Rationally Designed Topological Quantum Dots in Bottom-Up Graphene Nanoribbons

Rizzo, Daniel J.; Jiang, Jingwei; Joshi, Dharati; Veber, Gregory; Bronner, Christopher; Durr, Rebecca A.; Jacobse, Peter H.; Cao, Ting; Kalayjian, Alin Miksi; Rodriguez, Henry; Butler, Paul; Chen, Ting; Louie, Steven G.; Fischer, Felix R.; Crommie, Michael F.

doi:10.1021/acsnano.1c09503

Cited by 30 publications

(46 citation statements)

References 41 publications

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“…Chirality in 2D materials has spanned diverse compounds and structures, including graphene quantum dots (GQDs), nanodisks, and nanoribbons, − nanoplatelets of CdSe, MoS 2 layers, colloidal semiconductor quantum wells of different types, and transition-metal dichalcogenide semimetals . One of the earliest systems to show chiral properties in strictly 2D was graphene flakes or QDs (GQD) covalently modified by l - or d -cysteine moieties .…”

Section: Chiral Light–matter Interactionsmentioning

confidence: 99%

A Chirality-Based Quantum Leap

Aiello¹,

Abbas²,

Abendroth³

et al. 2022

ACS Nano

108

126

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There is increasing interest in the study of chiral degrees of freedom occurring in matter and in electromagnetic fields. Opportunities in quantum sciences will likely exploit two main areas that are the focus of this Review: (1) recent observations of the chiral-induced spin selectivity (CISS) effect in chiral molecules and engineered nanomaterials and (2) rapidly evolving nanophotonic strategies designed to amplify chiral light–matter interactions. On the one hand, the CISS effect underpins the observation that charge transport through nanoscopic chiral structures favors a particular electronic spin orientation, resulting in large room-temperature spin polarizations. Observations of the CISS effect suggest opportunities for spin control and for the design and fabrication of room-temperature quantum devices from the bottom up, with atomic-scale precision and molecular modularity. On the other hand, chiral–optical effects that depend on both spin- and orbital-angular momentum of photons could offer key advantages in all-optical and quantum information technologies. In particular, amplification of these chiral light–matter interactions using rationally designed plasmonic and dielectric nanomaterials provide approaches to manipulate light intensity, polarization, and phase in confined nanoscale geometries. Any technology that relies on optimal charge transport, or optical control and readout, including quantum devices for logic, sensing, and storage, may benefit from chiral quantum properties. These properties can be theoretically and experimentally investigated from a quantum information perspective, which has not yet been fully developed. There are uncharted implications for the quantum sciences once chiral couplings can be engineered to control the storage, transduction, and manipulation of quantum information. This forward-looking Review provides a survey of the experimental and theoretical fundamentals of chiral-influenced quantum effects and presents a vision for their possible future roles in enabling room-temperature quantum technologies.

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Section: Chiral Light–matter Interactionsmentioning

confidence: 99%

A Chirality-Based Quantum Leap

Aiello¹,

Abbas²,

Abendroth³

et al. 2022

ACS Nano

108

126

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“…The different N‐doping sites are marked in cyan and blue, respectively. The d I /d V spectrum in Figure 3d acquired at the position marked by the red dot in Figure 3a reveals two prominent peaks at the energy of −350 mV and 1400 mV, which exhibits a slightly wider band gap than that of the pristine 9‐AGNRs (−300 mV and 1100 mV) reported previously [6, 40] . Band structure calculations for pristine 9‐AGNRs and N‐9‐AGNR (C−C) are shown in Figures 3e and f, respectively.…”

Section: Figurementioning

confidence: 63%

On‐Surface Synthesis of a Nitrogen‐Doped Graphene Nanoribbon with Multiple Substitutional Sites

Zhang

et al. 2022

Angewandte Chemie

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Doped graphene nanoribbons (GNRs) with heteroatoms are a principal strategy to fine-tune the electronic structures of GNRs for future device applications. Here, we successfully synthesized the N = 9 nitrogen-doped armchair GNR on the Au(111) surface. Due to the flexibility of precursor molecules, three different covalent bonds (CÀ C, CÀ N, NÀ N) are formed in the GNR backbone. Scanning tunneling spectroscopy analysis together with band structure calculations reveals that the band gap of the N-9-AGNRs (CÀ C) will be enlarged compared to pristine 9-AGNRs, and the CÀ N bond and NÀ N bond at the isolated site of N-9-AGNR (CÀ C) will introduce new defect states near the Fermi level. DFT calculations reveal that the electronic structure of N-9-AGNR (CÀ C) shows semiconductor character, while N-9-AGNR (CÀ N) and N-9-AGNR (NÀ N) display metallic character. Our results provide a promising route for creating more complex molecular heterostructures with tunable band gaps, which may be useful for future molecular electronics and memory device applications.

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“…Note that t eff increases with an increased tail of the end state and may therefore be thought to be inversely proportional to the bandgap. Here, t eff is more strongly correlated to the inverse width of the GNR, as the end states in wider GNRs localize more strongly on the zigzag edges than expected purely based on a simple bandgap argument [110]. Nevertheless, the parameters U eff and t eff can still be extracted empirically, and the effective Hubbard model is always valid.…”

Section: Understanding the Magnetic Phase Transitionmentioning

confidence: 89%