Conformational Tuning of Magnetic Interactions in Coupled Nanographenes

IF 9.6 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2024-09-30 DOI:10.1021/acs.nanolett.4c03518

Gonçalo Catarina, Elia Turco, Nils Krane, Max Bommert, Andres Ortega-Guerrero, Oliver Gröning, Pascal Ruffieux, Roman Fasel, Carlo A. Pignedoli

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Abstract

Phenalenyl (C₁₃H₉) is an open-shell spin-1/2 nanographene. Using scanning tunneling microscopy (STM) inelastic electron tunneling spectroscopy (IETS), covalently bonded phenalenyl dimers have been shown to feature conductance steps associated with singlet–triplet excitations of a spin-1/2 dimer with antiferromagnetic exchange. Here, we address the possibility of tuning the magnitude of the exchange interactions by varying the dihedral angle between the two molecules within a dimer. Theoretical methods ranging from density functional theory calculations to many-body model Hamiltonians solved within different levels of approximation are used to explain STM-IETS measurements of phenalenyl dimers on a hexagonal boron nitride (h-BN)/Rh(111) surface, which exhibit signatures of twisting. By means of first-principles calculations, we also propose strategies to induce sizable twist angles in surface-adsorbed phenalenyl dimers via functional groups, including a photoswitchable scheme. This work paves the way toward tuning magnetic couplings in carbon-based spin chains and two-dimensional lattices.

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耦合纳米石墨烯中磁性相互作用的构象调谐

苯戊烯（C13H9）是一种开壳自旋-1/2 纳米锗。利用扫描隧道显微镜（STM）非弹性电子隧道光谱（IETS），共价键合的苯丙烯基二聚体被证明具有与自旋-1/2 二聚体的单三重激发和反铁磁交换相关的电导阶跃。在此，我们探讨了通过改变二聚体中两个分子之间的二面角来调整交换相互作用大小的可能性。从密度泛函理论计算到在不同近似水平下求解的多体模型哈密顿，这些理论方法都被用来解释在六方氮化硼（h-BN）/Rh(111)表面上对苯亚甲基二聚体进行的 STM-IETS 测量。通过第一原理计算，我们还提出了通过官能团诱导表面吸附的苯亚甲基二聚体产生可观扭转角的策略，包括一种光开关方案。这项工作为调整碳基自旋链和二维晶格中的磁耦合铺平了道路。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.