Article
Green & Sustainable Science & Technology
Gabriella Buscemi, Danilo Vona, Roberta Ragni, Roberto Comparelli, Massimo Trotta, Francesco Milano, Gianluca Maria Farinola
Summary: Photoactive biohybrid soft nanoparticles, obtained by embedding Rhodobacter sphaeroides Reaction Center (RC) in polydopamine (PDA) suspended aggregates and treating them with ethylenediamine (EDA), demonstrate improved water dispersity, light collection ability, and photocurrent generation in photoelectrochemical cells compared to pure PDA@RC precursors. This enhanced performance is attributed to the ability of PDA:EDA@RC nanoparticles to maintain the structural and functional integrity of the photosynthetic protein, resulting in nearly doubled photocurrents compared to PDA@RC due to the increased charge separated state generation. These findings highlight the potential of biohybrid composites as effective functional nanostructures for sunlight photoconversion in biocompatible polymer composites.
ADVANCED SUSTAINABLE SYSTEMS
(2021)
Article
Biochemistry & Molecular Biology
Nikki Cecil M. Magdaong, James C. Buhrmaster, Kaitlyn M. Faries, Haijun Liu, Gregory A. Tira, Jonathan S. Lindsey, Deborah K. Hanson, Dewey Holten, Philip D. Laible, Christine Kirmaier
Summary: The study describes the substitution of all possible natural amino acids for LeuL185 near the B-side bacteriopheophytin in bacterial reaction center. Different mutations result in the presence of magnesium chlorin or bacteriochlorophyll a in the place of H-B, leading to the formation of a charge-separated state P+CB- in some cases. This finding suggests new strategies for amino acid control over pigment type at specific sites in photosynthetic proteins.
Article
Chemistry, Physical
Toru Kondo, Risa Mutoh, Shun Arai, Genji Kurisu, Hirozo Oh-Oka, Satoru Fujiyoshi, Michio Matsushita
Summary: This study investigates the polarization dependence and role of red-Bchl g in the photosynthetic reaction center. A candidate molecule for red-Bchl g is proposed based on fluorescence spectra and structural data. The study finds that while the energy transfer network in the reaction center can be perturbed by local conformational dynamics, the overall energy transfer efficiency remains relatively stable.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Vytautas Bubilaitis, Olga Rancova, Darius Abramavicius
Summary: Exciton energy relaxation in a bacterial Reaction Center (bRC) pigment-protein aggregate may involve emission of high energy vibrational quanta. The study assessed this hypothesis using vibronic two-particle theory and found that specific high frequency vibrations may be responsible for the excitation relaxation process.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Thomas Schnappinger, Regina de Vivie-Riedle
Summary: Researchers use ultrafast optical techniques to study molecular dynamics involving both nuclear and electronic motions, and theoretical approaches are needed for interpretation. They revisit and expand a coupled description method for simulating molecular dynamics and aim to control the system dynamics using laser pulses.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Biochemistry & Molecular Biology
Jing-Hua Chen, Weiwei Wang, Chen Wang, Tingyun Kuang, Jian-Ren Shen, Xing Zhang
Summary: This study reports the structure of the photosynthetic reaction center complex (RCC) in green sulfur bacteria, which consists of a RC core, two FMO trimers, and two new subunits. The structure reveals a new bacteriochlorophyll and provides insights into the energy transfer network within this photosynthetic apparatus.
JOURNAL OF INTEGRATIVE PLANT BIOLOGY
(2023)
Review
Chemistry, Multidisciplinary
Samantha M. Harvey, Michael R. Wasielewski
Summary: Research has shown that spin-polarized radical pair spectra are observed in chemical and photosynthetic systems when the distance between the two radicals is restricted, leading to the formation of spin-correlated radical pairs. These spin-correlated radical pairs can serve as spin qubit pairs, allowing for manipulation of spin dynamics to study various quantum phenomena in the field of quantum information science.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Physics, Multidisciplinary
A. Shumilin, D. S. Smirnov
Summary: The study provides a compact analytical solution for the nuclear spin dynamics in the central spin box model under the condition of many nuclear spins, revealing the behavior of nuclear spins in a magnetic field and their correlation with electron spins. The results are beneficial for calculating the nuclear spin noise spectrum and describing effects such as nuclear spin squeezing and many-body entanglement.
