Abstract

We demonstrate high contrast quantum interference between one-photon and three-photon absorption pathways in an organic solid at room temperature. Illumination of a thin polymer film activated with fluorescing dendrimer chromophores of large three photon absorption cross section with two simultaneous femtosecond pulses at near-IR frequency ω and its third harmonic UV frequency 3ω results in a spatial interference fringe pattern observable by eye.

© 2005 Optical Society of America

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  1. M.O. Scully and M. S. Zubairy, Quantum Optics (Oxford University Press, 1996).
  2. E.A. Manykin and A. M. Afanas’ev, “On one possibility of making a medium transparent by multiquantum resonance,” Sov. Phys. JETP 25, 828–830 (1967).
  3. P. Brumer and M. Shapiro, “Control of unimolecular reactions using coherent light,” Chem. Phys. Lett. 126, 541–546 (1986).
    [CrossRef]
  4. C. Chen, Y-Y. Yin, and D. S. Elliott, “Interference between optical transitions,” Phys. Rev. Lett. 64, 507–510 (1990).
    [CrossRef] [PubMed]
  5. L. Zhu, V. Kleinman, X. Li, S. P. Lu, K. Trentelman, and R. Gordon,“Coherent laser control of the product distribution obtained in the photoexcitation of HI,” Science,  207, 77–80 (1995).
    [CrossRef]
  6. G. Xing, X. Wang, X. Huang, R. Bersohn, and B. Katz, “Modulation of resonant multiphoton ionization of CH3I by laser phase variation,” J. Chem. Phys. 104, 826–828 (1996).
    [CrossRef]
  7. S. A. Rice, “Interfering for the good of a chemical reaction”, Nature 406, 422–426 (2001).
    [CrossRef]
  8. M. Drobizhev, A. Karotki, A. Rebane, and C.W. Spangler, “New dendrimer molecules with record large two-photon absorption cross-section,” Opt. Lett. 26, 1081–1083 (2001).
    [CrossRef]
  9. M. Drobizhev, A. Karotki, Y. Dzenis, A. Rebane, Zhiyong Suo, and C.W. Spangler, “Strong cooperative enhancement of two-photon absorption in dendrimers,” J. Phys. Chem. B 107, 7540–7543 (2003).
    [CrossRef]
  10. M. Drobizhev, A. Karotki, M. Kruk, Yu. Dzenis, A. Rebane, Z. Suo, and C.W. Spangler, “Uncovering coherent domain structure in a series of p-conjugated dendrimers by simultaneous three-photon absorption,” J. Phys. Chem. B 108, 4221–4226 (2004).
    [CrossRef]
  11. C. Y. Ye, V. A. Sautenkov, Y. V. Rostovtsev, and M. O. Scully, “Fast optical switching via stimulated Raman adiabatic passage,” Opt. Lett. 28, 2213–2215 (2003).
    [CrossRef] [PubMed]
  12. M. Bajcsy, A. S. Zibrov, and M. D. Lukin, “Stationary pulses of light in an atomic medium,” Nature 426, 638–641(2003).
    [CrossRef] [PubMed]
  13. A. P. Heberle, J. J. Baumberg, and K. Koeler “Ultrafast coherent control and destruction of excitons inquantum wells,” Phys. Rev. Lett. 75, 2598–2601 (1995).
    [CrossRef] [PubMed]
  14. A. Hache, J. E. Sipe, and H. M. Driel, “Quantum interference control of electrical currents in GaAs,” IEEE J. Quantum Electron. 14, 1144–1154 (1998).
    [CrossRef]
  15. M. Albota, J.-L. Bredas, S. Marder, J. W. Perry, and W. W. Webb, “Design of organic molecules with large two-photon absorption cross sections,” Science 281, 1653–1657 (1998).
    [CrossRef] [PubMed]
  16. B. H. Cumpston, S. P. Ananthavel, S. Barlow, D. L Dyer, J. E. Ehrlich, L. L. Erskine, A. A. Heikal, S. M. Kuebler, I.-Y. S. Lee, D. McCord-Maughon, J. Qin, S. R. Marder, and J. W. Perry, “Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication,” Nature 398, 51–54 (1999).
    [CrossRef]
  17. G. S. He, P. P. Markowicz, T.-C. Lin, and P. Prasad, “Observation of stimulated emission by direct three-photon excitation,” Nature 415, 767–770 (2002).
    [CrossRef] [PubMed]
  18. C. W. Spangler, Z. Suo, M. Drobizhev, A. Karotki, and A. Rebane, “New organic dendrimers with greatly enhanced multi-photon absorption for photonic applications,” in: Organic Nanophotonics, F. Charra, V. M. Agranovich, and F. Kajzar, eds. (Kluwer Academiv Pub., Dadrech, 2003), pp.139–153.
  19. R. N. Dixon, D. W. Heang, X. F. Yang, S. Harich, J. J. Lin, and X. Yang, “Chemical “Double slits”: Dynamical interference of photodissociation pathways in water,” Science 285, 1249–1253 (1999).
    [CrossRef] [PubMed]
  20. R. J. Gordon, L. Zhu, and T. Seideman, “Using the phase of light as a photochemical tool,” J. Phys. Chem. A 105, 4387–4394 (2001).
    [CrossRef]

