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

Wave-packet squeezing by iterative pump-dump control in diatomic molecules

Bo Y. Chang, Sungyul Lee, Ignacio R. Solá, Jesús Santamarı́a

Published Feb 10, 2006• 9 citations
Publisher

Abstract

Iterative vibrational wave packet squeezing by a sequence of femtosecond pulses is proposed. Analytic formulas are derived for the harmonic oscillator case, and the practical implementation of the scheme is tested on different electronic transitions in ${\mathrm{Rb}}_{2}$.

DOI
10.1103/physreva.73.023407

Related papers

Ultrashort-pulse-train pump and dump excitation of a diatomic molecule

Luı́s E. E. de Araujo

An excitation scheme is proposed for transferring population between ground-vibrational levels of a molecule. The transfer is accomplished by pumping and dumping population with a pair of coherent ultrashort-pulse trains via a stationary state. By mismatching the teeth of the frequency combs associated with the pulse trains to the vibrational levels, high selectivity in the excitation, along with high transfer efficiency, is predicted. The pump-dump scheme does not suffer from spontaneous emission losses, it is insensitive to the pump-dump-train delay, and it requires only basic pulse shaping.

Physical Review A•Sep 23, 2010•1 citation

Pump-dump control and the related transient absorption spectroscopies

Zhenwen Shen, YiJing Yan, Ji‐Xin Cheng +3 more

We combine theories of optimal pump-dump control and the related transient probe absorption spectroscopy in order to elucidate the relation between these two optical processes and the possibility of experimental realization. In the weak response regime, we identify the globally optimal pair of pump-dump control fields, and further propose a second-order difference detection scheme to monitor the wave packets dynamics that is jointly controlled by both the pump and dump fields. The globally optimal solution serves also as the initial input for the iterative search for the optimal control fields in the strong response regime. We use a model I2 molecule to demonstrate numerically the pump-dump control and the detection of a highly vibrationally excited wave packet focusing dynamics on the ground X surface in both the weak and strong response regimes. The I2B surface serves as the intermediate to assist the pump-dump control and the optical detection processes. Demonstrated in the strong response regime are the optimal pair of pump-dump molecular-π pulses that invert nearly total population onto the predefined target region within a half period of vibration motion.

The Journal of Chemical Physics•Apr 15, 1999•21 citations

Femtosecond wave packet engineering in a cyanine dye molecule

Kazuhiko Misawa, Isao Matsuda, Roy Lang

Quantum wave packet engineering is demonstrated using a phase-programmable femtosecond optical source. This paper describes development of a programmable phase modulator and coherent control of quantum wave packets. Wave packet motion in a cyanine dye molecule is observed to be dependent on the chirp direction and rate of excitation pulses. Strong reduction in excited state population is efficient for negatively chirped pulses in the cyanine dye molecule, which is explained in terms of a pump-dump process. We discuss a possibility of mutual conversion between the optical and electronic phase information by means of nonlinear light-matter interaction.

Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE•Dec 1, 2002•2 citations

Coherent control of electronic and vibrational wave packets using phase-locked optical pulses

Elizabeth Durrell Boleat

Experimental and theoretical work is presented on the control of wave packet dynamics in atomic and molecular systems. Using sequences of phase-locked optical pulses, the link between optical phase and quantum mechanical phase is explored in the Na atom and Naj dimer, representing a step towards the logical engineering of quantum states in more complicated systems. A novel apparatus, constructed to study and control the vibrational dynamics of vibrational wave packets on the Na ionic potential surface, is described in chapter 3. Theoretical simulations for proposed experiment are presented in chapter 4. Control is achieved by exploiting the phase-evolution of the constituent vibrational quantum states within the wave packet superposition. The phase relationship and the accumulated phase difference between the various components of the wave packet is determined, and a sequence of phase-locked optical pulses is employed to selectively enhance or depopulate specific vibrational states, or sets of vibrational states. The quantum state composition of the resulting wave packet, and the efficiency of the control scheme, is determined by calculating the multi-pulse response of the time-dependent vibrational state populations. In chapter 5, the quantum interference between Rydberg electron wave packets in the Na atom is investigated using pairs of phase-locked wave packets, allowing manipulation of the total orbital angular momentum of Na Rydberg atoms. Initially the wave packet is composed of a superposition of s and d Rydberg series. Exploitation of the difference between the quantum defects of the two series allows specific angular momentum compositions within the resultant wave packet to be engineered. Experimentally, this final quantum state distribution is analysed in the frequency domain using state selective field ionisation, and in the time domain using the optical Ramsey method. The theoretical calculations show how the phase difference between pairs of optical pulses is linked to the corresponding Rydberg frequency spectrum, therefore enabling the control of the quantum state composition of the wave packets.

•Jan 1, 2005•0 citations

Quantum control by stimulated Raman scattering

R. Pausch, M. Heid, T. Chen +2 more

In a model system, i.e. the K2 dimer molecule, a vibrationally excited wave packet around a prechosen target state in the electronic ground state is generated by an ultrafast resonant stimulated Raman process. By choosing the pump and dump wavelengths along the difference potential between the excited electronic |B〉-state and the electronic ground state |X〉 and optimizing the delay time between the pump and dump processes, one can increase considerably the efficiency of the population transfer of this quantum control experiment. Copyright © 2000 John Wiley & Sons, Ltd.

