DOI: 10.1063/1.437318. Vibrational excitation and surface reactivity: An examination of the ν3 and 2ν3 modes of CH4

Vibrational excitation and surface reactivity: An examination of the ν3 and 2ν3 modes of CH4

10.1063/1.437318

Crossref journal-article

AIP Publishing

The Journal of Chemical Physics (317)

Abstract

The effect of vibrational excitation upon the chemisorption of methane on thin films of rhodium has been investigated. Vibrational modes of the gas are selectively excited by infrared radiation. The rate of reaction is measured by following the pressure decrease in a closed system containing CH4 in contact with the metal surface. Neither irradiation with a He–Ne laser at 3.39 μ to excite the ν3 mode, nor using an arc source with wavelengths in the range overlapping 2ν3, produces any detectable changes in the rate. From these experiments we estimate that the reaction probability of CH4 is &lt;1×10−4 in the first excited state of ν3, and &lt;7×10−2 in 2ν3. Other excitations must be involved in overcoming the barrier of ?7 kcal/mole which has previously been found for the chemisorption of CH4 on rhodium.

Bibliography

Brass, S. G., Reed, D. A., & Ehrlich, G. (1979). Vibrational excitation and surface reactivity: An examination of the Î½3 and 2Î½3 modes of CH4. The Journal of Chemical Physics, 70(11), 5244â5250.

Authors 3

Stephen G. Brass (first)
David A. Reed (additional)
Gert Ehrlich (additional)

References 31 Referenced 50

10.1063/1.430415 / J. Chem. Phys. (1975)
10.1016/0039-6028(75)90389-1 / Surf. Sci. (1975)
10.1016/0039-6028(78)90378-3 / Surf. Sci. (1978)
10.1016/0039-6028(77)90359-4 / Surf. Sci. (1977)
10.1016/0009-2614(72)80491-3 / Chem. Phys. Lett. (1972)
10.1063/1.430722 / J. Chem. Phys. (1975)
10.1063/1.432717 / J. Chem. Phys. (1976)
10.1147/rd.223.0260 / IBM J. Res. Dev. (1978)
{'key': '2024020917475224100_r6'}
{'key': '2024020917475224100_r7'}
10.1016/0022-2852(59)90057-8 / J. Mol. Spectrosc. (1959)
{'key': '2024020917475224100_r9'}
{'key': '2024020917475224100_r10'}
{'key': '2024020917475224100_r11'}
{'key': '2024020917475224100_r12', 'first-page': '19', 'volume': '7–8', 'year': '1958', 'journal-title': 'Vacuum'} / Vacuum (1958)
{'key': '2024020917475224100_r12a'}
{'key': '2024020917475224100_r13'}
10.1116/1.1317943 / J. Vac. Sci. Technol. (1973)
{'key': '2024020917475224100_r15'}
10.1364/JOSA.66.000097 / J. Opt. Soc. Am. (1976)
10.1016/0371-1951(60)80030-6 / Spectrochim. Acta (1960)
{'key': '2024020917475224100_r18', 'first-page': '489', 'volume': '7', 'year': '1930', 'journal-title': 'Ann. Phys.'} / Ann. Phys. (1930)
{'key': '2024020917475224100_r19'}
10.1063/1.1670199 / J. Chem. Phys. (1968)
10.1063/1.433346 / J. Chem. Phys. (1976)
{'key': '2024020917475224100_r22', 'first-page': '490', 'volume': '86', 'year': '1977', 'journal-title': 'Physica (Utrecht) A'} / Physica (Utrecht) A (1977)
{'key': '2024020917475224100_r23'}
{'key': '2024020917475224100_r24', 'first-page': '356', 'volume': '14', 'year': '1974', 'journal-title': 'J. Quant. Spectrosc. Radiat. Transfer'} / J. Quant. Spectrosc. Radiat. Transfer (1974)
{'key': '2024020917475224100_r25'}
{'key': '2024020917475224100_r26'}
{'key': '2024020917475224100_r27'}

Dates

Type	When
Created	22 years, 5 months ago (Feb. 27, 2003, 5:52 p.m.)
Deposited	1 year, 6 months ago (Feb. 9, 2024, 2:45 p.m.)
Indexed	1 year, 6 months ago (Feb. 11, 2024, 1:05 a.m.)
Issued	46 years, 2 months ago (June 1, 1979)
Published	46 years, 2 months ago (June 1, 1979)
Published Print	46 years, 2 months ago (June 1, 1979)

Funders 0

None

BibTeX

@article{Brass_1979, title={Vibrational excitation and surface reactivity: An examination of the ν3 and 2ν3 modes of CH4}, volume={70}, ISSN={1089-7690}, url={http://dx.doi.org/10.1063/1.437318}, DOI={10.1063/1.437318}, number={11}, journal={The Journal of Chemical Physics}, publisher={AIP Publishing}, author={Brass, Stephen G. and Reed, David A. and Ehrlich, Gert}, year={1979}, month=jun, pages={5244–5250} }

