Very recently,experimental evidence showed that the hydrogen is retained in dithiol-terminated single-molecule junction under the widely adopted preparation conditions,which is in contrast to the accepted view[Nat.Che...Very recently,experimental evidence showed that the hydrogen is retained in dithiol-terminated single-molecule junction under the widely adopted preparation conditions,which is in contrast to the accepted view[Nat.Chem.11351(2019)].However,the hydrogen is generally assumed to be lost in the previous physical models of single-molecule junctions.Whether the retention of the hydrogen at the gold-sulfur interface exerts a significant effect on the theoretical prediction of spin transport properties is an open question.Therefore,here in this paper we carry out a comparative study of spin transport in M-tetraphenylporphyrin-based(M=V,Cr,Mn,Fe,and Co;M-TPP)single-molecule junction through Au-SR and Au-S(H)R bondings.The results show that the hydrogen at the gold-sulfur interface may dramatically affect the spin-filtering efficiency of M-TPP-based single-molecule junction,depending on the type of transition metal ions embedded into porphyrin ring.Moreover,we find that for the Co-TPP-based molecular junction,the hydrogen at the gold-sulfur interface has no obvious effect on transmission at the Fermi level,but it has a significant effect on the spin-dependent transmission dip induced by the quantum interference on the occupied side.Thus the fate of hydrogen should be concerned in the physical model according to the actual preparation condition,which is important for our fundamental understanding of spin transport in the single-molecule junctions.Our work also provides guidance in how to experimentally identify the nature of gold-sulfur interface in the single-molecule junction with spin-polarized transport.展开更多
天马山硫金矿是铜陵矿集区典型的层控热液叠加改造型矿床,层状矿体中发育大量的矽卡岩矿物。为查明该矿床中矽卡岩矿物的类型及形成环境,探讨矽卡岩与硫、金成矿之间的关系,对主要的矽卡岩矿物开展了矿物学及矿物化学研究,并对矿石进行...天马山硫金矿是铜陵矿集区典型的层控热液叠加改造型矿床,层状矿体中发育大量的矽卡岩矿物。为查明该矿床中矽卡岩矿物的类型及形成环境,探讨矽卡岩与硫、金成矿之间的关系,对主要的矽卡岩矿物开展了矿物学及矿物化学研究,并对矿石进行了硫同位素地球化学研究。研究表明:矿区内的矽卡岩矿物以石榴子石和辉石为主,其中石榴子石以钙铁榴石为主,属于钙铁榴石-钙铝榴石固熔体系列(Gro 0~18.73 And 80.54~99.00 Spe+Pyr+Alm 0.54~1.47);辉石以透辉石为主,其次为钙铁辉石,属于透辉石-钙铁辉石系列(Di 62.35~97.65 Hd 1.89~36.27 Jo 0.31~1.55)。天马山硫金矿的矿物组合(钙铁辉石+透辉石)属于氧化型矽卡岩,表明矽卡岩形成于相对高温和高氧逸度的条件。石榴子石和辉石端元组分特征及辉石Mn/Fe值(0.02~0.07)具有典型的矽卡岩型铜、金矿床特征。矿石硫同位素具有岩浆源的特征,与区内燕山期岩浆-成矿作用形成的矿石一致,而明显区别于喷流-沉积作用形成的矿石,显示成矿作用与燕山期岩浆活动具有密切的成因联系。燕山期中酸性岩浆交代碳酸盐岩围岩形成大量矽卡岩,矽卡岩矿物的形成增加了岩石的孔隙度和渗透率,为晚期硫、金矿床的形成提供了有利条件。展开更多
基金the National Natural Science Foundation of China(Grant Nos.11674092,11804093,and 61764005)the Natural Science Foundation of Hunan Province,China(Grant No.2019JJ40006)+2 种基金the Scientific Research Fund of the Education Department of Hunan Province,China(Grant No.18B368)the Science and Technology Development Plan Project of Hengyang City,China(Grant No.2018KJ121)the Science and Technology Plan Project of Hunan Province,China(Grant No.2016TP1020).
文摘Very recently,experimental evidence showed that the hydrogen is retained in dithiol-terminated single-molecule junction under the widely adopted preparation conditions,which is in contrast to the accepted view[Nat.Chem.11351(2019)].However,the hydrogen is generally assumed to be lost in the previous physical models of single-molecule junctions.Whether the retention of the hydrogen at the gold-sulfur interface exerts a significant effect on the theoretical prediction of spin transport properties is an open question.Therefore,here in this paper we carry out a comparative study of spin transport in M-tetraphenylporphyrin-based(M=V,Cr,Mn,Fe,and Co;M-TPP)single-molecule junction through Au-SR and Au-S(H)R bondings.The results show that the hydrogen at the gold-sulfur interface may dramatically affect the spin-filtering efficiency of M-TPP-based single-molecule junction,depending on the type of transition metal ions embedded into porphyrin ring.Moreover,we find that for the Co-TPP-based molecular junction,the hydrogen at the gold-sulfur interface has no obvious effect on transmission at the Fermi level,but it has a significant effect on the spin-dependent transmission dip induced by the quantum interference on the occupied side.Thus the fate of hydrogen should be concerned in the physical model according to the actual preparation condition,which is important for our fundamental understanding of spin transport in the single-molecule junctions.Our work also provides guidance in how to experimentally identify the nature of gold-sulfur interface in the single-molecule junction with spin-polarized transport.
文摘天马山硫金矿是铜陵矿集区典型的层控热液叠加改造型矿床,层状矿体中发育大量的矽卡岩矿物。为查明该矿床中矽卡岩矿物的类型及形成环境,探讨矽卡岩与硫、金成矿之间的关系,对主要的矽卡岩矿物开展了矿物学及矿物化学研究,并对矿石进行了硫同位素地球化学研究。研究表明:矿区内的矽卡岩矿物以石榴子石和辉石为主,其中石榴子石以钙铁榴石为主,属于钙铁榴石-钙铝榴石固熔体系列(Gro 0~18.73 And 80.54~99.00 Spe+Pyr+Alm 0.54~1.47);辉石以透辉石为主,其次为钙铁辉石,属于透辉石-钙铁辉石系列(Di 62.35~97.65 Hd 1.89~36.27 Jo 0.31~1.55)。天马山硫金矿的矿物组合(钙铁辉石+透辉石)属于氧化型矽卡岩,表明矽卡岩形成于相对高温和高氧逸度的条件。石榴子石和辉石端元组分特征及辉石Mn/Fe值(0.02~0.07)具有典型的矽卡岩型铜、金矿床特征。矿石硫同位素具有岩浆源的特征,与区内燕山期岩浆-成矿作用形成的矿石一致,而明显区别于喷流-沉积作用形成的矿石,显示成矿作用与燕山期岩浆活动具有密切的成因联系。燕山期中酸性岩浆交代碳酸盐岩围岩形成大量矽卡岩,矽卡岩矿物的形成增加了岩石的孔隙度和渗透率,为晚期硫、金矿床的形成提供了有利条件。
