Abstract

We present a single-shot detection technique for field-free molecular alignment. The method is based on probing the time-varying birefringence of an aligned sample by use of a chirped probe pulse, thus encoding the dependence of the alignment on time onto the spectral domain. The technique is applied to alignment of O2. The recorded signals are well described by an analytical formula.

© 2005 Optical Society of America

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  1. H. Stapelfeldt and T. Seideman, Rev. Mod. Phys. 75, 543 (2003).
    [Crossref]
  2. J. J. Larsen, H. Sakai, C. P. Safvan, I. Wendt-Larsen, and H. Stapelfeldt, J. Chem. Phys. 111, 7774 (1999).
    [Crossref]
  3. F. Rosca-Pruna and M. J.J. Vrakking, Phys. Rev. Lett. 87, 153902 (2001).
    [Crossref]
  4. E. Hertz, O. Faucher, B. Lavorel, F. Dalla Via, and R. Chaux, Phys. Rev. A 61, 033816 (2000).
    [Crossref]
  5. J. G. Underwood, M. Spanner, M. Y. Ivanov, J. Mottershead, B. J. Sussman, and A. Stolow, Phys. Rev. Lett. 90, 223001 (2003).
    [Crossref]
  6. C. H. Lin, J. P. Heritage, T. K. Gustafson, R. Y. Chiao, and J. P. McTague, Phys. Rev. A 13, 813 (1976).
    [Crossref]
  7. Z. Jiang and X.-C. Zhang, Appl. Phys. Lett. 72, 1945 (1998).
    [Crossref]
  8. I. Wilke, A. M. MacLeod, W. A. Gillespie, G. Berden, G. M.H. Knippels, and A. F.G. van der Meer, Phys. Rev. Lett. 88, 124801 (2002).
    [Crossref]
  9. K. W. DeLong and J. Yumoto, J. Opt. Soc. Am. B 9, 1593 (1992).
    [Crossref]
  10. T. Lang and M. Motzkus, J. Opt. Soc. Am. B 19, 340 (2002).
    [Crossref]
  11. M. Morgen, W. Price, L. Hunziker, P. Ludowize, M. Blackwell, and Y. Chen, Chem. Phys. Lett. 209, 1 (1993).
    [Crossref]
  12. B. Lavorel, O. Faucher, M. Morgen, and R. Chaux, J. Raman Spectrosc. 31, 77 (2000).
    [Crossref]
  13. V. Renard, M. Renard, S. Guérin, Y. T. Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, Phys. Rev. Lett. 90, 153601 (2003).
    [Crossref]

2003 (3)

H. Stapelfeldt and T. Seideman, Rev. Mod. Phys. 75, 543 (2003).
[Crossref]

J. G. Underwood, M. Spanner, M. Y. Ivanov, J. Mottershead, B. J. Sussman, and A. Stolow, Phys. Rev. Lett. 90, 223001 (2003).
[Crossref]

V. Renard, M. Renard, S. Guérin, Y. T. Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, Phys. Rev. Lett. 90, 153601 (2003).
[Crossref]

2002 (2)

T. Lang and M. Motzkus, J. Opt. Soc. Am. B 19, 340 (2002).
[Crossref]

I. Wilke, A. M. MacLeod, W. A. Gillespie, G. Berden, G. M.H. Knippels, and A. F.G. van der Meer, Phys. Rev. Lett. 88, 124801 (2002).
[Crossref]

2001 (1)

F. Rosca-Pruna and M. J.J. Vrakking, Phys. Rev. Lett. 87, 153902 (2001).
[Crossref]

2000 (2)

E. Hertz, O. Faucher, B. Lavorel, F. Dalla Via, and R. Chaux, Phys. Rev. A 61, 033816 (2000).
[Crossref]

B. Lavorel, O. Faucher, M. Morgen, and R. Chaux, J. Raman Spectrosc. 31, 77 (2000).
[Crossref]

1999 (1)

