Abstract

We investigate the bleaching of two-photon absorption by single-photon excitation using femtosecond transient absorption measurements on the prototypical polyfluorene (F8), and thus introduce single-photon pumping and two-photon probing spectroscopy for the determination of absorption cross-sections in an organic semiconductor. Single-photon excitation at 3.1 eV rearranges the population distributions on the singlet excited state (1Bu ) and on the ground state (1Ag ), and probe pulses at 1.55 eV will thus be absorbed both by the singlet excited state through a single-photon process and by the partially depopulated ground state for two-photon transition from 1Ag to mAg . As a result, the two-photon absorption will be partially bleached, introducing a modulation to the total transient absorption. Probe intensity dependence of the transient absorption enables simultaneous determination of the two-photon absorption (mAg1Ag ) and exciton absorption (kAg1Bu ) cross-sections at 1.55 eV.

© 2005 Optical Society of America

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  1. A. J. Bain , R. J. Marsh , D. A. Armoogum , O. Mongint , L. Porrest , and M. Blanchard-Descet , “ Time-resolved stimulated emission depletion in two-photon excited states ,” Biochem. Soc. Trans.: Intermolecular Associations in 2D and 3D   31 , 1047 ( 2003 ).
    [Crossref]
  2. Saulius Juodkazis , Vygantas Mizeikis , Kock Khuen Seet , Masafumi Miwa , and Hiroaki Misawa , “ Two-photon lithography of nanorods in SU-8 photoresist ,” Nanotechnology   16 , 846 ( 2005 ).
    [Crossref]
  3. G. J. Brakenhoff , J. Squier , T. Norris , A. C. Bliton , M. H. Wade , and B. Athey , “ Real-time two-photon confocal microscopy using a femtosecond, amplified, Ti:Sapphire system ,” J. Microscopy   181 , 253 ( 1995 ).
    [Crossref]
  4. T. Sun , Bosco K. K. Fung , I. K. Sou , G. K. L. Wong , K. S. Wong , and G. Lanzani , “ Two-photon absorption autocorrelation of visible to ultraviolet femtosecond laser pulses using ZnS-based photodetectors ,” IEEE Photonics Technol. Lett.   14 , 86 ( 2002 ).
    [Crossref]
  5. A. Gambetta , T. Virgili , and G. Lanzani , “ Ultrafast excitation cross-correlation photoconductivity in polyfluorene photodiodes ,” Appl. Phys. Lett.   86 , 253509 ( 2005 ).
    [Crossref]
  6. W. Blau and A. Penzkofer , “ Intensity detection of picosecond ruby laser pulses by two photon absorption ,” Opt. Commun.   36 , 419 ( 1981 ).
    [Crossref]
  7. Guang S. He , Tzu-Chau Lin , and Paras N. Prasad , “ New technique for degenerate two-photon absorption spectral measurements using femtosecond continuum generation ,” Opt. Express   10 , 566 ( 2002 ). http://www.opticsexpress.org/abstract.cfm?URI=OPEX-10-13-566
    [PubMed]
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    [Crossref]
  9. R. A. Negres , J. M. Hales , A. Kobyakov , D. J. Hagan , and E. W. Van Stryland , “ Two-photon spectroscopy and analysis with a white-light continuum probe ,” Opt. Lett.   27 , 270 ( 2002 ).
    [Crossref]
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    [Crossref]
  11. Mikhail Drobizhev , Yuriy Stepanenko , Yuliya Dzenis , Aliaksandr Karotki , Aleksander Rebane , Peter N. Taylor , and Harry L. Anderson , “ Understanding Strong Two-Photon Absorption in -Conjugated Porphyrin Dimers via Double-Resonance Enhancement in a Three-Level Model ,” J. Am. Chem. Soc.   126 , 15352 ( 2004 ).
    [Crossref] [PubMed]
  12. L. M. Herz and R. T. Phillips , “ Effects of interchain interactions, polarization anisotropy, and photo-oxidation on the ultrafast photoluminescence decay from a polyfluorene ,” Phys. Rev. B   61 , 13691 ( 2000 ).
    [Crossref]
  13. Amena L. T. Khan , Paiboon Sreearunothai , Lura M. Herz , Michael J. Banach , and Anna Kö , “ Morphology-dependent energy transfer within polyfluorene thin films ,” Phys. Rev. B   69 , 085201 ( 2004 ).
    [Crossref]
  14. M. G. Harrison , G. Urbasch , R. F. Mahrt , H. Giessen , H. Bässler , and U. Scherf , “ Two-photon fluorescence and femtosecond two-photon absorption studies of MeLPPP, a ladder-type poly(phenylene) with low intra-chain disorder ,” Chem. Phys. Lett.   313 , 755 ( 1999 ).
    [Crossref]
  15. S. V. Frolov , Z. Bao , M. Wohlgenannt , and Z. V. Vardeny , “ Ultrafast Spectroscopy of Even-Parity States in pi -Conjugated Polymers ,” Phys. Rev. Lett.   85 , 2196 ( 2000 ).
    [Crossref] [PubMed]
  16. Mark A. Stevens , Carlos Silva , David M. Russell , and Richard H. Friend , “ Exciton dissociation mechanisms in the polymeric semiconductors poly(9,9-dioctylfluorene) and poly(9,9-dioctylfluorene-co-benzothiadiazole) ,” Phys. Rev. B   63 , 165213 ( 2001 ).
    [Crossref]

