Abstract

A time-resolved reflection pump-probe method was combined with a surface plasmon resonance technique in Kretschmann geometry for the investigation of ultrafast light-induced processes in thin films. Transient changes in the gold layer's reflectivity were observed when the layer was excited by 3 ps duration pulses with photon energy exceeding the interband transition and by probing with photon energy close to the interband transition. Comparison of the experimental and modeling results has shown that the imaginary part of the dielectric function of gold increases linearly during excitation, whereas the real part remains unchanged. The decay of the light-induced changes has two components. The first component is faster than the pulse duration, and the second is much longer than 1.5 ns; they are related to cooling of the electron plasma and lattice, respectively.

© 2006 Optical Society of America

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  1. G. Steiner, "Surface plasmon resonance imaging," Anal. Bioanal. Chem. 379, 328-331 (2004).
  2. E. Kretschmann, "Die Bestimmung optischer Konstanten von Metallen durch Anregung von Oberflachenplasmaschwingungen," Z. Phys. 241, 313-324 (1971).
  3. S. Wang, S. Boussaad, and N. J. Tao, "Surface plasmon resonance enhanced optical absorption spectroscopy for studying molecular adsorbates," Rev. Sci. Instrum. 72, 3055-3060 (2001).
  4. P. M. Norris, A. P. Caffrey, R. J. Stevens, J. M. Klopf, J. T. McLeskey, Jr., and A. N. Smith, "Femtosecond pump-probe nondestructive examination of materials (invited)," Rev. Sci. Instrum. 74, 400-406 (2003).
  5. R. H. M. Groeneveld, R. Sprik, and A. Lagendijk, "Femtosecond spectroscopy of electron-electron and electron-phonon energy relaxation in Ag and Au," Phys. Rev. B 51, 11,433-11,445 (1995).
  6. M. Bonn, D. N. Denzler, S. Funk, M. Wolf, S. Wellershoff, and J. Hohlfeld, "Ultrafast electron dynamics at metal surfaces: competition between electron-phonon coupling and hot-electron transport," Phys. Rev. B 61, 1101-1105 (2000).
  7. H. E. Elsayed-Ali, T. Juhasz, G. O. Smith, and W. E. Bron, "Femtosecond thermoreflectivity and thermotransmissisivity of polycrystalline and single-crystalline gold films," Phys. Rev. B 43, 4488-4491 (1991).
  8. M. Fox, Optical Properties of Solids (Oxford U. Press, 2001).
  9. H. J. Kop, "Time-resolved interferometry on metals and disordered systems," Ph.D. dissertation (Universiteit van Amsterdam, 1998).
  10. J. Hohlfeld, S. S. Wellershoff, J. Gudde, U. Conrad, V. Jahnke, and E. Matthias, "Electron and lattice dynamics following optical excitation of metals," Chem. Phys. 251, 237-258 (2000).
  11. W. J. Scouler, "Temperature modulated reflectance of gold from 2 to 10 eV," Phys. Rev. Lett. 18, 445-448 (1967).
  12. R. Matzdorf, A. Gerlach, F. Theilmann, G. Meister, and A. Goldmann, "New lifetime estimates for d-band holes at noble metal surfaces," Appl. Phys. B 68, 393-395 (1999).
  13. M. Aeschlimann, M. Bauer, S. Pawlik, R. Knorren, G. Bouzerar, and K. H. Bennemann, "Transport and dynamics of optically excited electrons in metals," Appl. Phys. A 71, 485-491 (2000).
  14. S. I. Anisimov, B. L. Kapeliovich, and T. L. Perel'man, "Electron emission from metal surfaces exposed to ultrashort laser pulses," Sov. Phys. JETP 39, 375-377 (1974).
  15. M. Yamamoto, "Surface plasmon resonance (SPR) theory: tutorial," Rev. Polarogr. 48, 209-236 (2002).
  16. P. B. Johnson and R. W. Christy, "Optical constants of the noble metals," Phys. Rev. B 6, 4370-4379 (1972).

