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Front Cover: Redox Reaction in Ti−Mn Redox Flow Battery Studied by X-ray Absorption Spectroscopy (Chem. Asian J. 1/2023)

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Chemistry – An Asian Journal 2022年第1期18卷

作者： Dr. Daisuke Asakura Dr. Eiji Hosono Dr. Miho Kitamura Dr. Koji Horiba Dr. Eisuke Magome Dr. Hiroyuki Setoyama Dr. Eiichi Kobayashi Dr. Hayato Yuzawa Dr. Takuji Ohigashi Dr. Takaaki Sakai Dr. Ryoichi Kanega Dr. Takashi Funaki Dr. Yukari Sato Dr. Akihiro Ohira Research Institute for Energy Conservation National Institute of Advanced Industrial Science and Technology (AIST) 1-1-1 Higashi Tsukuba Ibaraki 305-8565 Japan Global Zero Emission Research Center National Institute of Advanced Industrial Science and Technology (AIST) 16-1 Onogawa Tsukuba Ibaraki 305-8569 Japan AIST-University of Tokyo Advanced Operando-Measurement Open Innovation Laboratory 5-1-5 Kashiwanoha Kashiwa Chiba 277-8565 Japan Photon Factory Institute of Materials Structure Science High Energy Accelerator Research Organization (KEK) 1-1 Oho Tsukuba Ibaraki 305-0801 Japan SOKENDAI The Graduate University for Advanced Studies 1-1 Oho Tsukuba Ibaraki 305-0801 Japan Institute for Advanced Synchrotron Light Source National Institutes for Quantum Science and Technology (QST) 6-6-11-901 Aoba Aramaki Aoba-ku Sendai Miyagi 980-8579 Japan SAGA Light Source Kyushu Synchrotron Light Research Center 8-7 Yayoigaoka Tosu Saga 841-0005 Japan UVSOR Synchrotron Facility Institute for Molecular Science (IMS) 38 Nishigo-Naka Myodaiji Okazaki Aichi 444-8585 Japan

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Two-Step Electronic Response to Magnetic Ordering in a van der Waals Ferromagnet

arXiv

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arXiv 2023年

作者： Wu, Han Zhu, Jian-Xin Chen, Lebing Butcher, Matthew W. Yue, Ziqin Yuan, Dongsheng He, Yu Oh, Ji Seop Huang, Jianwei Wu, Shan Gong, Cheng Guo, Yucheng Mo, Sung-Kwan Denlinger, Jonathan D. Lu, Donghui Hashimoto, Makoto Stone, Matthew B. Kolesnikov, Alexander I. Chi, Songxue Kono, Junichiro Nevidomskyy, Andriy H. Birgeneau, Robert J. Dai, Pengcheng Yi, Ming Department of Physics and Astronomy Rice Center for Quantum Materials Rice University HoustonTX77005 United States Theoretical Division Los Alamos National Laboratory Los AlamosNM87545 United States Center for Integrated Nanotechnologies Los Alamos National Laboratory Los AlamosNM87545 United States Department of Physics University of California at Berkeley BerkeleyCA94720 United States Applied Physics Graduate Program Smalley-Curl Institute Rice University HoustonTX77005 United States Materials Sciences Division Lawrence Berkeley National Laboratory BerkeleyCA94720 United States 1-1 Namiki Ibaraki Tsukuba305-0044 Japan Department of Applied Physics Yale University New HavenCT06511 United States Department of Electrical and Computer Engineering Quantum Technology Center University of Maryland College ParkMD20742 United States Advanced Light Source Lawrence Berkeley National Laboratory BerkeleyCA94720 United States Stanford Synchrotron Radiation Lightsource SLAC National Accelerator Laboratory Menlo ParkCA94025 United States Neutron Scattering Division Oak Ridge National Laboratory Oak RidgeTN37831 United States Department of Electrical and Computer Engineering Rice University HoustonTX77005 United States Smalley-Curl Institute Rice University HoustonTX77005 United States Department of Material Science and NanoEngineering Rice University HoustonTX77005 United States Department of Materials Science and Engineering University of California Berkeley United States

