Abstract

We have experimentally demonstrated coherent anti-Stokes Raman scattering in both forward and backward directions from thin samples of dipicolinic acid crystalline. The signal observed in the backscattered, phased-mismatched direction is 3 orders of magnitude stronger than would be expected without scattering from the crystal’s inhomogeneities. We present a theoretical explanation of these results, based on the theory of random diffraction gratings and discuss possible applications.

© 2005 Optical Society of America

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    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
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    [CrossRef]
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    [CrossRef]
  24. J. C. Vaughan, T. Hornung, T. Feurer, and K. A. Nelson, "Diffraction-based femtosecond pulse shaping with a two-dimensional spatial light modulator," Opt. Lett. 30, 323-325 (2005).
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    [CrossRef] [PubMed]
  26. Erwin Schanda, Physical Fundamentals of Remote Sensing (Springer-Verlag, 1986).
    [CrossRef]

2005 (2)

J. C. Vaughan, T. Hornung, T. Feurer, and K. A. Nelson, "Diffraction-based femtosecond pulse shaping with a two-dimensional spatial light modulator," Opt. Lett. 30, 323-325 (2005).
[CrossRef] [PubMed]

V. Kocharovsky, S. Cameron, K. Lehmann, R. Lucht, R. Miles, Y. Rostovtsev, W. Warren, G. R. Welch, and M. O. Scully, "Gain-swept superradiance applied to the stand-off detection of trace impurities in the atmosphere," Proc. Natl. Acad. Sci. U.S.A. 102, 7806-7811 (2005).
[CrossRef] [PubMed]

2004 (1)

V. A. Sautenkov, C. Y. Ye, Y. V. Rostovtsev, G. R. Welch, andM. O. Scully, "Enhancement of field generation via maximal atomic coherence prepared by fast adiabatic passage in Rb vapor," Phys. Rev. A 70, 033406 (2004).
[CrossRef]

2002 (3)

M. O. Scully, G. W. Kattawar, P. R. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," Proc. Natl. Acad. Sci. U.S.A. 99, 10994-11001 (2002).
[CrossRef] [PubMed]

A. V. Turukhin, V. S. Sudarshanam, M. S. Shahriar, J. A. Musser, B. S. Ham, and P. R. Hemmer, "Observation of ultraslow and stored light pulses in a solid," Phys. Rev. Lett. 88, 023602 (2002).
[CrossRef] [PubMed]

A. S. Zibrov, A. B. Matsko, O. Kocharovskaya, Y. V. Rostovtsev, G. R. Welch, and M. O. Scully, "Transporting and time reversing light via atomic coherence," Phys. Rev. Lett. 88, 103601 (2002).
[CrossRef] [PubMed]

2001 (4)

A. B. Matsko, O. Kocharovskaya, Y. Rostovtsev, G. R. Welch, A. S. Zibrov, and M. O. Scully, "Slow, ultraslow, stored, and frozen light," Adv. At., Mol. Opt. Phys. 46, 191-242 (2001).
[CrossRef]

C. Liu, Z. Dutton, C. H. Behroozi, and L. V. Hau, "Observation of coherent optical information storage in an atomic medium using halted light pulses," Nature 409, 490-493 (2001).
[CrossRef] [PubMed]

D. F. Phillips, A. Fleischhauer, A. Mair, R. L. Walsworth, and M. D. Lukin, "Storage of light in atomic vapor," Phys. Rev. Lett. 86, 783-786 (2001).
[CrossRef] [PubMed]

H. Wang, D. Goorskey, and M. Xiao, "Enhanced Kerr nonlinearity via atomic coherence in a three-level atomic system," Phys. Rev. Lett. 87, 073601 (2001).
[CrossRef] [PubMed]

2000 (1)

A. J. Merriam, S. J. Sharpe, M. Shverdin, D. Manuszak, G. Y. Yin, and S. E. Harris, "Efficient nonlinear frequency conversion in an all-resonant double-lambda system," Phys. Rev. Lett. 84, 5308-5311 (2000).
[CrossRef] [PubMed]

1998 (1)

S. E. Harris and A. V. Sokolov, "Subfemtosecond pulse generation by molecular modulation," Phys. Rev. Lett. 81, 2894-2897 (1998).
[CrossRef]

1997 (1)

S. E. Harris, G. Y. Yin, M. Jain, and A. J. Merriam, "Nonlinear optics at maximum coherence," Philos. Trans. R. Soc. London, Ser. A 355, 2291-2304 (1997).
[CrossRef]

1996 (1)

M. Jain, H. Xia, G. Y. Yin, A. J. Merriam, and S. E. Harris, "Efficient nonlinear frequency conversion with maximal atomic coherence," Phys. Rev. Lett. 77, 4326-4329 (1996).
[CrossRef] [PubMed]

1992 (2)

K. Hakuta, L. Marmet, and B. P. Stoicheff, "Nonlinear optical-generation with reduced absorption using electric-field coupling in atomic hydrogen," Phys. Rev. A 45, 5152-5159 (1992).
[CrossRef] [PubMed]