JSON

{
  "indexed": {
    "date-parts": [
      [
        2024,
        2,
        11
      ]
    ],
    "date-time": "2024-02-11T06:05:42Z",
    "timestamp": 1707631542254
  },
  "reference-count": 31,
  "publisher": "AIP Publishing",
  "issue": "11",
  "content-domain": {
    "domain": [
      "pubs.aip.org"
    ],
    "crossmark-restriction": true
  },
  "published-print": {
    "date-parts": [
      [
        1979,
        6,
        1
      ]
    ]
  },
  "abstract": "<jats:p>The effect of vibrational excitation upon the chemisorption of methane on thin films of rhodium has been investigated. Vibrational modes of the gas are selectively excited by infrared radiation. The rate of reaction is measured by following the pressure decrease in a closed system containing CH4 in contact with the metal surface. Neither irradiation with a He\u2013Ne laser at 3.39 \u03bc to excite the \u03bd3 mode, nor using an arc source with wavelengths in the range overlapping 2\u03bd3, produces any detectable changes in the rate. From these experiments we estimate that the reaction probability of CH4 is &amp;lt;1\u00d710\u22124 in the first excited state of \u03bd3, and &amp;lt;7\u00d710\u22122 in 2\u03bd3. Other excitations must be involved in overcoming the barrier of ?7 kcal/mole which has previously been found for the chemisorption of CH4 on rhodium.</jats:p>",
  "DOI": "10.1063/1.437318",
  "type": "journal-article",
  "created": {
    "date-parts": [
      [
        2003,
        2,
        27
      ]
    ],
    "date-time": "2003-02-27T22:52:53Z",
    "timestamp": 1046386373000
  },
  "page": "5244-5250",
  "update-policy": "http://dx.doi.org/10.1063/aip-crossmark-policy-page",
  "source": "Crossref",
  "is-referenced-by-count": 50,
  "title": "Vibrational excitation and surface reactivity: An examination of the \u03bd3 and 2\u03bd3 modes of CH4",
  "prefix": "10.1063",
  "volume": "70",
  "author": [
    {
      "given": "Stephen G.",
      "family": "Brass",
      "sequence": "first",
      "affiliation": [
        {
          "name": "Coordinated Science Laboratory, Department of Metallurgy, and Department of Physics, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801"
        }
      ]
    },
    {
      "given": "David A.",
      "family": "Reed",
      "sequence": "additional",
      "affiliation": [
        {
          "name": "Coordinated Science Laboratory, Department of Metallurgy, and Department of Physics, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801"
        }
      ]
    },
    {
      "given": "Gert",
      "family": "Ehrlich",
      "sequence": "additional",
      "affiliation": [
        {
          "name": "Coordinated Science Laboratory, Department of Metallurgy, and Department of Physics, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801"
        }
      ]
    }
  ],
  "member": "317",
  "reference": [
    {
      "key": "2024020917475224100_r1",
      "doi-asserted-by": "crossref",
      "first-page": "4672",
      "DOI": "10.1063/1.430415",
      "volume": "62",
      "year": "1975",
      "journal-title": "J. Chem. Phys."
    },
    {
      "key": "2024020917475224100_r2",
      "doi-asserted-by": "crossref",
      "first-page": "377",
      "DOI": "10.1016/0039-6028(75)90389-1",
      "volume": "51",
      "year": "1975",
      "journal-title": "Surf. Sci."
    },
    {
      "key": "2024020917475224100_r2a",
      "doi-asserted-by": "crossref",
      "first-page": "61",
      "DOI": "10.1016/0039-6028(78)90378-3",
      "volume": "72",
      "year": "1978",
      "journal-title": "Surf. Sci."
    },
    {
      "key": "2024020917475224100_r3",
      "doi-asserted-by": "crossref",
      "first-page": "460",
      "DOI": "10.1016/0039-6028(77)90359-4",
      "volume": "63",
      "year": "1977",
      "journal-title": "Surf. Sci."
    },
    {
      "key": "2024020917475224100_r4",
      "doi-asserted-by": "crossref",
      "first-page": "203",
      "DOI": "10.1016/0009-2614(72)80491-3",
      "volume": "16",
      "year": "1972",
      "journal-title": "Chem. Phys. Lett."
    },
    {
      "key": "2024020917475224100_r5",
      "doi-asserted-by": "crossref",
      "first-page": "2454",
      "DOI": "10.1063/1.430722",
      "volume": "62",
      "year": "1975",
      "journal-title": "J. Chem. Phys."
    },
    {
      "key": "2024020917475224100_r5a",
      "doi-asserted-by": "crossref",
      "first-page": "3495",
      "DOI": "10.1063/1.432717",
      "volume": "64",
      "year": "1976",
      "journal-title": "J. Chem. Phys."
    },
    {
      "key": "2024020917475224100_r5b",
