Analytical model for quantitative prediction of material contrasts in scattering-type near-field optical microscopy
Optics Express, Vol. 15, Issue 14, pp. 8550-8565 (2007)
http://dx.doi.org/10.1364/OE.15.008550
Acrobat PDF (457 KB)
Abstract
Nanometer-scale mapping of complex optical constants by scattering-type near-field microscopy has been suffering from quantitative discrepancies between the theory and experiments. To resolve this problem, a novel analytical model is presented here. The comparison with experimental data demonstrates that the model quantitatively reproduces approach curves on a Au surface and yields an unprecedented agreement with amplitude and phase spectra recorded on a phonon-polariton resonant SiC sample. The simple closed-form solution derived here should enable the determination of the local complex dielectric function on an unknown sample, thereby identifying its nanoscale chemical composition, crystal structure and conductivity.
© 2007 Optical Society of America
1. Introduction
F. Zenhausern, M. Oboyle, and H. Wickramasinghe, “Apertureless near-field optical microscope,” Appl. Phys. Lett. 65, 1623–1625 (1994). [CrossRef]
O. J. F. Martin and C. Girard, “Controlling and tuning strong optical field gradients at a local probe microscope tip apex,” Appl. Phys. Lett. 70, 705–707 (1997). [CrossRef]
T. Taubner, R. Hillenbrand, and F. Keilmann, “Performance of visible and mid-infrared scattering-type near-field optical microscopes,” J. Microsc.-Oxf. 210, 311–314 (2003). [CrossRef]
B. Knoll and F. Keilmann, “Near-field probing of vibrational absorption for chemical microscopy,” Nature 399, 134–137 (1999). [CrossRef]
T. Taubner, R. Hillenbrand, and F. Keilmann, “Nanoscale polymer recognition by spectral signature in scattering infrared near-field microscopy,” Appl. Phys. Lett. 85, 5064–5066 (2004). [CrossRef]
N. Ocelic and R. Hillenbrand, “Subwavelength-scale tailoring of surface phonon polaritons by focused ion-beam implantation,” Nat. Mater. 3, 606–609 (2004). [CrossRef] [PubMed]
A. Huber, N. Ocelic, T. Taubner, and R. Hillenbrand, “Nanoscale resolved infrared probing of crystal structure and of plasmon-phonon coupling,” Nano Lett. 6, 774–778 (2006). [CrossRef] [PubMed]
B. Knoll and F. Keilmann, “Infrared conductivity mapping for nanoelectronics,” Appl. Phys. Lett. 77, 3980–3982 (2000). [CrossRef]
B. Knoll and F. Keilmann, “Near-field probing of vibrational absorption for chemical microscopy,” Nature 399, 134–137 (1999). [CrossRef]
J. Gersten and A. Nitzan, “Electromagnetic theory of enhanced Raman-scattering by molecules adsorbed on rough surfaces,” J. Chem. Phys. 73, 3023–3037 (1980). [CrossRef]
T. Taubner, R. Hillenbrand, and F. Keilmann, “Nanoscale polymer recognition by spectral signature in scattering infrared near-field microscopy,” Appl. Phys. Lett. 85, 5064–5066 (2004). [CrossRef]
J. S. Samson, G. Wollny, E. Brundermann, A. Bergner, A. Hecker, G. Schwaab, A. D. Wieck, and M. Havenith, “Setup of a scanning near field infrared microscope (SNIM): Imaging of sub-surface nano-structures in gallium-doped silicon,” Phys. Chem. Chem. Phys. 8, 753 – 758 (2006). [CrossRef] [PubMed]