J. J. Larsen, H. Sakai, C. P. Safvan, I. Wendt-Larsen, and H. Stapelfeldt, J. Chem. Phys. 111, 7774 (1999).
[Crossref]

1998 (1)

Z. Jiang and X.-C. Zhang, Appl. Phys. Lett. 72, 1945 (1998).
[Crossref]

1993 (1)

M. Morgen, W. Price, L. Hunziker, P. Ludowize, M. Blackwell, and Y. Chen, Chem. Phys. Lett. 209, 1 (1993).
[Crossref]

1992 (1)

1976 (1)

C. H. Lin, J. P. Heritage, T. K. Gustafson, R. Y. Chiao, and J. P. McTague, Phys. Rev. A 13, 813 (1976).
[Crossref]

Berden, G.

I. Wilke, A. M. MacLeod, W. A. Gillespie, G. Berden, G. M.H. Knippels, and A. F.G. van der Meer, Phys. Rev. Lett. 88, 124801 (2002).
[Crossref]

Blackwell, M.

M. Morgen, W. Price, L. Hunziker, P. Ludowize, M. Blackwell, and Y. Chen, Chem. Phys. Lett. 209, 1 (1993).
[Crossref]

Chaux, R.

B. Lavorel, O. Faucher, M. Morgen, and R. Chaux, J. Raman Spectrosc. 31, 77 (2000).
[Crossref]

E. Hertz, O. Faucher, B. Lavorel, F. Dalla Via, and R. Chaux, Phys. Rev. A 61, 033816 (2000).
[Crossref]

Chen, Y.

M. Morgen, W. Price, L. Hunziker, P. Ludowize, M. Blackwell, and Y. Chen, Chem. Phys. Lett. 209, 1 (1993).
[Crossref]

Chiao, R. Y.

C. H. Lin, J. P. Heritage, T. K. Gustafson, R. Y. Chiao, and J. P. McTague, Phys. Rev. A 13, 813 (1976).
[Crossref]

DeLong, K. W.

Faucher, O.

V. Renard, M. Renard, S. Guérin, Y. T. Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, Phys. Rev. Lett. 90, 153601 (2003).
[Crossref]

B. Lavorel, O. Faucher, M. Morgen, and R. Chaux, J. Raman Spectrosc. 31, 77 (2000).
[Crossref]

E. Hertz, O. Faucher, B. Lavorel, F. Dalla Via, and R. Chaux, Phys. Rev. A 61, 033816 (2000).
[Crossref]

Gillespie, W. A.

I. Wilke, A. M. MacLeod, W. A. Gillespie, G. Berden, G. M.H. Knippels, and A. F.G. van der Meer, Phys. Rev. Lett. 88, 124801 (2002).
[Crossref]

Guérin, S.

V. Renard, M. Renard, S. Guérin, Y. T. Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, Phys. Rev. Lett. 90, 153601 (2003).
[Crossref]

Gustafson, T. K.

C. H. Lin, J. P. Heritage, T. K. Gustafson, R. Y. Chiao, and J. P. McTague, Phys. Rev. A 13, 813 (1976).
[Crossref]

Heritage, J. P.

C. H. Lin, J. P. Heritage, T. K. Gustafson, R. Y. Chiao, and J. P. McTague, Phys. Rev. A 13, 813 (1976).
[Crossref]

Hertz, E.

E. Hertz, O. Faucher, B. Lavorel, F. Dalla Via, and R. Chaux, Phys. Rev. A 61, 033816 (2000).
[Crossref]

Hunziker, L.

M. Morgen, W. Price, L. Hunziker, P. Ludowize, M. Blackwell, and Y. Chen, Chem. Phys. Lett. 209, 1 (1993).
[Crossref]

Ivanov, M. Y.

J. G. Underwood, M. Spanner, M. Y. Ivanov, J. Mottershead, B. J. Sussman, and A. Stolow, Phys. Rev. Lett. 90, 223001 (2003).
[Crossref]

Jauslin, H. R.

