Abstract

The viability of pulsed laser photofragment emission (PFE) is evaluated for the in situ measurement of vapor-phase mercuric chloride (HgCl2) concentration in combustion flue gas. Dispersed emissions from both the Hg(6P13) and HgCl(BΣ+2) photoproducts are presented, and the dependence of the HgCl2 PFE signal originating from Hg(6P13) on the collisional environment is examined for buffer-gas mixtures of N 2, O 2, and CO2. Integrated PFE intensity measurements as a function of buffer gas pressure support the assumption that the primary effect of the relevant flue gas constituents is to quench emission from Hg(6P13). The quenching rate constants for PFE from HgCl2 were measured to be 1.37(±0.16)×105Torr1s1 for N 2, 9.35(±0.25)×106Torr1s1 for O 2, and 1.49(±0.29)×106Torr1s1 for CO2. These values are in good accord with literature values for the quenching of Hg(6P13). The emission cross section for Hg(6P13) generated by photodissociation of HgCl2 in 760  Torr  N 2 is found to be 1.0(±0.2)×1025m 2 by comparing the PFE signal to N 2 Raman scattering.

© 2006 Optical Society of America

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  1. C. L. Senior, J. J. Helble, and A. F. Sarofim, "Emissions of mercury, trace elements, and fine particles from stationary combustion devices," Fuel Process. Technol. 65-66, 263-288 (2000).
    [CrossRef]
  2. V. M. Fthenakis, F. W. Lipfert, P. D. Moskowitz, and L. Saroff, "An assessment of mercury emissions and health risks from a coal-fired power plant," J. Hazard. Mater. 44, 267-283 (1995).
    [CrossRef]
  3. G. Offen, N. Shick, R. Chang, P. Chu, C. Dene, and R. Rhudy, "Mercury controls for coal-fired power plants--status and challenges," Modern Power Syst. 25, 24-29 (2005).
  4. P. Monkhouse, "On-line diagnostic methods for metal species in industrial process gas," Prog. Energy Combust. Sci. 28, 331-381 (2002).
    [CrossRef]
  5. J. B. Simeonsson and R. C. Sausa, "A critical review of laser photofragmentation/fragment detection techniques for gas-phase chemical analysis," Appl. Spectrosc. Rev. 31, 1-72 (1996).
    [CrossRef]
  6. U. Gottwald and P. Monkhouse, "Single-port optical access for spectroscopic measurements in industrial flue gas ducts," Appl. Phys. B 69, 151-154 (1999).
    [CrossRef]
  7. P. Templet, J. R. McDonald, S. P. McGlynn, C. H. Kendrow, J. L. Roebber, and K. Weiss, "Ultraviolet absorption spectra of mercuric halides," J. Chem. Phys. 56, 5746 (1972).
    [CrossRef]
  8. C. Roxlo and A. Mandl, "Vacuum ultraviolet absorption cross sections for halogen containing molecules," J. Appl. Phys. 51, 2969-2972 (1980).
    [CrossRef]
  9. D. Spence, R.-G. Wang, and M. A. Dillon, "Pseudo-optical absorption spectra in HgCl2 and HgBr2 from 4 to 14 eV," Appl. Phys. Lett. 41, 1021-1023 (1982).
    [CrossRef]
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    [CrossRef]
  11. W. R. Wadt, "The electronic structure of HgCl2 and HgBr2 and its relationship to photodissociation," J. Chem. Phys. 72, 2469-2478 (1980).
    [CrossRef]
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    [CrossRef]
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    [CrossRef]
  14. C. Whitehurst and T. A. King, "Multiphoton excitation of mercury atoms by photodissociation of HgX2 (X = Cl, Br, I)," J. Phys. B: At. Mol. Phys. 20, 4053-4064 (1987).
    [CrossRef]
  15. R. B. Barat and A. T. Poulos, "Detection of mercury compounds in the gas phase by laser photofragmentation/emission spectroscopy," Appl. Spectrosc. 52, 1360-1363 (1998).
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    [CrossRef]
  18. L. J. Curtis, R. E. Irving, M. Henderson, R. Matulioniene, C. F. Fischer, and E. H. Pinnington, "Measurements and predictions of the 6s6p1,3P1 lifetimes in the Hg isoelectronic sequence," Phys. Rev. A 63, 042502-1-7 (2001).
    [CrossRef]
  19. A. Sibata, M. Takahasi, H. Mikuni, H. Horiguchi, and S. Tsuchiya, "Chemiionization of excited mercury atom with 253.7 nm irradiation in the presence of N2 and CH4," Bull. Chem. Soc. Jpn. 52, 15-20 (1979).
    [CrossRef]
  20. J. Pitre, K. Hammond, and L. Krause, "63P1--63P0 excitation transfer in mercury, induced in collisions with N2 molecules," Phys. Rev. A 6, 2101-2106 (1972).
    [CrossRef]
  21. J. S. Deech, J. Pitre, and L. Krause, "Quenching and depolarization of mercury resonance radiation," Can. J. Phys. 49, 1976-1981 (1971).
    [CrossRef]
  22. J. Calvert and J. Pitts, Photochemistry (Wiley, 1966), p. 74.
  23. J. V. Michael and G. N. Suess, "Absolute quenching cross sections of Hg (3P1) with various molecules," J. Phys. Chem. 78, 482-487 (1974).
    [CrossRef]
  24. J. P. Barrat, D. Casalta, J. L. Cojan, and J. Hamel, "Depolarisation et (quenching) du niveau 63P1 du mercure lors de collisions avec des gaz etrangers," J. Phys. (Paris) 27, 608-618 (1966).
    [CrossRef]
  25. A. J. Yarwood, O. P. Strausz, and H. E. Gunning, "Quenching of 2537-Å resonance radiation of mercury," J. Chem. Phys. 41, 1705-1713 (1964).
    [CrossRef]
  26. H. Horiguchi and S. Tsuchiya, "Quenching of excited mercury atoms (63P1 and 63P0) in molecular collisions," Bull. Chem. Soc. Jpn. 47, 2768-2774 (1974).
    [CrossRef]
  27. The N2 Raman cross section was calculated from the information provided by A. C. Eckbreth, Laser Diagnostics for Combustion Temperature and Species, 2nd ed. (Gordon and Breach, 1996), Chap. 5. The N2 depolarization ratio is 0.024.
  28. A. A. Hoops, Sandia National Laboratories, P. O. Box 969, MS 9056, Livermore, California 94551, and T. A. Reichardt are preparing a manuscript to be called "Time-resolved measurement of HgCl2 photofragment emission."
  29. D. A. V. Kliner, F. Di Teodoro, J. P. Koplow, S. W. Moore, and A. V. Smith, "Efficient second, third, fourth, and fifth harmonic generation of a Yb-doped fiber amplifier," Opt. Commun. 210, 393-398 (2002).
    [CrossRef]

