Electrical
breakdown is a critical problem in electronics. In molecular
electronics, it becomes more problematic because ultrathin molecular
monolayers have delicate and defective structures and exhibit intrinsically
low breakdown voltages, which limit device performances. Here, we
show that interstitially mixed self-assembled monolayers (imSAMs)
remarkably enhance electrical stability of molecular-scale electronic
devices without deteriorating function and reliability. The SAM of
the sterically bulky matrix (SC11BIPY rectifier) molecule
is diluted with a skinny reinforcement (SC
n
) molecule via the new approach, so-called repeated surface exchange
of molecules (ReSEM). Combined experiments and simulations reveal
that the ReSEM yields imSAMs wherein interstices between the matrix
molecules are filled with the reinforcement molecules and leads to
significantly enhanced breakdown voltage inaccessible by traditional
pure or mixed SAMs. Thanks to this, bias-driven disappearance and
inversion of rectification is unprecedentedly observed. Our work may
help to overcome the shortcoming of SAM’s instability and expand
the functionalities.
Chlorosulfolipids
(CSLs) are major components of flagellar membranes
in sea algae. Unlike typical biological lipids, CSLs contain hydrophilic
sulfate and chloride groups in the hydrocarbon tail; this has deterred
the prediction of the CSL membrane structure since 1960. In this study,
we combine coarse-grained (CG) and atomistic molecular dynamics (MD)
simulations to gain significant insights into the membrane structure
of Danicalipin A, which is one of the typical CSLs. It is observed
from the CG MD that Danicalipin A lipids form a stable monolayer membrane
structure wherein the hydrocarbon moieties are sandwiched by hydrophilic
sulfate and chloride groups in both the head and tail regions. On
the basis of the mesoscopic structure, we built the corresponding
atomistic model to investigate the integrity of the CSL monolayer
membrane structure. The monolayer membrane comprising bent lipids
shows high thermal stability up to 313 K. The gel–liquid crystalline
phase transition is observed around 300 K.
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