Abstract

We combine different wavelengths from an intense high-order harmonics source with variable delay at the focus of a split-mirror interferometer to conduct pump–probe experiments on gas-phase molecules. We report measurements of the time resolution (<44fs) and spatial profiles (4μm×12μm) at the focus of the apparatus. We demonstrate the utility of this two-color, high-order-harmonic technique by time resolving molecular hydrogen elimination from C2H4 excited into its absorption band at 161nm.

© 2010 Optical Society of America

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  1. T. Brabec and F. Krausz, Rev. Mod. Phys. 72, 545 (2000).
    [CrossRef]
  2. J. van Tilborg, T. K. Allison, T. W. Wright, M. P. Hertlein, R. W. Falcone, Y. Liu, H. Merdji, and A. Belkacem, J. Phys. B 42, 081002 (2009).
    [CrossRef]
  3. E. Gagnon, P. Ranitovic, X.-M. Tong, C. L. Cocke, M. M. Murnane, H. C. Kapteyn, and A. S. Sandhu, Science 317, 1374 (2007).
    [CrossRef] [PubMed]
  4. K. Kosma, S. A. Trushin, W. Fuss, and W. E. Schmid, J. Phys. Chem. A 112, 7514 (2008).
    [CrossRef] [PubMed]
  5. T. K. Allison, “Femtosecond molecular dynamics studied with vacuum ultraviolet pulse pairs,” Ph.D. thesis (University of California at Berkeley, 2010).
  6. E. Takahashi, H. Hasegawa, Y. Nabekawa, and K. Midorikawa, Opt. Lett. 29, 507 (2004).
    [CrossRef] [PubMed]
  7. P. Tzallas, D. Charalambidis, N. A. Papadogiannis, K. Witte, and G. D. Tsakiris, Nature 426, 267 (2003).
    [CrossRef] [PubMed]
  8. H. Mashiko, A. Suda, and K. Midorikawa, Appl. Phys. B. 87, 221 (2007).
    [CrossRef]
  9. T. K. Allison, J. van Tilborg, T. W. Wright, M. P. Hertlein, R. W. Falcone, and A. Belkacem, Opt. Express 17, 8941 (2009).
    [CrossRef] [PubMed]
  10. S. A. Trushin, W. E. Schmid, and W. Fuss, Chem. Phys. Lett. 468, 9 (2009).
    [CrossRef]
  11. A. J. Merer and R. S. Mulliken, Chem. Rev. 69, 639 (1969).
    [CrossRef]
  12. H. Tao, B. G. Levine, and T. J. Martínez, J. Phys. Chem. A 113, 13656 (2009).
    [CrossRef] [PubMed]
  13. S.-H. Lee, Y. T. Lee, and X. Yang, J. Chem. Phys. 120, 10983 (2004).
    [CrossRef] [PubMed]
  14. A. Peralta Conde, J. Kruse, O. Faucher, P. Tzallas, E. P. Benis, and D. Charalambidis, Phys. Rev. A 79, 061405 (2009).
    [CrossRef]
  15. T. K. Allison, H. Tao, T. W. Wright, A. M. Stooke, C. Khurmi, J. van Tilborg, Y. Liu, R. W. Falcone, T. J. Martinez, and A. Belkacem are preparing a manuscript to be called “Ultrafast internal conversion in ethylene.”

2009 (5)

J. van Tilborg, T. K. Allison, T. W. Wright, M. P. Hertlein, R. W. Falcone, Y. Liu, H. Merdji, and A. Belkacem, J. Phys. B 42, 081002 (2009).
[CrossRef]

S. A. Trushin, W. E. Schmid, and W. Fuss, Chem. Phys. Lett. 468, 9 (2009).
[CrossRef]

H. Tao, B. G. Levine, and T. J. Martínez, J. Phys. Chem. A 113, 13656 (2009).
[CrossRef] [PubMed]

A. Peralta Conde, J. Kruse, O. Faucher, P. Tzallas, E. P. Benis, and D. Charalambidis, Phys. Rev. A 79, 061405 (2009).
[CrossRef]

T. K. Allison, J. van Tilborg, T. W. Wright, M. P. Hertlein, R. W. Falcone, and A. Belkacem, Opt. Express 17, 8941 (2009).
[CrossRef] [PubMed]

2008 (1)

K. Kosma, S. A. Trushin, W. Fuss, and W. E. Schmid, J. Phys. Chem. A 112, 7514 (2008).
[CrossRef] [PubMed]

2007 (2)