The two-dimensional (2D) material Cr2Ge2Te6 is a member of the class of insulating van der Waals magnets. Here, using high resolution angle-resolved photoemission spectroscopy in a detailed temperature dependence study, we identify a clear response of the electronic structure to a dimensional crossover in the form of two distinct temperature scales marking onsets of modifications in the electronic structure. Specifically, we observe Te p-orbital-dominated bands to undergo changes at the Curie transition temperature TC while the Cr d-orbital-dominated bands begin evolving at a higher temperature scale. Combined with neutron scattering, density functional theory calculations, and Monte Carlo simulations, we find that the electronic system can be consistently understood to respond sequentially to the distinct temperatures at which in-plane and out-of-plane spin correlations exceed a characteristic length scale. Our findings reveal the sensitivity of the orbital-selective electronic structure for probing the dynamical evolution of local moment correlations in vdW insulating magnets. © 2023, CC BY.

关键词： Electronic structure

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Tunable and enhanced Rashba spin-orbit coupling in iridate-manganite heterostructures

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Physical Review B 2020年第12期102卷 125145-125145页

作者： T. S. Suraj Ganesh Ji Omar Hariom Jani M. M. Juvaid Sonu Hooda Anindita Chaudhuri Andrivo Rusydi K. Sethupathi Thirumalai Venkatesan Ariando Ariando M. S. Ramachandra Rao Department of Physics Nano Functional Materials Technology Center Material Science Research Center Indian Institute of Technology Madras Chennai 600036 India Low Temperature Physics Lab Department of Physics Indian Institute of Technology Madras Chennai 600036 India Department of Physics National University of Singapore Singapore 117542 Singapore NUSNNI-NanoCore National University of Singapore Singapore 117411 Singapore National University of Singapore Graduate School for Integrative Sciences and Engineering (NGS) University Hall 21 Lower Kent Ridge Road Singapore 119077 Singapore Singapore Synchrotron Light Source National University of Singapore 5 Research Link Singapore 117603 Singapore Department of Electrical and Computer Engineering National University of Singapore Singapore 117576 Singapore

Tailoring spin-orbit interactions and Coulomb repulsion are the key features to observe exotic physical phenomena such as magnetic anisotropy and topological spin texture at oxide interfaces. Our study proposes a platform for engineering magnetism and spin-orbit coupling at the LaMnO3/SrIrO3 (3d−5d) oxide interface by tuning the LaMnO3 growth conditions, which controls the lattice displacement and spin-correlated interfacial coupling through charge transfer. We report a tunable and enhanced interface-induced Rashba spin-orbit coupling where the spin relaxation mechanism varies with magnetic behavior of the underlying LaMnO3 layer. The x-ray spectroscopy measurements reveal the quantitative valence states of Mn and their impact on charge transfer. Our angle-dependent magnetoresistance measurements also reflects the signature of magnetic proximity effect in SrIrO3 and can be tuned with the magnetic nature of LaMnO3 in a LaMnO3/SrIrO3 bilayer. Our work demonstrates a route to engineer the interface-induced Rashba spin-orbit coupling and magnetic proximity effect at the 3d−5d oxide interface for spintronics applications.

关键词： Magnetoresistance Rashba coupling Spin relaxation Spin-orbit coupling Interfaces Strongly correlated systems