2004 (1)

M. Drobizhev, A. Karotki, M. Kruk, Yu. Dzenis, A. Rebane, Z. Suo, and C.W. Spangler, “Uncovering coherent domain structure in a series of p-conjugated dendrimers by simultaneous three-photon absorption,” J. Phys. Chem. B 108, 4221–4226 (2004).
[CrossRef]

2003 (3)

C. Y. Ye, V. A. Sautenkov, Y. V. Rostovtsev, and M. O. Scully, “Fast optical switching via stimulated Raman adiabatic passage,” Opt. Lett. 28, 2213–2215 (2003).
[CrossRef] [PubMed]

M. Bajcsy, A. S. Zibrov, and M. D. Lukin, “Stationary pulses of light in an atomic medium,” Nature 426, 638–641(2003).
[CrossRef] [PubMed]

M. Drobizhev, A. Karotki, Y. Dzenis, A. Rebane, Zhiyong Suo, and C.W. Spangler, “Strong cooperative enhancement of two-photon absorption in dendrimers,” J. Phys. Chem. B 107, 7540–7543 (2003).
[CrossRef]

2002 (1)

G. S. He, P. P. Markowicz, T.-C. Lin, and P. Prasad, “Observation of stimulated emission by direct three-photon excitation,” Nature 415, 767–770 (2002).
[CrossRef] [PubMed]

2001 (3)

S. A. Rice, “Interfering for the good of a chemical reaction”, Nature 406, 422–426 (2001).
[CrossRef]

M. Drobizhev, A. Karotki, A. Rebane, and C.W. Spangler, “New dendrimer molecules with record large two-photon absorption cross-section,” Opt. Lett. 26, 1081–1083 (2001).
[CrossRef]

R. J. Gordon, L. Zhu, and T. Seideman, “Using the phase of light as a photochemical tool,” J. Phys. Chem. A 105, 4387–4394 (2001).
[CrossRef]

1999 (2)

B. H. Cumpston, S. P. Ananthavel, S. Barlow, D. L Dyer, J. E. Ehrlich, L. L. Erskine, A. A. Heikal, S. M. Kuebler, I.-Y. S. Lee, D. McCord-Maughon, J. Qin, S. R. Marder, and J. W. Perry, “Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication,” Nature 398, 51–54 (1999).
[CrossRef]

R. N. Dixon, D. W. Heang, X. F. Yang, S. Harich, J. J. Lin, and X. Yang, “Chemical “Double slits”: Dynamical interference of photodissociation pathways in water,” Science 285, 1249–1253 (1999).
[CrossRef] [PubMed]

1998 (2)

A. Hache, J. E. Sipe, and H. M. Driel, “Quantum interference control of electrical currents in GaAs,” IEEE J. Quantum Electron. 14, 1144–1154 (1998).
[CrossRef]

M. Albota, J.-L. Bredas, S. Marder, J. W. Perry, and W. W. Webb, “Design of organic molecules with large two-photon absorption cross sections,” Science 281, 1653–1657 (1998).
[CrossRef] [PubMed]

1996 (1)

G. Xing, X. Wang, X. Huang, R. Bersohn, and B. Katz, “Modulation of resonant multiphoton ionization of CH3I by laser phase variation,” J. Chem. Phys. 104, 826–828 (1996).
[CrossRef]

1995 (2)

L. Zhu, V. Kleinman, X. Li, S. P. Lu, K. Trentelman, and R. Gordon,“Coherent laser control of the product distribution obtained in the photoexcitation of HI,” Science,  207, 77–80 (1995).
[CrossRef]

A. P. Heberle, J. J. Baumberg, and K. Koeler “Ultrafast coherent control and destruction of excitons inquantum wells,” Phys. Rev. Lett. 75, 2598–2601 (1995).
[CrossRef] [PubMed]

1990 (1)

C. Chen, Y-Y. Yin, and D. S. Elliott, “Interference between optical transitions,” Phys. Rev. Lett. 64, 507–510 (1990).
[CrossRef] [PubMed]

1986 (1)

P. Brumer and M. Shapiro, “Control of unimolecular reactions using coherent light,” Chem. Phys. Lett. 126, 541–546 (1986).
[CrossRef]

1967 (1)

E.A. Manykin and A. M. Afanas’ev, “On one possibility of making a medium transparent by multiquantum resonance,” Sov. Phys. JETP 25, 828–830 (1967).