2005 (2)

Saulius Juodkazis , Vygantas Mizeikis , Kock Khuen Seet , Masafumi Miwa , and Hiroaki Misawa , “ Two-photon lithography of nanorods in SU-8 photoresist ,” Nanotechnology   16 , 846 ( 2005 ).
[Crossref]

A. Gambetta , T. Virgili , and G. Lanzani , “ Ultrafast excitation cross-correlation photoconductivity in polyfluorene photodiodes ,” Appl. Phys. Lett.   86 , 253509 ( 2005 ).
[Crossref]

2004 (2)

Mikhail Drobizhev , Yuriy Stepanenko , Yuliya Dzenis , Aliaksandr Karotki , Aleksander Rebane , Peter N. Taylor , and Harry L. Anderson , “ Understanding Strong Two-Photon Absorption in -Conjugated Porphyrin Dimers via Double-Resonance Enhancement in a Three-Level Model ,” J. Am. Chem. Soc.   126 , 15352 ( 2004 ).
[Crossref] [PubMed]

Amena L. T. Khan , Paiboon Sreearunothai , Lura M. Herz , Michael J. Banach , and Anna Kö , “ Morphology-dependent energy transfer within polyfluorene thin films ,” Phys. Rev. B   69 , 085201 ( 2004 ).
[Crossref]

2003 (1)

A. J. Bain , R. J. Marsh , D. A. Armoogum , O. Mongint , L. Porrest , and M. Blanchard-Descet , “ Time-resolved stimulated emission depletion in two-photon excited states ,” Biochem. Soc. Trans.: Intermolecular Associations in 2D and 3D   31 , 1047 ( 2003 ).
[Crossref]

2002 (3)

2001 (1)

Mark A. Stevens , Carlos Silva , David M. Russell , and Richard H. Friend , “ Exciton dissociation mechanisms in the polymeric semiconductors poly(9,9-dioctylfluorene) and poly(9,9-dioctylfluorene-co-benzothiadiazole) ,” Phys. Rev. B   63 , 165213 ( 2001 ).
[Crossref]

2000 (2)

S. V. Frolov , Z. Bao , M. Wohlgenannt , and Z. V. Vardeny , “ Ultrafast Spectroscopy of Even-Parity States in pi -Conjugated Polymers ,” Phys. Rev. Lett.   85 , 2196 ( 2000 ).
[Crossref] [PubMed]

L. M. Herz and R. T. Phillips , “ Effects of interchain interactions, polarization anisotropy, and photo-oxidation on the ultrafast photoluminescence decay from a polyfluorene ,” Phys. Rev. B   61 , 13691 ( 2000 ).
[Crossref]

1999 (1)

