PMMA Domains Research Articles

Spatially Templated Nanolines of Ru and RuO2 by Sequential Infiltration Synthesis

Nanoscale patterning of inorganics is crucial for the fabrication of advanced electronic, photonic, and energy devices. The emerging sequential infiltration synthesis (SIS) method fabricates nanofeatures by block-selective vapor-phase growth in block copolymer templates with tunable patterns. Yet, SIS has been demonstrated mainly for Al2O3 and a few other metal oxides, while deriving metal nanostructures from a single SIS process is a challenge. Here, we present SIS of the Ru metal in polystyrene-block-polymethyl methacrylate (PS-b-PMMA) templates without any pretreatment, using alternating infiltration of RuO4 and H2. RuO4 interacts selectively and strongly with the aromatic C═C and C–H groups in PS, leaving the PMMA domains inert. Density functional theory calculations corroborate that the PS–RuO4 interaction is energetically favorable, with a calculated interaction energy of −1.65 eV, whereas for PMMA–RuO4, the calculated energy of −0.05 eV indicates an unfavorable interaction. Morphological analysis on the di-BCP after the RuO4-H2 process indicates an increase in contrast as a function of SIS cycles and templated Ru incorporation. The crystalline nature of the Ru deposits is confirmed using grazing incidence wide-angle X-ray scattering. Plasma-aided removal of the organic components yields Ru nanolines with lateral dimensions of ca 20 nm. We further highlight the broad potential of RuO4 as a reactant for SIS by generating RuO2 nanopatterns via alternating RuO4 and methanol infiltration.

Thermo-responsive programmable shape memory polymer based on amidation cured natural rubber grafted with poly(methyl methacrylate)

This work proposes a facile and new approach that uses graft copolymerization and amidation reaction to prepare shape memory polymer (SMP) based on natural rubber (NR). The poly(methyl methacrylate) modified NR (MGNR) is cross-linked with diamine through an amidation reaction. In this kind of approach, a novel type of cross-linked MGNR with a three-dimensional network of amide linkage was prepared. The solvent resistance, mechanical properties, and phase morphology of MGNRs were significantly improved after being cross-linked by a diamine cross-linker. Additionally, the cross-linked MGNR40 also exhibited excellent shape fixation and shape recovery. This is a direct result of the vitrification of the grafted PMMA domains at low temperatures, preventing elastic recovery. Meanwhile, a cross-linked network from amide linkage facilitates recovery force upon heating. Hence, the shape memory performance of MGNRs can be tuned with both grafted PMMA content and the degree of diamine cross-link. The strategy in this research work offered an effective and convenient method to obtain cross-linked MGNR with unique molecular architecture. Consequently, this cross-linked MGNR delivered excellent mechanical strength and shape memory performance.

Fabrication of Block Copolymer Templated Extended Surface Model Electrocatalysts By Atomic Layer Deposition and Physical Vapor Deposition

Templating platinum group metal (PGM) nanostructures from microphase separated block copolymers (BCPs) allows for electrocatalytic activity to be studied on highly ordered, model surfaces with precisely controlled feature sizes and morphologies, thereby allowing catalyst electroactivity and stability to be probed as a function of nanoscale geometry. In our previous work [1], BCP templated electrocatalysts fabricated via incipient wetness impregnation of PGM precursors were tested for hydrogen oxidation/evolution and water-splitting activity on interdigitated electrodes using liquid and solid polymer electrolytes. This talk presents the fabrication of such electrocatalysts via Atomic Layer Deposition (ALD) and Physical Vapor Deposition (PVD) techniques (e-beam evaporation and sputtering). Self-assembled lamellae of poly-(styrene-block-methylmethacrylate) (PSbPMMA) thin films on Si wafer and glassy carbon substrates were subjected to 5 - 15 ALD cycles with trimethylaluminium (TMA) precursor to induce selective growth of alumina in the PMMA domains via Sequential Infiltration Synthesis. Thereafter, the polymer template was removed via Reactive Ion Etching (RIE) with oxygen plasma. The resultant alumina nanostructures templated from self-assembled PSbPMMA was then used as a substrate either for Platinum ALD with (trimethyl)methylcyclopentadienylplatinum(IV) precursor atop a Titanium Nitride adhesive layer, or for sputtering of Pt atop a Ti adhesive layer to obtain conformal Pt coatings of up to 20 nm in thickness. When e-beam evaporation was used, The PMMA domains were selectively removed by successive wet and dry etch steps, followed by deposition and lift-off. The PGM electrocatalyst nanostructures were characterized via a combination of electron microcopy, X-ray diffraction, and X-ray photoelectron spectroscopy, and the Pt content of the catalysts were determined via microwave leaching and digestion of the electrocatalyst thin film followed by Inductively Coupled Plasma Mass Spectroscopy. The nanostructured electrocatalysts were tested for oxygen reduction (ORR) activity in a conventional rotating disk electrode setup using 0.1 M perchloric acid electrolyte, and the ORR mass activities and active surface area were obtained.[1] Bhattacharya, D., Arges, C. G., et al., Small, 2021, 17, 2100437

