Enhanced Ion Transport and Molecular Packing Stability in Asymmetric 2D Nanostructured π‐Conjugated Thieno[3,2‐b]Thiophene‐Based Liquid Crystal

Wang, Chaoqiuyu; Sun, Yangyang; Wang, Zhongyang; Chen, Wen; Liu, Danya; Strzalka, Joseph; Patel, Shrayesh N.; Nealey, Paul F.; Ober, Christopher K.; Escobedo, Fernando A.

doi:10.1002/adfm.202423541

Enhanced Ion Transport and Molecular Packing Stability in Asymmetric 2D Nanostructured π‐Conjugated Thieno[3,2‐b]Thiophene‐Based Liquid Crystal

Journal Article · Tue Mar 04 00:00:00 EST 2025 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.202423541· OSTI ID:3006431

^[1]; ^[1]; ^[2]; Chen, Wen ^[3]; Liu, Danya ^[1]; ^[4]; Patel, Shrayesh N. ^[3]; Nealey, Paul F. ^[3]; Ober, Christopher K. ^[1]; ^[1]

Cornell Univ., Ithaca, NY (United States)
Univ. of Chicago, IL (United States); Univ. of Alabama, Tuscaloosa, AL (United States)
Univ. of Chicago, IL (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)

Organic semiconductors based on liquid crystal (LC) molecules have attracted increasing interest. Here, in this work, two linear LCs based on 2,5‐bis(thien‐2‐yl)thieno[3,2‐b]thiophene (BTTT) mesogen are designed and synthesized, including BTTT/dEO3 with two symmetrically attached tri(ethylene oxide) groups and BTTT/mEO6 with one asymmetrically attached hexa(ethylene oxide) group. These two molecules have comparable functional‐group compositions but different molecular geometries, leading to their moderately different material performances. Both LCs show smectic mesophases with relatively low transition temperatures as confirmed by differential scanning calorimetry and polarized optical microscopy. A combination of experimental grazing incidence wide‐angle X‐ray scattering and molecular dynamics (MD) simulations reveals a herringbone packing motif of BTTT segments in both LCs while a smaller molecular tilt angle in BTTT/mEO6. Ionic conductivities are measured by doping LCs with different amounts of ionic dopants, lithium bis(trifluoromethanesulfonyl)imide (LiTFSI). BTTT/mEO6 shows better smectic phase stability to higher LiTFSI doping ratios. Both LCs exhibit similar ionic conductivities in the smectic phases, but BTTT/mEO6 outperforms BTTT/dEO3 by a factor of three in the amorphous phase at higher temperatures. MD simulations, performed to examine the ion solvation environment, reveal that BTTT/mEO6 is more efficient in coordinating Li‐ions and screening their interactions with TFSI‐ions which further promote ionic transport.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 3006431

Alternate ID(s):: OSTI ID: 2530235

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 24 Vol. 35; ISSN 1616-301X; ISSN 1616-3028

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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grazing incidence wide-angle X-ray scattering
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