M. G. Harrison , G. Urbasch , R. F. Mahrt , H. Giessen , H. Bässler , and U. Scherf , “ Two-photon fluorescence and femtosecond two-photon absorption studies of MeLPPP, a ladder-type poly(phenylene) with low intra-chain disorder ,” Chem. Phys. Lett.   313 , 755 ( 1999 ).
[Crossref]

1997 (1)

N. Mukherjee , A. Mukherjee , and B. A. Reinhardt , “ Measurement of two-photon absorption cross sections of dye molecules doped in thin films of polymethylmethacrylate ,” Appl. Phys. Lett.   70 , 1524 ( 1997 ).
[Crossref]

1995 (1)

G. J. Brakenhoff , J. Squier , T. Norris , A. C. Bliton , M. H. Wade , and B. Athey , “ Real-time two-photon confocal microscopy using a femtosecond, amplified, Ti:Sapphire system ,” J. Microscopy   181 , 253 ( 1995 ).
[Crossref]

1994 (1)

1981 (1)

W. Blau and A. Penzkofer , “ Intensity detection of picosecond ruby laser pulses by two photon absorption ,” Opt. Commun.   36 , 419 ( 1981 ).
[Crossref]

Anderson, Harry L.

Mikhail Drobizhev , Yuriy Stepanenko , Yuliya Dzenis , Aliaksandr Karotki , Aleksander Rebane , Peter N. Taylor , and Harry L. Anderson , “ Understanding Strong Two-Photon Absorption in -Conjugated Porphyrin Dimers via Double-Resonance Enhancement in a Three-Level Model ,” J. Am. Chem. Soc.   126 , 15352 ( 2004 ).
[Crossref] [PubMed]

Armoogum, D. A.

A. J. Bain , R. J. Marsh , D. A. Armoogum , O. Mongint , L. Porrest , and M. Blanchard-Descet , “ Time-resolved stimulated emission depletion in two-photon excited states ,” Biochem. Soc. Trans.: Intermolecular Associations in 2D and 3D   31 , 1047 ( 2003 ).
[Crossref]

Athey, B.

G. J. Brakenhoff , J. Squier , T. Norris , A. C. Bliton , M. H. Wade , and B. Athey , “ Real-time two-photon confocal microscopy using a femtosecond, amplified, Ti:Sapphire system ,” J. Microscopy   181 , 253 ( 1995 ).
[Crossref]

Bain, A. J.

A. J. Bain , R. J. Marsh , D. A. Armoogum , O. Mongint , L. Porrest , and M. Blanchard-Descet , “ Time-resolved stimulated emission depletion in two-photon excited states ,” Biochem. Soc. Trans.: Intermolecular Associations in 2D and 3D   31 , 1047 ( 2003 ).
[Crossref]

Banach, Michael J.

Amena L. T. Khan , Paiboon Sreearunothai , Lura M. Herz , Michael J. Banach , and Anna Kö , “ Morphology-dependent energy transfer within polyfluorene thin films ,” Phys. Rev. B   69 , 085201 ( 2004 ).
[Crossref]

Bao, Z.

S. V. Frolov , Z. Bao , M. Wohlgenannt , and Z. V. Vardeny , “ Ultrafast Spectroscopy of Even-Parity States in pi -Conjugated Polymers ,” Phys. Rev. Lett.   85 , 2196 ( 2000 ).
[Crossref] [PubMed]

Bässler, H.

M. G. Harrison , G. Urbasch , R. F. Mahrt , H. Giessen , H. Bässler , and U. Scherf , “ Two-photon fluorescence and femtosecond two-photon absorption studies of MeLPPP, a ladder-type poly(phenylene) with low intra-chain disorder ,” Chem. Phys. Lett.   313 , 755 ( 1999 ).
[Crossref]

Blanchard-Descet, M.

A. J. Bain , R. J. Marsh , D. A. Armoogum , O. Mongint , L. Porrest , and M. Blanchard-Descet , “ Time-resolved stimulated emission depletion in two-photon excited states ,” Biochem. Soc. Trans.: Intermolecular Associations in 2D and 3D   31 , 1047 ( 2003 ).
[Crossref]

Blau, W.

