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Recently, they also attract interest as promising candidates for spintronics. In materials lacking inversion symmetry, spin\u2010orbit coupling (SOC) leads to the Rashba\u2010Dresselhaus effect, offering a pathway for spin current control. Therefore, inversion symmetry breaking in MHPs, which are characterized by strong SOC, has crucial implications. Yet, in complex low\u2010dimensional hybrid organic\u2010inorganic perovskites (HOIPs), the presence of and structural contributions to inversion symmetry breaking remain elusive. Here, employing intense THz fields, lattice dynamics carrying spectroscopic fingerprints of inversion symmetry breaking are coherently driven and observed in Ruddlesden\u2010Popper (PEA)\n                    <jats:sub>2<\/jats:sub>\n                    (MA)\n                    <jats:italic>\n                      <jats:sub>n<\/jats:sub>\n                    <\/jats:italic>\n                    <jats:sub>\u20101<\/jats:sub>\n                    Pb\n                    <jats:italic>\n                      <jats:sub>n<\/jats:sub>\n                    <\/jats:italic>\n                    I\n                    <jats:sub>3<\/jats:sub>\n                    <jats:italic>\n                      <jats:sub>n<\/jats:sub>\n                    <\/jats:italic>\n                    <jats:sub>+1<\/jats:sub>\n                    perovskites, which are globally assigned to a centrosymmetric space group. We demonstrante coherent control by THz pulses over specific phonons, which are assigned to either purely inorganic or highly anharmonic hybridized cage\u2010ligand vibrations. By developing a general polarization analysis for THz\u2010driven phonons, linear and nonlinear driving mechanisms are pinpointed. From this, simultaneous IR\u2010 and Raman\u2010activity of inorganic cage modes below 1.5 THz is identified, indicating mode\u2010selective inversion symmetry breaking. By exploring the driving pathways of these coherent phonons, the groundwork is laid for simultaneous ultrafast control of optoelectronic and spintronic properties in 2D HOIPs.\n                  <\/jats:p>","DOI":"10.1002\/adma.202502204","type":"journal-article","created":{"date-parts":[[2025,10,3]],"date-time":"2025-10-03T11:15:31Z","timestamp":1759490131000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":9,"title":["THz\u2010Driven Coherent Phonon Fingerprints of Hidden Symmetry Breaking in 2D Layered Hybrid Perovskites"],"prefix":"10.1002","volume":"38","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-9092-9678","authenticated-orcid":false,"given":"Joanna M.","family":"Urban","sequence":"first","affiliation":[{"name":"Department of Physical Chemistry Fritz Haber Institute of the Max Planck Society  Faradayweg 4\u20106 14195 Berlin 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