메뉴 건너뛰기




Volumn 284, Issue 5420, 1999, Pages 1647-1650

Enhanced reactivity of highly vibrationally excited molecules on metal surfaces

Author keywords

[No Author keywords available]

Indexed keywords

COPPER; CRYSTAL ORIENTATION; NITROGEN COMPOUNDS; PROBABILITY; SURFACE CHEMISTRY;

EID: 0033522807     PISSN: 00368075     EISSN: None     Source Type: Journal    
DOI: 10.1126/science.284.5420.1647     Document Type: Article
Times cited : (76)

References (35)
  • 2
    • 36449006822 scopus 로고
    • A. Sinha, J. D. Thoernke, F. Crim, J. Chem. Phys. 96, 372 (1992); D. W. Arnold, M. Korolik, C. Wittig, H. Reisler, Chem. Phys. Lett. 282, 313 (1998); C. A. Michaels, A. S. Mullin, J. Park, J. Z. Chou, G. W. Flynn, J. Chem. Phys. 108, 2744 (1998); R. L. Miller et al., Science 265, 1831 (1994).
    • (1992) J. Chem. Phys. , vol.96 , pp. 372
    • Sinha, A.1    Thoernke, J.D.2    Crim, F.3
  • 3
    • 0032535872 scopus 로고    scopus 로고
    • A. Sinha, J. D. Thoernke, F. Crim, J. Chem. Phys. 96, 372 (1992); D. W. Arnold, M. Korolik, C. Wittig, H. Reisler, Chem. Phys. Lett. 282, 313 (1998); C. A. Michaels, A. S. Mullin, J. Park, J. Z. Chou, G. W. Flynn, J. Chem. Phys. 108, 2744 (1998); R. L. Miller et al., Science 265, 1831 (1994).
    • (1998) Chem. Phys. Lett. , vol.282 , pp. 313
    • Arnold, D.W.1    Korolik, M.2    Wittig, C.3    Reisler, H.4
  • 4
    • 0000801168 scopus 로고    scopus 로고
    • A. Sinha, J. D. Thoernke, F. Crim, J. Chem. Phys. 96, 372 (1992); D. W. Arnold, M. Korolik, C. Wittig, H. Reisler, Chem. Phys. Lett. 282, 313 (1998); C. A. Michaels, A. S. Mullin, J. Park, J. Z. Chou, G. W. Flynn, J. Chem. Phys. 108, 2744 (1998); R. L. Miller et al., Science 265, 1831 (1994).
    • (1998) J. Chem. Phys. , vol.108 , pp. 2744
    • Michaels, C.A.1    Mullin, A.S.2    Park, J.3    Chou, J.Z.4    Flynn, G.W.5
  • 5
    • 0028564064 scopus 로고
    • A. Sinha, J. D. Thoernke, F. Crim, J. Chem. Phys. 96, 372 (1992); D. W. Arnold, M. Korolik, C. Wittig, H. Reisler, Chem. Phys. Lett. 282, 313 (1998); C. A. Michaels, A. S. Mullin, J. Park, J. Z. Chou, G. W. Flynn, J. Chem. Phys. 108, 2744 (1998); R. L. Miller et al., Science 265, 1831 (1994).
    • (1994) Science , vol.265 , pp. 1831
    • Miller, R.L.1
  • 11
    • 0345138669 scopus 로고    scopus 로고
    • note
    • 1/2(5,0) transition for the pump step. For NO in a supersonic expansion (rotational temperature ∼5 K), it was possible to transfer ∼0.2% of the total population in the illuminated part of the molecular beam into the v = 15, J = 2.5 state.
  • 13
    • 0345138668 scopus 로고    scopus 로고
    • note
    • pump was generated as follows. The output of an argon ion (Spectra Physics 171) pumped single-mode ring dye laser (Coherent CR-699) operated with Rhodamine 6G was pulse-amplified in a homemade three-stage amplifier chain, filled with a mixture of Rhodamine 610 and Rhodamine 640 dyes. The amplifier cuvettes were pumped by a frequency-doubled, Q-switched, injection-seeded Nd-yttrium-aluminum-garnet laser (Continuum Powerlite 7010-IS) with a pulse energy of 400 mJ at 532 nm and a pulse duration of ∼5 ns. The amplified visible radiation was frequency-doubled in a KDP crystal to yield 15 mJ of ultraviolet light around 300 nm. After passing a λ/2 plate, the doubled and residual fundamental radiation were frequency-summed in a BBO crystal (length 1 cm) to yield light near 198 nm with a pulse energy of typically 0.5 to 1.0 mJ and a near-Fourier transform limited bandwidth of less than 150 MHz.
  • 14
    • 0344708152 scopus 로고    scopus 로고
    • note
    • A XeCl pumped dye laser system (Lambda Physik EMG200MSC/FL3002) was used for the dump transitions.
  • 15
    • 0344708149 scopus 로고    scopus 로고
    • note
    • The loss of side fluorescence to the photomultiplier tube due to enhanced stimulated emission along the dump laser propagation axis is referred to as a fluorescence dip. See, for example, (7).
  • 16
    • 0344708150 scopus 로고    scopus 로고
    • note
    • Extreme care was taken to ensure that there were no impurities in the beam that might oxidize the surface.
  • 18
    • 0344708146 scopus 로고    scopus 로고
    • note
    • 2O (which desorbs) + O, which is known to be important at low surface temperatures when the NO coverage is high.
