Abstract

A form of optical second-harmonic microscopy has been developed that spatially resolves concentration gradients of surface adsorbates. Surface concentration profiles at submonolayer levels are illuminated with a pulsed laser, and the reflected second-harmonic light is imaged into a photodiode array. Micrometer-scale resolution is obtainable while the surface damage and the spurious chemistry induced by more conventional electron- or ion-based techniques are avoided. We have used this microscopy to monitor the surface diffusion of Sb on Ge(111).

© 1993 Optical Society of America

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References

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  1. Y. R. Shen, “Surface studies by optical second harmonic generation: an overview,” J. Vac. Sci. Technol. B 3, 1464–1466 (1985).
    [Crossref]
  2. G. L. Richmond, J. M. Robinson, and V. L. Shannon, “Second harmonic generation studies of interfacial structure and dynamics,” Prog. Surf. Sci. 281–70 (1988), and references therein.
    [Crossref]
  3. T. F. Heinz and M. M. T. Loy, “Optical second harmonic generation from semiconductor surfaces,” in Advances in Laser Science III, A. C. Tam, J. L. Gole, and W. C. Stwalley, eds. (American Institute of Physics, New York, 1988), pp. 452–459, and references therein.
  4. T. Stehlin, M. Feller, P. Guyot-Sionnest, and Y. R. Shen, “Optical second harmonic generation as a surface probe for noncentrosymmetric media,” Opt. Lett. 13, 389–391 (1988).
    [Crossref]
  5. R. J. Pressley, ed., Handbook of Lasers (CRC, Cleveland, Ohio, 1971), p. 489.
  6. V. T. Binh, ed., Surface Mobilities on Solid Materials–Fundamental Concepts and Applications (Plenum, New York, 1983).
    [Crossref]
  7. G. T. Boyd, Y. R. Shen, and T. W. Hänsch, “Continuous-wave second harmonic generation as a surface microprobe,” Opt. Lett. 11, 97–99 (1986).
    [Crossref]
  8. V. P. Kesan, S. S. Iyer, and J. M. Cotte, “Dopant Incorporation in epitaxial germanium growth on Ge(100) substrates by MBE,” J. Cryst. Growth 111, 847–855 (1991).
    [Crossref]
  9. J. M. C. Thornton, A. A. Williams, J. E. Macdonald, R. G. van Siefhout, J. F. van der Veen, M. Finney, and C. Norris, “The influence of Sb as a surfactant on the strain relaxation of Ge/Si(001),” J. Vac. Sci. Technol. B 9, 2146–2149 (1991).
    [Crossref]
  10. J. Crank, The Mathematics of Diffusion (Clarendon, Oxford, 1975), p. 104.
  11. X. D. Zhu, T. Rasing, and Y. R. Shen, “Surface diffusion of CO on Ni(111) studied by diffraction of optical second-harmonic generation of a monolayer grating,” Phys. Rev. Lett. 66, 2883–2885 (1988).
    [Crossref]
  12. G. A. Reider, U. Höfer, and T. F. Heinz, “Surface diffusion of hydrogen on Si(111) 7×7,” Phys. Rev. Lett. 66, 1994–1997 (1991).
    [Crossref] [PubMed]
  13. E. G. Seebauer, A. C. F. Kong, and L. D. Schmidt, “Adsorption and desorption of NO, CO, and H2on Pt(111): laser-induced thermal desorption studies,” Surf. Sci. 176, 134–156 (1986).
    [Crossref]
  14. K. A. Schultz, I. I. Suni, C. E. Allen, and E. G. Seebauer, “Optical second harmonic study of Sb adsorption on Ge(111),” Surf. Sci. 276, 40–49 (1992).
    [Crossref]
  15. K. A. Schultz and E. G. Seebauer, “Low-stress, coolable sample mount for ultrahigh vacuum studies of fragile semiconductors,” Rev. Sci. Instrum. 63, 218–219 (1992).
    [Crossref]
  16. M. T. Keif, product Rep. (MDC Corporation, Hayward, Calif., 1989).
  17. R. Reinisch and M. Neviére, “Electromagnetic theory of diffraction in nonlinear optics and surface-enhanced nonlinear optical effects,” Phys. Rev. B 28, 1870–1882 (1983).
    [Crossref]
  18. P. S. Considine, “Effects of coherence on imaging systems,” J. Opt. Soc. Am. 56, 1001–1009 (1966).
    [Crossref]
  19. W. N. Charman, “Some experimental measurements of diffraction images in low-resolution microscopy,” J. Opt. Soc. Am. 53, 410–414 (1963).
    [Crossref]
  20. R. Kingslake, Optical System Design (Academic, New York, 1983), p. 196.
  21. G. W. Stroke and R. G. Zech, “A posteriori image-correcting deconvolution by holographic Fourier-transform division,” Phys. Lett. 25A, 89–90 (1967), and references therein.
  22. A. Basuray, S. K. Sarkar, and M. De, “A new method for edge image analysis,” Opt. Acta 26, 349–356 (1979).
    [Crossref]
  23. K. A. Schultz and E. G. Seebauer, “Surface diffusion of Sb on Ge(111) monitored quantitatively with optical second harmonic microscopy,” J. Chem. Phys. 97, 6958–6967 (1992).
    [Crossref]

