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首页> 外文期刊>Journal of the American Chemical Society >First Observation of a Kondo Resonance for a Stable Neutral Pure Organic Radical, 1,3/5-Triphenyl-6-oxoverdazyl, Adsorbed on the Au(111) Surface
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First Observation of a Kondo Resonance for a Stable Neutral Pure Organic Radical, 1,3/5-Triphenyl-6-oxoverdazyl, Adsorbed on the Au(111) Surface

机译:吸附在Au(111)表面上的稳定中性纯有机自由基1,3 / 5-Triphenyl-6-oxoverdazyl的近藤共振的首次观察

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摘要

We investigated spin states of stable neutral pure-organic radical molecules of 1,3,5-triphenyl-6-oxoverdazyl (TOV) and 1,3,S-triphenyl-6-thioxoverdazly (TTV) adsorbed on an Au(111) surface, which appears as a Kondo resonance because of spin-electron interaction. By using scanning tunneling spectroscopy (STS), a clear Kondo resonance was detected for the TOV molecule. However, no Kondo resonance was detected for TOV molecules with protrusions in the occupied state image and for TTV molecules. Spin-resolved DFT calculations showed that an unpaired n electron was delocalized over the adsorbed TOV molecule, which was the origin of the Kondo resonance. For the TOV molecules with protrusions, we proposed a model in which an additional H atom was attached to the TOV molecule. Calculations showed that, upon transfer of an electron to the verdazyl ring, the unpaired n electron disappeared, accounting for the absence of a Kondo resonance in the STS spectra. The absence of a Kondo resonance for the TTV molecule can be explained in a similar manner. In other words, electron transfer to the verdazyl ring occurs because of Au-S bond formation.
机译:我们调查了稳定的中性纯有机自由基分子的1,3,5-三苯基-6-氧杂铜(TOV)和1,3,S-三苯基-6-硫杂铜(TTV)吸附在Au(111)表面上的自旋态,由于自旋电子相互作用而表现为近藤共振。通过使用扫描隧道光谱(STS),检测到TOV分子的清晰近藤共振。但是,对于在占据状态图像中具有凸起的TOV分子和TTV分子,未检测到近藤共振。自旋分辨DFT计算表明,未成对的n电子在吸附的TOV分子上离域化,这是近藤共振的起源。对于具有突起的TOV分子,我们提出了一个模型,其中一个附加的H原子连接到TOV分子上。计算表明,当电子转移到Verdazyl环上时,未配对的n电子消失,这说明在STS光谱中不存在近藤共振。 TTV分子不存在近藤共振可以用类似的方式解释。换句话说,由于形成了Au-S键,所以发生了电子转移到Verdazyl环上。

著录项

  • 来源
    《Journal of the American Chemical Society 》 |2013年第2期| 651-658| 共8页
  • 作者单位

    Institute of Multidisciplinary Research for Advanced Materials (IMRAM, Tagen), Tohoku University, 2-1-1, Katahira, Aoba-Ku, Sendai 980-0877, Japan,Department of Chemistry, Graduate School of Science, Tohoku University, Aramaki-Aza-Aoba, Aoba-Ku, Sendai 980-8578, Japan;

    Institute of Multidisciplinary Research for Advanced Materials (IMRAM, Tagen), Tohoku University, 2-1-1, Katahira, Aoba-Ku, Sendai 980-0877, Japan,Department of Chemistry, Graduate School of Science, Tohoku University, Aramaki-Aza-Aoba, Aoba-Ku, Sendai 980-8578, Japan;

    Department of Chemistry, Graduate School of Science, Tohoku University, Aramaki-Aza-Aoba, Aoba-Ku, Sendai 980-8578, Japan,JST, CREST, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012, Japan;

    Department of Chemistry, Graduate School of Science, Tohoku University, Aramaki-Aza-Aoba, Aoba-Ku, Sendai 980-8578, Japan;

    Department of Chemistry, Graduate School of Science, Tohoku University, Aramaki-Aza-Aoba, Aoba-Ku, Sendai 980-8578, Japan;

    Department of Chemistry, Graduate School of Science, Tohoku University, Aramaki-Aza-Aoba, Aoba-Ku, Sendai 980-8578, Japan,JST, CREST, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012, Japan;

    Institute of Multidisciplinary Research for Advanced Materials (IMRAM, Tagen), Tohoku University, 2-1-1, Katahira, Aoba-Ku, Sendai 980-0877, Japan,JST, CREST, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012, Japan;

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