PHYSICAL REVIEW LETTERS
(2021)
Article
Chemistry, Physical
Giordano Amoruso, Juntai Liu, Daniel W. Polak, Kavita Tiwari, Michael R. Jones, Thomas A. A. Oliver
Summary: RCs are crucial components of natural photosystems, converting solar energy into a potential difference that powers much of biology. By coupling RCs with synthetic light-harvesting materials, such as a nanoconjugate assembled from a synthetic quantum dot (QD) antenna and a tailored fluorescent RC, the efficiency of energy transfer from QDs to attached RCs can be achieved within a short timescale of 26.6 ns with high efficiency of 0.75.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Biochemistry & Molecular Biology
Emiliano Altamura, Francesco Milano, Pasquale Stano, Fabio Mavelli
Summary: The charge recombination kinetics of bacterial photosynthetic protein Reaction Center is highly sensitive to the actual occupancy of ubiquinone-10 in its Q(B)-binding site, allowing for assessment of the growth and aggregation/fusion of phosphocholine vesicles embedding RC in their membrane when treated with sodium oleate.
PHOTOCHEMICAL & PHOTOBIOLOGICAL SCIENCES
(2021)
Article
Multidisciplinary Sciences
Dmitry Shcherbakov, Petr Stepanov, Shahriar Memaran, Yaxian Wang, Yan Xin, Jiawei Yang, Kaya Wei, Ryan Baumbach, Wenkai Zheng, Kenji Watanabe, Takashi Taniguchi, Marc Bockrath, Dmitry Smirnov, Theo Siegrist, Wolfgang Windl, Luis Balicas, Chun Ning Lau
Summary: Spin-orbit coupling (SOC) is a relativistic effect that can eliminate spin degeneracy and lead to various magnetic, spintronic, and topological phenomena. In atomically thin InSe, SOC and intrinsic spin splitting can be widely adjusted and even enhanced in some devices.
Article
Chemistry, Physical
Jie Fang, Zi-Hao Chen, Yu Su, Zi-Fan Zhu, Yao Wang, Rui-Xue Xu, YiJing Yan
Summary: This study proposes a mixed dynamic approach to investigate open systems in photosynthesis. By considering the non-Markovian quantum phonon bath and the Lindblad master equation, the non-Markovian quantum coherent effects on photosynthetic processes are revealed. These findings have important implications for the design of organic photovoltaic devices.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Physics, Applied
Hyma H. Vallabhapurapu, James P. Slack-Smith, Vikas K. Sewani, Chris Adambukulam, Andrea Morello, Jarryd J. Pla, Arne Laucht
Summary: The study demonstrates fast and coherent control of a negatively charged nitrogen-vacancy spin ensemble using a high permittivity KTaO3 dielectric resonator at cryogenic temperatures. Rabi frequencies up to 48 MHz were achieved, with a high power-to-field conversion factor. The dielectric resonator offers advantages such as ease of assembly, in situ tunability, high magnetic field conversion efficiency, low-volume footprint, and optical transparency, making it a promising platform for microwave field delivery for spin control at cryogenic temperatures.
PHYSICAL REVIEW APPLIED
(2021)
Article
Chemistry, Physical
S. Kollarics, F. Simon, A. Bojtor, K. Koltai, G. Klujber, M. Szieberth, B. G. Markus, D. Beke, K. Kamaras, A. Gali, D. Amirari, R. Berry, S. Boucher, D. Gavryushkin, G. Jeschke, J. P. Cleveland, S. Takahashi, P. Szirmai, L. Forro, E. Emmanouilidou, R. Singh, K. Holczer
Summary: High concentration of negatively charged nitrogen-vacancy (NV-) centers was successfully created in diamond single crystals containing approximately 100 ppm nitrogen using electron and neutron irradiation and subsequent thermal annealing. The formation process and properties of NV- centers were observed, with about 25% of vacancies forming NVs during the annealing process, and high precision measurement of hyperfine and quadrupole coupling constants was achieved using EPR techniques.
Article
Materials Science, Multidisciplinary
Jun Ishihara, Takuya Suzuki, Go Kitazawa, Takachika Mori, Yuzo Ohno, Kensuke Miyajima
Summary: The spatiotemporal spin dynamics of two-dimensional electron spins in a GaAs quantum well were investigated using magneto-optical Kerr rotation measurements. The results showed that the ballistic movement of photoexcited spins resulted in a wave-packet-like motion of the spin distribution, which disappeared at higher spin densities and converged to the helical spin mode observed in the diffusive regime.
