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Alterations to the lattice often provide distinctive opportunities to finely tune specific properties, particularly in strongly correlated systems. A paradigmatic case is the iron\u2010based high\u2010temperature superconductors, where the microstructure plays an important role in modulating superconductivity. In this work, aberration\u2010corrected scanning transmission electron microscopy (STEM) is employed to investigate the microstructure and intrinsic chemical heterogeneity of Fe\n                    <jats:sub>1+y<\/jats:sub>\n                    Te, Fe\n                    <jats:sub>1+y<\/jats:sub>\n                    Te\n                    <jats:sub>0.8<\/jats:sub>\n                    Se\n                    <jats:sub>0.2<\/jats:sub>\n                    , and Fe\n                    <jats:sub>1+y<\/jats:sub>\n                    Te\n                    <jats:sub>0.5<\/jats:sub>\n                    Se\n                    <jats:sub>0.5<\/jats:sub>\n                    . A previously unforeseen superstructure phase, characterized by a wave vector\n                    <jats:bold>\n                      <jats:italic>q<\/jats:italic>\n                    <\/jats:bold>\n                    = (0.4, 0, 0.5), arising from the ordered arrangement of interstitial iron atoms, is clearly visible in the parent compound Fe\n                    <jats:sub>1+y<\/jats:sub>\n                    Te. Under these specific structural conditions, interstitial iron atoms interact with adjacent Fe atoms, forming iron polycomplexes that induce pronounced distortions in the FeTe\n                    <jats:sub>4<\/jats:sub>\n                    tetrahedra and may potentially foster the emergence of ferromagnetic clusters. The experimental findings further illustrate that appropriate Se substitution effectively suppresses interstitial iron concentration and ordering, with Fe\n                    <jats:sub>1+y<\/jats:sub>\n                    Te\n                    <jats:sub>0.5<\/jats:sub>\n                    Se\n                    <jats:sub>0.5<\/jats:sub>\n                    notably exhibiting the lowest concentration. The observations also suggest that Se substitution occurs randomly and Te\/Se\u2010induced nanoscale phase separation, driven by chemical heterogeneity is commonly observed within Fe\n                    <jats:sub>1+y<\/jats:sub>\n                    Te\n                    <jats:sub>1\u2212x<\/jats:sub>\n                    Se\n                    <jats:sub>x<\/jats:sub>\n                    crystals.\n                  <\/jats:p>","DOI":"10.1002\/smll.202410691","type":"journal-article","created":{"date-parts":[[2025,3,12]],"date-time":"2025-03-12T00:47:33Z","timestamp":1741740453000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Ordering of Interstitial Iron Atoms and Local Structural Distortion Induced by Iron Polycomplex in Fe\n                    <sub>1+y<\/sub>\n                    Te\n                    <sub>1\u2212x<\/sub>\n                    Se\n                    <sub>x<\/sub>\n                    as Seen via Transmission Electron Microscopy"],"prefix":"10.1002","volume":"21","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-4864-3027","authenticated-orcid":false,"given":"Xiao\u2010Ping","family":"Ma","sequence":"first","affiliation":[{"name":"Beijing National Laboratory for Condensed Matter Physics and Institute of Physics Chinese Academy of Sciences  Beijing 100190 P. R. China"},{"name":"Department of Physics Renmin University of China  Beijing 100872 P. R. China"},{"name":"Beijing Key Laboratory of Opto\u2010electronic Functional Materials &amp; Micro\u2010nano Devices Renmin University of China  Beijing 100872 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lu","family":"Zhang","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Condensed Matter Physics and Institute of Physics Chinese Academy of Sciences  Beijing 100190 P. R. China"},{"name":"School of Physical Sciences University of Chinese Academy of Sciences  Beijing 100190 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wen\u2010Tao","family":"Wang","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Condensed Matter Physics and Institute of Physics Chinese Academy of Sciences  Beijing 100190 P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shi\u2010Long","family":"Wu","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Condensed Matter Physics and Institute of Physics Chinese Academy of Sciences  Beijing 100190 P. R. China"},{"name":"School of Physical Sciences University of Chinese Academy of Sciences  Beijing 100190 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuai\u2010Shuai","family":"Sun","sequence":"additional","affiliation":[{"name":"Beijing National Laboratory for Condensed Matter Physics and Institute of Physics Chinese Academy of Sciences  Beijing 100190 P. R. China"},{"name":"School of Physical Sciences University of Chinese Academy of Sciences  Beijing 100190 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tian\u2010Long","family":"Xia","sequence":"additional","affiliation":[{"name":"Department of Physics Renmin University of China  Beijing 100872 P. 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