Electronic Structure of Nanoribbons

The primary reason why I investigate graphene nanoribbons is because of their unique electronic properties. These properties, such as high charge carrier mobility and tunable band gap add to their inherently fascinating property of being the flattest stable material known. Together, these characteristics have rightfully given GNRs the status of candidates for next-generation nanoelectronics. We are working towards a future of transistors, diodes, resistors, logic devices that are even smaller, even more sustainable with a lower heat output and much faster than we can achieve in silicon.


Because of their unbelievably tiny size, GNR's electronic properties emerge directly from the laws of quantum mechanics. More accurately, graphene nanoribbons embrace the definition of nanoscience, where in its confined dimensions the laws of quantum mechanics dominate, whereas mesoscopic charge transport may hold sway in the unconfined directions.


In addition to band gap tuning (with implications to transistor performance) we have, as a field, recently ventured into the realm of spin physics and magnetism. We are starting to master not only the transport of charge carriers, but also their localization. We use tools based on concepts of symmetry and topology to hold electrons in place. We hope to elevate these concepts to full-blown spintronic devices or memory cells.


In my previous work, I have investigated the effect of straining graphene nanoribbons on the electronic structure.[1] We have made new types of heterostructure graphene nanoribbons that function as electronic components like tunnel diodes.[2] And importantly, we have developed new tools in characterizing the charge transport through various types of graphene nanoribbons.[3,4]

We have made nitrogen core-doped graphene nanoribbons. In these GNRs, the nitrogen atoms are forced into positions that are normally occupied by carbon atoms. The valence mismatch causes the nitrogen atoms to shed their electrons, with some electrons being absorbed by the gold substrate and the others behaving as little magnets. Although screened by magnetic interactions of electrons in the gold through the Kondo effect (making the GNR a Kondo lattice), interactions between neighboring spins are revealed when the nanoribbons are slightly peeled off the surface.[5]

We have studied the intricacies of charge transport through graphene nanoribbons both in STM lifting conductance measurements (where we attach the tip to the GNR end and lift it off the surface) and in quantum mechanical modelling. In doing so, we have laid bare the intricate interplay between eigenstate localization, charge distribution, topology, magnetism, and emergent negative differential resistance. Our work lays a blueprint to engineering nanoribbons with desired behavior for nanoelectronics.[4]

We have recently explored the synthesis and the electronic structure of a new type of graphene nanoribbon: the cyclobutadienoid GNR. In addition to the usual carbon hexagons, this ribbon features carbon tetragons, or four-membered rings. These highly unusual motifs are associated with chemical reactivity (which makes their synthesis challenging) but new electronic behavior as well. In our collaboration with the group of Colin Nuckolls as Columbia University, we reveal not only the successful preparation of such nanoribbons, but we also reveal a general blueprint for quantum engineering electronic properties based on these four-membered rings as new functional elements.[6]

The electronic structure and quantum mechanical wave functions inside graphene nanoribbons satisfy numerous interesting fundamental symmetries. Having knowledge of the interplay of the structure of a nanoribbon and electronic behavior is important to rationally design electronic components with well-defined functionality. Our collaborators from the group of Steven Louie discovered that modulating the width of a graphene nanoribbon in a well-defined way necessarily gives rise to localized electronic states, which can be explained in the mathematical framework of topology. We have used this insight to create quantum dots inside graphene nanoribbons: structures in which we have captured a number of electrons in the center section.[7]

Publications

  1. Bending and Buckling of Narrow Armchair Graphene Nanoribbons via STM Manipulation. Joost van der Lit, Peter H. Jacobse, Daniel Vanmaekelbergh, Ingmar Swart, New Journ. of Phys. 17 (2015)

  2. Electronic Components Embedded in a Single Graphene Nanoribbons. Peter H. Jacobse, Amina Kimouche, Tim Gebraad, Mikko M. Ervasti, Joseph M. Thijssen, Peter Liljeroth, Ingmar Swart, Nat. Comm. 8 (2017)

  3. Mapping the Conductance of Electronically Decoupled Graphene Nanoribbons. Peter H. Jacobse, Mark J. J. Mangnus, Stephan J. M. Zevenhuizen, Ingmar Swart, ACS Nano 12 (2018)

  4. Charge transport in topological graphene nanoribbons and nanoribbon heterostructures. Mark J. J. Mangnus, Felix R. Fischer, Michael F. Crommie, Ingmar Swart, Peter H. Jacobse, Phys. Rev. B 105 (2022)

  5. Magnetic Interactions in Substitutional Core Doped Graphene Nanoribbons. Ethan C. H. Wen, Peter H. Jacobse, Jingwei Jiang, Ziyi Wang, Ryan D. McCurdy, Steven G. Louie, Michael F. Crommie, Felix R. Fischer, J. Am. Chem. Soc. 144 (2022)

  6. Pseudo-atomic orbital behavior in graphene nanoribbons with four-membered rings. Peter H. Jacobse, Zexin Jin, Jingwei Jiang, Samuel Peurifoy, Ziqin Yue, Ziyi Wang, Daniel J. Rizzo, Steven G. Louie, Colin Nuckolls, Michael F. Crommie, Sci. Adv. 7 (2021)

  7. Rationally Designed Topological Quantum Dots in Bottom-Up Graphene Nanoribbons. Daniel J. Rizzo, Jingwei Jiang, Dharati Joshi, Gregory Veber, Christopher Bronner, Rebecca A. Durr, Peter H. Jacobse, Ting Cao, Alin Kalayjian, Henry Rodriguez, Paul Butler, Ting Chen, Steven G. Louie, Felix R. Fischer, Michael F. Crommie, ACS Nano 15 (2021)