W. Blau and A. Penzkofer , “ Intensity detection of picosecond ruby laser pulses by two photon absorption ,” Opt. Commun.   36 , 419 ( 1981 ).
[Crossref]

Bliton, A. C.

G. J. Brakenhoff , J. Squier , T. Norris , A. C. Bliton , M. H. Wade , and B. Athey , “ Real-time two-photon confocal microscopy using a femtosecond, amplified, Ti:Sapphire system ,” J. Microscopy   181 , 253 ( 1995 ).
[Crossref]

Brakenhoff, G. J.

G. J. Brakenhoff , J. Squier , T. Norris , A. C. Bliton , M. H. Wade , and B. Athey , “ Real-time two-photon confocal microscopy using a femtosecond, amplified, Ti:Sapphire system ,” J. Microscopy   181 , 253 ( 1995 ).
[Crossref]

Drobizhev, Mikhail

Mikhail Drobizhev , Yuriy Stepanenko , Yuliya Dzenis , Aliaksandr Karotki , Aleksander Rebane , Peter N. Taylor , and Harry L. Anderson , “ Understanding Strong Two-Photon Absorption in -Conjugated Porphyrin Dimers via Double-Resonance Enhancement in a Three-Level Model ,” J. Am. Chem. Soc.   126 , 15352 ( 2004 ).
[Crossref] [PubMed]

Dzenis, Yuliya

Mikhail Drobizhev , Yuriy Stepanenko , Yuliya Dzenis , Aliaksandr Karotki , Aleksander Rebane , Peter N. Taylor , and Harry L. Anderson , “ Understanding Strong Two-Photon Absorption in -Conjugated Porphyrin Dimers via Double-Resonance Enhancement in a Three-Level Model ,” J. Am. Chem. Soc.   126 , 15352 ( 2004 ).
[Crossref] [PubMed]

Friend, Richard H.

Mark A. Stevens , Carlos Silva , David M. Russell , and Richard H. Friend , “ Exciton dissociation mechanisms in the polymeric semiconductors poly(9,9-dioctylfluorene) and poly(9,9-dioctylfluorene-co-benzothiadiazole) ,” Phys. Rev. B   63 , 165213 ( 2001 ).
[Crossref]

Frolov, S. V.

S. V. Frolov , Z. Bao , M. Wohlgenannt , and Z. V. Vardeny , “ Ultrafast Spectroscopy of Even-Parity States in pi -Conjugated Polymers ,” Phys. Rev. Lett.   85 , 2196 ( 2000 ).
[Crossref] [PubMed]

Fung, Bosco K. K.

T. Sun , Bosco K. K. Fung , I. K. Sou , G. K. L. Wong , K. S. Wong , and G. Lanzani , “ Two-photon absorption autocorrelation of visible to ultraviolet femtosecond laser pulses using ZnS-based photodetectors ,” IEEE Photonics Technol. Lett.   14 , 86 ( 2002 ).
[Crossref]

Gambetta, A.

A. Gambetta , T. Virgili , and G. Lanzani , “ Ultrafast excitation cross-correlation photoconductivity in polyfluorene photodiodes ,” Appl. Phys. Lett.   86 , 253509 ( 2005 ).
[Crossref]

Giessen, H.

M. G. Harrison , G. Urbasch , R. F. Mahrt , H. Giessen , H. Bässler , and U. Scherf , “ Two-photon fluorescence and femtosecond two-photon absorption studies of MeLPPP, a ladder-type poly(phenylene) with low intra-chain disorder ,” Chem. Phys. Lett.   313 , 755 ( 1999 ).
[Crossref]

Hagan, D. J.

Hales, J. M.

Harrison, M. G.

M. G. Harrison , G. Urbasch , R. F. Mahrt , H. Giessen , H. Bässler , and U. Scherf , “ Two-photon fluorescence and femtosecond two-photon absorption studies of MeLPPP, a ladder-type poly(phenylene) with low intra-chain disorder ,” Chem. Phys. Lett.   313 , 755 ( 1999 ).
[Crossref]

He, Guang S.