2005 (1)

G. Offen, N. Shick, R. Chang, P. Chu, C. Dene, and R. Rhudy, "Mercury controls for coal-fired power plants--status and challenges," Modern Power Syst. 25, 24-29 (2005).

2002 (2)

P. Monkhouse, "On-line diagnostic methods for metal species in industrial process gas," Prog. Energy Combust. Sci. 28, 331-381 (2002).
[CrossRef]

D. A. V. Kliner, F. Di Teodoro, J. P. Koplow, S. W. Moore, and A. V. Smith, "Efficient second, third, fourth, and fifth harmonic generation of a Yb-doped fiber amplifier," Opt. Commun. 210, 393-398 (2002).
[CrossRef]

2001 (1)

L. J. Curtis, R. E. Irving, M. Henderson, R. Matulioniene, C. F. Fischer, and E. H. Pinnington, "Measurements and predictions of the 6s6p1,3P1 lifetimes in the Hg isoelectronic sequence," Phys. Rev. A 63, 042502-1-7 (2001).
[CrossRef]

2000 (1)

C. L. Senior, J. J. Helble, and A. F. Sarofim, "Emissions of mercury, trace elements, and fine particles from stationary combustion devices," Fuel Process. Technol. 65-66, 263-288 (2000).
[CrossRef]

1999 (2)

U. Gottwald and P. Monkhouse, "Single-port optical access for spectroscopic measurements in industrial flue gas ducts," Appl. Phys. B 69, 151-154 (1999).
[CrossRef]

G. Stark, P. L. Smith, J. Rufus, A. P. Thorne, J. C. Pickering, and G. Cox, "High-resolution photoabsorption cross-section measurements of SO2 at 295 K between 198 and 220 nm," J. Geophys. Res. 104, 16585-16590 (1999).
[CrossRef]

1998 (1)

R. B. Barat and A. T. Poulos, "Detection of mercury compounds in the gas phase by laser photofragmentation/emission spectroscopy," Appl. Spectrosc. 52, 1360-1363 (1998).

1996 (1)

J. B. Simeonsson and R. C. Sausa, "A critical review of laser photofragmentation/fragment detection techniques for gas-phase chemical analysis," Appl. Spectrosc. Rev. 31, 1-72 (1996).
[CrossRef]

1995 (1)

V. M. Fthenakis, F. W. Lipfert, P. D. Moskowitz, and L. Saroff, "An assessment of mercury emissions and health risks from a coal-fired power plant," J. Hazard. Mater. 44, 267-283 (1995).
[CrossRef]

1987 (1)

C. Whitehurst and T. A. King, "Multiphoton excitation of mercury atoms by photodissociation of HgX2 (X = Cl, Br, I)," J. Phys. B: At. Mol. Phys. 20, 4053-4064 (1987).
[CrossRef]

1985 (1)

D. Spence, R.-G. Wang, and M. A. Dillon, "Excitation of Rydberg states of HgCl2 and HgBr2 by electron impact," J. Chem. Phys. 82, 1883-1889 (1985).
[CrossRef]

1982 (1)

D. Spence, R.-G. Wang, and M. A. Dillon, "Pseudo-optical absorption spectra in HgCl2 and HgBr2 from 4 to 14 eV," Appl. Phys. Lett. 41, 1021-1023 (1982).
[CrossRef]

1980 (2)

C. Roxlo and A. Mandl, "Vacuum ultraviolet absorption cross sections for halogen containing molecules," J. Appl. Phys. 51, 2969-2972 (1980).
[CrossRef]

W. R. Wadt, "The electronic structure of HgCl2 and HgBr2 and its relationship to photodissociation," J. Chem. Phys. 72, 2469-2478 (1980).
[CrossRef]

1979 (2)

W. R. Wadt, "The electronic structure of HgCl and HgBr," Appl. Phys. Lett. 34, 658-660 (1979).
[CrossRef]

A. Sibata, M. Takahasi, H. Mikuni, H. Horiguchi, and S. Tsuchiya, "Chemiionization of excited mercury atom with 253.7 nm irradiation in the presence of N2 and CH4," Bull. Chem. Soc. Jpn. 52, 15-20 (1979).
[CrossRef]

