Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Physical Review A

Laser-assisted molecular engineering of bond lengths and vibrational motion

Ignacio R. Solá

Published Mar 9, 2004• 24 citations
Publisher

Abstract

In this paper we propose to control the bond length of a diatomic molecule and its vibrational coherent motion over arbitrary distances. The method requires (a) mixing a dissociative potential with bound electronic configurations in order to stabilize the continuum, and (b) manipulating the wave-packet transfer below the threshold of adiabatic passage. Using asymmetric pulses it is possible to implement sudden-adiabatic transitions to stop or induce the motion in the light-induced potential, controlling the nonadiabatic dynamics in a most efficient way.

DOI
10.1103/physreva.69.033401

Related papers

Inducing changes in the bond length of diatomic molecules by time-symmetric chirped pulses

Bo Y. Chang, Seokmin Shin, Ignacio R. Solá

We show numerically that it is possible to change the structure of a simple molecule, that is, a diatomic molecule, where the bond length is modified at a precise timing with symmetrically chirped laser pulses. In the adiabatic regime, the process is fully time reversible, making it possible to design slow vibrations with large bond elongations. The scheme relies on the preparation of a separable state of both nuclear and electronic degrees of freedom with predominant amplitude on the dissociative (antibonding) electronic wave function. Shorter laser pulses can be used to dynamically induce larger bond elongations, preparing a highly excited vibrational wave packet in the ground potential as the laser is switched off.

Physical Review A•Dec 27, 2010•21 citations

Tailoring of vibrational state populations with light-induced potentials in molecules

Mirta Rodríguez, Kalle‐Antti Suominen, B. M. Garraway

Summary form only given. We propose a method for achieving highly efficient transfer between the vibrational states in a diatomic molecule. The process is mediated by strong laser pulses and can be understood in terms of light-induced potentials. Light-induced potentials were also key to understanding APLIP (adiabatic passage by light induced potentials), where a wave packet is guided from one ground vibrational state to another. However, in the new process we show how to target specific vibrational states with strong short pulses. In addition to describing a specific molecular system, our results show how, in general, one can manipulate the populations of the different quantum states in double well systems.

Conference on Lasers and Electro-Optics•Aug 29, 2005•1 citation

Short-pulse chirped adiabatic population transfer in diatomic molecules

Shimshon Kallush, Y. B. Band

Using the concept of light-induced potentials introduced by Garraway and Suominen [Phys. Rev. Lett. 80, 932 (1998)], we study alternative schemes of adiabatic population transfer in a diatomic molecule from the lowest vibrational level of the ground electronic state to the lowest vibrational level of a third electronic state via allowed optical transitions from the ground and third electronic states to a second electronic state. Our chirped-pulse rapid adiabatic passage scheme is implemented with short-duration optical pulses, and can be understood in terms of ``road design engineering'' of the light-induced time-dependent adiabatic potential upon which the dynamics occurs. We explicitly show that complete adiabatic vibronic population transfer occurs using chirped picosecond-duration pulses in the sodium dimer example.

Physical Review A•Feb 28, 2000•49 citations

Control of molecular processes by a sequence of linearly chirped pulses

K. Nagaya, Yoshiaki Teranishi, Hiroki Nakamura

A new scheme of controlling molecular processes by a sequence of linearly chirped pulses is proposed and is applied to selective excitation of an energy level among closely lying ones and to complete electronic excitation of a diatomic molecule. The basic idea is quite different from the conventional ones utilizing chirped pulses in the sense that the present one does not rely on the idea of adiabatic rapid passage at all, but tries to control basic nonadiabatic transitions explicitly. Control of molecular processes can be achieved by controlling nonadiabatic transitions among Floquet (or dressed) states with use of the interference effects. The scheme can be formulated with use of the analytical theories of nonadiabatic transitions, and the proper control parameters can be estimated theoretically. Numerical demonstrations are provided to confirm the robustness of the method in comparison with the other conventional ones. Namely, the present scheme is shown to be stable against the variation of pulse area, complete and selective in population transfer, and fast to accomplish the transition. It is expected that the method can be applied to general multilevel systems and various types of wave packet dynamics. Its experimental realizability can also be expected, since linear chirping can now be relatively easily realized and manipulated.

The Journal of Chemical Physics•Nov 14, 2002•15 citations

Adiabatic climbing of vibrational ladders using Raman transitions with a chirped pump laser

Szczepan Chelkowski, George N. Gibson

We present detailed calculations of a new scheme for the adiabatic transfer of population in molecular vibrational ladders and for controlling chemical reactions: Raman chirped adiabatic passage. The scheme makes use of far-off-resonant Raman transitions with one chirped and one monochromatic laser pulse. We show that this method can be used to climb vibrational ladders in molecular systems and, with sufficiently large chirping, can vibrationally dissociate diatomic molecules.

