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Effect of Molecular Weight and Layer Thickness on the Dielectric Breakdown Strength of Neat and Homopolymer Swollen Lamellar Block Copolymer Films



Saumil Samant, Monali Basutkar, Maninderjeet Singh, Ali Masud, Christopher A. Grabowski, Kim Kisslinger, Joseph Strzalka, Guangcui Yuan, Sushil K. Satija, Ikeoluwa Apata, Dharmaraj Raghavan, Michael Durstock, Alamgir Karim


Designing next generation light-weight pulsed power sources hinges on understanding the factors influencing the performance of high energy density storage materials. In prior work, we demonstrated the use of Cold Zone Annealing with Soft Shear (CZA-SS) as a processing strategy to fabricate highly stratified lamellar block copolymer (L-BCP) films which resulted in approximately equal} 50 % enhancement in breakdown voltage (EBD) or approximately equal} 225 % increase in stored energy density (U), compared to unordered as-cast, or oven annealed ordered, though not-fully stratified parallel to substrate L-BCP films11. Notably, low molecular weight (Mn) L-BCPs have low domain spacing, (d approximately equal} Mn0.66, d = half L-BCP domain size) with a larger amount of chain ends compared to high Mn L-BCP films. This work reports interesting differences between increasing L-BCP layer thickness, d, that increases EBD, versus increasing chain end density (ρc) within film layers that decreases EBD, by acting as defect sites for promoting breakdown in polymer films. We delineate these effects by increasing d while decreasing ρc with increasing molecular weight (Mn) of L-BCP, versus adding homopolymer block components to a low molecular weight L-BCP that increases both d and ρc simultaneously. Neutron Reflectivity and X-ray scattering (GISAXS) measurements confirm stratified lamellar structure. Notably, EBD was found to increase linearly with Mn of neat L-BCP. We hypothesize that the increase of EBD with Mn is coupled to enhanced interfacial segregation of chain ends due to increase in χN. The high molecular weight films of amorphous L-BCP of PS-b-PMMA with layered morphology exhibited U of 4.8 J/cm3, comparable to the industry standard of semi-crystalline biaxially oriented polypropylene (BOPP) films of approximately equal} 5 J/cm3. In contrast, swelling L-BCP domains with homopolymers also increases EBD with an increase of d, however, these values are approximately equal} 30 % lower than neat L-BCP films with same d due to an increased chain end density within domain from the added homopolymers. These findings can be vital in the selection of L-BCP for designing next generation high energy density solid-state polymer capacitors.
ACS Applied Polymer Materials


electrostatic capacitors, barrier effect, breakdown strength, block copolymers, directed self-assembly, cold zone annealing-soft shear


Samant, S. , Basutkar, M. , Singh, M. , Masud, A. , Grabowski, C. , Kisslinger, K. , Strzalka, J. , Yuan, G. , Satija, S. , Apata, I. , Raghavan, D. , Durstock, M. and Karim, A. (2020), Effect of Molecular Weight and Layer Thickness on the Dielectric Breakdown Strength of Neat and Homopolymer Swollen Lamellar Block Copolymer Films, ACS Applied Polymer Materials, [online], (Accessed June 21, 2024)


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Created July 31, 2020, Updated July 27, 2022