Afanas’ev, A. M.

E.A. Manykin and A. M. Afanas’ev, “On one possibility of making a medium transparent by multiquantum resonance,” Sov. Phys. JETP 25, 828–830 (1967).

Albota, M.

M. Albota, J.-L. Bredas, S. Marder, J. W. Perry, and W. W. Webb, “Design of organic molecules with large two-photon absorption cross sections,” Science 281, 1653–1657 (1998).
[CrossRef] [PubMed]

Ananthavel, S. P.

B. H. Cumpston, S. P. Ananthavel, S. Barlow, D. L Dyer, J. E. Ehrlich, L. L. Erskine, A. A. Heikal, S. M. Kuebler, I.-Y. S. Lee, D. McCord-Maughon, J. Qin, S. R. Marder, and J. W. Perry, “Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication,” Nature 398, 51–54 (1999).
[CrossRef]

Bajcsy, M.

M. Bajcsy, A. S. Zibrov, and M. D. Lukin, “Stationary pulses of light in an atomic medium,” Nature 426, 638–641(2003).
[CrossRef] [PubMed]

Barlow, S.

B. H. Cumpston, S. P. Ananthavel, S. Barlow, D. L Dyer, J. E. Ehrlich, L. L. Erskine, A. A. Heikal, S. M. Kuebler, I.-Y. S. Lee, D. McCord-Maughon, J. Qin, S. R. Marder, and J. W. Perry, “Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication,” Nature 398, 51–54 (1999).
[CrossRef]

Baumberg, J. J.

A. P. Heberle, J. J. Baumberg, and K. Koeler “Ultrafast coherent control and destruction of excitons inquantum wells,” Phys. Rev. Lett. 75, 2598–2601 (1995).
[CrossRef] [PubMed]

Bersohn, R.

G. Xing, X. Wang, X. Huang, R. Bersohn, and B. Katz, “Modulation of resonant multiphoton ionization of CH3I by laser phase variation,” J. Chem. Phys. 104, 826–828 (1996).
[CrossRef]

Bredas, J.-L.

M. Albota, J.-L. Bredas, S. Marder, J. W. Perry, and W. W. Webb, “Design of organic molecules with large two-photon absorption cross sections,” Science 281, 1653–1657 (1998).
[CrossRef] [PubMed]

Brumer, P.

P. Brumer and M. Shapiro, “Control of unimolecular reactions using coherent light,” Chem. Phys. Lett. 126, 541–546 (1986).
[CrossRef]

Chen, C.

C. Chen, Y-Y. Yin, and D. S. Elliott, “Interference between optical transitions,” Phys. Rev. Lett. 64, 507–510 (1990).
[CrossRef] [PubMed]

Cumpston, B. H.

B. H. Cumpston, S. P. Ananthavel, S. Barlow, D. L Dyer, J. E. Ehrlich, L. L. Erskine, A. A. Heikal, S. M. Kuebler, I.-Y. S. Lee, D. McCord-Maughon, J. Qin, S. R. Marder, and J. W. Perry, “Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication,” Nature 398, 51–54 (1999).
[CrossRef]

Dixon, R. N.

R. N. Dixon, D. W. Heang, X. F. Yang, S. Harich, J. J. Lin, and X. Yang, “Chemical “Double slits”: Dynamical interference of photodissociation pathways in water,” Science 285, 1249–1253 (1999).
[CrossRef] [PubMed]

Driel, H. M.

A. Hache, J. E. Sipe, and H. M. Driel, “Quantum interference control of electrical currents in GaAs,” IEEE J. Quantum Electron. 14, 1144–1154 (1998).
[CrossRef]

Drobizhev, M.

M. Drobizhev, A. Karotki, M. Kruk, Yu. Dzenis, A. Rebane, Z. Suo, and C.W. Spangler, “Uncovering coherent domain structure in a series of p-conjugated dendrimers by simultaneous three-photon absorption,” J. Phys. Chem. B 108, 4221–4226 (2004).
[CrossRef]

M. Drobizhev, A. Karotki, Y. Dzenis, A. Rebane, Zhiyong Suo, and C.W. Spangler, “Strong cooperative enhancement of two-photon absorption in dendrimers,” J. Phys. Chem. B 107, 7540–7543 (2003).
[CrossRef]

M. Drobizhev, A. Karotki, A. Rebane, and C.W. Spangler, “New dendrimer molecules with record large two-photon absorption cross-section,” Opt. Lett. 26, 1081–1083 (2001).
[CrossRef]

C. W. Spangler, Z. Suo, M. Drobizhev, A. Karotki, and A. Rebane, “New organic dendrimers with greatly enhanced multi-photon absorption for photonic applications,” in: Organic Nanophotonics, F. Charra, V. M. Agranovich, and F. Kajzar, eds. (Kluwer Academiv Pub., Dadrech, 2003), pp.139–153.