E. Gagnon, P. Ranitovic, X.-M. Tong, C. L. Cocke, M. M. Murnane, H. C. Kapteyn, and A. S. Sandhu, Science 317, 1374 (2007).
[CrossRef] [PubMed]

H. Mashiko, A. Suda, and K. Midorikawa, Appl. Phys. B. 87, 221 (2007).
[CrossRef]

2004 (2)

2003 (1)

P. Tzallas, D. Charalambidis, N. A. Papadogiannis, K. Witte, and G. D. Tsakiris, Nature 426, 267 (2003).
[CrossRef] [PubMed]

2000 (1)

T. Brabec and F. Krausz, Rev. Mod. Phys. 72, 545 (2000).
[CrossRef]

1969 (1)

A. J. Merer and R. S. Mulliken, Chem. Rev. 69, 639 (1969).
[CrossRef]

Allison, T. K.

J. van Tilborg, T. K. Allison, T. W. Wright, M. P. Hertlein, R. W. Falcone, Y. Liu, H. Merdji, and A. Belkacem, J. Phys. B 42, 081002 (2009).
[CrossRef]

T. K. Allison, J. van Tilborg, T. W. Wright, M. P. Hertlein, R. W. Falcone, and A. Belkacem, Opt. Express 17, 8941 (2009).
[CrossRef] [PubMed]

T. K. Allison, “Femtosecond molecular dynamics studied with vacuum ultraviolet pulse pairs,” Ph.D. thesis (University of California at Berkeley, 2010).

T. K. Allison, H. Tao, T. W. Wright, A. M. Stooke, C. Khurmi, J. van Tilborg, Y. Liu, R. W. Falcone, T. J. Martinez, and A. Belkacem are preparing a manuscript to be called “Ultrafast internal conversion in ethylene.”

Belkacem, A.

T. K. Allison, J. van Tilborg, T. W. Wright, M. P. Hertlein, R. W. Falcone, and A. Belkacem, Opt. Express 17, 8941 (2009).
[CrossRef] [PubMed]

J. van Tilborg, T. K. Allison, T. W. Wright, M. P. Hertlein, R. W. Falcone, Y. Liu, H. Merdji, and A. Belkacem, J. Phys. B 42, 081002 (2009).
[CrossRef]

T. K. Allison, H. Tao, T. W. Wright, A. M. Stooke, C. Khurmi, J. van Tilborg, Y. Liu, R. W. Falcone, T. J. Martinez, and A. Belkacem are preparing a manuscript to be called “Ultrafast internal conversion in ethylene.”

Benis, E. P.

A. Peralta Conde, J. Kruse, O. Faucher, P. Tzallas, E. P. Benis, and D. Charalambidis, Phys. Rev. A 79, 061405 (2009).
[CrossRef]

Brabec, T.

T. Brabec and F. Krausz, Rev. Mod. Phys. 72, 545 (2000).
[CrossRef]

Charalambidis, D.

A. Peralta Conde, J. Kruse, O. Faucher, P. Tzallas, E. P. Benis, and D. Charalambidis, Phys. Rev. A 79, 061405 (2009).
[CrossRef]

P. Tzallas, D. Charalambidis, N. A. Papadogiannis, K. Witte, and G. D. Tsakiris, Nature 426, 267 (2003).
[CrossRef] [PubMed]

Cocke, C. L.

E. Gagnon, P. Ranitovic, X.-M. Tong, C. L. Cocke, M. M. Murnane, H. C. Kapteyn, and A. S. Sandhu, Science 317, 1374 (2007).
[CrossRef] [PubMed]

Conde, A. Peralta

A. Peralta Conde, J. Kruse, O. Faucher, P. Tzallas, E. P. Benis, and D. Charalambidis, Phys. Rev. A 79, 061405 (2009).
[CrossRef]

Falcone, R. W.

T. K. Allison, J. van Tilborg, T. W. Wright, M. P. Hertlein, R. W. Falcone, and A. Belkacem, Opt. Express 17, 8941 (2009).
[CrossRef] [PubMed]

J. van Tilborg, T. K. Allison, T. W. Wright, M. P. Hertlein, R. W. Falcone, Y. Liu, H. Merdji, and A. Belkacem, J. Phys. B 42, 081002 (2009).
[CrossRef]

T. K. Allison, H. Tao, T. W. Wright, A. M. Stooke, C. Khurmi, J. van Tilborg, Y. Liu, R. W. Falcone, T. J. Martinez, and A. Belkacem are preparing a manuscript to be called “Ultrafast internal conversion in ethylene.”

Faucher, O.

A. Peralta Conde, J. Kruse, O. Faucher, P. Tzallas, E. P. Benis, and D. Charalambidis, Phys. Rev. A 79, 061405 (2009).
[CrossRef]

Fuss, W.

