Abstract

A sum frequency generation (SFG) vibrational micro-spectroscopy system was developed to examine buried heterogeneous biointerfaces. A compact optical microscope was constructed with total-internal reflection (TIR) SFG geometry to monitor the tightly focused SFG laser spots on interfaces, providing the capability of selectively probing different regions on heterogeneous biointerfaces. The TIR configuration ensures and enhances the SFG signal generated only from the sample/substrate interfacial area. As an example for possible applications in biointerfaces studies, the system was used to probe and compare buried interfacial structures of different biological samples attached to underwater surfaces. We studied the interface of a single mouse oocyte on a silica prism to demonstrate the feasibility of tracing and studying a single live cell and substrate interface using SFG. We also examined the interface between a marine mussel adhesive plaque and a CaF2 substrate, showing the removal of interface-bonded water molecules. This work also paves the way for future integration of other microscopic techniques such as TIR-fluorescence microscopy or nonlinear optical imaging with SFG spectroscopy for multimodal surface or interface studies.

© 2014 Optical Society of America

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2013 (2)

C. Zhang, J. N. Myers, and Z. Chen, Soft Matter 9, 4738 (2013).
[CrossRef]

S. Roeters, C. van Dijk, A. Torres-Knoop, E. Backus, R. Campen, M. Bonn, and S. Woutersen, J. Phys. Chem. A 117, 6311 (2013).
[CrossRef]

2012 (1)

K. A. Smith and J. C. Conboy, Anal. Chem. 84, 8122 (2012).
[CrossRef]

2011 (5)

C. Zhang, J. Wang, A. Khmaladze, Y. Liu, B. Ding, J. Jasensky, and Z. Chen, Opt. Lett. 36, 2272 (2011).
[CrossRef]

K. C. Jena, K.-K. Hung, T. R. Schwantje, and D. K. Hore, J. Chem. Phys. 135, 044704 (2011).
[CrossRef]

E. Bulard, Z. Guo, W. Zheng, H. Dubost, M. P. Fontaine-Aupart, M. N. Bellon-Fontaine, J. M. Herry, R. Briandet, and B. Bourguignon, Langmuir 27, 4928 (2011).
[CrossRef]

V. Raghunathan, Y. Han, O. Korth, N. H. Ge, and E. O. Potma, Opt. Lett. 36, 3891 (2011).
[CrossRef]

H. C. Hieu, N. A. Tuan, H. Li, Y. Miyauchi, and G. Mizutani, Appl. Spectrosc. 65, 1254 (2011).
[CrossRef]

2010 (3)

2009 (1)

K. T. Nguyen, S. V. Le Clair, S. Ye, and Z. Chen, J. Phys. Chem. B 113, 12169 (2009).
[CrossRef]

2008 (1)

C. Howell, M. O. Diesner, M. Grunze, and P. Koelsch, Langmuir 24, 13819 (2008).
[CrossRef]

2007 (2)

N. Acevedo, J. Ding, and G. D. Smith, Biol. Reprod. 77, 872 (2007).
[CrossRef]

H. G. Silverman and F. F. Roberto, Mar. Biotechnol. 9, 661 (2007).
[CrossRef]

2006 (2)

M. S. Yeganeh, S. M. Dougal, and B. G. Silbernagel, Langmuir 22, 637 (2006).
[CrossRef]

K. Cimatu and S. Baldelli, J. Phys. Chem. B 110, 1807 (2006).
[CrossRef]

2005 (2)

A. G. Lambert, P. B. Davies, and D. J. Neivandt, Appl. Spectrosc. Rev. 40, 103 (2005).
[CrossRef]

J. Wang, X. Y. Chen, M. L. Clarke, and Z. Chen, Proc. Natl. Acad. Sci. USA 102, 4978 (2005).
[CrossRef]

2004 (1)

J. Liu and J. C. Conboy, J. Am. Chem. Soc. 126, 8376 (2004).
[CrossRef]

2003 (1)

Y. Liu and M. C. Messmer, J. Phys. Chem. B 107, 9774 (2003).
[CrossRef]

2002 (2)