A. M. Weiner, D. E. Leaird, J. S. Patel, and J. R. Wullert, "Programmable shaping of femtosecond optical pulses by use of 128-element liquid-crystal phase modulator," IEEE J. Quantum Electron. 28, 908-920 (1992).
[CrossRef]

1990 (1)

Y. H. Rim, J. W. Haus, and J. Schroeder, "Forward and backward scattering of light in inhomegeneous-media," Phys. Rev. A 42, 2385-2400 (1990).
[CrossRef] [PubMed]

1980 (1)

P. Carmona, "Vibrational-spectra and structure of crystalline dipicolinic acid and calcium dipicolinic trihydrate," Spectrochim. Acta, Part A 36A, 705-712 (1980).
[CrossRef]

1975 (1)

R. Bonifacio, F. A. Hopf, P. Meystre, and M. O. Scully, "Steady-state pulses and superradiance in short-wavelength, swept-gain amplifiers," Phys. Rev. A 12, 2568-2573 (1975).
[CrossRef]

Behroozi, C. H.

C. Liu, Z. Dutton, C. H. Behroozi, and L. V. Hau, "Observation of coherent optical information storage in an atomic medium using halted light pulses," Nature 409, 490-493 (2001).
[CrossRef] [PubMed]

Bonifacio, R.

R. Bonifacio, F. A. Hopf, P. Meystre, and M. O. Scully, "Steady-state pulses and superradiance in short-wavelength, swept-gain amplifiers," Phys. Rev. A 12, 2568-2573 (1975).
[CrossRef]

Boyd, R. W.

R. W. Boyd, Nonlinear Optics (Academic, 1992).

Cameron, S.

V. Kocharovsky, S. Cameron, K. Lehmann, R. Lucht, R. Miles, Y. Rostovtsev, W. Warren, G. R. Welch, and M. O. Scully, "Gain-swept superradiance applied to the stand-off detection of trace impurities in the atmosphere," Proc. Natl. Acad. Sci. U.S.A. 102, 7806-7811 (2005).
[CrossRef] [PubMed]

Carmona, P.

P. Carmona, "Vibrational-spectra and structure of crystalline dipicolinic acid and calcium dipicolinic trihydrate," Spectrochim. Acta, Part A 36A, 705-712 (1980).
[CrossRef]

Dutton, Z.

C. Liu, Z. Dutton, C. H. Behroozi, and L. V. Hau, "Observation of coherent optical information storage in an atomic medium using halted light pulses," Nature 409, 490-493 (2001).
[CrossRef] [PubMed]

Eesley, G. L.

G. L. Eesley, CARS Spectroscopy (Pergamon, 1981).

Feurer, T.

Fleischhauer, A.

D. F. Phillips, A. Fleischhauer, A. Mair, R. L. Walsworth, and M. D. Lukin, "Storage of light in atomic vapor," Phys. Rev. Lett. 86, 783-786 (2001).
[CrossRef] [PubMed]

Goorskey, D.

H. Wang, D. Goorskey, and M. Xiao, "Enhanced Kerr nonlinearity via atomic coherence in a three-level atomic system," Phys. Rev. Lett. 87, 073601 (2001).
[CrossRef] [PubMed]

Hakuta, K.

K. Hakuta, L. Marmet, and B. P. Stoicheff, "Nonlinear optical-generation with reduced absorption using electric-field coupling in atomic hydrogen," Phys. Rev. A 45, 5152-5159 (1992).
[CrossRef] [PubMed]

Ham, B. S.

A. V. Turukhin, V. S. Sudarshanam, M. S. Shahriar, J. A. Musser, B. S. Ham, and P. R. Hemmer, "Observation of ultraslow and stored light pulses in a solid," Phys. Rev. Lett. 88, 023602 (2002).
[CrossRef] [PubMed]

Harris, S. E.

A. J. Merriam, S. J. Sharpe, M. Shverdin, D. Manuszak, G. Y. Yin, and S. E. Harris, "Efficient nonlinear frequency conversion in an all-resonant double-lambda system," Phys. Rev. Lett. 84, 5308-5311 (2000).
[CrossRef] [PubMed]

S. E. Harris and A. V. Sokolov, "Subfemtosecond pulse generation by molecular modulation," Phys. Rev. Lett. 81, 2894-2897 (1998).
[CrossRef]

S. E. Harris, G. Y. Yin, M. Jain, and A. J. Merriam, "Nonlinear optics at maximum coherence," Philos. Trans. R. Soc. London, Ser. A 355, 2291-2304 (1997).
[CrossRef]

M. Jain, H. Xia, G. Y. Yin, A. J. Merriam, and S. E. Harris, "Efficient nonlinear frequency conversion with maximal atomic coherence," Phys. Rev. Lett. 77, 4326-4329 (1996).
[CrossRef] [PubMed]

Hau, L. V.

C. Liu, Z. Dutton, C. H. Behroozi, and L. V. Hau, "Observation of coherent optical information storage in an atomic medium using halted light pulses," Nature 409, 490-493 (2001).
[CrossRef] [PubMed]

Haus, J. W.

