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

arXiv:physics/0203049

Non-adiabatic coupling and adiabatic population transfer in quantum molecular systems

Ignacio R. Solá, Vladimir S. Malinovsky

Published Mar 15, 2002• 0 citations
arXivHTMLPDF

Abstract

We show that a counter-intuitive pulse sequence leads to adiabatic passage between the vibrational levels of three harmonic potentials through parallel dark states in adiabatic approximation. However, the adiabatic assumptions break down for very intense pulses and non-adiabatic couplings result in the population transfer by light-induced potential shaping.

DOI
10.48550/arxiv.physics/0203049

Related papers

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

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

Coherent population transfer beyond the adiabatic limit: Generalized matched pulses and higher-order trapping states

Michael Fleischhauer, Razmik G. Unanyan, Bruce W. Shore +1 more

We show that the physical mechanism of population transfer in a three-level system with a closed loop of coherent couplings is not equivalent to an adiabatic rotation of the dark state of the Hamiltonian, but corresponds to a rotation of a higher-order trapping state in a generalized adiabatic basis. The concept of generalized adiabatic basis sets is used as a constructive tool to design pulse sequences for stimulated Raman adiabatic passage, which also give maximum population transfer under conditions when the usual condition of adiabaticty is only poorly fulfilled. Under certain conditions for the pulses (generalized matched pulses), there exists a higher-order trapping state, which is an exact constant of motion, and analytic solutions for the atomic dynamics can be derived.

arXiv:quant-ph/9811007•Physical Review A•May 1, 1999•29 citations

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

Adiabatic Passage in a Three-State System with Non-Markovian Relaxation: The Role of Excited-State Absorption and Two-Exciton Processes†

Boris D. Fainberg, Vladimir A. Gorbunov

The influence of excited-state absorption (ESA) and two-exciton processes on a coherent population transfer with intense ultrashort chirped pulses in molecular systems in solution has been studied. A unified treatment of adiabatic rapid passage (ARP) in such systems has been developed using a three-state electronic system with relaxation treated as a diffusion on electronic potential energy surfaces. We have shown that ESA has a profound effect on coherent population transfer in large molecules that necessitates a more accurate interpretation of experimental data. A simple and physically clear model for ARP in molecules with three electronic states in solution has been developed by extending the Landau-Zener calculations putting in a third level to random crossing of levels. A method for quantum control of two-exciton states in molecular complexes has been proposed. 1.

•Jan 1, 2007•5 citations

Assisted Adiabatic Passage Revisited

Mustafa Demirplak, Stuart A. Rice

We report the results of studies of various aspects of the counter diabatic field paradigm, a recipe that generates adiabatic population transfer between levels by assisting a given field so that the total field generates the population transfer that the adiabatic approximation suggests for the given field. The sensitivity of this recipe to the pulse parameters and to Gaussian stochastic phase fluctuations between the fields has been investigated. Ladder-climbing population transfer between the vibrational levels of a nonrotating Morse oscillator is examined, and a numerical demonstration of the efficiency of the scheme is given.

The Journal of Physical Chemistry B•Feb 8, 2005•389 citations
We show that a counter-intuitive pulse sequence leads to adiabatic passage between the vibrational levels of three harmonic potentials through parallel dark states in adiabatic approximation. However, the adiabatic assumptions break down for very intense pulses and non-adiabatic couplings result in the population transfer by light-induced potential shaping.
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.
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.
We show that the physical mechanism of population transfer in a three-level system with a closed loop of coherent couplings is not equivalent to an adiabatic rotation of the dark state of the Hamiltonian, but corresponds to a rotation of a higher-order trapping state in a generalized adiabatic basis. The concept of generalized adiabatic basis sets is used as a constructive tool to design pulse sequences for stimulated Raman adiabatic passage, which also give maximum population transfer under conditions when the usual condition of adiabaticty is only poorly fulfilled. Under certain conditions for the pulses (generalized matched pulses), there exists a higher-order trapping state, which is an exact constant of motion, and analytic solutions for the atomic dynamics can be derived.
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.
The influence of excited-state absorption (ESA) and two-exciton processes on a coherent population transfer with intense ultrashort chirped pulses in molecular systems in solution has been studied. A unified treatment of adiabatic rapid passage (ARP) in such systems has been developed using a three-state electronic system with relaxation treated as a diffusion on electronic potential energy surfaces. We have shown that ESA has a profound effect on coherent population transfer in large molecules that necessitates a more accurate interpretation of experimental data. A simple and physically clear model for ARP in molecules with three electronic states in solution has been developed by extending the Landau-Zener calculations putting in a third level to random crossing of levels. A method for quantum control of two-exciton states in molecular complexes has been proposed. 1.
We report the results of studies of various aspects of the counter diabatic field paradigm, a recipe that generates adiabatic population transfer between levels by assisting a given field so that the total field generates the population transfer that the adiabatic approximation suggests for the given field. The sensitivity of this recipe to the pulse parameters and to Gaussian stochastic phase fluctuations between the fields has been investigated. Ladder-climbing population transfer between the vibrational levels of a nonrotating Morse oscillator is examined, and a numerical demonstration of the efficiency of the scheme is given.