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Instruments / Technical Area	Publication Details	Published
Detectors	Report of high data rate macromolecular crystallography (HDRMX) meeting, 23 July 2025 Christine Beavers , Herbert J. Bernstein , Aaron S. Brewster , Max Burian , Nicholas Devenish , Jiaxin Dawn Duan , Daniel Eriksson , Diego Gämperle , Yang Ha , David R. Hall , James M. Holton , Peter Keller , Louise Kroon-Batenburg , David W. Mittan-Moreau , Yasukazu Nakaye , Daniel W. Paley , Ezra Peisach , Nicholas K. Sauter , Sofia Trampari , Clemens Vonrhein , David G. Waterman , Thomas A. White , Graeme Winter Structural Dynamics 13 DOI: 10.1063/4.0001196 Open Access Show Abstract ▼ Abstract: This paper is a report of the High Data Rate Macromolecular Crystallography workshop held on 23 July 2025 as part of the 2025 meeting of the American Crystallographic Association in Lombard, IL, USA, 18–23 July 2025. This report summarizes the discussions, questions, action items, and recommendations that arose from the meeting and includes links to the presentations. The sessions were moderated by Aaron S. Brewster and Graeme Winter. There was particularly lively discussion about the possible need for lossy compression as data rates increase, as multimodal experiments become more popular and as research budgets are squeezed.	May 2026
I19-Small Molecule Single Crystal Diffraction	Substituent-directed assembly of 1D and 2D silver aryl tellurolates with tunable emission Komal Rani , Anietie W. Williams , Tarun Kaushik , Daniel W. Paley , Maggie C Willson , Masha Aleksich , Patience A. Kotei , Mark R. Warren , Adrian P. Mancuso , Kerry Gilmore , Aaron S. Brewster , J. Nathan Hohman Materials Advances DOI: 10.1039/D5MA01354B Diamond Proposal Number(s): [35300] Open Access Show Abstract ▼ Abstract: Metal-organic chalcogenolates (MOChas) are hybrid materials notable for excellent air and water stability and strong light-matter interactions. Tellurium-based MOChas have been limited to only a single example, tethrene (AgTePh). We modified a Grignard-based synthetic approach to prepare bis(4-methoxyphenyl) ditelluride and bis(3-methoxyphenyl) ditelluride, then prepared the corresponding MOChas. We used synchrotron serial crystallography at the Diamond Light Source, merging 90-degree sweeps from six selected microcrystals using "needle-in-a-haystack" approach to solve the crystal structure of AgTe-4M, revealing the tethrene-like 2-dimensional layered system. We also identified a bright red luminescent AgTe-3M derivative that is consistent with a 1-dimensional system. In parallel, we observed that elemental tellurium is a problematic contaminant that negatively impacts crystal morphology and yield when present during the synthesis. We demonstrate that inclusion of elemental tellurium is generally tolerated when <1% by weight.	Apr 2026
	Stabilizing structural transitional states between 1- and 2-dimensional topologies via hydrogen bond-mediated crystal engineering Mariya Aleksich , Adriana J. Ladera , Avery Lamonica , Kara Christensen , Daniel W. Paley , David W. Mittan-Moreau , Vanessa Oklejas , Matthias Zeller , Maggie C. Willson , Patience A. Kotei , Komal Rani , Elyse A. Schriber , Aria Mansouri Tehrani , Mohammad Vakili , Christopher J. Milne , Joana Valerio , Marco Kloos , Doriana Vinci , Adam Round , Dmitry Khakhulin , Fernando Ardana-Lamas , Frederico Lima , Yohei Uemura , Adrian P. Mancuso , Hazem Yousef , Shigeki Owada , Ichiro Inoue , Kensuke Tono , Nicholas K. Sauter , Aaron S. Brewster , Tess Smidt , James N. Hohman Journal Of The American Chemical Society DOI: 10.1021/jacs.5c09213 Show Abstract ▼ Abstract: Metal–organic chalcogenolates (MOChas) are hybrid materials composed of metal-chalcogenide networks coordinated by organic ligands, offering a versatile platform for structural and electronic tunability. The use of molecular ligand design to steer material formation represents a powerful strategy for accessing new solid-state topologies. In this work, we report two new silver benzenethiolate MOChas incorporating protic meta-functionalized ligands─hydroxy (−OH) and amine (−NH2)─which exhibit hydrogen-bond-driven supramolecular organization and novel inorganic connectivities. Rather than modifying existing materials, we contextualize these compounds as distinct outcomes within a structural continuum. Silver para- and meta-methoxy-benzenethiolates (p-OCH3 and m-OCH3) serve as control points for known 2D and 1D topologies, respectively. The new materials, m-OH and m-NH2, were structurally characterized using small molecule serial femtosecond crystallography (smSFX), and their intermediate energetic and electronic properties were confirmed through density functional theory (DFT) calculations. We introduce the concept of supramolecular distortion to describe how ligand-driven intermolecular interactions reshape inorganic topology─not as deviations from a fixed state, but as distinct, kinetically accessible ground-state architectures. This work establishes a design paradigm linking organic ligand identity to predictable shifts in inorganic dimensionality in MOChas.	Mar 2026
