Abstract

Time-resolved Raman spectroscopy is evaluated as a tool for studying reactions in aerosol microdroplets. As a test reaction, the absorption of D2O vapor by an optically levitated glycerol droplet is considered. With the present apparatus, time scales of the order of 1 s have been resolved. By considering the relative amplitude of various features, the composition of the suspended droplet can be estimated as a function of time. In addition, for the D2O–glycerol system the average temperature of the optically levitated droplet can be deduced.

© 1990 Optical Society of America

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References

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  1. W. F. Hsieh, J. B. Zheng, C. F. Wood, B. T. Chu, R. K. Chang, “Propagation Velocity of Laser-Induced Plasma Inside and Outside a Transparent Droplet,” Opt. Lett. 12, 576–578 (1987).
    [Crossref] [PubMed]
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    [Crossref]
  3. S. Ataman, D. Hanson, “Measurement of Charged Drops,” Ind. Eng. Chem. Fundam. 8, 833–836 (1969).
    [Crossref]
  4. G. O. Rubel, “Evaporation of Single Aerosol Binary Oil Droplets,” J. Colloid Interface Sci. 85, 549–555 (1982).
    [Crossref]
  5. I. N. Tang, H. R. Munkelwitz, “An Investigation of Solute Nucleation in Levitated Solution Droplets,” J. Colloid Interface Sci. 98, 430–438 (1984).
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    [Crossref]
  7. R. Thurn, W. Kiefer, “Raman-Microsampling Technique Applying Optical Levitation by Radiation Pressure,” Appl. Spectrosc. 38, 78–83 (1984).
    [Crossref]
  8. R. Thurn, W. Kiefer, “Structural Resonances Observed in the Raman Spectra of Optically Levitated Liquid Droplets,” Appl. Opt. 24, 1515– (1985).
    [Crossref] [PubMed]
  9. T. R. Lettieri, R. E. Preston, “Observation of Sharp Resonances in the Spontaneous Raman Spectrum of a Single Optically Levitated Microdroplet,” Opt. Commun. 54, 349–352 (1985).
    [Crossref]
  10. K. H. Fung, I. N. Tang, “Raman Scattering from Single Solution Droplets,” Appl. Opt. 27, 206–208 (1988).
    [Crossref] [PubMed]
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    [Crossref]
  14. D. V. Fenby, G. L. Bertrand, “Statistical Mechanics of Deuterium Exchange Reactions: Relationships Between Equilibrium Constants and Enthalpies of Reaction,” Aust. J. Chem. 35, 237–245 (1982).
    [Crossref]
  15. I. Weinberg, J. R. Zimmerman, “Concentration Dependence of Chemical Exchange and NMR Multiplet Structure in Water-Ethanol Mixtures,” J. Chem. Phys. 23, 748–749 (1955).
    [Crossref]
  16. N. S. Isaac, Physical Organic Chemistry (Wiley, New York, 1987).
  17. A. R. Carr, R. E. Townsend, W. L. Badger, “Vapor Pressures of Glycerol–Water and Glycerol–Water–Sodium Chloride Systems,” Ind. Eng. Chem. 17, 643–646 (1925).
    [Crossref]

1988 (1)

1987 (2)

G. S. Grader, R. C. Flagan, J. H. Seinfeld, “Fourier transform infrared spectroscopy of a single aerosol particle,” Rev. Sci. Instrum. 58, 584–587 (1987).
[Crossref]

W. F. Hsieh, J. B. Zheng, C. F. Wood, B. T. Chu, R. K. Chang, “Propagation Velocity of Laser-Induced Plasma Inside and Outside a Transparent Droplet,” Opt. Lett. 12, 576–578 (1987).
[Crossref] [PubMed]

1986 (1)

1985 (3)

1984 (3)

1982 (2)

G. O. Rubel, “Evaporation of Single Aerosol Binary Oil Droplets,” J. Colloid Interface Sci. 85, 549–555 (1982).
[Crossref]

D. V. Fenby, G. L. Bertrand, “Statistical Mechanics of Deuterium Exchange Reactions: Relationships Between Equilibrium Constants and Enthalpies of Reaction,” Aust. J. Chem. 35, 237–245 (1982).
[Crossref]

1971 (1)

A. Ashkin, J. M. Dziedzic, “Optical Levitation by Radiation Pressure,” Appl. Phys. Lett. 19, 283–285 (1971).
[Crossref]

1969 (1)

S. Ataman, D. Hanson, “Measurement of Charged Drops,” Ind. Eng. Chem. Fundam. 8, 833–836 (1969).
[Crossref]

1955 (1)

I. Weinberg, J. R. Zimmerman, “Concentration Dependence of Chemical Exchange and NMR Multiplet Structure in Water-Ethanol Mixtures,” J. Chem. Phys. 23, 748–749 (1955).
[Crossref]

1925 (1)

A. R. Carr, R. E. Townsend, W. L. Badger, “Vapor Pressures of Glycerol–Water and Glycerol–Water–Sodium Chloride Systems,” Ind. Eng. Chem. 17, 643–646 (1925).
[Crossref]

Arnold, S.