Herz, L. M.

L. M. Herz and R. T. Phillips , “ Effects of interchain interactions, polarization anisotropy, and photo-oxidation on the ultrafast photoluminescence decay from a polyfluorene ,” Phys. Rev. B   61 , 13691 ( 2000 ).
[Crossref]

Herz, Lura M.

Amena L. T. Khan , Paiboon Sreearunothai , Lura M. Herz , Michael J. Banach , and Anna Kö , “ Morphology-dependent energy transfer within polyfluorene thin films ,” Phys. Rev. B   69 , 085201 ( 2004 ).
[Crossref]

Juodkazis, Saulius

Saulius Juodkazis , Vygantas Mizeikis , Kock Khuen Seet , Masafumi Miwa , and Hiroaki Misawa , “ Two-photon lithography of nanorods in SU-8 photoresist ,” Nanotechnology   16 , 846 ( 2005 ).
[Crossref]

Karotki, Aliaksandr

Mikhail Drobizhev , Yuriy Stepanenko , Yuliya Dzenis , Aliaksandr Karotki , Aleksander Rebane , Peter N. Taylor , and Harry L. Anderson , “ Understanding Strong Two-Photon Absorption in -Conjugated Porphyrin Dimers via Double-Resonance Enhancement in a Three-Level Model ,” J. Am. Chem. Soc.   126 , 15352 ( 2004 ).
[Crossref] [PubMed]

Khan, Amena L. T.

Amena L. T. Khan , Paiboon Sreearunothai , Lura M. Herz , Michael J. Banach , and Anna Kö , “ Morphology-dependent energy transfer within polyfluorene thin films ,” Phys. Rev. B   69 , 085201 ( 2004 ).
[Crossref]

Kö, Anna

Amena L. T. Khan , Paiboon Sreearunothai , Lura M. Herz , Michael J. Banach , and Anna Kö , “ Morphology-dependent energy transfer within polyfluorene thin films ,” Phys. Rev. B   69 , 085201 ( 2004 ).
[Crossref]

Kobyakov, A.

Lanzani, G.

A. Gambetta , T. Virgili , and G. Lanzani , “ Ultrafast excitation cross-correlation photoconductivity in polyfluorene photodiodes ,” Appl. Phys. Lett.   86 , 253509 ( 2005 ).
[Crossref]

T. Sun , Bosco K. K. Fung , I. K. Sou , G. K. L. Wong , K. S. Wong , and G. Lanzani , “ Two-photon absorption autocorrelation of visible to ultraviolet femtosecond laser pulses using ZnS-based photodetectors ,” IEEE Photonics Technol. Lett.   14 , 86 ( 2002 ).
[Crossref]

Lin, Tzu-Chau

Mahrt, R. F.

M. G. Harrison , G. Urbasch , R. F. Mahrt , H. Giessen , H. Bässler , and U. Scherf , “ Two-photon fluorescence and femtosecond two-photon absorption studies of MeLPPP, a ladder-type poly(phenylene) with low intra-chain disorder ,” Chem. Phys. Lett.   313 , 755 ( 1999 ).
[Crossref]

Marsh, R. J.

A. J. Bain , R. J. Marsh , D. A. Armoogum , O. Mongint , L. Porrest , and M. Blanchard-Descet , “ Time-resolved stimulated emission depletion in two-photon excited states ,” Biochem. Soc. Trans.: Intermolecular Associations in 2D and 3D   31 , 1047 ( 2003 ).
[Crossref]

Misawa, Hiroaki

Saulius Juodkazis , Vygantas Mizeikis , Kock Khuen Seet , Masafumi Miwa , and Hiroaki Misawa , “ Two-photon lithography of nanorods in SU-8 photoresist ,” Nanotechnology   16 , 846 ( 2005 ).
[Crossref]

Miwa, Masafumi

Saulius Juodkazis , Vygantas Mizeikis , Kock Khuen Seet , Masafumi Miwa , and Hiroaki Misawa , “ Two-photon lithography of nanorods in SU-8 photoresist ,” Nanotechnology   16 , 846 ( 2005 ).
[Crossref]

Mizeikis, Vygantas

Saulius Juodkazis , Vygantas Mizeikis , Kock Khuen Seet , Masafumi Miwa , and Hiroaki Misawa , “ Two-photon lithography of nanorods in SU-8 photoresist ,” Nanotechnology   16 , 846 ( 2005 ).
[Crossref]

Mongint, O.

