Physical Review Letters

Efficient coherent population transfer in NO molecules using pulsed lasers

S. Schiemann, Axel Kuhn, S. Steuerwald, Klaas Bergmann

Published Nov 29, 1993• 214 citations

Abstract

Highly efficient and selective population transfer in NO molecules in the electronic ground state (${\mathit{X}}^{2}$${\mathrm{\ensuremath{\Pi}}}_{1/2}$) from the vibrational level v''=0 to the level v''=6 is demonstrated. It shows, for the first time with pulsed lasers, that a rather generally applicable scheme for complete control over the level population in atoms and molecules is now available. The efficiency relies on a counterintuitive interaction sequence of two lasers with the molecule in a process of stimulated Raman scattering involving adiabatic passage.

DOI: 10.1103/physrevlett.71.3637

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Efficient coherent population transfer in NO-molecules using pulsed lasers

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Highly efficient and selective population transfer in NO molecules in the electronic ground state (X2Π1/2) from the vibrational level v‘=0 to the level v‘=6 is demonstrated. A rather generally applicable scheme for complete control over the level population in atoms and molecules is now available. The efficiency relies on a counter‐intuitive interaction sequence of two lasers with the molecule in a process of stimulated Raman scattering involving adiabatic passage (STIRAP).

AIP conference proceedingsJan 1, 19951 citation

Population transfer by stimulated Raman scattering with delayed pulses: the concept, some problems, and experimental demonstration

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Coherent population transfer and dark resonances in SO2

Thomas Halfmann, K. Bergmann

Highly efficient population transfer between the (0,0,0) and the (9,1,0) vibrational levels of the electronic ground state X̃ 1A1 of SO2 is demonstrated. The process relies on stimulated Raman scattering with adiabatic passage induced by two suitably delayed ultraviolet laser pulses with nearly transform-limited bandwidth. A transfer efficiency of 100% is achieved. The associated dark resonance is observed. Properties of the latter are compared for delayed and fully overlapping pulses.

The Journal of Chemical PhysicsMay 8, 199692 citations

Physical Review Letters

Efficient coherent population transfer in NO molecules using pulsed lasers

S. Schiemann, Axel Kuhn, S. Steuerwald, Klaas Bergmann

Published Nov 29, 1993• 214 citations

Publisher

Abstract

Highly efficient and selective population transfer in NO molecules in the electronic ground state (

{\mathit{X}}^{2}$${\mathrm{\ensuremath{\Pi}}}_{1/2}

) from the vibrational level v''=0 to the level v''=6 is demonstrated. It shows, for the first time with pulsed lasers, that a rather generally applicable scheme for complete control over the level population in atoms and molecules is now available. The efficiency relies on a counterintuitive interaction sequence of two lasers with the molecule in a process of stimulated Raman scattering involving adiabatic passage.

DOI: 10.1103/physrevlett.71.3637

Related papers

Efficient coherent population transfer in NO-molecules using pulsed lasers

S. Steuerwald, S. Schiemann, Axel Kuhn +1 more

AIP conference proceedingsJan 1, 19951 citation

Population transfer by stimulated Raman scattering with delayed pulses: the concept, some problems, and experimental demonstration

Klaas Bergmann, S. Schiemann, Andreas Kuhn

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIEApr 1, 19920 citations

Population transfer between molecular vibrational levels by stimulated Raman scattering with partially overlapping laser fields. A new concept and experimental results

U. Gaubatz, P. Rudecki, S. Schiemann +1 more

The feasibility of a novel technique for efficient and selective population transfer from a thermally populated level 1 via an intermediate state 2 to level 3 is experimentally demonstrated. It is shown for sodium dimers that the process of on- or near-resonance stimulated Raman scattering with only partially overlapping laser beams is, in particular, useful for the selective population of high vibrational levels of particles in a molecular beam. This is achieved when the interaction with the Stokes laser, coupling levels 2 and 3, begins earlier than the interaction with the pump laser. The phenomenon, which is closely related to the formation of ‘‘trapped states,’’ is quantitatively explained using the basis of eigenstates of molecules strongly coupled to the radiation fields. The similarity and difference to related techniques such as rapid adiabatic passage phenomena in two-level systems, off-resonant stimulated Raman scattering, or stimulated emission pumping is briefly discussed.The feasibility of a novel technique for efficient and selective population transfer from a thermally populated level 1 via an intermediate state 2 to level 3 is experimentally demonstrated. It is shown for sodium dimers that the process of on- or near-resonance stimulated Raman scattering with only partially overlapping laser beams is, in particular, useful for the selective population of high vibrational levels of particles in a molecular beam. This is achieved when the interaction with the Stokes laser, coupling levels 2 and 3, begins earlier than the interaction with the pump laser. The phenomenon, which is closely related to the formation of ‘‘trapped states,’’ is quantitatively explained using the basis of eigenstates of molecules strongly coupled to the radiation fields. The similarity and difference to related techniques such as rapid adiabatic passage phenomena in two-level systems, off-resonant stimulated Raman scattering, or stimulated emission pumping is briefly discussed.