1978 (1)

T. A. Cool, J. A. McGarvey, Jr., and A. C. Erlandson, "Two-photon excitation of mercury atoms by photodissociation of mercury halides," Chem. Phys. Lett. 58, 108-113 (1978).
[CrossRef]

1974 (2)

J. V. Michael and G. N. Suess, "Absolute quenching cross sections of Hg (3P1) with various molecules," J. Phys. Chem. 78, 482-487 (1974).
[CrossRef]

H. Horiguchi and S. Tsuchiya, "Quenching of excited mercury atoms (63P1 and 63P0) in molecular collisions," Bull. Chem. Soc. Jpn. 47, 2768-2774 (1974).
[CrossRef]

1972 (2)

J. Pitre, K. Hammond, and L. Krause, "63P1--63P0 excitation transfer in mercury, induced in collisions with N2 molecules," Phys. Rev. A 6, 2101-2106 (1972).
[CrossRef]

P. Templet, J. R. McDonald, S. P. McGlynn, C. H. Kendrow, J. L. Roebber, and K. Weiss, "Ultraviolet absorption spectra of mercuric halides," J. Chem. Phys. 56, 5746 (1972).
[CrossRef]

1971 (1)

J. S. Deech, J. Pitre, and L. Krause, "Quenching and depolarization of mercury resonance radiation," Can. J. Phys. 49, 1976-1981 (1971).
[CrossRef]

1966 (1)

J. P. Barrat, D. Casalta, J. L. Cojan, and J. Hamel, "Depolarisation et (quenching) du niveau 63P1 du mercure lors de collisions avec des gaz etrangers," J. Phys. (Paris) 27, 608-618 (1966).
[CrossRef]

1964 (1)

A. J. Yarwood, O. P. Strausz, and H. E. Gunning, "Quenching of 2537-Å resonance radiation of mercury," J. Chem. Phys. 41, 1705-1713 (1964).
[CrossRef]

Barat, R. B.

R. B. Barat and A. T. Poulos, "Detection of mercury compounds in the gas phase by laser photofragmentation/emission spectroscopy," Appl. Spectrosc. 52, 1360-1363 (1998).

Barrat, J. P.

J. P. Barrat, D. Casalta, J. L. Cojan, and J. Hamel, "Depolarisation et (quenching) du niveau 63P1 du mercure lors de collisions avec des gaz etrangers," J. Phys. (Paris) 27, 608-618 (1966).
[CrossRef]

Calvert, J.

J. Calvert and J. Pitts, Photochemistry (Wiley, 1966), p. 74.

Casalta, D.

J. P. Barrat, D. Casalta, J. L. Cojan, and J. Hamel, "Depolarisation et (quenching) du niveau 63P1 du mercure lors de collisions avec des gaz etrangers," J. Phys. (Paris) 27, 608-618 (1966).
[CrossRef]

Chang, R.

G. Offen, N. Shick, R. Chang, P. Chu, C. Dene, and R. Rhudy, "Mercury controls for coal-fired power plants--status and challenges," Modern Power Syst. 25, 24-29 (2005).

Chu, P.

G. Offen, N. Shick, R. Chang, P. Chu, C. Dene, and R. Rhudy, "Mercury controls for coal-fired power plants--status and challenges," Modern Power Syst. 25, 24-29 (2005).

Cojan, J. L.

J. P. Barrat, D. Casalta, J. L. Cojan, and J. Hamel, "Depolarisation et (quenching) du niveau 63P1 du mercure lors de collisions avec des gaz etrangers," J. Phys. (Paris) 27, 608-618 (1966).
[CrossRef]

Cool, T. A.

T. A. Cool, J. A. McGarvey, Jr., and A. C. Erlandson, "Two-photon excitation of mercury atoms by photodissociation of mercury halides," Chem. Phys. Lett. 58, 108-113 (1978).
[CrossRef]

Cox, G.

G. Stark, P. L. Smith, J. Rufus, A. P. Thorne, J. C. Pickering, and G. Cox, "High-resolution photoabsorption cross-section measurements of SO2 at 295 K between 198 and 220 nm," J. Geophys. Res. 104, 16585-16590 (1999).
[CrossRef]

Curtis, L. J.

L. J. Curtis, R. E. Irving, M. Henderson, R. Matulioniene, C. F. Fischer, and E. H. Pinnington, "Measurements and predictions of the 6s6p1,3P1 lifetimes in the Hg isoelectronic sequence," Phys. Rev. A 63, 042502-1-7 (2001).
[CrossRef]

Deech, J. S.

J. S. Deech, J. Pitre, and L. Krause, "Quenching and depolarization of mercury resonance radiation," Can. J. Phys. 49, 1976-1981 (1971).
[CrossRef]

Dene, C.

G. Offen, N. Shick, R. Chang, P. Chu, C. Dene, and R. Rhudy, "Mercury controls for coal-fired power plants--status and challenges," Modern Power Syst. 25, 24-29 (2005).

Di Teodoro, F.

D. A. V. Kliner, F. Di Teodoro, J. P. Koplow, S. W. Moore, and A. V. Smith, "Efficient second, third, fourth, and fifth harmonic generation of a Yb-doped fiber amplifier," Opt. Commun. 210, 393-398 (2002).
[CrossRef]

Dillon, M. A.