Z. Chen, Y. R. Shen, and G. A. Somorjai, Annu. Rev. Phys. Chem. 53, 437 (2002).
[CrossRef]

D. Hoffmann, K. Kuhnke, and K. Kern, Rev. Sci. Instrum. 73, 3221 (2002).
[CrossRef]

2001 (1)

S. Ye, S. Nihonyanagi, and K. Uosaki, Phys. Chem. Chem. Phys. 3, 3463 (2001).
[CrossRef]

2000 (1)

K. S. Gautam, A. D. Schwab, A. Dhinojwala, D. Zhang, S. M. Dougal, and M. S. Yeganeh, Phys. Rev. Lett. 85, 3854 (2000).
[CrossRef]

1999 (1)

M. Flörsheimer, C. Brillert, and H. Fuchs, Langmuir 15, 5437 (1999).
[CrossRef]

1989 (1)

Y. R. Shen, Nature 337, 519 (1989).
[CrossRef]

Acevedo, N.

N. Acevedo, J. Ding, and G. D. Smith, Biol. Reprod. 77, 872 (2007).
[CrossRef]

Backus, E.

S. Roeters, C. van Dijk, A. Torres-Knoop, E. Backus, R. Campen, M. Bonn, and S. Woutersen, J. Phys. Chem. A 117, 6311 (2013).
[CrossRef]

Baldelli, S.

K. Cimatu and S. Baldelli, J. Phys. Chem. B 110, 1807 (2006).
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Bellon-Fontaine, M. N.

E. Bulard, Z. Guo, W. Zheng, H. Dubost, M. P. Fontaine-Aupart, M. N. Bellon-Fontaine, J. M. Herry, R. Briandet, and B. Bourguignon, Langmuir 27, 4928 (2011).
[CrossRef]

Bonn, M.

S. Roeters, C. van Dijk, A. Torres-Knoop, E. Backus, R. Campen, M. Bonn, and S. Woutersen, J. Phys. Chem. A 117, 6311 (2013).
[CrossRef]

Bourguignon, B.

E. Bulard, Z. Guo, W. Zheng, H. Dubost, M. P. Fontaine-Aupart, M. N. Bellon-Fontaine, J. M. Herry, R. Briandet, and B. Bourguignon, Langmuir 27, 4928 (2011).
[CrossRef]

Briandet, R.

E. Bulard, Z. Guo, W. Zheng, H. Dubost, M. P. Fontaine-Aupart, M. N. Bellon-Fontaine, J. M. Herry, R. Briandet, and B. Bourguignon, Langmuir 27, 4928 (2011).
[CrossRef]

Brillert, C.

M. Flörsheimer, C. Brillert, and H. Fuchs, Langmuir 15, 5437 (1999).
[CrossRef]

Bulard, E.

E. Bulard, Z. Guo, W. Zheng, H. Dubost, M. P. Fontaine-Aupart, M. N. Bellon-Fontaine, J. M. Herry, R. Briandet, and B. Bourguignon, Langmuir 27, 4928 (2011).
[CrossRef]

Campen, R.

S. Roeters, C. van Dijk, A. Torres-Knoop, E. Backus, R. Campen, M. Bonn, and S. Woutersen, J. Phys. Chem. A 117, 6311 (2013).
[CrossRef]

Chen, X. Y.

J. Wang, X. Y. Chen, M. L. Clarke, and Z. Chen, Proc. Natl. Acad. Sci. USA 102, 4978 (2005).
[CrossRef]

Chen, Z.

C. Zhang, J. N. Myers, and Z. Chen, Soft Matter 9, 4738 (2013).
[CrossRef]

C. Zhang, J. Wang, A. Khmaladze, Y. Liu, B. Ding, J. Jasensky, and Z. Chen, Opt. Lett. 36, 2272 (2011).
[CrossRef]

K. T. Nguyen, S. V. Le Clair, S. Ye, and Z. Chen, J. Phys. Chem. B 113, 12169 (2009).
[CrossRef]

J. Wang, X. Y. Chen, M. L. Clarke, and Z. Chen, Proc. Natl. Acad. Sci. USA 102, 4978 (2005).
[CrossRef]

Z. Chen, Y. R. Shen, and G. A. Somorjai, Annu. Rev. Phys. Chem. 53, 437 (2002).
[CrossRef]

Cimatu, K.