V. Renard, M. Renard, S. Guérin, Y. T. Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, Phys. Rev. Lett. 90, 153601 (2003).
[Crossref]

Jiang, Z.

Z. Jiang and X.-C. Zhang, Appl. Phys. Lett. 72, 1945 (1998).
[Crossref]

Knippels, G. M.H.

I. Wilke, A. M. MacLeod, W. A. Gillespie, G. Berden, G. M.H. Knippels, and A. F.G. van der Meer, Phys. Rev. Lett. 88, 124801 (2002).
[Crossref]

Lang, T.

Larsen, J. J.

J. J. Larsen, H. Sakai, C. P. Safvan, I. Wendt-Larsen, and H. Stapelfeldt, J. Chem. Phys. 111, 7774 (1999).
[Crossref]

Lavorel, B.

V. Renard, M. Renard, S. Guérin, Y. T. Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, Phys. Rev. Lett. 90, 153601 (2003).
[Crossref]

B. Lavorel, O. Faucher, M. Morgen, and R. Chaux, J. Raman Spectrosc. 31, 77 (2000).
[Crossref]

E. Hertz, O. Faucher, B. Lavorel, F. Dalla Via, and R. Chaux, Phys. Rev. A 61, 033816 (2000).
[Crossref]

Lin, C. H.

C. H. Lin, J. P. Heritage, T. K. Gustafson, R. Y. Chiao, and J. P. McTague, Phys. Rev. A 13, 813 (1976).
[Crossref]

Ludowize, P.

M. Morgen, W. Price, L. Hunziker, P. Ludowize, M. Blackwell, and Y. Chen, Chem. Phys. Lett. 209, 1 (1993).
[Crossref]

MacLeod, A. M.

I. Wilke, A. M. MacLeod, W. A. Gillespie, G. Berden, G. M.H. Knippels, and A. F.G. van der Meer, Phys. Rev. Lett. 88, 124801 (2002).
[Crossref]

McTague, J. P.

C. H. Lin, J. P. Heritage, T. K. Gustafson, R. Y. Chiao, and J. P. McTague, Phys. Rev. A 13, 813 (1976).
[Crossref]

Morgen, M.

B. Lavorel, O. Faucher, M. Morgen, and R. Chaux, J. Raman Spectrosc. 31, 77 (2000).
[Crossref]

M. Morgen, W. Price, L. Hunziker, P. Ludowize, M. Blackwell, and Y. Chen, Chem. Phys. Lett. 209, 1 (1993).
[Crossref]

Mottershead, J.

J. G. Underwood, M. Spanner, M. Y. Ivanov, J. Mottershead, B. J. Sussman, and A. Stolow, Phys. Rev. Lett. 90, 223001 (2003).
[Crossref]

Motzkus, M.

Pashayan, Y. T.

V. Renard, M. Renard, S. Guérin, Y. T. Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, Phys. Rev. Lett. 90, 153601 (2003).
[Crossref]

Price, W.

M. Morgen, W. Price, L. Hunziker, P. Ludowize, M. Blackwell, and Y. Chen, Chem. Phys. Lett. 209, 1 (1993).
[Crossref]

Renard, M.

V. Renard, M. Renard, S. Guérin, Y. T. Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, Phys. Rev. Lett. 90, 153601 (2003).
[Crossref]

Renard, V.

V. Renard, M. Renard, S. Guérin, Y. T. Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, Phys. Rev. Lett. 90, 153601 (2003).
[Crossref]

Rosca-Pruna, F.

F. Rosca-Pruna and M. J.J. Vrakking, Phys. Rev. Lett. 87, 153902 (2001).
[Crossref]

Safvan, C. P.

J. J. Larsen, H. Sakai, C. P. Safvan, I. Wendt-Larsen, and H. Stapelfeldt, J. Chem. Phys. 111, 7774 (1999).
[Crossref]

Sakai, H.