Dyer, D. L

B. H. Cumpston, S. P. Ananthavel, S. Barlow, D. L Dyer, J. E. Ehrlich, L. L. Erskine, A. A. Heikal, S. M. Kuebler, I.-Y. S. Lee, D. McCord-Maughon, J. Qin, S. R. Marder, and J. W. Perry, “Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication,” Nature 398, 51–54 (1999).
[CrossRef]

Dzenis, Y.

M. Drobizhev, A. Karotki, Y. Dzenis, A. Rebane, Zhiyong Suo, and C.W. Spangler, “Strong cooperative enhancement of two-photon absorption in dendrimers,” J. Phys. Chem. B 107, 7540–7543 (2003).
[CrossRef]

Dzenis, Yu.

M. Drobizhev, A. Karotki, M. Kruk, Yu. Dzenis, A. Rebane, Z. Suo, and C.W. Spangler, “Uncovering coherent domain structure in a series of p-conjugated dendrimers by simultaneous three-photon absorption,” J. Phys. Chem. B 108, 4221–4226 (2004).
[CrossRef]

Ehrlich, J. E.

B. H. Cumpston, S. P. Ananthavel, S. Barlow, D. L Dyer, J. E. Ehrlich, L. L. Erskine, A. A. Heikal, S. M. Kuebler, I.-Y. S. Lee, D. McCord-Maughon, J. Qin, S. R. Marder, and J. W. Perry, “Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication,” Nature 398, 51–54 (1999).
[CrossRef]

Elliott, D. S.

C. Chen, Y-Y. Yin, and D. S. Elliott, “Interference between optical transitions,” Phys. Rev. Lett. 64, 507–510 (1990).
[CrossRef] [PubMed]

Erskine, L. L.

B. H. Cumpston, S. P. Ananthavel, S. Barlow, D. L Dyer, J. E. Ehrlich, L. L. Erskine, A. A. Heikal, S. M. Kuebler, I.-Y. S. Lee, D. McCord-Maughon, J. Qin, S. R. Marder, and J. W. Perry, “Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication,” Nature 398, 51–54 (1999).
[CrossRef]

Gordon, R.

L. Zhu, V. Kleinman, X. Li, S. P. Lu, K. Trentelman, and R. Gordon,“Coherent laser control of the product distribution obtained in the photoexcitation of HI,” Science,  207, 77–80 (1995).
[CrossRef]

Gordon, R. J.

R. J. Gordon, L. Zhu, and T. Seideman, “Using the phase of light as a photochemical tool,” J. Phys. Chem. A 105, 4387–4394 (2001).
[CrossRef]

Hache, A.

A. Hache, J. E. Sipe, and H. M. Driel, “Quantum interference control of electrical currents in GaAs,” IEEE J. Quantum Electron. 14, 1144–1154 (1998).
[CrossRef]

Harich, S.

R. N. Dixon, D. W. Heang, X. F. Yang, S. Harich, J. J. Lin, and X. Yang, “Chemical “Double slits”: Dynamical interference of photodissociation pathways in water,” Science 285, 1249–1253 (1999).
[CrossRef] [PubMed]

He, G. S.

G. S. He, P. P. Markowicz, T.-C. Lin, and P. Prasad, “Observation of stimulated emission by direct three-photon excitation,” Nature 415, 767–770 (2002).
[CrossRef] [PubMed]

Heang, D. W.

R. N. Dixon, D. W. Heang, X. F. Yang, S. Harich, J. J. Lin, and X. Yang, “Chemical “Double slits”: Dynamical interference of photodissociation pathways in water,” Science 285, 1249–1253 (1999).
[CrossRef] [PubMed]

Heberle, A. P.

A. P. Heberle, J. J. Baumberg, and K. Koeler “Ultrafast coherent control and destruction of excitons inquantum wells,” Phys. Rev. Lett. 75, 2598–2601 (1995).
[CrossRef] [PubMed]

Heikal, A. A.

B. H. Cumpston, S. P. Ananthavel, S. Barlow, D. L Dyer, J. E. Ehrlich, L. L. Erskine, A. A. Heikal, S. M. Kuebler, I.-Y. S. Lee, D. McCord-Maughon, J. Qin, S. R. Marder, and J. W. Perry, “Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication,” Nature 398, 51–54 (1999).
[CrossRef]

Huang, X.