K. Cimatu and S. Baldelli, J. Phys. Chem. B 110, 1807 (2006).
[CrossRef]

Clarke, M. L.

J. Wang, X. Y. Chen, M. L. Clarke, and Z. Chen, Proc. Natl. Acad. Sci. USA 102, 4978 (2005).
[CrossRef]

Conboy, J. C.

K. A. Smith and J. C. Conboy, Anal. Chem. 84, 8122 (2012).
[CrossRef]

J. Liu and J. C. Conboy, J. Am. Chem. Soc. 126, 8376 (2004).
[CrossRef]

Davies, P. B.

A. G. Lambert, P. B. Davies, and D. J. Neivandt, Appl. Spectrosc. Rev. 40, 103 (2005).
[CrossRef]

Dhinojwala, A.

K. S. Gautam, A. D. Schwab, A. Dhinojwala, D. Zhang, S. M. Dougal, and M. S. Yeganeh, Phys. Rev. Lett. 85, 3854 (2000).
[CrossRef]

Diesner, M. O.

M. O. Diesner, C. Howell, V. Kurz, D. Verreault, and P. Koelsch, J. Phys. Chem. Lett. 1, 2339 (2010).
[CrossRef]

C. Howell, M. O. Diesner, M. Grunze, and P. Koelsch, Langmuir 24, 13819 (2008).
[CrossRef]

Ding, B.

Ding, J.

N. Acevedo, J. Ding, and G. D. Smith, Biol. Reprod. 77, 872 (2007).
[CrossRef]

Dougal, S. M.

M. S. Yeganeh, S. M. Dougal, and B. G. Silbernagel, Langmuir 22, 637 (2006).
[CrossRef]

K. S. Gautam, A. D. Schwab, A. Dhinojwala, D. Zhang, S. M. Dougal, and M. S. Yeganeh, Phys. Rev. Lett. 85, 3854 (2000).
[CrossRef]

Dubost, H.

E. Bulard, Z. Guo, W. Zheng, H. Dubost, M. P. Fontaine-Aupart, M. N. Bellon-Fontaine, J. M. Herry, R. Briandet, and B. Bourguignon, Langmuir 27, 4928 (2011).
[CrossRef]

Flörsheimer, M.

M. Flörsheimer, C. Brillert, and H. Fuchs, Langmuir 15, 5437 (1999).
[CrossRef]

Fontaine-Aupart, M. P.

E. Bulard, Z. Guo, W. Zheng, H. Dubost, M. P. Fontaine-Aupart, M. N. Bellon-Fontaine, J. M. Herry, R. Briandet, and B. Bourguignon, Langmuir 27, 4928 (2011).
[CrossRef]

Fuchs, H.

M. Flörsheimer, C. Brillert, and H. Fuchs, Langmuir 15, 5437 (1999).
[CrossRef]

Fujii, M.

Gautam, K. S.

K. S. Gautam, A. D. Schwab, A. Dhinojwala, D. Zhang, S. M. Dougal, and M. S. Yeganeh, Phys. Rev. Lett. 85, 3854 (2000).
[CrossRef]

Ge, N. H.

Grunze, M.

C. Howell, M. O. Diesner, M. Grunze, and P. Koelsch, Langmuir 24, 13819 (2008).
[CrossRef]

Guo, Z.

E. Bulard, Z. Guo, W. Zheng, H. Dubost, M. P. Fontaine-Aupart, M. N. Bellon-Fontaine, J. M. Herry, R. Briandet, and B. Bourguignon, Langmuir 27, 4928 (2011).
[CrossRef]

Han, Y.

Herry, J. M.

E. Bulard, Z. Guo, W. Zheng, H. Dubost, M. P. Fontaine-Aupart, M. N. Bellon-Fontaine, J. M. Herry, R. Briandet, and B. Bourguignon, Langmuir 27, 4928 (2011).
[CrossRef]

Hieu, H. C.

Hoffmann, D.