In-depth probing of thermally-driven phase separation behavior of lamella-forming PS-b-PMMA films by infrared nanoscopy

A non-invasive, image-based analytic method utilizing scattering-type scanning near-field optical microscopy (s-SNOM) is suggested to evaluate the phase separation behavior of lamella-forming polystyrene-b-poly(methyl methacrylate) (PS-b-PMMA) block copolymer films. Taking advantage of the penetrability of the tip-enhanced IR signal into the films, the spatio-spectral maps of each component are constructed. Subsequently, the effect of a sole and combinatorial applications of the self-assembly procedures, such as solvent vapor annealing (SVA) and/or thermal annealing (TA), on the spatial distribution of PS or PMMA components is quantitatively assessed in terms of the areal portions of the PS domain, PMMA domain, and the mixed zone that is adjacent to the domain border. Additionally, by statistically comparing the local concentration profiles, the chemical contrast between the domains turns out to be dependent upon the annealing procedures (namely, SVA and SVA + TA). This technique can pave the way to an uncomplicated but precise investigation of the polymer nanostructure-based thin film devices whose performances are critically governed by the spatial arrangement of the chemical elements.

Correlating Optical Reflectance with the Topology of Aluminum Nanocluster Layers Growing on Partially Conjugated Diblock Copolymer Templates.

Large-scale fabrication of metal cluster layers for usage in sensor applications and photovoltaics is a huge challenge. Physical vapor deposition offers large-scale fabrication of metal cluster layers on templates and polymer surfaces. In the case of aluminum (Al), only little is known about the formation and interaction of Al clusters during sputter deposition. Complex polymer surface morphologies can tailor the deposited Al cluster layer. Here, a poly(methyl methacrylate)-block-poly(3-hexylthiophen-2,5-diyl) (PMMA-b-P3HT) diblock copolymer template is used to investigate the nanostructure formation of Al cluster layers on the different polymer domains and to compare it with the respective homopolymers PMMA and P3HT. The optical properties relevant for sensor applications are monitored with ultraviolet-visible (UV-vis) measurements during the sputter deposition. The formation of Al clusters is followed in situ with grazing-incidence small-angle X-ray scattering (GISAXS), and the chemical interaction is revealed by X-ray photoelectron spectroscopy (XPS). Furthermore, atomic force microscopy (AFM) and field emission scanning electron microscopy (FESEM) yield topographical information about selective wetting of Al on the P3HT domains and embedding in the PMMA domains in the early stages, followed by four distinct growth stages describing the Al nanostructure formation.

Formation of biomimetic hierarchical nanostructure in homopolymers and block copolymer ternary blend particles

In order to mimic hierarchical nanostructures in nature, particles of polymer blends consisting of poly(4-butyltriphenylamine) (PBTPA), poly(methyl methacrylate) (PMMA) and PBTPA-block-PMMA were fabricated by a solvent evaporation method. Effects of the molecular weight and the chemical composition of PBTPA-b-PMMA, molecular weights of homopolymers, and the composition of the blend on the morphology were investigated. The polymer blend particle consisting of PBTPA and PMMA homopolymers exhibited thermodynamically favored core-shell structure, in which more hydrophilic PMMA-shell surrounded PBTPA-core. The addition of 10 wt% of PBTPA-b-PMMA caused the morphological transition from core-shell to Janus or inversed core-shell, in which PBTPA-shell surrounded PMMA-core, depending on the molecular weight of PBTPA segment in PBTPA-b-PMMA. When the molecular weight of PMMA segment was higher than that of PMMA homopolymer, watermelon-like particles in which small PBTPA domain less than 80 nm dispersed in the PMMA domain surrounded by PBTPA shell were observed. As the ratio of PBTPA-b-PMMA increased, the interface of the macrophase separation became obscure. At 50 wt% of the PBTPA-b-PMMA, only microphase separation was observed. The measurement of interfacial tension by pendant drop method demonstrated that PBTPA-b-PMMA lower the interfacial tension between PBTPA and the aqueous phase to the value similar to that of PMMA with the aqueous phase.

