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Tuesday, 30 October 2012

Tuesday, 2 October 2012

Seb: Oriented Rotational Wave-Packet Dynamics Studies via High Harmonic Generation


Phys. Rev. Lett. 109, 113901 (2012) [5 pages]

Oriented Rotational Wave-Packet Dynamics Studies via High Harmonic Generation

Abstract
No Citing Articles
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E. Frumker1,2,3,*C. T. Hebeisen1N. Kajumba1,4J. B. Bertrand1H. J. Wörner1,5M. Spanner6D. M. Villeneuve1A. Naumov1, and P. B. Corkum1,†
1Joint Attosecond Science Laboratory, University of Ottawa and National Research Council of Canada, 100 Sussex Drive, Ottawa, ON K1A 0R6, Canada
2Max-Planck-Institut für Quantenoptik, Hans-Kopfermann-Strasse 1, D-85748 Garching, Germany
3Department of Physics, Texas A&M University, College Station,Texas 77843, USA
4Department für Physik der Ludwig-Maximilians-Universität, Schellingstrasse 4, D-80799 Munich, Germany
5Laboratorium für physikalische Chemie, ETH Zürich, Wolfgang-Pauli-Strasse 10, 8093 Zürich, Switzerland
6Steacie Institute for Molecular Sciences, National Research Council of Canada, Ottawa, ON K1A 0R6, Canada
Received 12 April 2012; published 12 September 2012
We produce oriented rotational wave packets in CO and measure their characteristics via high harmonic generation. The wave packet is created using an intense, femtosecond laser pulse and its second harmonic. A delayed 800 nm pulse probes the wave packet, generating even-order high harmonics that arise from the broken symmetry induced by the orientation dynamics. The even-order harmonic radiation that we measure appears on a zero background, enabling us to accurately follow the temporal evolution of the wave packet. Our measurements reveal that, for the conditions optimum for harmonic generation, the orientation is produced by preferential ionization which depletes the sample of molecules of one orientation.
Published by the American Physical Society
URL:
http://link.aps.org/doi/10.1103/PhysRevLett.109.113901
DOI:
10.1103/PhysRevLett.109.113901
PACS:
42.65.Ky, 07.57.-c

Tuesday, 25 September 2012

Simon:Wave packet theory of dynamic absorption spectra in femtosecond pump–probe experiments


J. Chem. Phys. 92, 4012 (1990); http://dx.doi.org/10.1063/1.457815 (18 pages)

Wave packet theory of dynamic absorption spectra in femtosecond pump–probe experiments

W. Thomas PollardSoo‐Y. Lee, and Richard A. Mathies
Department of Chemistry, University of California, Berkeley, California 94720 
(Received 18 July 1989; accepted 8 December 1989)

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The large spectral width of ultrashort optical pulses makes it possible to measure the complete time‐resolved absorption spectrum of a sample with a single pulse, offering simultaneously high resolution in both the time and frequency domains. To quantitatively interpret these experiments, we start with the usual perturbative density matrix theory for the third‐order susceptibility of a multilevel system. However, the theory is formulated in terms of four‐time correlation functions which are interpreted as the time‐dependent overlap of bra and ket vibrational wave packets propagating independently on the ground and excited electronic state potential surfaces. This approach captures the critical distinction between electronic population decay and pure dephasing processes, while retaining the intuitive physical picture offered by the time‐dependent wave packet theories of molecular spectroscopy. A useful simplification is achieved by considering the absorption of the probe pulse as the firstorder spectroscopy of the nonstationary state created by the pump pulse. In this case, the dynamic spectrum is obtained through the Fourier transform of the time‐dependent overlap of the initial wave packet propagating on its potential surface and a second wave packet, created by the probe pulse, which evolves simultaneously on the final surface. Calculations for model systems using harmonic surfaces and δ‐function pulses are presented to illustrate the application of this theory and to clarify the unique spectral behavior of the nonstationary states created in femtosecond pump–probe experiments. Finally, we demonstrate the practical application of the theory for anharmonic surfaces and finite pulses by analyzing the dynamic spectroscopy of the excited state torsional isomerization of the bacteriorhodopsin chromophore.

Tuesday, 18 September 2012

Sebastien: Attosecond Control of Orbital Parity Mix Interferences and the Relative Phase of Even and Odd Harmonics in an Attosecond Pulse Train


Phys. Rev. Lett. 109, 083001 (2012) [5 pages]

Attosecond Control of Orbital Parity Mix Interferences and the Relative Phase of Even and Odd Harmonics in an Attosecond Pulse Train

Abstract
No Citing Articles
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G. Laurent*W. CaoH. LiZ. WangI. Ben-Itzhak, and C. L. Cocke
Physics Department, James R. Macdonald Laboratory, Kansas State University, Manhattan, Kansas 66506, USA
Received 19 March 2012; published 20 August 2012
We experimentally demonstrate that atomic orbital parity mix interferences can be temporally controlled on an attosecond time scale. Electron wave packets are formed by ionizing argon gas with a comb of odd and even high-order harmonics, in the presence of a weak infrared field. Consequently, a mix of energy-degenerate even and odd parity states is fed in the continuum by one- and two-photon transitions. These interfere, leading to an asymmetric electron emission along the polarization vector. The direction of the emission can be controlled by varying the time delay between the comb and infrared field pulses. We show that such asymmetric emission provides information on the relative phase of consecutive odd and even order harmonics in the attosecond pulse train.
© 2012 American Physical Society
URL:
http://link.aps.org/doi/10.1103/PhysRevLett.109.083001
DOI:
10.1103/PhysRevLett.109.083001
PACS:
32.80.Rm, 32.80.Qk, 42.65.Ky