J. J. Larsen, H. Sakai, C. P. Safvan, I. Wendt-Larsen, and H. Stapelfeldt, J. Chem. Phys. 111, 7774 (1999).
[Crossref]

Seideman, T.

H. Stapelfeldt and T. Seideman, Rev. Mod. Phys. 75, 543 (2003).
[Crossref]

Spanner, M.

J. G. Underwood, M. Spanner, M. Y. Ivanov, J. Mottershead, B. J. Sussman, and A. Stolow, Phys. Rev. Lett. 90, 223001 (2003).
[Crossref]

Stapelfeldt, H.

H. Stapelfeldt and T. Seideman, Rev. Mod. Phys. 75, 543 (2003).
[Crossref]

J. J. Larsen, H. Sakai, C. P. Safvan, I. Wendt-Larsen, and H. Stapelfeldt, J. Chem. Phys. 111, 7774 (1999).
[Crossref]

Stolow, A.

J. G. Underwood, M. Spanner, M. Y. Ivanov, J. Mottershead, B. J. Sussman, and A. Stolow, Phys. Rev. Lett. 90, 223001 (2003).
[Crossref]

Sussman, B. J.

J. G. Underwood, M. Spanner, M. Y. Ivanov, J. Mottershead, B. J. Sussman, and A. Stolow, Phys. Rev. Lett. 90, 223001 (2003).
[Crossref]

Underwood, J. G.

J. G. Underwood, M. Spanner, M. Y. Ivanov, J. Mottershead, B. J. Sussman, and A. Stolow, Phys. Rev. Lett. 90, 223001 (2003).
[Crossref]

van der Meer, A. F.G.

I. Wilke, A. M. MacLeod, W. A. Gillespie, G. Berden, G. M.H. Knippels, and A. F.G. van der Meer, Phys. Rev. Lett. 88, 124801 (2002).
[Crossref]

Via, F. Dalla

E. Hertz, O. Faucher, B. Lavorel, F. Dalla Via, and R. Chaux, Phys. Rev. A 61, 033816 (2000).
[Crossref]

Vrakking, M. J.J.

F. Rosca-Pruna and M. J.J. Vrakking, Phys. Rev. Lett. 87, 153902 (2001).
[Crossref]

Wendt-Larsen, I.

J. J. Larsen, H. Sakai, C. P. Safvan, I. Wendt-Larsen, and H. Stapelfeldt, J. Chem. Phys. 111, 7774 (1999).
[Crossref]

Wilke, I.

I. Wilke, A. M. MacLeod, W. A. Gillespie, G. Berden, G. M.H. Knippels, and A. F.G. van der Meer, Phys. Rev. Lett. 88, 124801 (2002).
[Crossref]

Yumoto, J.

Zhang, X.-C.

Z. Jiang and X.-C. Zhang, Appl. Phys. Lett. 72, 1945 (1998).
[Crossref]

Appl. Phys. Lett. (1)

Z. Jiang and X.-C. Zhang, Appl. Phys. Lett. 72, 1945 (1998).
[Crossref]

Chem. Phys. Lett. (1)

M. Morgen, W. Price, L. Hunziker, P. Ludowize, M. Blackwell, and Y. Chen, Chem. Phys. Lett. 209, 1 (1993).
[Crossref]

J. Chem. Phys. (1)

J. J. Larsen, H. Sakai, C. P. Safvan, I. Wendt-Larsen, and H. Stapelfeldt, J. Chem. Phys. 111, 7774 (1999).
[Crossref]

J. Opt. Soc. Am. B (2)

J. Raman Spectrosc. (1)

B. Lavorel, O. Faucher, M. Morgen, and R. Chaux, J. Raman Spectrosc. 31, 77 (2000).
[Crossref]

Phys. Rev. A (2)

