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Excited-State Interaction of Semiconducting Single-Walled Carbon Nanotubes with Their Wrapping Polymers.

ABSTRACT: We employ photoluminescence and pump-probe spectroscopy on films of semiconducting single-walled carbon nanotubes (CNTs) of different chirality wrapped with either a wide band gap polyfluorene derivative (PF12) or a polythiophene with narrower gap (P3DDT) to elucidate the excited states' interplay between the two materials. Excitation above the polymer band gap gives way to an ultrafast electron transfer from both polymers toward the CNTs. By monitoring the hole polaron on the polymer via its mid infrared signature, we show that also illumination below the polymer band gap leads to the formation of this fingerprint and infer that holes are also transferred toward the polymer. As this contradicts the standard way of discussing the involved energy levels, we propose that polymer-wrapped CNTs should be considered as a single hybrid system, exhibiting states shared between the two components. This proposition is validated through quantum chemical calculations that show hybridization of the first excited states, especially for the thiophene-CNT sample.

SUBMITTER: Kahmann S

PROVIDER: S-EPMC5694966 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Charge Transfer from Photoexcited Semiconducting Single-Walled Carbon Nanotubes to Wide-Bandgap Wrapping Polymer.

Project description:As narrow optical bandgap materials, semiconducting single-walled carbon nanotubes (SWCNTs) are rarely regarded as charge donors in photoinduced charge-transfer (PCT) reactions. However, the unique band structure and unusual exciton dynamics of SWCNTs add more possibilities to the classical PCT mechanism. In this work, we demonstrate PCT from photoexcited semiconducting (6,5) SWCNTs to a wide-bandgap wrapping poly-[(9,9-dioctylfluorenyl-2,7-diyl)-alt-(6,6')-(2,2'-bipyridine)] (PFO-BPy) via femtosecond transient absorption spectroscopy. By monitoring the spectral dynamics of the SWCNT polaron, we show that charge transfer from photoexcited SWCNTs to PFO-BPy can be driven not only by the energetically favorable E33 transition but also by the energetically unfavorable E22 excitation under high pump fluence. This unusual PCT from narrow-bandgap SWCNTs toward a wide-bandgap polymer originates from the up-converted high-energy excitonic state (E33 or higher) that is promoted by the Auger recombination of excitons and charge carriers in SWCNTs. These insights provide new pathways for charge separation in SWCNT-based photodetectors and photovoltaic cells.

| S-EPMC8154833 | biostudies-literature

Enrichment mechanism of semiconducting single-walled carbon nanotubes by surfactant amines.

Project description:Utilization of single-walled carbon nanotubes (SWNTs) in high-end applications hinges on separating metallic (met-) from semiconducting (sem-) SWNTs. Surfactant amines, like octadecylamine (ODA) have proven instrumental for the selective extraction of sem-SWNTs from tetrahydrofuran (THF) nanotube suspensions. The chemical shift differences along the tail of an asymmetric, diacetylenic surfactant amine were used to probe the molecular dynamics in the presence and absence of nanotubes via NMR. The results suggest that the surfactant amine head is firmly immobilized onto the nanotube surface together with acidic water, while the aliphatic tail progressively gains larger mobility as it gets farther from the SWNT. X-ray and high-resolution TEM studies indicate that the sem-enriched sample is populated mainly by small nanotube bundles containing ca. three SWNTs. Molecular simulations in conjunction with previously determined HNO(3)/H(2)SO(4) oxidation depths for met- and sem-SWNTs indicate that the strong pinning of the amine surfactants on the sem-enriched SWNTs bundles is a result of a well-ordered arrangement of nitrate/amine salts separated with a monomolecular layer of H(2)O. Such continuous 2D arrangement of nitrate/amine salts shields the local environment adjacent to sem-enriched SWNTs bundles and maintains an acidic pH that preserves nanotube oxidation (i.e., SWNT(n+)). This, in turn, results in strong interactions with charge-balancing NO(3)(-) counterions that through their association with neutralized surfactant amines provide effective THF dispersion and consequent sem enrichment.

| S-EPMC2767324 | biostudies-literature

Photoinduced spontaneous free-carrier generation in semiconducting single-walled carbon nanotubes.