1992 (3)

K. A. Schultz, I. I. Suni, C. E. Allen, and E. G. Seebauer, “Optical second harmonic study of Sb adsorption on Ge(111),” Surf. Sci. 276, 40–49 (1992).
[Crossref]

K. A. Schultz and E. G. Seebauer, “Low-stress, coolable sample mount for ultrahigh vacuum studies of fragile semiconductors,” Rev. Sci. Instrum. 63, 218–219 (1992).
[Crossref]

K. A. Schultz and E. G. Seebauer, “Surface diffusion of Sb on Ge(111) monitored quantitatively with optical second harmonic microscopy,” J. Chem. Phys. 97, 6958–6967 (1992).
[Crossref]

1991 (3)

G. A. Reider, U. Höfer, and T. F. Heinz, “Surface diffusion of hydrogen on Si(111) 7×7,” Phys. Rev. Lett. 66, 1994–1997 (1991).
[Crossref] [PubMed]

V. P. Kesan, S. S. Iyer, and J. M. Cotte, “Dopant Incorporation in epitaxial germanium growth on Ge(100) substrates by MBE,” J. Cryst. Growth 111, 847–855 (1991).
[Crossref]

J. M. C. Thornton, A. A. Williams, J. E. Macdonald, R. G. van Siefhout, J. F. van der Veen, M. Finney, and C. Norris, “The influence of Sb as a surfactant on the strain relaxation of Ge/Si(001),” J. Vac. Sci. Technol. B 9, 2146–2149 (1991).
[Crossref]

1988 (3)

X. D. Zhu, T. Rasing, and Y. R. Shen, “Surface diffusion of CO on Ni(111) studied by diffraction of optical second-harmonic generation of a monolayer grating,” Phys. Rev. Lett. 66, 2883–2885 (1988).
[Crossref]

G. L. Richmond, J. M. Robinson, and V. L. Shannon, “Second harmonic generation studies of interfacial structure and dynamics,” Prog. Surf. Sci. 281–70 (1988), and references therein.
[Crossref]

T. Stehlin, M. Feller, P. Guyot-Sionnest, and Y. R. Shen, “Optical second harmonic generation as a surface probe for noncentrosymmetric media,” Opt. Lett. 13, 389–391 (1988).
[Crossref]

1986 (2)

G. T. Boyd, Y. R. Shen, and T. W. Hänsch, “Continuous-wave second harmonic generation as a surface microprobe,” Opt. Lett. 11, 97–99 (1986).
[Crossref]

E. G. Seebauer, A. C. F. Kong, and L. D. Schmidt, “Adsorption and desorption of NO, CO, and H2on Pt(111): laser-induced thermal desorption studies,” Surf. Sci. 176, 134–156 (1986).
[Crossref]

1985 (1)

Y. R. Shen, “Surface studies by optical second harmonic generation: an overview,” J. Vac. Sci. Technol. B 3, 1464–1466 (1985).
[Crossref]

1983 (1)

R. Reinisch and M. Neviére, “Electromagnetic theory of diffraction in nonlinear optics and surface-enhanced nonlinear optical effects,” Phys. Rev. B 28, 1870–1882 (1983).
[Crossref]

1979 (1)

A. Basuray, S. K. Sarkar, and M. De, “A new method for edge image analysis,” Opt. Acta 26, 349–356 (1979).
[Crossref]

1967 (1)

G. W. Stroke and R. G. Zech, “A posteriori image-correcting deconvolution by holographic Fourier-transform division,” Phys. Lett. 25A, 89–90 (1967), and references therein.

