Adiabatic climbing of vibrational ladders using Raman transitions with chirped pump lasers(J.Raman.Spectro.) - D.S.Tchitchekova

Research Article

Adiabatic climbing of vibrational ladders using Raman transitions with chirped pump lasers: effect of higher electronic surfaces and control of the shapes of vibrational wave packets

Deyana S. Tchitchekova *, Szczepan Chelkowski, André D. Bandrauk
Département de Chimie, Faculté des Sciences, Université de Sherbrooke, Sherbrooke, Québec J1K 2R1, Canada

email: Deyana S. Tchitchekova (Deyana.Tchitchekova@USherbrooke.ca)
*Correspondence to Deyana S. Tchitchekova, Université de Sherbrooke, 1500, Boul. de l'Université, J1K 2R1, Sherbrooke(Québec), Canada.

Keywords
vibrational excitation; H2; control of wave packets

Abstract

Using numerical solutions of the time-dependent Schrödinger equation for the H2 molecule in intense laser fields we calculate the vibrational excitation induced by the Raman chirped adiabatic process (RCAP). We show that adding several higher electronic surfaces to a simple two-surface model improves the efficiency of the ladder-climbing process at intensities below the adiabaticity threshold. Furthermore, we show that although using photon energies close to the one-photon electronic transition frequency allows the use of lower pump and Stokes intensities, in general, this leads to more population transfer to the upper electronic surfaces accompanied by a loss of selectivity in the vibrational excitation on the ground-state surface. By contrast, considerable dissociation yields can be achieved when higher energy photons are used. We also investigate the structure of time-dependant vibrational wave packets prepared by RCAP. We find that at specific times the wave packet is very well localised at large inter-nuclear separations at which ionisation occurs with a probability 3 orders of magnitude larger than at the equilibrium separation.

Copyright © 2007 John Wiley & Sons, Ltd.
Received: 25 August 2006; Accepted: 31 January 2007
Digital Object Identifier (DOI)

Femtosecond quantum control of molecular dynamics in the condensed phase (PCCP) - Patrick Nuernberger

Article citation: Patrick Nuernberger, Phys. Chem. Chem. Phys., 2007, DOI: 10.1039/b618760a

Femtosecond quantum control of molecular dynamics in the condensed phase

Patrick Nuernberger, Gerhard Vogt, Tobias Brixner and Gustav Gerber

We review the progress in controlling quantum dynamical processes in the condensed phase with femtosecond laser pulses. Due to its high particle density the condensed phase has both high relevance and appeal for chemical synthesis. Thus, in recent years different methods have been developed to manipulate the dynamics of condensed-phase systems by changing one or multiple laser pulse parameters. Single-parameter control is often achieved by variation of the excitation pulses wavelength, its linear chirp or its temporal subpulse separation in case of pulse sequences. Multiparameter control schemes are more flexible and provide a much larger parameter space for an optimal solution. This is realized in adaptive femtosecond quantum control, in which the optimal solution is iteratively obtained through the combination of an experimental feedback signal and an automated learning algorithm. Several experiments are presented that illustrate the different control concepts and highlight their broad applicability. These fascinating achievements show the continuous progress on the way towards the control of complex quantum reactions in the condensed phase.

Vibrationally State-Selective Spin-Orbit Transfer with Strong Nonresonant Pulses (JPhysChem A.) - Jesús González-Vázquez

J. Phys. Chem. A, ASAP Article 10.1021/jp066825y S1089-5639(06)06825-3 Web Release Date: March 20, 2007 Copyright © 2007 American Chemical Society

Vibrationally State-Selective Spin-Orbit Transfer with Strong Nonresonant Pulses

Jesús Gonzlez-Vzquez, Ignacio R. Sola,* Jesus Santamaria, and Vladimir S. Malinovsky

Departamento de Química Física, Universidad Complutense, 28040 Madrid, Spain, and MagiQ Technologies, Inc., 171 Madison Avenue, Suite 1300, New York, New York 10016

Received: October 17, 2006
In Final Form: February 2, 2007

Abstract:
By dynamic Stark shift using strong nonresonant pulses, we show that it is in principle possible to prepare arbitrary superposition states of mixed multiplicity. By a proper choice of parameters, the transfer of population is shown to follow the Rabi formula, where the initial and target states are now vibrational states of two light-induced molecular potentials of different multiplicity. Starting from nonstationary wave packets, the spin transfer can proceed via parallel transfer using a single pulse or by sequential transfer using a pulse sequence. A simple model is proposed to analyze the properties of both schemes and the feasibility of their experimental implementation for spin-orbit transitions in Rb2.