D. Spence, R.-G. Wang, and M. A. Dillon, "Excitation of Rydberg states of HgCl2 and HgBr2 by electron impact," J. Chem. Phys. 82, 1883-1889 (1985).
[CrossRef]

D. Spence, R.-G. Wang, and M. A. Dillon, "Pseudo-optical absorption spectra in HgCl2 and HgBr2 from 4 to 14 eV," Appl. Phys. Lett. 41, 1021-1023 (1982).
[CrossRef]

Erlandson, A. C.

T. A. Cool, J. A. McGarvey, Jr., and A. C. Erlandson, "Two-photon excitation of mercury atoms by photodissociation of mercury halides," Chem. Phys. Lett. 58, 108-113 (1978).
[CrossRef]

Fischer, C. F.

L. J. Curtis, R. E. Irving, M. Henderson, R. Matulioniene, C. F. Fischer, and E. H. Pinnington, "Measurements and predictions of the 6s6p1,3P1 lifetimes in the Hg isoelectronic sequence," Phys. Rev. A 63, 042502-1-7 (2001).
[CrossRef]

Fthenakis, V. M.

V. M. Fthenakis, F. W. Lipfert, P. D. Moskowitz, and L. Saroff, "An assessment of mercury emissions and health risks from a coal-fired power plant," J. Hazard. Mater. 44, 267-283 (1995).
[CrossRef]

Gottwald, U.

U. Gottwald and P. Monkhouse, "Single-port optical access for spectroscopic measurements in industrial flue gas ducts," Appl. Phys. B 69, 151-154 (1999).
[CrossRef]

Gunning, H. E.

A. J. Yarwood, O. P. Strausz, and H. E. Gunning, "Quenching of 2537-Å resonance radiation of mercury," J. Chem. Phys. 41, 1705-1713 (1964).
[CrossRef]

Hamel, J.

J. P. Barrat, D. Casalta, J. L. Cojan, and J. Hamel, "Depolarisation et (quenching) du niveau 63P1 du mercure lors de collisions avec des gaz etrangers," J. Phys. (Paris) 27, 608-618 (1966).
[CrossRef]

Hammond, K.

J. Pitre, K. Hammond, and L. Krause, "63P1--63P0 excitation transfer in mercury, induced in collisions with N2 molecules," Phys. Rev. A 6, 2101-2106 (1972).
[CrossRef]

Helble, J. J.

C. L. Senior, J. J. Helble, and A. F. Sarofim, "Emissions of mercury, trace elements, and fine particles from stationary combustion devices," Fuel Process. Technol. 65-66, 263-288 (2000).
[CrossRef]

Henderson, M.

L. J. Curtis, R. E. Irving, M. Henderson, R. Matulioniene, C. F. Fischer, and E. H. Pinnington, "Measurements and predictions of the 6s6p1,3P1 lifetimes in the Hg isoelectronic sequence," Phys. Rev. A 63, 042502-1-7 (2001).
[CrossRef]

Hoops, A. A.

A. A. Hoops, Sandia National Laboratories, P. O. Box 969, MS 9056, Livermore, California 94551, and T. A. Reichardt are preparing a manuscript to be called "Time-resolved measurement of HgCl2 photofragment emission."

Horiguchi, H.

A. Sibata, M. Takahasi, H. Mikuni, H. Horiguchi, and S. Tsuchiya, "Chemiionization of excited mercury atom with 253.7 nm irradiation in the presence of N2 and CH4," Bull. Chem. Soc. Jpn. 52, 15-20 (1979).
[CrossRef]

H. Horiguchi and S. Tsuchiya, "Quenching of excited mercury atoms (63P1 and 63P0) in molecular collisions," Bull. Chem. Soc. Jpn. 47, 2768-2774 (1974).
[CrossRef]

Irving, R. E.

L. J. Curtis, R. E. Irving, M. Henderson, R. Matulioniene, C. F. Fischer, and E. H. Pinnington, "Measurements and predictions of the 6s6p1,3P1 lifetimes in the Hg isoelectronic sequence," Phys. Rev. A 63, 042502-1-7 (2001).
[CrossRef]

Kendrow, C. H.

P. Templet, J. R. McDonald, S. P. McGlynn, C. H. Kendrow, J. L. Roebber, and K. Weiss, "Ultraviolet absorption spectra of mercuric halides," J. Chem. Phys. 56, 5746 (1972).
[CrossRef]

King, T. A.

C. Whitehurst and T. A. King, "Multiphoton excitation of mercury atoms by photodissociation of HgX2 (X = Cl, Br, I)," J. Phys. B: At. Mol. Phys. 20, 4053-4064 (1987).
[CrossRef]

Kliner, D. A. V.

D. A. V. Kliner, F. Di Teodoro, J. P. Koplow, S. W. Moore, and A. V. Smith, "Efficient second, third, fourth, and fifth harmonic generation of a Yb-doped fiber amplifier," Opt. Commun. 210, 393-398 (2002).
[CrossRef]

Koplow, J. P.

D. A. V. Kliner, F. Di Teodoro, J. P. Koplow, S. W. Moore, and A. V. Smith, "Efficient second, third, fourth, and fifth harmonic generation of a Yb-doped fiber amplifier," Opt. Commun. 210, 393-398 (2002).
[CrossRef]

Krause, L.

J. Pitre, K. Hammond, and L. Krause, "63P1--63P0 excitation transfer in mercury, induced in collisions with N2 molecules," Phys. Rev. A 6, 2101-2106 (1972).
[CrossRef]

J. S. Deech, J. Pitre, and L. Krause, "Quenching and depolarization of mercury resonance radiation," Can. J. Phys. 49, 1976-1981 (1971).
[CrossRef]

Lipfert, F. W.

