We propose a new differential imaging technique to visualize the fine structures and the edges of a sample in coherent anti-Stokes Raman Scattering (CARS) microscopy. Both the pump and Stokes excitation fields are modulated simultaneously with a spiral phase mask which transforms them from Gaussian modes into Laguerre-Gaussian modes of LG01 for CARS excitation. With an accurate three dimensional finite-difference time-domain (FDTD) method, the intensity and phase distributions of focused input fields, the scattering pattern of generated CARS signal as well as the formation of differential images are studied detailedly, and by simulating the sensitivity range and reliability of this method, we have verified that it is much suitable for visualizing structures with a scale comparable to the excitation wavelength and has higher reliability in retrieving chemical structural information of the sample compared to common CARS microscopy.

© 2007 Optical Society of America

1. R. J.H. Clark and R. E. Hester, Advances in Nonlinear Spectroscopy, (Wiley, New York, 1988) 15.
2. P.D. Maker and R.W. Terhune, "Study of optical effects due to an induced polarization third order in the electric field strength," Phys, Rev. 137, A801-A818 (1965). [CrossRef]
3. Y. R. Shen, The principles of nonlinear optics (Wiley, New York, 1984).
4. J. X. Cheng and X. S. Xie, "Coherent Anti-Stokes Scattering Microscopy: Instrumentation, Theory, and Application," J. Phys. Chem. B. 108,827-840 (2004). [CrossRef]
5. J. X. Cheng, A. Volkmer, and X. S. Xie, "Theoretical and experimental characterization of Coherent anti-Stokes Raman scattering microscopy," J. Opt. Soc. Am. B. 19, 1363-1375 (2002). [CrossRef]
6. H. Wang, Y. Fu, P. Zickmund, R. Shi, and J. X. Cheng, "Coherent Anti-Stokes Raman Scattering Imaging of Axonal Myelin in Live Spinal Tissues," Biophysical Journal 89, 581-591 (2005). [CrossRef] [PubMed]
7. E. O. Potma, C. L. Evans, and X. S. Xie, "Heterodyne Coherent anti-Stokes Raman scattering (CARS) imaging," Opt. Lett. 31, 241-243 (2006). [CrossRef] [PubMed]
8. J. P. Ogilvie, E. Beaurepire, A. Alexandrou, and M. Joffre, "Fourier-transform coherent anti-Stokes Raman scattering microscopy," Opt. Lett. 31, 480- 482 (2006). [CrossRef] [PubMed]
9. D. Oron, N. Dudovich, and Y. Silberberg, "Single-Pulse Phase-contrast nonlinear Raman Spectroscopy," Phys. Rev. Lett. 89, 273001-273004 (2002). [CrossRef]
10. E. R. Andresen, H. N. Paulsen, V. Birkedl "Broadband multiplex coherent anti-Stokes Raman scattering microscopy employing photonic-crystal fibers," J. Opt. Am. B. 22, 1934-1938 (2005). [CrossRef]
11. J. X. Cheng and X. S. Xie, "Green’s function formulation for third-harmonic generation microscopy," J. Opt. Soc. Am. B. 19, 1604-1610 (2002). [CrossRef]
12. V. V. Krishnamachari, E. O. Potma, "Focus-engineered coherent anti-Stokes Raman scattering microscopy: a numerical investigation," J. Opt. Soc. Am. A 24, 1138-1147 (2007). [CrossRef]
13. K. S. Yee. "Numerical solution of initial boundary value problem involving Maxwell equations in isotropic media,".IEEE Trans. Antennas Propagat. 14, 302-307 (1966). [CrossRef]
14. A. Taflove, Computational Electrodynamics: The Finite-Difference Time-Domain Method (Artech House, Boston, 1995).
15. R. W. Boyd, Nonlinear Optics (Academic, Boston, Mass., 1992).
16. S. Mukamel, Principles of Nonlinear Optical Spectroscopy (Oxford U. Press New York, 1995).
17. M.W. Beijersbergen, R.P.C. Coewinkel, M. Kristensen, J.P. Woerdman, "Helical-wavefront laser beams produced with a spiral phase plate," Opt. Comm. 112, 321-327 (1994) [CrossRef]
18. K. Crabtree, J. A. Davis, and I. Moreno, "Optical processing with votex-producing lenses," Appl. Opt. 43, 1360-1367(2004). [CrossRef] [PubMed]
19. K. Takeda, Y. Ito and C. Munakata, "Simultaneous measurement of size and refractive index of a fine particle in flowing liquid," Meas. Sci. Technol. 3, 27-32 (1992). [CrossRef]
20. M. Hashimoto and T. Araki, "Three-dimensional transfer functions of coherent anti-Stokes Raman scattering microscopy," J. Opt. Soc. Am. A 18,771-776 (2001). [CrossRef]
21. L. Cheng, H. Zhiwei, L. Fake, Z. Wei, H. W. Dietmar, S. Colin "Near-field effects on coherent anti-Stokes Raman scattering microscopy imaging," Opt. Express 15, 4118-4131(2007). [CrossRef]

Appl. Opt.

• K. Crabtree, J. A. Davis, and I. Moreno, "Optical processing with votex-producing lenses," Appl. Opt. 43, 1360-1367(2004). [CrossRef] [PubMed]

Biophysical Journal

• H. Wang, Y. Fu, P. Zickmund, R. Shi, and J. X. Cheng, "Coherent Anti-Stokes Raman Scattering Imaging of Axonal Myelin in Live Spinal Tissues," Biophysical Journal 89, 581-591 (2005). [CrossRef] [PubMed]

IEEE Trans. Antennas Propagat.