1966 (1)

1963 (1)

Allen, C. E.

K. A. Schultz, I. I. Suni, C. E. Allen, and E. G. Seebauer, “Optical second harmonic study of Sb adsorption on Ge(111),” Surf. Sci. 276, 40–49 (1992).
[Crossref]

Basuray, A.

A. Basuray, S. K. Sarkar, and M. De, “A new method for edge image analysis,” Opt. Acta 26, 349–356 (1979).
[Crossref]

Boyd, G. T.

Charman, W. N.

Considine, P. S.

Cotte, J. M.

V. P. Kesan, S. S. Iyer, and J. M. Cotte, “Dopant Incorporation in epitaxial germanium growth on Ge(100) substrates by MBE,” J. Cryst. Growth 111, 847–855 (1991).
[Crossref]

Crank, J.

J. Crank, The Mathematics of Diffusion (Clarendon, Oxford, 1975), p. 104.

De, M.

A. Basuray, S. K. Sarkar, and M. De, “A new method for edge image analysis,” Opt. Acta 26, 349–356 (1979).
[Crossref]

Feller, M.

Finney, M.

J. M. C. Thornton, A. A. Williams, J. E. Macdonald, R. G. van Siefhout, J. F. van der Veen, M. Finney, and C. Norris, “The influence of Sb as a surfactant on the strain relaxation of Ge/Si(001),” J. Vac. Sci. Technol. B 9, 2146–2149 (1991).
[Crossref]

Guyot-Sionnest, P.

Hänsch, T. W.

Heinz, T. F.

G. A. Reider, U. Höfer, and T. F. Heinz, “Surface diffusion of hydrogen on Si(111) 7×7,” Phys. Rev. Lett. 66, 1994–1997 (1991).
[Crossref] [PubMed]

T. F. Heinz and M. M. T. Loy, “Optical second harmonic generation from semiconductor surfaces,” in Advances in Laser Science III, A. C. Tam, J. L. Gole, and W. C. Stwalley, eds. (American Institute of Physics, New York, 1988), pp. 452–459, and references therein.

Höfer, U.

G. A. Reider, U. Höfer, and T. F. Heinz, “Surface diffusion of hydrogen on Si(111) 7×7,” Phys. Rev. Lett. 66, 1994–1997 (1991).
[Crossref] [PubMed]

Iyer, S. S.

V. P. Kesan, S. S. Iyer, and J. M. Cotte, “Dopant Incorporation in epitaxial germanium growth on Ge(100) substrates by MBE,” J. Cryst. Growth 111, 847–855 (1991).
[Crossref]

Keif, M. T.

M. T. Keif, product Rep. (MDC Corporation, Hayward, Calif., 1989).

Kesan, V. P.

V. P. Kesan, S. S. Iyer, and J. M. Cotte, “Dopant Incorporation in epitaxial germanium growth on Ge(100) substrates by MBE,” J. Cryst. Growth 111, 847–855 (1991).
[Crossref]

Kingslake, R.

R. Kingslake, Optical System Design (Academic, New York, 1983), p. 196.

Kong, A. C. F.

E. G. Seebauer, A. C. F. Kong, and L. D. Schmidt, “Adsorption and desorption of NO, CO, and H2on Pt(111): laser-induced thermal desorption studies,” Surf. Sci. 176, 134–156 (1986).
[Crossref]

Loy, M. M. T.

T. F. Heinz and M. M. T. Loy, “Optical second harmonic generation from semiconductor surfaces,” in Advances in Laser Science III, A. C. Tam, J. L. Gole, and W. C. Stwalley, eds. (American Institute of Physics, New York, 1988), pp. 452–459, and references therein.

Macdonald, J. E.

J. M. C. Thornton, A. A. Williams, J. E. Macdonald, R. G. van Siefhout, J. F. van der Veen, M. Finney, and C. Norris, “The influence of Sb as a surfactant on the strain relaxation of Ge/Si(001),” J. Vac. Sci. Technol. B 9, 2146–2149 (1991).
[Crossref]

Neviére, M.