V. M. Fthenakis, F. W. Lipfert, P. D. Moskowitz, and L. Saroff, "An assessment of mercury emissions and health risks from a coal-fired power plant," J. Hazard. Mater. 44, 267-283 (1995).
[CrossRef]

Mandl, A.

C. Roxlo and A. Mandl, "Vacuum ultraviolet absorption cross sections for halogen containing molecules," J. Appl. Phys. 51, 2969-2972 (1980).
[CrossRef]

Matulioniene, R.

L. J. Curtis, R. E. Irving, M. Henderson, R. Matulioniene, C. F. Fischer, and E. H. Pinnington, "Measurements and predictions of the 6s6p1,3P1 lifetimes in the Hg isoelectronic sequence," Phys. Rev. A 63, 042502-1-7 (2001).
[CrossRef]

McDonald, J. R.

P. Templet, J. R. McDonald, S. P. McGlynn, C. H. Kendrow, J. L. Roebber, and K. Weiss, "Ultraviolet absorption spectra of mercuric halides," J. Chem. Phys. 56, 5746 (1972).
[CrossRef]

McGarvey, J. A.

T. A. Cool, J. A. McGarvey, Jr., and A. C. Erlandson, "Two-photon excitation of mercury atoms by photodissociation of mercury halides," Chem. Phys. Lett. 58, 108-113 (1978).
[CrossRef]

McGlynn, S. P.

P. Templet, J. R. McDonald, S. P. McGlynn, C. H. Kendrow, J. L. Roebber, and K. Weiss, "Ultraviolet absorption spectra of mercuric halides," J. Chem. Phys. 56, 5746 (1972).
[CrossRef]

Michael, J. V.

J. V. Michael and G. N. Suess, "Absolute quenching cross sections of Hg (3P1) with various molecules," J. Phys. Chem. 78, 482-487 (1974).
[CrossRef]

Mikuni, H.

A. Sibata, M. Takahasi, H. Mikuni, H. Horiguchi, and S. Tsuchiya, "Chemiionization of excited mercury atom with 253.7 nm irradiation in the presence of N2 and CH4," Bull. Chem. Soc. Jpn. 52, 15-20 (1979).
[CrossRef]

Monkhouse, P.

P. Monkhouse, "On-line diagnostic methods for metal species in industrial process gas," Prog. Energy Combust. Sci. 28, 331-381 (2002).
[CrossRef]

U. Gottwald and P. Monkhouse, "Single-port optical access for spectroscopic measurements in industrial flue gas ducts," Appl. Phys. B 69, 151-154 (1999).
[CrossRef]

Moore, S. W.

D. A. V. Kliner, F. Di Teodoro, J. P. Koplow, S. W. Moore, and A. V. Smith, "Efficient second, third, fourth, and fifth harmonic generation of a Yb-doped fiber amplifier," Opt. Commun. 210, 393-398 (2002).
[CrossRef]

Moskowitz, P. D.

V. M. Fthenakis, F. W. Lipfert, P. D. Moskowitz, and L. Saroff, "An assessment of mercury emissions and health risks from a coal-fired power plant," J. Hazard. Mater. 44, 267-283 (1995).
[CrossRef]

Offen, G.

G. Offen, N. Shick, R. Chang, P. Chu, C. Dene, and R. Rhudy, "Mercury controls for coal-fired power plants--status and challenges," Modern Power Syst. 25, 24-29 (2005).

Pickering, J. C.

G. Stark, P. L. Smith, J. Rufus, A. P. Thorne, J. C. Pickering, and G. Cox, "High-resolution photoabsorption cross-section measurements of SO2 at 295 K between 198 and 220 nm," J. Geophys. Res. 104, 16585-16590 (1999).
[CrossRef]

Pinnington, E. H.

L. J. Curtis, R. E. Irving, M. Henderson, R. Matulioniene, C. F. Fischer, and E. H. Pinnington, "Measurements and predictions of the 6s6p1,3P1 lifetimes in the Hg isoelectronic sequence," Phys. Rev. A 63, 042502-1-7 (2001).
[CrossRef]

Pitre, J.

J. Pitre, K. Hammond, and L. Krause, "63P1--63P0 excitation transfer in mercury, induced in collisions with N2 molecules," Phys. Rev. A 6, 2101-2106 (1972).
[CrossRef]

J. S. Deech, J. Pitre, and L. Krause, "Quenching and depolarization of mercury resonance radiation," Can. J. Phys. 49, 1976-1981 (1971).
[CrossRef]

Pitts, J.

J. Calvert and J. Pitts, Photochemistry (Wiley, 1966), p. 74.

Poulos, A. T.

R. B. Barat and A. T. Poulos, "Detection of mercury compounds in the gas phase by laser photofragmentation/emission spectroscopy," Appl. Spectrosc. 52, 1360-1363 (1998).

Rhudy, R.

G. Offen, N. Shick, R. Chang, P. Chu, C. Dene, and R. Rhudy, "Mercury controls for coal-fired power plants--status and challenges," Modern Power Syst. 25, 24-29 (2005).

Roebber, J. L.

P. Templet, J. R. McDonald, S. P. McGlynn, C. H. Kendrow, J. L. Roebber, and K. Weiss, "Ultraviolet absorption spectra of mercuric halides," J. Chem. Phys. 56, 5746 (1972).
[CrossRef]

Roxlo, C.

C. Roxlo and A. Mandl, "Vacuum ultraviolet absorption cross sections for halogen containing molecules," J. Appl. Phys. 51, 2969-2972 (1980).
[CrossRef]

Rufus, J.

