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1.
J Phys Chem Lett ; 13(44): 10275-10281, 2022 Nov 10.
Article in English | MEDLINE | ID: mdl-36305559

ABSTRACT

Viscoelastic liquid coacervate phases that are highly enriched in nonconjugated polyelectrolytes are currently the subject of highly active research from biological and soft-materials perspectives. However, formation of a liquid, electronically active coacervate has proved highly elusive, since extended π-electron interactions strongly favor the solid state. Herein we show that a conjugated polyelectrolyte can be rationally designed to undergo aqueous liquid/liquid phase separation to form a liquid coacervate phase. This result is significant both because it adds to the fundamental understanding of liquid/liquid phase separation but also because it opens intriguing applications in light harvesting and beyond. We find that the semiconducting coacervate is intrinsically excitonically coupled, allowing for long-range exciton diffusion in a strongly correlated, fluctuating environment. The emergent excitonic states are comprised of both excimers and H-aggregates.


Subject(s)
Water , Hydrogen-Ion Concentration , Polyelectrolytes , Diffusion
2.
Angew Chem Int Ed Engl ; 61(20): e202117759, 2022 05 09.
Article in English | MEDLINE | ID: mdl-35229429

ABSTRACT

The ability to assemble artificial systems that mimic aspects of natural light-harvesting functions is fascinating and attractive for materials design. Given the complexity of such a system, a simple design pathway is desirable. Here, we argue that associative phase separation of oppositely charged conjugated polyelectrolytes (CPEs) can provide such a path in an environmentally benign medium: water. We find that complexation between an exciton-donor and acceptor CPE leads to formation of a complex fluid. We interrogate exciton transfer from the donor to the acceptor CPE within the complex fluid and find that transfer is highly efficient. We also find that excess molecular ions can tune the modulus of the inter-CPE complex fluid. Even at high ion concentrations, CPEs remain complexed with significantly delocalized electronic wavefunctions. Our work lays the rational foundation for complex, tunable aqueous light-harvesting systems via the intrinsic thermodynamics of associative phase separation.


Subject(s)
Electronics , Water , Polyelectrolytes , Thermodynamics
3.
Arch Pediatr ; 27(1): 29-32, 2020 Jan.
Article in English | MEDLINE | ID: mdl-31767499

ABSTRACT

PURPOSE: The aim of this study was to evaluate retinal hemorrhages (RHs) in newborns after therapeutic hypothermia performed for hypoxic-ischemic encephalopathy (HIE). METHODS: From 2014 January to October 2016, full-term newborns who were referred to us from the neonatal intensive care unit at our hospital for ophthalmological examination were evaluated retrospectively. Neonates diagnosed with HIE were examined with a RetCam Digital Retinal Camera (Massie Research Laboratories Inc., Pleasanton, CA) using a 130-degree or binocular indirect ophthalmoscope (Heine, Herrsching, Germany) imaging tool and were classified into three groups. Group 1 included patients without HIE, group 2 included patients with stage I HIE, and group 3 included patients with stage II or III HIE. The RH rates in cases of HIE were retrospectively reviewed. RESULTS: A total of 148 eyes of 74 patients were included in the study. RH was detected in 36 eyes (24.3%); there were two eyes (3.7%), 14 eyes (20.6%), and 20 eyes (76.9%), in groups 1, 2, and 3, respectively. In group 3, RH was mostly seen in a widespread form. RHs involving the macula were resorbed later than haemorrhages in other locations. CONCLUSION: RHs are frequent in neonates with HIE. RHs were seen significantly more frequently in stage II-III HIE. These haemorrhages may require treatment, especially when the macula is involved.


Subject(s)
Hypothermia, Induced , Hypoxia-Ischemia, Brain/complications , Retinal Hemorrhage/epidemiology , Female , Humans , Infant, Newborn , Intensive Care Units, Neonatal , Male , Ophthalmoscopy , Retinal Vessels/pathology , Retrospective Studies , Tomography, Optical Coherence
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