Abstract

We apply femtosecond pulse shaping to generate optical pulse trains that directly access a material’s nonlinear refractive index (n2) and can thus determine time-resolved optical Kerr-effect (OKE) dynamics. Two types of static pulse trains are discussed: The first uses two identical fields delayed in time, plus a pump field at a different wavelength. Time-resolved OKE dynamics are retrieved by monitoring the phase of the interference pattern produced by the two identical fields in the Fourier-domain (FD) as a function of pump–probe–time–delay (where the probe is one of the two identical fields). The second pulse train uses three fields with equal time delays, but with the center field phase shifted by π/2. In this pulse scheme, changes on a sample’s nonlinear refractive index produce a new frequency in the FD signal, which in turn yields background-free intensity changes in the conjugate (time) domain and provides superior signal-to-noise ratios. The demonstrated sensitivity improvements enable, for the first time to our knowledge, molecular imaging based on OKE dynamics.

© 2014 Optical Society of America

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2013 (4)

N. G. Horton, K. Wang, D. Kobat, C. G. Clark, F. W. Wise, C. B. Schaffer, and C. Xu, Nat. Photonics 7, 205 (2013).
[CrossRef]

F. E. Robles, J. W. Wilson, and W. S. Warren, J. Biomed. Opt. 18, 120502 (2013).
[CrossRef]

J. W. Wilson, L. Vajzovic, F. E. Robles, T. J. Cummings, P. Mruthyunjaya, and W. S. Warren, Investig. Ophthalmol. Vis. Sci. 54, 6867 (2013).
[CrossRef]

F. E. Robles, P. Samineni, J. W. Wilson, and W. S. Warren, Opt. Express 21, 9353 (2013).
[CrossRef]

2012 (3)

2011 (2)

T. E. Matthews, I. R. Piletic, M. A. Selim, M. J. Simpson, and W. S. Warren, Sci. Trans. Med. 3, 71ra15 (2011).

F. E. Robles, L. L. Satterwhite, and A. Wax, Opt. Lett. 36, 4665 (2011).
[CrossRef]

2010 (2)

B. G. Saar, C. W. Freudiger, J. Reichman, C. M. Stanley, G. R. Holtom, and X. S. Xie, Science 330, 1368 (2010).
[CrossRef]

P. Samineni, Z. Perret, W. Warren, and M. C. Fischer, Opt. Express 18, 12727 (2010).
[CrossRef]

2008 (2)

2005 (2)

M. Fischer, T. Ye, G. Yurtsever, A. Miller, M. Ciocca, W. Wagner, and W. Warren, Opt. Lett. 30, 1551 (2005).
[CrossRef]

I. A. Heisler, R. R. B. Correia, T. Buckup, S. L. S. Cunha, and N. P. da Silveira, J. Chem. Phys. 123, 054509 (2005).
[CrossRef]

2001 (1)

E. O. Potma, W. P. de Boeij, and D. A. Wiersma, Biophys. J. 80, 3019 (2001).
[CrossRef]

1997 (2)

M. A. Dugan, J. X. Tull, and W. S. Warren, J. Opt. Soc. Am. B 14, 2348 (1997).
[CrossRef]

P. B. Chapple, J. Staromlynska, J. A. Hermann, T. J. McKay, and R. G. McDuff, J. Nonlinear Opt. Phys. Mater. 6, 251 (1997).
[CrossRef]

1993 (1)

Y. J. Chang and E. W. Castner, J. Chem. Phys. 99, 113 (1993).
[CrossRef]

1990 (1)

W. Denk, J. H. Strickler, and W. W. Webb, Science 248, 73 (1990).
[CrossRef]

1983 (1)

G. C. Bjorklund, M. D. Levenson, W. Lenth, and C. Ortiz, Appl. Phys. B 32, 145 (1983).
[CrossRef]

Bjorklund, G. C.

G. C. Bjorklund, M. D. Levenson, W. Lenth, and C. Ortiz, Appl. Phys. B 32, 145 (1983).
[CrossRef]

Buckup, T.

I. A. Heisler, R. R. B. Correia, T. Buckup, S. L. S. Cunha, and N. P. da Silveira, J. Chem. Phys. 123, 054509 (2005).
[CrossRef]

Castner, E. W.

