TY - JOUR
T1 - Micro- To macro-phase separation transition in sequence-defined coacervates
AU - Sing, Charles E.
N1 - Funding Information:
This material is based upon work supported by the National Science Foundation under NSF CAREER Award No. DMR-1654158.
PY - 2020/1/14
Y1 - 2020/1/14
N2 - Phase separation can be driven by the association of oppositely charged polyelectrolytes in solution, a process known as complex coacervation. This can manifest as macrophase separation, which arises when both polymer species are homopolyelectrolytes, or can lead to microphase separation when one or both of the charged species are block copolyelectrolytes. This is not a strict dichotomy; recently, macrophase separation was observed for a number of copolymers containing sequence-defined patterns of neutral vs charged monomers, including patterns with lengthy blocks. The specific pattern can affect the strength of this macrophase separation, yet at some block length, microphase separation is expected to emerge. In this article, we describe how to incorporate a theory of sequence-defined coacervation into self-consistent field theory, allowing the study of sequence-defined polyelectrolytes in inhomogeneous systems. We show that blocky sequences can affect electrostatically driven macrophase separation and can transition to microphase separation as the blockiness of sequences increases. This micro- to macrophase separation transition is a function of both the blockiness of the sequence, the number of blocks, and the concentration of salt.
AB - Phase separation can be driven by the association of oppositely charged polyelectrolytes in solution, a process known as complex coacervation. This can manifest as macrophase separation, which arises when both polymer species are homopolyelectrolytes, or can lead to microphase separation when one or both of the charged species are block copolyelectrolytes. This is not a strict dichotomy; recently, macrophase separation was observed for a number of copolymers containing sequence-defined patterns of neutral vs charged monomers, including patterns with lengthy blocks. The specific pattern can affect the strength of this macrophase separation, yet at some block length, microphase separation is expected to emerge. In this article, we describe how to incorporate a theory of sequence-defined coacervation into self-consistent field theory, allowing the study of sequence-defined polyelectrolytes in inhomogeneous systems. We show that blocky sequences can affect electrostatically driven macrophase separation and can transition to microphase separation as the blockiness of sequences increases. This micro- to macrophase separation transition is a function of both the blockiness of the sequence, the number of blocks, and the concentration of salt.
UR - http://www.scopus.com/inward/record.url?scp=85077941442&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85077941442&partnerID=8YFLogxK
U2 - 10.1063/1.5140756
DO - 10.1063/1.5140756
M3 - Article
C2 - 31941285
AN - SCOPUS:85077941442
VL - 152
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
SN - 0021-9606
IS - 2
M1 - 024902
ER -