Ashkin, A.

A. Ashkin, J. M. Dziedzic, “Optical Levitation by Radiation Pressure,” Appl. Phys. Lett. 19, 283–285 (1971).
[Crossref]

Ataman, S.

S. Ataman, D. Hanson, “Measurement of Charged Drops,” Ind. Eng. Chem. Fundam. 8, 833–836 (1969).
[Crossref]

Badger, W. L.

A. R. Carr, R. E. Townsend, W. L. Badger, “Vapor Pressures of Glycerol–Water and Glycerol–Water–Sodium Chloride Systems,” Ind. Eng. Chem. 17, 643–646 (1925).
[Crossref]

Bertrand, G. L.

D. V. Fenby, G. L. Bertrand, “Statistical Mechanics of Deuterium Exchange Reactions: Relationships Between Equilibrium Constants and Enthalpies of Reaction,” Aust. J. Chem. 35, 237–245 (1982).
[Crossref]

Campillo, A. J.

Carr, A. R.

A. R. Carr, R. E. Townsend, W. L. Badger, “Vapor Pressures of Glycerol–Water and Glycerol–Water–Sodium Chloride Systems,” Ind. Eng. Chem. 17, 643–646 (1925).
[Crossref]

Chang, R. K.

Chu, B. T.

Dziedzic, J. M.

A. Ashkin, J. M. Dziedzic, “Optical Levitation by Radiation Pressure,” Appl. Phys. Lett. 19, 283–285 (1971).
[Crossref]

Fenby, D. V.

D. V. Fenby, G. L. Bertrand, “Statistical Mechanics of Deuterium Exchange Reactions: Relationships Between Equilibrium Constants and Enthalpies of Reaction,” Aust. J. Chem. 35, 237–245 (1982).
[Crossref]

Flagan, R. C.

G. S. Grader, R. C. Flagan, J. H. Seinfeld, “Fourier transform infrared spectroscopy of a single aerosol particle,” Rev. Sci. Instrum. 58, 584–587 (1987).
[Crossref]

Fung, K. H.

Grader, G. S.

G. S. Grader, R. C. Flagan, J. H. Seinfeld, “Fourier transform infrared spectroscopy of a single aerosol particle,” Rev. Sci. Instrum. 58, 584–587 (1987).
[Crossref]

Hanson, D.

S. Ataman, D. Hanson, “Measurement of Charged Drops,” Ind. Eng. Chem. Fundam. 8, 833–836 (1969).
[Crossref]

Hsieh, W. F.

Isaac, N. S.

N. S. Isaac, Physical Organic Chemistry (Wiley, New York, 1987).

Kiefer, W.

Lettieri, T. R.

T. R. Lettieri, R. E. Preston, “Observation of Sharp Resonances in the Spontaneous Raman Spectrum of a Single Optically Levitated Microdroplet,” Opt. Commun. 54, 349–352 (1985).
[Crossref]

Lin, H. B.

Munkelwitz, H. R.

I. N. Tang, H. R. Munkelwitz, “An Investigation of Solute Nucleation in Levitated Solution Droplets,” J. Colloid Interface Sci. 98, 430–438 (1984).

Neuman, M.

Pluchino, A.

Preston, R. E.

T. R. Lettieri, R. E. Preston, “Observation of Sharp Resonances in the Spontaneous Raman Spectrum of a Single Optically Levitated Microdroplet,” Opt. Commun. 54, 349–352 (1985).
[Crossref]

Qian, S. X.

Rubel, G. O.

G. O. Rubel, “Evaporation of Single Aerosol Binary Oil Droplets,” J. Colloid Interface Sci. 85, 549–555 (1982).
[Crossref]

Seinfeld, J. H.

G. S. Grader, R. C. Flagan, J. H. Seinfeld, “Fourier transform infrared spectroscopy of a single aerosol particle,” Rev. Sci. Instrum. 58, 584–587 (1987).
[Crossref]

Snow, J. B.

Tang, I. N.

K. H. Fung, I. N. Tang, “Raman Scattering from Single Solution Droplets,” Appl. Opt. 27, 206–208 (1988).
[Crossref] [PubMed]

I. N. Tang, H. R. Munkelwitz, “An Investigation of Solute Nucleation in Levitated Solution Droplets,” J. Colloid Interface Sci. 98, 430–438 (1984).

Thurn, R.

Townsend, R. E.

A. R. Carr, R. E. Townsend, W. L. Badger, “Vapor Pressures of Glycerol–Water and Glycerol–Water–Sodium Chloride Systems,” Ind. Eng. Chem. 17, 643–646 (1925).
[Crossref]

Weinberg, I.