M. B. Raschke and C. Lienau, “Apertureless near-field optical microscopy: Tip-sample coupling in elastic light scattering,” Appl. Phys. Lett. 83, 5089–5091 (2003). [CrossRef]
R. Hillenbrand, T. Taubner, and F. Keilmann, “Phonon-enhanced light-matter interaction at the nanometre scale,” Nature 418, 159–162 (2002). [CrossRef] [PubMed]
T. Taubner, F. Keilmann, and R. Hillenbrand, “Nanomechanical resonance tuning and phase effects in optical near-field interaction,” Nano Lett. 4, 1669–1672 (2004). [CrossRef]
L. Stebounova, B. B. Akhremitchev, and G. C. Walker, “Enhancement of the weak scattered signal in apertureless near-field scanning infrared microscopy,” Rev. Sci. Instrum. 74, 3670–3674 (2003). [CrossRef]
N. Ocelic and R. Hillenbrand, “Subwavelength-scale tailoring of surface phonon polaritons by focused ion-beam implantation,” Nat. Mater. 3, 606–609 (2004). [CrossRef] [PubMed]
A. Huber, N. Ocelic, T. Taubner, and R. Hillenbrand, “Nanoscale resolved infrared probing of crystal structure and of plasmon-phonon coupling,” Nano Lett. 6, 774–778 (2006). [CrossRef] [PubMed]
R. Hillenbrand, T. Taubner, and F. Keilmann, “Phonon-enhanced light-matter interaction at the nanometre scale,” Nature 418, 159–162 (2002). [CrossRef] [PubMed]
N. Ocelic and R. Hillenbrand, “Subwavelength-scale tailoring of surface phonon polaritons by focused ion-beam implantation,” Nat. Mater. 3, 606–609 (2004). [CrossRef] [PubMed]
A. Huber, N. Ocelic, T. Taubner, and R. Hillenbrand, “Nanoscale resolved infrared probing of crystal structure and of plasmon-phonon coupling,” Nano Lett. 6, 774–778 (2006). [CrossRef] [PubMed]
R. Fikri, D. Barchiesi, F. H’Dhili, R. Bachelot, A. Vial, and P. Royer, “Modeling recent experiments of aperture-less near-field optical microscopy using 2D finite element method,” Opt. Commun. 221, 13–22 (2003). [CrossRef]
A. Cvitkovic, N. Ocelic, J. Aizpurua, R. Guckenberger, and R. Hillenbrand, “Infrared imaging of single nanopar-ticles via strong field enhancement in a scanning nanogap,” Phys. Rev. Lett. 97, (2006). [CrossRef] [PubMed]
J. L. Bohn, D. J. Nesbitt, and A. Gallagher, “Field enhancement in apertureless near-field scanning optical microscopy,” J. Opt. Soc. Am. A-Opt. Image Sci. Vis. 18, 2998–3006 (2001). [CrossRef]
S. V. Sukhov, “Role of multipole moment of the probe in apertureless near-field optical microscopy,” Ultrami-croscopy 101, 111–122 (2004). [CrossRef]
H. Hatano and S. Kawata, “Applicability of deconvolution and nonlinear optimization for reconstructing optical images from near-field optical microscope images,” J. Microsc.-Oxf. 194, 230 – 234 (1999). [CrossRef]
B. Knoll and F. Keilmann, “Enhanced dielectric contrast in scattering-type scanning near-field optical microscopy,” Opt. Commun. 182, 321–328 (2000). [CrossRef]
M. Labardi, S. Patane, and M. Allegrini, “Artifact-free near-field optical imaging by apertureless microscopy,” Appl. Phys. Lett. 77, 621–623 (2000). [CrossRef]
N. Ocelic and R. Hillenbrand, “Subwavelength-scale tailoring of surface phonon polaritons by focused ion-beam implantation,” Nat. Mater. 3, 606–609 (2004). [CrossRef] [PubMed]
A. Huber, N. Ocelic, T. Taubner, and R. Hillenbrand, “Nanoscale resolved infrared probing of crystal structure and of plasmon-phonon coupling,” Nano Lett. 6, 774–778 (2006). [CrossRef] [PubMed]