Project description:Strong quantum confinement and low dielectric screening impart single-walled carbon nanotubes with exciton-binding energies substantially exceeding kBT at room temperature. Despite these large binding energies, reported photoluminescence quantum yields are typically low and some studies suggest that photoexcitation of carbon nanotube excitonic transitions can produce free charge carriers. Here we report the direct measurement of long-lived free-carrier generation in chirality-pure, single-walled carbon nanotubes in a low dielectric solvent. Time-resolved microwave conductivity enables contactless and quantitative measurement of the real and imaginary photoconductance of individually suspended nanotubes. The conditions of the microwave conductivity measurement allow us to avoid the complications of most previous measurements of nanotube free-carrier generation, including tube-tube/tube-electrode contact, dielectric screening by nearby excitons and many-body interactions. Even at low photon fluence (approximately 0.05 excitons per μm length of tubes), we directly observe free carriers on excitation of the first and second carbon nanotube exciton transitions.

| S-EPMC4667683 | biostudies-literature

Electronic Raman scattering on individual semiconducting single walled carbon nanotubes.

Project description:We report experimental measurements of electronic Raman scattering by electrons (holes) in individual single-walled carbon nanotubes (SWNTs) under resonant conditions. The Raman scattering at low frequency range reveals a single particle excitation feature. And the dispersion of electronic structure around the center of Brillouin zone of a semiconducting SWNT (14, 13) is extracted.

| S-EPMC4122977 | biostudies-other

Polyaniline photoluminescence quenching induced by single-walled carbon nanotubes enriched in metallic and semiconducting tubes.

Project description:The influence of single-walled carbon nanotubes enriched in semiconductor (S-SWNTs) and metallic (M-SWNTs) tubes on the photoluminescence (PL) of polyaniline (PANI), electrosynthesized in the presence of the H2SO4 and HCl solutions, is reported. The emission bands peaked at 407-418 and 440-520?nm indicate that the electropolymerization of aniline (ANI) leads to the formation of short and longer macromolecular chains (MCs), respectively. We demonstrate that the reaction product consists of ANI tetramers (TT) and trimers (TR) as well as PANI-salt. Using Raman scattering and IR absorption spectroscopy, a covalent functionalization of SWNTs with shorter and longer MCs of PANI-salt is demonstrated. The presence of S-SWNTs and M-SWNTs induces a decrease in ANI TT weight in the reaction product mass consisting in S-SWNTs and M-SWNTs covalently functionalized with PANI-emeraldine salt (ES) and PANI-leucoemeraldine salt (LS), respectively. A PANI PL quenching is reported to be induced of the S-SWNTs and M-SWNTs. A de-excitation mechanism is proposed to explain PANI PL quenching.

| S-EPMC6015054 | biostudies-literature

Sorting and decoration of semiconducting single-walled carbon nanotubes <i>via</i> the quaternization reaction.

Project description:A study for the selective separation and functionalization of alcohol-soluble semiconducting single-walled carbon nanotubes (sc-SWCNTs) is carried out by polymer main-chain engineering. Introducing tertiary amine groups endows the functionalized sc-SWCNTs with alcohol-soluble properties and introducing the pyrimidine rings allows to increase the selective purity of sc-SWCNTs. In this study, a series of poly[(9,9-dioctylfluorene)-2,7-(9,9-bis(3'-(N,N-dimethylamino)propyl)-fluorene)] m -alt-[2-methylpyrimidine-2,7-(9,9-dioctylfluorene)] n (PFPy) are used for the selective dispersion of semiconducting single-walled carbon nanotubes, where n and m are the composition ratio of the copolymer. When m = n, the effective isolation of sc-SWCNTs with purity greater than 99% is achieved. The alcohol-soluble sc-SWCNTs with a diameter in the range of 1.1-1.4 nm are obtained through designing reasonable molecular structure. Moreover, the particular preference of PFPy (m = n) for sc-SWCNTs was studied via density functional theory (DFT) calculations and it was proved to be a promising method for the separation and functionalization of sc-SWCNTs.

| S-EPMC8693859 | biostudies-literature

Single Walled BiI3 Nanotubes Encapsulated within Carbon Nanotubes.