Journal of Raman Spectroscopy•Jan 1, 2000•39 citations

Optical Control of the Rotational Angular Momentum of a Molecular Rydberg Wave Packet

Russell S. Minns, R. Patel, Jan R. R. Verlet +1 more

An intuitive scheme for controlling the rotational quantum state of a Rydberg molecule is demonstrated experimentally. We determine the accumulated phase difference between the various components of a molecular electron wave packet, and then employ a sequence of phase-locked optical pulses to selectively enhance or depopulate specific rotational states. The angular momentum composition of the resulting wave packet, and the efficiency of the control scheme, is determined by calculating the multipulse response of the time-dependent Rydberg populations.

Physical Review Letters•Dec 10, 2003•30 citations
Iterative vibrational wave packet squeezing by a sequence of femtosecond pulses is proposed. Analytic formulas are derived for the harmonic oscillator case, and the practical implementation of the scheme is tested on different electronic transitions in Rb2{\mathrm{Rb}}_{2}Rb2​.
An excitation scheme is proposed for transferring population between ground-vibrational levels of a molecule. The transfer is accomplished by pumping and dumping population with a pair of coherent ultrashort-pulse trains via a stationary state. By mismatching the teeth of the frequency combs associated with the pulse trains to the vibrational levels, high selectivity in the excitation, along with high transfer efficiency, is predicted. The pump-dump scheme does not suffer from spontaneous emission losses, it is insensitive to the pump-dump-train delay, and it requires only basic pulse shaping.
We combine theories of optimal pump-dump control and the related transient probe absorption spectroscopy in order to elucidate the relation between these two optical processes and the possibility of experimental realization. In the weak response regime, we identify the globally optimal pair of pump-dump control fields, and further propose a second-order difference detection scheme to monitor the wave packets dynamics that is jointly controlled by both the pump and dump fields. The globally optimal solution serves also as the initial input for the iterative search for the optimal control fields in the strong response regime. We use a model I2 molecule to demonstrate numerically the pump-dump control and the detection of a highly vibrationally excited wave packet focusing dynamics on the ground X surface in both the weak and strong response regimes. The I2B surface serves as the intermediate to assist the pump-dump control and the optical detection processes. Demonstrated in the strong response regime are the optimal pair of pump-dump molecular-π pulses that invert nearly total population onto the predefined target region within a half period of vibration motion.
Quantum wave packet engineering is demonstrated using a phase-programmable femtosecond optical source. This paper describes development of a programmable phase modulator and coherent control of quantum wave packets. Wave packet motion in a cyanine dye molecule is observed to be dependent on the chirp direction and rate of excitation pulses. Strong reduction in excited state population is efficient for negatively chirped pulses in the cyanine dye molecule, which is explained in terms of a pump-dump process. We discuss a possibility of mutual conversion between the optical and electronic phase information by means of nonlinear light-matter interaction.
Experimental and theoretical work is presented on the control of wave packet dynamics in atomic and molecular systems. Using sequences of phase-locked optical pulses, the link between optical phase and quantum mechanical phase is explored in the Na atom and Naj dimer, representing a step towards the logical engineering of quantum states in more complicated systems. A novel apparatus, constructed to study and control the vibrational dynamics of vibrational wave packets on the Na ionic potential surface, is described in chapter 3. Theoretical simulations for proposed experiment are presented in chapter 4. Control is achieved by exploiting the phase-evolution of the constituent vibrational quantum states within the wave packet superposition. The phase relationship and the accumulated phase difference between the various components of the wave packet is determined, and a sequence of phase-locked optical pulses is employed to selectively enhance or depopulate specific vibrational states, or sets of vibrational states. The quantum state composition of the resulting wave packet, and the efficiency of the control scheme, is determined by calculating the multi-pulse response of the time-dependent vibrational state populations. In chapter 5, the quantum interference between Rydberg electron wave packets in the Na atom is investigated using pairs of phase-locked wave packets, allowing manipulation of the total orbital angular momentum of Na Rydberg atoms. Initially the wave packet is composed of a superposition of s and d Rydberg series. Exploitation of the difference between the quantum defects of the two series allows specific angular momentum compositions within the resultant wave packet to be engineered. Experimentally, this final quantum state distribution is analysed in the frequency domain using state selective field ionisation, and in the time domain using the optical Ramsey method. The theoretical calculations show how the phase difference between pairs of optical pulses is linked to the corresponding Rydberg frequency spectrum, therefore enabling the control of the quantum state composition of the wave packets.
In a model system, i.e. the K2 dimer molecule, a vibrationally excited wave packet around a prechosen target state in the electronic ground state is generated by an ultrafast resonant stimulated Raman process. By choosing the pump and dump wavelengths along the difference potential between the excited electronic |B〉-state and the electronic ground state |X〉 and optimizing the delay time between the pump and dump processes, one can increase considerably the efficiency of the population transfer of this quantum control experiment. Copyright © 2000 John Wiley & Sons, Ltd.
An intuitive scheme for controlling the rotational quantum state of a Rydberg molecule is demonstrated experimentally. We determine the accumulated phase difference between the various components of a molecular electron wave packet, and then employ a sequence of phase-locked optical pulses to selectively enhance or depopulate specific rotational states. The angular momentum composition of the resulting wave packet, and the efficiency of the control scheme, is determined by calculating the multipulse response of the time-dependent Rydberg populations.