A. J. Bain , R. J. Marsh , D. A. Armoogum , O. Mongint , L. Porrest , and M. Blanchard-Descet , “ Time-resolved stimulated emission depletion in two-photon excited states ,” Biochem. Soc. Trans.: Intermolecular Associations in 2D and 3D   31 , 1047 ( 2003 ).
[Crossref]

Mukherjee, A.

N. Mukherjee , A. Mukherjee , and B. A. Reinhardt , “ Measurement of two-photon absorption cross sections of dye molecules doped in thin films of polymethylmethacrylate ,” Appl. Phys. Lett.   70 , 1524 ( 1997 ).
[Crossref]

Mukherjee, N.

N. Mukherjee , A. Mukherjee , and B. A. Reinhardt , “ Measurement of two-photon absorption cross sections of dye molecules doped in thin films of polymethylmethacrylate ,” Appl. Phys. Lett.   70 , 1524 ( 1997 ).
[Crossref]

Negres, R. A.

Norris, T.

G. J. Brakenhoff , J. Squier , T. Norris , A. C. Bliton , M. H. Wade , and B. Athey , “ Real-time two-photon confocal microscopy using a femtosecond, amplified, Ti:Sapphire system ,” J. Microscopy   181 , 253 ( 1995 ).
[Crossref]

Penzkofer, A.

W. Blau and A. Penzkofer , “ Intensity detection of picosecond ruby laser pulses by two photon absorption ,” Opt. Commun.   36 , 419 ( 1981 ).
[Crossref]

Phillips, R. T.

L. M. Herz and R. T. Phillips , “ Effects of interchain interactions, polarization anisotropy, and photo-oxidation on the ultrafast photoluminescence decay from a polyfluorene ,” Phys. Rev. B   61 , 13691 ( 2000 ).
[Crossref]

Porrest, L.

A. J. Bain , R. J. Marsh , D. A. Armoogum , O. Mongint , L. Porrest , and M. Blanchard-Descet , “ Time-resolved stimulated emission depletion in two-photon excited states ,” Biochem. Soc. Trans.: Intermolecular Associations in 2D and 3D   31 , 1047 ( 2003 ).
[Crossref]

Prasad, Paras N.

Rebane, Aleksander

Mikhail Drobizhev , Yuriy Stepanenko , Yuliya Dzenis , Aliaksandr Karotki , Aleksander Rebane , Peter N. Taylor , and Harry L. Anderson , “ Understanding Strong Two-Photon Absorption in -Conjugated Porphyrin Dimers via Double-Resonance Enhancement in a Three-Level Model ,” J. Am. Chem. Soc.   126 , 15352 ( 2004 ).
[Crossref] [PubMed]

Reinhardt, B. A.

N. Mukherjee , A. Mukherjee , and B. A. Reinhardt , “ Measurement of two-photon absorption cross sections of dye molecules doped in thin films of polymethylmethacrylate ,” Appl. Phys. Lett.   70 , 1524 ( 1997 ).
[Crossref]

Russell, David M.

Mark A. Stevens , Carlos Silva , David M. Russell , and Richard H. Friend , “ Exciton dissociation mechanisms in the polymeric semiconductors poly(9,9-dioctylfluorene) and poly(9,9-dioctylfluorene-co-benzothiadiazole) ,” Phys. Rev. B   63 , 165213 ( 2001 ).
[Crossref]

Scherf, U.

