Wave-packet dynamics in the Li2 E(1Σ g +) shelf state: Simultaneous observation of vibrational and rotational recurrences with single rovibronic control of an intermediate state

John M. Papanikolas*, Richard M. Williams, Paul D. Kleiber, Jeffrey L. Hart, Carsten Brink, Stephen D. Price, Stephen R. Leone

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Resumé

A three-step excitation sequence is used to study the wave-packet dynamics in the E(1 Σg +) "shelf" state of lithium dimer. In the first excitation step, a continuous wave (cw) dye laser prepares a single rovibrational level (v=14, J=22) in the intermediate 7Li 2 A (1 Σu +) state. Ultrafast excitation of this single level with a 200 fs laser pulse centered at 803 nm creates a rovibrational wave packet (v=13-16; J=21 and 23) in the shelf region of the E(1Σg +) state. The motion of this three-dimensional wave packet is probed via ionization by a second ultrafast laser pulse of the same color. The initial cw excitation step allows precise control of the states that compose the wave packet. Fourier analysis of the pump-probe transients shows 15 frequency components that correspond to energy differences between the levels that constitute the wave packet. Because of the large rotational energy splitting, the rotational beats occur in the same frequency range as the vibrational beats. Experiments performed with parallel and perpendicular pump-probe polarizations provide a "magic angle" transient in which only the pure vibrational beats are observed, thus aiding in the spectroscopic assignment. The observed beat frequencies agree well with conventional high resolution frequency-domain spectroscopy. Applications of the intermediate-state control of the initial wave packet are discussed.

OriginalsprogEngelsk
TidsskriftThe Journal of Chemical Physics
Vol/bind103
Udgave nummer17
Sider (fra-til)7269-7276
Antal sider8
ISSN0021-9606
DOI
StatusUdgivet - 1. jan. 1995

Fingeraftryk

Wave packets
shelves
wave packets
synchronism
Laser pulses
Pumps
pumps
excitation
Ultrafast lasers
beat frequencies
Continuous wave lasers
Dye lasers
Fourier analysis
probes
wave excitation
continuous wave lasers
pulses
Lithium
dye lasers
Dimers

Citer dette

Papanikolas, John M. ; Williams, Richard M. ; Kleiber, Paul D. ; Hart, Jeffrey L. ; Brink, Carsten ; Price, Stephen D. ; Leone, Stephen R. / Wave-packet dynamics in the Li2 E(1Σ g +) shelf state : Simultaneous observation of vibrational and rotational recurrences with single rovibronic control of an intermediate state. I: The Journal of Chemical Physics. 1995 ; Bind 103, Nr. 17. s. 7269-7276.
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title = "Wave-packet dynamics in the Li2 E(1Σ g +) shelf state: Simultaneous observation of vibrational and rotational recurrences with single rovibronic control of an intermediate state",
abstract = "A three-step excitation sequence is used to study the wave-packet dynamics in the E(1 Σg +) {"}shelf{"} state of lithium dimer. In the first excitation step, a continuous wave (cw) dye laser prepares a single rovibrational level (v=14, J=22) in the intermediate 7Li 2 A (1 Σu +) state. Ultrafast excitation of this single level with a 200 fs laser pulse centered at 803 nm creates a rovibrational wave packet (v=13-16; J=21 and 23) in the shelf region of the E(1Σg +) state. The motion of this three-dimensional wave packet is probed via ionization by a second ultrafast laser pulse of the same color. The initial cw excitation step allows precise control of the states that compose the wave packet. Fourier analysis of the pump-probe transients shows 15 frequency components that correspond to energy differences between the levels that constitute the wave packet. Because of the large rotational energy splitting, the rotational beats occur in the same frequency range as the vibrational beats. Experiments performed with parallel and perpendicular pump-probe polarizations provide a {"}magic angle{"} transient in which only the pure vibrational beats are observed, thus aiding in the spectroscopic assignment. The observed beat frequencies agree well with conventional high resolution frequency-domain spectroscopy. Applications of the intermediate-state control of the initial wave packet are discussed.",
author = "Papanikolas, {John M.} and Williams, {Richard M.} and Kleiber, {Paul D.} and Hart, {Jeffrey L.} and Carsten Brink and Price, {Stephen D.} and Leone, {Stephen R.}",
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Wave-packet dynamics in the Li2 E(1Σ g +) shelf state : Simultaneous observation of vibrational and rotational recurrences with single rovibronic control of an intermediate state. / Papanikolas, John M.; Williams, Richard M.; Kleiber, Paul D.; Hart, Jeffrey L.; Brink, Carsten; Price, Stephen D.; Leone, Stephen R.

