Tuning charge and correlation effects for a single molecule on a graphene device

Wickenburg, Sebastian; Lu, Jiong; Lischner, Johannes; Tsai, Hsin‐Zon; Omrani, Arash A.; Riss, Alexander; Karrasch, Christoph; Bradley, Aaron J.; Jung, Han Sae; Khajeh, Ramin; Wong, Dillon; Watanabe, Kenji; Taniguchi, Takashi; Zettl, Alex; Neto, A. H. Castro; Louie, Steven G.; Crommie, Michael F.

doi:10.1038/ncomms13553

Cited by 92 publications

(103 citation statements)

References 54 publications

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“…First, organic molecules can prompt doping effects in 2D materials16171819, causing local modifications of their surface potential202122. Second, these molecules form ordered 2D crystalline structures when physisorbed on graphene and other 2D materials23242526272829303132333435.…”

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Periodic potentials in hybrid van der Waals heterostructures formed by supramolecular lattices on graphene

et al. 2017

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The rise of 2D materials made it possible to form heterostructures held together by weak interplanar van der Waals interactions. Within such van der Waals heterostructures, the occurrence of 2D periodic potentials significantly modifies the electronic structure of single sheets within the stack, therefore modulating the material properties. However, these periodic potentials are determined by the mechanical alignment of adjacent 2D materials, which is cumbersome and time-consuming. Here we show that programmable 1D periodic potentials extending over areas exceeding 104 nm2 and stable at ambient conditions arise when graphene is covered by a self-assembled supramolecular lattice. The amplitude and sign of the potential can be modified without altering its periodicity by employing photoreactive molecules or their reaction products. In this regard, the supramolecular lattice/graphene bilayer represents the hybrid analogue of fully inorganic van der Waals heterostructures, highlighting the rich prospects that molecular design offers to create ad hoc materials.

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Periodic potentials in hybrid van der Waals heterostructures formed by supramolecular lattices on graphene

et al. 2017

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“…[10,49,66,67] Auch das STM hat diese Option, [68] aber mit AFM kann man zusätzlich die Adsorptionshçhe genau messen; [49] wegen der unebenen Topographie und elektronischer Effekte ist dies mit der STM nicht mçglich. In atomar auflçsenden Aufnahmen von Substrat und Molekül kann man die Position der Adsorption des Moleküls und die Ausrichtung in der Ebene auf dem Substrat studieren.…”

Section: Adsorptionsgeometrieunclassified

Rasterkraftmikroskopie für die molekulare Strukturaufklärung

et al. 2018

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Mit der Rastersondenmikroskopie kann man auf einer Oberfläche adsorbierte Moleküle individuell und mit hoher Auflösung untersuchen. Die Technik, die bei tiefen Temperaturen und im Ultrahochvakuum durchgeführt wird, liefert Informationen über Struktur, Konfiguration, Ladungszustand, Aromatizität und die Beteiligung von Resonanzstrukturen. Durch Funktionalisierung der Spitze eines Rasterkraftmikroskops mit einem CO‐Molekül können Einzelmoleküle mit atomarer Auflösung abgebildet werden, ihre Adsorptionsgeometrie kann gemessen und die Bindungsordnungen im Molekül können bestimmt werden. Mit der Rastertunnelmikroskopie und der Kelvinsondenkraftmikroskopie kann man zudem die Elektronendichte der molekularen Grenzorbitale bzw. die Ladungsverteilung innerhalb des Moleküls kartieren. In Kombination ergeben diese Methoden ein hochauflösendes Verfahren zur Identifizierung und Charakterisierung von Einzelmolekülen. Die Empfindlichkeit auf Einzelmoleküle sowie die Option, durch Manipulation von Atomen mit der Spitze des Mikroskops chemische Reaktionen auszulösen, eröffnen einzigartige chemische Anwendungsmöglichkeiten und heben die Rastersondenmikroskopie von den klassischen Methoden zur molekularen Strukturaufklärung heraus. Somit kann die Rasterkraftmikroskopie nicht nur bei der Identifizierung von schwer zu bestimmenden Naturstoffen helfen, sondern sie ist auch ein leistungsstarkes und besonders gut geeignetes Instrument, um Oberflächenreaktionen zu untersuchen und Radikale und molekulare Mischungen zu charakterisieren. In diesem Aufsatz zeigen wir auf, welche Entwicklung die hochauflösende Rastersondenmikroskopie mit funktionalisierter Spitze bei der molekularen Strukturaufklärung und ‐charakterisierung in den vergangenen Jahren genommen hat, und erörtern die Herausforderungen der kommenden Jahre.

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“…[9] However, isolating individual molecules is more challenging. [10] In contrast, new possibilities for templating emerge from nanostructuring that …”

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“…[9] However, isolating individual molecules is more challenging. [10] In contrast, new possibilities for templating emerge from nanostructuring that its atomistic structure. In particular, silicene on ZrB 2 occurs in a (√3 × √3)R30° reconstruction where five of the Si atoms per unit cell are essentially in a single plane, with the sixth Si atom protruding above the plane by 1.6 Å.…”

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Guided Molecular Assembly on a Locally Reactive 2D Material

et al. 2017

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occurs when 2D materials are placed on a substrate, such as when they are epitaxially grown upon a metallic surface. [11,12] For example, it has been shown that molecules can become trapped within nanopores of hexagonal boron nitride grown on Ru (0001) because of dipolar interactions; [13,14] similar results have also been observed for nanopores on the surface of bulk SiC. [15] Physisorption of a molecule to a surface (i.e., van der Waals bonding) is often not strong enough to fix the molecule's position at room temperature, particularly on the surface of bulk metal crystals. This is more readily accomplished by anchoring the mole cule to the surface through chemisorption of part of the molecule to the surface. [16][17][18] However, care must be taken to limit hybridization that can cause detrimental modifications of the molecule and its frontier orbitals, [19,20] especially on different surface reconstructions of bulk semiconductors like silicon. [15,17] It is therefore of interest to investigate the interface between molecules and more reactive 2D materials in an attempt to isolate individual molecules at room temperature while retaining their localized electronic states.With its mixed sp 2 -sp 3 character, silicene-the silicon analogue of graphene-has the potential to provide unique properties for molecular templating. This is particularly true because the structural and electronic properties of silicene are more susceptible to modification [21][22][23][24][25][26] once it is formed upon a surface, owing to its greater reactivity than graphene and the flexibility of The interactions between atomic or molecular adsorbates and the surfaces of 2D materials are of interest for applications ranging from catalysis [1] and molecular sensing [2] to molecular electronics and spintronics. [3][4][5] For the prototypical 2D material graphene, there are typically only weak van der Waals interactions between molecules and the surface. [6] This allows for the fabrication of functional self-assembled monolayers [6][7][8] that are reminiscent of the ordered supramolecular arrangements that can be formed on the surfaces of bulk (3D) materials. [9] However, isolating individual molecules is more challenging. [10] In contrast, new possibilities for templating emerge from nanostructuring that

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Tuning charge and correlation effects for a single molecule on a graphene device

Cited by 92 publications

References 54 publications

Periodic potentials in hybrid van der Waals heterostructures formed by supramolecular lattices on graphene

Periodic potentials in hybrid van der Waals heterostructures formed by supramolecular lattices on graphene

Rasterkraftmikroskopie für die molekulare Strukturaufklärung

Guided Molecular Assembly on a Locally Reactive 2D Material

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