M. G. Harrison , G. Urbasch , R. F. Mahrt , H. Giessen , H. Bässler , and U. Scherf , “ Two-photon fluorescence and femtosecond two-photon absorption studies of MeLPPP, a ladder-type poly(phenylene) with low intra-chain disorder ,” Chem. Phys. Lett.   313 , 755 ( 1999 ).
[Crossref]

Seet, Kock Khuen

Saulius Juodkazis , Vygantas Mizeikis , Kock Khuen Seet , Masafumi Miwa , and Hiroaki Misawa , “ Two-photon lithography of nanorods in SU-8 photoresist ,” Nanotechnology   16 , 846 ( 2005 ).
[Crossref]

Silva, Carlos

Mark A. Stevens , Carlos Silva , David M. Russell , and Richard H. Friend , “ Exciton dissociation mechanisms in the polymeric semiconductors poly(9,9-dioctylfluorene) and poly(9,9-dioctylfluorene-co-benzothiadiazole) ,” Phys. Rev. B   63 , 165213 ( 2001 ).
[Crossref]

Sou, I. K.

T. Sun , Bosco K. K. Fung , I. K. Sou , G. K. L. Wong , K. S. Wong , and G. Lanzani , “ Two-photon absorption autocorrelation of visible to ultraviolet femtosecond laser pulses using ZnS-based photodetectors ,” IEEE Photonics Technol. Lett.   14 , 86 ( 2002 ).
[Crossref]

Squier, J.

G. J. Brakenhoff , J. Squier , T. Norris , A. C. Bliton , M. H. Wade , and B. Athey , “ Real-time two-photon confocal microscopy using a femtosecond, amplified, Ti:Sapphire system ,” J. Microscopy   181 , 253 ( 1995 ).
[Crossref]

Sreearunothai, Paiboon

Amena L. T. Khan , Paiboon Sreearunothai , Lura M. Herz , Michael J. Banach , and Anna Kö , “ Morphology-dependent energy transfer within polyfluorene thin films ,” Phys. Rev. B   69 , 085201 ( 2004 ).
[Crossref]

Stepanenko, Yuriy

Mikhail Drobizhev , Yuriy Stepanenko , Yuliya Dzenis , Aliaksandr Karotki , Aleksander Rebane , Peter N. Taylor , and Harry L. Anderson , “ Understanding Strong Two-Photon Absorption in -Conjugated Porphyrin Dimers via Double-Resonance Enhancement in a Three-Level Model ,” J. Am. Chem. Soc.   126 , 15352 ( 2004 ).
[Crossref] [PubMed]

Stevens, Mark A.

Mark A. Stevens , Carlos Silva , David M. Russell , and Richard H. Friend , “ Exciton dissociation mechanisms in the polymeric semiconductors poly(9,9-dioctylfluorene) and poly(9,9-dioctylfluorene-co-benzothiadiazole) ,” Phys. Rev. B   63 , 165213 ( 2001 ).
[Crossref]

Stryland, E. W. Van

Sun, T.

T. Sun , Bosco K. K. Fung , I. K. Sou , G. K. L. Wong , K. S. Wong , and G. Lanzani , “ Two-photon absorption autocorrelation of visible to ultraviolet femtosecond laser pulses using ZnS-based photodetectors ,” IEEE Photonics Technol. Lett.   14 , 86 ( 2002 ).
[Crossref]

Taylor, Peter N.

Mikhail Drobizhev , Yuriy Stepanenko , Yuliya Dzenis , Aliaksandr Karotki , Aleksander Rebane , Peter N. Taylor , and Harry L. Anderson , “ Understanding Strong Two-Photon Absorption in -Conjugated Porphyrin Dimers via Double-Resonance Enhancement in a Three-Level Model ,” J. Am. Chem. Soc.   126 , 15352 ( 2004 ).
[Crossref] [PubMed]

Urbasch, G.

M. G. Harrison , G. Urbasch , R. F. Mahrt , H. Giessen , H. Bässler , and U. Scherf , “ Two-photon fluorescence and femtosecond two-photon absorption studies of MeLPPP, a ladder-type poly(phenylene) with low intra-chain disorder ,” Chem. Phys. Lett.   313 , 755 ( 1999 ).
[Crossref]

Vardeny, Z. V.