R. Hillenbrand, T. Taubner, and F. Keilmann, “Phonon-enhanced light-matter interaction at the nanometre scale,” Nature 418, 159–162 (2002). [CrossRef] [PubMed]
J. Gersten and A. Nitzan, “Electromagnetic theory of enhanced Raman-scattering by molecules adsorbed on rough surfaces,” J. Chem. Phys. 73, 3023–3037 (1980). [CrossRef]
J. L. Bohn, D. J. Nesbitt, and A. Gallagher, “Field enhancement in apertureless near-field scanning optical microscopy,” J. Opt. Soc. Am. A-Opt. Image Sci. Vis. 18, 2998–3006 (2001). [CrossRef]
A. Wokaun, “Surface enhancement of optical-fields - mechanism and applications,” Mol. Phys. 56, 1 – 33 (1985). [CrossRef]
A. Huber, N. Ocelic, T. Taubner, and R. Hillenbrand, “Nanoscale resolved infrared probing of crystal structure and of plasmon-phonon coupling,” Nano Lett. 6, 774–778 (2006). [CrossRef] [PubMed]
R. Hillenbrand, T. Taubner, and F. Keilmann, “Phonon-enhanced light-matter interaction at the nanometre scale,” Nature 418, 159–162 (2002). [CrossRef] [PubMed]
T. Taubner, F. Keilmann, and R. Hillenbrand, “Nanomechanical resonance tuning and phase effects in optical near-field interaction,” Nano Lett. 4, 1669–1672 (2004). [CrossRef]
2. Finite-dipole model of the probe-sample near-field interaction
2.1. Monopole approximation of the probing tip near fields
J. L. Bohn, D. J. Nesbitt, and A. Gallagher, “Field enhancement in apertureless near-field scanning optical microscopy,” J. Opt. Soc. Am. A-Opt. Image Sci. Vis. 18, 2998–3006 (2001). [CrossRef]
Y. C. Martin, H. F. Hamann, and H. K. Wickramasinghe, “Strength of the electric field in apertureless near-field optical microscopy,” J. Appl. Phys. 89, 5774–5778 (2001). [CrossRef]
N. Calander and M. Willander, “Theory of surface-plasmon resonance optical-field enhancement at prolate spheroids,” J. Appl. Phys. 92, 4878–4884 (2002). [CrossRef]
C. F. Bohren and D. R. Huffman, Absorption and Scattering of Light by Small Particles (John Wiley & Sons Inc, 1998). [CrossRef]
2.2. Spheroid in an external monopole field
I. V. Lindell, G. Dassios, and K. I. Nikoskinen, “Electrostatic image theory for the conducting prolate spheroid,” J. Phys. D-Appl. Phys. 34, 2302–2307 (2001). [CrossRef]
D. V. Redzic, “An electrostatic problem - a point-charge outside a prolate dielectric spheroid,” Am. J. Phys. 62, 1118 – 1121 (1994). [CrossRef]
I. V. Lindell, G. Dassios, and K. I. Nikoskinen, “Electrostatic image theory for the conducting prolate spheroid,” J. Phys. D-Appl. Phys. 34, 2302–2307 (2001). [CrossRef]
I. V. Lindell, G. Dassios, and K. I. Nikoskinen, “Electrostatic image theory for the conducting prolate spheroid,” J. Phys. D-Appl. Phys. 34, 2302–2307 (2001). [CrossRef]
2.3. Spheroid-sample near-field interaction
I. V. Lindell, G. Dassios, and K. I. Nikoskinen, “Electrostatic image theory for the conducting prolate spheroid,” J. Phys. D-Appl. Phys. 34, 2302–2307 (2001). [CrossRef]
D. V. Redzic, “Image of a moving spheroidal conductor,” Am. J. Phys. 60, 506–508 (1992). [CrossRef]
2.4. Light scattering by the probe and effective probe polarizability
F. Keilmann and R. Hillenbrand, “Near-field microscopy by elastic light scattering from a tip,” Philos. Trans. R. Soc. Lond. Ser. A-Math. Phys. Eng. Sci. 362, 787–805 (2004). [CrossRef]