Y. J. Chang and E. W. Castner, J. Chem. Phys. 99, 113 (1993).
[CrossRef]

Chang, Y. J.

Y. J. Chang and E. W. Castner, J. Chem. Phys. 99, 113 (1993).
[CrossRef]

Chapple, P. B.

P. B. Chapple, J. Staromlynska, J. A. Hermann, T. J. McKay, and R. G. McDuff, J. Nonlinear Opt. Phys. Mater. 6, 251 (1997).
[CrossRef]

Ciocca, M.

Clark, C. G.

N. G. Horton, K. Wang, D. Kobat, C. G. Clark, F. W. Wise, C. B. Schaffer, and C. Xu, Nat. Photonics 7, 205 (2013).
[CrossRef]

Claytor, K. E.

Correia, R. R. B.

I. A. Heisler, R. R. B. Correia, T. Buckup, S. L. S. Cunha, and N. P. da Silveira, J. Chem. Phys. 123, 054509 (2005).
[CrossRef]

Cummings, T. J.

J. W. Wilson, L. Vajzovic, F. E. Robles, T. J. Cummings, P. Mruthyunjaya, and W. S. Warren, Investig. Ophthalmol. Vis. Sci. 54, 6867 (2013).
[CrossRef]

Cunha, S. L. S.

I. A. Heisler, R. R. B. Correia, T. Buckup, S. L. S. Cunha, and N. P. da Silveira, J. Chem. Phys. 123, 054509 (2005).
[CrossRef]

da Silveira, N. P.

I. A. Heisler, R. R. B. Correia, T. Buckup, S. L. S. Cunha, and N. P. da Silveira, J. Chem. Phys. 123, 054509 (2005).
[CrossRef]

de Boeij, W. P.

E. O. Potma, W. P. de Boeij, and D. A. Wiersma, Biophys. J. 80, 3019 (2001).
[CrossRef]

Denk, W.

W. Denk, J. H. Strickler, and W. W. Webb, Science 248, 73 (1990).
[CrossRef]

Dugan, M. A.

Escobedo-Lozoya, Y.

Fischer, M.

Fischer, M. C.

Freudiger, C. W.

B. G. Saar, C. W. Freudiger, J. Reichman, C. M. Stanley, G. R. Holtom, and X. S. Xie, Science 330, 1368 (2010).
[CrossRef]

Heisler, I. A.

I. A. Heisler, R. R. B. Correia, T. Buckup, S. L. S. Cunha, and N. P. da Silveira, J. Chem. Phys. 123, 054509 (2005).
[CrossRef]

Hermann, J. A.

P. B. Chapple, J. Staromlynska, J. A. Hermann, T. J. McKay, and R. G. McDuff, J. Nonlinear Opt. Phys. Mater. 6, 251 (1997).
[CrossRef]

Holtom, G. R.

B. G. Saar, C. W. Freudiger, J. Reichman, C. M. Stanley, G. R. Holtom, and X. S. Xie, Science 330, 1368 (2010).
[CrossRef]

Horton, N. G.

N. G. Horton, K. Wang, D. Kobat, C. G. Clark, F. W. Wise, C. B. Schaffer, and C. Xu, Nat. Photonics 7, 205 (2013).
[CrossRef]

Kobat, D.

N. G. Horton, K. Wang, D. Kobat, C. G. Clark, F. W. Wise, C. B. Schaffer, and C. Xu, Nat. Photonics 7, 205 (2013).
[CrossRef]

Lenth, W.

G. C. Bjorklund, M. D. Levenson, W. Lenth, and C. Ortiz, Appl. Phys. B 32, 145 (1983).
[CrossRef]

Levenson, M. D.

G. C. Bjorklund, M. D. Levenson, W. Lenth, and C. Ortiz, Appl. Phys. B 32, 145 (1983).
[CrossRef]

Li, B.

Liu, H. C.

Matthews, T. E.

T. E. Matthews, I. R. Piletic, M. A. Selim, M. J. Simpson, and W. S. Warren, Sci. Trans. Med. 3, 71ra15 (2011).

McDuff, R. G.