Additive Effects of Lithium Salts with Various Anionic Species in Poly (Methyl Methacrylate).

We report that lithium salts in lithium-ion batteries effectively modify the physical properties of poly (methyl methacrylate) (PMMA). The glass transition temperature (Tg) is an indicator of the heat resistance of amorphous polymers. The anionic species of the salts strongly affected the glass transition behavior of PMMA. We focused on the additive effects of various lithium salts, such as LiCF3SO3, LiCOOCF3, LiClO4, and LiBr, on the Tg of PMMA. The large anions of the former three salts caused them to form macroscopic aggregates that acted as fillers in the PMMA matrix and to combine the PMMA domains, increasing Tg. On the other hand, LiBr salts dispersed microscopically in the PMMA matrix at the molecular scale, leading to the linking of the PMMA chains. Thus, the addition of LiBr to PMMA increased Tg as well as the relaxation time in the range of glass to rubber transition.

Carbon nanotube functional group-dependent compatibilization of polyamide 6 and poly(methyl methacrylate) nanocomposites

Nanocomposites of polyamide 6 (PA6)–poly(methyl methacrylate) (PMMA)–functionalized single-wall carbon nanotubes (f-SWCNTs) with hydroxyl (SWCNTOH) and carboxylic acid (SWCNTCOOH) in weight ratios of 79.5–19.5–1, 49.5–49.5–1, and 19.5–79.5–1 were fabricated and investigated in terms of morphology, mechanical and XRD studies. Blends of 80–20, 50–50, and 20–80 weight ratios of PA6–PMMA have functioned as references. The scanning electron microscopy images of nanocomposites showed a relatively uniform dispersion of PMMA domains as co-continuous phase morphology in the continuous phase of PA6 compared to their respective blends. The f-SWCNTs acted as functional group-dependent compatibilizers for the PA6–PMMA blend system. Compatibilization of PA6-PMMA blends was higher in the presence of functionalized SWCNTs. XRD analysis indicated that the αI and αII phases of the PA6 were dependent on the weight ratio of the PA6 and PMMA and the nature of the f-SWCNTs. The PMMA-rich blends and nanocomposites exhibited the rich αI phase. The melt strength of the nanocomposites was higher compared to that of the PA6–PMMA blends. All the nanocomposites exhibited higher tensile strength than their corresponding blends. Tensile modulus increased with increasing weight percent of PMMA in blends (from 810 to 1135 MPa) and in nanocomposites (from 854 to 1298 MPa). PA6–PMMA–SWCNTOH19.5–79.5–1 nanocomposites exhibited higher tensile modulus (1298 MPa) compared to all the blends and PA6–PMMA–SWCNTCOOH nanocomposites.

Rheological behavior, electrical conductivity, and morphology of multi‐walled carbon nanotube filled poly(ethylene‐co‐vinyl acetate)/poly(methyl methacrylate) nanocomposites: Effect of nanofiller content

AbstractNanocomposites derived from poly(methyl methacrylate) (PMMA) and poly(ethylene‐co‐vinyl acetate) (EVA) with 30 wt% EVA and 0–10 wt% multi‐walled carbon nanotube (MWCNT) content were prepared. Scanning electron microscope images showed a two‐phase morphology for the unfilled blend in which the EVA droplets were dispersed within the PMMA domain. However, the size of EVA droplets was considerably smaller in the nanocomposites than that of the unfilled blend. The tensile results revealed that the maximum elastic modulus, tensile strength, yield stress, and strain at break were achieved for the nanocomposite containing 5 wt% MWCNT. The electrical conductivity sharply increased for the nanocomposite containing 2.5 wt% MWCNT, in comparison with that of the unfilled blend, beyond which the conductivity was less dependent on the MWCNT content. The rheological characterization showed that the normalized relaxation time increased up to 5 wt% nanofiller and remained reasonably constant for higher amounts of MWCNT.