	Can ferric-oxyl excited states explain elongated iron-oxygen bonds in heme peroxidase catalytic intermediates? Lewis J. Williams , Jos J. A. G. Kamps , Adrian M. V. Brânzanic , Maria Lehene , Kristoffer J. M. Lundgren , Ulf Ryde , Kuntal Chatterjee , Margaret D. Doyle , Philipp S. Simon , Hiroki Makita , Amy J. Thompson , Aaron S. Brewster , Tiankun Zhou , Marina Lucic , Michael T. Wilson , Pierre Aller , Juan Sanchez-Weatherby , Leland Gee , Sebastian Dehe , Sandra Mous , Junko Yano , Vittal K. Yachandra , Michael A. Hough , Allen M. Orville , Jan F. Kern , Radu L. Silaghi-Dumitrescu , Jonathan A. R. Worrall Nature Communications 114 DOI: 10.1038/s41467-026-69192-8 Open Access Show Abstract ▼ Abstract: The use of X-ray structures to determine and interpret the ferryl iron-oxygen bond order in molecular oxygen-activating heme enzymes has, in the past, been controversial. This has mainly stemmed from the susceptibility of ferryl species to X-ray-induced electronic state changes. In this work we establishe using time-resolved serial femtosecond X-ray crystallography (tr-SFX) on a dye-decolourising peroxidase that the ferryl intermediate species (Compounds I and II) captured following in situ mixing of microcrystals with H2O2 have single, rather than the double bond character expected. X-ray emission validated tr-SFX data with quantum refinement, time-dependent-DFT calculations and QM/MM geometry optimizations together support the concept that the single iron-oxygen bond character is not an indication of ferryl reduction or a protonated form (FeIV-OH) but is instead attributed to the existence of accessible excited states possessing ferric-oxyl (FeIII–O•–) character. Such states offer insight into the nature of ferryl heme.	Feb 2026
I19-Small Molecule Single Crystal Diffraction	Supramolecular support of cuprophilic network bonding in 2-D copper n-alkanethiolates Maggie C. Willson , Daniel W. Paley , Elyse A. Schriber , Daniel J. Rosenberg , Daniel M. Tchon , Patience A. Kotei , Komal Rani , Cynthia Melendrez , Matthias Zeller , Tarun Kaushik , Qiaoling Fan , Chamathka Dehiwala Liyanage , Jungmin Kang , Ichiro Inoue , Kensuke Tono , Yuichi Inubushi , Aaron S. Brewster , J. Nathan Hohman Inorganic Chemistry DOI: 10.1021/acs.inorgchem.5c02024 Diamond Proposal Number(s): [35300] Show Abstract ▼ Abstract: The development of heterogeneous materials, catalysts, and semiconductors is often reliant on precise control of self-assembly and crystal packing. Many new materials are initially synthesized as microcrystalline powders, making them incompatible with typical methods of structure determination, such as single-crystal X-ray diffraction. This resultant lack of structural information has made thorough investigation into the effect of metal substitution on crystal structure in metal–organic chalcogenolates (MOChas) challenging. Here, we use small molecule serial femtosecond crystallography (smSFX) to present the structures of four copper n-alkanethiolates: CuSC4, CuSC5, CuSC6, and CuSC7. Divergent patterns of alkyl chain packing are identified from microcrystalline powders via smSFX. An odd–even effect in crystal packing has been identified and attributed to different orientations of symmetry elements in the even- and odd-numbered chains. This results in minute changes in the azimuthal organization of the even-numbered chains and the network of cuprophilic interactions. Additionally, we present a synthesis of crystalline gold n-alkanethiolates to provide the first comparison between three d10 coinage metals (Cu, Ag, and Au) and their resultant n-alkanethiolates.	Aug 2025
	Serial-femtosecond crystallography reveals how a phytochrome variant couples chromophore and protein structural changes 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 , George N. Phillips , 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 Science Advances 11 DOI: 10.1126/sciadv.adp2665 Open Access Show Abstract ▼ Abstract: 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.	May 2025