D. Hoffmann, K. Kuhnke, and K. Kern, Rev. Sci. Instrum. 73, 3221 (2002).
[CrossRef]

Hore, D. K.

K. C. Jena, K.-K. Hung, T. R. Schwantje, and D. K. Hore, J. Chem. Phys. 135, 044704 (2011).
[CrossRef]

Howell, C.

M. O. Diesner, C. Howell, V. Kurz, D. Verreault, and P. Koelsch, J. Phys. Chem. Lett. 1, 2339 (2010).
[CrossRef]

C. Howell, M. O. Diesner, M. Grunze, and P. Koelsch, Langmuir 24, 13819 (2008).
[CrossRef]

Hung, K.-K.

K. C. Jena, K.-K. Hung, T. R. Schwantje, and D. K. Hore, J. Chem. Phys. 135, 044704 (2011).
[CrossRef]

Inoue, K.

Ishihara, M.

Jasensky, J.

Jena, K. C.

K. C. Jena, K.-K. Hung, T. R. Schwantje, and D. K. Hore, J. Chem. Phys. 135, 044704 (2011).
[CrossRef]

Kern, K.

D. Hoffmann, K. Kuhnke, and K. Kern, Rev. Sci. Instrum. 73, 3221 (2002).
[CrossRef]

Khmaladze, A.

Kikuchi, M.

Koelsch, P.

M. O. Diesner, C. Howell, V. Kurz, D. Verreault, and P. Koelsch, J. Phys. Chem. Lett. 1, 2339 (2010).
[CrossRef]

C. Howell, M. O. Diesner, M. Grunze, and P. Koelsch, Langmuir 24, 13819 (2008).
[CrossRef]

Kogure, S.

Korth, O.

Kuhnke, K.

D. Hoffmann, K. Kuhnke, and K. Kern, Rev. Sci. Instrum. 73, 3221 (2002).
[CrossRef]

Kurz, V.

M. O. Diesner, C. Howell, V. Kurz, D. Verreault, and P. Koelsch, J. Phys. Chem. Lett. 1, 2339 (2010).
[CrossRef]

Lambert, A. G.

A. G. Lambert, P. B. Davies, and D. J. Neivandt, Appl. Spectrosc. Rev. 40, 103 (2005).
[CrossRef]

Le Clair, S. V.

K. T. Nguyen, S. V. Le Clair, S. Ye, and Z. Chen, J. Phys. Chem. B 113, 12169 (2009).
[CrossRef]

Li, H.

Liu, J.

J. Liu and J. C. Conboy, J. Am. Chem. Soc. 126, 8376 (2004).
[CrossRef]

Liu, Y.

Messmer, M. C.

Y. Liu and M. C. Messmer, J. Phys. Chem. B 107, 9774 (2003).
[CrossRef]

Miyauchi, Y.

Mizutani, G.

Myers, J. N.

C. Zhang, J. N. Myers, and Z. Chen, Soft Matter 9, 4738 (2013).
[CrossRef]

Neivandt, D. J.

A. G. Lambert, P. B. Davies, and D. J. Neivandt, Appl. Spectrosc. Rev. 40, 103 (2005).
[CrossRef]

Nguyen, K. T.

K. T. Nguyen, S. V. Le Clair, S. Ye, and Z. Chen, J. Phys. Chem. B 113, 12169 (2009).
[CrossRef]

Nihonyanagi, S.

S. Ye, S. Nihonyanagi, and K. Uosaki, Phys. Chem. Chem. Phys. 3, 3463 (2001).
[CrossRef]

Ohmori, T.

Potma, E. O.

Raghunathan, V.

Roberto, F. F.

H. G. Silverman and F. F. Roberto, Mar. Biotechnol. 9, 661 (2007).
[CrossRef]

Roeters, S.

S. Roeters, C. van Dijk, A. Torres-Knoop, E. Backus, R. Campen, M. Bonn, and S. Woutersen, J. Phys. Chem. A 117, 6311 (2013).
[CrossRef]

Sakai, M.

Schwab, A. D.

K. S. Gautam, A. D. Schwab, A. Dhinojwala, D. Zhang, S. M. Dougal, and M. S. Yeganeh, Phys. Rev. Lett. 85, 3854 (2000).
[CrossRef]

Schwantje, T. R.

