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Shigehiro Yamaguchi

Publications and source records attributed to Shigehiro Yamaguchi.

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Bridging Pico-to-Nanonewtons with a Ratiometric Force Probe for Monitoring Nanoscale Polymer Physics Before Damage

Understanding the transmission of nanoscale forces in the pico-to-nanonewton range is important in polymer physics. While physical approaches have limitations in analyzing the local force distribution in condensed environments, chemical analysis using force probes is promising. However, there are stringent requirements for probing the local forces generated before structural damage. The magnitude of those forces corresponds to the range below covalent bond scission (from 200 pN to several nN) and above thermal fluctuation (several pN). Here, we report a conformationally flexible dual-fluorescence force probe with a theoretically estimated threshold of approximately 100 pN. This probe enables ratiometric analysis of the distribution of local forces in a stretched polymer chain network. Without changing the intrinsic properties of the polymer, the force distribution was reversibly monitored in real time. Chemical control of the probe location demonstrated that the local stress concentration is twice as biased at crosslinkers than at main chains, particularly in a strain-hardening region. Due to the high sensitivity, the percentage of stressed force probes was estimated to be more than 1000 times higher than the activation rate of a conventional mechanophore.

cond-mat.soft

Magnetism of topological boundary states induced by boron substitution in graphene nanoribbons

Graphene nanoribbons (GNRs), low-dimensional platforms for carbon-based electronics, show the promising perspective to also incorporate spin polarization in their conjugated electron system. However, magnetism in GNRs is generally associated to localized states around zigzag edges, difficult to fabricate and with high reactivity. Here we demonstrate that magnetism can also be induced away from physical GNR zigzag edges through atomically precise engineering topological defects in its interior. A pair of substitutional boron atoms inserted in the carbon backbone breaks the conjugation of their topological bands and builds two spin-polarized boundary states around. The spin state was detected in electrical transport measurements through boron-substituted GNRs suspended between tip and sample of a scanning tunneling microscope. First-principle simulations find that boron pairs induce a spin 1, which is modified by tuning the spacing between pairs. Our results demonstrate a route to embed spin chains in GNRs, turning them basic elements of spintronic devices.

cond-mat.mes-hall

Electronic Properties of Substitutionally Boron-doped Graphene Nanoribbons on a Au(111) Surface

High quality graphene nanoribbons (GNRs) grown by on-surface synthesis strategies with atomic precision can be controllably doped by inserting heteroatoms or chemical groups in the molecular precursors. Here, we study the electronic structure of armchair GNRs substitutionally doped with di-boron moieties at the center, through a combination of scanning tunneling spectroscopy, angle-resolved photoemission, and density functional theory simulations. Boron atoms appear with a small displacement towards the surface signaling their stronger interaction with the metal. We find two boron-rich flat bands emerging as impurity states inside the GNR band gap, one of them particularly broadened after its hybridization with the gold surface states. In addition, the boron atoms shift the conduction and valence bands of the pristine GNR away from the gap edge, and leave unaffected the bands above and below, which become the new frontier bands and have negligible boron character. This is due to the selective mixing of boron states with GNR bands according to their symmetry. Our results depict that the GNRs band structure can be tuned by modifying the separation between di-boron moieties.

cond-mat.mes-hall