R. Reinisch and M. Neviére, “Electromagnetic theory of diffraction in nonlinear optics and surface-enhanced nonlinear optical effects,” Phys. Rev. B 28, 1870–1882 (1983).
[Crossref]

Norris, C.

J. M. C. Thornton, A. A. Williams, J. E. Macdonald, R. G. van Siefhout, J. F. van der Veen, M. Finney, and C. Norris, “The influence of Sb as a surfactant on the strain relaxation of Ge/Si(001),” J. Vac. Sci. Technol. B 9, 2146–2149 (1991).
[Crossref]

Rasing, T.

X. D. Zhu, T. Rasing, and Y. R. Shen, “Surface diffusion of CO on Ni(111) studied by diffraction of optical second-harmonic generation of a monolayer grating,” Phys. Rev. Lett. 66, 2883–2885 (1988).
[Crossref]

Reider, G. A.

G. A. Reider, U. Höfer, and T. F. Heinz, “Surface diffusion of hydrogen on Si(111) 7×7,” Phys. Rev. Lett. 66, 1994–1997 (1991).
[Crossref] [PubMed]

Reinisch, R.

R. Reinisch and M. Neviére, “Electromagnetic theory of diffraction in nonlinear optics and surface-enhanced nonlinear optical effects,” Phys. Rev. B 28, 1870–1882 (1983).
[Crossref]

Richmond, G. L.

G. L. Richmond, J. M. Robinson, and V. L. Shannon, “Second harmonic generation studies of interfacial structure and dynamics,” Prog. Surf. Sci. 281–70 (1988), and references therein.
[Crossref]

Robinson, J. M.

G. L. Richmond, J. M. Robinson, and V. L. Shannon, “Second harmonic generation studies of interfacial structure and dynamics,” Prog. Surf. Sci. 281–70 (1988), and references therein.
[Crossref]

Sarkar, S. K.

A. Basuray, S. K. Sarkar, and M. De, “A new method for edge image analysis,” Opt. Acta 26, 349–356 (1979).
[Crossref]

Schmidt, L. D.

E. G. Seebauer, A. C. F. Kong, and L. D. Schmidt, “Adsorption and desorption of NO, CO, and H2on Pt(111): laser-induced thermal desorption studies,” Surf. Sci. 176, 134–156 (1986).
[Crossref]

Schultz, K. A.

K. A. Schultz, I. I. Suni, C. E. Allen, and E. G. Seebauer, “Optical second harmonic study of Sb adsorption on Ge(111),” Surf. Sci. 276, 40–49 (1992).
[Crossref]

K. A. Schultz and E. G. Seebauer, “Low-stress, coolable sample mount for ultrahigh vacuum studies of fragile semiconductors,” Rev. Sci. Instrum. 63, 218–219 (1992).
[Crossref]

K. A. Schultz and E. G. Seebauer, “Surface diffusion of Sb on Ge(111) monitored quantitatively with optical second harmonic microscopy,” J. Chem. Phys. 97, 6958–6967 (1992).
[Crossref]

Seebauer, E. G.

K. A. Schultz and E. G. Seebauer, “Surface diffusion of Sb on Ge(111) monitored quantitatively with optical second harmonic microscopy,” J. Chem. Phys. 97, 6958–6967 (1992).
[Crossref]

K. A. Schultz and E. G. Seebauer, “Low-stress, coolable sample mount for ultrahigh vacuum studies of fragile semiconductors,” Rev. Sci. Instrum. 63, 218–219 (1992).
[Crossref]

K. A. Schultz, I. I. Suni, C. E. Allen, and E. G. Seebauer, “Optical second harmonic study of Sb adsorption on Ge(111),” Surf. Sci. 276, 40–49 (1992).
[Crossref]

E. G. Seebauer, A. C. F. Kong, and L. D. Schmidt, “Adsorption and desorption of NO, CO, and H2on Pt(111): laser-induced thermal desorption studies,” Surf. Sci. 176, 134–156 (1986).
[Crossref]

Shannon, V. L.

G. L. Richmond, J. M. Robinson, and V. L. Shannon, “Second harmonic generation studies of interfacial structure and dynamics,” Prog. Surf. Sci. 281–70 (1988), and references therein.
[Crossref]

Shen, Y. R.

