Abstract

Single molecular systems are typical quantum confinement systems, which have rich electronic states, photon states and spin states due to their discrete energy levels, localized orbitals and diverse chemical structures. The states determined by quantum mechanics in these molecular systems make it possible to serve as great physical entities for future quantum information technology. The detection and manipulation of quantum states on a single molecule scale are beneficial to the bottom-up construction of quantum devices. Owing to the highly limited spatial localization of single molecular systems, it is difficult to accurately address and manipulate them with conventional macroscopic characterization methods. Scanning tunneling microscope (STM) is such a powerful tool that it can achieve high-resolution real-space imaging as well as spectroscopic investigation, with the ability to <i>in-situ</i> manipulating the individual atoms or molecules. It can also work jointly with various near-field or external field characterization techniques, making it a most important technique for precisely detecting and manipulating quantum properties at a single molecule level. In this paper, we review recent research progress of quantum states of surface-supported single molecules and relevant structures based on scanning tunneling microscopy. We start from the methods for the synthesis of molecular structures with desired quantum states, and then we review the recent advances in the local spin states for single molecular systems and the optical properties of single molecules serving as a single-photon source. An emerging family of molecular nanographene systems showing intriguing topological properties and magnetic properties is also reviewed. In the last part, we summarize the research progress made recently and prospect the future development of the quantum states at a single molecular level.

Highlights

  • Hydrogen atoms 2 and 3 of one lobe were dissociated in the experiments. (b) Diagram of the dehydrogenation induced by the Scanning tunneling microscope (STM) current. (c) dI/dV spectra of CoPc and dehydrogenated CoPc (d-CoPc) at different temperatures. (d) STM images showing the sequential tip-induced dehydrogenation of a CoPc on Au(111)[48]. 2.2 表面分子原位合成 STM 原位操纵虽然可以非常有目的的针对特定的局域化学键和基团进行操

  • Synthetic strategy to produce chGNRs combining solution and on-surface synthesis.(a–d)Solution synthesis protocols for producing molecular precursors1,2,3, for the synthesis of 3,1,w-chGNRs with different widths, and precursor 4 for 3,2,8chGNRs. (e–h) Targeted chemical structures of chGNRs by using the four molecular precursors in a–d, respectively. (i–l) STM overview images of the chGNRs formed on a Au(111) surface[59]

  • 图 5 (a) 针尖增强光致发光实验模型。(b) ZnPC 分子的 STM 图(左)和光子图 (右)。(c) 在光子图像(b)中虚白线 A-B 的光子强度侧面图[85]。(d) STM-PL 实验 示意图。(e) H2Pc 分子的放大 STM 图,STM 图(左)中的圆圈显示的是光谱 测量时针尖的位置,其颜色与相应光谱的颜色匹配[86]。 Fig.5. (a) Schematic of the experimental of Sub-nanometre-resolved single-molecule TEPL.(b)Simultaneously recorded STM image and TEPL photon image of a single ZnPc molecule.(c)Photon intensity profile for the dashed white line A–B in the photon image in b(right)[85](. d)Schematic depiction of STM-PL measurement. (e)A magnified STM image of a H2Pc molecule,The measurement tip positions for the spectra shown in STM image(left)are indicated with circles whose color matches that of the corresponding spectrum[86]

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Summary

Introduction

(b) Diagram of the dehydrogenation induced by the STM current. (d) STM images showing the sequential tip-induced dehydrogenation of a CoPc on Au(111)[48]. (i–l) STM overview images of the chGNRs formed on a Au(111) surface[59]. Electroluminescence spectra from a single H2Pc molecule at different bias voltages. (e)A magnified STM image of a H2Pc molecule,The measurement tip positions for the spectra shown in STM image(left)are indicated with circles whose color matches that of the corresponding spectrum[86].

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