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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References

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  1. W. Denk, J. H. Strickler, and W. W. Webb, Science 248, 73 (1990).
    [CrossRef]
  2. 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]
  3. B. G. Saar, C. W. Freudiger, J. Reichman, C. M. Stanley, G. R. Holtom, and X. S. Xie, Science 330, 1368 (2010).
    [CrossRef]
  4. T. E. Matthews, I. R. Piletic, M. A. Selim, M. J. Simpson, and W. S. Warren, Sci. Trans. Med. 3, 71ra15 (2011).
  5. F. E. Robles, J. W. Wilson, and W. S. Warren, J. Biomed. Opt. 18, 120502 (2013).
    [CrossRef]
  6. 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]
  7. P. B. Chapple, J. Staromlynska, J. A. Hermann, T. J. McKay, and R. G. McDuff, J. Nonlinear Opt. Phys. Mater. 6, 251 (1997).
    [CrossRef]
  8. P. Samineni, Z. Perret, W. Warren, and M. C. Fischer, Opt. Express 18, 12727 (2010).
    [CrossRef]
  9. M. Fischer, T. Ye, G. Yurtsever, A. Miller, M. Ciocca, W. Wagner, and W. Warren, Opt. Lett. 30, 1551 (2005).
    [CrossRef]
  10. M. C. Fischer, H. C. Liu, I. R. Piletic, Y. Escobedo-Lozoya, R. Yasuda, and W. S. Warren, Opt. Lett. 33, 219 (2008).
    [CrossRef]
  11. P. Samineni, B. Li, J. W. Wilson, W. S. Warren, and M. C. Fischer, Opt. Lett. 37, 800 (2012).
    [CrossRef]
  12. J. W. Wilson, P. Samineni, W. S. Warren, and M. C. Fischer, Biomed. Opt. Express 3, 854 (2012).
    [CrossRef]
  13. B. Li, K. E. Claytor, H. Yuan, T. Vo-Dinh, W. S. Warren, and M. C. Fischer, Opt. Lett. 37, 2763 (2012).
    [CrossRef]
  14. E. O. Potma, W. P. de Boeij, and D. A. Wiersma, Biophys. J. 80, 3019 (2001).
    [CrossRef]
  15. 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]
  16. Y. J. Chang and E. W. Castner, J. Chem. Phys. 99, 113 (1993).
    [CrossRef]
  17. F. E. Robles, P. Samineni, J. W. Wilson, and W. S. Warren, Opt. Express 21, 9353 (2013).
    [CrossRef]
  18. M. A. Dugan, J. X. Tull, and W. S. Warren, J. Opt. Soc. Am. B 14, 2348 (1997).
    [CrossRef]
  19. F. E. Robles, L. L. Satterwhite, and A. Wax, Opt. Lett. 36, 4665 (2011).
    [CrossRef]
  20. G. C. Bjorklund, M. D. Levenson, W. Lenth, and C. Ortiz, Appl. Phys. B 32, 145 (1983).
    [CrossRef]
  21. M. C. Fischer, H. C. Liu, I. R. Piletic, and W. S. Warren, Opt. Express 16, 4192 (2008).
    [CrossRef]

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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Figures (5)

Fig. 1.
Fig. 1.

(a) Detected FD signal of two-field pulse train. The inset shows the pulse train where the two identical fields (ref. and probe) are delayed by T1=3ps and the pump arrives after ref. to produce the temporal nonlinear dynamics. (b) Absolute value of the FT of (a). The phase at the peak (red circle) reveals the OKE dynamics. (c) Measured CS2 OKE dynamics along with the expected response. (d) Measured OKE dynamics of water and glass. The inset shows the experimental (circles) and expected (red line) difference after normalizing.

Fig. 2.
Fig. 2.

Theoretical [17] and experimental spectral-phase dynamics for CS2, water, and glass. The dashed black line indicates τ=0.

Fig. 3.
Fig. 3.

(a) Raw interferometric data at two pu-pr time delays (solid blue line and dotted black line). The red line is the difference between the two, which highlights the generated frequency when nonlinear phase changes occur. (b) FT of interferometric data as a function of pu-pr time delay.

Fig. 4.
Fig. 4.

(a) Water and glass (electronic response) OKE dynamics measured using the three-field pulse train. (b) Difference between water and electronic response after normalizing each.

Fig. 5.
Fig. 5.

(a) Image of a single layer of epidermal cells from an onion with molecular contrast based on OKE dynamics. The image uses a HSV color mode, where the hue encodes differences in the OKE dynamics. Pump power is 300 μW and pulse-train power is 10 μW. Acquisition time per time-delay is 60s. (b) OKE dynamics of two regions of interest: cell body (dashed green) and cell wall (red).

Equations (4)

Equations on this page are rendered with MathJax. Learn more.

Etrain(t)=Eref(t)+Epr(t)=E0(t)+E0(t+T1)·eiϕ(τ),
I(ω)=I[Etrain(t)·Etrain(t)*]=2|E0(ω)|2·[1+cos(ωT1+ϕ(τ))].
Etrain(t)=E0(t+T1)+E0(t)·ei·(π/2ϕ(τ))+E0(tT1)
I(ω)=|E0(ω)|2·(3+4ϕ(τ)·cos(ωT1)+2cos(2ωT1)),

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