Insight into the structure of polystyrene-poly(methyl methacrylate) core-shell particles synthesized by seeded suspension polymerization

Core-shell particles were synthesized employing seeded suspension polymerization. Suspension polystyrene (PS) particles were used as seeds, and poly(methyl methacrylate) (PMMA) was synthesized in the presence of polystyrene seeds. A combination of solvent extraction, Fourier transform infrared spectroscopy, scanning electron microscopy, and transmission electron microscopy techniques were employed to study the structure and morphology of synthesized particles. The results suggested a core-inner shell-outer shell structure for the synthesized particles in which the PS core was covered by a PMMA-rich inner shell and a very thin PS-rich outer shell. The size and concentration of PMMA domains decreased from the outer shell toward the core of the particle, and particle morphology was mainly controlled by the limitations to the diffusion of MMA through the polymer particle.

Tough, Transparent, Photocurable Hybrid Elastomers.

We investigated polydimethylsiloxane/poly(methyl methacrylate) (PDMS/PMMA) interpenetrating polymer networks (IPNs) by both sequential and simultaneous syntheses. In the sequential IPN, the PDMS network was first thermally cured after which methyl methacrylate was swelled in and UV photopolymerized in situ. The simultaneous IPN consists of a one-pot, single-step UV cure of both components. Pure shear fracture and tensile tests were used to extract the Young's modulus, critical fracture strain, and fracture energy of the materials at varying PMMA fractions (up to 50 wt %). At high PMMA fractions, a maximum increase in Young's modulus (42×) and fracture energy (21×) was observed with little sacrifice in the optical properties and the extensibility of notched samples. The Krieger-Dougherty model for particle reinforcement was fit to the modulus data as a function of the PMMA fraction and showed good agreement. The optical properties and microstructure of the IPNs were investigated by UV-visible light transmission, small-angle X-ray scattering (SAXS), and atomic force microscopy (AFM). As the weight fraction of PMMA increased, the simultaneous IPN became less transparent, while the sequential material showed the opposite trend. In the sequential IPN, the minority phase size decreased with increasing PMMA fraction, while it was constant for the simultaneous IPN. Therefore, it was concluded that the sequential IPN transparency is controlled by the size of the PMMA domains, but the simultaneous IPN transparency is controlled by the PMMA fraction. SAXS and AFM also showed evidence of bicontinuous network formation in the simultaneous IPN, which may affect the optical and mechanical properties.

Acoustic Radiation Force on a Spherical Fluid or Solid Elastic Particle Placed Close to a Fluid or Solid Elastic Half-Space

The acoustic radiation force acting on a spherical particle placed close to the interface of two infinite half-spaces that is excited by a normally incident traveling wave is investigated using the finite element method (FEM). The medium surrounding the particle is water, whereas different material models are used for the particle itself and the second half-space. Recently, acoustic force spectroscopy has been developed, a technology that uses acoustic forces to measure the mechanical properties of small filaments. If acoustics are used to manipulate particles that are placed very close to an interface then the acoustic interactions between the particle and interface lead to an acoustic interaction force. This interaction force was neglected in previous studies and is included in the total acoustic radiation force obtained by our FEM model. Comparing our results to the primary radiation force that can be obtained using the Gor'kov potential, we found that, for cells (red blood cells or fat cells) immersed in water and placed close to a PMMA, glass, or silicon domain, the magnitude of the acoustic interaction force can exceed 10% of the magnitude of the primary radiation force. In other cases, the acoustic interaction force can be even larger in amplitude and of opposite sign than the primary force.

Fabrication of inverse core–shell and Janus-structured microspheres of blends of poly(4-butyltriphenylamine) and poly(methyl methacrylate)

We here report the facile fabrication of inverse core–shell and Janus structured particles consisting of poly(4-butyltriphenylamine) (PBTPA) and poly(methyl methacrylate) (PMMA) via a solvent evaporation from solution droplets of a polymer blend dispersed in an aqueous phase. Janus structured composite particles in which the PBTPA domain was partially coated by the PMMA domain were obtained using poly(vinyl alcohol) (PVA) as a suspension stabilizer. On the other hand, when sodium dodecyl sulfate (SDS) was added as a surfactant together with PVA, “inverse core–shell” particles in which the PMMA core was covered by the PBTPA shell were formed as well as Janus particles. TEM observation showed that the PMMA core was located at the center of the sphere and PBTPA layer has uniform thickness in inverse core–shell particles. The increase of the composition of PBTPA or the concentration of SDS increased the ratio of the inverse core–shell particles to the Janus ones.

