Chemical crystallography by serial femtosecond X-ray diffraction.
Chemical crystallography by serial femtosecond X-ray diffraction.
复制标题
DOI：
10.1038/s41586-021-04218-3
复制
发表时间：
2022-01
期刊：
影响因子：
64.8
通讯作者：
Hohman JN
中科院分区：
文献类型：
--
作者：
Schriber EA;Paley DW;Bolotovsky R;Rosenberg DJ;Sierra RG;Aquila A;Mendez D;Poitevin F;Blaschke JP;Bhowmick A;Kelly RP;Hunter M;Hayes B;Popple DC;Yeung M;Pareja-Rivera C;Lisova S;Tono K;Sugahara M;Owada S;Kuykendall T;Yao K;Schuck PJ;Solis-Ibarra D;Sauter NK;Brewster AS;Hohman JN
无机-有机杂化材料由于其简单的合成路线和可定制的特性，在新报道的结构中占有很大的份额。这种扩散导致了表征瓶颈：许多杂化材料是专性微晶体，具有低对称性和严重的辐射灵敏度，干扰了单晶x射线衍射和电子微衍射的标准技术。在这里，我们展示了小分子序列飞秒x射线晶体学（smSFX），用于从微晶体中确定材料晶体结构。我们将微晶悬浮液置于x射线自由电子激光辐射下，得到了数千种随机取向的衍射图。我们通过将斑点发现结果聚合到高分辨率粉末衍射图中来确定单位细胞。通过图论方法对稀疏序列模式进行索引后，可以使用单晶衍射数据的标准工具对结果数据集进行求解和细化。我们描述了从头算的结构解，其中后两种是以前未知的结构，其中甲基甲苯（AgSePh），噻吩（AgSPh）和乙烯（AgTePh）。在硫代rene中，我们确定了银-银键合网络的几何变化，这与其发散的光电特性有关。我们证明smSFX可以作为在近环境温度和压力下确定光束敏感微晶材料结构的一般技术。小分子序列飞秒x射线晶体学（smSFX）通过索引稀疏序列XFEL衍射帧来表征微晶体，在室温和压力下制备少量样品，没有光束损伤。
Inorganic–organic hybrid materials represent a large share of newly reported structures, owing to their simple synthetic routes and customizable properties. This proliferation has led to a characterization bottleneck: many hybrid materials are obligate microcrystals with low symmetry and severe radiation sensitivity, interfering with the standard techniques of single-crystal X-ray diffraction and electron microdiffraction. Here we demonstrate small-molecule serial femtosecond X-ray crystallography (smSFX) for the determination of material crystal structures from microcrystals. We subjected microcrystalline suspensions to X-ray free-electron laser radiation and obtained thousands of randomly oriented diffraction patterns. We determined unit cells by aggregating spot-finding results into high-resolution powder diffractograms. After indexing the sparse serial patterns by a graph theory approach, the resulting datasets can be solved and refined using standard tools for single-crystal diffraction data. We describe the ab initio structure solutions of mithrene (AgSePh), thiorene (AgSPh) and tethrene (AgTePh), of which the latter two were previously unknown structures. In thiorene, we identify a geometric change in the silver–silver bonding network that is linked to its divergent optoelectronic properties. We demonstrate that smSFX can be applied as a general technique for structure determination of beam-sensitive microcrystalline materials at near-ambient temperature and pressure. Small-molecule serial femtosecond X-ray crystallography (smSFX) characterizes microcrystals by indexing sparse serial XFEL diffraction frames, with little sample preparation, without beam damage, and at room temperature and pressure.
登录
查看更多内容
影响因子：
3.9
作者：
Dejoie C;Smeets S;Baerlocher C;Tamura N;Pattison P;Abela R;McCusker LB
通讯作者：
McCusker LB
DOI：
10.1107/s2059798319012877
发表时间：
2019-11-01
影响因子：
2.2
作者：
Brewster, Aaron S.;Bhowmick, Asmit;Sauter, Nicholas K.
通讯作者：
Sauter, Nicholas K.
影响因子：
2.5
作者：
Chatterjee, Ruchira;Weninger, Clemens;Yano, Junko
通讯作者：
Yano, Junko
影响因子：
3.9
作者：
Christensen, Jeppe;Horton, Peter N.;Coles, Simon J.
通讯作者：
Coles, Simon J.
影响因子：
4.6
作者：
DANCE, IG;FISHER, KJ;SCUDDER, ML
通讯作者：
SCUDDER, ML