Abstract

We report on a double L-scan technique for the simultaneous measurements of polarization-dependent nonlinear absorption. The high sensitivity of this method resides on the synchronized measurements of “twin” laser pulses to compensate for energy and mode fluctuations in the sample. This technique was successfully applied to the accurate determination of two-photon absorption (2PA) circular dichroism and 2PA circular-linear dichroism in a chiral solution. To our knowledge, this is the first time these nonlinear optical effects have been accurately measured. Our technique is expected to lead efforts in the study of biological systems and in the design of metamaterials with a negative refractive index.

© 2008 Optical Society of America

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  1. Y. Inoue and V. Ramamurthy, eds., Chiral Photochemistry (Marcel-Dekker, 2004).
    [CrossRef]
  2. J. B. Pendry, Science 306, 1353 (2004).
    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
  4. K. Nakanishi, N. Berova, and R. W. Woody, eds., Circular Dichroism: Principles and Applications (Wiley, 1994).
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    [CrossRef] [PubMed]
  6. M. A. Belkin, S. H. Han, X. Wei, and Y. R. Shen, Phys. Rev. Lett. 87, 113001 (2001).
    [CrossRef] [PubMed]
  7. N. Ji, V. Ostroverkhov, M. Belkin, Y. J. Shiu, and Y. R. Shen, J. Am. Chem. Soc. 128, 8845 (2006).
    [CrossRef] [PubMed]
  8. J. M. Hicks and T. Petralli-Mallow, Appl. Phys. B 68, 589 (1999).
    [CrossRef]
  9. I. Tinoco, J. Chem. Phys. 62, 1006 (1975).
    [CrossRef]
  10. E. A. Power, J. Chem. Phys. 63, 1348 (1975).
    [CrossRef]
  11. H. Mesnil, M. C. Schanne-Klein, F. Hache, M. Alexandre, G. Lemercier, and C. Andraud, Chem. Phys. Lett. 338, 269 (2001).
    [CrossRef]
  12. D. Wanapun, R. D. Wampler, N. J. Begue, and G. J. Simpson, Chem. Phys. Lett. 455, 6 (2008).
    [CrossRef]
  13. P. Fischer and F. Hache, Chirality 17, 421 (2005).
    [CrossRef] [PubMed]
  14. B. Jansik, A. Rizzo, and H. Agren, J. Phys. Chem. B 111, 446 (2007).
    [CrossRef] [PubMed]
  15. B. Jansík, A. Rizzo, H. Ågren, and B. Champagne, J. Chem. Theory Comput. 4, 457 (2008).
    [CrossRef]
  16. N. Engheta and P. G. Zablocky, Electron. Lett. 26, 2132 (1990).
    [CrossRef]
  17. P. P. Markowicz, M. Samoc, J. Cerne, P. N. Prasad, A. Pucci, and G. Ruggeri, Opt. Express 12, 5209 (2004).
    [CrossRef] [PubMed]
  18. M. Sheik-Bahae, A. Said, T. Wei, D. Hagan, and E. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
    [CrossRef]
  19. M. Samoc, A. Samoc, A. Miniewicz, P. P. Markowicz, P. N. Prasad, and J. G. Grote, Proc. SPIE 6646, 66460A1 (2007).
  20. L. Antonov, K. Kamada, K. Ohta, and F. S. Kamounah, Phys. Chem. Chem. Phys. 5, 1193 (2003).
    [CrossRef]
  21. M. A. Kriech and J. C. Conboy, Appl. Spectrosc. 59, 746 (2005).
    [CrossRef] [PubMed]