S. A. Trushin, W. E. Schmid, and W. Fuss, Chem. Phys. Lett. 468, 9 (2009).
[CrossRef]

K. Kosma, S. A. Trushin, W. Fuss, and W. E. Schmid, J. Phys. Chem. A 112, 7514 (2008).
[CrossRef] [PubMed]

Gagnon, E.

E. Gagnon, P. Ranitovic, X.-M. Tong, C. L. Cocke, M. M. Murnane, H. C. Kapteyn, and A. S. Sandhu, Science 317, 1374 (2007).
[CrossRef] [PubMed]

Hasegawa, H.

Hertlein, M. P.

J. van Tilborg, T. K. Allison, T. W. Wright, M. P. Hertlein, R. W. Falcone, Y. Liu, H. Merdji, and A. Belkacem, J. Phys. B 42, 081002 (2009).
[CrossRef]

T. K. Allison, J. van Tilborg, T. W. Wright, M. P. Hertlein, R. W. Falcone, and A. Belkacem, Opt. Express 17, 8941 (2009).
[CrossRef] [PubMed]

Kapteyn, H. C.

E. Gagnon, P. Ranitovic, X.-M. Tong, C. L. Cocke, M. M. Murnane, H. C. Kapteyn, and A. S. Sandhu, Science 317, 1374 (2007).
[CrossRef] [PubMed]

Khurmi, C.

T. K. Allison, H. Tao, T. W. Wright, A. M. Stooke, C. Khurmi, J. van Tilborg, Y. Liu, R. W. Falcone, T. J. Martinez, and A. Belkacem are preparing a manuscript to be called “Ultrafast internal conversion in ethylene.”

Kosma, K.

K. Kosma, S. A. Trushin, W. Fuss, and W. E. Schmid, J. Phys. Chem. A 112, 7514 (2008).
[CrossRef] [PubMed]

Krausz, F.

T. Brabec and F. Krausz, Rev. Mod. Phys. 72, 545 (2000).
[CrossRef]

Kruse, J.

A. Peralta Conde, J. Kruse, O. Faucher, P. Tzallas, E. P. Benis, and D. Charalambidis, Phys. Rev. A 79, 061405 (2009).
[CrossRef]

Lee, S.-H.

S.-H. Lee, Y. T. Lee, and X. Yang, J. Chem. Phys. 120, 10983 (2004).
[CrossRef] [PubMed]

Lee, Y. T.

S.-H. Lee, Y. T. Lee, and X. Yang, J. Chem. Phys. 120, 10983 (2004).
[CrossRef] [PubMed]

Levine, B. G.

H. Tao, B. G. Levine, and T. J. Martínez, J. Phys. Chem. A 113, 13656 (2009).
[CrossRef] [PubMed]

Liu, Y.

J. van Tilborg, T. K. Allison, T. W. Wright, M. P. Hertlein, R. W. Falcone, Y. Liu, H. Merdji, and A. Belkacem, J. Phys. B 42, 081002 (2009).
[CrossRef]

T. K. Allison, H. Tao, T. W. Wright, A. M. Stooke, C. Khurmi, J. van Tilborg, Y. Liu, R. W. Falcone, T. J. Martinez, and A. Belkacem are preparing a manuscript to be called “Ultrafast internal conversion in ethylene.”

Martinez, T. J.

T. K. Allison, H. Tao, T. W. Wright, A. M. Stooke, C. Khurmi, J. van Tilborg, Y. Liu, R. W. Falcone, T. J. Martinez, and A. Belkacem are preparing a manuscript to be called “Ultrafast internal conversion in ethylene.”

Martínez, T. J.

H. Tao, B. G. Levine, and T. J. Martínez, J. Phys. Chem. A 113, 13656 (2009).
[CrossRef] [PubMed]

Mashiko, H.

H. Mashiko, A. Suda, and K. Midorikawa, Appl. Phys. B. 87, 221 (2007).
[CrossRef]

Merdji, H.

J. van Tilborg, T. K. Allison, T. W. Wright, M. P. Hertlein, R. W. Falcone, Y. Liu, H. Merdji, and A. Belkacem, J. Phys. B 42, 081002 (2009).
[CrossRef]

Merer, A. J.

A. J. Merer and R. S. Mulliken, Chem. Rev. 69, 639 (1969).
[CrossRef]

Midorikawa, K.

Mulliken, R. S.

A. J. Merer and R. S. Mulliken, Chem. Rev. 69, 639 (1969).
[CrossRef]

Murnane, M. M.