Self-Assembly of Large Magnetic Nanoparticles in Ultrahigh Molecular Weight Linear Diblock Copolymer Films.

The development of diblock copolymer (DBC) nanocomposite films containing magnetic nanoparticles (NPs) with diameters (D) over 20 nm is a challenging task. To host large iron oxide NPs (Fe3O4, D = 27 ± 0.6 nm), an ultrahigh molecular weight (UHMW) linear DBC polystyrene-block-poly(methyl methacrylate) (PS-b-PMMA) is used as a template in the present work. Due to hydrogen bonding between the carboxylic acid ligands of the NPs and the ester groups in PMMA, the NPs show an affinity to the PMMA block. The localization of the NPs inside the DBC is investigated as a function of the NP concentration. At low NP concentrations, NPs are located preferentially at the interface between PS and PMMA domains to minimize the interfacial tension caused by the strong segregation strength of the UHMW DBC. At high NP concentrations (≥10 wt %), chain-like NP aggregates (a head-to-tail orientation) are observed in the PMMA domains, resulting in a change of the morphology from sphere to ellipsoid for part of the PMMA domains. Magnetic properties of the hybrid films are probed via superconducting quantum interference device magnetometry. All hybrid films show ferrimagnetism and are promising for potential applications in magnetic data storage.

Strained Bottlebrushes in Super-Soft Physical Networks.

ABA triblock copolymers composed of a poly(dimethylsiloxane) (PDMS) bottlebrush central block and linear poly(methyl methacrylate) (PMMA) terminal blocks self-assemble into a physical network of PDMS bottlebrush strands connected by PMMA spherical domains. A combination of small- and ultrasmall-angle X-ray scattering techniques was used to concurrently examine dimensions of PMMA spherical domains and PDMS bottlebrush strands both in the bulk and at the PMMA-PDMS interface. In agreement with scaling model predictions, the degrees of polymerization of the bottlebrush backbone (nbb) and PMMA block (nA) correlate with the measured PMMA domain size and area per molecule at the PMMA-PDMS interface as DA ∝ (nbbnA)1/3 and S ∝ nA2/3nbb-1/3, respectively. In the bulk, bottlebrush strands are extended due to steric repulsion between the side chains and unfavorable interactions between the different blocks. At the PMMA-PDMS interface with large curvature, packing constraints require additional bottlebrush backbone extension and alignment of side chains along the backbone in the direction perpendicular to the interface.

Cellulose nanocrystal driven microphase separated nanocomposites: Enhanced mechanical performance and nanostructured morphology.

The interest in the modification of cellulose nanocrystals (CNCs) lies in the potential to homogenously disperse CNCs in hydrophobic polymer matrices and to promote interfacial adhesion. In this work, poly(methyl methacrylate) (PMMA) and poly(butyl acrylate) (PBA) were grafted onto CNCs, thereby imparting their hydrophobic traits. The successful grafting modification led to the increased thermal stability of modified CNCs (MCNCs), and the hydrophobic surface modification was integrated with crystalline structure and morphology of CNCs. The nanocomposites with 7 wt% MCNCs/PBA-co-PMMA had an increase in Young's modulus of >25-fold and in tensile strength at about 3 times compared to these of neat PBA-co-PMMA copolymer. In addition, a micro-phase separated morphology (PBA soft domains, and PMMA and CNC hard domains) of MCNCs/PBA-co-PMMA nanocomposites was observed. The large increase in the storage moduli (glass transition temperatures) and organized morphology of MCNCs/PBA-co-PMMA nanocomposites also elucidated the relationship between mechanical properties and micro-phase separated morphology. Therefore, the MCNCs are effective reinforcing agents for the PBA-co-PMMA thermoplastic elastomers, opening up opportunities for their wide-spread applications in polymer composites.

Fabrication of Interpenetrating Polymer Networks of SBR and PMMA with Nano Domains

Interpenetrating polymer networks (IPNs) are one of the important hybrid polymeric systems with specific peculiarities. IPN based on styrene butadiene rubber (SBR) and poly [methyl methacrylate] (PMMA) has been fabricated by sequential polymerisation technique. The different mechanical properties of IPNs are investigated in detail. The effect of blend ratio on mechanical properties of IPNs is evaluated. Morphological analysis of IPNs through TEM provides clear insight of their component distribution in it. IPN with co-continuous morphological pattern and nanometre sized PMMA domains show better mechanical properties.