2008

D. Wanapun, R. D. Wampler, N. J. Begue, and G. J. Simpson, Chem. Phys. Lett. 455, 6 (2008).
[CrossRef]

B. Jansík, A. Rizzo, H. Ågren, and B. Champagne, J. Chem. Theory Comput. 4, 457 (2008).
[CrossRef]

2007

B. Jansik, A. Rizzo, and H. Agren, J. Phys. Chem. B 111, 446 (2007).
[CrossRef] [PubMed]

M. Samoc, A. Samoc, A. Miniewicz, P. P. Markowicz, P. N. Prasad, and J. G. Grote, Proc. SPIE 6646, 66460A1 (2007).

2006

R. Hassey, E. J. Swain, N. I. Hammer, D. Venkataraman, and M. D. Barnes, Science 314, 1437 (2006).
[CrossRef] [PubMed]

N. Ji, V. Ostroverkhov, M. Belkin, Y. J. Shiu, and Y. R. Shen, J. Am. Chem. Soc. 128, 8845 (2006).
[CrossRef] [PubMed]

2005

C. Monzon and D. W. Forester, Phys. Rev. Lett. 95, 123904 (2005).
[CrossRef] [PubMed]

P. Fischer and F. Hache, Chirality 17, 421 (2005).
[CrossRef] [PubMed]

M. A. Kriech and J. C. Conboy, Appl. Spectrosc. 59, 746 (2005).
[CrossRef] [PubMed]

2004

2003

L. Antonov, K. Kamada, K. Ohta, and F. S. Kamounah, Phys. Chem. Chem. Phys. 5, 1193 (2003).
[CrossRef]

2001

M. A. Belkin, S. H. Han, X. Wei, and Y. R. Shen, Phys. Rev. Lett. 87, 113001 (2001).
[CrossRef] [PubMed]

H. Mesnil, M. C. Schanne-Klein, F. Hache, M. Alexandre, G. Lemercier, and C. Andraud, Chem. Phys. Lett. 338, 269 (2001).
[CrossRef]

1999

J. M. Hicks and T. Petralli-Mallow, Appl. Phys. B 68, 589 (1999).
[CrossRef]

1990

M. Sheik-Bahae, A. Said, T. Wei, D. Hagan, and E. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

N. Engheta and P. G. Zablocky, Electron. Lett. 26, 2132 (1990).
[CrossRef]

1975

I. Tinoco, J. Chem. Phys. 62, 1006 (1975).
[CrossRef]

E. A. Power, J. Chem. Phys. 63, 1348 (1975).
[CrossRef]

Agren, H.

B. Jansik, A. Rizzo, and H. Agren, J. Phys. Chem. B 111, 446 (2007).
[CrossRef] [PubMed]

Ågren, H.

B. Jansík, A. Rizzo, H. Ågren, and B. Champagne, J. Chem. Theory Comput. 4, 457 (2008).
[CrossRef]

Alexandre, M.

H. Mesnil, M. C. Schanne-Klein, F. Hache, M. Alexandre, G. Lemercier, and C. Andraud, Chem. Phys. Lett. 338, 269 (2001).
[CrossRef]

Andraud, C.

H. Mesnil, M. C. Schanne-Klein, F. Hache, M. Alexandre, G. Lemercier, and C. Andraud, Chem. Phys. Lett. 338, 269 (2001).
[CrossRef]

Antonov, L.

L. Antonov, K. Kamada, K. Ohta, and F. S. Kamounah, Phys. Chem. Chem. Phys. 5, 1193 (2003).
[CrossRef]

Barnes, M. D.

R. Hassey, E. J. Swain, N. I. Hammer, D. Venkataraman, and M. D. Barnes, Science 314, 1437 (2006).
[CrossRef] [PubMed]

Begue, N. J.

D. Wanapun, R. D. Wampler, N. J. Begue, and G. J. Simpson, Chem. Phys. Lett. 455, 6 (2008).
[CrossRef]

Belkin, M.

N. Ji, V. Ostroverkhov, M. Belkin, Y. J. Shiu, and Y. R. Shen, J. Am. Chem. Soc. 128, 8845 (2006).
[CrossRef] [PubMed]

Belkin, M. A.

M. A. Belkin, S. H. Han, X. Wei, and Y. R. Shen, Phys. Rev. Lett. 87, 113001 (2001).
[CrossRef] [PubMed]

Berova, N.

K. Nakanishi, N. Berova, and R. W. Woody, eds., Circular Dichroism: Principles and Applications (Wiley, 1994).

Cerne, J.

Champagne, B.

B. Jansík, A. Rizzo, H. Ågren, and B. Champagne, J. Chem. Theory Comput. 4, 457 (2008).
[CrossRef]

Conboy, J. C.

Engheta, N.

N. Engheta and P. G. Zablocky, Electron. Lett. 26, 2132 (1990).
[CrossRef]

Fischer, P.

P. Fischer and F. Hache, Chirality 17, 421 (2005).
[CrossRef] [PubMed]

Forester, D. W.

C. Monzon and D. W. Forester, Phys. Rev. Lett. 95, 123904 (2005).
[CrossRef] [PubMed]

Grote, J. G.

M. Samoc, A. Samoc, A. Miniewicz, P. P. Markowicz, P. N. Prasad, and J. G. Grote, Proc. SPIE 6646, 66460A1 (2007).

Hache, F.

