Article
Chemistry, Multidisciplinary
Martin T. Peschel, Piotr Kabacinski, Daniel P. Schwinger, Erling Thyrhaug, Giulio Cerullo, Thorsten Bach, Juergen Hauer, Regina de Vivie-Riedle
Summary: Lewis acids have been recognized as catalysts for enantioselective photochemical transformations, but mechanistic studies on these systems are rare. This work overcomes the challenges by using sub-30-fs transient absorption in the UV and accurate theoretical treatment. Investigations on the 2-cyclohexenone and boron trifluoride complex reveal that the Lewis acid remains attached to the substrate in the triplet state, leading to high enantioselectivity.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Pavel A. Kusochek, Andrei Scherbinin, Anastasia Bochenkova
Summary: Research on the light-driven sodium-pump rhodopsin KR2 revealed the presence of reactive and nonreactive states, exploring the mechanisms through molecular dynamics simulations and large-scale QM/MM modeling. By calculating vibronic band shapes, insights into the early-time excited-state dynamics of PSBR were gained, highlighting the role of the protein environment in facilitating photoisomerization. The study also emphasized the importance of a strong hydrogen bond between the retinal Schiff base and its counterion for ultrafast reaction dynamics.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Chemistry, Physical
Summer L. Sherman, Kathleen A. Nickson, Etienne Garand
Summary: This viewpoint re-examines the conclusions of a study comparing the structure of microsolvated ions formed by electrospray ionization and a cryogenic ion trap approach. Additional experiments show that the observed differences in IR spectra can be explained by different spectroscopic action schemes. After considering these spectral effects, both methods yield similar cluster structures.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Nanoscience & Nanotechnology
Yinuo Xu, Binzhang Jiao, Yingchen Wang, Songyan Xue, Hui Gao, Kewang Yu, Xuhao Fan, Yuncheng Liu, Yufeng Tao, Leimin Deng, Wei Xiong
Summary: Molybdenum disulfide (MoS2) is widely used in various applications due to its unique optoelectrical and chemical characteristics. In this work, a single-step femtosecond laser-induced photochemical method is proposed for the fabrication of microscale MoS2 patterns with high efficiency. The method enables the synthesis of MoS2 at a rate 2 orders of magnitude faster than existing methods, while maintaining resolution and quality. Additionally, the method is demonstrated for the fabrication of high-sensitivity MoS2-based gas detectors. The proposed method not only offers a cost-effective and precise approach for MoS2 patterns and devices, but also provides potential for other transition metal sulfides and functional materials.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Biochemistry & Molecular Biology
Martin Hajek, Tomas Hajek, David Kocian, Karel Frolich, Andras Peller
Summary: This paper investigates the epoxidation of methyl esters derived from oil crops with different profiles of higher fatty acids, particularly unsaturated ones found in non-edible linseed and Camelina sativa oil (second generation). The study focuses on separating and identifying all products with oxirane rings formed during the reaction, as well as determining the time course. Multiple intermediates and final products, including epoxides with varying numbers and positions of oxirane rings in the carbon chain, were formed through the epoxidation process. Three main methods (infrared spectroscopy, high-pressure liquid chromatography, and gas chromatography with mass spectrometry) were used for the determination, with gas chromatography being the only one capable of separating individual epoxides. This method allowed for identification based on mass spectra, molecule ion, and time course. The determination of intermediates provides control over the epoxidation process, detailed analysis of epoxide mixtures, and calculation of selectivity for each product. As a result, epoxidation can be more environmentally friendly, especially for utilizing non-edible oil crops with high levels of unsaturated fatty acids.
Article
Multidisciplinary Sciences
Kristina S. Zinchenko, Fernando Ardana-Lamas, Issaka Seidu, Simon P. Neville, Joscelyn van der Veen, Valentina Utrio Lanfaloni, Michael S. Schuurman, Hans Jakob Worner
Summary: In this study, the fastest electronic relaxation dynamics to date was observed using attosecond transient-absorption spectroscopy (ATAS) extended to the carbon K-edge. By selectively launching wave packets in the two lowest electronic states of C2H4+, the electronic relaxation process was visualized and multidimensional structural dynamics of the molecule were simultaneously observed. These results demonstrate the capability to resolve the fastest electronic and structural dynamics in a broad class of organic molecules, showing that electronic relaxation in organic chromophores can occur within less than a single vibrational period.
