OSA's Digital Library

Journal of the Optical Society of America B

Journal of the Optical Society of America B


  • Vol. 20, Iss. 12 — Dec. 1, 2003
  • pp: 2548–2561

Second-harmonic amplitude and phase spectroscopy by use of broad-bandwidth femtosecond pulses

P. T. Wilson, Y. Jiang, R. Carriles, and M. C. Downer  »View Author Affiliations

JOSA B, Vol. 20, Issue 12, pp. 2548-2561 (2003)

View Full Text Article

Enhanced HTML    Acrobat PDF (468 KB)

Browse Journals / Lookup Meetings

Browse by Journal and Year


Lookup Conference Papers

Close Browse Journals / Lookup Meetings

Article Tools



We present an in-depth experimental study of frequency-domain (FD) methods for measuring second-harmonic (SH) amplitude and phase spectra of surfaces by use of a 60-nm bandwidth femtosecond source and spectral dispersion of generated SH light. We directly compare FD with conventional scanning approaches, in which a narrowband laser is tuned over resonant features, by applying them to common Si1-xGex,Si1-x-yGexCy, and Si(001)SiO2Cr metal–oxide–semiconductor (MOS) samples. FD methods yield chirp-independentχ(2) amplitude spectra in good agreement with more time-consuming conventionally measured spectra. FD interferometric SH (FDISH) phase spectroscopy avoids the need for an interferometer scan at each frequency and yields detailed, reproducible phase spectra of the MOS capacitor. To validate the measured phase spectra, we reproduce their bias-dependent features in detail with a model of a resonant electric-field-induced SH polarization superposed coherently upon a field-independent background.

© 2003 Optical Society of America

OCIS Codes
(190.4350) Nonlinear optics : Nonlinear optics at surfaces
(240.4350) Optics at surfaces : Nonlinear optics at surfaces
(240.6490) Optics at surfaces : Spectroscopy, surface
(320.7110) Ultrafast optics : Ultrafast nonlinear optics

P. T. Wilson, Y. Jiang, R. Carriles, and M. C. Downer, "Second-harmonic amplitude and phase spectroscopy by use of broad-bandwidth femtosecond pulses," J. Opt. Soc. Am. B 20, 2548-2561 (2003)