P. Fischer and F. Hache, Chirality 17, 421 (2005).
[CrossRef] [PubMed]

H. Mesnil, M. C. Schanne-Klein, F. Hache, M. Alexandre, G. Lemercier, and C. Andraud, Chem. Phys. Lett. 338, 269 (2001).
[CrossRef]

Hagan, D.

M. Sheik-Bahae, A. Said, T. Wei, D. Hagan, and E. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

Hammer, N. I.

R. Hassey, E. J. Swain, N. I. Hammer, D. Venkataraman, and M. D. Barnes, Science 314, 1437 (2006).
[CrossRef] [PubMed]

Han, S. H.

M. A. Belkin, S. H. Han, X. Wei, and Y. R. Shen, Phys. Rev. Lett. 87, 113001 (2001).
[CrossRef] [PubMed]

Hassey, R.

R. Hassey, E. J. Swain, N. I. Hammer, D. Venkataraman, and M. D. Barnes, Science 314, 1437 (2006).
[CrossRef] [PubMed]

Hicks, J. M.

J. M. Hicks and T. Petralli-Mallow, Appl. Phys. B 68, 589 (1999).
[CrossRef]

Inoue, Y.

Y. Inoue and V. Ramamurthy, eds., Chiral Photochemistry (Marcel-Dekker, 2004).
[CrossRef]

Jansik, B.

B. Jansik, A. Rizzo, and H. Agren, J. Phys. Chem. B 111, 446 (2007).
[CrossRef] [PubMed]

Jansík, B.

B. Jansík, A. Rizzo, H. Ågren, and B. Champagne, J. Chem. Theory Comput. 4, 457 (2008).
[CrossRef]

Ji, N.

N. Ji, V. Ostroverkhov, M. Belkin, Y. J. Shiu, and Y. R. Shen, J. Am. Chem. Soc. 128, 8845 (2006).
[CrossRef] [PubMed]

Kamada, K.

L. Antonov, K. Kamada, K. Ohta, and F. S. Kamounah, Phys. Chem. Chem. Phys. 5, 1193 (2003).
[CrossRef]

Kamounah, F. S.

L. Antonov, K. Kamada, K. Ohta, and F. S. Kamounah, Phys. Chem. Chem. Phys. 5, 1193 (2003).
[CrossRef]

Kriech, M. A.

Lemercier, G.

H. Mesnil, M. C. Schanne-Klein, F. Hache, M. Alexandre, G. Lemercier, and C. Andraud, Chem. Phys. Lett. 338, 269 (2001).
[CrossRef]

Markowicz, P. P.

M. Samoc, A. Samoc, A. Miniewicz, P. P. Markowicz, P. N. Prasad, and J. G. Grote, Proc. SPIE 6646, 66460A1 (2007).

P. P. Markowicz, M. Samoc, J. Cerne, P. N. Prasad, A. Pucci, and G. Ruggeri, Opt. Express 12, 5209 (2004).
[CrossRef] [PubMed]

Mesnil, H.

H. Mesnil, M. C. Schanne-Klein, F. Hache, M. Alexandre, G. Lemercier, and C. Andraud, Chem. Phys. Lett. 338, 269 (2001).
[CrossRef]

Miniewicz, A.

M. Samoc, A. Samoc, A. Miniewicz, P. P. Markowicz, P. N. Prasad, and J. G. Grote, Proc. SPIE 6646, 66460A1 (2007).

Monzon, C.

C. Monzon and D. W. Forester, Phys. Rev. Lett. 95, 123904 (2005).
[CrossRef] [PubMed]

Nakanishi, K.

K. Nakanishi, N. Berova, and R. W. Woody, eds., Circular Dichroism: Principles and Applications (Wiley, 1994).

Ohta, K.

L. Antonov, K. Kamada, K. Ohta, and F. S. Kamounah, Phys. Chem. Chem. Phys. 5, 1193 (2003).
[CrossRef]

Ostroverkhov, V.

N. Ji, V. Ostroverkhov, M. Belkin, Y. J. Shiu, and Y. R. Shen, J. Am. Chem. Soc. 128, 8845 (2006).
[CrossRef] [PubMed]

Pendry, J. B.

J. B. Pendry, Science 306, 1353 (2004).
[CrossRef] [PubMed]

Petralli-Mallow, T.

J. M. Hicks and T. Petralli-Mallow, Appl. Phys. B 68, 589 (1999).
[CrossRef]

Power, E. A.