Project description:Inorganic nanotubes are morphological counterparts of carbon nanotubes (CNTs). Yet, only graphene-like BN layer has been readily organized into single walled nanotubes so far. In this study, we present a simple route to obtain inorganic single walled nanotubes - a novel ultrathin morphology for bismuth iodide (BiI3), embedded within CNTs. The synthesis involves the capillary filling of BiI3 into CNT, which acts as a nanotemplate, by annealing the BiI3-CNT mixture above the melting point of BiI3. Aberration corrected scanning/transmission electron microscopy is used in characterizing the novel morphology of BiI3. A critical diameter which enables the formation of BiI3 nanotubes, against BiI3 nanorods is identified. The relative stability of these phases is investigated with the density functional theory calculations. Remarkably, the calculations reveal that the single walled BiI3 nanotubes are semiconductors with a direct band gap, which remain stable even without the host CNTs.

| S-EPMC6031677 | biostudies-literature

Wide dynamic range enrichment method of semiconducting single-walled carbon nanotubes with weak field centrifugation.

Project description:The potential of single-walled carbon nanotubes (SWCNTs) to outperform silicon in electronic application was finally enabled through selective separation of semiconducting nanotubes from the as-synthesized statistical mix with polymeric dispersants. Such separation methods provide typically high semiconducting purity samples with narrow diameter distribution, i.e. almost single chiralities. But for a wide range of applications high purity mixtures of small and large diameters are sufficient or even required. Here we proof that weak field centrifugation is a diameter independent method for enrichment of semiconducting nanotubes. We show that the non-selective and strong adsorption of polyarylether dispersants on nanostructured carbon surfaces enables simple separation of diverse raw materials with different SWCNT diameter. In addition and for the first time, we demonstrate that increased temperature enables higher purity separation. Furthermore we show that the mode of action behind this electronic enrichment is strongly connected to both colloidal stability and protonation. By giving simple access to electronically sorted SWCNTs of any diameter, the wide dynamic range of weak field centrifugation can provide economical relevance to SWCNTs.

| S-EPMC5357843 | biostudies-other

Interaction between multi-walled carbon nanotubes and propranolol.

Project description:Carbon nanotubes could accumulate in organism and have a negative impact on the structure and function of the ecosystem when they were discharged into environment. Furthermore, it will affect the migration and fate of pollutants in the water body. The study is mainly to explore the adsorption behavior and mechanism of beta-blocker on multi-walled carbon nanotubes (MWCNTs). Propranolol (PRO) was selected as the representative of beta-blocker. The effects of different environmental factors such as pH, ionic strength and humic acid (HA) on the adsorption process were investigated. The adsorption results were characterized by Zeta potential. At the same time, the effects of different types of drugs on the adsorption process were explored and the possible adsorption mechanisms were analyzed. The experimental results showed that the adsorption behavior was significantly different under different pH conditions. ?-? EDA interaction, hydrophobic interaction and hydrogen bonding were speculated to be the main adsorption mechanisms for PRO adsorption on MWCNTs.

| S-EPMC7314780 | biostudies-literature

Thermoelectric properties of sorted semiconducting single-walled carbon nanotube sheets.

Project description:Single-walled carbon nanotubes (SWNTs), especially their semiconducting type, are promising thermoelectric (TE) materials due to their high Seebeck coefficient. In this study, the in-plane Seebeck coefficient (S), electrical conductivity (σ), and thermal conductivity (κ) of sorted semiconducting SWNT (s-SWNT) free-standing sheets with different s-SWNT purities are measured to determine the figure of merit ZT. We find that the ZT value of the sheets increases with increasing s-SWNT purity, mainly due to an increase in Seebeck coefficient while the thermal conductivity remaining constant, which experimentally proved the superiority of the high purity s-SWNT as TE materials for the first time. In addition, from the comparison between sorted and unsorted SWNT sheets, it is recognized that the difference of ZT between unsorted SWNT and high-purity s-SWNT sheet is not remarkable, which suggests the control of carrier density is necessary to further clarify the superiority of SWNT sorting for TE applications.

| S-EPMC6454402 | biostudies-literature

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