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Klaas Bergmann

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Bulletin of the American Physical SocietyMay 1, 19930 citations

Coherent control of vibrational population transfer in the Li2 molecule with femtosecond laser pulses in the presence of manifolds of rotational levels

Chitrakshya Sarkar, Santanu Bhattacharyya, Samir Saha

We have theoretically investigated the vibrational population transfer in the presence of manifolds of rotational levels in a model 15-level ${\text{Li}}_{2}$ molecular system by stimulated Raman adiabatic passage with intense unchirped femtosecond laser pulses. We have considered five rotational levels ${J}_{g}=0,2,\dots{},8$ associated with the initial vibrational level ${v}_{g}=0$ of the ground electronic state $X\text{ }{^{1}\ensuremath{\Sigma}}_{g}^{+}$, five rotational levels ${J}_{i}=1,3,\dots{},9$ associated with the vibrational level ${v}_{i}=1$ of the intermediate excited electronic state $A\text{ }{^{1}\ensuremath{\Sigma}}_{u}^{+}$, and five rotational levels ${J}_{f}=0,2,\dots{},8$ associated with the final target vibrational levels ${v}_{f}=1,2$ of the $X\text{ }{^{1}\ensuremath{\Sigma}}_{g}^{+}$ state of the ${\text{Li}}_{2}$ alkali dimer. The pump and Stokes laser pulses are taken to have the same temporal (Gaussian) shapes, pulse widths, and linear parallel polarizations. The laser wavelengths are in the (visible) range of 700--740 nm. The (peak) intensities of the pulses are of the order of $1\ifmmode\times\else\texttimes\fi{}{10}^{12}--2.5\ifmmode\times\else\texttimes\fi{}{10}^{13}\text{ }\text{W}/{\text{cm}}^{2}$ and the pulse widths are of the order of 20--50 fs. We have solved the 15 coupled time-dependent Schr\"odinger equations to study the population transfer to the target-excited vibrational levels. We have observed that, even with ``mushrooming'' of closely spaced rotational levels, efficient and selective population transfer to excited vibrational levels in ${\text{Li}}_{2}$ alkali dimer can be achieved for counterintuitive pulse sequence by controlling the pump and Stokes laser parameters. We have endeavored to explain the results within the framework of adiabatic picture.We have theoretically investigated the vibrational population transfer in the presence of manifolds of rotational levels in a model 15-level ${\text{Li}}_{2}$ molecular system by stimulated Raman adiabatic passage with intense unchirped femtosecond laser pulses. We have considered five rotational levels ${J}_{g}=0,2,\dots{},8$ associated with the initial vibrational level ${v}_{g}=0$ of the ground electronic state $X\text{ }{^{1}\ensuremath{\Sigma}}_{g}^{+}$, five rotational levels ${J}_{i}=1,3,\dots{},9$ associated with the vibrational level ${v}_{i}=1$ of the intermediate excited electronic state $A\text{ }{^{1}\ensuremath{\Sigma}}_{u}^{+}$, and five rotational levels ${J}_{f}=0,2,\dots{},8$ associated with the final target vibrational levels ${v}_{f}=1,2$ of the $X\text{ }{^{1}\ensuremath{\Sigma}}_{g}^{+}$ state of the ${\text{Li}}_{2}$ alkali dimer. The pump and Stokes laser pulses are taken to have the same temporal (Gaussian) shapes, pulse widths, and linear parallel polarizations. The laser wavelengths are in the (visible) range of 700--740 nm. The (peak) intensities of the pulses are of the order of $1\ifmmode\times\else\texttimes\fi{}{10}^{12}--2.5\ifmmode\times\else\texttimes\fi{}{10}^{13}\text{ }\text{W}/{\text{cm}}^{2}$ and the pulse widths are of the order of 20--50 fs. We have solved the 15 coupled time-dependent Schr\"odinger equations to study the population transfer to the target-excited vibrational levels. We have observed that, even with ``mushrooming'' of closely spaced rotational levels, efficient and selective population transfer to excited vibrational levels in ${\text{Li}}_{2}$ alkali dimer can be achieved for counterintuitive pulse sequence by controlling the pump and Stokes laser parameters. We have endeavored to explain the results within the framework of adiabatic picture.

Physical Review AAug 11, 20093 citations

Coherent population transfer and dark resonances in SO2

Thomas Halfmann, K. Bergmann

The Journal of Chemical PhysicsMay 8, 199692 citations

We have theoretically investigated the vibrational population transfer in the presence of manifolds of rotational levels in a model 15-level

{\text{Li}}_{2}

molecular system by stimulated Raman adiabatic passage with intense unchirped femtosecond laser pulses. We have considered five rotational levels

{J}_{g}=0,2,\dots{},8

associated with the initial vibrational level

{v}_{g}=0

of the ground electronic state $X\text{ }{^{1}\ensuremath{\Sigma}}_{g}^{+}$, five rotational levels

{J}_{i}=1,3,\dots{},9

associated with the vibrational level

{v}_{i}=1

of the intermediate excited electronic state $A\text{ }{^{1}\ensuremath{\Sigma}}_{u}^{+}$, and five rotational levels

{J}_{f}=0,2,\dots{},8

associated with the final target vibrational levels

{v}_{f}=1,2

of the $X\text{ }{^{1}\ensuremath{\Sigma}}_{g}^{+}$ state of the

{\text{Li}}_{2}

alkali dimer. The pump and Stokes laser pulses are taken to have the same temporal (Gaussian) shapes, pulse widths, and linear parallel polarizations. The laser wavelengths are in the (visible) range of 700--740 nm. The (peak) intensities of the pulses are of the order of $1\ifmmode\times\else\texttimes\fi{}{10}^{12}--2.5\ifmmode\times\else\texttimes\fi{}{10}^{13}\text{ }\text{W}/{\text{cm}}^{2}$ and the pulse widths are of the order of 20--50 fs. We have solved the 15 coupled time-dependent Schr\"odinger equations to study the population transfer to the target-excited vibrational levels. We have observed that, even with ``mushrooming'' of closely spaced rotational levels, efficient and selective population transfer to excited vibrational levels in

{\text{Li}}_{2}

alkali dimer can be achieved for counterintuitive pulse sequence by controlling the pump and Stokes laser parameters. We have endeavored to explain the results within the framework of adiabatic picture.