Role of Chain Connectivity across an Interface on the Dynamics of a Nanostructured Block Copolymer.

Fluorescence labeling enables component- and location-specific measurements of the glass transition temperature (T_{g}) in complex polymer systems. Here we characterize the T_{g} of fluorescently labeled poly(methyl methacrylate) homopolymers (PMMA-py) blended at low concentrations into an unlabeled lamellar poly(n-butyl methacrylate-b-methyl methacrylate) diblock copolymer (PBMA-PMMA). In this system, the PMMA-py homopolymer is sequestered within the PMMA domains of the diblock copolymer and subject to soft confinement by the domains of the lower-T_{g} PBMA block, which lowers the homopolymer T_{g} by ∼5 K beyond the contribution of segmental mixing. In contrast to the PMMA block in the diblock copolymer, the PMMA-py homopolymer is not covalently bound to the interdomain interface. A comparison of T_{g} for the homopolymers in the blends to T_{g} for diblock copolymers with equivalent labeled segment density profiles reveals that the homopolymer's T_{g} is consistently ∼10 K higher than for diblock segments at the same location within the domain structure, highlighting the dominant contribution of a covalent bond across the interface to the perturbation of the chain dynamics in the block copolymer.

Alignment of Nanoplates in Lamellar Diblock Copolymer Domains and the Effect of Particle Volume Fraction on Phase Behavior.

Polymer nanocomposites (PNCs) that employ diblock copolymers (BCPs) to organize and align anisotropic nanoparticles (NPs) have the potential to facilitate self-assembling hierarchical structures. However, limited studies have been completed to understand the parameters that guide the assembly of nonspherical NPs in BCPs. In this work, we establish a well-defined nanoplate system to investigate the alignment of two-dimensional materials in a lamellar-forming poly(styrene-b-methyl methacrylate) (PS-b-PMMA) BCP with domains oriented parallel to the substrate. Monodisperse gadolinium trifluoride rhombic nanoplates doped with ytterbium and erbium [GdF3:Yb/Er (20/2 mol %)] are synthesized and grafted with phosphoric acid functionalized polyethylene glycol (PEG-PO3H2). Designed with chemical specificity to one block, the nanoplates align in the PMMA domain at low volume fractions (ϕ = 0.0083 and ϕ = 0.017). At these low NP loadings, the BCP lamellae are ordered and induce preferential alignment of the GdF3:Yb/Er nanoplates. However, at high volume fractions (ϕ = 0.050 and ϕ = 0.064), the BCP lamellae are disordered with isotropically dispersed nanoplates. The transition from an ordered BCP system with aligned nanoplates to a disordered BCP with unaligned nanoplates coincides with the calculated overlap volume fraction, ϕ* = 0.051, where the pervaded space of the NPs begins to overlap. Two phenomena are observed in the results: the effect of lamellar formation on nanoplate orientation and the overall phase behavior of the PNCs. The presented research not only expands our knowledge of PNC phase behavior but also introduces a framework to further study the parameters that affect nanoplate alignment in BCP nanocomposites. Our ability to control anisotropic NP orientation in PNCs through self-assembling techniques lends itself to creating multifunctional materials with unique properties for various applications such as photovoltaic cells and barrier coatings.

Structural Evolution of Two-Phase Blends of Polycarbonate and PMMA by Simultaneous Biaxial Stretching.

We investigated the structural evolution of the two-phase blends of polycarbonate (PC) and poly(methyl methacrylate) (PMMA) at various blend compositions by simultaneous biaxial stretching, using optical microscopy and SEM observation. The spherical PMMA domains and PC matrix of 30/70 PC/PMMA were enlarged uniformly at the all in-plane direction, while the anisotropic-shaped co-continuous structure in 50/50 PC/PMMA was deformed to a crosshatched structure by the in-plane bimodal orientation. In 70/30 PC/PMMA, the phase inversion was found to occur by simultaneous biaxial stretching; that is, the spherical PMMA domains were changed to a crosshatched matrix by the in-plane bimodal orientation due to coalescence of the PMMA domains during the stretching. Owing to the phase inversion, the surface hardness estimated by the pencil hardness test became harder, from 2B to 2H, increasing the strain from 1.0 to 2.0.