Covalent 2D‐Engineering of Graphene by Spatially Resolved Laser Writing/Reading/Erasing

Edelthalhammer, Konstantin F.; Dasler, Daniela; Jurkiewicz, Lisa; Nagel, Thomas; Al-Fogra, Sabrin; Hauke, Frank; Hirsch, Andreas

doi:10.1002/anie.202006874

Cited by 30 publications

(47 citation statements)

References 40 publications

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“…The DBPO decomposed at around 80°C to aryl radicals, which subsequently attached the exposed surface of graphene, forming covalent patterns at the micrometer scale. Four years later, Edelthalhammer et al, (2020 ) modified the method by locally cleaving the DBPO compounds on a graphene substrate via laser-writing activation, achieving a pattering resolution of 2 μm. Surprisingly, the covalent functionalization process was totally reversible, which allowed the write/read/erase control over the covalent chemical information stored on the graphene surface.…”

Section: Covalent Patterning With Microscale Periodicitymentioning

confidence: 99%

Covalent Patterning of Graphene for Controllable Functionalization from Microscale to Nanoscale: A Mini-Review

et al. 2022

Front. Chem.

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Covalent patterning of graphene opens many application possibilities in the field of photonics, electronics, sensors, and catalysis due to order-dependent optical properties, band structure engineering, and processibility and reactivity improvement. Owing to the low reactivity of the graphene basal plane, harsh reagents (e.g., radicals) used for covalent functionalization normally result in poor spatial control, which largely compromises the intrinsic properties of graphene. Therefore, precisely spatial control on covalent patterning of graphene is of great importance. Herein, we summarize recent advances for covalent patterning of graphene from the microscale to nanoscale resolution using different techniques such as laser or electrochemical writing, template-directed growth, and tip-induced nanoshaving.

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Section: Covalent Patterning With Microscale Periodicitymentioning

confidence: 99%

Covalent Patterning of Graphene for Controllable Functionalization from Microscale to Nanoscale: A Mini-Review

et al. 2022

Front. Chem.

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“…In this regard, our group has recently carried out a related investigation in detail ( Figure ). [ 194 ] The best conditions that we identified for an efficient graphene functionalization are the irradiation of the graphene/functionality with a 532 nm laser with a power of 1.4 mW for 5 min. Under these optimized conditions a letter pattern of “FAU” was written on graphene.…”

Section: Chemical Patterningmentioning

confidence: 99%

Evolution of Graphene Patterning: From Dimension Regulation to Molecular Engineering

2021

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The realization that nanostructured graphene featuring nanoscale width can confine electrons to open its bandgap has aroused scientists’ attention to the regulation of graphene structures, where the concept of graphene patterns emerged. Exploring various effective methods for creating graphene patterns has led to the birth of a new field termed graphene patterning, which has evolved into the most vigorous and intriguing branch of graphene research during the past decade. The efforts in this field have resulted in the development of numerous strategies to structure graphene, affording a variety of graphene patterns with tailored shapes and sizes. The established patterning approaches combined with graphene chemistry yields a novel chemical patterning route via molecular engineering, which opens up a new era in graphene research. In this review, the currently developed graphene patterning strategies is systematically outlined, with emphasis on the chemical patterning. In addition to introducing the basic concepts and the important progress of traditional methods, which are generally categorized into top‐down, bottom‐up technologies, an exhaustive review of established protocols for emerging chemical patterning is presented. At the end, an outlook for future development and challenges is proposed.

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“…[ 23 ] At the same time, using benzoyl peroxides for the laser writing allow only for the establishment of relatively low degrees of functionalization—located in the low functionalization regime of the Cançado curve [ 24 ] —requiring also rather extended long irradiation periods. [ 10,11,22 ] Despite the relatively high degree of functionalization provided by the CYTOP polymer and silver trifluoroacetate, their post‐patterning removal remains a severe challenge, which is difficult to overcome when targeting the high standards for real applications of graphene nanoarchitectures. Specifically, the removal of polymer CYTOP requires not only a special stripper but also a very long time, [ 8 ] and the usage of silver trifluoroacetate unavoidably generates in situ conductive silver nanoparticles at the patterned areas, which restricts the applications, for example, in electronics.…”

Section: Introductionmentioning

confidence: 99%

Hypervalent Iodine Compounds as Versatile Reagents for Extremely Efficient and Reversible Patterning of Graphene with Nanoscale Precision

et al. 2021

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Rational patterning and tailoring of graphene relies on the disclosure of suitable reagents for structuring the target functionalities on the 2D‐carbon network. Here, a series of hypervalent iodine compounds, namely, 1‐chloro‐1,2‐benziodoxol‐3(1H)‐one, 1,3‐dihydro‐1‐hydroxy‐3,3‐dimethyl‐1,2‐benziodoxole, and 3,3‐dimethyl‐1‐(trifluoromethyl)‐1,2‐benziodoxole is reported to be extremely efficient for a diversified graphene patterning. The decomposition of these compounds generates highly reactive Cl, OH, and CF3 radicals exclusively in the irradiated areas, which subsequently attach onto the graphene leading to locally controlled chlorination, hydroxylation, and trifluoromethylation, respectively. This is the first realization of a patterned hydroxylation of graphene, and the degrees of functionalization of the patterned chlorination and trifluoromethylation are both unprecedented. The usage of these mild reagents here is reasonably facile compared to the reported methods using hazardous Cl2 or ICl and allows for sophisticated pattern designs with nanoscale precision, promising for arbitrary nanomanipulation of graphene's properties like hydrophilicity and conductivity by the three distinct functionalities (Cl, OH, and CF3). Moreover, the attachment of functional entities to these highly functionalized graphene nanoarchitectures is fully reversible upon thermal annealing, enabling a full writing/storing/reading/erasing control over the chemical information stored within graphene. This work provides an exciting clue for target 2D functionalization and modulation of graphene by using suitable hypervalent iodine compounds.

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Covalent 2D‐Engineering of Graphene by Spatially Resolved Laser Writing/Reading/Erasing

Cited by 30 publications

References 40 publications

Covalent Patterning of Graphene for Controllable Functionalization from Microscale to Nanoscale: A Mini-Review

Covalent Patterning of Graphene for Controllable Functionalization from Microscale to Nanoscale: A Mini-Review

Evolution of Graphene Patterning: From Dimension Regulation to Molecular Engineering

Hypervalent Iodine Compounds as Versatile Reagents for Extremely Efficient and Reversible Patterning of Graphene with Nanoscale Precision

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