  • 19
    • 21544433076 scopus 로고
    • The ratio of AES signals for Cu and O on this surface revealed a ratio of O adatom to surface Cu atom of ∼1:3. This relied on a calibration of the AES response [F. H. P. M. Habraken, E. P. Kieffer, G. A. Bootsma, Surf. Sci. 83, 45 (1979)].
    • (1979) Surf. Sci. , vol.83 , pp. 45
    • Habraken, F.H.P.M.1    Kieffer, E.P.2    Bootsma, G.A.3
  • 21
    • 0344708147 scopus 로고    scopus 로고
    • note
    • + state. For the experiments reported here, neither step of the REMPI process was saturated.
  • 23
    • 0345138666 scopus 로고    scopus 로고
    • note
    • net was normalized to the square of the probe laser power.
  • 24
    • 0004161642 scopus 로고
    • Wiley-Interscience, New York
    • 21 branch]. Energy levels of the ground state are from C. Amiot, J. Mol. Spectrosc. 94, 150 (1982). Energy levels for the A state derive from R. Engleman Jr., P. E. Rouse, H. M. Peek, V. D. Baiamonte, Los Alamos Science Lab Report LA-4364 (1970); R. Engleman Jr. and P. E. Rouse, J. Mol. Spectrosc. 37, 240 (1971). The rotational state populations were modeled by a Boltzmann distribution.
    • (1987) Angular Momentum , pp. 314
    • Zare, R.N.1
  • 25
    • 0000387214 scopus 로고
    • 21 branch]. Energy levels of the ground state are from C. Amiot, J. Mol. Spectrosc. 94, 150 (1982). Energy levels for the A state derive from R. Engleman Jr., P. E. Rouse, H. M. Peek, V. D. Baiamonte, Los Alamos Science Lab Report LA-4364 (1970); R. Engleman Jr. and P. E. Rouse, J. Mol. Spectrosc. 37, 240 (1971). The rotational state populations were modeled by a Boltzmann distribution.
    • (1982) J. Mol. Spectrosc. , vol.94 , pp. 150
    • Amiot, C.1
  • 26
    • 0343184932 scopus 로고
    • 21 branch]. Energy levels of the ground state are from C. Amiot, J. Mol. Spectrosc. 94, 150 (1982). Energy levels for the A state derive from R. Engleman Jr., P. E. Rouse, H. M. Peek, V. D. Baiamonte, Los Alamos Science Lab Report LA-4364 (1970); R. Engleman Jr. and P. E. Rouse, J. Mol. Spectrosc. 37, 240 (1971). The rotational state populations were modeled by a Boltzmann distribution.
    • (1970) Los Alamos Science Lab Report LA-4364
    • Engleman R., Jr.1    Rouse, P.E.2    Peek, H.M.3    Baiamonte, V.D.4
  • 27
    • 0001304188 scopus 로고
    • 21 branch]. Energy levels of the ground state are from C. Amiot, J. Mol. Spectrosc. 94, 150 (1982). Energy levels for the A state derive from R. Engleman Jr., P. E. Rouse, H. M. Peek, V. D. Baiamonte, Los Alamos Science Lab Report LA-4364 (1970); R. Engleman Jr. and P. E. Rouse, J. Mol. Spectrosc. 37, 240 (1971). The rotational state populations were modeled by a Boltzmann distribution.
    • (1971) J. Mol. Spectrosc. , vol.37 , pp. 240
    • Engleman R., Jr.1    Rouse, P.E.2
  • 28
    • 0344708144 scopus 로고    scopus 로고
    • note
    • -2.
  • 29
    • 0344276147 scopus 로고    scopus 로고
    • note
    • The following channels were observed (v = 15 → 13, 15 → 10, 13 → 12, 13 → 10, 13 → 9, 12 → 9).
  • 30
    • 0344708140 scopus 로고    scopus 로고
    • note
    • Because of the difficulty of ensuring an absolutely oxygen-free surface and the high sensitivity of the REMPI signal to oxygen coverage, we consider this number to be a lower limit to the true value. The error bars represent one standard deviation.
  • 31
    • 0344708142 scopus 로고    scopus 로고
    • note
    • Temperatures between 300 and 500 K were studied. Two molecular beams were compared with collision energies of 29 and 67 kJ/mol.
  • 33
    • 0001478448 scopus 로고
    • J. C. Polanyi, Acc. Chem. Res. 5, 161 (1972); _ and W. H. Wong, J. Chem. Phys. 51, 1439 (1969).
    • (1972) Acc. Chem. Res. , vol.5 , pp. 161
    • Polanyi, J.C.1
  • 34
    • 0001478448 scopus 로고
    • J. C. Polanyi, Acc. Chem. Res. 5, 161 (1972); _ and W. H. Wong, J. Chem. Phys. 51, 1439 (1969).
    • (1969) J. Chem. Phys. , vol.51 , pp. 1439
    • Wong, W.H.1
  • 35
    • 0344708137 scopus 로고    scopus 로고
    • note
    • Supported by the U.S. Air Force Office of Scientific Research (grant F49620-95-1-0234) and the U.S. Department of Energy Office of Basic Energy Sciences (grant DE-FG03-94ER14492/A000).


* 이 정보는 Elsevier사의 SCOPUS DB에서 KISTI가 분석하여 추출한 것입니다.