B. Knoll and F. Keilmann, “Enhanced dielectric contrast in scattering-type scanning near-field optical microscopy,” Opt. Commun. 182, 321–328 (2000). [CrossRef]
M. B. Raschke and C. Lienau, “Apertureless near-field optical microscopy: Tip-sample coupling in elastic light scattering,” Appl. Phys. Lett. 83, 5089–5091 (2003). [CrossRef]
F. Keilmann and R. Hillenbrand, “Near-field microscopy by elastic light scattering from a tip,” Philos. Trans. R. Soc. Lond. Ser. A-Math. Phys. Eng. Sci. 362, 787–805 (2004). [CrossRef]
N. Ocelic and R. Hillenbrand, “Subwavelength-scale tailoring of surface phonon polaritons by focused ion-beam implantation,” Nat. Mater. 3, 606–609 (2004). [CrossRef] [PubMed]
A. Huber, N. Ocelic, T. Taubner, and R. Hillenbrand, “Nanoscale resolved infrared probing of crystal structure and of plasmon-phonon coupling,” Nano Lett. 6, 774–778 (2006). [CrossRef] [PubMed]
B. Knoll and F. Keilmann, “Enhanced dielectric contrast in scattering-type scanning near-field optical microscopy,” Opt. Commun. 182, 321–328 (2000). [CrossRef]
Z. H. Kim, B. Liu, and S. R. Leone, “Nanometer-scale optical imaging of epitaxially grown GaN and InN islands using apertureless near-field microscopy,” J. Phys. Chem. B 109, 8503–8508 (2005). [CrossRef]
R. Hillenbrand, T. Taubner, and F. Keilmann, “Phonon-enhanced light-matter interaction at the nanometre scale,” Nature 418, 159–162 (2002). [CrossRef] [PubMed]
L. Stebounova, B. B. Akhremitchev, and G. C. Walker, “Enhancement of the weak scattered signal in apertureless near-field scanning infrared microscopy,” Rev. Sci. Instrum. 74, 3670–3674 (2003). [CrossRef]
M. B. Raschke and C. Lienau, “Apertureless near-field optical microscopy: Tip-sample coupling in elastic light scattering,” Appl. Phys. Lett. 83, 5089–5091 (2003). [CrossRef]
2.5. Parameters of the model
3. Experiment vs. finite-dipole model
3.1. Microscope setup and experimental details
F. Keilmann and R. Hillenbrand, “Near-field microscopy by elastic light scattering from a tip,” Philos. Trans. R. Soc. Lond. Ser. A-Math. Phys. Eng. Sci. 362, 787–805 (2004). [CrossRef]
N. Ocelic, A. Huber, and R. Hillenbrand, “Pseudoheterodyne detection for background-free near-field spec-troscopy,” Appl. Phys. Lett. 89, (2006). [CrossRef]
M. Labardi, S. Patane, and M. Allegrini, “Artifact-free near-field optical imaging by apertureless microscopy,” Appl. Phys. Lett. 77, 621–623 (2000). [CrossRef]
R. Hillenbrand and F. Keilmann, “Complex optical constants on a subwavelength scale,” Phys. Rev. Lett. 85, 3029–3032 (2000). [CrossRef] [PubMed]
R. Bachelot, G. Wurtz, and P. Royer, “An application of the apertureless scanning near-field optical microscopy: imaging a GaAlAs laser diode in operation,” Appl. Phys. Lett. 73, 3333–3335 (1998). [CrossRef]
B. Knoll and F. Keilmann, “Electromagnetic fields in the cutoff regime of tapered metallic waveguides,” Opt. Commun. 162, 177–181 (1999). [CrossRef]
3.2. Approach curves on a Au sample
A. Cvitkovic, N. Ocelic, J. Aizpurua, R. Guckenberger, and R. Hillenbrand, “Infrared imaging of single nanopar-ticles via strong field enhancement in a scanning nanogap,” Phys. Rev. Lett. 97, (2006). [CrossRef] [PubMed]