G. Xing, X. Wang, X. Huang, R. Bersohn, and B. Katz, “Modulation of resonant multiphoton ionization of CH3I by laser phase variation,” J. Chem. Phys. 104, 826–828 (1996).
[CrossRef]

Karotki, A.

M. Drobizhev, A. Karotki, M. Kruk, Yu. Dzenis, A. Rebane, Z. Suo, and C.W. Spangler, “Uncovering coherent domain structure in a series of p-conjugated dendrimers by simultaneous three-photon absorption,” J. Phys. Chem. B 108, 4221–4226 (2004).
[CrossRef]

M. Drobizhev, A. Karotki, Y. Dzenis, A. Rebane, Zhiyong Suo, and C.W. Spangler, “Strong cooperative enhancement of two-photon absorption in dendrimers,” J. Phys. Chem. B 107, 7540–7543 (2003).
[CrossRef]

M. Drobizhev, A. Karotki, A. Rebane, and C.W. Spangler, “New dendrimer molecules with record large two-photon absorption cross-section,” Opt. Lett. 26, 1081–1083 (2001).
[CrossRef]

C. W. Spangler, Z. Suo, M. Drobizhev, A. Karotki, and A. Rebane, “New organic dendrimers with greatly enhanced multi-photon absorption for photonic applications,” in: Organic Nanophotonics, F. Charra, V. M. Agranovich, and F. Kajzar, eds. (Kluwer Academiv Pub., Dadrech, 2003), pp.139–153.

Katz, B.

G. Xing, X. Wang, X. Huang, R. Bersohn, and B. Katz, “Modulation of resonant multiphoton ionization of CH3I by laser phase variation,” J. Chem. Phys. 104, 826–828 (1996).
[CrossRef]

Kleinman, V.

L. Zhu, V. Kleinman, X. Li, S. P. Lu, K. Trentelman, and R. Gordon,“Coherent laser control of the product distribution obtained in the photoexcitation of HI,” Science,  207, 77–80 (1995).
[CrossRef]

Koeler, K.

A. P. Heberle, J. J. Baumberg, and K. Koeler “Ultrafast coherent control and destruction of excitons inquantum wells,” Phys. Rev. Lett. 75, 2598–2601 (1995).
[CrossRef] [PubMed]

Kruk, M.

M. Drobizhev, A. Karotki, M. Kruk, Yu. Dzenis, A. Rebane, Z. Suo, and C.W. Spangler, “Uncovering coherent domain structure in a series of p-conjugated dendrimers by simultaneous three-photon absorption,” J. Phys. Chem. B 108, 4221–4226 (2004).
[CrossRef]

Kuebler, S. M.

B. H. Cumpston, S. P. Ananthavel, S. Barlow, D. L Dyer, J. E. Ehrlich, L. L. Erskine, A. A. Heikal, S. M. Kuebler, I.-Y. S. Lee, D. McCord-Maughon, J. Qin, S. R. Marder, and J. W. Perry, “Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication,” Nature 398, 51–54 (1999).
[CrossRef]

Lee, I.-Y. S.

B. H. Cumpston, S. P. Ananthavel, S. Barlow, D. L Dyer, J. E. Ehrlich, L. L. Erskine, A. A. Heikal, S. M. Kuebler, I.-Y. S. Lee, D. McCord-Maughon, J. Qin, S. R. Marder, and J. W. Perry, “Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication,” Nature 398, 51–54 (1999).
[CrossRef]

Li, X.

L. Zhu, V. Kleinman, X. Li, S. P. Lu, K. Trentelman, and R. Gordon,“Coherent laser control of the product distribution obtained in the photoexcitation of HI,” Science,  207, 77–80 (1995).
[CrossRef]

Lin, J. J.

R. N. Dixon, D. W. Heang, X. F. Yang, S. Harich, J. J. Lin, and X. Yang, “Chemical “Double slits”: Dynamical interference of photodissociation pathways in water,” Science 285, 1249–1253 (1999).
[CrossRef] [PubMed]

Lin, T.-C.

G. S. He, P. P. Markowicz, T.-C. Lin, and P. Prasad, “Observation of stimulated emission by direct three-photon excitation,” Nature 415, 767–770 (2002).
[CrossRef] [PubMed]

Lu, S. P.

L. Zhu, V. Kleinman, X. Li, S. P. Lu, K. Trentelman, and R. Gordon,“Coherent laser control of the product distribution obtained in the photoexcitation of HI,” Science,  207, 77–80 (1995).
[CrossRef]

Lukin, M. D.