S. V. Frolov , Z. Bao , M. Wohlgenannt , and Z. V. Vardeny , “ Ultrafast Spectroscopy of Even-Parity States in pi -Conjugated Polymers ,” Phys. Rev. Lett.   85 , 2196 ( 2000 ).
[Crossref] [PubMed]

Virgili, T.

A. Gambetta , T. Virgili , and G. Lanzani , “ Ultrafast excitation cross-correlation photoconductivity in polyfluorene photodiodes ,” Appl. Phys. Lett.   86 , 253509 ( 2005 ).
[Crossref]

Wade, M. H.

G. J. Brakenhoff , J. Squier , T. Norris , A. C. Bliton , M. H. Wade , and B. Athey , “ Real-time two-photon confocal microscopy using a femtosecond, amplified, Ti:Sapphire system ,” J. Microscopy   181 , 253 ( 1995 ).
[Crossref]

Wohlgenannt, M.

S. V. Frolov , Z. Bao , M. Wohlgenannt , and Z. V. Vardeny , “ Ultrafast Spectroscopy of Even-Parity States in pi -Conjugated Polymers ,” Phys. Rev. Lett.   85 , 2196 ( 2000 ).
[Crossref] [PubMed]

Wong, G. K. L.

T. Sun , Bosco K. K. Fung , I. K. Sou , G. K. L. Wong , K. S. Wong , and G. Lanzani , “ Two-photon absorption autocorrelation of visible to ultraviolet femtosecond laser pulses using ZnS-based photodetectors ,” IEEE Photonics Technol. Lett.   14 , 86 ( 2002 ).
[Crossref]

Wong, K. S.

T. Sun , Bosco K. K. Fung , I. K. Sou , G. K. L. Wong , K. S. Wong , and G. Lanzani , “ Two-photon absorption autocorrelation of visible to ultraviolet femtosecond laser pulses using ZnS-based photodetectors ,” IEEE Photonics Technol. Lett.   14 , 86 ( 2002 ).
[Crossref]

Xu, Gen C.

Appl. Phys. Lett. (2)

A. Gambetta , T. Virgili , and G. Lanzani , “ Ultrafast excitation cross-correlation photoconductivity in polyfluorene photodiodes ,” Appl. Phys. Lett.   86 , 253509 ( 2005 ).
[Crossref]

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Figures (5)

Fig. 1.
Fig. 1.

Transition mechanisms related to the transient absorption in single-photon pumping (at 2ω) and two-photon probing (at 2ω) spectroscopy.

Fig. 2.
Fig. 2.

Absorption spectrum of the F8/p-Xylene solution with a concentration of 0.1 mg/ml. Inset: the chemical structure of F8.

Fig. 3.
Fig. 3.

Dependence of the TA dynamics on the probe (1.55 eV) intensities at a pump (3.1 eV) intensity of 96 μJ/cm2. The filled circles are TA dynamics measurements at 2 eV for the lifetime comparison. The calculation of the absorption cross-sections have been performed for a delay of 4 ps, as marked by the dash-dotted vertical line.

Fig. 4.
Fig. 4.

Pump intensity dependence of the TA dynamics at the two-photon frequency. The pump fluence at 3.1 eV was changed from 22 μJ/cm2 to 176 μJ/cm2 with the probe fluence at 1.55 eV fixed at (a) 199 μJ/cm2 and (b) 1.99 mJ/cm2, respectively. (c) Comparison between the measurements in (a) and (b) with the simulations using the measured absorption cross-sections.

Fig. 5.
Fig. 5.

Simulated contour lines showing the absolute values of the TA (|ΔT/T|) as a function of the pump and the probe fluences.

Equations (7)

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N 2 t = N 2 τ 2 + N 1 P 1
N 2 ( t ) = N 0 P 1 τ 2 1 + P 1 τ 2 [ 1 e ( 1 τ 2 + P 1 ) τ P ] · e ( t τ P ) τ 2 ,
N 3 t = N 3 τ 3 + N 1 P 2
N 2 t = N 2 τ 2 + N 3 τ 3 N 2 P 3
N 0 N 1 + N 2 + N 3
d I ω dz = β 1 I ω β 2 I ω 2 .
Δ T T = I ω on I ω off 1

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