Facile charge-displacement at silicon gives spaced-out reaction

Maryam Ebrahimi; Kai Huang; Xuekun Lu; Iain R. McNab; John C. Polanyi; Zafar Waqar; Jody Yang; Haiping Lin; Werner A. Hofer

doi:10.1021/ja205716t

Facile charge-displacement at silicon gives spaced-out reaction

Maryam Ebrahimi, Kai Huang, Xuekun Lu, Iain R. McNab, John C. Polanyi^*, Zafar Waqar, Jody Yang, Haiping Lin, Werner A. Hofer

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

6 Scopus citations

Abstract

Adsorbates on metals, but not previously on semiconductors, have been observed to display long-range repulsive interactions. On metals, due to efficient dissipation, the repulsions are weak, typically on the order of 5 meV at 10 Å. On the 7×7 reconstruction of the Si(111) surface, charge transport through the surface has been demonstrated by others using charge injection by STM tips. Here we show that for both physisorbed brominated molecules, and for chemisorbed Br-atoms, induced charge-transfer in the Si(111)-7×7 surface can lead to a strong repulsive interaction between adsorbates, calculated as 200 meV at 13.4 Å. This large repulsive interaction must be channeled through the surface since it causes widely spaced "one-per-corner-hole" patterns of physisorption (three cases-directly observed here) and subsequent chemisorption (four cases observed). The patterns were observed by ultrahigh vacuum scanning tunneling microscopy for four different brominated hydrocarbon adsorbates; 1,2-dibromoethane, 1-bromopropane, 1-bromopentane, and bromobenzene, deposited individually on the surface. In every case, adsorbates were overwhelmingly more likely to be found singly than multiply adjacent to a corner-hole, constituting a distinctive pattern having a probability p = 7 × 10 ^-5 compared to a random distribution.

Original language	English
Pages (from-to)	16560-16565
Number of pages	6
Journal	Journal of the American Chemical Society
Volume	133
Issue number	41
DOIs	https://doi.org/10.1021/ja205716t
State	Published - 19 Oct 2011
Externally published	Yes

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@article{c94cf4ea3189481f8509038caf827643,

title = "Facile charge-displacement at silicon gives spaced-out reaction",

abstract = "Adsorbates on metals, but not previously on semiconductors, have been observed to display long-range repulsive interactions. On metals, due to efficient dissipation, the repulsions are weak, typically on the order of 5 meV at 10 {\AA}. On the 7×7 reconstruction of the Si(111) surface, charge transport through the surface has been demonstrated by others using charge injection by STM tips. Here we show that for both physisorbed brominated molecules, and for chemisorbed Br-atoms, induced charge-transfer in the Si(111)-7×7 surface can lead to a strong repulsive interaction between adsorbates, calculated as 200 meV at 13.4 {\AA}. This large repulsive interaction must be channeled through the surface since it causes widely spaced {"}one-per-corner-hole{"} patterns of physisorption (three cases-directly observed here) and subsequent chemisorption (four cases observed). The patterns were observed by ultrahigh vacuum scanning tunneling microscopy for four different brominated hydrocarbon adsorbates; 1,2-dibromoethane, 1-bromopropane, 1-bromopentane, and bromobenzene, deposited individually on the surface. In every case, adsorbates were overwhelmingly more likely to be found singly than multiply adjacent to a corner-hole, constituting a distinctive pattern having a probability p = 7 × 10 -5 compared to a random distribution.",

author = "Maryam Ebrahimi and Kai Huang and Xuekun Lu and McNab, {Iain R.} and Polanyi, {John C.} and Zafar Waqar and Jody Yang and Haiping Lin and Hofer, {Werner A.}",

note = "Funding Information: Formaldehyde was prepared by the method of Spence and Wild 6. Alpha polyoxymethylene was utilized as the starting material in place of paraformaldehyde to take advantage of the lesser degree of hydration of the former polymer. The deuterium used was of 99.5-per cent enrichment or better. Formaldehyde.deuterium mixtures were made up and stored in a mixing vessel maintained at about 120~ in order to minimize formaldehyde polymerization. The pressure in the mixing vessel was monitored before each run to correct for the small amounts of polymerization that occurred. The photolysis cell consisted of a quartz cylinder, 25 mm in diameter and 20 cm long, with optically flat windows fused onto the ends. This vessel was placed in a cylindrical brass furnace electronically regulated to :kl~ All This research is a part of the work by the Bureau of Mines on Order No. CS-670-54-9, supported by Headquarters, Air Research and Development Command, Office of Scientific Research, through Project SQUID.",

year = "2011",

month = oct,

day = "19",

doi = "10.1021/ja205716t",

language = "英语",

volume = "133",

pages = "16560--16565",

journal = "Journal of the American Chemical Society",

issn = "0002-7863",

publisher = "American Chemical Society",

number = "41",

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T1 - Facile charge-displacement at silicon gives spaced-out reaction

AU - Ebrahimi, Maryam

AU - Huang, Kai

AU - Lu, Xuekun

AU - McNab, Iain R.