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2024 Roadmap on Magnetic Microscopy Techniques and Their Applications in Materials science

arXiv

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arXiv 2024年

作者： Christensen, Dennis V. Staub, Urs Devidas, T.R. Kalisky, B. Nowack, K.C. Webb, J.L. Andersen, U.L. Huck, A. Broadway, David A. Wagner, Kai Maletinsky, Patrick van der Sar, Toeno Du, Chunhui Rita Yacoby, Amir Collomb, David Bending, Simon Oral, Ahmet Hug, Hans J. Mandru, Andrada-Oana Neu, Volker Schumacher, Hans Werner Sievers, Sibylle Saito, Hitoshi Khajetoorians, A.A. Hauptmann, N. Baumann, S. Eichler, Alexander Degen, Christian L. McCord, Jeffrey Vogel, Michael Fiebig, Manfred Fischer, Peter Hierro-Rodriguez, Aurelio Finizio, Simon Dhesi, Sarnjeet S. Donnelly, Claire Büttner, Felix Kfir, Ofer Hu, Wen Zayko, Sergey Eisebitt, Stefan Pfau, Bastian Frömter, Robert Kläui, Mathias Yasin, Fehmi S. McMorran, Benjamin J. Seki, Shinichiro Yu, Xiuzhen Lubk, Axel Wolf, Daniel Pryds, Nini Makarov, Denys Poggio, Martino Department of Energy Conversion and Storage Technical University of Denmark Kgs. LyngbyDK-2800 Denmark Swiss Light Source Paul Scherrer Institute Villigen PSI5232 Switzerland Department of Physics Institute of Nanotechnology and Advanced Materials Bar-Ilan University Ramat Gan5290002 Israel Laboratory of Atomic and Solid-State Physics Cornell University IthacaNY14853 United States Kavli Institute Cornell for Nanoscale Science IthacaNY14853 United States Department of Physics Technical University of Denmark Kongens Lyngby2800 Denmark Department of Physics University of Basel Basel4056 Switzerland School of Science RMIT University MelbourneVIC Australia Department of Quantum Nanoscience Kavli Institute of Nanoscience Delft University of Technology Lorentzweg 1 Delft2628 CJ Netherlands Department of Physics University of California San Diego La Jolla CA92093 United States Department of Physics Harvard University 17 Oxford Street CambridgeMA02138 United States Quantum Brilliance GmbH Tullastraße 72 Freiburg im Breisgau Germany Department of Physics University of Bath BathBA2 7AY United Kingdom NanoMagnetics Instruments Ltd Suite 290 266 Banbury Road OxfordOX2 7DL United Kingdom Empa Materials Science and Technology Ueberlandstrasse 129 Duebendorf8600 Switzerland Leibniz Institute for Solid State and Materials Research DresdenD-01069 Germany Physikalisch-Technische Bundesanstalt Braunschweig38116 Germany Department of Mathematical Science and Electrical-Electronic-Computer Engineering Graduate School of Engineering Science Akita University Akita Japan Scanning Probe Microscopy Department Institute for Molecules and Materials Radboud University Nijmegen Netherlands University of Stuttgart Institute for Functional Matter and Quantum Technologies Stuttgart Germany Laboratory for Solid State Physics ETH Zürich Zürich8093 Switzerland Department for Materials Science Kiel University Kiel Germany Kiel University Kiel Germany D

Considering the growing interest in magnetic materials for unconventional computing, data storage, and sensor applications, there is active research not only on material synthesis but also characterisation of their properties. In addition to structural and integral magnetic characterisations, imaging of magnetization patterns, current distributions and magnetic fields at nano- and microscale is of major importance to understand the material responses and qualify them for specific applications. In this roadmap, we aim to cover a broad portfolio of techniques to perform nano- and microscale magnetic imaging using SQUIDs, spin center and Hall effect magnetometries, scanning probe microscopies, x-ray- and electron-based methods as well as magnetooptics and nanoMRI. The roadmap is aimed as a single access point of information for experts in the field as well as the young generation of students outlining prospects of the development of magnetic imaging technologies for the upcoming decade with a focus on physics, materials science, and chemistry of planar, 3D and geometrically curved objects of different material classes including 2D materials, complex oxides, semi-metals, multiferroics, skyrmions, antiferromagnets, frustrated magnets, magnetic molecules/nanoparticles, ionic conductors, superconductors, spintronic and spinorbitronic materials. Copyright © 2024, The Authors. All rights reserved.