P. B. Chapple, J. Staromlynska, J. A. Hermann, T. J. McKay, and R. G. McDuff, J. Nonlinear Opt. Phys. Mater. 6, 251 (1997).
[CrossRef]

McKay, T. J.

P. B. Chapple, J. Staromlynska, J. A. Hermann, T. J. McKay, and R. G. McDuff, J. Nonlinear Opt. Phys. Mater. 6, 251 (1997).
[CrossRef]

Miller, A.

Mruthyunjaya, P.

J. W. Wilson, L. Vajzovic, F. E. Robles, T. J. Cummings, P. Mruthyunjaya, and W. S. Warren, Investig. Ophthalmol. Vis. Sci. 54, 6867 (2013).
[CrossRef]

Ortiz, C.

G. C. Bjorklund, M. D. Levenson, W. Lenth, and C. Ortiz, Appl. Phys. B 32, 145 (1983).
[CrossRef]

Perret, Z.

Piletic, I. R.

Potma, E. O.

E. O. Potma, W. P. de Boeij, and D. A. Wiersma, Biophys. J. 80, 3019 (2001).
[CrossRef]

Reichman, J.

B. G. Saar, C. W. Freudiger, J. Reichman, C. M. Stanley, G. R. Holtom, and X. S. Xie, Science 330, 1368 (2010).
[CrossRef]

Robles, F. E.

F. E. Robles, P. Samineni, J. W. Wilson, and W. S. Warren, Opt. Express 21, 9353 (2013).
[CrossRef]

J. W. Wilson, L. Vajzovic, F. E. Robles, T. J. Cummings, P. Mruthyunjaya, and W. S. Warren, Investig. Ophthalmol. Vis. Sci. 54, 6867 (2013).
[CrossRef]

F. E. Robles, J. W. Wilson, and W. S. Warren, J. Biomed. Opt. 18, 120502 (2013).
[CrossRef]

F. E. Robles, L. L. Satterwhite, and A. Wax, Opt. Lett. 36, 4665 (2011).
[CrossRef]

Saar, B. G.

B. G. Saar, C. W. Freudiger, J. Reichman, C. M. Stanley, G. R. Holtom, and X. S. Xie, Science 330, 1368 (2010).
[CrossRef]

Samineni, P.

Satterwhite, L. L.

Schaffer, C. B.

N. G. Horton, K. Wang, D. Kobat, C. G. Clark, F. W. Wise, C. B. Schaffer, and C. Xu, Nat. Photonics 7, 205 (2013).
[CrossRef]

Selim, M. A.

T. E. Matthews, I. R. Piletic, M. A. Selim, M. J. Simpson, and W. S. Warren, Sci. Trans. Med. 3, 71ra15 (2011).

Simpson, M. J.

T. E. Matthews, I. R. Piletic, M. A. Selim, M. J. Simpson, and W. S. Warren, Sci. Trans. Med. 3, 71ra15 (2011).

Stanley, C. M.

B. G. Saar, C. W. Freudiger, J. Reichman, C. M. Stanley, G. R. Holtom, and X. S. Xie, Science 330, 1368 (2010).
[CrossRef]

Staromlynska, J.

P. B. Chapple, J. Staromlynska, J. A. Hermann, T. J. McKay, and R. G. McDuff, J. Nonlinear Opt. Phys. Mater. 6, 251 (1997).
[CrossRef]

Strickler, J. H.

W. Denk, J. H. Strickler, and W. W. Webb, Science 248, 73 (1990).
[CrossRef]

Tull, J. X.

Vajzovic, L.

J. W. Wilson, L. Vajzovic, F. E. Robles, T. J. Cummings, P. Mruthyunjaya, and W. S. Warren, Investig. Ophthalmol. Vis. Sci. 54, 6867 (2013).
[CrossRef]

Vo-Dinh, T.

Wagner, W.

Wang, K.

N. G. Horton, K. Wang, D. Kobat, C. G. Clark, F. W. Wise, C. B. Schaffer, and C. Xu, Nat. Photonics 7, 205 (2013).
[CrossRef]

Warren, W.

Warren, W. S.

Wax, A.

Webb, W. W.

W. Denk, J. H. Strickler, and W. W. Webb, Science 248, 73 (1990).
[CrossRef]

Wiersma, D. A.