Article
Chemistry, Physical
Tobias Unruh, Luis I. Domenianni, Peter Vohringer
Summary: The elementary light-triggered dynamics of the transition metal complex were investigated using femtosecond mid-infrared and UV-Vis spectroscopies, revealing the sequential intramolecular electron transfer process involved in the system.
Article
Biochemistry & Molecular Biology
Jack Dalton, Gareth W. Richings, Jack M. Woolley, Temitope T. Abiola, Scott Habershon, Vasilios G. Stavros
Summary: In this study, the S-1(pi pi*) lifetime of the s-cis conformer of para-hydroxy methylcinnamate was accurately measured to be around 2.5 picoseconds, with the major non-radiative decay route following the [(1)pi pi*->(1)n pi*->(3)pi pi*-> S-0] pathway. These findings are consistent with previous photodynamical studies on structurally similar molecules such as para-coumaric acid and methylcinnamate.
Article
Spectroscopy
Adam Pastorek, Victoria H. J. Clark, Sergei N. Yurchenko, Martin Ferus, Svatopluk Civis
Summary: This work presents a time-resolved FTIR spectroscopic study on the kinetics of atomic and molecular species generated in a glow discharge of formamide-nitrogen-water mixture in a helium buffer gas. The study focuses on CO, CN radical, N-2, HCN, and CO2, which play important roles in prebiotic synthesis of organic molecules. The research includes analysis of decomposition products, energy transfer between excited nitrogen and CO, and theoretical modeling of formamide decomposition process.
SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
(2022)
Article
Nanoscience & Nanotechnology
Dorothee Menzel, Alvaro Tejada, Amran Al-Ashouri, Igal Levine, Jorge Andres Guerra, Bernd Rech, Steve Albrecht, Lars Korte
Summary: This study employs advanced near-UV photoemission spectroscopy to investigate the density of occupied states in the valence band and band gap of a triple-cation lead halide perovskite. A valence band model is established to accurately determine valence band maxima at different k-vectors, providing insights into defect states formation during perovskite decomposition. The research highlights the effectiveness of near-UV CFSYS with modeling in characterizing the valence band and quantifying defect states in lead halide perovskites.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Review
Chemistry, Multidisciplinary
Xue Zhanghttps, Xiaoyu Zhao, Kaiyue Yehttps, Jianzhang Zhao
Summary: The photophysical processes involved in TADF emitters are complex and controversial, with consensus that at least three states are involved. Steady state and time-resolved luminescence spectroscopic methods cannot directly provide evidence for the dark states and their interconversion. Transient absorption spectroscopy is of particular interest as it can detect both emissive and dark states, and reveal the interconversion of states involved in TADF process. This review article focuses on the recent development of using transient absorption spectra to study the photophysics of TADF emitters.
CHEMISTRY-A EUROPEAN JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Mauro Falconieri, Davide Tedeschi, Serena Gagliardi, Flaminia Rondino, Michele Marrocco, Waruna D. D. Kulatilaka
Summary: Femtosecond coherent Raman techniques are valuable for sensitive and non-intrusive measurements of temperature, pressure, and composition of gas mixtures. This paper demonstrates an experimental setup using a low-energy and low-average-power femtosecond oscillator to measure the pure-rotational spectrum of nitrogen at atmospheric pressure. Gas temperature can be derived with reasonable accuracy using a simplified model to analyze the experimental data.
APPLIED SCIENCES-BASEL
(2022)
Article
Optics
Chengcheng Zhu, Ben Chen, Yini Chen, Tao Yang, Hailing Wang, Jianping Yin
Summary: The pendular spectra of linear (HCCCN)(n) (n = 1-3) molecules were calculated under various rotational temperatures and electric field strengths. The normalized Q-branch intensity and its gradient were investigated. The study analyzed the range and sensitivity of measuring electric field strength with these molecules and proposed a high sensitivity scheme.