关键词： Spin dynamics

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Depth Dependence of the Photoelectron Emission Profile for Cathode Lens Microscopy

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Microscopy and Microanalysis 2018年第S2期24卷 154-155页

作者： Huang, Yen Chuang, Tzu-Hung Lu, Chun-I Huang, Chih-Heng Lin, Deng-Sung Kuo, Chien-Chen Wei, Der-Hsin Graduate Program of Science and Technology of Synchrotron Light Source National Tsing Hua University Hsinchu Taiwan National Synchrotron Radiation Research Center Hsinchu Taiwan Program of Synchrotron Radiation and Neutron Beam Applications National Sun Yat-sen University Kaohsiung Taiwan Department of Physics National Tsing Hua University Hsinchu Taiwan

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Correction: Shear-induced polydomain structures of nematic lyotropic chromonic liquid crystal disodium cromoglycate

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Soft matter 2021年第21期17卷 5444页

作者： Hend Baza Taras Turiv Bing-Xiang Li Ruipeng Li Benjamin M Yavitt Masafumi Fukuto Oleg D Lavrentovich Department of Physics Kent State University Kent OH 44242 USA. olavrent@kent.edu and Advanced Materials and Liquid Crystal Institute Kent State University Kent OH 44242 USA. Advanced Materials and Liquid Crystal Institute Kent State University Kent OH 44242 USA and Materials Science Graduate Program Kent State University Kent OH 44242 USA. National Synchrotron Light Source II Brookhaven National Laboratory Upton NY 11973 USA. National Synchrotron Light Source II Brookhaven National Laboratory Upton NY 11973 USA and Department of Materials Science and Chemical Engineering Stony Brook University Stony Brook NY 11794 USA. Department of Physics Kent State University Kent OH 44242 USA. olavrent@kent.edu and Advanced Materials and Liquid Crystal Institute Kent State University Kent OH 44242 USA and Materials Science Graduate Program Kent State University Kent OH 44242 USA.

Correction for 'Shear-induced polydomain structures of nematic lyotropic chromonic liquid crystal disodium cromoglycate' by Hend Baza et al., Soft Matter, 2020, 16, 8565-8576.

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Surface molecular doping of all-inorganic perovskite using zethrenes molecules

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Nano Research 2019年第1期12卷 77-84页

作者： Arramel Hu Pan Aozhen Xie Songyan Hou Xinmao Yin Chi Sin Tang Nguyen T.Hoa Muhammad D.Birowosuto Hong Wang Cuong Dang Andrivo Rusydi Andrew T.S.Wee Jishan Wu Department of Physics National University of Singapore2 Science Drive 3Singapore 117542Singapore Centre for Advanced 2D Materials National University of SingaporeBlock S14Level 66 Science Drive 2Singapore 117546Singapore Department of Chemistry National University of Singapore3 Science Drive 3Singapore 117543Singapore CINTRA UMICNRS/NTU/THALES 3288 Research Techno Plaza50 Nanyang DriveLevel 6Border X BlockSingapore 637553Singapore School of Electrical and Electronic Engineering Nanyang Technological University50 Nanyang AvenueSingapore 639798Singapore Energy Research Institute@NTU(ERI@N) Nanyang Technological UniversityResearch Techno PlazaX-Frontier BlockLevel 550 Nanyang DriveSingapore 637553Singapore Singapore Synchrotron Light Source National University of Singapore5 Research LinkSingapore 1176033Singapore NUS Graduate School for Integrative Sciences and Engineering(NGS) National University of SingaporeSingapore 117456Singapore NUSNNI-NanoCore National University of SingaporeSingapore 117411Singapore Institute of Materials Research&Engineering(IMRE) Agency far ScienceTechnology and Research(A^*STAR)2 Fusionopolis WayInnovisSingapore 138634Singapore