E. O. Potma, W. P. de Boeij, and D. A. Wiersma, Biophys. J. 80, 3019 (2001).
[CrossRef]

Wilson, J. W.

F. E. Robles, J. W. Wilson, and W. S. Warren, J. Biomed. Opt. 18, 120502 (2013).
[CrossRef]

J. W. Wilson, L. Vajzovic, F. E. Robles, T. J. Cummings, P. Mruthyunjaya, and W. S. Warren, Investig. Ophthalmol. Vis. Sci. 54, 6867 (2013).
[CrossRef]

F. E. Robles, P. Samineni, J. W. Wilson, and W. S. Warren, Opt. Express 21, 9353 (2013).
[CrossRef]

P. Samineni, B. Li, J. W. Wilson, W. S. Warren, and M. C. Fischer, Opt. Lett. 37, 800 (2012).
[CrossRef]

J. W. Wilson, P. Samineni, W. S. Warren, and M. C. Fischer, Biomed. Opt. Express 3, 854 (2012).
[CrossRef]

Wise, F. W.

N. G. Horton, K. Wang, D. Kobat, C. G. Clark, F. W. Wise, C. B. Schaffer, and C. Xu, Nat. Photonics 7, 205 (2013).
[CrossRef]

Xie, X. S.

B. G. Saar, C. W. Freudiger, J. Reichman, C. M. Stanley, G. R. Holtom, and X. S. Xie, Science 330, 1368 (2010).
[CrossRef]

Xu, C.

N. G. Horton, K. Wang, D. Kobat, C. G. Clark, F. W. Wise, C. B. Schaffer, and C. Xu, Nat. Photonics 7, 205 (2013).
[CrossRef]

Yasuda, R.

Ye, T.

Yuan, H.

Yurtsever, G.

Appl. Phys. B (1)

G. C. Bjorklund, M. D. Levenson, W. Lenth, and C. Ortiz, Appl. Phys. B 32, 145 (1983).
[CrossRef]

Biomed. Opt. Express (1)

Biophys. J. (1)

E. O. Potma, W. P. de Boeij, and D. A. Wiersma, Biophys. J. 80, 3019 (2001).
[CrossRef]

Investig. Ophthalmol. Vis. Sci. (1)

J. W. Wilson, L. Vajzovic, F. E. Robles, T. J. Cummings, P. Mruthyunjaya, and W. S. Warren, Investig. Ophthalmol. Vis. Sci. 54, 6867 (2013).
[CrossRef]

J. Biomed. Opt. (1)

F. E. Robles, J. W. Wilson, and W. S. Warren, J. Biomed. Opt. 18, 120502 (2013).
[CrossRef]

J. Chem. Phys. (2)

I. A. Heisler, R. R. B. Correia, T. Buckup, S. L. S. Cunha, and N. P. da Silveira, J. Chem. Phys. 123, 054509 (2005).
[CrossRef]

Y. J. Chang and E. W. Castner, J. Chem. Phys. 99, 113 (1993).
[CrossRef]

J. Nonlinear Opt. Phys. Mater. (1)

P. B. Chapple, J. Staromlynska, J. A. Hermann, T. J. McKay, and R. G. McDuff, J. Nonlinear Opt. Phys. Mater. 6, 251 (1997).
[CrossRef]

J. Opt. Soc. Am. B (1)

Nat. Photonics (1)

N. G. Horton, K. Wang, D. Kobat, C. G. Clark, F. W. Wise, C. B. Schaffer, and C. Xu, Nat. Photonics 7, 205 (2013).
[CrossRef]

Opt. Express (3)

Opt. Lett. (5)

Sci. Trans. Med. (1)

T. E. Matthews, I. R. Piletic, M. A. Selim, M. J. Simpson, and W. S. Warren, Sci. Trans. Med. 3, 71ra15 (2011).

Science (2)

W. Denk, J. H. Strickler, and W. W. Webb, Science 248, 73 (1990).
[CrossRef]

B. G. Saar, C. W. Freudiger, J. Reichman, C. M. Stanley, G. R. Holtom, and X. S. Xie, Science 330, 1368 (2010).
[CrossRef]

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