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Title: Atomically Defined Edge-Doping of Graphene Nanoribbons for Mesoscale Electronics

Abstract

The outstanding transformative potential of graphene, an infinite two-dimensional sheet of carbon atoms tightly packed into a honeycomb lattice, has been recognized mostly due to its exceptionally high electric conductivity, thermal conductivity, and tensile strength. These undeniably very desirable properties, however, represent only a very small facet of the true potential of all-sp2 carbon materials and its promise to revolutionize the field of molecular electronics. Graphene's most unusual characteristics emerge when the infinite macroscopic sheet is scaled down to nanometer dimensions. The exploration, realization, and implementation of these truly exotic magnetic and electronic properties rely on the development of innovative synthetic strategies that provide atomically precise control over the self-assembly of mesoscale objects. While traditional device architectures based on inorganic semiconductors have been fabricated using a top-down approach, we pursued a diametrically opposite strategy. Our design of a new generation of high-performance electronic materials relies on a modular bottom-up strategy. This highly multidisciplinary research program has been rooted in the synthesis of functional organic materials with precisely defined properties, their controlled assembly into hierarchical structures, and the evaluation of their performance at the molecular and the macroscopic scale. A part of this research program we have developed the chemical toolsmore » required to synthesize and to fine-tune the physical properties of graphene nanoribbons (GNR) with atomic precision. We further demonstrated that the innovative techniques and the expanded knowledge can be used to rationally tailor desired physical properties and function into nanometer-scale carbon-based electronic devices; e.g. transistors as logic gates in computing, data storage media based on electrically gated spin valves, or molecular amplifiers, all functionally integrated in atomically defined GNRs. • We demonstrated the design and experimental realization of a rationally engineered graphene nanoribbon superlattice that hosts a 1D array of symmetry-protected topological states. • We developed a hierarchical bottom-up fabrication strategy for graphene nanoribbons that preferentially exhibit a single heterojunction interface rather than a random statistical sequence of junctions along the ribbon. • We reported the bottom-up synthesis of a series of atomically precise graphene nanoribbons featuring trigonal planar heteroatom dopants (nitrogen, oxygen, and sulfur) along the edges that induce a narrowing of the intrinsic band gap by ~0.2–0.3 eV per dopant atom. • We reported the bottom-up synthesis of a graphene nanoribbon heterostructure featuring a highly tunable porphyrin quantum dot embedded at the center of a solution processable graphene nanoribbon. • We reported a new technique for fabricating bottom-up graphene nanoribbon heterojunctions through a late-stage chemical transformation that results in atomically sharp heterojunction structures from a single precursor. • We demonstrated the intrinsic performance enhancement of a composite material comprised of gold nanoparticles (AuNPs) embedded in a bottom-up synthesized graphene nanoribbon matrix for the electrocatalytic reduction of CO2. • We developed a scalable, solution-based approach toward the synthesis of an exotic class of polycyclic aromatic hydrocarbons that exhibit unusual electronic and magnetic properties in the ground state. • We reported the bottom-up synthesis and characterization of atomically-defined graphene nanoribbons featuring a regioregular pattern of group III dopant atoms (boron) along the backbone of the ribbon.« less

Authors:
ORCiD logo [1];  [2];  [2];  [2];  [2];  [2];  [2];  [2];  [2];  [2]
  1. Department of Chemistry, University of California Berkeley, Berkeley, California 94720, United States; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States; Kavli Energy Nanosciences Institute at the University of California Berkeley and Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States
  2. Department of Chemistry, University of California Berkeley, Berkeley, California 94720, United States;
Publication Date:
Research Org.:
Univ. of California, Oakland, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1542610
Report Number(s):
Final Report: DOE-CAL-DE-SC-0010409
DOE Contract Number:  
SC0010409
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Graphene Nanoribbons, Bottom-up, Orgamic Semiconductors

