Synchrotron X‐Ray Analysis and Morphology Evidence for Stereo‐Assemblies of Periodic Aggregates in Poly(3‐hydroxybutyrate) with Unusual Photonic Iridescence

Liao, Yu-Hsuan; Nagarajan, Selvaraj; Chuang, Wei‐Tsung; Tsai, Yi-Wei

doi:10.1002/marc.202100281

Cited by 16 publications

(29 citation statements)

References 59 publications

(77 reference statements)

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“…Semicrystalline polymers can crystallize into a variety of aggregated patterns with specific orders and morphologies, and it has been shown that polymeric spherulitic textures, assembled by crystal self-assembly, could be precisely tailor-made for potential applications, such as photonic nano- or microstructures. − As examples, Zheng et al demonstrated that mesogenic helical architectures could be manipulated to provide a promising avenue toward chiro-optic materials and Yang et al comprehensively reviewed literature work on 3D chiral photonic nanostructures and techniques that may have potential as advanced photonic systems with custom-tailor functionalities. Geng et al prepared poly( l -lactic acid) (PLLA) forms with selective crystals of shish-kebab architectures on skins and in core layers of spherulites, and this specific morphological arrangement could enhance the mechanical impact toughness and excellent storage modulus.…”

Section: Introductionmentioning

confidence: 99%

Unique Optical Periodicity Assembly of Discrete Dendritic Lamellae and Pyramidal Single Crystals in Poly(ε-caprolactone)

Nagarajan

2021

ACS Appl. Mater. Interfaces

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A unique zig-zag banded morphology poly(ε-caprolactone) (PCL), crystallized at high T c = 46−47 °C and confined in thin films (<1 μm), is found to be assembled of parallel cogrowth of two totally crystal entities: edge-on dendritic lamellar protrusion from surfaces and flat-on pyramidal single crystals. The alternating PCL optical bands are assembled as flat-on single crystals aligned as straight dendrites as a valley band in series with edge-on branches as a ridge band, leading to a unique assembly mechanism of periodic optical rings where these two crystal pieces are assembled in series. Detailed assembly mechanisms are proposed to explain how the composite bands in the PCL aggregates are correlated to optical birefringence periodicity. By techniques of melt crystallization via periodic species drainage, PCL single crystals could be prepared and tailor-made to a variety of nanopatterns as templates for applications.

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Section: Introductionmentioning

confidence: 99%

Unique Optical Periodicity Assembly of Discrete Dendritic Lamellae and Pyramidal Single Crystals in Poly(ε-caprolactone)

Nagarajan

2021

ACS Appl. Mater. Interfaces

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“…From several recent literature results on other polymers, such as poly(butylene adipate) (PBA), poly(ε-caprolactone) (PCL), and poly([3-hydroxybutyrate] (PHB), poly(nonamethylene terephthalate) (PNT), high-density polyethylene (PE), etc. [ 42 , 43 , 44 , 45 , 46 , 47 , 48 , 49 ], the periodic morphology is certainly not limited to top surfaces. Still, it also distributes in 3D bulks throughout the entire sample volume.…”

Section: Resultsmentioning

confidence: 99%

Unique Periodic Rings Composed of Fractal-Growth Dendritic Branching in Poly(p-dioxanone)

Huang

Nagarajan

2022

Polymers

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Amorphous poly(p-vinyl phenol) (PVPh) was added into semicrystalline poly(p-dioxanone) (PPDO) to induce a uniquely novel dendritic/ringed morphology. Polarized-light optical, atomic-force and scanning electron microscopy (POM, AFM, and SEM) techniques were used to observe the crystal arrangement of a uniquely peculiar cactus-like dendritic PPDO spherulite, with periodic ring bands not continuingly circular such as those conventional types reported in the literature, but discrete and detached to self-assemble on each of the branches of the lobs. Correlations and responsible mechanisms for the formation of this peculiar banded-dendritic structure were analyzed. The periodic bands on the top surface and interior of each of the cactus-like lobs were discussed. The banded pattern was composed of feather-like lamellae in random fractals alternately varying their orientations from the radial direction to the tangential one. The tail ends of lamellae at the growth front spawned nucleation cites for new branches; in cycles, the feather-like lamellae self-divided into multiple branches following the Fibonacci sequence to fill the ever-expanding space with the increase of the radius. The branching fractals in the sequence and the periodic ring-banded assembly on each of the segregated lobs of cactus-like dendrites were the key characteristics leading to the formation of this unique dendritic/ringed PPDO spherulite.

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“…A few notable examples can be cited here: poly(1,4-butylene adipate) (PBA), poly(ε-caprolactone) (PCL), and poly([β-hydroxybutyrate] (PHB), poly(nonamethylene terephthalate) (PNT), high-density polyethylene (PE), etc. [ 36 , 37 , 38 , 39 , 40 , 41 , 42 ]. This is a continuous extension of one of our previous works on PPDO [ 35 ].…”

Section: Introductionmentioning

confidence: 99%

Crystal-by-Crystal Assembly in Two Types of Periodically Banded Aggregates of Poly(p-Dioxanone)

Huang

Huang²,

Lee³

et al. 2023

Polymers

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The exterior and interior lamellar assemblies of poly(p-dioxanone) (PPDO) crystallized at 76 °C yield the most regular ones to interpret the 3D assembly mechanisms and potential for structural coloration iridescence, which are investigated using atomic-force microscopy (AFM), and scanning electron microscopy (SEM). PPDO displays two types of ring-banded spherulites within a range of Tc with dual-type birefringent spherulites (positive and negative-type) only within a narrow range of Tcs = 70–78 °C. At Tc > 80 °C, the inter-band spacing decreases from a maximum and the crystal assembly becomes irregularly corrupted and loses the capacity for light interference. Periodic grating assemblies are probed by in-depth 3D dissection into periodically banded crystal aggregates of poly(p-dioxanone) (PPDO) to disclose such layered gratings possessing iridescence features similar to nature’s structural coloration. This work amply demonstrates that grating assembly by orderly stacked crystal layers is feasible not only for accounting for the periodic birefringent ring bands with polarized light but also the distinct iridescence by interfering with white light.

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Synchrotron X‐Ray Analysis and Morphology Evidence for Stereo‐Assemblies of Periodic Aggregates in Poly(3‐hydroxybutyrate) with Unusual Photonic Iridescence

Cited by 16 publications

References 59 publications

Unique Optical Periodicity Assembly of Discrete Dendritic Lamellae and Pyramidal Single Crystals in Poly(ε-caprolactone)

Unique Optical Periodicity Assembly of Discrete Dendritic Lamellae and Pyramidal Single Crystals in Poly(ε-caprolactone)

Unique Periodic Rings Composed of Fractal-Growth Dendritic Branching in Poly(p-dioxanone)

Crystal-by-Crystal Assembly in Two Types of Periodically Banded Aggregates of Poly(p-Dioxanone)

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