from 2010 to 2020, highlighting the importance of isomerization reactions in synthesis and their suitability for computational evaluation. It emphasizes the insights that relatively simple calculations can provide in understanding isomerization reactions.
NATURAL PRODUCT REPORTS
(2021)
Article
Chemistry, Physical
Anne P. Rasmusssen, Henrik B. Pedersen, Lars H. Andersen
Summary: This study utilizes time-resolved action spectroscopy and fs-pump probe scheme in an electrostatic ion-storage ring to investigate the lifetimes of specific vibrational levels in electronically excited states. The results show a significant decrease in lifetime when exciting higher vibrational levels, attributed to the opening of internal conversion over an excited-state energy barrier. These findings provide a new method to uncover small energy barriers in excited-state dynamics.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Alisia Fadini, Christopher D. M. Hutchison, Dmitry Morozov, Jeffrey Chang, Karim Maghlaoui, Samuel Perrett, Fangjia Luo, Jeslyn C. X. Kho, Matthew G. Romei, R. Marc L. Morgan, Christian M. Orr, Violeta Cordon-Preciado, Takaaki Fujiwara, Nipawan Nuemket, Takehiko Tosha, Rie Tanaka, Shigeki Owada, Kensuke Tono, So Iwata, Steven G. Boxer, Gerrit Groenhof, Eriko Nango, Jasper J. van Thor
Summary: This study successfully visualizes the hula twist mechanism in a fluorescent protein and provides the first experimental evidence of the mechanism on a femtosecond-to-picosecond timescale. It also shows how chromophore isomerization and twisting lead to rearrangement of the protein's secondary structure.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Ming-Ju Li, Yen-Hsun Lin, Robert Sung, Kuangsen Sung
Summary: In this study, the E-Z isomerization mechanism of p-HBDI in water through remote-proton-dissociation-regulated direct mechanism was explored, indicating that the proton dissociation from the phenol group of p-HBDI remotely regulates its E-Z isomerization, rather than the water-assisted addition/elimination mechanism.
JOURNAL OF PHYSICAL CHEMISTRY A
(2021)
Article
Polymer Science
Peng Zhang, Jianmin Gao, Fu Liu, Yao Chen, Yao Peng
Summary: This study used conventional thermal treatment to regulate the color of Eucalyptus wood, making it similar to Burma padauk, a precious wood species. The color change was analyzed using chromaticity index and UV-Vis, while the chromophore structures and discoloration mechanisms were characterized using FTIR, XPS, NMR, etc. The results showed that the color of eucalyptus could be regulated to resemble Burma padauk through thermal treatment, with changes in chromophore structures and degradation of hemicelluloses playing a significant role.
Article
Chemistry, Applied
J. M. Herrera, M. E. Penoff, M. J. Galante
Summary: The authors synthesized a fluorinated epoxy-isocyanate thermosetting coating modified with an azobenzene derivative. By UV irradiation, the fluorinated azobenzene derivative migrated to the coating surface, resulting in changes in the surface hydrophobicity. These reversible photo-induced surface property switching coatings have potential applications in various technological fields.
PROGRESS IN ORGANIC COATINGS
(2023)
Article
Chemistry, Physical
Sergey Yu. Ketkov, Sheng-Yuan Tzeng, Elena A. Rychagova, Anton N. Lukoyanov, Wen-Bih Tzeng
Summary: Metallocenes, including methylcobaltocene, play important roles in various fields of chemistry. The ionization energy and vibrational structure of (Cp ')(Cp)Co can be influenced by introducing methyl substituents. The mass-analyzed threshold ionization spectrum and DFT calculations provide accurate information about the properties and transformations of (Cp ')(Cp)Co.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Review
Chemistry, Physical
Qifeng Mu, Jian Hu
Summary: Polymer mechanochemistry has experienced a renaissance due to the rapid development of mechanophores and principles governing mechanochemical transduction or material strengthening. It has not only provided fundamental guidelines for converting mechanical energy into chemical output, but also found applications in engineering and smart devices.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Da Hye Yang, Francesco Ricci, Fredrik L. Nordstrom, Na Li
Summary: Through systematic evaluation of the oiling-out behavior of procaine, we identified both stable and metastable liquid-liquid phase separation, and established phase diagrams to assist in rational selection of crystallization strategies.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Vikki Anand Varma, Simmie Jaglan, Mohd Yasir Khan, Sujin B. Babu
Summary: Designing engineering structures like nanocages, shells, and containers through self-assembly of colloids is a challenging problem. This work proposes a simple model for the subunit, which leads to the formation of monodispersed spherical cages or containers. The model with only one control parameter can be used to design cages with the desired radius.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Hainan Jiang, Yaolong He, Xiaolin Li, Zhiyao Jin, Huijie Yu, Dawei Li
Summary: The cycling lifespan and coulombic efficiency of lithium-ion batteries are crucial for high C-rate applications. The Li-ion concentration plays a crucial role in determining the mechanical integrity and structural stability of electrodes. This study focuses on graphite as the working electrode and establishes an experimental system to investigate the mechanical properties of composite graphite electrode at different C-rates. Considering the effect of Li-ion concentration in stress analysis is found to be significant.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Zhiye Wang, Yunchuan Li, Mingjun Sun
Summary: This study investigates the influence of intramolecular pi-pi interactions on the electronic transport capabilities of molecules. By designing and analyzing three pi-conjugated molecules, the researchers observe that different pi-conjugated structures have varying effects on electron transport. The findings provide a theoretical foundation for designing single-molecule electronic devices with multiple electron channels based on intramolecular pi-pi interactions.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Yuandong Xu, Haoyang Feng, Chaoyang Dong, Yuqing Yang, Meng Zhou, Yajun Wei, Hui Guo, Yaqing Wei, Jishan Su, Yingying Ben, Xia Zhang