Citation Formats

Fischer, Felix, Haberer, Danny, Marangoni, Tomas, Toma, Francesca, Veber, Gregory, Joshi, Dharati, Cloke, Ryan, Durr, Rebecca, Perkins, Wade, and Rogers, Cameron. Atomically Defined Edge-Doping of Graphene Nanoribbons for Mesoscale Electronics. United States: N. p., 2019. Web. doi:10.2172/1542610.
Fischer, Felix, Haberer, Danny, Marangoni, Tomas, Toma, Francesca, Veber, Gregory, Joshi, Dharati, Cloke, Ryan, Durr, Rebecca, Perkins, Wade, & Rogers, Cameron. Atomically Defined Edge-Doping of Graphene Nanoribbons for Mesoscale Electronics. United States. doi:10.2172/1542610.
Fischer, Felix, Haberer, Danny, Marangoni, Tomas, Toma, Francesca, Veber, Gregory, Joshi, Dharati, Cloke, Ryan, Durr, Rebecca, Perkins, Wade, and Rogers, Cameron. Tue . "Atomically Defined Edge-Doping of Graphene Nanoribbons for Mesoscale Electronics". United States. doi:10.2172/1542610. https://www.osti.gov/servlets/purl/1542610.
@article{osti_1542610,
title = {Atomically Defined Edge-Doping of Graphene Nanoribbons for Mesoscale Electronics},
author = {Fischer, Felix and Haberer, Danny and Marangoni, Tomas and Toma, Francesca and Veber, Gregory and Joshi, Dharati and Cloke, Ryan and Durr, Rebecca and Perkins, Wade and Rogers, Cameron},
abstractNote = {The outstanding transformative potential of graphene, an infinite two-dimensional sheet of carbon atoms tightly packed into a honeycomb lattice, has been recognized mostly due to its exceptionally high electric conductivity, thermal conductivity, and tensile strength. These undeniably very desirable properties, however, represent only a very small facet of the true potential of all-sp2 carbon materials and its promise to revolutionize the field of molecular electronics. Graphene's most unusual characteristics emerge when the infinite macroscopic sheet is scaled down to nanometer dimensions. The exploration, realization, and implementation of these truly exotic magnetic and electronic properties rely on the development of innovative synthetic strategies that provide atomically precise control over the self-assembly of mesoscale objects. While traditional device architectures based on inorganic semiconductors have been fabricated using a top-down approach, we pursued a diametrically opposite strategy. Our design of a new generation of high-performance electronic materials relies on a modular bottom-up strategy. This highly multidisciplinary research program has been rooted in the synthesis of functional organic materials with precisely defined properties, their controlled assembly into hierarchical structures, and the evaluation of their performance at the molecular and the macroscopic scale. A part of this research program we have developed the chemical tools required to synthesize and to fine-tune the physical properties of graphene nanoribbons (GNR) with atomic precision. We further demonstrated that the innovative techniques and the expanded knowledge can be used to rationally tailor desired physical properties and function into nanometer-scale carbon-based electronic devices; e.g. transistors as logic gates in computing, data storage media based on electrically gated spin valves, or molecular amplifiers, all functionally integrated in atomically defined GNRs. • We demonstrated the design and experimental realization of a rationally engineered graphene nanoribbon superlattice that hosts a 1D array of symmetry-protected topological states. • We developed a hierarchical bottom-up fabrication strategy for graphene nanoribbons that preferentially exhibit a single heterojunction interface rather than a random statistical sequence of junctions along the ribbon. • We reported the bottom-up synthesis of a series of atomically precise graphene nanoribbons featuring trigonal planar heteroatom dopants (nitrogen, oxygen, and sulfur) along the edges that induce a narrowing of the intrinsic band gap by ~0.2–0.3 eV per dopant atom. • We reported the bottom-up synthesis of a graphene nanoribbon heterostructure featuring a highly tunable porphyrin quantum dot embedded at the center of a solution processable graphene nanoribbon. • We reported a new technique for fabricating bottom-up graphene nanoribbon heterojunctions through a late-stage chemical transformation that results in atomically sharp heterojunction structures from a single precursor. • We demonstrated the intrinsic performance enhancement of a composite material comprised of gold nanoparticles (AuNPs) embedded in a bottom-up synthesized graphene nanoribbon matrix for the electrocatalytic reduction of CO2. • We developed a scalable, solution-based approach toward the synthesis of an exotic class of polycyclic aromatic hydrocarbons that exhibit unusual electronic and magnetic properties in the ground state. • We reported the bottom-up synthesis and characterization of atomically-defined graphene nanoribbons featuring a regioregular pattern of group III dopant atoms (boron) along the backbone of the ribbon.},
doi = {10.2172/1542610},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2019},
month = {7}
}