M. Bajcsy, A. S. Zibrov, and M. D. Lukin, “Stationary pulses of light in an atomic medium,” Nature 426, 638–641(2003).
[CrossRef] [PubMed]

Manykin, E.A.

E.A. Manykin and A. M. Afanas’ev, “On one possibility of making a medium transparent by multiquantum resonance,” Sov. Phys. JETP 25, 828–830 (1967).

Marder, S.

M. Albota, J.-L. Bredas, S. Marder, J. W. Perry, and W. W. Webb, “Design of organic molecules with large two-photon absorption cross sections,” Science 281, 1653–1657 (1998).
[CrossRef] [PubMed]

Marder, S. R.

B. H. Cumpston, S. P. Ananthavel, S. Barlow, D. L Dyer, J. E. Ehrlich, L. L. Erskine, A. A. Heikal, S. M. Kuebler, I.-Y. S. Lee, D. McCord-Maughon, J. Qin, S. R. Marder, and J. W. Perry, “Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication,” Nature 398, 51–54 (1999).
[CrossRef]

Markowicz, P. P.

G. S. He, P. P. Markowicz, T.-C. Lin, and P. Prasad, “Observation of stimulated emission by direct three-photon excitation,” Nature 415, 767–770 (2002).
[CrossRef] [PubMed]

McCord-Maughon, D.

B. H. Cumpston, S. P. Ananthavel, S. Barlow, D. L Dyer, J. E. Ehrlich, L. L. Erskine, A. A. Heikal, S. M. Kuebler, I.-Y. S. Lee, D. McCord-Maughon, J. Qin, S. R. Marder, and J. W. Perry, “Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication,” Nature 398, 51–54 (1999).
[CrossRef]

Perry, J. W.

B. H. Cumpston, S. P. Ananthavel, S. Barlow, D. L Dyer, J. E. Ehrlich, L. L. Erskine, A. A. Heikal, S. M. Kuebler, I.-Y. S. Lee, D. McCord-Maughon, J. Qin, S. R. Marder, and J. W. Perry, “Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication,” Nature 398, 51–54 (1999).
[CrossRef]

M. Albota, J.-L. Bredas, S. Marder, J. W. Perry, and W. W. Webb, “Design of organic molecules with large two-photon absorption cross sections,” Science 281, 1653–1657 (1998).
[CrossRef] [PubMed]

Prasad, P.

G. S. He, P. P. Markowicz, T.-C. Lin, and P. Prasad, “Observation of stimulated emission by direct three-photon excitation,” Nature 415, 767–770 (2002).
[CrossRef] [PubMed]

Qin, J.

B. H. Cumpston, S. P. Ananthavel, S. Barlow, D. L Dyer, J. E. Ehrlich, L. L. Erskine, A. A. Heikal, S. M. Kuebler, I.-Y. S. Lee, D. McCord-Maughon, J. Qin, S. R. Marder, and J. W. Perry, “Two-photon polymerization initiators for three-dimensional optical data storage and microfabrication,” Nature 398, 51–54 (1999).
[CrossRef]

Rebane, A.

M. Drobizhev, A. Karotki, M. Kruk, Yu. Dzenis, A. Rebane, Z. Suo, and C.W. Spangler, “Uncovering coherent domain structure in a series of p-conjugated dendrimers by simultaneous three-photon absorption,” J. Phys. Chem. B 108, 4221–4226 (2004).
[CrossRef]

M. Drobizhev, A. Karotki, Y. Dzenis, A. Rebane, Zhiyong Suo, and C.W. Spangler, “Strong cooperative enhancement of two-photon absorption in dendrimers,” J. Phys. Chem. B 107, 7540–7543 (2003).
[CrossRef]

M. Drobizhev, A. Karotki, A. Rebane, and C.W. Spangler, “New dendrimer molecules with record large two-photon absorption cross-section,” Opt. Lett. 26, 1081–1083 (2001).
[CrossRef]

C. W. Spangler, Z. Suo, M. Drobizhev, A. Karotki, and A. Rebane, “New organic dendrimers with greatly enhanced multi-photon absorption for photonic applications,” in: Organic Nanophotonics, F. Charra, V. M. Agranovich, and F. Kajzar, eds. (Kluwer Academiv Pub., Dadrech, 2003), pp.139–153.

Rice, S. A.

S. A. Rice, “Interfering for the good of a chemical reaction”, Nature 406, 422–426 (2001).
[CrossRef]

Rostovtsev, Y. V.

Sautenkov, V. A.

Scully, M. O.

Scully, M.O.

M.O. Scully and M. S. Zubairy, Quantum Optics (Oxford University Press, 1996).