Summary: Hollow MoS2 cubes and spheres were successfully synthesized using a one-step hydrothermal method with the hard template method. The hollow MoS2 cubes exhibited higher specific capacitance and energy density compared to the hollow MoS2 spheres. The symmetrical supercapacitors assembled with these hollow structures showed good performance and high capacity retention after multiple cycles. These findings suggest that controlling the pore structure and surface characteristics of MoS2 is crucial for enhancing its electrochemical properties.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Ainhoa Oliden-Sanchez, Rebeca Sola-Llano, Joaquin Perez-Pariente, Luis Gomez-Hortiguela, Virginia Martinez-Martinez
Summary: The combination of photoactive molecules and inorganic structures is important for the development of advanced materials in optics. In this study, bulky dyes were successfully encapsulated in a zeolitic framework, resulting in emission throughout the visible spectrum.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Miaomiao Zhang, Cunyuan Pei, Qiqi Xiang, Lintao Liu, Zhongxu Dai, Huijuan Ma, Shibing Ni
Summary: The design of a solid electrolyte interphase (SEI) plays a crucial role in improving the electrochemical performance of anode materials. In this study, lithium difluoro(oxalate)borate (LiDFOB) is used as an electrolyte additive to form a protective SEI film on Li3VO4 (LVO) anodes. The addition of LiDFOB results in a dense, uniform, stable, and LiF-richer SEI, which enhances the Li-ion storage kinetics. The generated SEI also prevents further decomposition of the electrolyte and maintains the morphology of LVO anodes during charge/discharge processes. This work demonstrates the effectiveness of LiDFOB as a multi-functional additive for LiPF6 electrolytes and provides insights into SEI construction for high-performance LVO anodes.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
B. V. Andryushechkin, T. V. Pavlova, V. M. Shevlyuga
Summary: The atomic structure of the Ag(111)-p(4 x 4)-O phase was reexamined and two phases with the same periodicity were discovered. It was demonstrated that the accepted Ag6 model is incompatible with high-resolution oxygen-sensitive STM images.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
S. L. Romo-Avila, D. Marquez-Ruiz, R. A. Guirado-Lopez
Summary: In this study, we used density functional theory (DFT) calculations to investigate the interaction between model graphene oxide (GO) nanostructures and chlorine monoxide ClO. We aimed to understand the role of this highly oxidizing species in breaking C-C bonds and forming significant holes on GO sheets. Our results showed that C-C bonds in a single graphene oxide sheet can be broken through a simple mechanism involving the dissociation of two chemically attached ClO molecules. The formation of carbonyl groups and holes on the GO surface was also observed. This study provides important insights into the degradation of carbon nanotubes and the stability of GO during the myeloperoxidase (MPO) catalytic cycle.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Alberto Garcia-Fernandez, Birgit Kammlander, Stefania Riva, Hakan Rensmo, Ute B. Cappel
Summary: In this study, the X-ray stability of five different lead halide perovskite compositions (MAPbI3, MAPbCl3, MAPbBr3, FAPbBr3, CsPbBr3) was investigated using photoelectron spectroscopy. Different degradation mechanisms and resistance to X-ray were observed depending on the crystal composition. Overall, perovskite compositions based on the MA+ cation were found to be less stable than those based on FA+ or Cs+. Metallic lead formation was most easily observed in the chloride perovskite, followed by bromide, and very little in MAPbI3. Multiple degradation processes were identified for the bromide compositions, including ion migration, formation of volatile and solid products, as well as metallic lead. CsBr was formed as a solid degradation product on the surface of CsPbBr3.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Timofei Rostilov, Vadim Ziborov, Alexander Dolgoborodov, Mikhail Kuskov
Summary: The shock-loading behavior of nanomaterials is investigated in this study. It is found that shock compaction waves exhibit a distinct two-step structure, with the formation of faster precursor waves that travel ahead of the main compaction waves. The complexity of the shock Hugoniot curve of the tested nanomaterial is described, and the effect of initial porosity on the compressed states is demonstrated.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Sergey S. Nikitin, Alexander D. Koryakov, Elizaveta A. Antipinskaya, Alexey A. Markov, Mikhail V. Patrakeev
Summary: The stability of La1/3Sr2/3Fe1-xMnxO3-delta, a perovskite-type oxide, under reducing conditions is dependent on the manganese content. Increasing the manganese content leads to a decrease in stability. The behavior of iron and manganese in the oxide shows distinct differences, which can be attributed to the difference in the enthalpy of oxidation reactions. Additionally, the change in the La/Sr ratio affects the concentration of iron and manganese ions.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)
Article
Chemistry, Physical
Mosayeb Naseri, Shirin Amirian, Mehrdad Faraji, Mohammad Abdur Rashid, Maicon Pierre Lourenco, Venkataraman Thangadurai, D. R. Salahub
Summary: Inspired by the successful transfer of freestanding ultrathin films of SrTiO3 and BiFeO3, this study assessed the structural stability and investigated the electronic, optical, and thermoelectric properties of a group of two-dimensional perovskite-type materials called perovskenes. The findings revealed that these materials are wide bandgap semiconductors with potential application in UV shielding. Moreover, they exhibit better electrical and thermal conductivity at high temperatures, enabling efficient power generation in thermoelectric devices.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2024)