Article
Chemistry, Physical
S. Kollarics, F. Simon, A. Bojtor, K. Koltai, G. Klujber, M. Szieberth, B. G. Markus, D. Beke, K. Kamaras, A. Gali, D. Amirari, R. Berry, S. Boucher, D. Gavryushkin, G. Jeschke, J. P. Cleveland, S. Takahashi, P. Szirmai, L. Forro, E. Emmanouilidou, R. Singh, K. Holczer
Summary: High concentration of negatively charged nitrogen-vacancy (NV-) centers was successfully created in diamond single crystals containing approximately 100 ppm nitrogen using electron and neutron irradiation and subsequent thermal annealing. The formation process and properties of NV- centers were observed, with about 25% of vacancies forming NVs during the annealing process, and high precision measurement of hyperfine and quadrupole coupling constants was achieved using EPR techniques.
Article
Biochemistry & Molecular Biology
Chandrima Jash, Akiva Feintuch, Shira Nudelman, Nurit Manukovsky, Elwy H. Abdelkader, Sudeshna Bhattacharya, Gunnar Jeschke, Gottfried Otting, Daniella Goldfarb
Summary: This study compared the solution binding modes of MARCKS and IQ peptides with CaM using DEER and paramagnetic NMR techniques. It was found that MARCKS binding with CaM did not result in a closed conformation, while IQ binding generated a closed conformation. A solution structure model derived from elastic network modeling was in good agreement with the crystal structure.
Article
Chemistry, Multidisciplinary
Irina Ritsch, Elisabeth Lehmann, Leonidas Emmanouilidis, Maxim Yulikov, Frederic Allain, Gunnar Jeschke
Summary: The interaction between hnRNP A1 and specific RNA induces liquid-droplet formation, which depends on RNA concentration and sequence. Additionally, point mutations in RNA affect local protein dynamics.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Physical
Yu Rao, Chad T. Palumbo, Amrit Venkatesh, Megan Keener, Gabriele Stevanato, Anne-Sophie Chauvin, Georges Menzildjian, Sergei Kuzin, Maxim Yulikov, Gunnar Jeschke, Anne Lesage, Marinella Mazzanti, Lyndon Emsley
Summary: Nuclear magnetic resonance has low sensitivity, but this can be overcome by dynamic nuclear polarization (DNP). New Gd(III) complexes offer potential for more efficient magic angle spinning DNP.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Multidisciplinary
Lukas Rochlitz, Quentin Pessemesse, Jorg W. A. Fischer, Daniel Klose, Adam H. Clark, Milivoj Plodinec, Gunnar Jeschke, Pierre-Adrien Payard, Christophe Coperet
Summary: The development of highly performing propane dehydrogenation (PDH) catalysts that can withstand harsh regeneration conditions is crucial due to the increasing demand for short chain olefins like propene for plastics production. In this study, a nanometric, bimetallic Pt-Mn material supported on silica was prepared using a combination of surface organometallic chemistry and thermolytic molecular precursor approach. The material exhibited excellent performance in the PDH reaction with low deactivation rate and outstanding robustness during repeated regeneration cycles.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Multidisciplinary Sciences
Liam Grunwald, Martin Clemancey, Daniel Klose, Lionel Dubois, Serge Gambarelli, Gunnar Jeschke, Michael Worle, Genevieve Blondin, Victor Mougel
Summary: A complete series of [Fe4S4](n) complexes spanning all redox states accessible by 1-electron transformations of the individual iron atoms has been successfully synthesized using a bulky arylthiolate ligand. The characterization results suggest a systematic correlation between the geometry of the Fe4S4 core and the oxidation state.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Multidisciplinary Sciences
Alexandra Born, Janne Soetbeer, Morkos A. Henen, Frauke Breitgoff, Yevhen Polyhach, Gunnar Jeschke, Beat Voegeli
Summary: Pin1 is a cell regulator with two domains. Ligand binding can change the conformation of these domains, thus affecting its catalytic site.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Dario Faust Akl, Georgios Giannakakis, Andrea Ruiz-Ferrando, Mikhail Agrachev, Juan D. Medrano-Garcia, Gonzalo Guillen-Gosalbez, Gunnar Jeschke, Adam H. Clark, Olga V. Safonova, Sharon Mitchell, Nuria Lopez, Javier Perez-Ramirez
Summary: Copper catalysts are promising for Hg-free VCM production, but the optimal architecture at the nanoscale is not well understood. This study modifies the metal precursor and annealing temperature to prepare copper nanoparticles or single atoms on an unmodified carbon support. The performance of all materials converges to the stable VCM productivity of the single-atom catalyst. Advanced characterization techniques uncover a reaction-induced formation of low-valent, single atom Cu(I)Cl site motif, regardless of the initial nanostructure. The study highlights the sustainability of Cu-based catalysts for VCM production.
