We present a new algorithm for the analysis of whispering gallery modes (WGMs) found in the cavity enhanced Raman spectra retrieved from optically tweezed droplets. Our algorithm improves the computational scaling when analyzing core–shell droplets ( i.e. phase-separated or biphasic droplets) in the aerosol optical tweezers (AOT), making it computationally practical to analyze spectra collected at a few Hz over hours-long experiments. This enables the determination of the size and refractive index of both the core and shell phases with high accuracy, at 0.5 Hz time resolution. Phase-separated core–shell droplets are common morphologies in a wide variety of biophysical, colloidal, and aerosolized chemical systems, and have recently become a major focus in understanding the atmospheric chemistry of particulate matter. Our new approach reduces the number of parameters directly searched for, decreasing computational demands. We assess the accuracy of the diameters and refractive indices retrieved from a homogeneous or core–shell droplet. We demonstrate the performance of the new algorithm using experimental data from a droplet of aqueous glycerol coated by squalane. We demonstrate that a shell formation causes adjacent WGMs to split from each other in their wavenumber position through the addition of a secondary organic aerosol shell around a NaCl(aq) droplet. Our new algorithm paves the way for more in-depth physiochemical experiments into liquid–liquid phase separation and their consequences for interfacial chemistry—a topic with growing experimental needs for understanding the dynamics and chemistry of atmospheric aerosol particles, and in biochemical systems.
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Nanoparticle-laden droplets of liquid crystals: Interactive morphogenesis and dynamic assembly
Defects in liquid crystals serve as templates for nanoparticle (NP) organization; however, NP assembly in cholesteric (Ch) liquid crystals is only beginning to emerge. We show interactive morphogenesis of NP assemblies and a Ch liquid crystalline host formed by cellulose nanocrystals (CNCs), in which both the host and the guest experience marked changes in shape and structure as a function of concentration. At low NP loading, Ch-CNC droplets exhibit flat-ellipsoidal packing of Ch pseudolayers, while the NPs form a toroidal ring- or two cone–shaped assemblies at droplet poles. Increase in NP loading triggers reversible droplet transformation to gain a core-shell morphology with an isotropic core and a Ch shell, with NPs partitioning in the core and in disclinations. We show programmable assembly of droplets carrying magnetic NPs. This work offers a strategy for NP organization in Ch liquid crystals, thus broadening the spectrum of architectures of soft nanostructured materials.
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- Award ID(s):
- 1729509
- NSF-PAR ID:
- 10184866
- Date Published:
- Journal Name:
- Science Advances
- Volume:
- 5
- Issue:
- 7
- ISSN:
- 2375-2548
- Page Range / eLocation ID:
- eaav1035
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1126/sciadv.aav1035