K. C. Jena, K.-K. Hung, T. R. Schwantje, and D. K. Hore, J. Chem. Phys. 135, 044704 (2011).
[CrossRef]

Shen, Y. R.

Z. Chen, Y. R. Shen, and G. A. Somorjai, Annu. Rev. Phys. Chem. 53, 437 (2002).
[CrossRef]

Y. R. Shen, Nature 337, 519 (1989).
[CrossRef]

Silbernagel, B. G.

M. S. Yeganeh, S. M. Dougal, and B. G. Silbernagel, Langmuir 22, 637 (2006).
[CrossRef]

Silverman, H. G.

H. G. Silverman and F. F. Roberto, Mar. Biotechnol. 9, 661 (2007).
[CrossRef]

Smith, G. D.

N. Acevedo, J. Ding, and G. D. Smith, Biol. Reprod. 77, 872 (2007).
[CrossRef]

Smith, K. A.

K. A. Smith and J. C. Conboy, Anal. Chem. 84, 8122 (2012).
[CrossRef]

Somorjai, G. A.

Z. Chen, Y. R. Shen, and G. A. Somorjai, Annu. Rev. Phys. Chem. 53, 437 (2002).
[CrossRef]

Torres-Knoop, A.

S. Roeters, C. van Dijk, A. Torres-Knoop, E. Backus, R. Campen, M. Bonn, and S. Woutersen, J. Phys. Chem. A 117, 6311 (2013).
[CrossRef]

Tuan, N. A.

Uosaki, K.

S. Ye, S. Nihonyanagi, and K. Uosaki, Phys. Chem. Chem. Phys. 3, 3463 (2001).
[CrossRef]

van Dijk, C.

S. Roeters, C. van Dijk, A. Torres-Knoop, E. Backus, R. Campen, M. Bonn, and S. Woutersen, J. Phys. Chem. A 117, 6311 (2013).
[CrossRef]

Verreault, D.

M. O. Diesner, C. Howell, V. Kurz, D. Verreault, and P. Koelsch, J. Phys. Chem. Lett. 1, 2339 (2010).
[CrossRef]

Wang, J.

C. Zhang, J. Wang, A. Khmaladze, Y. Liu, B. Ding, J. Jasensky, and Z. Chen, Opt. Lett. 36, 2272 (2011).
[CrossRef]

J. Wang, X. Y. Chen, M. L. Clarke, and Z. Chen, Proc. Natl. Acad. Sci. USA 102, 4978 (2005).
[CrossRef]

Woutersen, S.

S. Roeters, C. van Dijk, A. Torres-Knoop, E. Backus, R. Campen, M. Bonn, and S. Woutersen, J. Phys. Chem. A 117, 6311 (2013).
[CrossRef]

Ye, S.

K. T. Nguyen, S. V. Le Clair, S. Ye, and Z. Chen, J. Phys. Chem. B 113, 12169 (2009).
[CrossRef]

S. Ye, S. Nihonyanagi, and K. Uosaki, Phys. Chem. Chem. Phys. 3, 3463 (2001).
[CrossRef]

Yeganeh, M. S.

M. S. Yeganeh, S. M. Dougal, and B. G. Silbernagel, Langmuir 22, 637 (2006).
[CrossRef]

K. S. Gautam, A. D. Schwab, A. Dhinojwala, D. Zhang, S. M. Dougal, and M. S. Yeganeh, Phys. Rev. Lett. 85, 3854 (2000).
[CrossRef]

Zhang, C.

Zhang, D.

K. S. Gautam, A. D. Schwab, A. Dhinojwala, D. Zhang, S. M. Dougal, and M. S. Yeganeh, Phys. Rev. Lett. 85, 3854 (2000).
[CrossRef]

Zheng, W.