2004

G. Steiner, "Surface plasmon resonance imaging," Anal. Bioanal. Chem. 379, 328-331 (2004).

2003

P. M. Norris, A. P. Caffrey, R. J. Stevens, J. M. Klopf, J. T. McLeskey, Jr., and A. N. Smith, "Femtosecond pump-probe nondestructive examination of materials (invited)," Rev. Sci. Instrum. 74, 400-406 (2003).

2002

M. Yamamoto, "Surface plasmon resonance (SPR) theory: tutorial," Rev. Polarogr. 48, 209-236 (2002).

2001

S. Wang, S. Boussaad, and N. J. Tao, "Surface plasmon resonance enhanced optical absorption spectroscopy for studying molecular adsorbates," Rev. Sci. Instrum. 72, 3055-3060 (2001).

2000

M. Aeschlimann, M. Bauer, S. Pawlik, R. Knorren, G. Bouzerar, and K. H. Bennemann, "Transport and dynamics of optically excited electrons in metals," Appl. Phys. A 71, 485-491 (2000).

M. Bonn, D. N. Denzler, S. Funk, M. Wolf, S. Wellershoff, and J. Hohlfeld, "Ultrafast electron dynamics at metal surfaces: competition between electron-phonon coupling and hot-electron transport," Phys. Rev. B 61, 1101-1105 (2000).

J. Hohlfeld, S. S. Wellershoff, J. Gudde, U. Conrad, V. Jahnke, and E. Matthias, "Electron and lattice dynamics following optical excitation of metals," Chem. Phys. 251, 237-258 (2000).

1999

R. Matzdorf, A. Gerlach, F. Theilmann, G. Meister, and A. Goldmann, "New lifetime estimates for d-band holes at noble metal surfaces," Appl. Phys. B 68, 393-395 (1999).

1995

R. H. M. Groeneveld, R. Sprik, and A. Lagendijk, "Femtosecond spectroscopy of electron-electron and electron-phonon energy relaxation in Ag and Au," Phys. Rev. B 51, 11,433-11,445 (1995).

1991

H. E. Elsayed-Ali, T. Juhasz, G. O. Smith, and W. E. Bron, "Femtosecond thermoreflectivity and thermotransmissisivity of polycrystalline and single-crystalline gold films," Phys. Rev. B 43, 4488-4491 (1991).

1974

S. I. Anisimov, B. L. Kapeliovich, and T. L. Perel'man, "Electron emission from metal surfaces exposed to ultrashort laser pulses," Sov. Phys. JETP 39, 375-377 (1974).

1972

P. B. Johnson and R. W. Christy, "Optical constants of the noble metals," Phys. Rev. B 6, 4370-4379 (1972).

1971

E. Kretschmann, "Die Bestimmung optischer Konstanten von Metallen durch Anregung von Oberflachenplasmaschwingungen," Z. Phys. 241, 313-324 (1971).

1967

W. J. Scouler, "Temperature modulated reflectance of gold from 2 to 10 eV," Phys. Rev. Lett. 18, 445-448 (1967).

Aeschlimann, M.

M. Aeschlimann, M. Bauer, S. Pawlik, R. Knorren, G. Bouzerar, and K. H. Bennemann, "Transport and dynamics of optically excited electrons in metals," Appl. Phys. A 71, 485-491 (2000).

Anisimov, S. I.

S. I. Anisimov, B. L. Kapeliovich, and T. L. Perel'man, "Electron emission from metal surfaces exposed to ultrashort laser pulses," Sov. Phys. JETP 39, 375-377 (1974).

Bauer, M.

M. Aeschlimann, M. Bauer, S. Pawlik, R. Knorren, G. Bouzerar, and K. H. Bennemann, "Transport and dynamics of optically excited electrons in metals," Appl. Phys. A 71, 485-491 (2000).