X. D. Zhu, T. Rasing, and Y. R. Shen, “Surface diffusion of CO on Ni(111) studied by diffraction of optical second-harmonic generation of a monolayer grating,” Phys. Rev. Lett. 66, 2883–2885 (1988).
[Crossref]

T. Stehlin, M. Feller, P. Guyot-Sionnest, and Y. R. Shen, “Optical second harmonic generation as a surface probe for noncentrosymmetric media,” Opt. Lett. 13, 389–391 (1988).
[Crossref]

G. T. Boyd, Y. R. Shen, and T. W. Hänsch, “Continuous-wave second harmonic generation as a surface microprobe,” Opt. Lett. 11, 97–99 (1986).
[Crossref]

Y. R. Shen, “Surface studies by optical second harmonic generation: an overview,” J. Vac. Sci. Technol. B 3, 1464–1466 (1985).
[Crossref]

Stehlin, T.

Stroke, G. W.

G. W. Stroke and R. G. Zech, “A posteriori image-correcting deconvolution by holographic Fourier-transform division,” Phys. Lett. 25A, 89–90 (1967), and references therein.

Suni, I. I.

K. A. Schultz, I. I. Suni, C. E. Allen, and E. G. Seebauer, “Optical second harmonic study of Sb adsorption on Ge(111),” Surf. Sci. 276, 40–49 (1992).
[Crossref]

Thornton, J. M. C.

J. M. C. Thornton, A. A. Williams, J. E. Macdonald, R. G. van Siefhout, J. F. van der Veen, M. Finney, and C. Norris, “The influence of Sb as a surfactant on the strain relaxation of Ge/Si(001),” J. Vac. Sci. Technol. B 9, 2146–2149 (1991).
[Crossref]

van der Veen, J. F.

J. M. C. Thornton, A. A. Williams, J. E. Macdonald, R. G. van Siefhout, J. F. van der Veen, M. Finney, and C. Norris, “The influence of Sb as a surfactant on the strain relaxation of Ge/Si(001),” J. Vac. Sci. Technol. B 9, 2146–2149 (1991).
[Crossref]

van Siefhout, R. G.

J. M. C. Thornton, A. A. Williams, J. E. Macdonald, R. G. van Siefhout, J. F. van der Veen, M. Finney, and C. Norris, “The influence of Sb as a surfactant on the strain relaxation of Ge/Si(001),” J. Vac. Sci. Technol. B 9, 2146–2149 (1991).
[Crossref]

Williams, A. A.

J. M. C. Thornton, A. A. Williams, J. E. Macdonald, R. G. van Siefhout, J. F. van der Veen, M. Finney, and C. Norris, “The influence of Sb as a surfactant on the strain relaxation of Ge/Si(001),” J. Vac. Sci. Technol. B 9, 2146–2149 (1991).
[Crossref]

Zech, R. G.

G. W. Stroke and R. G. Zech, “A posteriori image-correcting deconvolution by holographic Fourier-transform division,” Phys. Lett. 25A, 89–90 (1967), and references therein.

Zhu, X. D.

X. D. Zhu, T. Rasing, and Y. R. Shen, “Surface diffusion of CO on Ni(111) studied by diffraction of optical second-harmonic generation of a monolayer grating,” Phys. Rev. Lett. 66, 2883–2885 (1988).
[Crossref]

J. Chem. Phys. (1)

K. A. Schultz and E. G. Seebauer, “Surface diffusion of Sb on Ge(111) monitored quantitatively with optical second harmonic microscopy,” J. Chem. Phys. 97, 6958–6967 (1992).
[Crossref]

J. Cryst. Growth (1)

V. P. Kesan, S. S. Iyer, and J. M. Cotte, “Dopant Incorporation in epitaxial germanium growth on Ge(100) substrates by MBE,” J. Cryst. Growth 111, 847–855 (1991).
[Crossref]

J. Opt. Soc. Am. (2)

J. Vac. Sci. Technol. B (2)

J. M. C. Thornton, A. A. Williams, J. E. Macdonald, R. G. van Siefhout, J. F. van der Veen, M. Finney, and C. Norris, “The influence of Sb as a surfactant on the strain relaxation of Ge/Si(001),” J. Vac. Sci. Technol. B 9, 2146–2149 (1991).
[Crossref]

Y. R. Shen, “Surface studies by optical second harmonic generation: an overview,” J. Vac. Sci. Technol. B 3, 1464–1466 (1985).
[Crossref]

Opt. Acta (1)

A. Basuray, S. K. Sarkar, and M. De, “A new method for edge image analysis,” Opt. Acta 26, 349–356 (1979).
[Crossref]

Opt. Lett. (2)

Phys. Lett. (1)

G. W. Stroke and R. G. Zech, “A posteriori image-correcting deconvolution by holographic Fourier-transform division,” Phys. Lett. 25A, 89–90 (1967), and references therein.