3.3. Near-field spectra of a phonon-polariton resonant SiC sample
N. Ocelic and R. Hillenbrand, “Subwavelength-scale tailoring of surface phonon polaritons by focused ion-beam implantation,” Nat. Mater. 3, 606–609 (2004). [CrossRef] [PubMed]
A. Huber, N. Ocelic, T. Taubner, and R. Hillenbrand, “Nanoscale resolved infrared probing of crystal structure and of plasmon-phonon coupling,” Nano Lett. 6, 774–778 (2006). [CrossRef] [PubMed]
R. Hillenbrand, T. Taubner, and F. Keilmann, “Phonon-enhanced light-matter interaction at the nanometre scale,” Nature 418, 159–162 (2002). [CrossRef] [PubMed]
B. Knoll and F. Keilmann, “Infrared conductivity mapping for nanoelectronics,” Appl. Phys. Lett. 77, 3980–3982 (2000). [CrossRef]
N. Ocelic and R. Hillenbrand, “Subwavelength-scale tailoring of surface phonon polaritons by focused ion-beam implantation,” Nat. Mater. 3, 606–609 (2004). [CrossRef] [PubMed]
A. Huber, N. Ocelic, T. Taubner, and R. Hillenbrand, “Nanoscale resolved infrared probing of crystal structure and of plasmon-phonon coupling,” Nano Lett. 6, 774–778 (2006). [CrossRef] [PubMed]
R. Hillenbrand, T. Taubner, and F. Keilmann, “Phonon-enhanced light-matter interaction at the nanometre scale,” Nature 418, 159–162 (2002). [CrossRef] [PubMed]
T. Taubner, F. Keilmann, and R. Hillenbrand, “Nanomechanical resonance tuning and phase effects in optical near-field interaction,” Nano Lett. 4, 1669–1672 (2004). [CrossRef]
A. Huber, N. Ocelic, D. Kazantsev, and R. Hillenbrand, “Near-field imaging of mid-infrared surface phonon polariton propagation,” Appl. Phys. Lett. 87, (2005). [CrossRef]
F. Engelbrecht and R. Helbig, “Effect of crystal anisotropy on the infrared reflectivity of 6H-SiC,” Phys. Rev. B 48, 15,698 – 15,707 (1993). [CrossRef]
| E ∥ c | E ⊥ c | |
|---|---|---|
| ε ∞ [57] | 6.78 | 6.56 |
|
ωTO
[58 M. Hofmann, A. Zywietz, K. Karch, and F. Bechstedt, “Lattice-dynamics of SiC polytypes within the bond-charge model,” Phys. Rev. B 50, 13,401–13,411 (1994). [CrossRef] | 782 cm-1 | 797 cm-1 |
|
ωLO
[58 M. Hofmann, A. Zywietz, K. Karch, and F. Bechstedt, “Lattice-dynamics of SiC polytypes within the bond-charge model,” Phys. Rev. B 50, 13,401–13,411 (1994). [CrossRef] | 967 cm-1 | 971 cm-1 |
|
γ [59 H. Harima, S. Nakashima, and T. Uemura, “Raman-scattering from anisotropic LO-phonon-plasmon-coupled mode in n-type 4H-SiC and 6H-SiC,” J. Appl. Phys. 78, 1996–2005 (1995). [CrossRef] | 6.6 cm-1 | 6.6 cm-1 |
I. V. Lindell, K. I. Nikoskinen, and M. J. Flykt, “Electrostatic image theory for an anisotropic half-space slightly deviating from transverse isotropy,” Radio Sci. 31, 1361 – 1368 (1996). [CrossRef]
4. Conclusion
I. V. Lindell, G. Dassios, and K. I. Nikoskinen, “Electrostatic image theory for the conducting prolate spheroid,” J. Phys. D-Appl. Phys. 34, 2302–2307 (2001). [CrossRef]
M. A. Ordal et al., “Optical properties of the metals Al, Co,Cu,Au,Fe,Pb,Ni,Pd,Pt,Ag,Ti and W in the infrared and far infrared,” Appl. Opt. 22, (1983). [CrossRef] [PubMed]
Acknowledgments
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Z. H. Kim and S. R. Leone, “High-resolution apertureless near-field optical imaging using gold nanosphere probes,” J. Phys. Chem. B 110, 19,804–19,809 (2006). | |