Bennemann, K. H.

M. Aeschlimann, M. Bauer, S. Pawlik, R. Knorren, G. Bouzerar, and K. H. Bennemann, "Transport and dynamics of optically excited electrons in metals," Appl. Phys. A 71, 485-491 (2000).

Bonn, M.

M. Bonn, D. N. Denzler, S. Funk, M. Wolf, S. Wellershoff, and J. Hohlfeld, "Ultrafast electron dynamics at metal surfaces: competition between electron-phonon coupling and hot-electron transport," Phys. Rev. B 61, 1101-1105 (2000).

Boussaad, S.

S. Wang, S. Boussaad, and N. J. Tao, "Surface plasmon resonance enhanced optical absorption spectroscopy for studying molecular adsorbates," Rev. Sci. Instrum. 72, 3055-3060 (2001).

Bouzerar, G.

M. Aeschlimann, M. Bauer, S. Pawlik, R. Knorren, G. Bouzerar, and K. H. Bennemann, "Transport and dynamics of optically excited electrons in metals," Appl. Phys. A 71, 485-491 (2000).

Bron, W. E.

H. E. Elsayed-Ali, T. Juhasz, G. O. Smith, and W. E. Bron, "Femtosecond thermoreflectivity and thermotransmissisivity of polycrystalline and single-crystalline gold films," Phys. Rev. B 43, 4488-4491 (1991).

Caffrey, A. P.

P. M. Norris, A. P. Caffrey, R. J. Stevens, J. M. Klopf, J. T. McLeskey, Jr., and A. N. Smith, "Femtosecond pump-probe nondestructive examination of materials (invited)," Rev. Sci. Instrum. 74, 400-406 (2003).

Christy, R. W.

P. B. Johnson and R. W. Christy, "Optical constants of the noble metals," Phys. Rev. B 6, 4370-4379 (1972).

Conrad, U.

J. Hohlfeld, S. S. Wellershoff, J. Gudde, U. Conrad, V. Jahnke, and E. Matthias, "Electron and lattice dynamics following optical excitation of metals," Chem. Phys. 251, 237-258 (2000).

Denzler, D. N.

M. Bonn, D. N. Denzler, S. Funk, M. Wolf, S. Wellershoff, and J. Hohlfeld, "Ultrafast electron dynamics at metal surfaces: competition between electron-phonon coupling and hot-electron transport," Phys. Rev. B 61, 1101-1105 (2000).

Elsayed-Ali, H. E.

H. E. Elsayed-Ali, T. Juhasz, G. O. Smith, and W. E. Bron, "Femtosecond thermoreflectivity and thermotransmissisivity of polycrystalline and single-crystalline gold films," Phys. Rev. B 43, 4488-4491 (1991).

Fox, M.

M. Fox, Optical Properties of Solids (Oxford U. Press, 2001).

Funk, S.

M. Bonn, D. N. Denzler, S. Funk, M. Wolf, S. Wellershoff, and J. Hohlfeld, "Ultrafast electron dynamics at metal surfaces: competition between electron-phonon coupling and hot-electron transport," Phys. Rev. B 61, 1101-1105 (2000).

Gerlach, A.

R. Matzdorf, A. Gerlach, F. Theilmann, G. Meister, and A. Goldmann, "New lifetime estimates for d-band holes at noble metal surfaces," Appl. Phys. B 68, 393-395 (1999).

Goldmann, A.

R. Matzdorf, A. Gerlach, F. Theilmann, G. Meister, and A. Goldmann, "New lifetime estimates for d-band holes at noble metal surfaces," Appl. Phys. B 68, 393-395 (1999).

Groeneveld, R. H. M.

R. H. M. Groeneveld, R. Sprik, and A. Lagendijk, "Femtosecond spectroscopy of electron-electron and electron-phonon energy relaxation in Ag and Au," Phys. Rev. B 51, 11,433-11,445 (1995).