Physical Review A•Nov 1, 1995•101 citations

Adiabatic Passage by Light-Induced Potentials in Molecules

B. M. Garraway, Kalle‐Antti Suominen

We present the process of adiabatic passage by light-induced potentials for transferring a wave packet from one molecular potential to the displaced ground vibrational state of another. The process uses a counterintuitive sequence of light pulses to couple three molecular states. It shares many features with the process of stimulated Raman adiabatic passage, such as high efficiency and insensitivity to pulse parameters. However, in the former there is no two-photon resonance, and the main mechanism for the transport of the wave packet is a light-induced potential.

arXiv:physics/9709005•Physical Review Letters•Feb 2, 1998•185 citations
In this paper we propose to control the bond length of a diatomic molecule and its vibrational coherent motion over arbitrary distances. The method requires (a) mixing a dissociative potential with bound electronic configurations in order to stabilize the continuum, and (b) manipulating the wave-packet transfer below the threshold of adiabatic passage. Using asymmetric pulses it is possible to implement sudden-adiabatic transitions to stop or induce the motion in the light-induced potential, controlling the nonadiabatic dynamics in a most efficient way.
We show numerically that it is possible to change the structure of a simple molecule, that is, a diatomic molecule, where the bond length is modified at a precise timing with symmetrically chirped laser pulses. In the adiabatic regime, the process is fully time reversible, making it possible to design slow vibrations with large bond elongations. The scheme relies on the preparation of a separable state of both nuclear and electronic degrees of freedom with predominant amplitude on the dissociative (antibonding) electronic wave function. Shorter laser pulses can be used to dynamically induce larger bond elongations, preparing a highly excited vibrational wave packet in the ground potential as the laser is switched off.
Summary form only given. We propose a method for achieving highly efficient transfer between the vibrational states in a diatomic molecule. The process is mediated by strong laser pulses and can be understood in terms of light-induced potentials. Light-induced potentials were also key to understanding APLIP (adiabatic passage by light induced potentials), where a wave packet is guided from one ground vibrational state to another. However, in the new process we show how to target specific vibrational states with strong short pulses. In addition to describing a specific molecular system, our results show how, in general, one can manipulate the populations of the different quantum states in double well systems.
Using the concept of light-induced potentials introduced by Garraway and Suominen [Phys. Rev. Lett. 80, 932 (1998)], we study alternative schemes of adiabatic population transfer in a diatomic molecule from the lowest vibrational level of the ground electronic state to the lowest vibrational level of a third electronic state via allowed optical transitions from the ground and third electronic states to a second electronic state. Our chirped-pulse rapid adiabatic passage scheme is implemented with short-duration optical pulses, and can be understood in terms of ``road design engineering'' of the light-induced time-dependent adiabatic potential upon which the dynamics occurs. We explicitly show that complete adiabatic vibronic population transfer occurs using chirped picosecond-duration pulses in the sodium dimer example.
A new scheme of controlling molecular processes by a sequence of linearly chirped pulses is proposed and is applied to selective excitation of an energy level among closely lying ones and to complete electronic excitation of a diatomic molecule. The basic idea is quite different from the conventional ones utilizing chirped pulses in the sense that the present one does not rely on the idea of adiabatic rapid passage at all, but tries to control basic nonadiabatic transitions explicitly. Control of molecular processes can be achieved by controlling nonadiabatic transitions among Floquet (or dressed) states with use of the interference effects. The scheme can be formulated with use of the analytical theories of nonadiabatic transitions, and the proper control parameters can be estimated theoretically. Numerical demonstrations are provided to confirm the robustness of the method in comparison with the other conventional ones. Namely, the present scheme is shown to be stable against the variation of pulse area, complete and selective in population transfer, and fast to accomplish the transition. It is expected that the method can be applied to general multilevel systems and various types of wave packet dynamics. Its experimental realizability can also be expected, since linear chirping can now be relatively easily realized and manipulated.
We present the process of adiabatic passage by light-induced potentials for transferring a wave packet from one molecular potential to the displaced ground vibrational state of another. The process uses a counterintuitive sequence of light pulses to couple three molecular states. It shares many features with the process of stimulated Raman adiabatic passage, such as high efficiency and insensitivity to pulse parameters. However, in the former there is no two-photon resonance, and the main mechanism for the transport of the wave packet is a light-induced potential.