Sort:  Author  |  Year  |  Journal  |  Reset  


  1. R. W. Collins, I. An, H. Fujiwara, J. Lee, Y. Lu, J. Koh, and P. I. Rovira, “Advances in multichannel spectroscopic ellipsometry,” Thin Solid Films 313–314, 18–32 (1998). [CrossRef]
  2. L. Mantese, K. Selinidis, P. T. Wilson, D. Lim, Y. Jiang, J. G. Ekerdt, and M. C. Downer, “In situ control and monitoring of doped and compositionally graded SiGe films using spectroscopic ellipsometry and second harmonic generation,” Appl. Surf. Sci. 154–155, 229–237 (2000). [CrossRef]
  3. M. C. Downer, Y. Jiang, D. Lim, L. Mantese, P. T. Wilson, B. S. Mendoza, and V. I. Gavrilenko, “Optical second harmonic spectroscopy of silicon surfaces, interfaces and nanocrystals,” Phys. Status Solidi A 188, 1371–1380 (2001). [CrossRef]
  4. Y. R. Shen, “Surface properties probed by second-harmonic and sum-frequency generation,” Nature 337, 519–525 (1989). [CrossRef]
  5. G. Lüpke, “Characterization of semiconductor interfaces by second-harmonic generation,” Surf. Sci. Rep. 35, 75–162 (1999). [CrossRef]
  6. W. Daum, H.-J. Krause, U. Reichel, and H. Ibach, “Identification of strained silicon layers at Si–SiO2 interfaces and clean Si surfaces by nonlinear optical spectroscopy,” Phys. Rev. Lett. 71, 1234–1237 (1993). [CrossRef] [PubMed]
  7. R. K. Chang, J. Ducuing, and N. Bloembergen, “Relative phase measurement between fundamental and second-harmonic light,” Phys. Rev. Lett. 15, 6–8 (1965). [CrossRef]
  8. R. Stolle, G. Marowsky, E. Schwarzberg, and G. Berkovic, “Phase measurements in nonlinear optics,” Appl. Phys. B 63, 491–498 (1996). [CrossRef]
  9. G. Erley and W. Daum, “Silicon interband transitions observed at Si(100)–SiO2 interfaces,” Phys. Rev. B 58, R1734–1737 (1998). [CrossRef]
  10. O. A. Aktsipetrov, T. V. Dolgova, A. A. Fedyanin, D. Schuhmacher, and G. Marowsky, “Optical second-harmonic phase spectroscopy of the Si(111)–SiO2 interface,” Thin Solid Films 364, 91–94 (2000). [CrossRef]
  11. E. W. M. van der Ham, Q. H. F. Vrehen, and E. R. Eliel, “Self-dispersive sum-frequency generation at interfaces,” Opt. Lett. 21, 1448–1450 (1998). [CrossRef]
  12. L. J. Richter, T. P. Petralli-Mallow, and J. C. Stephenson, “Vibrationally resolved sumfrequency generation with broad-bandwidth infrared pulses,” Opt. Lett. 23, 1594–1596 (1998). [CrossRef]
  13. J. A. McGuire, W. Beck, X. Wei, and Y. R. Shen, “Fourier-transform sum-frequency surface vibrational spectroscopy with femtosecond pulses,” Opt. Lett. 24, 1877–1879 (1999). [CrossRef]
  14. P. T. Wilson, K. A. Briggman, W. E. Wallace, J. C. Stephenson, and L. J. Richter, “Selective study of polymer/dielectric interfaces with vibrationally resonant sum frequency generation via thin-film interference,” Appl. Phys. Lett. 80, 3084–3086 (2002). [CrossRef]
  15. P. T. Wilson, L. J. Richter, W. E. Wallace, K. A. Briggman, and J. C. Stephenson, “Correlation of molecular orientation with adhesion at polystyrene/solid interfaces,” Chem. Phys. Lett. 363, 161–168 (2002). [CrossRef]
  16. P. T. Wilson, Y. Jiang, O. A. Aktsipetrov, E. D. Mishina, and M. C. Downer, “Frequency-domain interferometric second-harmonic spectroscopy,” Opt. Lett. 24, 496–498 (1999). [CrossRef]
  17. M. T. Asaki, C.-P. Huang, D. Garvey, J. Zhou, H. C. Kapteyn, and M. M. Murnane, “Generation of 11-fs pulses from a self-mode-locked Ti:sapphire laser,” Opt. Lett. 18, 977–979 (1993). [CrossRef] [PubMed]
  18. R. Trebino, K. W. Delong, D. N. Fittinghoff, J. N. Sweetser, M. A. Krummbügel, and B. A. Richman, “Measuring ultrashort laser pulses in the time-frequency domain using frequency-resolved optical gating,” Rev. Sci. Instrum. 68, 3277–3295 (1997). [CrossRef]
  19. R. Carriles, P. T. Wilson, M. C. Downer, and R. S. Windeler, “Second harmonic phase spectroscopy: frequency vs. time domain,” in Conference on Lasers and Electro-Optics, Vol. 73 of OSA Trends in Optics and Photonics Series (Optical Society of America, Washington, D.C., 2002), pp. 449–450.
  20. T. A. Birks, W. J. Wadsworth, and P. St. J. Russell, “Supercontinuum generation in tapered fibers,” Opt. Lett. 25, 1415–1417 (2000). [CrossRef]
  21. J. K. Ranka, R. S. Windeler, and A. J. Stentz, “Visible continuum generation in air–silica microstructure optical fibers with anomalous dispersion at 800 nm,” Opt. Lett. 25, 25–27 (2000). [CrossRef]
  22. W. M. Duncan, S. A. Henck, J. W. Kuehne, L. M. Loewenstein, and S. Maung, “High-speed spectral ellipsometry for in situ diagnostics and process control,” J. Vac. Sci. Technol. B 12, 2779–2784 (1994). [CrossRef]
