Enabling Strategies in Organic Electronics Using Ordered Block Copolymer Nanostructures

Rosa, Claudio De; Auriemma, Finizia; Girolamo, Rocco Di; Pepe, Giovanni Piero; Napolitano, Teresa; Scaldaferri, R.

doi:10.1002/adma.201002649

Cited by 53 publications

(52 citation statements)

References 44 publications

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“…The memory switching behaviors of composite materials using various charge-storage filled additives (metal [17][18][19][20][21][22] or fullerene derivatives [23][24][25][26][27][28][29] ) in the supporting matrices were identified as being achieved via several proposed mechanisms, such as charge trapping/detrapping, 18,23,24 charge-transfer effect, 17,21,22,27-29 filament formation, 19,20 and polarization effect. 25,26 When the recording domains are down to the nanoscale, new materials and advanced techniques must be explored to satisfy the need of storage capacity.…”

Section: -29mentioning

confidence: 99%

“…[34][35][36] Besides the ordered cylindrical nanostructures of BCP being used to selectively sequester the Au NPs, they also exhibited resistive switching. 21 The distribution of charge-storage sites within the thin memory film layer indeed determines the memory device performance. Recently, we demonstrated a supramolecular approach to prepare controlled domain sizes of poly(fluorenylstyrene)-blockpoly-(2-vinylpyridine) P(StFl-b-P2VP):PCBM composite thin films for use in a non-volatile memory device.…”

Section: -32mentioning

confidence: 99%

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Tunable electrical memory characteristics by the morphology of self-assembled block copolymers:PCBM nanocomposite films

et al. 2012

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Resistive switchable memory devices were fabricated using self-assembled composite thin films of asymmetric poly(styrene-block-4-vinylpyridine) (PS-b-P4VP) block copolymers (BCP) and fullerene derivatives (PCBM). L1 (with a longer PS block) was comprised of discrete vertical P4VP nanocylinders embedded within the PS matrix whereas L2 (with a longer P4VP block) revealed a reverse morphology with a horizontal orientation. They were used to control the spatial location or distribution of the PCBM and the resultant memory characteristics. The devices with ITO/BCP:PCBM/ Al configurations exhibited variable multi-electronic characteristics, changing from insulating to bistable memory switching and highly conducting, as the PCBM content increased. The L1:PCBM memory device showed non-volatile write-once-read-many-times (WORM) memory behavior but the L2:PCBM device exhibited a volatile nature of static random access memory (SRAM). Both L1 and L2: PCBM composite devices revealed the improved switching performance upon solvent annealing procedures of the composite thin film. Our results suggested that the controlled morphology of the BCP/PCBM composite could create nanoscale charge-storage elements for a high density memory device with a reduced bit cell size.

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Section: -29mentioning

confidence: 99%

Section: -32mentioning

confidence: 99%

Tunable electrical memory characteristics by the morphology of self-assembled block copolymers:PCBM nanocomposite films

et al. 2012

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“…In the last few decades, many approaches have been proposed for organic nonvolatile memory application, 20−22 for example, the use of polyimides with donor−acceptor units 23 and the hybrid of polymer/metal NPs. 24,25 Previously, we have proposed the combination of redox-active TEMPO and BCPs, and the significance of tailoring BCP morphologies, such as spheres, cylinders, and lamellae to modulate charge transport through the radical/ion-containing BCP layer: (a) nonswitching behavior for lamellae in parallel orientation, (b) write-once and read-many-times (WORM) memory for cylindrical morphology, and (c) rewritable and nonvolatile memory characteristics for spherical domains. 26 Our initial findings for charge-transport modulation through functional BCP nanodomains (morphologies, orientation, and ordering) have a potential impact for the rational design of more efficient organic-based electronic devices.…”

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confidence: 98%

Ionic Liquid-Triggered Redox Molecule Placement in Block Copolymer Nanotemplates toward an Organic Resistive Memory