We present an optical and photoelectron spectroscopic study to elucidate the interfacial electronic properties of organic-inorganic semiconductor heterojunctions formed in a kinetically blocked heptazethrene triisopropylsilyl ethynylene (HZ-TIPS) and its homologue,octazethrene (OZ-TIPS) on an all-inorganic perovskite cesium lead bromide (CsPbBr3) *** photoluminescence behavior of the underlying perovskites upon differing molecular doping conditions was *** turns out that the charge transfer dynamics of thermally-evaporated OZ-TIPS molecule exhibited a faster average lifetime than that of the HZ-TIPS case suggesting the importance of the biradical state in the former *** interfacial dipole was formed at the interface due to the competing interaction between the dispersion force of the bulky TIPS-substituent group and the attractive van der Waals interaction at the first few *** spectroscopy of the physisorbed HZ-TIPS shows chemical shifts,which indicates electron transfer from HZ-TIPS molecules to the CsPbBr3 perovskite single *** contrast,the adsorbed OZ-TIPS molecular layer on CsPbBr3 demonstrates the opposite trend indicating a hole transfer *** average molecular orientation as determined by near edge X-ray absorption fine structure (NEXAFS) suggests that the HZ-TIPS molecular plane is generally lifted with respect to the perovskite *** suggest that the nature of the closed-shell electronic ground state of HZ-TIPS could contribute to the formation of interfacial dipole at the molecule/perovskite interface.

关键词： zethrene photoelectron spectroscopy perovskite near edge X-ray absorption fine structure and molecular doping

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Exciton Localization of High-Quality ZnO/Mg_xZn_1-xO Multiple Quantum Wells on Si (111) with a Y₂O₃ Buffer Layer (vol 1, pg 3829, 2018)

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ACS APPLIED NANO MATERIALS 2018年第10期1卷 5958-5958页

作者： Liu, Wei-Rein Huang, Wei-Lun Wu, Yung-Chi Lai, Liang-Hsun Hsu, Chia-Hung Hsieh, Wen-Feng Chiang, Tsung-Hung Wan, H. W. Hong, M. Kao, J. National Synchrotron Radiation Research Center Hsinchu 30076 Taiwan Program for Science and Technology of Accelerator Light Source National Chiao Tung University Hsinchu 30010 Taiwan Department of Photonics College of Electrical and Computer Engineering National Chiao Tung University Hsinchu 30010 Taiwan Department of Photonics College of Electrical and Computer Engineering National Chiao Tung University Hsinchu 30010 Taiwan Department of Materials Science & Engineering National Tsing Hua University Hsinchu 30013 Taiwan Graduate Institute of Applied Physics and Department of Physics National Taiwan University Taipei 10617 Taiwan Department of Physics National Tsing Hua University Hsinchu 30013 Taiwan

We report the structural and optical properties of ten-period ZnO/MgxZn1–xO multiple quantum wells (MQWs) prepared on the most widely used semiconductor material, Si. The introduction of a nanometer thick high-k Y2O3transition layer between Si (111) substrate and a ZnO buffer layer significantly improves the structural perfection of the MQWs grown on top of it. The high structural quality of the ZnO/MgxZn1–xO MQWs is evidenced by the appearance of pronounced high order satellite peaks in X-ray crystal truncation rods; high resolution cross-sectional transmission electron microscopy images also confirmed the regularly arranged well and barrier layers. When the well width is less than ∼2.7 nm, the quantum-confined Stark effect in MQWs can be negligible. Not only the increasing exciton-binding energy but also reducing exciton–phonon coupling determined in temperature-dependent photoluminescence spectra indicate quantum-size effect. Our results demonstrate that ZnO/MgxZn1–xO MQWs integrated on Si have great potential in UV optoelectronic device applications.