Phys. Rev. B (1)

R. Reinisch and M. Neviére, “Electromagnetic theory of diffraction in nonlinear optics and surface-enhanced nonlinear optical effects,” Phys. Rev. B 28, 1870–1882 (1983).
[Crossref]

Phys. Rev. Lett. (2)

X. D. Zhu, T. Rasing, and Y. R. Shen, “Surface diffusion of CO on Ni(111) studied by diffraction of optical second-harmonic generation of a monolayer grating,” Phys. Rev. Lett. 66, 2883–2885 (1988).
[Crossref]

G. A. Reider, U. Höfer, and T. F. Heinz, “Surface diffusion of hydrogen on Si(111) 7×7,” Phys. Rev. Lett. 66, 1994–1997 (1991).
[Crossref] [PubMed]

Prog. Surf. Sci. (1)

G. L. Richmond, J. M. Robinson, and V. L. Shannon, “Second harmonic generation studies of interfacial structure and dynamics,” Prog. Surf. Sci. 281–70 (1988), and references therein.
[Crossref]

Rev. Sci. Instrum. (1)

K. A. Schultz and E. G. Seebauer, “Low-stress, coolable sample mount for ultrahigh vacuum studies of fragile semiconductors,” Rev. Sci. Instrum. 63, 218–219 (1992).
[Crossref]

Surf. Sci. (2)

E. G. Seebauer, A. C. F. Kong, and L. D. Schmidt, “Adsorption and desorption of NO, CO, and H2on Pt(111): laser-induced thermal desorption studies,” Surf. Sci. 176, 134–156 (1986).
[Crossref]

K. A. Schultz, I. I. Suni, C. E. Allen, and E. G. Seebauer, “Optical second harmonic study of Sb adsorption on Ge(111),” Surf. Sci. 276, 40–49 (1992).
[Crossref]

Other (6)

T. F. Heinz and M. M. T. Loy, “Optical second harmonic generation from semiconductor surfaces,” in Advances in Laser Science III, A. C. Tam, J. L. Gole, and W. C. Stwalley, eds. (American Institute of Physics, New York, 1988), pp. 452–459, and references therein.

R. J. Pressley, ed., Handbook of Lasers (CRC, Cleveland, Ohio, 1971), p. 489.

V. T. Binh, ed., Surface Mobilities on Solid Materials–Fundamental Concepts and Applications (Plenum, New York, 1983).
[Crossref]

M. T. Keif, product Rep. (MDC Corporation, Hayward, Calif., 1989).

J. Crank, The Mathematics of Diffusion (Clarendon, Oxford, 1975), p. 104.

R. Kingslake, Optical System Design (Academic, New York, 1983), p. 196.

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Figures (7)

Fig. 1
Fig. 1

Imaging surface diffusion by optical SH microscopy.

Fig. 2
Fig. 2

Schematic diagram of experimental setup.

Fig. 3
Fig. 3

Calibration curve of SH signal (all polarizations collected) as a function of Sb concentration θ determined by AES. Pump light was plane polarized 30° from the planed defined by the surface normal and the [ 1 ¯10] crystal direction. Results were compiled from several experiments. One monolayer corresponds to θ = 1.

Fig. 4
Fig. 4

SH images of the initial step and diffusion profile after 30 min at 610°C.

Fig. 5
Fig. 5

Concentration profile obtained by combining the data of Figs. 3 and 4.

Fig. 6
Fig. 6

Step concentration profile before and after deconvolution of the optical response function.

Fig. 7
Fig. 7

Diffusivity D as a function of Sb concentration at 610°C.

Equations (1)

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D ( θ ) = - 1 2 t ( d θ d x ) θ = 0 θ 1 θ x d θ .

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