  23. S. Zollner, J. Hildreth, R. Liu, P. Zaumseil, M. Weidner, and B. Tillack, “Optical constants and ellipsometric thickness determination of strained Si1−xGex:C layers on Si (100) and related heterostructures,” J. Appl. Phys. 88, 4102–4108 (2000). [CrossRef]
  24. L. Lepetit, G. Cheriaux, and M. Joffre, “Linear techniques of phase measurement by femtosecond interferometry for applications in spectroscopy,” J. Opt. Soc. Am. B 12, 2467–2474 (1995). [CrossRef]
  25. P. T. Wilson, “Second-harmonic generation spectroscopy using broad bandwidth femtosecond pulses,” Ph.D. dissertation (University of Texas at Austin, Austin, Tex., 2000).
  26. S. John, E. Quinones, B. Ferguson, S. Ray, B. Ananthram, S. Middlebrooks, C. Mullins, J. G. Ekerdt, J. Rawlings, and S. Banerjee, “Properties of Si1−x−yGexCy epitaxial films grown by ultrahigh vacuum chemical vapor deposition,” J. Electrochem. Soc. 146, 4611–4615 (1999). [CrossRef]
  27. R. People, “Physics and applications of GexSi1−x/Si strained-layer heterostructures,” IEEE J. Quantum Electron. 22, 1696–1710 (1986). [CrossRef]
  28. S. Sego, R. J. Culbertson, D. J. Smith, Z. Atzmon, and A. E. Bair, “Strain measurements of SiGeC heteroepitaxial layers on Si(001) using ion beam analysis,” J. Vac. Sci. Technol. A 14, 441–446 (1996). [CrossRef]
  29. O. A. Aktsipetrov, A. A. Fedyanin, A. V. Melnikov, E. D. Mishina, A. N. Rubtsov, M. H. Anderson, P. T. Wilson, M. ter Beek, X. F. Hu, J. I. Dadap, and M. C. Downer, “dc-electric-field-induced and low-frequency electromodulation second-harmonic generation spectroscopy of Si(001)–SiO2 interfaces,” Phys. Rev. B 60, 8924–8938 (1999). [CrossRef]
  30. J. I. Dadap, X. F. Hu, M. H. Anderson, M. C. Downer, J. K. Lowell, and O. A. Aktsipetrov, “Optical second-harmonic electroreflectance spectroscopy of a Si(001) metal-oxide-semiconductor structure,” Phys. Rev. B 53, R7607–R7609 (1996). [CrossRef]
  31. R. C. Miller, “Optical second harmonic generation in piezoelectric crystals,” Appl. Phys. Lett. 5, 17–19 (1964). [CrossRef]
  32. E. D. Palik, Handbook of Optical Constants of Solids (Academic, San Diego, Calif., 1985).
  33. J. Bloch, J. G. Mihaychuk, and H. M. van Driel, “Electron photoinjection from silicon to ultrathin SiO2 films via ambient oxygen,” Phys. Rev. Lett. 77, 920–923 (1996). [CrossRef] [PubMed]
  34. C. Pickering, R. T. Carline, D. J. Robbins, W. Y. Leong, S. J. Barnett, A. D. Pitt, and A. G. Cullis, “Spectroscopic ellipsometry characterization of strained and relaxed Si1−xGex epitaxial layers,” J. Appl. Phys. 73, 239–250 (1993). [CrossRef]
  35. P. Zaumseil, “High resolution determination of the Ge depth profile in SiGe heterobipolar transistor structures by x-ray diffractometry,” Phys. Status Solidi A 165, 195–204 (1998). [CrossRef]
  36. J. I. Dadap, P. T. Wilson, M. H. Anderson, M. C. Downer, and M. ter Beek, “Femtosecond carrier-induced screening of dc electric-field-induced second-harmonic generation at the Si(001)–SiO2 interface,” Opt. Lett. 22, 901–903 (1997). [CrossRef] [PubMed]
  37. V. L. Malevich, “Dynamics of photoinduced field screening: THz pulse and second harmonic generation from semiconductor surface,” Surf. Sci. 454–456, 1074–1078 (2000). [CrossRef]
  38. E. D. Mishina, S. Nakabayashi, O. A. Aktsipetrov, and M. C. Downer, “Photomodulated second harmonic generation at silicon-silicon oxide interfaces: from modeling to application,” Jpn. J. Appl. Phys. (to be published).
  39. L. Kronik and Y. Shapira, “Photovoltage phenomena: theory, experiment and applications,” Surf. Sci. Rep. 37, 1–206 (1999). [CrossRef]
  40. D. Lim, M. C. Downer, and J. G. Ekerdt, “Second-harmonic spectroscopy of bulk boron-doped Si(001),” Appl. Phys. Lett. 77, 181–183 (2000). [CrossRef]
  41. J. G. Mihaychuk, N. Shamir, and H. M. van Driel, “Multiphoton photoemission and electric-field-induced optical second-harmonic generation as probes of charge transfer across the Si/SiO2 interface,” Phys. Rev. B 59, 2164–2173 (1999). [CrossRef]
  42. M. Cardona, Modulation Spectroscopy (Academic, New York, 1969).
  43. S. M. Sze, Physics of Semiconductor Devices (Wiley, New York, 1981), Chap. 7.

Cited By

Alert me when this paper is cited

OSA is able to provide readers links to articles that cite this paper by participating in CrossRef's Cited-By Linking service. CrossRef includes content from more than 3000 publishers and societies. In addition to listing OSA journal articles that cite this paper, citing articles from other participating publishers will also be listed.

« Previous Article  |  Next Article »

OSA is a member of CrossRef.

CrossCheck Deposited