E. Gagnon, P. Ranitovic, X.-M. Tong, C. L. Cocke, M. M. Murnane, H. C. Kapteyn, and A. S. Sandhu, Science 317, 1374 (2007).
[CrossRef] [PubMed]

Nabekawa, Y.

Papadogiannis, N. A.

P. Tzallas, D. Charalambidis, N. A. Papadogiannis, K. Witte, and G. D. Tsakiris, Nature 426, 267 (2003).
[CrossRef] [PubMed]

Ranitovic, P.

E. Gagnon, P. Ranitovic, X.-M. Tong, C. L. Cocke, M. M. Murnane, H. C. Kapteyn, and A. S. Sandhu, Science 317, 1374 (2007).
[CrossRef] [PubMed]

Sandhu, A. S.

E. Gagnon, P. Ranitovic, X.-M. Tong, C. L. Cocke, M. M. Murnane, H. C. Kapteyn, and A. S. Sandhu, Science 317, 1374 (2007).
[CrossRef] [PubMed]

Schmid, W. E.

S. A. Trushin, W. E. Schmid, and W. Fuss, Chem. Phys. Lett. 468, 9 (2009).
[CrossRef]

K. Kosma, S. A. Trushin, W. Fuss, and W. E. Schmid, J. Phys. Chem. A 112, 7514 (2008).
[CrossRef] [PubMed]

Stooke, A. M.

T. K. Allison, H. Tao, T. W. Wright, A. M. Stooke, C. Khurmi, J. van Tilborg, Y. Liu, R. W. Falcone, T. J. Martinez, and A. Belkacem are preparing a manuscript to be called “Ultrafast internal conversion in ethylene.”

Suda, A.

H. Mashiko, A. Suda, and K. Midorikawa, Appl. Phys. B. 87, 221 (2007).
[CrossRef]

Takahashi, E.

Tao, H.

H. Tao, B. G. Levine, and T. J. Martínez, J. Phys. Chem. A 113, 13656 (2009).
[CrossRef] [PubMed]

T. K. Allison, H. Tao, T. W. Wright, A. M. Stooke, C. Khurmi, J. van Tilborg, Y. Liu, R. W. Falcone, T. J. Martinez, and A. Belkacem are preparing a manuscript to be called “Ultrafast internal conversion in ethylene.”

Tong, X.-M.

E. Gagnon, P. Ranitovic, X.-M. Tong, C. L. Cocke, M. M. Murnane, H. C. Kapteyn, and A. S. Sandhu, Science 317, 1374 (2007).
[CrossRef] [PubMed]

Trushin, S. A.

S. A. Trushin, W. E. Schmid, and W. Fuss, Chem. Phys. Lett. 468, 9 (2009).
[CrossRef]

K. Kosma, S. A. Trushin, W. Fuss, and W. E. Schmid, J. Phys. Chem. A 112, 7514 (2008).
[CrossRef] [PubMed]

Tsakiris, G. D.

P. Tzallas, D. Charalambidis, N. A. Papadogiannis, K. Witte, and G. D. Tsakiris, Nature 426, 267 (2003).
[CrossRef] [PubMed]

Tzallas, P.

A. Peralta Conde, J. Kruse, O. Faucher, P. Tzallas, E. P. Benis, and D. Charalambidis, Phys. Rev. A 79, 061405 (2009).
[CrossRef]

P. Tzallas, D. Charalambidis, N. A. Papadogiannis, K. Witte, and G. D. Tsakiris, Nature 426, 267 (2003).
[CrossRef] [PubMed]

van Tilborg, J.

T. K. Allison, J. van Tilborg, T. W. Wright, M. P. Hertlein, R. W. Falcone, and A. Belkacem, Opt. Express 17, 8941 (2009).
[CrossRef] [PubMed]

J. van Tilborg, T. K. Allison, T. W. Wright, M. P. Hertlein, R. W. Falcone, Y. Liu, H. Merdji, and A. Belkacem, J. Phys. B 42, 081002 (2009).
[CrossRef]

T. K. Allison, H. Tao, T. W. Wright, A. M. Stooke, C. Khurmi, J. van Tilborg, Y. Liu, R. W. Falcone, T. J. Martinez, and A. Belkacem are preparing a manuscript to be called “Ultrafast internal conversion in ethylene.”

Witte, K.

P. Tzallas, D. Charalambidis, N. A. Papadogiannis, K. Witte, and G. D. Tsakiris, Nature 426, 267 (2003).
[CrossRef] [PubMed]

Wright, T. W.