E. A. Power, J. Chem. Phys. 63, 1348 (1975).
[CrossRef]

Prasad, P. N.

M. Samoc, A. Samoc, A. Miniewicz, P. P. Markowicz, P. N. Prasad, and J. G. Grote, Proc. SPIE 6646, 66460A1 (2007).

P. P. Markowicz, M. Samoc, J. Cerne, P. N. Prasad, A. Pucci, and G. Ruggeri, Opt. Express 12, 5209 (2004).
[CrossRef] [PubMed]

Pucci, A.

Ramamurthy, V.

Y. Inoue and V. Ramamurthy, eds., Chiral Photochemistry (Marcel-Dekker, 2004).
[CrossRef]

Rizzo, A.

B. Jansík, A. Rizzo, H. Ågren, and B. Champagne, J. Chem. Theory Comput. 4, 457 (2008).
[CrossRef]

B. Jansik, A. Rizzo, and H. Agren, J. Phys. Chem. B 111, 446 (2007).
[CrossRef] [PubMed]

Ruggeri, G.

Said, A.

M. Sheik-Bahae, A. Said, T. Wei, D. Hagan, and E. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

Samoc, A.

M. Samoc, A. Samoc, A. Miniewicz, P. P. Markowicz, P. N. Prasad, and J. G. Grote, Proc. SPIE 6646, 66460A1 (2007).

Samoc, M.

M. Samoc, A. Samoc, A. Miniewicz, P. P. Markowicz, P. N. Prasad, and J. G. Grote, Proc. SPIE 6646, 66460A1 (2007).

P. P. Markowicz, M. Samoc, J. Cerne, P. N. Prasad, A. Pucci, and G. Ruggeri, Opt. Express 12, 5209 (2004).
[CrossRef] [PubMed]

Schanne-Klein, M. C.

H. Mesnil, M. C. Schanne-Klein, F. Hache, M. Alexandre, G. Lemercier, and C. Andraud, Chem. Phys. Lett. 338, 269 (2001).
[CrossRef]

Sheik-Bahae, M.

M. Sheik-Bahae, A. Said, T. Wei, D. Hagan, and E. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

Shen, Y. R.

N. Ji, V. Ostroverkhov, M. Belkin, Y. J. Shiu, and Y. R. Shen, J. Am. Chem. Soc. 128, 8845 (2006).
[CrossRef] [PubMed]

M. A. Belkin, S. H. Han, X. Wei, and Y. R. Shen, Phys. Rev. Lett. 87, 113001 (2001).
[CrossRef] [PubMed]

Shiu, Y. J.

N. Ji, V. Ostroverkhov, M. Belkin, Y. J. Shiu, and Y. R. Shen, J. Am. Chem. Soc. 128, 8845 (2006).
[CrossRef] [PubMed]

Simpson, G. J.

D. Wanapun, R. D. Wampler, N. J. Begue, and G. J. Simpson, Chem. Phys. Lett. 455, 6 (2008).
[CrossRef]

Swain, E. J.

R. Hassey, E. J. Swain, N. I. Hammer, D. Venkataraman, and M. D. Barnes, Science 314, 1437 (2006).
[CrossRef] [PubMed]

Tinoco, I.

I. Tinoco, J. Chem. Phys. 62, 1006 (1975).
[CrossRef]

Van Stryland, E.

M. Sheik-Bahae, A. Said, T. Wei, D. Hagan, and E. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

Venkataraman, D.

R. Hassey, E. J. Swain, N. I. Hammer, D. Venkataraman, and M. D. Barnes, Science 314, 1437 (2006).
[CrossRef] [PubMed]

Wampler, R. D.

D. Wanapun, R. D. Wampler, N. J. Begue, and G. J. Simpson, Chem. Phys. Lett. 455, 6 (2008).
[CrossRef]

Wanapun, D.

D. Wanapun, R. D. Wampler, N. J. Begue, and G. J. Simpson, Chem. Phys. Lett. 455, 6 (2008).
[CrossRef]

Wei, T.

M. Sheik-Bahae, A. Said, T. Wei, D. Hagan, and E. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

Wei, X.

M. A. Belkin, S. H. Han, X. Wei, and Y. R. Shen, Phys. Rev. Lett. 87, 113001 (2001).
[CrossRef] [PubMed]

Woody, R. W.

K. Nakanishi, N. Berova, and R. W. Woody, eds., Circular Dichroism: Principles and Applications (Wiley, 1994).

Zablocky, P. G.

