This book presents the latest theoretical studies giving new predictions and interpretations on the quantum correlation in molecular dynamics induced by ultrashort laser pulses. The author quantifies the amount of correlation in terms of entanglement by employing methods developed in quantum information science, in particular applied to the photoionization of a hydrogen molecule. It is also revealed that the photoelectron–ion correlation affects the vibrational dynamics of the molecular ion and induces the attosecond-level time delay in the molecular vibration. Furthermore, the book also presents how molecular vibration can couple to photons in a plasmoic nanocavity.
Physicists and chemists interested in the ultrafast molecular dynamics would be the most relevant readers. They can learn how we can employ the quantum-information-science tools to understand the correlation in the molecular dynamics and why we should consider the correlation between the photoelectron and the molecular ion to describe the ion’s dynamics. They can also learn how to treat a molecule coupled to photons in a nanocavity. All the topics are related to the state-of-the-art experiments, and so, it is important to publish these results to enhance the understanding and to induce new experiments to confirm the theory presented.
Author(s): Takanori Nishi
Series: Springer Theses
Publisher: Springer
Year: 2022
Language: English
Pages: 102
City: Singapore
Supervisor’s Foreword
Preface
List of Publications
Contents
Part I Introduction
1 General Introduction
1.1 Entanglement
1.1.1 Bipartite System
1.1.2 Bipartite Entanglement
1.1.3 Entanglement in Atoms and Molecules
1.2 Ultrafast Coherent Motion
1.2.1 Coherent Motion of Ions
1.2.2 Wigner Delay
1.3 Molecule in a Cavity
1.3.1 Purcell Effect
1.3.2 Monte Carlo Wave Packet Method
1.4 Outline of the Book
1.4.1 Entanglement and Coherence
1.4.2 Time Delay in the Coherent Motion of H2+
1.4.3 Molecule in a Plasmonic Nanocavity
References
Part II Correlation Between an Ion and a Photoelectron
2 Entanglement and Coherence Created by Photoionization of H2
2.1 Entanglement and Coherence
2.1.1 Entanglement Between H2+ and e-
2.1.2 Coherence in the Vibrational State
2.2 Numerical Procedure
2.2.1 One-Dimensional Model
2.2.2 Symmetry Adapted Grid (SAG) Method
2.2.3 Time Propagation
2.3 Results and Discussion
2.3.1 Entanglement and Coherence: Pulse Duration Dependence and Wavelength Dependence
2.3.2 Entanglement and Coherence: Intensity Dependence
2.3.3 Purity, Coherence, and Population
2.3.4 Experimental Scheme for Determining the Reduced Density Matrix
2.4 Conclusion
References
3 Time Delay in the Coherent Vibrational Motion of H2+ Created by Photoionization of H2
3.1 Coherent Motion of Ions and Photoelectrons
3.2 Coherent Nuclear Motion Created by Ionization
3.2.1 Two-Center Coulomb Wave Function
3.2.2 Pump Process
3.2.3 Probe Process
3.2.4 Coincidence Detection of e-
3.3 Results and Discussion
3.3.1 Phase and Time Delay
3.3.2 Phase and Time Delay: Coincidence Detection of e-
3.3.3 Effect of the Chirp of the Pump Pulse
3.3.4 Relation to the Wigner Delay
3.4 Conclusion
References
Part III Correlation Between a Molecule and Photons
4 Molecule in a Plasmonic Nanocavity
4.1 Molecule–Photon Coupling in a Nanocavity
4.1.1 Master Equation for a Cavity–Molecule System
4.1.2 Effective Master Equation
4.1.3 Monte Carlo Wave Packet Method
4.2 Results and Discussion
4.2.1 Validity of the Effective Operator Method
4.2.2 Position-Dependent Decay Rate
4.3 Conclusion
References
Appendix Appendix A
A.1 Coulomb Wave Function
A.2 Two-Center Coulomb Wave Function
A.3 Transition Moment
Appendix Appendix B
B.1 General Formulation
B.2 Time-Independent Interaction
B.3 Derivation of the Jump Probability dp
