TY - JOUR
T1 - 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
AU - Liu, Jie
AU - Isshiki, Hironari
AU - Katoh, Keiichi
AU - Morita, Takaumi
AU - Breedlove, Brian K.
AU - Yamashita, Masahiro
AU - Komeda, Tadahiro
PY - 2013/1/16
Y1 - 2013/1/16
N2 - We investigated spin states of stable neutral pure-organic radical molecules of 1,3,5-triphenyl-6-oxoverdazyl (TOV) and 1,3,5-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 π 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 π 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.
AB - We investigated spin states of stable neutral pure-organic radical molecules of 1,3,5-triphenyl-6-oxoverdazyl (TOV) and 1,3,5-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 π 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 π 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.
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U2 - 10.1021/ja303510g
DO - 10.1021/ja303510g
M3 - Article
AN - SCOPUS:84872524815
SN - 0002-7863
VL - 135
SP - 651
EP - 658
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 2
ER -