Gudde, J.

J. Hohlfeld, S. S. Wellershoff, J. Gudde, U. Conrad, V. Jahnke, and E. Matthias, "Electron and lattice dynamics following optical excitation of metals," Chem. Phys. 251, 237-258 (2000).

Hohlfeld, J.

J. Hohlfeld, S. S. Wellershoff, J. Gudde, U. Conrad, V. Jahnke, and E. Matthias, "Electron and lattice dynamics following optical excitation of metals," Chem. Phys. 251, 237-258 (2000).

M. Bonn, D. N. Denzler, S. Funk, M. Wolf, S. Wellershoff, and J. Hohlfeld, "Ultrafast electron dynamics at metal surfaces: competition between electron-phonon coupling and hot-electron transport," Phys. Rev. B 61, 1101-1105 (2000).

Jahnke, V.

J. Hohlfeld, S. S. Wellershoff, J. Gudde, U. Conrad, V. Jahnke, and E. Matthias, "Electron and lattice dynamics following optical excitation of metals," Chem. Phys. 251, 237-258 (2000).

Johnson, P. B.

P. B. Johnson and R. W. Christy, "Optical constants of the noble metals," Phys. Rev. B 6, 4370-4379 (1972).

Juhasz, T.

H. E. Elsayed-Ali, T. Juhasz, G. O. Smith, and W. E. Bron, "Femtosecond thermoreflectivity and thermotransmissisivity of polycrystalline and single-crystalline gold films," Phys. Rev. B 43, 4488-4491 (1991).

Kapeliovich, B. L.

S. I. Anisimov, B. L. Kapeliovich, and T. L. Perel'man, "Electron emission from metal surfaces exposed to ultrashort laser pulses," Sov. Phys. JETP 39, 375-377 (1974).

Klopf, J. M.

P. M. Norris, A. P. Caffrey, R. J. Stevens, J. M. Klopf, J. T. McLeskey, Jr., and A. N. Smith, "Femtosecond pump-probe nondestructive examination of materials (invited)," Rev. Sci. Instrum. 74, 400-406 (2003).

Knorren, R.

M. Aeschlimann, M. Bauer, S. Pawlik, R. Knorren, G. Bouzerar, and K. H. Bennemann, "Transport and dynamics of optically excited electrons in metals," Appl. Phys. A 71, 485-491 (2000).

Kop, H. J.

H. J. Kop, "Time-resolved interferometry on metals and disordered systems," Ph.D. dissertation (Universiteit van Amsterdam, 1998).

Kretschmann, E.

E. Kretschmann, "Die Bestimmung optischer Konstanten von Metallen durch Anregung von Oberflachenplasmaschwingungen," Z. Phys. 241, 313-324 (1971).

Lagendijk, A.

R. H. M. Groeneveld, R. Sprik, and A. Lagendijk, "Femtosecond spectroscopy of electron-electron and electron-phonon energy relaxation in Ag and Au," Phys. Rev. B 51, 11,433-11,445 (1995).

Matthias, E.

J. Hohlfeld, S. S. Wellershoff, J. Gudde, U. Conrad, V. Jahnke, and E. Matthias, "Electron and lattice dynamics following optical excitation of metals," Chem. Phys. 251, 237-258 (2000).

Matzdorf, R.

R. Matzdorf, A. Gerlach, F. Theilmann, G. Meister, and A. Goldmann, "New lifetime estimates for d-band holes at noble metal surfaces," Appl. Phys. B 68, 393-395 (1999).

McLeskey, J. T.

P. M. Norris, A. P. Caffrey, R. J. Stevens, J. M. Klopf, J. T. McLeskey, Jr., and A. N. Smith, "Femtosecond pump-probe nondestructive examination of materials (invited)," Rev. Sci. Instrum. 74, 400-406 (2003).

Meister, G.