ADVANCED MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Joerg Wolfram Anselm Fischer, Andreas Brenig, Daniel Klose, Jeroen Anton van Bokhoven, Vitaly L. Sushkevich, Gunnar Jeschke
Summary: This study determined the Cu speciation in Cu-MOR materials with different Cu loadings using operando electron paramagnetic resonance (EPR), operando ultraviolet-visible (UV/Vis) spectroscopy, as well as in situ photoluminescence (PL) and Fourier-transform infrared (FTIR) spectroscopy. A novel pathway for CH4 oxidation involving paired [CuOH](+) and bare Cu2+ species was identified. The reduction of bare Cu2+ ions facilitated by adjacent [CuOH](+) demonstrates that the commonly assumed redox-inert Cu2+ centers do not generally apply. Site-specific reaction kinetics showed that dimeric Cu species exhibit a faster reaction rate and a higher apparent activation energy than monomeric Cu2+ active sites, highlighting their difference in the CH4 oxidation potential.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Chemistry, Physical
Thaylan Pinheiro Araujo, Jordi Morales-Vidal, Tangsheng Zou, Mikhail Agrachev, Simon Verstraeten, Patrik O. O. Willi, Robert N. N. Grass, Gunnar Jeschke, Sharon Mitchell, Nuria Lopez, Javier Perez-Ramirez
Summary: Mixed zinc-zirconium oxides, ZnZrOx, synthesized using flame spray pyrolysis (FSP) exhibit higher methanol productivity and enhanced performance compared to coprecipitated (CP) catalysts. In-depth characterization and theoretical simulations reveal that FSP maximizes surface area and atomically dispersed Zn2+ sites, leading to improved catalytic activity. The study also demonstrates the working mechanism of the flame-made catalyst and provides valuable insights for the development of cost-effective and earth-abundant catalysts for methanol synthesis.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Inorganic & Nuclear
Patrick Mueller, Patrick Finkelstein, Nils Trapp, Alessandro Bismuto, Gunnar Jeschke, Bill Morandi
Summary: This paper presents a broad applicability of a specific method for preparing monovalent nickel complexes, and demonstrates the diversity and versatility of these complexes.
INORGANIC CHEMISTRY
(2023)
Article
Multidisciplinary Sciences
Vera Giulimondi, Andrea Ruiz-Ferrando, Georgios Giannakakis, Ivan Surin, Mikhail Agrachev, Gunnar Jeschke, Frank Krumeich, Nuria Lopez, Adam H. Clark, Javier Perez-Ramirez
Summary: This study demonstrates the bifunctionality of carbon supports and metal sites in the acetylene hydrochlorination catalytic cycle, and proposes potential binding sites for acetylene and a viable reaction profile. The results highlight the importance of optimizing both metal and support components for catalyst design.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Lukas Rochlitz, Jorg W. A. Fischer, Quentin Pessemesse, Adam H. Clark, Anton Ashuiev, Daniel Klose, Pierre-Adrien Payard, Gunnar Jeschke, Christophe Coperet
Summary: This study investigates the effect of Ti doping on the catalytic performance of Pt and PtZn materials in propane dehydrogenation. The results show that Ti-doping significantly changes the electronic structure of nanoparticles and improves the stability of the materials.
Article
Chemistry, Multidisciplinary
Devi Prasad Adiyeri Saseendran, Jorg W. A. Fischer, Lea Muller, Daniel F. Abbott, Victor Mougel, Gunnar Jeschke, Carlos A. Triana, Greta R. Patzke
Summary: This report presents the synthesis and spectroscopic evidence of a new defect-cubane type copper complex that acts as a pre-catalyst for water oxidation. In situ and post-catalytic studies reveal that the tetrameric complex undergoes structural transformations into dimeric and monomeric species induced by water molecules and carbonate anions, respectively. Moreover, the observed electrocatalytic water oxidation activity is confirmed to arise from in situ-generated Cu(ii) oxidic nanostructures at the electrode interface.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Andrea Eggeling, Janne Soetbeer, Luis Fabregas-Ibanez, Daniel Klose, Gunnar Jeschke
Summary: This study introduces the methyl quantum rotor (MQR) model to describe the tunneling ESEEM originating from multiple methyl rotors coupled to the same electron spin. By formulating the MQR model based on a rotation barrier distribution P(V-3), the different local environments in a glassy matrix can be accounted for. The rotation barrier distribution of the methyl groups is determined from experimental data and shows good agreement with density functional theory (DFT) calculations.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
