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Ultimate Charge Transport Regimes in Doping-Controlled Graphene Laminates: Phonon-Assisted Processes Revealed by the Linear Magnetoresistance.

ABSTRACT: Understanding and controlling the electrical properties of solution-processed 2D materials is key to further printed electronics progress. Here, we demonstrate that the thermolysis of the aromatic intercalants utilized in nanosheet exfoliation for graphene laminates allows for high intrinsic mobility and the simultaneous control of doping type (n- and p-) and concentration over a wide range. We establish that the intraflake mobility is high by observing a linear magnetoresistance of such solution-processed graphene laminates and using it to devolve the interflake tunneling and intralayer magnetotransport. Consequently, we determine the temperature dependencies of the inter- and intralayer characteristics. The intraflake transport appears to be dominated by electron-phonon scattering processes at temperatures T > 20 K, while the interflake transport is governed by phonon-assisted tunneling. In particular, we identify the efficiency of phonon-assisted tunneling as the main limiting factor for electrical conductivity in graphene laminates at room temperature. We also demonstrate a thermoelectric sensitivity of around 50 μV·K^-1 in a solution-processed metal-free graphene-based thermocouple.

SUBMITTER: Moazzami Gudarzi M

PROVIDER: S-EPMC11342362 | biostudies-literature | 2024 Aug

REPOSITORIES: biostudies-literature

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Ultimate Charge Transport Regimes in Doping-Controlled Graphene Laminates: Phonon-Assisted Processes Revealed by the Linear Magnetoresistance.

Moazzami Gudarzi Mohsen M Slizovskiy Sergey S Mao Boyang B Tovari Endre E Pinter Gergo G Sanderson David D Asaad Maryana M Xiang Ying Y Wang Zhiyuan Z Guo Jianqiang J Spencer Ben F BF Geim Alexandra A Fal'ko Vladimir I VI Kretinin Andrey V AV

ACS nano 20240808 33

Understanding and controlling the electrical properties of solution-processed 2D materials is key to further printed electronics progress. Here, we demonstrate that the thermolysis of the aromatic intercalants utilized in nanosheet exfoliation for graphene laminates allows for high intrinsic mobility and the simultaneous control of doping type (<i>n</i>- and <i>p</i>-) and concentration over a wide range. We establish that the intraflake mobility is high by observing a linear magnetoresistance o ...[more]

PMID: 39116121

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Project description:We have established a design to increase the absorption capacity, optoelectronic, linear and nonlinear optical properties of the graphene oxide nanosheet (GON) based on the coronene molecule [C24H12] with the help of doping, using the aluminum atom. The attachment of functional groups to the coronene surface was defined according to the Lerf-Klinowski model, based on experimental predictions [1]. Two GON structures (GON1 and GON2 with formula (C24H11)(O)(OH)COOH)) have been proposed for this purpose, and it should be noted that each of them is distinguished by a different distribution of functional groups within their honeycomb lattice. A series of substitutions of the carbon atoms of the two isomers considered GON1 and GON2 were performed with the aluminum atom, resulting in the abbreviated derivative systems GON1-Alx and GON2-Alx (x = 1-6), respectively to each of the GON1 and GON2 units. In this work, we provide data carried out in the gas phase, from density functional theory (DFT) methods that allowed us to understand the effects of aluminum atom doping on the circular graphene oxide nanosheets. First, we report the wavenumber data related to the IR spectrum peak characteristics computed at the B3LYP, B3LYP-D3 and ωB97XD/6-31+G(d,p) levels of theory, that allowed us to validate the designs of both proposed graphene oxide models. Then, we provide electronic, reactivity, optoelectronic, linear and nonlinear optical data parameters of both graphene oxide nanosheets and their aluminum-doped derivatives computed at the B3LYP, B3LYP-D3 and /6-31+G(d,p) levels of theory. Finally the UV-vis spectra of the investigated compounds evaluated from time-dependent (TD) B3LYP and B3LYP-D3/6-31+G(d,p) levels of theory and the HOMO & LUMO orbitals of the derivatives of graphene oxide isomers computed at the B3LYP/6-31+G(d,p) level of theory are provided. In addition, the raw data of UV-vis spectra, optoelectronic parameters, Cartesian coordinates of all studied compounds and also those of IR spectra of both studied graphene oxide models are provided as supplementary file. The data reported in this work are useful to expose some specific positions of aluminum within circular model of graphene oxide nanosheet that improve its electronic, reactive, optoelectronic, linear and nonlinear optical characteristics. All the formulas and details of calculation performed to obtain the data reported in this work are provided in our previous work (Foadin et al., 2020) and summarized in the experimental section of this paper. To learn more about the ideal doping positions of the aluminum atom within both proposed graphene oxide designs that increase their electronic, reactivity, optoelectronic, linear optical and nonlinear optical properties, respectively, please see the corresponding main research paper (Foadin et al., 2022).

Dataset Information

Ultimate Charge Transport Regimes in Doping-Controlled Graphene Laminates: Phonon-Assisted Processes Revealed by the Linear Magnetoresistance.

Publications

Ultimate Charge Transport Regimes in Doping-Controlled Graphene Laminates: Phonon-Assisted Processes Revealed by the Linear Magnetoresistance.

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