Y. H. Rim, J. W. Haus, and J. Schroeder, "Forward and backward scattering of light in inhomegeneous-media," Phys. Rev. A 42, 2385-2400 (1990).
[CrossRef] [PubMed]

Hemmer, P. R.

A. V. Turukhin, V. S. Sudarshanam, M. S. Shahriar, J. A. Musser, B. S. Ham, and P. R. Hemmer, "Observation of ultraslow and stored light pulses in a solid," Phys. Rev. Lett. 88, 023602 (2002).
[CrossRef] [PubMed]

Hopf, F. A.

R. Bonifacio, F. A. Hopf, P. Meystre, and M. O. Scully, "Steady-state pulses and superradiance in short-wavelength, swept-gain amplifiers," Phys. Rev. A 12, 2568-2573 (1975).
[CrossRef]

Hornung, T.

Jain, M.

S. E. Harris, G. Y. Yin, M. Jain, and A. J. Merriam, "Nonlinear optics at maximum coherence," Philos. Trans. R. Soc. London, Ser. A 355, 2291-2304 (1997).
[CrossRef]

M. Jain, H. Xia, G. Y. Yin, A. J. Merriam, and S. E. Harris, "Efficient nonlinear frequency conversion with maximal atomic coherence," Phys. Rev. Lett. 77, 4326-4329 (1996).
[CrossRef] [PubMed]

Kano, S. S.

M. D. Levenson and S. S. Kano, Introduction of Nonlinear Spectroscopy (Academic, 1988).

Kattawar, G. W.

M. O. Scully, G. W. Kattawar, P. R. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," Proc. Natl. Acad. Sci. U.S.A. 99, 10994-11001 (2002).
[CrossRef] [PubMed]

Kocharovskaya, O.

A. S. Zibrov, A. B. Matsko, O. Kocharovskaya, Y. V. Rostovtsev, G. R. Welch, and M. O. Scully, "Transporting and time reversing light via atomic coherence," Phys. Rev. Lett. 88, 103601 (2002).
[CrossRef] [PubMed]

A. B. Matsko, O. Kocharovskaya, Y. Rostovtsev, G. R. Welch, A. S. Zibrov, and M. O. Scully, "Slow, ultraslow, stored, and frozen light," Adv. At., Mol. Opt. Phys. 46, 191-242 (2001).
[CrossRef]

Kocharovsky, V.

V. Kocharovsky, S. Cameron, K. Lehmann, R. Lucht, R. Miles, Y. Rostovtsev, W. Warren, G. R. Welch, and M. O. Scully, "Gain-swept superradiance applied to the stand-off detection of trace impurities in the atmosphere," Proc. Natl. Acad. Sci. U.S.A. 102, 7806-7811 (2005).
[CrossRef] [PubMed]

Leaird, D. E.

A. M. Weiner, D. E. Leaird, J. S. Patel, and J. R. Wullert, "Programmable shaping of femtosecond optical pulses by use of 128-element liquid-crystal phase modulator," IEEE J. Quantum Electron. 28, 908-920 (1992).
[CrossRef]

Lehmann, K.

V. Kocharovsky, S. Cameron, K. Lehmann, R. Lucht, R. Miles, Y. Rostovtsev, W. Warren, G. R. Welch, and M. O. Scully, "Gain-swept superradiance applied to the stand-off detection of trace impurities in the atmosphere," Proc. Natl. Acad. Sci. U.S.A. 102, 7806-7811 (2005).
[CrossRef] [PubMed]

Levenson, M. D.

M. D. Levenson and S. S. Kano, Introduction of Nonlinear Spectroscopy (Academic, 1988).

Liu, C.

C. Liu, Z. Dutton, C. H. Behroozi, and L. V. Hau, "Observation of coherent optical information storage in an atomic medium using halted light pulses," Nature 409, 490-493 (2001).
[CrossRef] [PubMed]

Lucht, P. R.

M. O. Scully, G. W. Kattawar, P. R. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," Proc. Natl. Acad. Sci. U.S.A. 99, 10994-11001 (2002).
[CrossRef] [PubMed]

Lucht, R.

V. Kocharovsky, S. Cameron, K. Lehmann, R. Lucht, R. Miles, Y. Rostovtsev, W. Warren, G. R. Welch, and M. O. Scully, "Gain-swept superradiance applied to the stand-off detection of trace impurities in the atmosphere," Proc. Natl. Acad. Sci. U.S.A. 102, 7806-7811 (2005).
[CrossRef] [PubMed]

Lukin, M. D.

D. F. Phillips, A. Fleischhauer, A. Mair, R. L. Walsworth, and M. D. Lukin, "Storage of light in atomic vapor," Phys. Rev. Lett. 86, 783-786 (2001).
[CrossRef] [PubMed]

Mair, A.

D. F. Phillips, A. Fleischhauer, A. Mair, R. L. Walsworth, and M. D. Lukin, "Storage of light in atomic vapor," Phys. Rev. Lett. 86, 783-786 (2001).
[CrossRef] [PubMed]

Manuszak, D.