R. Matzdorf, A. Gerlach, F. Theilmann, G. Meister, and A. Goldmann, "New lifetime estimates for d-band holes at noble metal surfaces," Appl. Phys. B 68, 393-395 (1999).

Norris, P. M.

P. M. Norris, A. P. Caffrey, R. J. Stevens, J. M. Klopf, J. T. McLeskey, Jr., and A. N. Smith, "Femtosecond pump-probe nondestructive examination of materials (invited)," Rev. Sci. Instrum. 74, 400-406 (2003).

Pawlik, S.

M. Aeschlimann, M. Bauer, S. Pawlik, R. Knorren, G. Bouzerar, and K. H. Bennemann, "Transport and dynamics of optically excited electrons in metals," Appl. Phys. A 71, 485-491 (2000).

Perel'man, T. L.

S. I. Anisimov, B. L. Kapeliovich, and T. L. Perel'man, "Electron emission from metal surfaces exposed to ultrashort laser pulses," Sov. Phys. JETP 39, 375-377 (1974).

Scouler, W. J.

W. J. Scouler, "Temperature modulated reflectance of gold from 2 to 10 eV," Phys. Rev. Lett. 18, 445-448 (1967).

Smith, A. N.

P. M. Norris, A. P. Caffrey, R. J. Stevens, J. M. Klopf, J. T. McLeskey, Jr., and A. N. Smith, "Femtosecond pump-probe nondestructive examination of materials (invited)," Rev. Sci. Instrum. 74, 400-406 (2003).

Smith, G. O.

H. E. Elsayed-Ali, T. Juhasz, G. O. Smith, and W. E. Bron, "Femtosecond thermoreflectivity and thermotransmissisivity of polycrystalline and single-crystalline gold films," Phys. Rev. B 43, 4488-4491 (1991).

Sprik, R.

R. H. M. Groeneveld, R. Sprik, and A. Lagendijk, "Femtosecond spectroscopy of electron-electron and electron-phonon energy relaxation in Ag and Au," Phys. Rev. B 51, 11,433-11,445 (1995).

Steiner, G.

G. Steiner, "Surface plasmon resonance imaging," Anal. Bioanal. Chem. 379, 328-331 (2004).

Stevens, R. J.

P. M. Norris, A. P. Caffrey, R. J. Stevens, J. M. Klopf, J. T. McLeskey, Jr., and A. N. Smith, "Femtosecond pump-probe nondestructive examination of materials (invited)," Rev. Sci. Instrum. 74, 400-406 (2003).

Tao, N. J.

S. Wang, S. Boussaad, and N. J. Tao, "Surface plasmon resonance enhanced optical absorption spectroscopy for studying molecular adsorbates," Rev. Sci. Instrum. 72, 3055-3060 (2001).

Theilmann, F.

R. Matzdorf, A. Gerlach, F. Theilmann, G. Meister, and A. Goldmann, "New lifetime estimates for d-band holes at noble metal surfaces," Appl. Phys. B 68, 393-395 (1999).

Wang, S.

S. Wang, S. Boussaad, and N. J. Tao, "Surface plasmon resonance enhanced optical absorption spectroscopy for studying molecular adsorbates," Rev. Sci. Instrum. 72, 3055-3060 (2001).

Wellershoff, S.

M. Bonn, D. N. Denzler, S. Funk, M. Wolf, S. Wellershoff, and J. Hohlfeld, "Ultrafast electron dynamics at metal surfaces: competition between electron-phonon coupling and hot-electron transport," Phys. Rev. B 61, 1101-1105 (2000).

Wellershoff, S. S.

J. Hohlfeld, S. S. Wellershoff, J. Gudde, U. Conrad, V. Jahnke, and E. Matthias, "Electron and lattice dynamics following optical excitation of metals," Chem. Phys. 251, 237-258 (2000).

Wolf, M.