关键词： Excitons Phonons Oxides Binding energy Layers

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SARS-CoV-2 identified through crystallographic screening and computational docking

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science Advances 2021年第16期7卷

作者： Schuller, Marion Correy, Galen J. Gahbauer, Stefan Fearon, Daren Wu, Taiasean Díaz, Roberto Efraín Young, Iris D. Martins, Luan Carvalho Smith, Dominique H. Schulze-Gahmen, Ursula Owens, Tristan W. Deshpande, Ishan Merz, Gregory E. Thwin, Aye C. Biel, Justin T. Peters, Jessica K. Moritz, Michelle Herrera, Nadia Kratochvil, Huong T. Aimon, Anthony Bennett, James M. Neto, Jose Brandao Cohen, Aina E. Dias, Alexandre Douangamath, Alice Dunnett, Louise Fedorov, Oleg Ferla, Matteo P. Fuchs, Martin R. Gorrie-Stone, Tyler J. Holton, James M. Johnson, Michael G. Krojer, Tobias Meigs, George Powell, Ailsa J. Rack, Johannes Gregor Matthias Rangel, Victor L. Russi, Silvia Skyner, Rachael E. Smith, Clyde A. Soares, Alexei S. Wierman, Jennifer L. Zhu, Kang O Brien, Peter Jura, Natalia Ashworth, Alan Irwin, John J. Thompson, Michael C. Gestwicki, Jason E. Von Delft, Frank Shoichet, Brian K. Fraser, James S. Ahel, Ivan Sir William Dunn School of Pathology University of Oxford South Parks Road OxfordOX1 3RE United Kingdom Department of Bioengineering and Therapeutic Sciences University of California San Francisco San FranciscoCA94158 United States Department of Pharmaceutical Chemistry University of California San Francisco San FranciscoCA94158 United States Diamond Light Source Ltd. Harwell Science and Innovation Campus DidcotOX11 0DE United Kingdom Institute for Neurodegenerative Disease University of California San Francisco San FranciscoCA94158 United States Chemistry and Chemical Biology Graduate Program University of California San Francisco San FranciscoCA94158 United States Tetrad Graduate Program University of California San Francisco San FranciscoCA94158 United States Coronavirus Research Group Structural Biology Consortium University of California San Francisco San FranciscoCA94158 United States Biochemistry Department Institute for Biological Sciences Federal University of Minas Gerais Belo Horizonte Brazil Helen Diller Family Comprehensive Cancer University of California San Francisco San FranciscoCA94158 United States Centre for Medicines Discovery University of Oxford South Parks Road HeadingtonOX3 7DQ United Kingdom Stanford Synchrotron Radiation Lightsource Slac National Accelerator Center Menlo ParkCA94025 United States Wellcome Centre for Human Genetics University of Oxford Old Road Campus OxfordOX3 7BN United Kingdom National Synchrotron Light Source Ii Brookhaven National Laboratory UptonNY11973 United States Department of Biochemistry and Biophysics University of California San Francisco San FranciscoCA94158 United States Department of Molecular Biophysics and Integrated Bioimaging Lawrence Berkeley National Laboratory BerkeleyCA94720 United States ChemPartner Corporation South San FranciscoCA94080 United States Structural Genomics Consortium University of Oxford Old Road Campus HeadingtonOX3 7DQ United Kingdom School of

The severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) macrodomain within the nonstructural protein 3 counteracts host-mediated antiviral adenosine diphosphate ribosylation signaling. This enzyme is a promising antiviral target because catalytic mutations render viruses nonpathogenic. Here, we report a massive crystallographic screening and computational docking effort, identifying new chemical matter primarily targeting the active site of the macrodomain. Crystallographic screening of 2533 diverse fragments resulted in 214 unique macrodomain-binders. An additional 60 molecules were selected from docking more than 20 million fragments, of which 20 were crystallographically confirmed. X-ray data collection to ultra-high resolution and at physiological temperature enabled assessment of the conformational heterogeneity around the active site. Several fragment hits were confirmed by solution binding using three biophysical techniques (differential scanning fluorimetry, homogeneous time-resolved fluorescence, and isothermal titration calorimetry). The 234 fragment structures explore a wide range of chemotypes and provide starting points for development of potent SARS-CoV-2 macrodomain inhibitors. © 2021 American Association for the Advancement of science. All rights reserved.