A. J. Merriam, S. J. Sharpe, M. Shverdin, D. Manuszak, G. Y. Yin, and S. E. Harris, "Efficient nonlinear frequency conversion in an all-resonant double-lambda system," Phys. Rev. Lett. 84, 5308-5311 (2000).
[CrossRef] [PubMed]

Marmet, L.

K. Hakuta, L. Marmet, and B. P. Stoicheff, "Nonlinear optical-generation with reduced absorption using electric-field coupling in atomic hydrogen," Phys. Rev. A 45, 5152-5159 (1992).
[CrossRef] [PubMed]

Matsko, A. B.

A. S. Zibrov, A. B. Matsko, O. Kocharovskaya, Y. V. Rostovtsev, G. R. Welch, and M. O. Scully, "Transporting and time reversing light via atomic coherence," Phys. Rev. Lett. 88, 103601 (2002).
[CrossRef] [PubMed]

A. B. Matsko, O. Kocharovskaya, Y. Rostovtsev, G. R. Welch, A. S. Zibrov, and M. O. Scully, "Slow, ultraslow, stored, and frozen light," Adv. At., Mol. Opt. Phys. 46, 191-242 (2001).
[CrossRef]

Merriam, A. J.

A. J. Merriam, S. J. Sharpe, M. Shverdin, D. Manuszak, G. Y. Yin, and S. E. Harris, "Efficient nonlinear frequency conversion in an all-resonant double-lambda system," Phys. Rev. Lett. 84, 5308-5311 (2000).
[CrossRef] [PubMed]

S. E. Harris, G. Y. Yin, M. Jain, and A. J. Merriam, "Nonlinear optics at maximum coherence," Philos. Trans. R. Soc. London, Ser. A 355, 2291-2304 (1997).
[CrossRef]

M. Jain, H. Xia, G. Y. Yin, A. J. Merriam, and S. E. Harris, "Efficient nonlinear frequency conversion with maximal atomic coherence," Phys. Rev. Lett. 77, 4326-4329 (1996).
[CrossRef] [PubMed]

Meystre, P.

R. Bonifacio, F. A. Hopf, P. Meystre, and M. O. Scully, "Steady-state pulses and superradiance in short-wavelength, swept-gain amplifiers," Phys. Rev. A 12, 2568-2573 (1975).
[CrossRef]

Miles, R.

V. Kocharovsky, S. Cameron, K. Lehmann, R. Lucht, R. Miles, Y. Rostovtsev, W. Warren, G. R. Welch, and M. O. Scully, "Gain-swept superradiance applied to the stand-off detection of trace impurities in the atmosphere," Proc. Natl. Acad. Sci. U.S.A. 102, 7806-7811 (2005).
[CrossRef] [PubMed]

Musser, J. A.

A. V. Turukhin, V. S. Sudarshanam, M. S. Shahriar, J. A. Musser, B. S. Ham, and P. R. Hemmer, "Observation of ultraslow and stored light pulses in a solid," Phys. Rev. Lett. 88, 023602 (2002).
[CrossRef] [PubMed]

Nelson, K. A.

Opatrny, T.

M. O. Scully, G. W. Kattawar, P. R. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," Proc. Natl. Acad. Sci. U.S.A. 99, 10994-11001 (2002).
[CrossRef] [PubMed]

Patel, J. S.

A. M. Weiner, D. E. Leaird, J. S. Patel, and J. R. Wullert, "Programmable shaping of femtosecond optical pulses by use of 128-element liquid-crystal phase modulator," IEEE J. Quantum Electron. 28, 908-920 (1992).
[CrossRef]

Phillips, D. F.

D. F. Phillips, A. Fleischhauer, A. Mair, R. L. Walsworth, and M. D. Lukin, "Storage of light in atomic vapor," Phys. Rev. Lett. 86, 783-786 (2001).
[CrossRef] [PubMed]

Pilloff, H.

M. O. Scully, G. W. Kattawar, P. R. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," Proc. Natl. Acad. Sci. U.S.A. 99, 10994-11001 (2002).
[CrossRef] [PubMed]

Rebane, A.

M. O. Scully, G. W. Kattawar, P. R. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," Proc. Natl. Acad. Sci. U.S.A. 99, 10994-11001 (2002).
[CrossRef] [PubMed]

Rim, Y. H.

Y. H. Rim, J. W. Haus, and J. Schroeder, "Forward and backward scattering of light in inhomegeneous-media," Phys. Rev. A 42, 2385-2400 (1990).
[CrossRef] [PubMed]

Rostovtsev, Y.

V. Kocharovsky, S. Cameron, K. Lehmann, R. Lucht, R. Miles, Y. Rostovtsev, W. Warren, G. R. Welch, and M. O. Scully, "Gain-swept superradiance applied to the stand-off detection of trace impurities in the atmosphere," Proc. Natl. Acad. Sci. U.S.A. 102, 7806-7811 (2005).
[CrossRef] [PubMed]

A. B. Matsko, O. Kocharovskaya, Y. Rostovtsev, G. R. Welch, A. S. Zibrov, and M. O. Scully, "Slow, ultraslow, stored, and frozen light," Adv. At., Mol. Opt. Phys. 46, 191-242 (2001).
[CrossRef]

Rostovtsev, Y. V.