      "doi-asserted-by": "crossref",
      "first-page": "260",
      "DOI": "10.1147/rd.223.0260",
      "volume": "22",
      "year": "1978",
      "journal-title": "IBM J. Res. Dev."
    },
    {
      "key": "2024020917475224100_r6"
    },
    {
      "key": "2024020917475224100_r7"
    },
    {
      "key": "2024020917475224100_r8",
      "doi-asserted-by": "crossref",
      "first-page": "632",
      "DOI": "10.1016/0022-2852(59)90057-8",
      "volume": "3",
      "year": "1959",
      "journal-title": "J. Mol. Spectrosc."
    },
    {
      "key": "2024020917475224100_r9"
    },
    {
      "key": "2024020917475224100_r10"
    },
    {
      "key": "2024020917475224100_r11"
    },
    {
      "key": "2024020917475224100_r12",
      "first-page": "19",
      "volume": "7\u20138",
      "year": "1958",
      "journal-title": "Vacuum"
    },
    {
      "key": "2024020917475224100_r12a"
    },
    {
      "key": "2024020917475224100_r13"
    },
    {
      "key": "2024020917475224100_r14",
      "doi-asserted-by": "crossref",
      "first-page": "212",
      "DOI": "10.1116/1.1317943",
      "volume": "10",
      "year": "1973",
      "journal-title": "J. Vac. Sci. Technol."
    },
    {
      "key": "2024020917475224100_r15"
    },
    {
      "key": "2024020917475224100_r16",
      "doi-asserted-by": "crossref",
      "first-page": "97",
      "DOI": "10.1364/JOSA.66.000097",
      "volume": "66",
      "year": "1976",
      "journal-title": "J. Opt. Soc. Am."
    },
    {
      "key": "2024020917475224100_r17",
      "doi-asserted-by": "crossref",
      "first-page": "840",
      "DOI": "10.1016/0371-1951(60)80030-6",
      "volume": "16",
      "year": "1960",
      "journal-title": "Spectrochim. Acta"
    },
    {
      "key": "2024020917475224100_r18",
      "first-page": "489",
      "volume": "7",
      "year": "1930",
      "journal-title": "Ann. Phys."
    },
    {
      "key": "2024020917475224100_r19"
    },
    {
      "key": "2024020917475224100_r20",
      "doi-asserted-by": "crossref",
      "first-page": "1111",
      "DOI": "10.1063/1.1670199",
      "volume": "49",
      "year": "1968",
      "journal-title": "J. Chem. Phys."
    },
    {
      "key": "2024020917475224100_r21",
      "doi-asserted-by": "crossref",
      "first-page": "2339",
      "DOI": "10.1063/1.433346",
      "volume": "65",
      "year": "1976",
      "journal-title": "J. Chem. Phys."
    },
    {
      "key": "2024020917475224100_r22",
      "first-page": "490",
      "volume": "86",
      "year": "1977",
      "journal-title": "Physica (Utrecht) A"
    },
    {
      "key": "2024020917475224100_r23"
    },
    {
      "key": "2024020917475224100_r24",
      "first-page": "356",
      "volume": "14",
      "year": "1974",
      "journal-title": "J. Quant. Spectrosc. Radiat. Transfer"
    },
    {
      "key": "2024020917475224100_r25"
    },
    {
      "key": "2024020917475224100_r26"
    },
    {
      "key": "2024020917475224100_r27"
    }
  ],
  "container-title": "The Journal of Chemical Physics",
  "original-title": [],
  "language": "en",
  "link": [
    {
      "URL": "https://pubs.aip.org/aip/jcp/article-pdf/70/11/5244/18916910/5244_1_online.pdf",
      "content-type": "application/pdf",
      "content-version": "vor",
      "intended-application": "syndication"
    },
    {
      "URL": "https://pubs.aip.org/aip/jcp/article-pdf/70/11/5244/18916910/5244_1_online.pdf",
      "content-type": "unspecified",
      "content-version": "vor",
      "intended-application": "similarity-checking"
    }
  ],
  "deposited": {
    "date-parts": [
      [
        2024,
        2,
        9
      ]
    ],
    "date-time": "2024-02-09T19:45:28Z",
    "timestamp": 1707507928000
  },
  "score": 1,
  "resource": {
    "primary": {
      "URL": "https://pubs.aip.org/jcp/article/70/11/5244/776962/Vibrational-excitation-and-surface-reactivity-An"
    }
  },
  "subtitle": [],
  "short-title": [],
  "issued": {
    "date-parts": [
      [
        1979,
        6,
        1
      ]
    ]
  },
  "references-count": 31,
  "journal-issue": {
    "issue": "11",
    "published-print": {
      "date-parts": [
        [
          1979,
          6,
          1
        ]
      ]
    }
  },
  "URL": "http://dx.doi.org/10.1063/1.437318",
  "relation": {},
  "ISSN": [
    "0021-9606",
    "1089-7690"
  ],
  "subject": [],
  "published-other": {
    "date-parts": [
      [
        1979,
        6,
        1
      ]
    ]
  },
  "published": {
    "date-parts": [
      [
        1979,
        6,
        1
      ]
    ]
  }
}