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R. J. Gordon, L. Zhu, and T. Seideman, “Using the phase of light as a photochemical tool,” J. Phys. Chem. A 105, 4387–4394 (2001).
[CrossRef]

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P. Brumer and M. Shapiro, “Control of unimolecular reactions using coherent light,” Chem. Phys. Lett. 126, 541–546 (1986).
[CrossRef]

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A. Hache, J. E. Sipe, and H. M. Driel, “Quantum interference control of electrical currents in GaAs,” IEEE J. Quantum Electron. 14, 1144–1154 (1998).
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C. W. Spangler, Z. Suo, M. Drobizhev, A. Karotki, and A. Rebane, “New organic dendrimers with greatly enhanced multi-photon absorption for photonic applications,” in: Organic Nanophotonics, F. Charra, V. M. Agranovich, and F. Kajzar, eds. (Kluwer Academiv Pub., Dadrech, 2003), pp.139–153.

Spangler, C.W.

M. Drobizhev, A. Karotki, M. Kruk, Yu. Dzenis, A. Rebane, Z. Suo, and C.W. Spangler, “Uncovering coherent domain structure in a series of p-conjugated dendrimers by simultaneous three-photon absorption,” J. Phys. Chem. B 108, 4221–4226 (2004).
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M. Drobizhev, A. Karotki, Y. Dzenis, A. Rebane, Zhiyong Suo, and C.W. Spangler, “Strong cooperative enhancement of two-photon absorption in dendrimers,” J. Phys. Chem. B 107, 7540–7543 (2003).
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M. Drobizhev, A. Karotki, A. Rebane, and C.W. Spangler, “New dendrimer molecules with record large two-photon absorption cross-section,” Opt. Lett. 26, 1081–1083 (2001).
[CrossRef]

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M. Drobizhev, A. Karotki, M. Kruk, Yu. Dzenis, A. Rebane, Z. Suo, and C.W. Spangler, “Uncovering coherent domain structure in a series of p-conjugated dendrimers by simultaneous three-photon absorption,” J. Phys. Chem. B 108, 4221–4226 (2004).
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C. W. Spangler, Z. Suo, M. Drobizhev, A. Karotki, and A. Rebane, “New organic dendrimers with greatly enhanced multi-photon absorption for photonic applications,” in: Organic Nanophotonics, F. Charra, V. M. Agranovich, and F. Kajzar, eds. (Kluwer Academiv Pub., Dadrech, 2003), pp.139–153.

Suo, Zhiyong

M. Drobizhev, A. Karotki, Y. Dzenis, A. Rebane, Zhiyong Suo, and C.W. Spangler, “Strong cooperative enhancement of two-photon absorption in dendrimers,” J. Phys. Chem. B 107, 7540–7543 (2003).
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M. Albota, J.-L. Bredas, S. Marder, J. W. Perry, and W. W. Webb, “Design of organic molecules with large two-photon absorption cross sections,” Science 281, 1653–1657 (1998).
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G. Xing, X. Wang, X. Huang, R. Bersohn, and B. Katz, “Modulation of resonant multiphoton ionization of CH3I by laser phase variation,” J. Chem. Phys. 104, 826–828 (1996).
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R. N. Dixon, D. W. Heang, X. F. Yang, S. Harich, J. J. Lin, and X. Yang, “Chemical “Double slits”: Dynamical interference of photodissociation pathways in water,” Science 285, 1249–1253 (1999).
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R. N. Dixon, D. W. Heang, X. F. Yang, S. Harich, J. J. Lin, and X. Yang, “Chemical “Double slits”: Dynamical interference of photodissociation pathways in water,” Science 285, 1249–1253 (1999).
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C. Chen, Y-Y. Yin, and D. S. Elliott, “Interference between optical transitions,” Phys. Rev. Lett. 64, 507–510 (1990).
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R. J. Gordon, L. Zhu, and T. Seideman, “Using the phase of light as a photochemical tool,” J. Phys. Chem. A 105, 4387–4394 (2001).
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L. Zhu, V. Kleinman, X. Li, S. P. Lu, K. Trentelman, and R. Gordon,“Coherent laser control of the product distribution obtained in the photoexcitation of HI,” Science,  207, 77–80 (1995).
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M. Bajcsy, A. S. Zibrov, and M. D. Lukin, “Stationary pulses of light in an atomic medium,” Nature 426, 638–641(2003).
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M.O. Scully and M. S. Zubairy, Quantum Optics (Oxford University Press, 1996).