I: The Journal of Chemical Physics, Bind 103, Nr. 17, 01.01.1995, s. 7269-7276.

Publikation: Bidrag til tidsskriftTidsskriftartikelForskningpeer review

TY - JOUR

T1 - Wave-packet dynamics in the Li2 E(1Σ g +) shelf state

T2 - Simultaneous observation of vibrational and rotational recurrences with single rovibronic control of an intermediate state

AU - Papanikolas, John M.

AU - Williams, Richard M.

AU - Kleiber, Paul D.

AU - Hart, Jeffrey L.

AU - Brink, Carsten

AU - Price, Stephen D.

AU - Leone, Stephen R.

PY - 1995/1/1

Y1 - 1995/1/1

N2 - A three-step excitation sequence is used to study the wave-packet dynamics in the E(1 Σg +) "shelf" state of lithium dimer. In the first excitation step, a continuous wave (cw) dye laser prepares a single rovibrational level (v=14, J=22) in the intermediate 7Li 2 A (1 Σu +) state. Ultrafast excitation of this single level with a 200 fs laser pulse centered at 803 nm creates a rovibrational wave packet (v=13-16; J=21 and 23) in the shelf region of the E(1Σg +) state. The motion of this three-dimensional wave packet is probed via ionization by a second ultrafast laser pulse of the same color. The initial cw excitation step allows precise control of the states that compose the wave packet. Fourier analysis of the pump-probe transients shows 15 frequency components that correspond to energy differences between the levels that constitute the wave packet. Because of the large rotational energy splitting, the rotational beats occur in the same frequency range as the vibrational beats. Experiments performed with parallel and perpendicular pump-probe polarizations provide a "magic angle" transient in which only the pure vibrational beats are observed, thus aiding in the spectroscopic assignment. The observed beat frequencies agree well with conventional high resolution frequency-domain spectroscopy. Applications of the intermediate-state control of the initial wave packet are discussed.

AB - A three-step excitation sequence is used to study the wave-packet dynamics in the E(1 Σg +) "shelf" state of lithium dimer. In the first excitation step, a continuous wave (cw) dye laser prepares a single rovibrational level (v=14, J=22) in the intermediate 7Li 2 A (1 Σu +) state. Ultrafast excitation of this single level with a 200 fs laser pulse centered at 803 nm creates a rovibrational wave packet (v=13-16; J=21 and 23) in the shelf region of the E(1Σg +) state. The motion of this three-dimensional wave packet is probed via ionization by a second ultrafast laser pulse of the same color. The initial cw excitation step allows precise control of the states that compose the wave packet. Fourier analysis of the pump-probe transients shows 15 frequency components that correspond to energy differences between the levels that constitute the wave packet. Because of the large rotational energy splitting, the rotational beats occur in the same frequency range as the vibrational beats. Experiments performed with parallel and perpendicular pump-probe polarizations provide a "magic angle" transient in which only the pure vibrational beats are observed, thus aiding in the spectroscopic assignment. The observed beat frequencies agree well with conventional high resolution frequency-domain spectroscopy. Applications of the intermediate-state control of the initial wave packet are discussed.

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