I19-Small Molecule Single Crystal Diffraction	Ligand-mediated quantum yield enhancement in 1-D silver organothiolate metal–organic chalcogenolates Mariya Aleksich , Yeongsu Cho , Daniel W. Paley , Maggie C. Willson , Hawi N. Nyiera , Patience A. Kotei , Vanessa Oklejas , David W. Mittan-Moreau , Elyse A. Schriber , Kara Christensen , Ichiro Inoue , Shigeki Owada , Kensuke Tono , Michihiro Sugahara , Satomi Inaba-Inoue , Mohammad Vakili , Christopher J. Milne , Fabio Dallantonia , Dmitry Khakhulin , Fernando Ardana-Lamas , Frederico Lima , Joana Valerio , Huijong Han , Tamires Gallo , Hazem Yousef , Oleksii Turkot , Ivette J. Bermudez Macias , Thomas Kluyver , Philipp Schmidt , Luca Gelisio , Adam R. Round , Yifeng Jiang , Doriana Vinci , Yohei Uemura , Marco Kloos , Adrian P. Mancuso , Mark Warren , Nicholas K. Sauter , Jing Zhao , Tess Smidt , Heather J. Kulik , Sahar Sharifzadeh , Aaron S. Brewster , J. Nathan Hohman Advanced Functional Materials 17 DOI: 10.1002/adfm.202414914 Diamond Proposal Number(s): [35300] Show Abstract ▼ Abstract: X-ray free electron laser (XFEL) microcrystallography and synchrotron single-crystal crystallography are used to evaluate the role of organic substituent position on the optoelectronic properties of metal–organic chalcogenolates (MOChas). MOChas are crystalline 1D and 2D semiconducting hybrid materials that have varying optoelectronic properties depending on composition, topology, and structure. While MOChas have attracted much interest, small crystal sizes impede routine crystal structure determination. A series of constitutional isomers where the aryl thiol is functionalized by either methoxy or methyl ester are solved by small molecule serial femtosecond X-ray crystallography (smSFX) and single crystal rotational crystallography. While all the methoxy examples have a low quantum yield (0-1%), the methyl ester in the ortho position yields a high quantum yield of 22%. The proximity of the oxygen atoms to the silver inorganic core correlates to a considerable enhancement of quantum yield. Four crystal structures are solved at a resolution range of 0.8–1.0 Å revealing a collapse of the 2D topology for functional groups in the 2- and 3- positions, resulting in needle-like crystals. Further analysis using density functional theory (DFT) and many-body perturbation theory (MBPT) enables the exploration of complex excitonic phenomena within easily prepared material systems.	Dec 2024
	In situ structural observation of a substrate- and peroxide-bound high-spin ferric-hydroperoxo intermediate in the P450 enzyme CYP12 Romie C. Nguyen , Ian Davis , Medhanjali Dasgupta , Yifan Wang , Philipp S. Simon , Agata Butryn , Hiroki Makita , Isabel Bogacz , Kednerlin Dornevil , Pierre Aller , Asmit Bhowmick , Ruchira Chatterjee , In-Sik Kim , Tiankun Zhou , Derek Mendez , Daniel W. Paley , Franklin Fuller , Roberto Alonso Mori , Alexander Batyuk , Nicholas K. Sauter , Aaron S. Brewster , Allen M. Orville , Vittal K. Yachandra , Junko Yano , Jan F. Kern , Aimin Liu Journal Of The American Chemical Society 10 DOI: 10.1021/jacs.3c04991 Show Abstract ▼ Abstract: The P450 enzyme CYP121 from Mycobacterium tuberculosis catalyzes a carbon–carbon (C–C) bond coupling cyclization of the dityrosine substrate containing a diketopiperazine ring, cyclo(l-tyrosine-l-tyrosine) (cYY). An unusual high-spin (S = 5/2) ferric intermediate maximizes its population in less than 5 ms in the rapid freeze-quenching study of CYP121 during the shunt reaction with peracetic acid or hydrogen peroxide in acetic acid solution. We show that this intermediate can also be observed in the crystalline state by EPR spectroscopy. By developing an on-demand-rapid-mixing method for time-resolved serial femtosecond crystallography with X-ray free-electron laser (tr-SFX-XFEL) technology covering the millisecond time domain and without freezing, we structurally monitored the reaction in situ at room temperature. After a 200 ms peracetic acid reaction with the cocrystallized enzyme–substrate microcrystal slurry, a ferric-hydroperoxo intermediate is observed, and its structure is determined at 1.85 Å resolution. The structure shows a hydroperoxyl ligand between the heme and the native substrate, cYY. The oxygen atoms of the hydroperoxo are 2.5 and 3.2 Å from the iron ion. The end-on binding ligand adopts a near-side-on geometry and is weakly associated with the iron ion, causing the unusual high-spin state. This compound 0 intermediate, spectroscopically and structurally observed during the catalytic shunt pathway, reveals a unique binding mode that deviates from the end-on compound 0 intermediates in other heme enzymes. The hydroperoxyl ligand is only 2.9 Å from the bound cYY, suggesting an active oxidant role of the intermediate for direct substrate oxidation in the nonhydroxylation C–C bond coupling chemistry.	Nov 2023