• K. S. Yee. "Numerical solution of initial boundary value problem involving Maxwell equations in isotropic media,".IEEE Trans. Antennas Propagat. 14, 302-307 (1966). [CrossRef]

J. Opt. Am. B.

• E. R. Andresen, H. N. Paulsen, V. Birkedl "Broadband multiplex coherent anti-Stokes Raman scattering microscopy employing photonic-crystal fibers," J. Opt. Am. B. 22, 1934-1938 (2005). [CrossRef]

J. Opt. Soc. Am. A

• V. V. Krishnamachari, E. O. Potma, "Focus-engineered coherent anti-Stokes Raman scattering microscopy: a numerical investigation," J. Opt. Soc. Am. A 24, 1138-1147 (2007). [CrossRef]
• M. Hashimoto and T. Araki, "Three-dimensional transfer functions of coherent anti-Stokes Raman scattering microscopy," J. Opt. Soc. Am. A 18,771-776 (2001). [CrossRef]

J. Opt. Soc. Am. B.

• J. X. Cheng, A. Volkmer, and X. S. Xie, "Theoretical and experimental characterization of Coherent anti-Stokes Raman scattering microscopy," J. Opt. Soc. Am. B. 19, 1363-1375 (2002). [CrossRef]
• J. X. Cheng and X. S. Xie, "Green’s function formulation for third-harmonic generation microscopy," J. Opt. Soc. Am. B. 19, 1604-1610 (2002). [CrossRef]

J. Phys. Chem. B.

• J. X. Cheng and X. S. Xie, "Coherent Anti-Stokes Scattering Microscopy: Instrumentation, Theory, and Application," J. Phys. Chem. B. 108,827-840 (2004). [CrossRef]

Meas. Sci. Technol.

• K. Takeda, Y. Ito and C. Munakata, "Simultaneous measurement of size and refractive index of a fine particle in flowing liquid," Meas. Sci. Technol. 3, 27-32 (1992). [CrossRef]

Opt. Comm.

• M.W. Beijersbergen, R.P.C. Coewinkel, M. Kristensen, J.P. Woerdman, "Helical-wavefront laser beams produced with a spiral phase plate," Opt. Comm. 112, 321-327 (1994) [CrossRef]

Opt. Express

• L. Cheng, H. Zhiwei, L. Fake, Z. Wei, H. W. Dietmar, S. Colin "Near-field effects on coherent anti-Stokes Raman scattering microscopy imaging," Opt. Express 15, 4118-4131(2007). [CrossRef]

Opt. Lett.

• E. O. Potma, C. L. Evans, and X. S. Xie, "Heterodyne Coherent anti-Stokes Raman scattering (CARS) imaging," Opt. Lett. 31, 241-243 (2006). [CrossRef] [PubMed]
• J. P. Ogilvie, E. Beaurepire, A. Alexandrou, and M. Joffre, "Fourier-transform coherent anti-Stokes Raman scattering microscopy," Opt. Lett. 31, 480- 482 (2006). [CrossRef] [PubMed]

Phys, Rev.

• P.D. Maker and R.W. Terhune, "Study of optical effects due to an induced polarization third order in the electric field strength," Phys, Rev. 137, A801-A818 (1965). [CrossRef]

Phys. Rev. Lett.

• D. Oron, N. Dudovich, and Y. Silberberg, "Single-Pulse Phase-contrast nonlinear Raman Spectroscopy," Phys. Rev. Lett. 89, 273001-273004 (2002). [CrossRef]

Other

• Y. R. Shen, The principles of nonlinear optics (Wiley, New York, 1984).
• R. J.H. Clark and R. E. Hester, Advances in Nonlinear Spectroscopy, (Wiley, New York, 1988) 15.
• A. Taflove, Computational Electrodynamics: The Finite-Difference Time-Domain Method (Artech House, Boston, 1995).
• R. W. Boyd, Nonlinear Optics (Academic, Boston, Mass., 1992).
• S. Mukamel, Principles of Nonlinear Optical Spectroscopy (Oxford U. Press New York, 1995).

Click here to see a list of articles that cite this paper

Related Journal Articles

• Pure Rotational Coherent Anti-Stokes Raman Scattering: Comparison of Evaluation Techniques for Determining Single-Shot Simultaneous Temperature and Relative N₂-O₂ Concentration (AO)
• Simultaneous Temperature and Relative O₂-N₂ Concentration Measurements by Single-Shot Pure Rotational Coherent Anti-Stokes Raman Scattering for Pressures as Great as 5 MPa (AO)
• Interline Transfer CCD Camera for Gated Broadband Coherent Anti-Stokes Raman-Scattering Measurements (AO)
• Near-resonance enhanced O2 detection for dual-broadband pure rotational coherent anti-Stokes Raman scattering with an ultraviolet-visible setup at 266 nm (AO)
• Differential imaging in coherent anti-Stokes Raman scattering microscopy II: a filter-assisted Laguerre-Gaussian beam detection scheme (OE)

Related Conference Papers

• Recent Advances in CARS Microscopy
• Biomedical and Biophysical Applications of Coherent Anti-Stokes Raman Scattering Microscopy
• Raman-Like Scattering from Acoustic Phonons in Photonic Crystal Fibre
• Raman Gain in Helium Ion Implanted Silicon Waveguides
• Coherent anti-Stokes Raman scattering microscopy with near-infrared ps pulses synchronized within 50 fs