E. Bulard, Z. Guo, W. Zheng, H. Dubost, M. P. Fontaine-Aupart, M. N. Bellon-Fontaine, J. M. Herry, R. Briandet, and B. Bourguignon, Langmuir 27, 4928 (2011).
[CrossRef]

Anal. Chem. (1)

K. A. Smith and J. C. Conboy, Anal. Chem. 84, 8122 (2012).
[CrossRef]

Annu. Rev. Phys. Chem. (1)

Z. Chen, Y. R. Shen, and G. A. Somorjai, Annu. Rev. Phys. Chem. 53, 437 (2002).
[CrossRef]

Appl. Spectrosc. (2)

Appl. Spectrosc. Rev. (1)

A. G. Lambert, P. B. Davies, and D. J. Neivandt, Appl. Spectrosc. Rev. 40, 103 (2005).
[CrossRef]

Biol. Reprod. (1)

N. Acevedo, J. Ding, and G. D. Smith, Biol. Reprod. 77, 872 (2007).
[CrossRef]

J. Am. Chem. Soc. (1)

J. Liu and J. C. Conboy, J. Am. Chem. Soc. 126, 8376 (2004).
[CrossRef]

J. Chem. Phys. (1)

K. C. Jena, K.-K. Hung, T. R. Schwantje, and D. K. Hore, J. Chem. Phys. 135, 044704 (2011).
[CrossRef]

J. Phys. Chem. A (1)

S. Roeters, C. van Dijk, A. Torres-Knoop, E. Backus, R. Campen, M. Bonn, and S. Woutersen, J. Phys. Chem. A 117, 6311 (2013).
[CrossRef]

J. Phys. Chem. B (3)

K. Cimatu and S. Baldelli, J. Phys. Chem. B 110, 1807 (2006).
[CrossRef]

K. T. Nguyen, S. V. Le Clair, S. Ye, and Z. Chen, J. Phys. Chem. B 113, 12169 (2009).
[CrossRef]

Y. Liu and M. C. Messmer, J. Phys. Chem. B 107, 9774 (2003).
[CrossRef]

J. Phys. Chem. Lett. (1)

M. O. Diesner, C. Howell, V. Kurz, D. Verreault, and P. Koelsch, J. Phys. Chem. Lett. 1, 2339 (2010).
[CrossRef]

Langmuir (4)

E. Bulard, Z. Guo, W. Zheng, H. Dubost, M. P. Fontaine-Aupart, M. N. Bellon-Fontaine, J. M. Herry, R. Briandet, and B. Bourguignon, Langmuir 27, 4928 (2011).
[CrossRef]

M. Flörsheimer, C. Brillert, and H. Fuchs, Langmuir 15, 5437 (1999).
[CrossRef]

C. Howell, M. O. Diesner, M. Grunze, and P. Koelsch, Langmuir 24, 13819 (2008).
[CrossRef]

M. S. Yeganeh, S. M. Dougal, and B. G. Silbernagel, Langmuir 22, 637 (2006).
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Mar. Biotechnol. (1)

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Figures (4)

Fig. 1.
Fig. 1.

Schematic of the beam tracking TIR-SFG system. The SFG spectrometer is not shown in the figure.

Fig. 2.
Fig. 2.

A, SFG spectra of a PMMA surface in air using 10, 20, and 30 μJ (bottom to top) incident visible pulse energies. The spectra (lines) were fit using the method shown in Ref. [6]. B, BF image of the PMMA surface when the SFG spectrum was being collected with 30 μJ incident visible beam pulse energy. The strong scattering indicates the surface photodamage. C, BF image of the same sample location collected using a white light source without the input lasers after the SFG signal collection.

Fig. 3.
Fig. 3.

A, BF image of the visible beam focused on the buffer/substrate interface. B, BF image of the visible beam focused on a mouse oocyte/substrate interface. C, SFG spectra taken on locations shown in A (top) and B (bottom). Dots are experimental collected data and lines are the fitting results.

Fig. 4.
Fig. 4.

A, schematic of the SFG experiment at a mussel plaque/CaF2 interface and a water/CaF2 interface. B, BF image of a position within the mussel plaque demonstrated in A. C, BF image of a position in a “blank” water/CaF2 area, demonstrated in A. D, SFG spectrum in the CO range collected in position 1. E, SFG spectrum in the CH/OH range collected in position 1. F, SFG spectrum in the CH/OH range collected in position 2.

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