JOURNAL OF THE OPTICAL SOCIETY OF AMERICA B-OPTICAL PHYSICS
(2021)
Article
Chemistry, Physical
Peter Salen, Luca Schio, Robert Richter, Michele Alagia, Stefano Stranges, Stefano Falcinelli, Vitali Zhaunerchyk
Summary: The potential for selective bond breaking of ClNO was investigated using electron spectroscopy and electron-ion coincidence experiments. The experimental results showed that the electron-ion coincidences produced specific spectator and participator states, with significantly different branching fractions for the spectator states compared to the participator states. It was also observed that the bonds broken for the spectator states correlated with the antibonding nature of the spectator-electron orbital.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Elena Spagnoli, Matteo Valt, Andrea Gaiardo, Barbara Fabbri, Vincenzo Guidi
Summary: The influence of Nb addition in the oxide solid solution of Sn and Ti was investigated for the production of chemoresistive gas sensors. The sensors based on (Sn,Ti,Nb)(x)O-2 showed promising features for ethanol monitoring with low sensitivity to relative humidity. However, there is still a lack of understanding on the gas reaction mechanisms occurring at the surface of these nanostructures.
Article
Chemistry, Multidisciplinary
Alexander M. Prophet, Kritanjan Polley, Gary J. Van Berkel, David T. Limmer, Kevin R. Wilson
Summary: The oxidation kinetics of iodide by ozone at the air-water interface is studied in single microdroplets. Molecular simulations and kinetic modeling are used to understand the underlying multiphase mechanism.
Article
Chemistry, Multidisciplinary
Rong Zhang, Jiajing Lan, Fei Wang, Shumei Chen, Jian Zhang
Summary: By utilizing 1,1'-ferrocene dicarboxylic acid as a chelating and surface protection ligand, we have synthesized multi-nuclear indium oxide clusters with varying nuclear sizes, including heptanuclear and thirteen-nuclear clusters. These clusters possess labile coordination sites, allowing for structural modification and self-assembly, resulting in the formation of various cluster structures.
Article
Chemistry, Multidisciplinary
Hui Wang, Hui Liu, Mingsen Wang, Jiaheng Hou, Yongjun Li, Yuancheng Wang, Yingjie Zhao
Summary: Two supramolecular complexes were prepared using CBs and M1, and their single-crystal structures were analyzed by SCXRD. The unexpected 1:2 self-assembly structure between M1 and CB[8] was discovered for the first time. These complexes exhibit unique photophysical properties and provide valuable information about the structure and photophysical properties of supramolecular complexes.
Article
Chemistry, Multidisciplinary
Chang-Hee Lee, Sookil Park, Sanggil Kim, Ji Young Hyun, Hyun Soo Lee, Injae Shin
Summary: The epidermal growth factor receptor (EGFR) is a cell-surface glycoprotein involved in cell proliferation and tumor development. This study used a fluorescently labeled EGFR to investigate its time-dependent endocytosis in live cells and found that appended glycans affect EGFR internalization. Additionally, the study detected sialic acid residues attached to EGFR on the live cell surface using FRET-based imaging. This research provides valuable insights into the cellular functions of EGFR.
Article
Chemistry, Multidisciplinary
Subhankar Sahu, Lokesh Kumar, Sumita Das, Dipti Gupta, Ruchi Anand
Summary: This study proposes a strategy that combines organic electronics with biosensor scaffolds to create a compact device for monitoring environmental aromatic pollution. By coupling biosensing protein MopR with an organic electrochemical transistor (OECT), a sensor module capable of efficient detection of phenol was designed. Exclusive phenol detection with minimal loss of sensitivity could be achieved in complex pollutant mixtures and real environmental samples.
Review
Chemistry, Multidisciplinary
Changseok Lee, Hyung-Joon Kang, Sungwoo Hong
Summary: The formation of C-N bonds through hydroamination reactions catalyzed by nickel hydrides has been a topic of recent interest. This approach offers a way to efficiently transform a variety of alkene and alkyne substrates into compounds enriched with C-N bonds. The review provides a concise overview of the underlying reaction mechanisms and aims to stimulate further progress in NiH-catalytic techniques and catalyst design.