Chem. Phys. Lett. (1)

P. Brumer and M. Shapiro, “Control of unimolecular reactions using coherent light,” Chem. Phys. Lett. 126, 541–546 (1986).
[CrossRef]

IEEE J. Quantum Electron. (1)

A. Hache, J. E. Sipe, and H. M. Driel, “Quantum interference control of electrical currents in GaAs,” IEEE J. Quantum Electron. 14, 1144–1154 (1998).
[CrossRef]

J. Chem. Phys. (1)

G. Xing, X. Wang, X. Huang, R. Bersohn, and B. Katz, “Modulation of resonant multiphoton ionization of CH3I by laser phase variation,” J. Chem. Phys. 104, 826–828 (1996).
[CrossRef]

J. Phys. Chem. A (1)

R. J. Gordon, L. Zhu, and T. Seideman, “Using the phase of light as a photochemical tool,” J. Phys. Chem. A 105, 4387–4394 (2001).
[CrossRef]

J. Phys. Chem. B (2)

M. Drobizhev, A. Karotki, Y. Dzenis, A. Rebane, Zhiyong Suo, and C.W. Spangler, “Strong cooperative enhancement of two-photon absorption in dendrimers,” J. Phys. Chem. B 107, 7540–7543 (2003).
[CrossRef]

M. Drobizhev, A. Karotki, M. Kruk, Yu. Dzenis, A. Rebane, Z. Suo, and C.W. Spangler, “Uncovering coherent domain structure in a series of p-conjugated dendrimers by simultaneous three-photon absorption,” J. Phys. Chem. B 108, 4221–4226 (2004).
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Phys. Rev. Lett. (2)

C. Chen, Y-Y. Yin, and D. S. Elliott, “Interference between optical transitions,” Phys. Rev. Lett. 64, 507–510 (1990).
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A. P. Heberle, J. J. Baumberg, and K. Koeler “Ultrafast coherent control and destruction of excitons inquantum wells,” Phys. Rev. Lett. 75, 2598–2601 (1995).
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M. Albota, J.-L. Bredas, S. Marder, J. W. Perry, and W. W. Webb, “Design of organic molecules with large two-photon absorption cross sections,” Science 281, 1653–1657 (1998).
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R. N. Dixon, D. W. Heang, X. F. Yang, S. Harich, J. J. Lin, and X. Yang, “Chemical “Double slits”: Dynamical interference of photodissociation pathways in water,” Science 285, 1249–1253 (1999).
[CrossRef] [PubMed]

L. Zhu, V. Kleinman, X. Li, S. P. Lu, K. Trentelman, and R. Gordon,“Coherent laser control of the product distribution obtained in the photoexcitation of HI,” Science,  207, 77–80 (1995).
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Other (2)

M.O. Scully and M. S. Zubairy, Quantum Optics (Oxford University Press, 1996).

C. W. Spangler, Z. Suo, M. Drobizhev, A. Karotki, and A. Rebane, “New organic dendrimers with greatly enhanced multi-photon absorption for photonic applications,” in: Organic Nanophotonics, F. Charra, V. M. Agranovich, and F. Kajzar, eds. (Kluwer Academiv Pub., Dadrech, 2003), pp.139–153.

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Figures (3)

Fig. 1.
Fig. 1.

Main figure: experimental set up. A thin film of compound 1 generates 3rd harmonic at 415 nm with efficiency 1%. Compound 2 absorbs simultaneously UV and IR, and produces visible fluorescence at 560nm wavelength. Inset: a, conventional detector observes no interference between frequency ω and 3ω because these IR and UV wavelengths are absorbed independently from each other. b, Interference appears if a special detector (compound 2) is used, which is capable of absorbing, in the same electronic transition, both UV and IR wavelengths.

Fig. 2.
Fig. 2.

Absorption spectrum (right vertical scale and lower horizontal scale) and chemical structure of three-arm G-0 dendrimer based on bis-diphenylamino stilbene (BDPAS) repeat units (compound 1), and four-arm hybrid G-0 dendrimer based on bis-diphenylamino di-styryl benzene (BDPADSB) core with attached BDPAS branches (compound 2). Maximum molar extinction is, ε(420nm)=1.1 105 M-1 cm-1 and ε(420nm)=2.5 105 M-1 cm-1, for the compound 1 and 2, correspondingly. Black squares present three photon absorption cross section of compound 2 (left vertical scale and upper horizontal scale for laser wavelength).

Fig. 3.
Fig. 3.

Image of the fluorescence when UV pulse (a) or IR pulse (b) is applied alone. c, Interference pattern observed when both UV and IR pulses are applied simultaneously. d, Vertical intensity profile of the three images (along dashed lines). Dashed curve, estimated pattern of maximum contrast interference.

Equations (2)

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D = c 3 ω 1 2 Sin θ 2 .
F QI F UV + e i ϕ F IR 2 ,

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