N. Engheta and P. G. Zablocky, Electron. Lett. 26, 2132 (1990).
[CrossRef]

Appl. Phys. B

J. M. Hicks and T. Petralli-Mallow, Appl. Phys. B 68, 589 (1999).
[CrossRef]

Appl. Spectrosc.

Chem. Phys. Lett.

H. Mesnil, M. C. Schanne-Klein, F. Hache, M. Alexandre, G. Lemercier, and C. Andraud, Chem. Phys. Lett. 338, 269 (2001).
[CrossRef]

D. Wanapun, R. D. Wampler, N. J. Begue, and G. J. Simpson, Chem. Phys. Lett. 455, 6 (2008).
[CrossRef]

Chirality

P. Fischer and F. Hache, Chirality 17, 421 (2005).
[CrossRef] [PubMed]

Electron. Lett.

N. Engheta and P. G. Zablocky, Electron. Lett. 26, 2132 (1990).
[CrossRef]

IEEE J. Quantum Electron.

M. Sheik-Bahae, A. Said, T. Wei, D. Hagan, and E. Van Stryland, IEEE J. Quantum Electron. 26, 760 (1990).
[CrossRef]

J. Am. Chem. Soc.

N. Ji, V. Ostroverkhov, M. Belkin, Y. J. Shiu, and Y. R. Shen, J. Am. Chem. Soc. 128, 8845 (2006).
[CrossRef] [PubMed]

J. Chem. Phys.

I. Tinoco, J. Chem. Phys. 62, 1006 (1975).
[CrossRef]

E. A. Power, J. Chem. Phys. 63, 1348 (1975).
[CrossRef]

J. Chem. Theory Comput.

B. Jansík, A. Rizzo, H. Ågren, and B. Champagne, J. Chem. Theory Comput. 4, 457 (2008).
[CrossRef]

J. Phys. Chem. B

B. Jansik, A. Rizzo, and H. Agren, J. Phys. Chem. B 111, 446 (2007).
[CrossRef] [PubMed]

Opt. Express

Phys. Chem. Chem. Phys.

L. Antonov, K. Kamada, K. Ohta, and F. S. Kamounah, Phys. Chem. Chem. Phys. 5, 1193 (2003).
[CrossRef]

Phys. Rev. Lett.

M. A. Belkin, S. H. Han, X. Wei, and Y. R. Shen, Phys. Rev. Lett. 87, 113001 (2001).
[CrossRef] [PubMed]

C. Monzon and D. W. Forester, Phys. Rev. Lett. 95, 123904 (2005).
[CrossRef] [PubMed]

Proc. SPIE

M. Samoc, A. Samoc, A. Miniewicz, P. P. Markowicz, P. N. Prasad, and J. G. Grote, Proc. SPIE 6646, 66460A1 (2007).

Science

J. B. Pendry, Science 306, 1353 (2004).
[CrossRef] [PubMed]

R. Hassey, E. J. Swain, N. I. Hammer, D. Venkataraman, and M. D. Barnes, Science 314, 1437 (2006).
[CrossRef] [PubMed]

Other

Y. Inoue and V. Ramamurthy, eds., Chiral Photochemistry (Marcel-Dekker, 2004).
[CrossRef]

K. Nakanishi, N. Berova, and R. W. Woody, eds., Circular Dichroism: Principles and Applications (Wiley, 1994).

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Figures (3)

Fig. 1
Fig. 1

Double L-scan geometry. Mirrors (M1, M2, M3); wave plates (WP1, WP2, WP3); Glan polarizer (P); beam splitters (BS1, BS2); convergent lenses (L1, L2, L3, L4, L5); silicon detectors (D1, D2, D3); neutral density filters (DF1, DF2, DF3); translation stages (TS1, TS2); step-motors (SM1, SM2); synchronization box (SB); sample (S), and control box (CB).

Fig. 2
Fig. 2

L-scan signatures and difference between normalized transmittance versus z position using different polarization state combinations pumping at 460 nm . (a) Linear–linear, (b) linear–circular (right), (c) linear–circular (left), and (d) circular–circular (left-right).

Fig. 3
Fig. 3

(a) Linear absorption spectrum of SBN/THF, 2PA cross section spectrum for linearly (LP) and circularly [right (RCP) and left (LCP)] polarized light and molecular structure (inset), (b) 2PA-CD spectrum, and (c) 2PA-CLD using right and left circularly polarized radiation.

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