AU - Polanyi, John C.

AU - Waqar, Zafar

AU - Yang, Jody

AU - Lin, Haiping

AU - Hofer, Werner A.

N1 - Funding Information: Formaldehyde was prepared by the method of Spence and Wild 6. Alpha polyoxymethylene was utilized as the starting material in place of paraformaldehyde to take advantage of the lesser degree of hydration of the former polymer. The deuterium used was of 99.5-per cent enrichment or better. Formaldehyde.deuterium mixtures were made up and stored in a mixing vessel maintained at about 120~ in order to minimize formaldehyde polymerization. The pressure in the mixing vessel was monitored before each run to correct for the small amounts of polymerization that occurred. The photolysis cell consisted of a quartz cylinder, 25 mm in diameter and 20 cm long, with optically flat windows fused onto the ends. This vessel was placed in a cylindrical brass furnace electronically regulated to :kl~ All This research is a part of the work by the Bureau of Mines on Order No. CS-670-54-9, supported by Headquarters, Air Research and Development Command, Office of Scientific Research, through Project SQUID.

PY - 2011/10/19

Y1 - 2011/10/19

N2 - Adsorbates on metals, but not previously on semiconductors, have been observed to display long-range repulsive interactions. On metals, due to efficient dissipation, the repulsions are weak, typically on the order of 5 meV at 10 Å. On the 7×7 reconstruction of the Si(111) surface, charge transport through the surface has been demonstrated by others using charge injection by STM tips. Here we show that for both physisorbed brominated molecules, and for chemisorbed Br-atoms, induced charge-transfer in the Si(111)-7×7 surface can lead to a strong repulsive interaction between adsorbates, calculated as 200 meV at 13.4 Å. This large repulsive interaction must be channeled through the surface since it causes widely spaced "one-per-corner-hole" patterns of physisorption (three cases-directly observed here) and subsequent chemisorption (four cases observed). The patterns were observed by ultrahigh vacuum scanning tunneling microscopy for four different brominated hydrocarbon adsorbates; 1,2-dibromoethane, 1-bromopropane, 1-bromopentane, and bromobenzene, deposited individually on the surface. In every case, adsorbates were overwhelmingly more likely to be found singly than multiply adjacent to a corner-hole, constituting a distinctive pattern having a probability p = 7 × 10 -5 compared to a random distribution.

AB - Adsorbates on metals, but not previously on semiconductors, have been observed to display long-range repulsive interactions. On metals, due to efficient dissipation, the repulsions are weak, typically on the order of 5 meV at 10 Å. On the 7×7 reconstruction of the Si(111) surface, charge transport through the surface has been demonstrated by others using charge injection by STM tips. Here we show that for both physisorbed brominated molecules, and for chemisorbed Br-atoms, induced charge-transfer in the Si(111)-7×7 surface can lead to a strong repulsive interaction between adsorbates, calculated as 200 meV at 13.4 Å. This large repulsive interaction must be channeled through the surface since it causes widely spaced "one-per-corner-hole" patterns of physisorption (three cases-directly observed here) and subsequent chemisorption (four cases observed). The patterns were observed by ultrahigh vacuum scanning tunneling microscopy for four different brominated hydrocarbon adsorbates; 1,2-dibromoethane, 1-bromopropane, 1-bromopentane, and bromobenzene, deposited individually on the surface. In every case, adsorbates were overwhelmingly more likely to be found singly than multiply adjacent to a corner-hole, constituting a distinctive pattern having a probability p = 7 × 10 -5 compared to a random distribution.

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U2 - 10.1021/ja205716t

DO - 10.1021/ja205716t

M3 - 文章

C2 - 21879758

AN - SCOPUS:80054761996

SN - 0002-7863

VL - 133

SP - 16560

EP - 16565

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 41

ER -

Facile charge-displacement at silicon gives spaced-out reaction

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