Article
Chemistry, Multidisciplinary
Yueci Wu, Lu-Lu Sun, Hai-Hao Han, Xiao-Peng He, Weiguo Cao, Tony D. James
Summary: Drug-induced liver injury (DILI) is a common cause of acute liver failure in the USA and Europe, but most cases can be recovered or prevented by discontinuing the offending drug. Recent research has found that peroxynitrite (ONOO-) can be used as a potential indicator for early diagnosis of DILI, and there is an urgent need to establish a method to detect and track peroxynitrite in DILI cases. In this study, a FRET-based nano fluorescent probe CD-N-I was developed, which showed high selectivity and sensitivity in detecting peroxynitrite. The probe successfully detected exogenous peroxynitrite in live cells and endogenous peroxynitrite in APAP-induced liver injury of HepG2 cells.
Article
Chemistry, Multidisciplinary
Dmitry L. Lipilin, Mikhail O. Zubkov, Mikhail D. Kosobokov, Alexander D. Dilman
Summary: This article describes a direct photocatalytic method for the thiolation of unprotected acids, which was previously challenging. By using a thionocarbonate reagent with an N-O bond, the efficient conversion of carboxylic acids to thiols is achieved.
Article
Chemistry, Multidisciplinary
Jason Malenfant, Lucille Kuster, Yohann Gagne, Kouassi Signo, Maxime Denis, Sylvain Canesi, Mathieu Frenette
Summary: Raman microscopy can reveal compound-specific vibrational fingerprints without sample preparation. The combination of efficient theoretical calculations and a user-friendly software can accurately predict peak positions and provide match scores to assist with structure determination.
Article
Chemistry, Multidisciplinary
Jayoh A. Hernandez, Paul S. Micus, Sean Alec Lois Sunga, Luca Mazzei, Stefano Ciurli, Gabriele Meloni
Summary: Essential trace metals play crucial roles in the survival and virulence of bacterial pathogens. Helicobacter pylori requires nickel for colonization and persistence in the stomach, and NixA is an essential nickel transporter in this process. This study characterizes the selectivity and electrogenic nature of NixA-mediated nickel transport.
Article
Chemistry, Multidisciplinary
Tarali Devi, Kuheli Dutta, Jennifer Deutscher, Stefan Mebs, Uwe Kuhlmann, Michael Haumann, Beatrice Cula, Holger Dau, Peter Hildebrandt, Kallol Ray
Summary: This study emphasizes the importance of subtle electronic changes and secondary interactions in the stability of biologically relevant metal-dioxygen intermediates. It also shows that the role of the chloride ligand in stabilizing the Fe-III-(OOBu)-Bu-t moiety can extend to other anions, including the thiolate ligand.
Article
Chemistry, Multidisciplinary
Jacqueline R. Santhouse, Jeremy M. G. Leung, Lillian T. Chong, W. Seth Horne
Summary: By studying the folding kinetics and mechanism of the BdpA sequence, researchers found that altering the backbone connectivity can affect protein folding. This suggests that protein mimetic chains have a significant degree of plasticity in transitioning between unfolded and folded states.
Article
Chemistry, Multidisciplinary
Divanshu Gupta, Ralf Einholz, Holger F. Bettinger
Summary: This study presents the first direct spectroscopic evidence of a cyclic seven-membered iminoborane. Compared to linear amino-iminoboranes, this cyclic iminoborane exhibits weakened bond strength and lower Lewis acidity value. The study suggests that the reduced ring strain of cyclic iminoborane prevents nitrogen fixation but allows facile (2 + 2) cycloaddition reaction with C2H4.
Article
Chemistry, Multidisciplinary
Renny Mathew, Aniruddha Mazumder, Praveen Kumar, Julie Matula, Sharmarke Mohamed, Petr Brazda, Mahesh Hariharan, Brijith Thomas
Summary: This study reveals the packing arrangement of partially disordered nitro-perylenediimide (NO2-PDI) using a synergistic approach that combines 3D ED, ssNMR, and DFT techniques. By overcoming these challenges, this methodology opens up new avenues for material characterization, driving exciting advancements in the field.