关键词： Coronavirus

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Serial-femtosecond crystallography reveals how a phytochrome variant couples chromophore and protein structural changes

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science advances 2025年第22期11卷 eadp2665页

作者： Luisa Sauthof Michal Szczepek Andrea Schmidt Asmit Bhowmick Medhanjali Dasgupta Megan J Mackintosh Sheraz Gul Franklin D Fuller Ruchira Chatterjee Iris D Young Norbert Michael Nicolas Andreas Heyder Brian Bauer Anja Koch Isabel Bogacz In-Sik Kim Philipp S Simon Agata Butryn Pierre Aller Volha U Chukhutsina James M Baxter Christopher D M Hutchison Dorothee Liebschner Billy Poon Nicholas K Sauter Mitchell D Miller Roberto Alonso-Mori Mark S Hunter Alexander Batyuk Shigeki Owada Kensuke Tono Rie Tanaka Jasper J van Thor Norbert Krauß Tilman Lamparter Aaron S Brewster Igor Schapiro Allen M Orville Vittal K Yachandra Junko Yano Peter Hildebrandt Jan F Kern Patrick Scheerer Charité-Universitätsmedizin Berlin corporate member of Freie Universität Berlin and Humboldt-Universität zu Berlin Institute of Medical Physics and Biophysics Group Structural Biology of Cellular Signaling Charitéplatz 1 D-10117 Berlin Germany. Molecular Biophysics and Integrated Bioimaging Division Lawrence Berkeley National Laboratory 1 Cyclotron Road Berkeley CA 94720 USA. Fritz Haber Center for Molecular Dynamics Research Institute of Chemistry The Hebrew University of Jerusalem Jerusalem 9190401 Israel. Linac Coherent Light Source (LCLS) SLAC National Accelerator Laboratory 2575 Sand Hill Road MS103 Menlo Park CA 94025 USA. Technische Universität Berlin Institut für Chemie Sekr. PC 14 Straße des 17. Juni 135 Berlin D-10623 Germany. Diamond Light Source Ltd. Harwell Science and Innovation Campus Didcot Oxfordshire OX11 0DE UK. Research Complex at Harwell Harwell Science and Innovation Campus Didcot Oxfordshire OX11 0FA UK. Imperial College London Life Sciences Department South Kensington Campus London SW7 2AZ UK. Rice University Department of Biosciences 6100 Main Street Houston TX 77005 USA. Japan Synchrotron Radiation Research Institute Kouto 1-1-1 Sayo Hyogo 679-5198 Japan. RIKEN SPring-8 Center 1-1-1 Kouto Sayo Hyogo 679-5148 Japan. Department of Cell Biology Graduate School of Medicine Kyoto University Yoshidakonoecho Sakyo-ku Kyoto 606-8501 Japan. Karlsruhe Institute of Technology (KIT) Joseph Gottlieb Kölreuter Institute of Plant Science (JKIP) Fritz Haber Weg 4 D-76131 Karlsruhe Germany. Department of Physics Technical University Dortmund Dortmund Germany. Research Center Chemical Sciences and Sustainability University Alliance Ruhr 44801 Bochum Germany.

The photoreaction and commensurate structural changes of a chromophore within biological photoreceptors elicit conformational transitions of the protein promoting the switch between deactivated and activated states. We investigated how this coupling is achieved in a bacterial phytochrome variant, Agp2-PAiRFP2. Contrary to classical protein crystallography, which only allows probing (cryo-trapped) stable states, we have used time-resolved serial femtosecond x-ray crystallography (tr-SFX) and pump-probe techniques with various illumination and delay times with respect to photoexcitation of the parent Pfr state. Thus, structural data for seven time frames were sorted into groups of molecular events along the reaction coordinate. They range from chromophore isomerization to the formation of Meta-F, the intermediate that precedes the functional relevant secondary structure transition of the tongue. Structural data for the early events were used to calculate the photoisomerization pathway to complement the experimental data. Late events allow identifying the molecular switch that is linked to the intramolecular proton transfer as a prerequisite for the following structural transitions.

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