V. A. Sautenkov, C. Y. Ye, Y. V. Rostovtsev, G. R. Welch, andM. O. Scully, "Enhancement of field generation via maximal atomic coherence prepared by fast adiabatic passage in Rb vapor," Phys. Rev. A 70, 033406 (2004).
[CrossRef]

A. S. Zibrov, A. B. Matsko, O. Kocharovskaya, Y. V. Rostovtsev, G. R. Welch, and M. O. Scully, "Transporting and time reversing light via atomic coherence," Phys. Rev. Lett. 88, 103601 (2002).
[CrossRef] [PubMed]

Sautenkov, V. A.

V. A. Sautenkov, C. Y. Ye, Y. V. Rostovtsev, G. R. Welch, andM. O. Scully, "Enhancement of field generation via maximal atomic coherence prepared by fast adiabatic passage in Rb vapor," Phys. Rev. A 70, 033406 (2004).
[CrossRef]

Schanda, Erwin

Erwin Schanda, Physical Fundamentals of Remote Sensing (Springer-Verlag, 1986).
[CrossRef]

Schroeder, J.

Y. H. Rim, J. W. Haus, and J. Schroeder, "Forward and backward scattering of light in inhomegeneous-media," Phys. Rev. A 42, 2385-2400 (1990).
[CrossRef] [PubMed]

Scully, M. O.

V. Kocharovsky, S. Cameron, K. Lehmann, R. Lucht, R. Miles, Y. Rostovtsev, W. Warren, G. R. Welch, and M. O. Scully, "Gain-swept superradiance applied to the stand-off detection of trace impurities in the atmosphere," Proc. Natl. Acad. Sci. U.S.A. 102, 7806-7811 (2005).
[CrossRef] [PubMed]

V. A. Sautenkov, C. Y. Ye, Y. V. Rostovtsev, G. R. Welch, andM. O. Scully, "Enhancement of field generation via maximal atomic coherence prepared by fast adiabatic passage in Rb vapor," Phys. Rev. A 70, 033406 (2004).
[CrossRef]

M. O. Scully, G. W. Kattawar, P. R. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," Proc. Natl. Acad. Sci. U.S.A. 99, 10994-11001 (2002).
[CrossRef] [PubMed]

A. S. Zibrov, A. B. Matsko, O. Kocharovskaya, Y. V. Rostovtsev, G. R. Welch, and M. O. Scully, "Transporting and time reversing light via atomic coherence," Phys. Rev. Lett. 88, 103601 (2002).
[CrossRef] [PubMed]

A. B. Matsko, O. Kocharovskaya, Y. Rostovtsev, G. R. Welch, A. S. Zibrov, and M. O. Scully, "Slow, ultraslow, stored, and frozen light," Adv. At., Mol. Opt. Phys. 46, 191-242 (2001).
[CrossRef]

R. Bonifacio, F. A. Hopf, P. Meystre, and M. O. Scully, "Steady-state pulses and superradiance in short-wavelength, swept-gain amplifiers," Phys. Rev. A 12, 2568-2573 (1975).
[CrossRef]

Shahriar, M. S.

A. V. Turukhin, V. S. Sudarshanam, M. S. Shahriar, J. A. Musser, B. S. Ham, and P. R. Hemmer, "Observation of ultraslow and stored light pulses in a solid," Phys. Rev. Lett. 88, 023602 (2002).
[CrossRef] [PubMed]

Sharpe, S. J.

A. J. Merriam, S. J. Sharpe, M. Shverdin, D. Manuszak, G. Y. Yin, and S. E. Harris, "Efficient nonlinear frequency conversion in an all-resonant double-lambda system," Phys. Rev. Lett. 84, 5308-5311 (2000).
[CrossRef] [PubMed]

Shen, Y. R.

Y. R. Shen, The Principles of Nonlinear Optics (Wiley, 1984).

Shverdin, M.

A. J. Merriam, S. J. Sharpe, M. Shverdin, D. Manuszak, G. Y. Yin, and S. E. Harris, "Efficient nonlinear frequency conversion in an all-resonant double-lambda system," Phys. Rev. Lett. 84, 5308-5311 (2000).
[CrossRef] [PubMed]

Sokolov, A. V.

M. O. Scully, G. W. Kattawar, P. R. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," Proc. Natl. Acad. Sci. U.S.A. 99, 10994-11001 (2002).
[CrossRef] [PubMed]

S. E. Harris and A. V. Sokolov, "Subfemtosecond pulse generation by molecular modulation," Phys. Rev. Lett. 81, 2894-2897 (1998).
[CrossRef]

Stoicheff, B. P.