T. K. Allison, J. van Tilborg, T. W. Wright, M. P. Hertlein, R. W. Falcone, and A. Belkacem, Opt. Express 17, 8941 (2009).
[CrossRef] [PubMed]

J. van Tilborg, T. K. Allison, T. W. Wright, M. P. Hertlein, R. W. Falcone, Y. Liu, H. Merdji, and A. Belkacem, J. Phys. B 42, 081002 (2009).
[CrossRef]

T. K. Allison, H. Tao, T. W. Wright, A. M. Stooke, C. Khurmi, J. van Tilborg, Y. Liu, R. W. Falcone, T. J. Martinez, and A. Belkacem are preparing a manuscript to be called “Ultrafast internal conversion in ethylene.”

Yang, X.

S.-H. Lee, Y. T. Lee, and X. Yang, J. Chem. Phys. 120, 10983 (2004).
[CrossRef] [PubMed]

Appl. Phys. B. (1)

H. Mashiko, A. Suda, and K. Midorikawa, Appl. Phys. B. 87, 221 (2007).
[CrossRef]

Chem. Phys. Lett. (1)

S. A. Trushin, W. E. Schmid, and W. Fuss, Chem. Phys. Lett. 468, 9 (2009).
[CrossRef]

Chem. Rev. (1)

A. J. Merer and R. S. Mulliken, Chem. Rev. 69, 639 (1969).
[CrossRef]

J. Chem. Phys. (1)

S.-H. Lee, Y. T. Lee, and X. Yang, J. Chem. Phys. 120, 10983 (2004).
[CrossRef] [PubMed]

J. Phys. B (1)

J. van Tilborg, T. K. Allison, T. W. Wright, M. P. Hertlein, R. W. Falcone, Y. Liu, H. Merdji, and A. Belkacem, J. Phys. B 42, 081002 (2009).
[CrossRef]

J. Phys. Chem. A (2)

K. Kosma, S. A. Trushin, W. Fuss, and W. E. Schmid, J. Phys. Chem. A 112, 7514 (2008).
[CrossRef] [PubMed]

H. Tao, B. G. Levine, and T. J. Martínez, J. Phys. Chem. A 113, 13656 (2009).
[CrossRef] [PubMed]

Nature (1)

P. Tzallas, D. Charalambidis, N. A. Papadogiannis, K. Witte, and G. D. Tsakiris, Nature 426, 267 (2003).
[CrossRef] [PubMed]

Opt. Express (1)

Opt. Lett. (1)

Phys. Rev. A (1)

A. Peralta Conde, J. Kruse, O. Faucher, P. Tzallas, E. P. Benis, and D. Charalambidis, Phys. Rev. A 79, 061405 (2009).
[CrossRef]

Rev. Mod. Phys. (1)

T. Brabec and F. Krausz, Rev. Mod. Phys. 72, 545 (2000).
[CrossRef]

Science (1)

E. Gagnon, P. Ranitovic, X.-M. Tong, C. L. Cocke, M. M. Murnane, H. C. Kapteyn, and A. S. Sandhu, Science 317, 1374 (2007).
[CrossRef] [PubMed]

Other (2)

T. K. Allison, “Femtosecond molecular dynamics studied with vacuum ultraviolet pulse pairs,” Ph.D. thesis (University of California at Berkeley, 2010).

T. K. Allison, H. Tao, T. W. Wright, A. M. Stooke, C. Khurmi, J. van Tilborg, Y. Liu, R. W. Falcone, T. J. Martinez, and A. Belkacem are preparing a manuscript to be called “Ultrafast internal conversion in ethylene.”

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Figures (3)

Fig. 1
Fig. 1

VUV/XUV pump–probe apparatus: high-order harmonics are recombined with a variable delay at the common focus of two spherical concave mirrors. Photoions are extracted from the focal region through a 500 μm pinhole with a strong electric field in the y direction.

Fig. 2
Fig. 2

Split-mirror foci spatial autocorrelation: multiphoton ionization of C 2 H 4 as a function of the overlap of the two SMI foci in the horizontal (top) and vertical (bottom) directions. Gaussian fits give a fifth-harmonic focus size of 4 μm × 12 μm .

Fig. 3
Fig. 3

Time-resolved photodissociation: (a) time-resolved OH + yield for H 2 O target gas. The OH + yield is fit with an error function fit (solid curve) to give an upper limit for the FIR of 44 10 + 15 fs FWHM. (b) Red points, H 2 + yield from C 2 H 4 ; red curve, exponential rise with 184 fs time constant; black points, C 2 H 4 + signal; black curve, adjacent point smoothed. Note the different x scales for (a) and (b).

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