M. Bonn, D. N. Denzler, S. Funk, M. Wolf, S. Wellershoff, and J. Hohlfeld, "Ultrafast electron dynamics at metal surfaces: competition between electron-phonon coupling and hot-electron transport," Phys. Rev. B 61, 1101-1105 (2000).

Yamamoto, M.

M. Yamamoto, "Surface plasmon resonance (SPR) theory: tutorial," Rev. Polarogr. 48, 209-236 (2002).

Anal. Bioanal. Chem.

G. Steiner, "Surface plasmon resonance imaging," Anal. Bioanal. Chem. 379, 328-331 (2004).

Appl. Phys. A

M. Aeschlimann, M. Bauer, S. Pawlik, R. Knorren, G. Bouzerar, and K. H. Bennemann, "Transport and dynamics of optically excited electrons in metals," Appl. Phys. A 71, 485-491 (2000).

Appl. Phys. B

R. Matzdorf, A. Gerlach, F. Theilmann, G. Meister, and A. Goldmann, "New lifetime estimates for d-band holes at noble metal surfaces," Appl. Phys. B 68, 393-395 (1999).

Chem. Phys.

J. Hohlfeld, S. S. Wellershoff, J. Gudde, U. Conrad, V. Jahnke, and E. Matthias, "Electron and lattice dynamics following optical excitation of metals," Chem. Phys. 251, 237-258 (2000).

Phys. Rev. B

P. B. Johnson and R. W. Christy, "Optical constants of the noble metals," Phys. Rev. B 6, 4370-4379 (1972).

R. H. M. Groeneveld, R. Sprik, and A. Lagendijk, "Femtosecond spectroscopy of electron-electron and electron-phonon energy relaxation in Ag and Au," Phys. Rev. B 51, 11,433-11,445 (1995).

M. Bonn, D. N. Denzler, S. Funk, M. Wolf, S. Wellershoff, and J. Hohlfeld, "Ultrafast electron dynamics at metal surfaces: competition between electron-phonon coupling and hot-electron transport," Phys. Rev. B 61, 1101-1105 (2000).

H. E. Elsayed-Ali, T. Juhasz, G. O. Smith, and W. E. Bron, "Femtosecond thermoreflectivity and thermotransmissisivity of polycrystalline and single-crystalline gold films," Phys. Rev. B 43, 4488-4491 (1991).

Phys. Rev. Lett.

W. J. Scouler, "Temperature modulated reflectance of gold from 2 to 10 eV," Phys. Rev. Lett. 18, 445-448 (1967).

Rev. Polarogr.

M. Yamamoto, "Surface plasmon resonance (SPR) theory: tutorial," Rev. Polarogr. 48, 209-236 (2002).

Rev. Sci. Instrum.

S. Wang, S. Boussaad, and N. J. Tao, "Surface plasmon resonance enhanced optical absorption spectroscopy for studying molecular adsorbates," Rev. Sci. Instrum. 72, 3055-3060 (2001).

P. M. Norris, A. P. Caffrey, R. J. Stevens, J. M. Klopf, J. T. McLeskey, Jr., and A. N. Smith, "Femtosecond pump-probe nondestructive examination of materials (invited)," Rev. Sci. Instrum. 74, 400-406 (2003).

Sov. Phys. JETP

S. I. Anisimov, B. L. Kapeliovich, and T. L. Perel'man, "Electron emission from metal surfaces exposed to ultrashort laser pulses," Sov. Phys. JETP 39, 375-377 (1974).

Z. Phys.

E. Kretschmann, "Die Bestimmung optischer Konstanten von Metallen durch Anregung von Oberflachenplasmaschwingungen," Z. Phys. 241, 313-324 (1971).

Other

M. Fox, Optical Properties of Solids (Oxford U. Press, 2001).

H. J. Kop, "Time-resolved interferometry on metals and disordered systems," Ph.D. dissertation (Universiteit van Amsterdam, 1998).

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