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Curriculum Vitae

Name: Hyeonho Choi

Affiliation: Researcher and Ph.D Candidate
Office: School of Chemistry, Seoul National University
E-mail: Hyeonho.choi@gmail.com
Tel: +82-2-880-4356
Fax: +82-2-889-1568

Education

03/1998-02/2002 Undergraduate Studies:

School of Chemistry, Seoul National University

03/2002-02/2007 Completing The Integrated MA/Ph.D course:

School of Chemistry, Seoul National University (Prof. Seokmin Shin)

03/2002- Doctoral Studies:

School of Chemistry, Seoul National University (Prof. Seokmin Shin)

Career

10/2007-03/2008 Research Assistant:

Institute for Molecular Science, Japan (Prof. Akiyoshi Hishikawa)

Original Paper

1. Bo. Y. Chang, Hyeonho Choi, Seokmin Shin, Ignacio R. Sola
“Quantum state selective two-photon excitation of multilevel systems assisted by Stark-shift”
Physical Review A., 75, 063405 (2007)

2. Hyeonho Choi, Won-Joon Son, Bo. Y. Chang, Ignacio R. Sola, Seokmin Shin
“Selective photodissociation in diatomic molecules by dynamical Stark-shift control”
The Journal of Chemical Physics, 128(7), (2008)

3. Hyeonho Choi, A. Hishikawa, A. Matsuda, M. Fushitani, Seokmin Shin
“Controlling population transfer between B and C states of NO molecule using polarized laser pulse"

now preparing.

4. Hyeonho Choi, Bo. Y. Chang, Won-Joon Son, Seokmin Shin

“The efficiency of SCRAP method in diatomic molecule beyond RWA approximation”
now preparing.

5. Hyeonho Choi, Bo. Y. Chang, Ignacio R. Sola, Seokmin Shin
“Selective two-photon excitation of diatomic molecule using SCRAP method”
now preparing.

Conference proceedings

1. 1st Asian Pacific Conference on Theoretical & Computational Chemistry, Okazaki, Japan

(May 12-15, 2004)

“Charge transfer and nonadiabatic dynamics of diatomic anion in clusters”
Hyeonho Choi, Eunseog Cho and Seokmin Shin

2. 12th International Congress of Quantum Chemistry, Kyoto, Japan

(May 21-26, 2006)

"Selective population transfer in molecular system by SCRAP method”
Hyeonho Choi, Won-joon Son and Seokmin Shin

3. 98th Korea Chemical Society National Meeting, Gwangju, Korea

(October 19-20, 2006)

“Quantum state selectivity in Stark-chirped rapid adiabatic passage”
Hyeonho Choi, Bo Y. Chang, Ignacio R. Sola, Seokmin Shin

4. 98th Korea Chemical Society National Meeting, Gwangju, Korea

(October 19-20, 2006)

“Laser control of molecular dissociation by SCRAP method”
Hyeonho Choi, Bo Y. Chang, Ignacio R. Sola, Seokmin Shin

5. 1st Winter School of JSPS ASIA CORE Program for Frontiers of Materials, Photo, and Theoretical

Molecular Science, Beijing, PR China

(December 5-9, 2006)
“An application of SCRAP method to dissociation dynamics”
Hyeonho Choi, Won-Joon Son, Seokmin Shin

6. Gordon Research Conference – Quantum Control of Light and Matter, Newport, RI, USA

(August 12-17, 2007)

“Selective two-photon excitation of quantum state using SCRAP method”
Hyeonho Choi, Won-Joon Son, Bo Y. Chang, Ignacio R. Sola, Seokmin Shin

7. 12th Korea-Japan Joint Symposium on Frontiers of Molecular Science & Physical Chemistry Summer

Symposium

(July 4-7, 2007)

“Quantum state selective two-photon excitation of diatomic molecular system assisted by Stark-

shift”
Hyeonho Choi, Won-Joon Son, Seokmin Shin

8. 16th International Symposium of SNU-UT-NTU Chemistry Departments

(February 1, 2008)

“The efficiency of Adiabatic Passage by Light Induced Potential beyond RWA Approximation”
Hyeonho Choi, Bo Y. Chang, Won-Joon Son, Seokmin Shin

School participation

1. 1st SOKENDAI Okazaki Lectures: Asian Winter School (IMS), Okazaki, Japan

(December 6-9, 2004)

2. 2nd SOKENDAI Okazaki Lectures: Asian Winter School (IMS), Okazaki, Japan

(February 2-5, 2006)

3. 1st Winter School of JSPS ASIA CORE Program for Frontiers of Materials, Photo, and Theoretical

Molecular Science, Beijing, PR China

(December 5-9, 2006)

4. The Winter School of Sokendai/Asian Core Program (IMS), Okazaki, Japan

(January 24-26, 2008)

Current Research Interest

• Optical control of small molecules by Stark-shift due to strong laser pulse (Stark-chirped rapid adiabatic passage)
  
• Optical control using Adiabatic Passage (Stimulated Raman adiabatic passage, Adiabatic passage by light induced potentials, Raman chirped adiabatic passage)
  
• Wavepacket dynamics in Non-Franck-Condon Regime & Rotating Wave Approximation
  
• Description nonadiabatic transition using One-electron model
  
• Quasi-stationary Floquet approach (Coulomb explosion, Above threshold dissociation etc.)
  
• Ultra-fast skeletal deformation in intense laser field
  

Future Research Interest

• Quantum Information and Computing
  
• Multi-Configuration Time-Dependent Hartree-Fock (MCTDHF)
  

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