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However, commonly used chiral cations with nonconductive aliphatic and aromatic structures exhibit large energy gaps between the highest occupied molecular orbital (HOMO) and the lowest unoccupied molecular orbital (LUMO) relative to those of the inorganic frameworks. This energy mismatch between the chiral spacer and the inorganic sublattice creates a barrier that hinders charge-carrier transport, leading to inefficient out-of-plane charge mobility and strong quantum confinement effects. To address this challenge, we design and synthesize chiral n-type naphthalenediimide (NDI)-based cations, (R)-2-(7-ethyl-1,3,6,8-tetraoxo-3,6,7,8-tetrahydrobenzo[lmn][3,8]phenanthrolin-2(1H)-yl)propan-1-aminium ((R)-NDIEPA+). We successfully tune the LUMO level of (R)-NDIEPA+ to align with that of the inorganic sublattice, and the resulting chiral one-dimensional (1D) (R-NDIEPA)PbI3 MHS demonstrates a type II band alignment that facilitates charge separation, as evidenced by quenched photoluminescence and transient absorption dynamics indicative of ultrafast charge transfer across the organic\u2013inorganic interface. As a result, these materials demonstrate an approximately 7-fold enhancement in electron mobility compared to the chiral 1D MHS incorporating nonconductive aromatic cations. (R-NDIEPA)PbI3 also exhibits a strong circular dichroism (CD) signal, confirming effective chirality transfer from the organic cation to the inorganic framework. These findings underscore the importance of leveraging the electronic properties of chiral organic cations while preserving strong chiroptical activity, highlighting the potential of (R-NDIEPA)PbI3 for chiroptoelectronic applications such as circularly polarized light photodetectors and other spintronic devices.<\/jats:p>","DOI":"10.1021\/jacs.6c09248","type":"journal-article","created":{"date-parts":[[2026,8,12]],"date-time":"2026-08-12T16:03:42Z","timestamp":1786550622000},"page":"35861-35874","source":"Crossref","is-referenced-by-count":0,"title":["Molecular Design of\nChiral Naphthalenediimide-Based\nCations for Chiral One-Dimensional Metal Halide Semiconductors with\nStrong Chiroptical Activity and Amplified Charge Transport Ability"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-6010-1108","authenticated-orcid":true,"given":"Xiaoyu","family":"Zhang","sequence":"first","affiliation":[{"name":"Cornell University , , Ithaca , , ,","place":["New York, New York, United States, 14853"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7920-0683","authenticated-orcid":true,"given":"Shripathi","family":"Ramakrishnan","sequence":"additional","affiliation":[{"name":"Cornell University , , Ithaca , , ,","place":["New York, New York, United States, 14853"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7598-4516","authenticated-orcid":true,"given":"Xiaoran","family":"Hu","sequence":"additional","affiliation":[{"name":"Cornell University , , Ithaca , , ,","place":["New York, New York, United States, 14853"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0310-107X","authenticated-orcid":true,"given":"Yi","family":"Xie","sequence":"additional","affiliation":[{"name":"Duke University , , , ,","place":["Durham, North Carolina, United States, 27708"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4873-6629","authenticated-orcid":true,"given":"Yuanze","family":"Xu","sequence":"additional","affiliation":[{"name":"Cornell University , , Ithaca , , ,","place":["New York, New York, United States, 14853"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7354-6421","authenticated-orcid":true,"given":"Adewale","family":"Babatunde","sequence":"additional","affiliation":[{"name":"Cornell University , , Ithaca , , ,","place":["New York, New York, United States, 14853"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Anna Niamh","family":"Alphenaar","sequence":"additional","affiliation":[{"name":"Cornell University , , Ithaca , , ,","place":["New York, New York, United States, 14853"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyu","family":"Yin","sequence":"additional","affiliation":[{"name":"Cornell University , , Ithaca , , ,","place":["New York, New York, United States, 14853"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiaozhou","family":"Zheng","sequence":"additional","affiliation":[{"name":"Cornell University , , Ithaca , , ,","place":["New York, New York, United States, 14853"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Letian","family":"Li","sequence":"additional","affiliation":[{"name":"Cornell University , , Ithaca , , ,","place":["New York, New York, United States, 14853"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0002-1322-2676","authenticated-orcid":true,"given":"Pingchuan","family":"Liu","sequence":"additional","affiliation":[{"name":"Cornell University , , Ithaca , , ,","place":["New York, New York, United States, 14853"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9433-1198","authenticated-orcid":true,"given":"Hao","family":"Li","sequence":"additional","affiliation":[{"name":"Cornell University , , Ithaca , , ,","place":["New York, New York, United States, 14853"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7832-1475","authenticated-orcid":true,"given":"Yugang","family":"Zhang","sequence":"additional","affiliation":[{"name":"Brookhaven National Laboratory , , Upton , , ,","place":["New York, New York, United States, 11973"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5024-3540","authenticated-orcid":true,"given":"Mircea","family":"Cotlet","sequence":"additional","affiliation":[{"name":"Brookhaven National Laboratory , , Upton , , ,","place":["New York, New York, United States, 11973"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9863-6899","authenticated-orcid":true,"given":"Shaoyi","family":"Jiang","sequence":"additional","affiliation":[{"name":"Cornell University , , Ithaca , , ,","place":["New York, New York, United States, 14853"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5189-4612","authenticated-orcid":true,"given":"David B.","family":"Mitzi","sequence":"additional","affiliation":[{"name":"Duke University , , , ,","place":["Durham, North Carolina, United States, 27708"]},{"name":"Duke University , , , ,","place":["Durham, North Carolina, United States, 27708"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2401-4664","authenticated-orcid":true,"given":"Qiuming","family":"Yu","sequence":"additional","affiliation":[{"name":"Cornell University , , Ithaca , , ,","place":["New York, New York, United States, 14853"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,12]]},"reference":[{"issue":"47","key":"2026090104500873200_cit1","doi-asserted-by":"publisher","first-page":"2005760","DOI":"10.1002\/adma.202005760","article-title":"Chiral Perovskites for Next-Generation Photonics: From\nChirality Transfer to Chiroptical Activity","volume":"33","author":"Ma","year":"2021","journal-title":"Adv. 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Am. Chem. Soc."},{"issue":"4","key":"2026090104500873200_cit36","doi-asserted-by":"publisher","first-page":"263","DOI":"10.1002\/(SICI)1520-636X(2000)12:4&lt;263::AID-CHIR12&gt;3.0.CO","article-title":"Chirality of Aromatic Bis-Imides from Their Circular\nDichroism Spectra","volume":"12","author":"Gawron\u0301ski","year":"2000","journal-title":"Chirality"},{"issue":"1","key":"2026090104500873200_cit37","doi-asserted-by":"publisher","first-page":"12825","DOI":"10.1038\/s41598-019-49235-5","article-title":"Supramolecular Super-Helix\nFormation via Self-Assembly of Naphthalene Diimide Functionalised\nwith Bile Acid Derivatives","volume":"9","author":"Wagalgave","year":"2019","journal-title":"Sci. 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