Abstract

We have developed a new instrument for monitoring electronic wavepacket dynamics using a single electromagnetic pulse pair. The operation of the device is analogous to that of single-shot cross-correlators commonly used to monitor the temporal evolution of short laser pulses. We have used the instrument to probe wavepacket evolution over time scales ranging from 100 psec to less than 1 fsec. The device reduces the amount of time required to collect pump-probe time delay data by orders of magnitude, greatly reducing the deleterious effects of experimental drifts. In addition, the single-shot feature provides real-time feedback as to the affect of various experimental parameters on the electron dynamics, allowing us to literally tune-up our equipment to enhance desired behavior at specific times.

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References

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  1. R.R. Jones and L.D. Noordam, "Electronic Wavepackets," in Adv. At. Mol. Opt. Phys., Vol. 38 (in press).
  2. L.D. Noordam and R.R. Jones, "Probing Rydberg Electron Dynamics," J. Mod. Optics (in press).
  3. N.F. Scherer, A.J. Ruggiero, M. Du, and G.R. Fleming, "Time resolved dynamics of isolated molecular systems studied with phase-locked femtosecond pulse pairs," J. Chem. Phys. 93, 856 (1990).
    [CrossRef]
  4. N.F. Scherer, R.J. Carlson, R.J. Matro, M. Du, A.J. Ruggiero, V. Romero-Rochin, J.A. Cina, G.R. Fleming, and S.A. Rice, "Fluoresence-detected wave packet interferometry: Time resolved molecular spectroscopy with sequences of femtosecond phase-locked pulses," J. Chem. Phys. 95, 1487 (1991).
    [CrossRef]
  5. L.D. Noordam, D.I. Duncan, and T.F. Gallagher, "Ramsey fringes in atomic Rydberg wave packets," Phys. Rev. A 45, 4734 (1992).
    [CrossRef] [PubMed]
  6. B. Broers, J.F. Christian, J.H. Hoogenraad, W.J. van der Zande, H.B. van Linden van den Heuvell, and L.D. Noordam, "Time-resolved dynamics of electronic wavepackets above the classical field-ionization threshold," Phys. Rev. Lett. 71, 344 (1993).
    [CrossRef] [PubMed]
  7. R.R. Jones, D.W. Schumacher, T.F. Gallager, and P.H. Bucksbaum, "Bound-state interferometry using incoherent light," J. Phys. B 28, 405 (1995).
    [CrossRef]
  8. R.R. Jones, "Creating and Probing Electronic Wave Packets Using Half-Cycle Pulses," Phys. Rev. Lett. 76, 3927-3930 (1996).
    [CrossRef] [PubMed]
  9. D. You, R.R. Jones, and P.H. Bucksbaum, "Generation of high-power sub-single-cycle 500 fs electromagnetic pulses," Opt. Lett. 18, 290 (1993).
    [CrossRef] [PubMed]
  10. R.R. Jones, D. You, and P.H. Bucksbaum, "Ionization of Rydberg atoms by subpicosecond half-cycle electromagnetic pulses," Phys. Rev. Lett. 70, 1236 (1993).
    [CrossRef] [PubMed]
  11. C. Raman, C.W.S. Conover, C.I. Sukenik, and P.H. Bucksbaum, "Ionization of Rydberg Wave Packets by Subpicosecond, Half-Cycle Electromagnetic Pulses," Phys. Rev. Lett. 76, 2436-2439 (1996).
    [CrossRef] [PubMed]

Other

R.R. Jones and L.D. Noordam, "Electronic Wavepackets," in Adv. At. Mol. Opt. Phys., Vol. 38 (in press).

L.D. Noordam and R.R. Jones, "Probing Rydberg Electron Dynamics," J. Mod. Optics (in press).

N.F. Scherer, A.J. Ruggiero, M. Du, and G.R. Fleming, "Time resolved dynamics of isolated molecular systems studied with phase-locked femtosecond pulse pairs," J. Chem. Phys. 93, 856 (1990).
[CrossRef]

N.F. Scherer, R.J. Carlson, R.J. Matro, M. Du, A.J. Ruggiero, V. Romero-Rochin, J.A. Cina, G.R. Fleming, and S.A. Rice, "Fluoresence-detected wave packet interferometry: Time resolved molecular spectroscopy with sequences of femtosecond phase-locked pulses," J. Chem. Phys. 95, 1487 (1991).
[CrossRef]

L.D. Noordam, D.I. Duncan, and T.F. Gallagher, "Ramsey fringes in atomic Rydberg wave packets," Phys. Rev. A 45, 4734 (1992).
[CrossRef] [PubMed]

B. Broers, J.F. Christian, J.H. Hoogenraad, W.J. van der Zande, H.B. van Linden van den Heuvell, and L.D. Noordam, "Time-resolved dynamics of electronic wavepackets above the classical field-ionization threshold," Phys. Rev. Lett. 71, 344 (1993).
[CrossRef] [PubMed]

R.R. Jones, D.W. Schumacher, T.F. Gallager, and P.H. Bucksbaum, "Bound-state interferometry using incoherent light," J. Phys. B 28, 405 (1995).
[CrossRef]

R.R. Jones, "Creating and Probing Electronic Wave Packets Using Half-Cycle Pulses," Phys. Rev. Lett. 76, 3927-3930 (1996).
[CrossRef] [PubMed]

D. You, R.R. Jones, and P.H. Bucksbaum, "Generation of high-power sub-single-cycle 500 fs electromagnetic pulses," Opt. Lett. 18, 290 (1993).
[CrossRef] [PubMed]

R.R. Jones, D. You, and P.H. Bucksbaum, "Ionization of Rydberg atoms by subpicosecond half-cycle electromagnetic pulses," Phys. Rev. Lett. 70, 1236 (1993).
[CrossRef] [PubMed]

C. Raman, C.W.S. Conover, C.I. Sukenik, and P.H. Bucksbaum, "Ionization of Rydberg Wave Packets by Subpicosecond, Half-Cycle Electromagnetic Pulses," Phys. Rev. Lett. 76, 2436-2439 (1996).
[CrossRef] [PubMed]

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Figures (4)

Figure 1.
Figure 1.

Operation schematic for a single-shot detector.

Figure 2.
Figure 2.

Schematic of the single-shot detector.

Figure 3.
Figure 3.

CCD image of the spatial distribution of the field ionization signal from a Rydberg wavepacket probed using bound-state interferometry in the single-shot configuration. The ion distribution reflects the temporal wavepacket interference. The period of the observed fringes is 1.3 fsec.

Figure 4.
Figure 4.

Single-shot image of wavepacket evolution obtained using a HCP probe in the counter-propagating beam geometry. The pump-probe delay increases from left to right and the interval across the full image is approximately 60 psec. The lower curve shows the intensity level integrated over the vertical axis in the image. Zero delay is near the left edge of the Figure.

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