I. Weinberg, J. R. Zimmerman, “Concentration Dependence of Chemical Exchange and NMR Multiplet Structure in Water-Ethanol Mixtures,” J. Chem. Phys. 23, 748–749 (1955).
[Crossref]

Wood, C. F.

Zheng, J. B.

Zimmerman, J. R.

I. Weinberg, J. R. Zimmerman, “Concentration Dependence of Chemical Exchange and NMR Multiplet Structure in Water-Ethanol Mixtures,” J. Chem. Phys. 23, 748–749 (1955).
[Crossref]

Appl. Opt. (3)

Appl. Phys. Lett. (1)

A. Ashkin, J. M. Dziedzic, “Optical Levitation by Radiation Pressure,” Appl. Phys. Lett. 19, 283–285 (1971).
[Crossref]

Appl. Spectrosc. (1)

Aust. J. Chem. (1)

D. V. Fenby, G. L. Bertrand, “Statistical Mechanics of Deuterium Exchange Reactions: Relationships Between Equilibrium Constants and Enthalpies of Reaction,” Aust. J. Chem. 35, 237–245 (1982).
[Crossref]

Ind. Eng. Chem. (1)

A. R. Carr, R. E. Townsend, W. L. Badger, “Vapor Pressures of Glycerol–Water and Glycerol–Water–Sodium Chloride Systems,” Ind. Eng. Chem. 17, 643–646 (1925).
[Crossref]

Ind. Eng. Chem. Fundam. (1)

S. Ataman, D. Hanson, “Measurement of Charged Drops,” Ind. Eng. Chem. Fundam. 8, 833–836 (1969).
[Crossref]

J. Chem. Phys. (1)

I. Weinberg, J. R. Zimmerman, “Concentration Dependence of Chemical Exchange and NMR Multiplet Structure in Water-Ethanol Mixtures,” J. Chem. Phys. 23, 748–749 (1955).
[Crossref]

J. Colloid Interface Sci. (2)

G. O. Rubel, “Evaporation of Single Aerosol Binary Oil Droplets,” J. Colloid Interface Sci. 85, 549–555 (1982).
[Crossref]

I. N. Tang, H. R. Munkelwitz, “An Investigation of Solute Nucleation in Levitated Solution Droplets,” J. Colloid Interface Sci. 98, 430–438 (1984).

Opt. Commun. (1)

T. R. Lettieri, R. E. Preston, “Observation of Sharp Resonances in the Spontaneous Raman Spectrum of a Single Optically Levitated Microdroplet,” Opt. Commun. 54, 349–352 (1985).
[Crossref]

Opt. Lett. (3)

Rev. Sci. Instrum. (1)

G. S. Grader, R. C. Flagan, J. H. Seinfeld, “Fourier transform infrared spectroscopy of a single aerosol particle,” Rev. Sci. Instrum. 58, 584–587 (1987).
[Crossref]

Other (1)

N. S. Isaac, Physical Organic Chemistry (Wiley, New York, 1987).

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Figures (7)

Fig. 1
Fig. 1

Raman spectra of dioctyl phthalate (DOP): upper trace, bulk DOP; lower trace, optically levitated DOP droplet.

Fig. 2
Fig. 2

Raman spectra of glycerol: upper trace, bulk glycerol; lower trace, optically levitated glycerol droplet.

Fig. 3
Fig. 3

Upper trace, Raman spectrum of bulk deuterium oxide (D2O); lower trace, Raman spectrum of optically levitated droplet composed of a 50–50 volume % mixture of D2O and glycerol.

Fig. 4
Fig. 4

Time-resolved sequence of droplet Raman spectra during the absorption of D2O by an optically levitated glycerol droplet; 1200-gr/mm grating.

Fig. 5
Fig. 5

Time-resolved sequence of droplet Raman spectra during the absorption of D2O by an optically levitated glycerol droplet; 2400-gr/mm grating.

Fig. 6
Fig. 6

(a) Integral of OD Raman peak as a function of time for absorption of D2O by an optically levitated glycerol droplet, (b) integral of CH Raman peak vs time, (c) area ratio of OD:CH Raman peak vs time.

Fig. 7
Fig. 7

Calibration data for bulk samples of glycerol–D2O mixtures giving relationship of area ratios of OD:CH Raman peaks to number ratios of OD:CH bonds in samples.

Equations (3)

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# ratio OD : CH = X D 2 O ( 2 O - D bonds molecule D 2 O ) X gly ( 5 C - H bonds molecule gly ) .
2 C 3 H 5 ( OH ) 3 + 3 D 2 O 2 C 3 H 5 ( OD ) 3 + 3 H 2 O
H 2 O + D 2 O 2 HDO

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