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Abstract
Living crystallization-driven self-assembly (CDSA) of semicrystalline block copolymers is a powerful method for the bottom-up construction of uniform polymer microstructures with complex hierarchies. Improving our ability to engineer such complex particles demands a better understanding of how to precisely control the self-assembly process. Here, we apply interferometric scattering (iSCAT) microscopy to observe the real-time growth of individual poly(caprolactone)-based fibers and platelets. This label-free method enables us to map the role of key reaction parameters on platelet growth rate, size, and morphology. Furthermore, iSCAT provides a contrast mechanism for studying multi-annulus platelets formed via the sequential addition of different unimers, offering new insights into the spatial distribution of polymer compositions within a single platelet.
Supplementary materials
Title
Movie S1: Raw movie of platelet growth monitored by iSCAT microscopy
Description
A 50 μL 2.51 nM seed solution was spin-coated onto a cleaned coverslip twice (3200 rpm for 50s followed by 4000 rpm for 30s). PCL45:PCL45-b-PDMA348 mixtures in THF were then diluted with methanol to achieve a final concentration of 0.32 μM. 150 μL unimer methanol
solution was added onto the seed-coated surface and iSCAT observation started immediately. A laser power density of 2 μW μm−2 at 637 nm, a camera exposure time of 800 μs, and an overall time-lapsed frame rate of 1.5 s−1 were chosen. This movie corresponds to the data in Fig. 2
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Title
Movie S2: Raw data of platelet growth recorded with high speed
Description
A 50 μL 2.51 nM seed solution was spin-coated onto the cleaned coverslip twice (3200 rpm for 50 s followed by 4000 rpm for 30 s). PCL45:PCL45-b-PDMA348 mixtures in THF were then diluted with methanol to achieve a final concentration of 0.59 μM. 150 μL of unimer methanol solution was added onto the seed-coated surface and iSCAT observation started immediately. A laser power density of 24 μW μm−2 at 637 nm, a camera exposure time of 80 μs, and an overall time-lapsed frame rate of 100 s−1 were chosen. This movie corresponds to the data in Fig. S2A and B
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Title
Movie S3: Raw data of platelet growth recorded with high speed
Description
50 μL 2.51 nM seed solution was spin-coated onto the cleaned coverslip twice (3200 rpm for 50 s followed by 4000 rpm for 30 s). PCL45:PCL45-b-PDMA348 mixtures in THF was then diluted with methanol to achieve final concentration of 0.29 μM. 150 μL unimer methanol solution was added onto the seed-coated surface and iSCAT observation started from the mid-stage of platelet growth. A laser power density of 24 μW μm−2 at 637 nm, a camera exposure time of 80 μs, and an overall time-lapsed frame rate of 3000 s−1 were chosen. This movie corresponds to the data in Fig. S2C and D
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Title
Movie S4: Raw data of four-layer platelet growth monitored by iSCAT microscopy
Description
50 μL 2.51 nM seed solution was spin-coated onto the cleaned coverslip twice (3200 rpm for 50s followed by 4000 rpm for 30s). Layer 1: 150 μL 0.18 μM PCL45:PCL45-
b-PDMA348 methanol solution; Layer 2: 150 μL 0.39 μM PCL45 unimer methanol solution; Layer 3: 150 μL 0.35 μM PCL45:PCL45-b-PDMA348 methanol solution; Layer 4: 150 μL 0.77 μM PCL45 unimer methanol solution. A laser power density of 4 μW μm−2 at 637 nm, a camera exposure time of 500 μs, and an overall time-lapsed frame rate of 1 s−1 were chosen. This movie corresponds to the data in Fig. 5B and C.
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Title
Movie S5: Raw data of three-layer platelet growth monitored by iSCAT microscopy
Description
50 μL 2.51 nM seed solution was spin-coated onto the cleaned coverslip twice (3200 rpm for 50 s followed by 4000 rpm for 30 s). PCL45:PCL45-b-PDMA348 mixtures
methanol solution was added sequentially with concentration of 0.44, 0.59 and 0.87 μM for
each layer. A laser power density of 4 μW μm−2 at 637 nm, a camera exposure time of 400 μs, and an overall time-lapsed frame rate of 0.5 s−1 were chosen. This movie corresponds to the data in Fig. 5F and G
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