G. Stark, P. L. Smith, J. Rufus, A. P. Thorne, J. C. Pickering, and G. Cox, "High-resolution photoabsorption cross-section measurements of SO2 at 295 K between 198 and 220 nm," J. Geophys. Res. 104, 16585-16590 (1999).
[CrossRef]

Saroff, L.

V. M. Fthenakis, F. W. Lipfert, P. D. Moskowitz, and L. Saroff, "An assessment of mercury emissions and health risks from a coal-fired power plant," J. Hazard. Mater. 44, 267-283 (1995).
[CrossRef]

Sarofim, A. F.

C. L. Senior, J. J. Helble, and A. F. Sarofim, "Emissions of mercury, trace elements, and fine particles from stationary combustion devices," Fuel Process. Technol. 65-66, 263-288 (2000).
[CrossRef]

Sausa, R. C.

J. B. Simeonsson and R. C. Sausa, "A critical review of laser photofragmentation/fragment detection techniques for gas-phase chemical analysis," Appl. Spectrosc. Rev. 31, 1-72 (1996).
[CrossRef]

Senior, C. L.

C. L. Senior, J. J. Helble, and A. F. Sarofim, "Emissions of mercury, trace elements, and fine particles from stationary combustion devices," Fuel Process. Technol. 65-66, 263-288 (2000).
[CrossRef]

Shick, N.

G. Offen, N. Shick, R. Chang, P. Chu, C. Dene, and R. Rhudy, "Mercury controls for coal-fired power plants--status and challenges," Modern Power Syst. 25, 24-29 (2005).

Sibata, A.

A. Sibata, M. Takahasi, H. Mikuni, H. Horiguchi, and S. Tsuchiya, "Chemiionization of excited mercury atom with 253.7 nm irradiation in the presence of N2 and CH4," Bull. Chem. Soc. Jpn. 52, 15-20 (1979).
[CrossRef]

Simeonsson, J. B.

J. B. Simeonsson and R. C. Sausa, "A critical review of laser photofragmentation/fragment detection techniques for gas-phase chemical analysis," Appl. Spectrosc. Rev. 31, 1-72 (1996).
[CrossRef]

Smith, A. V.

D. A. V. Kliner, F. Di Teodoro, J. P. Koplow, S. W. Moore, and A. V. Smith, "Efficient second, third, fourth, and fifth harmonic generation of a Yb-doped fiber amplifier," Opt. Commun. 210, 393-398 (2002).
[CrossRef]

Smith, P. L.

G. Stark, P. L. Smith, J. Rufus, A. P. Thorne, J. C. Pickering, and G. Cox, "High-resolution photoabsorption cross-section measurements of SO2 at 295 K between 198 and 220 nm," J. Geophys. Res. 104, 16585-16590 (1999).
[CrossRef]

Spence, D.

D. Spence, R.-G. Wang, and M. A. Dillon, "Excitation of Rydberg states of HgCl2 and HgBr2 by electron impact," J. Chem. Phys. 82, 1883-1889 (1985).
[CrossRef]

D. Spence, R.-G. Wang, and M. A. Dillon, "Pseudo-optical absorption spectra in HgCl2 and HgBr2 from 4 to 14 eV," Appl. Phys. Lett. 41, 1021-1023 (1982).
[CrossRef]

Stark, G.

G. Stark, P. L. Smith, J. Rufus, A. P. Thorne, J. C. Pickering, and G. Cox, "High-resolution photoabsorption cross-section measurements of SO2 at 295 K between 198 and 220 nm," J. Geophys. Res. 104, 16585-16590 (1999).
[CrossRef]

Strausz, O. P.

A. J. Yarwood, O. P. Strausz, and H. E. Gunning, "Quenching of 2537-Å resonance radiation of mercury," J. Chem. Phys. 41, 1705-1713 (1964).
[CrossRef]

Suess, G. N.

J. V. Michael and G. N. Suess, "Absolute quenching cross sections of Hg (3P1) with various molecules," J. Phys. Chem. 78, 482-487 (1974).
[CrossRef]

Takahasi, M.

A. Sibata, M. Takahasi, H. Mikuni, H. Horiguchi, and S. Tsuchiya, "Chemiionization of excited mercury atom with 253.7 nm irradiation in the presence of N2 and CH4," Bull. Chem. Soc. Jpn. 52, 15-20 (1979).
[CrossRef]

Templet, P.

P. Templet, J. R. McDonald, S. P. McGlynn, C. H. Kendrow, J. L. Roebber, and K. Weiss, "Ultraviolet absorption spectra of mercuric halides," J. Chem. Phys. 56, 5746 (1972).
[CrossRef]

Thorne, A. P.

G. Stark, P. L. Smith, J. Rufus, A. P. Thorne, J. C. Pickering, and G. Cox, "High-resolution photoabsorption cross-section measurements of SO2 at 295 K between 198 and 220 nm," J. Geophys. Res. 104, 16585-16590 (1999).
[CrossRef]

Tsuchiya, S.

A. Sibata, M. Takahasi, H. Mikuni, H. Horiguchi, and S. Tsuchiya, "Chemiionization of excited mercury atom with 253.7 nm irradiation in the presence of N2 and CH4," Bull. Chem. Soc. Jpn. 52, 15-20 (1979).
[CrossRef]

H. Horiguchi and S. Tsuchiya, "Quenching of excited mercury atoms (63P1 and 63P0) in molecular collisions," Bull. Chem. Soc. Jpn. 47, 2768-2774 (1974).
[CrossRef]

Wadt, W. R.

