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Inspired by the concept of average atomic volume (AAV), continuous regulation of thermal expansion from positive to zero to negative across a broad temperature range was achieved in the Rb\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    Mn\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    Lu\n                    <jats:sub>2\u2212<\/jats:sub>\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    Mo\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>12<\/jats:sub>\n                    system through the reverse design of the guest ion extraction process. Guest ion removal effectively enhances lattice flexibility, enabling Rb\n                    <jats:sub>0.4<\/jats:sub>\n                    Mn\n                    <jats:sub>0.4<\/jats:sub>\n                    Lu\n                    <jats:sub>1.6<\/jats:sub>\n                    Mo\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>12<\/jats:sub>\n                    to exhibit strong NTE performance (\n                    <jats:italic>\u03b1<\/jats:italic>\n                    <jats:sub>v<\/jats:sub>\n                    = \u221225.5 \u00d7 10\n                    <jats:sup>\u22126<\/jats:sup>\n                    K\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) over an ultra\u2010wide temperature range from 100 to 1300 K. A joint study of synchrotron x\u2010ray diffraction, Raman spectroscopy, and first\u2010principles calculations was conducted to investigate the structure, thermal expansion, and NTE mechanism. The coupling rotation between Mn\/LuO\n                    <jats:sub>6<\/jats:sub>\n                    octahedra and MoO\n                    <jats:sub>4<\/jats:sub>\n                    tetrahedra, excited by the transverse thermal vibrations of oxygen atoms, is responsible for the NTE in Rb\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    Mn\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    Lu\n                    <jats:sub>2\u2212<\/jats:sub>\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    Mo\n                    <jats:sub>3<\/jats:sub>\n                    O\n                    <jats:sub>12<\/jats:sub>\n                    . This work not only provides a wide temperature range NTE compounds, but also gives one way to design NTE with open\u2010framework structure materials.\n                  <\/jats:p>","DOI":"10.1002\/adma.75195","type":"journal-article","created":{"date-parts":[[2026,10,1]],"date-time":"2026-10-01T01:02:12Z","timestamp":1790816532000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Achieving Ultrawide Negative Thermal Expansion up to 1300 K via Structural Flexibility Engineering"],"prefix":"10.1002","author":[{"given":"Yaoyao","family":"Zhao","sequence":"first","affiliation":[{"name":"Key Laboratory of Materials Physics Ministry of Education School of Physics Zhengzhou University  Zhengzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yongqiang","family":"Qiao","sequence":"additional","affiliation":[{"name":"Key Laboratory of Materials Physics Ministry of Education School of Physics 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