K. Hakuta, L. Marmet, and B. P. Stoicheff, "Nonlinear optical-generation with reduced absorption using electric-field coupling in atomic hydrogen," Phys. Rev. A 45, 5152-5159 (1992).
[CrossRef] [PubMed]

Sudarshanam, V. S.

A. V. Turukhin, V. S. Sudarshanam, M. S. Shahriar, J. A. Musser, B. S. Ham, and P. R. Hemmer, "Observation of ultraslow and stored light pulses in a solid," Phys. Rev. Lett. 88, 023602 (2002).
[CrossRef] [PubMed]

Turukhin, A. V.

A. V. Turukhin, V. S. Sudarshanam, M. S. Shahriar, J. A. Musser, B. S. Ham, and P. R. Hemmer, "Observation of ultraslow and stored light pulses in a solid," Phys. Rev. Lett. 88, 023602 (2002).
[CrossRef] [PubMed]

Vaughan, J. C.

Voronovich, A. G.

A. G. Voronovich, Wave Scattering from Rough Surfaces (Springer-Verlag, 1994).
[CrossRef]

Walsworth, R. L.

D. F. Phillips, A. Fleischhauer, A. Mair, R. L. Walsworth, and M. D. Lukin, "Storage of light in atomic vapor," Phys. Rev. Lett. 86, 783-786 (2001).
[CrossRef] [PubMed]

Wang, H.

H. Wang, D. Goorskey, and M. Xiao, "Enhanced Kerr nonlinearity via atomic coherence in a three-level atomic system," Phys. Rev. Lett. 87, 073601 (2001).
[CrossRef] [PubMed]

Warren, W.

V. Kocharovsky, S. Cameron, K. Lehmann, R. Lucht, R. Miles, Y. Rostovtsev, W. Warren, G. R. Welch, and M. O. Scully, "Gain-swept superradiance applied to the stand-off detection of trace impurities in the atmosphere," Proc. Natl. Acad. Sci. U.S.A. 102, 7806-7811 (2005).
[CrossRef] [PubMed]

Weiner, A. M.

A. M. Weiner, D. E. Leaird, J. S. Patel, and J. R. Wullert, "Programmable shaping of femtosecond optical pulses by use of 128-element liquid-crystal phase modulator," IEEE J. Quantum Electron. 28, 908-920 (1992).
[CrossRef]

Welch, G. R.

V. Kocharovsky, S. Cameron, K. Lehmann, R. Lucht, R. Miles, Y. Rostovtsev, W. Warren, G. R. Welch, and M. O. Scully, "Gain-swept superradiance applied to the stand-off detection of trace impurities in the atmosphere," Proc. Natl. Acad. Sci. U.S.A. 102, 7806-7811 (2005).
[CrossRef] [PubMed]

V. A. Sautenkov, C. Y. Ye, Y. V. Rostovtsev, G. R. Welch, andM. O. Scully, "Enhancement of field generation via maximal atomic coherence prepared by fast adiabatic passage in Rb vapor," Phys. Rev. A 70, 033406 (2004).
[CrossRef]

A. S. Zibrov, A. B. Matsko, O. Kocharovskaya, Y. V. Rostovtsev, G. R. Welch, and M. O. Scully, "Transporting and time reversing light via atomic coherence," Phys. Rev. Lett. 88, 103601 (2002).
[CrossRef] [PubMed]

A. B. Matsko, O. Kocharovskaya, Y. Rostovtsev, G. R. Welch, A. S. Zibrov, and M. O. Scully, "Slow, ultraslow, stored, and frozen light," Adv. At., Mol. Opt. Phys. 46, 191-242 (2001).
[CrossRef]

Wullert, J. R.

A. M. Weiner, D. E. Leaird, J. S. Patel, and J. R. Wullert, "Programmable shaping of femtosecond optical pulses by use of 128-element liquid-crystal phase modulator," IEEE J. Quantum Electron. 28, 908-920 (1992).
[CrossRef]

Xia, H.

M. Jain, H. Xia, G. Y. Yin, A. J. Merriam, and S. E. Harris, "Efficient nonlinear frequency conversion with maximal atomic coherence," Phys. Rev. Lett. 77, 4326-4329 (1996).
[CrossRef] [PubMed]

Xiao, M.

H. Wang, D. Goorskey, and M. Xiao, "Enhanced Kerr nonlinearity via atomic coherence in a three-level atomic system," Phys. Rev. Lett. 87, 073601 (2001).
[CrossRef] [PubMed]

Ye, C. Y.

V. A. Sautenkov, C. Y. Ye, Y. V. Rostovtsev, G. R. Welch, andM. O. Scully, "Enhancement of field generation via maximal atomic coherence prepared by fast adiabatic passage in Rb vapor," Phys. Rev. A 70, 033406 (2004).
[CrossRef]

Yin, G. Y.

