Helical Complex Ladder Polymer with Amplification of Asymmetry

Yuzhe Wang; Yuchen Xie; Yifu Chen; Changhwan Oh; Qiyi Fang; Kaushik Chivukula; Honghu Zhang; Cheng Zhao; Sarah Zhang; Nandini Ananth; Heather J. Kulik; Yu Zhong

doi:10.1021/jacs.5c17973

Helical Complex Ladder Polymer with Amplification of Asymmetry

Yuzhe Wang (Co-first Author)
, Yuchen Xie (Co-first Author)
, Yifu Chen (Co-first Author)
, Changhwan Oh
, Qiyi Fang
, Kaushik Chivukula
, Honghu Zhang
, Cheng Zhao
, Sarah Zhang
, Nandini Ananth
, Heather J. Kulik
, Yu Zhong^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

Abstract

We report a Cu–salen helical complex ladder polymer (HLP-Cu) built from covalently fused Cu(Salen) units. Point chirality from enantiopure diamines directs the formation of a rigid, π-conjugated helix. Compared with a planar analogue (LLP-Cu) and the Cu(Salen) monomer, HLP-Cu exhibits up to 5-fold stronger circular dichroism and a maximum dissymmetry factor of 7.4 × 10^–3. Titration experiments suggest a cooperative amplification of asymmetry arising from extended conjugation and helical geometry during helix formation. Time-dependent density functional theory calculations are employed to support this hypothesis, showing that increasing conjugation length and helical order enhance the rotational strength of contributing excited states via elevated magnetic transition moments and improved alignment of electric and magnetic transition moments. Our findings provide a new polymer platform for designing functional chiral materials with tunable chiroptical and spin-dependent properties. © 2026 American Chemical Society.

Original language	English
Pages (from-to)	2864-2869
Number of pages	6
Journal	Journal of the American Chemical Society
Volume	148
Issue number	3
Online published	13 Jan 2026
DOIs	https://doi.org/10.1021/jacs.5c17973
Publication status	Published - 28 Jan 2026
Externally published	Yes

Funding

This work was supported by a grant from the Air Force Office of Scientific Research (FA9550-24-1-0125). The authors acknowledge the use of facilities and instrumentation supported by NSF through the Cornell University Materials Research Science and Engineering Center DMR-1719875. The authors also acknowledge support in the form of a seed grant from the Abdul Latif Jameel Water & Food Systems (JWAFS) Lab at MIT (H.J.K. and C.O.). This work made use of the Cornell University NMR Facility, which is supported, in part, by the NSF through MRI award CHE-1531632. This research used resources at the 11-BM Complex Materials Scattering (CMS) beamline of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. The authors acknowledge the MIT SuperCloud and Lincoln Laboratory Supercomputing Center for providing HPC resources that have contributed to the research results reported within this paper.

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title = "Helical Complex Ladder Polymer with Amplification of Asymmetry",

abstract = "We report a Cu–salen helical complex ladder polymer (HLP-Cu) built from covalently fused Cu(Salen) units. Point chirality from enantiopure diamines directs the formation of a rigid, π-conjugated helix. Compared with a planar analogue (LLP-Cu) and the Cu(Salen) monomer, HLP-Cu exhibits up to 5-fold stronger circular dichroism and a maximum dissymmetry factor of 7.4 × 10–3. Titration experiments suggest a cooperative amplification of asymmetry arising from extended conjugation and helical geometry during helix formation. Time-dependent density functional theory calculations are employed to support this hypothesis, showing that increasing conjugation length and helical order enhance the rotational strength of contributing excited states via elevated magnetic transition moments and improved alignment of electric and magnetic transition moments. Our findings provide a new polymer platform for designing functional chiral materials with tunable chiroptical and spin-dependent properties. {\textcopyright} 2026 American Chemical Society.",

author = "Yuzhe Wang and Yuchen Xie and Yifu Chen and Changhwan Oh and Qiyi Fang and Kaushik Chivukula and Honghu Zhang and Cheng Zhao and Sarah Zhang and Nandini Ananth and Kulik, \{Heather J.\} and Yu Zhong",

year = "2026",

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doi = "10.1021/jacs.5c17973",

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TY - JOUR

T1 - Helical Complex Ladder Polymer with Amplification of Asymmetry

AU - Wang, Yuzhe

AU - Xie, Yuchen

AU - Chen, Yifu

AU - Oh, Changhwan

AU - Fang, Qiyi

AU - Chivukula, Kaushik

AU - Zhang, Honghu

AU - Zhao, Cheng

AU - Zhang, Sarah

AU - Ananth, Nandini

AU - Kulik, Heather J.

AU - Zhong, Yu

PY - 2026/1/28

Y1 - 2026/1/28

N2 - We report a Cu–salen helical complex ladder polymer (HLP-Cu) built from covalently fused Cu(Salen) units. Point chirality from enantiopure diamines directs the formation of a rigid, π-conjugated helix. Compared with a planar analogue (LLP-Cu) and the Cu(Salen) monomer, HLP-Cu exhibits up to 5-fold stronger circular dichroism and a maximum dissymmetry factor of 7.4 × 10–3. Titration experiments suggest a cooperative amplification of asymmetry arising from extended conjugation and helical geometry during helix formation. Time-dependent density functional theory calculations are employed to support this hypothesis, showing that increasing conjugation length and helical order enhance the rotational strength of contributing excited states via elevated magnetic transition moments and improved alignment of electric and magnetic transition moments. Our findings provide a new polymer platform for designing functional chiral materials with tunable chiroptical and spin-dependent properties. © 2026 American Chemical Society.

AB - We report a Cu–salen helical complex ladder polymer (HLP-Cu) built from covalently fused Cu(Salen) units. Point chirality from enantiopure diamines directs the formation of a rigid, π-conjugated helix. Compared with a planar analogue (LLP-Cu) and the Cu(Salen) monomer, HLP-Cu exhibits up to 5-fold stronger circular dichroism and a maximum dissymmetry factor of 7.4 × 10–3. Titration experiments suggest a cooperative amplification of asymmetry arising from extended conjugation and helical geometry during helix formation. Time-dependent density functional theory calculations are employed to support this hypothesis, showing that increasing conjugation length and helical order enhance the rotational strength of contributing excited states via elevated magnetic transition moments and improved alignment of electric and magnetic transition moments. Our findings provide a new polymer platform for designing functional chiral materials with tunable chiroptical and spin-dependent properties. © 2026 American Chemical Society.

UR - https://www.scopus.com/pages/publications/105028937437

UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-105028937437&origin=recordpage

U2 - 10.1021/jacs.5c17973

DO - 10.1021/jacs.5c17973

M3 - RGC 21 - Publication in refereed journal

C2 - 41530099

SN - 0002-7863

VL - 148

SP - 2864

EP - 2869

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 3

ER -

Helical Complex Ladder Polymer with Amplification of Asymmetry

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