	Structure of a ribonucleotide reductase R2 protein radical Hugo Lebrette , Vivek Srinivas , Juliane John , Oskar Aurelius , Rohit Kumar , Daniel Lundin , Aaron S. Brewster , Asmit Bhowmick , Abhishek Sirohiwal , In-Sik Kim , Sheraz Gul , Cindy Pham , Kyle D. Sutherlin , Philipp Simon , Agata Butryn , Pierre Aller , Allen M. Orville , Franklin D. Fuller , Roberto Alonso-Mori , Alexander Batyuk , Nicholas K. Sauter , Vittal K. Yachandra , Junko Yano , Ville R. I. Kaila , Britt-Marie Sjöberg , Jan Kern , Katarina Roos , Martin Högbom Science 382, 109 - 113 DOI: 10.1126/science.adh8160 Show Abstract ▼ Abstract: Aerobic ribonucleotide reductases (RNRs) initiate synthesis of DNA building blocks by generating a free radical within the R2 subunit; the radical is subsequently shuttled to the catalytic R1 subunit through proton-coupled electron transfer (PCET). We present a high-resolution room temperature structure of the class Ie R2 protein radical captured by x-ray free electron laser serial femtosecond crystallography. The structure reveals conformational reorganization to shield the radical and connect it to the translocation path, with structural changes propagating to the surface where the protein interacts with the catalytic R1 subunit. Restructuring of the hydrogen bond network, including a notably short O–O interaction of 2.41 angstroms, likely tunes and gates the radical during PCET. These structural results help explain radical handling and mobilization in RNR and have general implications for radical transfer in proteins.	Oct 2023
	XFEL microcrystallography of self-assembling silver n-alkanethiolates Mariya Aleksich , Daniel W. Paley , Elyse A. Schriber , Will Linthicum , Vanessa Oklejas , David W. Mittan-Moreau , Ryan P. Kelly , Patience A. Kotei , Anita Ghodsi , Raymond G. Sierra , Andrew Aquila , Frédéric Poitevin , Johannes P. Blaschke , Mohammad Vakili , Christopher J. Milne , Fabio Dall’antonia , Dmitry Khakhulin , Fernando Ardana-Lamas , Frederico Lima , Joana Valerio , Huijong Han , Tamires Gallo , Hazem Yousef , Oleksii Turkot , Ivette J. Bermudez Macias , Thomas Kluyver , Philipp Schmidt , Luca Gelisio , Adam R. Round , Yifeng Jiang , Doriana Vinci , Yohei Uemura , Marco Kloos , Mark Hunter , Adrian P. Mancuso , Bryan D. Huey , Lucas R. Parent , Nicholas K. Sauter , Aaron S. Brewster , J. Nathan Hohman Journal Of The American Chemical Society DOI: 10.1021/jacs.3c02183 Show Abstract ▼ Abstract: New synthetic hybrid materials and their increasing complexity have placed growing demands on crystal growth for single-crystal X-ray diffraction analysis. Unfortunately, not all chemical systems are conducive to the isolation of single crystals for traditional characterization. Here, small-molecule serial femtosecond crystallography (smSFX) at atomic resolution (0.833 Å) is employed to characterize microcrystalline silver n-alkanethiolates with various alkyl chain lengths at X-ray free electron laser facilities, resolving long-standing controversies regarding the atomic connectivity and odd–even effects of layer stacking. smSFX provides high-quality crystal structures directly from the powder of the true unknowns, a capability that is particularly useful for systems having notoriously small or defective crystals. We present crystal structures of silver n-butanethiolate (C4), silver n-hexanethiolate (C6), and silver n-nonanethiolate (C9). We show that an odd–even effect originates from the orientation of the terminal methyl group and its role in packing efficiency. We also propose a secondary odd–even effect involving multiple mosaic blocks in the crystals containing even-numbered chains, identified by selected-area electron diffraction measurements. We conclude with a discussion of the merits of the synthetic preparation for the preparation of microdiffraction specimens and compare the long-range order in these crystals to that of self-assembled monolayers.	Jul 2023

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