N. Ocelic, A. Huber, and R. Hillenbrand, “Pseudoheterodyne detection for background-free near-field spec-troscopy,” Appl. Phys. Lett. 89, (2006). [CrossRef] | |
R. Bachelot, G. Wurtz, and P. Royer, “An application of the apertureless scanning near-field optical microscopy: imaging a GaAlAs laser diode in operation,” Appl. Phys. Lett. 73, 3333–3335 (1998). [CrossRef] | |
B. Knoll and F. Keilmann, “Electromagnetic fields in the cutoff regime of tapered metallic waveguides,” Opt. Commun. 162, 177–181 (1999). [CrossRef] | |
A. Huber, N. Ocelic, D. Kazantsev, and R. Hillenbrand, “Near-field imaging of mid-infrared surface phonon polariton propagation,” Appl. Phys. Lett. 87, (2005). [CrossRef] | |
F. Engelbrecht and R. Helbig, “Effect of crystal anisotropy on the infrared reflectivity of 6H-SiC,” Phys. Rev. B 48, 15,698 – 15,707 (1993). [CrossRef] | |
H. Mutschke, A. C. Andersen, D. Clement, T. Henning, and G. Peiter, “Infrared properties of SiC particles,” Astron. Astrophys. 345, 187–202 (1999). | |
M. Hofmann, A. Zywietz, K. Karch, and F. Bechstedt, “Lattice-dynamics of SiC polytypes within the bond-charge model,” Phys. Rev. B 50, 13,401–13,411 (1994). [CrossRef] | |
H. Harima, S. Nakashima, and T. Uemura, “Raman-scattering from anisotropic LO-phonon-plasmon-coupled mode in n-type 4H-SiC and 6H-SiC,” J. Appl. Phys. 78, 1996–2005 (1995). [CrossRef] | |
I. V. Lindell, K. I. Nikoskinen, and M. J. Flykt, “Electrostatic image theory for an anisotropic half-space slightly deviating from transverse isotropy,” Radio Sci. 31, 1361 – 1368 (1996). [CrossRef] | |
I. V. Lindell, K. I. Nikoskinen, and A. Viljanen, “Electrostatic image method for the anisotropic half space,” IEE Proc.-Sci. Meas. Technol. 144, 156 – 162 (1997). [CrossRef] | |
S. C. Schneider, S. Grafstrom, and L. M. Eng, “Scattering near-field optical microscopy of optically anisotropicsystems,” Phys. Rev. B 71, (2005). [CrossRef] | |
M. A. Ordal et al., “Optical properties of the metals Al, Co,Cu,Au,Fe,Pb,Ni,Pd,Pt,Ag,Ti and W in the infrared and far infrared,” Appl. Opt. 22, (1983). [CrossRef] [PubMed] |
OCIS Codes
(110.3080) Imaging systems : Infrared imaging
(120.5820) Instrumentation, measurement, and metrology : Scattering measurements
(180.5810) Microscopy : Scanning microscopy
(300.6340) Spectroscopy : Spectroscopy, infrared
ToC Category:
Microscopy
History
Original Manuscript: March 28, 2007
Revised Manuscript: May 6, 2007
Manuscript Accepted: May 10, 2007
Published: June 25, 2007
Virtual Issues
Vol. 2, Iss. 8 Virtual Journal for Biomedical Optics
Citation
A. Cvitkovic, N. Ocelic, and R. Hillenbrand, "Analytical model for quantitative prediction of material contrasts in
scattering-type near-field optical microscopy," Opt. Express 15, 8550-8565 (2007)
http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-15-14-8550
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- I. V. Lindell, K. I. Nikoskinen, and M. J. Flykt, "Electrostatic image theory for an anisotropic half-space slightly deviating from transverse isotropy," Radio Sci. 31, 1361 - 1368 (1996). [CrossRef]
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