A. J. Merriam, S. J. Sharpe, M. Shverdin, D. Manuszak, G. Y. Yin, and S. E. Harris, "Efficient nonlinear frequency conversion in an all-resonant double-lambda system," Phys. Rev. Lett. 84, 5308-5311 (2000).
[CrossRef] [PubMed]

S. E. Harris, G. Y. Yin, M. Jain, and A. J. Merriam, "Nonlinear optics at maximum coherence," Philos. Trans. R. Soc. London, Ser. A 355, 2291-2304 (1997).
[CrossRef]

M. Jain, H. Xia, G. Y. Yin, A. J. Merriam, and S. E. Harris, "Efficient nonlinear frequency conversion with maximal atomic coherence," Phys. Rev. Lett. 77, 4326-4329 (1996).
[CrossRef] [PubMed]

Zibrov, A. S.

A. S. Zibrov, A. B. Matsko, O. Kocharovskaya, Y. V. Rostovtsev, G. R. Welch, and M. O. Scully, "Transporting and time reversing light via atomic coherence," Phys. Rev. Lett. 88, 103601 (2002).
[CrossRef] [PubMed]

A. B. Matsko, O. Kocharovskaya, Y. Rostovtsev, G. R. Welch, A. S. Zibrov, and M. O. Scully, "Slow, ultraslow, stored, and frozen light," Adv. At., Mol. Opt. Phys. 46, 191-242 (2001).
[CrossRef]

Zubairy, M. S.

M. O. Scully, G. W. Kattawar, P. R. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," Proc. Natl. Acad. Sci. U.S.A. 99, 10994-11001 (2002).
[CrossRef] [PubMed]

Adv. At., Mol. Opt. Phys. (1)

A. B. Matsko, O. Kocharovskaya, Y. Rostovtsev, G. R. Welch, A. S. Zibrov, and M. O. Scully, "Slow, ultraslow, stored, and frozen light," Adv. At., Mol. Opt. Phys. 46, 191-242 (2001).
[CrossRef]

IEEE J. Quantum Electron. (1)

A. M. Weiner, D. E. Leaird, J. S. Patel, and J. R. Wullert, "Programmable shaping of femtosecond optical pulses by use of 128-element liquid-crystal phase modulator," IEEE J. Quantum Electron. 28, 908-920 (1992).
[CrossRef]

Nature (1)

C. Liu, Z. Dutton, C. H. Behroozi, and L. V. Hau, "Observation of coherent optical information storage in an atomic medium using halted light pulses," Nature 409, 490-493 (2001).
[CrossRef] [PubMed]

Opt. Lett. (1)

Philos. Trans. R. Soc. London, Ser. A (1)

S. E. Harris, G. Y. Yin, M. Jain, and A. J. Merriam, "Nonlinear optics at maximum coherence," Philos. Trans. R. Soc. London, Ser. A 355, 2291-2304 (1997).
[CrossRef]

Phys. Rev. A (4)

K. Hakuta, L. Marmet, and B. P. Stoicheff, "Nonlinear optical-generation with reduced absorption using electric-field coupling in atomic hydrogen," Phys. Rev. A 45, 5152-5159 (1992).
[CrossRef] [PubMed]

V. A. Sautenkov, C. Y. Ye, Y. V. Rostovtsev, G. R. Welch, andM. O. Scully, "Enhancement of field generation via maximal atomic coherence prepared by fast adiabatic passage in Rb vapor," Phys. Rev. A 70, 033406 (2004).
[CrossRef]

Y. H. Rim, J. W. Haus, and J. Schroeder, "Forward and backward scattering of light in inhomegeneous-media," Phys. Rev. A 42, 2385-2400 (1990).
[CrossRef] [PubMed]

R. Bonifacio, F. A. Hopf, P. Meystre, and M. O. Scully, "Steady-state pulses and superradiance in short-wavelength, swept-gain amplifiers," Phys. Rev. A 12, 2568-2573 (1975).
[CrossRef]

Phys. Rev. Lett. (7)

S. E. Harris and A. V. Sokolov, "Subfemtosecond pulse generation by molecular modulation," Phys. Rev. Lett. 81, 2894-2897 (1998).
[CrossRef]

D. F. Phillips, A. Fleischhauer, A. Mair, R. L. Walsworth, and M. D. Lukin, "Storage of light in atomic vapor," Phys. Rev. Lett. 86, 783-786 (2001).
[CrossRef] [PubMed]

A. S. Zibrov, A. B. Matsko, O. Kocharovskaya, Y. V. Rostovtsev, G. R. Welch, and M. O. Scully, "Transporting and time reversing light via atomic coherence," Phys. Rev. Lett. 88, 103601 (2002).
[CrossRef] [PubMed]

M. Jain, H. Xia, G. Y. Yin, A. J. Merriam, and S. E. Harris, "Efficient nonlinear frequency conversion with maximal atomic coherence," Phys. Rev. Lett. 77, 4326-4329 (1996).
[CrossRef] [PubMed]

A. J. Merriam, S. J. Sharpe, M. Shverdin, D. Manuszak, G. Y. Yin, and S. E. Harris, "Efficient nonlinear frequency conversion in an all-resonant double-lambda system," Phys. Rev. Lett. 84, 5308-5311 (2000).
[CrossRef] [PubMed]