W. R. Wadt, "The electronic structure of HgCl2 and HgBr2 and its relationship to photodissociation," J. Chem. Phys. 72, 2469-2478 (1980).
[CrossRef]

W. R. Wadt, "The electronic structure of HgCl and HgBr," Appl. Phys. Lett. 34, 658-660 (1979).
[CrossRef]

Wang, R.-G.

D. Spence, R.-G. Wang, and M. A. Dillon, "Excitation of Rydberg states of HgCl2 and HgBr2 by electron impact," J. Chem. Phys. 82, 1883-1889 (1985).
[CrossRef]

D. Spence, R.-G. Wang, and M. A. Dillon, "Pseudo-optical absorption spectra in HgCl2 and HgBr2 from 4 to 14 eV," Appl. Phys. Lett. 41, 1021-1023 (1982).
[CrossRef]

Weast, R. C.

R. C. Weast, ed., CRC Handbook of Chemistry and Physics, 67th ed. (CRC Press, 1986).

Weiss, K.

P. Templet, J. R. McDonald, S. P. McGlynn, C. H. Kendrow, J. L. Roebber, and K. Weiss, "Ultraviolet absorption spectra of mercuric halides," J. Chem. Phys. 56, 5746 (1972).
[CrossRef]

Whitehurst, C.

C. Whitehurst and T. A. King, "Multiphoton excitation of mercury atoms by photodissociation of HgX2 (X = Cl, Br, I)," J. Phys. B: At. Mol. Phys. 20, 4053-4064 (1987).
[CrossRef]

Yarwood, A. J.

A. J. Yarwood, O. P. Strausz, and H. E. Gunning, "Quenching of 2537-Å resonance radiation of mercury," J. Chem. Phys. 41, 1705-1713 (1964).
[CrossRef]

Appl. Phys. B (1)

U. Gottwald and P. Monkhouse, "Single-port optical access for spectroscopic measurements in industrial flue gas ducts," Appl. Phys. B 69, 151-154 (1999).
[CrossRef]

Appl. Phys. Lett. (2)

D. Spence, R.-G. Wang, and M. A. Dillon, "Pseudo-optical absorption spectra in HgCl2 and HgBr2 from 4 to 14 eV," Appl. Phys. Lett. 41, 1021-1023 (1982).
[CrossRef]

W. R. Wadt, "The electronic structure of HgCl and HgBr," Appl. Phys. Lett. 34, 658-660 (1979).
[CrossRef]

Appl. Spectrosc. (1)

R. B. Barat and A. T. Poulos, "Detection of mercury compounds in the gas phase by laser photofragmentation/emission spectroscopy," Appl. Spectrosc. 52, 1360-1363 (1998).

Appl. Spectrosc. Rev. (1)

J. B. Simeonsson and R. C. Sausa, "A critical review of laser photofragmentation/fragment detection techniques for gas-phase chemical analysis," Appl. Spectrosc. Rev. 31, 1-72 (1996).
[CrossRef]

Bull. Chem. Soc. Jpn. (2)

A. Sibata, M. Takahasi, H. Mikuni, H. Horiguchi, and S. Tsuchiya, "Chemiionization of excited mercury atom with 253.7 nm irradiation in the presence of N2 and CH4," Bull. Chem. Soc. Jpn. 52, 15-20 (1979).
[CrossRef]

H. Horiguchi and S. Tsuchiya, "Quenching of excited mercury atoms (63P1 and 63P0) in molecular collisions," Bull. Chem. Soc. Jpn. 47, 2768-2774 (1974).
[CrossRef]

Can. J. Phys. (1)

J. S. Deech, J. Pitre, and L. Krause, "Quenching and depolarization of mercury resonance radiation," Can. J. Phys. 49, 1976-1981 (1971).
[CrossRef]

Chem. Phys. Lett. (1)

T. A. Cool, J. A. McGarvey, Jr., and A. C. Erlandson, "Two-photon excitation of mercury atoms by photodissociation of mercury halides," Chem. Phys. Lett. 58, 108-113 (1978).
[CrossRef]

Fuel Process. Technol. (1)

C. L. Senior, J. J. Helble, and A. F. Sarofim, "Emissions of mercury, trace elements, and fine particles from stationary combustion devices," Fuel Process. Technol. 65-66, 263-288 (2000).
[CrossRef]

J. Appl. Phys. (1)

C. Roxlo and A. Mandl, "Vacuum ultraviolet absorption cross sections for halogen containing molecules," J. Appl. Phys. 51, 2969-2972 (1980).
[CrossRef]

J. Chem. Phys. (4)

P. Templet, J. R. McDonald, S. P. McGlynn, C. H. Kendrow, J. L. Roebber, and K. Weiss, "Ultraviolet absorption spectra of mercuric halides," J. Chem. Phys. 56, 5746 (1972).
[CrossRef]

D. Spence, R.-G. Wang, and M. A. Dillon, "Excitation of Rydberg states of HgCl2 and HgBr2 by electron impact," J. Chem. Phys. 82, 1883-1889 (1985).
[CrossRef]

W. R. Wadt, "The electronic structure of HgCl2 and HgBr2 and its relationship to photodissociation," J. Chem. Phys. 72, 2469-2478 (1980).
[CrossRef]

A. J. Yarwood, O. P. Strausz, and H. E. Gunning, "Quenching of 2537-Å resonance radiation of mercury," J. Chem. Phys. 41, 1705-1713 (1964).
[CrossRef]

