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Aggregation of the guest atoms\/molecules within the pore results in the formation of a cluster\/oligomer, and the size of the cluster\/oligomer is controlled by the pore. In this study, the host 2D\u2010MON consists of 1,3,5\u2010tris(pyridyl)benzene molecules and Cu atoms on Cu(111). The guest adsorbates are HCOOH molecules that form 1D zigzag chains by the intermolecular hydrogen bond on Cu(111). By scanning tunneling microscopy (STM) measurements and density functional theory (DFT) calculations, it is revealed that HCOOH tetramers (chains of four molecules) appear in the pores most frequently. The two\u2010coordinate Cu atom in the 2D\u2010MON attracts an HCOOH molecule, in which van der Waals interactions play an important role. A zigzag chain grows from this HCOOH molecule, and the end of the tetramer forms the attractive electrostatic interaction with the H atom of the 2D\u2010MON, stabilizing the tetramer in the pore. Thus, the oligomerization process of HCOOH molecules in the pore are controlled by the host\u2010guest interaction as well as the intermolecular hydrogen\u2010bonding.<\/jats:p>","DOI":"10.1002\/smll.202505213","type":"journal-article","created":{"date-parts":[[2025,9,27]],"date-time":"2025-09-27T12:30:53Z","timestamp":1758976253000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Microscopic Observation of the Oligomerization Process of HCOOH Molecules Confined by a 2D Metal\u2010Organic Network on Cu(111)"],"prefix":"10.1002","volume":"21","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-7063-0871","authenticated-orcid":false,"given":"Noriyuki","family":"Tsukahara","sequence":"first","affiliation":[{"name":"National Institute of Technology Gunma College  Toriba\u2010machi 580 Maebashi Gunma 371\u20108530 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