H. Wang, D. Goorskey, and M. Xiao, "Enhanced Kerr nonlinearity via atomic coherence in a three-level atomic system," Phys. Rev. Lett. 87, 073601 (2001).
[CrossRef] [PubMed]

A. V. Turukhin, V. S. Sudarshanam, M. S. Shahriar, J. A. Musser, B. S. Ham, and P. R. Hemmer, "Observation of ultraslow and stored light pulses in a solid," Phys. Rev. Lett. 88, 023602 (2002).
[CrossRef] [PubMed]

Proc. Natl. Acad. Sci. U.S.A. (2)

M. O. Scully, G. W. Kattawar, P. R. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, "FAST CARS: Engineering a laser spectroscopic technique for rapid identification of bacterial spores," Proc. Natl. Acad. Sci. U.S.A. 99, 10994-11001 (2002).
[CrossRef] [PubMed]

V. Kocharovsky, S. Cameron, K. Lehmann, R. Lucht, R. Miles, Y. Rostovtsev, W. Warren, G. R. Welch, and M. O. Scully, "Gain-swept superradiance applied to the stand-off detection of trace impurities in the atmosphere," Proc. Natl. Acad. Sci. U.S.A. 102, 7806-7811 (2005).
[CrossRef] [PubMed]

Spectrochim. Acta, Part A (1)

P. Carmona, "Vibrational-spectra and structure of crystalline dipicolinic acid and calcium dipicolinic trihydrate," Spectrochim. Acta, Part A 36A, 705-712 (1980).
[CrossRef]

Other (7)

R. W. Boyd, Nonlinear Optics (Academic, 1992).

M. D. Levenson and S. S. Kano, Introduction of Nonlinear Spectroscopy (Academic, 1988).

G. L. Eesley, CARS Spectroscopy (Pergamon, 1981).

Y. R. Shen, The Principles of Nonlinear Optics (Wiley, 1984).

Erwin Schanda, Physical Fundamentals of Remote Sensing (Springer-Verlag, 1986).
[CrossRef]

A. G. Voronovich, Wave Scattering from Rough Surfaces (Springer-Verlag, 1994).
[CrossRef]

M.Nieto-Vesperinas, ed., Scattering in Volumes and Surfaces (North-Holland, 1990).

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Figures (6)

Fig. 1
Fig. 1

Experimental setup.

Fig. 2
Fig. 2

Intensity of scattered light (arbitrary units) versus observation angle. Data taken for a “milky” crystal. The angular dependence of (a) scattered green light and (b) CARS signal are shown.

Fig. 3
Fig. 3

Data taken for flakes. The angular dependence of (a) scattered green light and (b) CARS signal are shown.

Fig. 4
Fig. 4

Dependence of the intensity of the CARS signal on the frequency obtained from the polycrystalline DPA.

Fig. 5
Fig. 5

Model of polycrystalline material consisting of a stack of crystals with rough surfaces. The light propagating through such a medium generates a new frequency via four-wave mixing and experiences scattering at the interfaces.

Fig. 6
Fig. 6

Simulations of the angular dependence of the CARS signal detected in the backward direction for different parameters of the model. (a) Broad angle distribution corresponds to “milky” crystal; (b) narrow angle distribution corresponds to flakes.

Equations (17)

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

k 4 = k 1 k 2 + k 3 ,
E s = E d S exp [ i ( k i r i k s r s ) ] ,
E s = E i x 1 x d x exp [ i k l ( x ) ] ,
l ( x ) = L [ sin ( θ 1 + ϕ ) sin ( θ 2 ϕ ) ] ,
tan ϕ = z ( x ) z ( x 1 ) x x 1 ,
h ( x ) = n a ( x n L ) θ ( x n L ) θ ( n L + L x ) ,
E s = exp [ i N k d ξ 2 ] sin ( N k d ξ 2 ) sin ( k d ξ 2 ) sin c ( k d ξ 2 ) E i ,
E s = E i exp [ i N k d ψ 1 ] 1 exp [ i k d ψ 1 ] 1 q J q ( k a ψ 0 ) exp ( i k d ψ 1 ) 1 i ( q + k d ψ 1 ) ,
E s = R E i = R exp [ i φ ] E i ,
Δ E 1 + ω 2 c 2 ( ε + δ ε ) E 1 = 0 ,
z E s = i 2 k Δ E s + i ω 2 c ϵ ϵ E in ,
E 1 s z = k E 1 s + R ̃ E 1 exp [ i ϕ ( z ) ] ,
E 1 s = E 10 exp ( k z ) L z d z R ̃ ( z , θ ) exp [ 2 k z + i ϕ ( z ) ] .
E 4 z = k E 4 + i η E 1 E 2 E 3 ,
E 4 s z = k E 4 s + R ̃ E 4 exp [ i ϕ ( z ) ] .
E 1 s = E 10 R [ 1 exp ( 2 k L ) 2 k ] ,
E 4 s = η E 1 0 E 20 E 30 R 2 [ 1 exp ( 2 k L ) 2 k ] 2 .

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