J. Geophys. Res. (1)

G. Stark, P. L. Smith, J. Rufus, A. P. Thorne, J. C. Pickering, and G. Cox, "High-resolution photoabsorption cross-section measurements of SO2 at 295 K between 198 and 220 nm," J. Geophys. Res. 104, 16585-16590 (1999).
[CrossRef]

J. Hazard. Mater. (1)

V. M. Fthenakis, F. W. Lipfert, P. D. Moskowitz, and L. Saroff, "An assessment of mercury emissions and health risks from a coal-fired power plant," J. Hazard. Mater. 44, 267-283 (1995).
[CrossRef]

J. Phys. (1)

J. P. Barrat, D. Casalta, J. L. Cojan, and J. Hamel, "Depolarisation et (quenching) du niveau 63P1 du mercure lors de collisions avec des gaz etrangers," J. Phys. (Paris) 27, 608-618 (1966).
[CrossRef]

J. Phys. B: At. Mol. Phys. (1)

C. Whitehurst and T. A. King, "Multiphoton excitation of mercury atoms by photodissociation of HgX2 (X = Cl, Br, I)," J. Phys. B: At. Mol. Phys. 20, 4053-4064 (1987).
[CrossRef]

J. Phys. Chem. (1)

J. V. Michael and G. N. Suess, "Absolute quenching cross sections of Hg (3P1) with various molecules," J. Phys. Chem. 78, 482-487 (1974).
[CrossRef]

Modern Power Syst. (1)

G. Offen, N. Shick, R. Chang, P. Chu, C. Dene, and R. Rhudy, "Mercury controls for coal-fired power plants--status and challenges," Modern Power Syst. 25, 24-29 (2005).

Opt. Commun. (1)

D. A. V. Kliner, F. Di Teodoro, J. P. Koplow, S. W. Moore, and A. V. Smith, "Efficient second, third, fourth, and fifth harmonic generation of a Yb-doped fiber amplifier," Opt. Commun. 210, 393-398 (2002).
[CrossRef]

Phys. Rev. A (2)

J. Pitre, K. Hammond, and L. Krause, "63P1--63P0 excitation transfer in mercury, induced in collisions with N2 molecules," Phys. Rev. A 6, 2101-2106 (1972).
[CrossRef]

L. J. Curtis, R. E. Irving, M. Henderson, R. Matulioniene, C. F. Fischer, and E. H. Pinnington, "Measurements and predictions of the 6s6p1,3P1 lifetimes in the Hg isoelectronic sequence," Phys. Rev. A 63, 042502-1-7 (2001).
[CrossRef]

Prog. Energy Combust. Sci. (1)

P. Monkhouse, "On-line diagnostic methods for metal species in industrial process gas," Prog. Energy Combust. Sci. 28, 331-381 (2002).
[CrossRef]

Other (4)

R. C. Weast, ed., CRC Handbook of Chemistry and Physics, 67th ed. (CRC Press, 1986).

J. Calvert and J. Pitts, Photochemistry (Wiley, 1966), p. 74.

The N2 Raman cross section was calculated from the information provided by A. C. Eckbreth, Laser Diagnostics for Combustion Temperature and Species, 2nd ed. (Gordon and Breach, 1996), Chap. 5. The N2 depolarization ratio is 0.024.

A. A. Hoops, Sandia National Laboratories, P. O. Box 969, MS 9056, Livermore, California 94551, and T. A. Reichardt are preparing a manuscript to be called "Time-resolved measurement of HgCl2 photofragment emission."

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Figures (5)

Fig. 1
Fig. 1

Energy-level diagram for HgCl 2 and dissociation product states relative to HgCl 2 ( 1 Σ g + 1 ) . The peaks of the transitions to excited levels of HgCl 2 are represented by solid lines, while the gray shaded regions indicate the energies spanned by the bands from Ref. 10. Electronic state correlations from Ref. 11 are depicted by dashed lines.

Fig. 2
Fig. 2

Emission collection optics.

Fig. 3
Fig. 3

Dispersed spectra of the HgCl 2 PFE signal. (a) Hg ( 6 P 1 3 6 S 0 1 ) transition in 760 Torr N 2 . (b) HgCl ( B Σ + 2 X Σ + 2 ) transition in 6   Torr   N 2 .

Fig. 4
Fig. 4

HgCl 2 PFE signal as a function of buffer gas pressure at 23 ° C . The experimental data points (●, ■, ▾) are the result of averaging 1000 laser shots, and the solid curves are the fits of these data to Eq. (1).

Fig. 5
Fig. 5

HgCl 2 PFE from the Hg ( 6 P 1 3 6 S 0 1 ) transition and N 2 Raman scattering as recorded with the spectrograph channel using vertically polarized light at 209.8   nm . The spectrum is composed of 500 laser shots.

Tables (1)

Tables Icon

Table 1 Quenching Rate Constants Measured by Fitting the HgCl2 PFE Signal Intensity as a Function of Buffer Gas Pressure to Eq. (1) versus Literature Values for Hg (6 3 P 1 → 6 1 S 0) Emission

Equations (5)

Equations on this page are rendered with MathJax. Learn more.

S j ( A + Q ) 1 ,
Q = i Q i .
Q i = N i v i j σ i j ,
σ PFE , 760   Torr   N 2 = σ N 2   Raman ( S PFE S N 2   Raman ) ( N N 2 N HgCl 2 ) = 1.0 ( ± 0.2 ) × 10 25 m 2 .
σ PFE = σ PFE , 760   Torr   N 2 ( A + Q 760   Torr   N 2 A + Q ) .

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