E. Hertz, O. Faucher, B. Lavorel, F. Dalla Via, and R. Chaux, Phys. Rev. A 61, 033816 (2000).
[Crossref]

C. H. Lin, J. P. Heritage, T. K. Gustafson, R. Y. Chiao, and J. P. McTague, Phys. Rev. A 13, 813 (1976).
[Crossref]

Phys. Rev. Lett. (4)

I. Wilke, A. M. MacLeod, W. A. Gillespie, G. Berden, G. M.H. Knippels, and A. F.G. van der Meer, Phys. Rev. Lett. 88, 124801 (2002).
[Crossref]

J. G. Underwood, M. Spanner, M. Y. Ivanov, J. Mottershead, B. J. Sussman, and A. Stolow, Phys. Rev. Lett. 90, 223001 (2003).
[Crossref]

F. Rosca-Pruna and M. J.J. Vrakking, Phys. Rev. Lett. 87, 153902 (2001).
[Crossref]

V. Renard, M. Renard, S. Guérin, Y. T. Pashayan, B. Lavorel, O. Faucher, and H. R. Jauslin, Phys. Rev. Lett. 90, 153601 (2003).
[Crossref]

Rev. Mod. Phys. (1)

H. Stapelfeldt and T. Seideman, Rev. Mod. Phys. 75, 543 (2003).
[Crossref]

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Figures (4)

Fig. 1
Fig. 1

Experimental setup: The pump and probe beams are separated by a beam splitter. The polarization of the probe beam is set at 45° with respect to the pump beam and is stretched in a double-pass two-grating setup. Next, it passes through a sequence of two crossed polarizers placed before and after a 1 m long cell filled with O 2 at a pressure of 1500 Torr. The pump and probe beams are focused and overlapped in the cell, and the part of the probe beam that is transmitted by the second polarizer as a result of the birefringence of the molecular sample is spectrally resolved.

Fig. 2
Fig. 2

(a) Time–wavelength contour plot showing the spectrum of the probe beam that is transmitted through two crossed polarizers as a result of the birefringence of the molecular sample, as a function of the delay between the pump laser pulse and the chirped probe pulse. For further details, see text. (b) Signal transmitted at 800 nm as a function of the pump–probe delay. (c) Spectrum of the probe beam at a pump–probe delay of 8.8 ps.

Fig. 3
Fig. 3

(a) Experimental and (b) theoretical time–wavelength contour plots, showing the spectrum of the transmitted probe laser pulse as a function of the pump–probe time delay. (c) Experimental and simulated signals at 800 nm as a function of the pump–probe delay.

Fig. 4
Fig. 4

Experimental spectra for pump–probe delays of (a) 2.9 and (b) 8.8 ps, where the wavelength scale has been converted to a time scale according to τ = τ + π c α λ (see text). (c), (d) Corresponding revival structures as observed by monitoring the signal at 800 nm as a function of the pump–probe delay.

Equations (6)

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E s ( t τ ) E c ( t τ ) l E p ( t ) 2 χ ( t t ) d t ,
χ ( t t ) J ( ρ J ρ J ) g J ( J + 1 ) ( J + 2 ) 2 J + 3 sin [ ω J ( t t ) ] exp [ γ J ( t t ) ] .
I ( ω , τ ) = + d t [ E s ( t τ ) + ϵ E c ( t τ ) ] exp ( i ω t ) 2 .
I ( ω , τ ) J g J ( ρ J ρ J ) ( J + 1 ) ( J + 2 ) ( 2 J + 3 ) [ A ( ω J ) A ( ω J ) ] + ϵ E ̃ ( ω ) 2 ,
A ( ω J ) = exp [ ( ω c Ω J ω ) 2 4 β + i Ω J τ τ p 2 Ω J 2 8 ]
× ( 1 ϕ { i Ω J ( β τ p 2 + 2 ) + 2 i ( ω c ω ) 2 β τ 2 [ 2 β ( β τ p 2 + 2 ) ] 1 2 } ) ,

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