Competing Effects of Network Architecture and Composition on Polydomain Liquid Crystal Elastomers

Yang, David Taeyeun; Zheng, Callie W.; Chan, Chun Lam Clement; Maguire, Shawn M.; Ostermann, Emily C.; Davidson, Emily C.

doi:10.1021/acs.macromol.5c02541

Competing Effects of Network Architecture and Composition on Polydomain Liquid Crystal Elastomers

Journal Article · Thu Jan 22 00:00:00 EST 2026 · Macromolecules

DOI:https://doi.org/10.1021/acs.macromol.5c02541· OSTI ID:3014301

Yang, David Taeyeun ^[1]; ^[2]; ^[3]; ^[1]; ^[1]; ^[1]

Princeton University, NJ (United States)
Princeton University, NJ (United States); Massachusetts Institute of Technology, Cambridge, MA (United States)
Princeton University, NJ (United States); University of Groningen (Netherlands)

Main-chain liquid crystal elastomers (LCEs) are synthesized to investigate the interplay of the composition and network structure on LCE nematic-to-isotropic (N–I) transitions. We focus on networks synthesized from liquid crystalline oligomers reacted with tri- or tetrafunctional nonmesogenic cross-linker molecules. We find that coupling between mesogens and the polymer backbone increases with the degree of cross-linking. However, this enhanced coupling competes with mesogenic dilution arising from the cross-linker molecules to determine the N–I transition temperature (T_NI). When cross-linker molecules are dilute, the degree of cross-linking directly correlates to the change in T_NI from the oligomer to LCE (ΔT_NI) through mesogen–backbone coupling. In this regime, ΔT_NI ranges from 2.9 to 12.2 °C and 2.9–13.9 °C for tri- and tetrafunctional cross-linkers, respectively. At high cross-linker concentrations, deviations from this linear relationship appear. Further, the fractional mesogen content within an oligomer chain induces molecular weight-dependent mesogenic dilution effects arising from the flexible spacer molecules. Analysis of the N–I transition peak reveals a maximum latent heat per gram of mesogen (ΔH_NI,mes) for this system.

View Accepted Manuscript (DOE)

Research Organization:: Princeton Univ., NJ (United States); Princeton University, NJ (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: SC0023021

OSTI ID:: 3014301

Alternate ID(s):: OSTI ID: 3017928
OSTI ID: 3025323

Journal Information:: Macromolecules, Journal Name: Macromolecules Journal Issue: 3 Vol. 59; ISSN 1520-5835; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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