2015

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The integration of functional components such as metal nanoparticles, metal salts, or ionic liquids with welldefined block copolymer (BCP) nanotemplates via noncovalent bond interactions has afforded hybrid functional materials. Here, we designed an ionic liquid (IL)-functionalized redox-active TEMPO (2,2,6,6-tetramethylpiperidine-Noxy) radical (guest), investigated phase-selective incorporation/ placement into host BCP nanostructured matrices, and established a rational approach to functionalize BCP templates. On-demand domain functionalization of poly(styrene-b-ethylene oxide) (PS-b-PEO) was triggered by ion−ionophore interaction, as verified by the suppression of PEO melting transition in DSC, and the swelling behavior of the PEO spherical domain in AFM, TEM, and X-ray scattering characterizations. The obtained BCP layer containing the redox-active TEMPO and IL was utilized as an active layer in the diode-structured memory device, which exhibited on/off resistive switching (on/off ratio >10 3 ). Systematic placement of TEMPO and IL in the BCP spherical domain allowed for tuning of the switching characteristics and revealed that the formation of a discontinuous redox-active domain was critical for rewritable resistive switching. P rompted by the significant progress in the precise control over size, shape, and long-range ordering of block copolymer (BCP) nanotemplates, 1−3 many research groups have focused on the integration of functional components such as metal nanoparticles (NPs), metal salts, or ionic liquids (ILs) into BCP nanodomains to embed (or deliver) their functionality. 4−7 The metal NPs selectively incorporated in each BCP domain or their interface have been investigated as hybrid materials for microelectronic and photonic applications. 8−10 Amphiphilic BCP−salt (e.g., Li + ) complex or −IL gels have been examined as polyelectrolytes with high ionic conductivity and mechanical durability, 11−13 leading to their potential applications in organic gate dielectrics, actuators, batteries, and fuel cells. 14 The key challenges in the design of such hybrid materials based on noncovalent bond interactions among functional components and BCP segments are to control the location and loading amount of functional components, yet retaining the well-defined phase morphologies. Hydrogen bonding interactions have been extensively examined as a class of domain-selective noncovalent bond interactions; 15,16 however, these weak interactions are comparative to the BCP self-assembly and are not trivial to tune the balance of segregation strength. In this study, we focused on rather stronger "ion−ionophore interactions" between the ILs and the ionophilic BCP segment and utilized ILs as the phaseselective "carrier" to drag functional molecules into BCP nanodomains. The advantages of using organic components in place of inorganic components are design flexibility of the functional groups, tunable compatibility, and facile integration to the polymeric matrices. We selected robust but redox-active organic molecules, in part...

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“…We have explored charge‐transport even in thin solid device configurations, such as diode‐like structured organic resistive memory, and proposed both complementary redox‐active TEMPO and charge‐compensating ion pairs as key components for solid devices . In the last few decades, many approaches have been proposed for organic nonvolatile memory applications, e.g., the use of polyimides with donor–acceptor units and of polymer/metal nanoparticle hybrids . Our earlier work has revealed the significance of the tailoring of block copolymer morphologies and of component locations (TEMPO and the ion pairs) in modulating charge transport through radical‐ and ion‐containing block copolymer layers for imparting characteristics like: (a) nonswitching behavior for lamellae in parallel orientation, (b) write‐once and read‐many‐times (WORM) memory for cylinders, and (c) rewritable and nonvolatile memory characteristics for spheres.…”

Section: Introductionmentioning

confidence: 99%

“Click” Incorporation of Radical/Ionic Sites into a Reactive Block Copolymer: A Facile and On‐Demand Domain Functionalization Approach toward Organic Resistive Memory

Suga

Aoki

Yashiro

et al. 2015

Macromol. Rapid Commun.

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Reversible addition-fragmentation chain transfer polymerization yields reactive block copolymers bearing the pentafluorophenyl ester (PFPA) group, and subsequent Click amidation using 2,2,6,6-tetramethylpiperidine-N-oxyl- and imidazolium-functionalized primary amines produces the corresponding functional block copolymers, leading to installation of statistical radical- and ionic sites into the PFPA segment. The monolayered thin film devices fabricated using the obtained block copolymers exhibit repeatable switching of electric conductivity (on/off ratio > 10 ) under a bias voltage, which reveals that the coexistence of radicals and ions in the same spherical domain of the copolymer layer is a prerequisite for repeatable switching memory.

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Enabling Strategies in Organic Electronics Using Ordered Block Copolymer Nanostructures

Cited by 53 publications

References 44 publications

Tunable electrical memory characteristics by the morphology of self-assembled block copolymers:PCBM nanocomposite films

Tunable electrical memory characteristics by the morphology of self-assembled block copolymers:PCBM nanocomposite films

Ionic Liquid-Triggered Redox Molecule Placement in Block Copolymer Nanotemplates toward an Organic Resistive Memory

“Click” Incorporation of Radical/Ionic Sites into a Reactive Block Copolymer: A Facile and On‐Demand Domain Functionalization Approach toward Organic Resistive Memory

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