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Time Resolved Quantum Tomography in Molecular Spectroscopy by the Maximal Entropy Approach.
Makhija, Varun; Gupta, Rishabh; Neville, Simon; Schuurman, Michael; Francisco, Joseph; Kais, Sabre.
Afiliación
  • Makhija V; Department of Chemistry and Physics, University of Mary Washington, Fredericksburg, Virginia 22401, United States.
  • Gupta R; Department of Chemistry, Purdue University, West Lafayette, Indiana 47907, United States.
  • Neville S; National Research Council Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada.
  • Schuurman M; National Research Council Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada.
  • Francisco J; Department of Chemistry, University of Ottawa, Ottawa, Ontario K1N 6N5, Canada.
  • Kais S; Department of Earth and Environmental Science and Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States.
J Phys Chem Lett ; 15(37): 9525-9534, 2024 Sep 19.
Article en En | MEDLINE | ID: mdl-39264357
ABSTRACT
Attosecond science offers unprecedented precision in probing the initial moments of chemical reactions, revealing the dynamics of molecular electrons that shape reaction pathways. A fundamental question emerges what role, if any, do quantum coherences between molecular electron states play in photochemical reactions? Answering this question necessitates quantum tomography─the determination of the electronic density matrix from experimental data, where the off-diagonal elements represent these coherences. The Maximal Entropy (MaxEnt) based Quantum State Tomography (QST) approach offers unique advantages in studying molecular dynamics, particularly with partial tomographic data. Here, we explore the application of MaxEnt-based QST on photoexcited ammonia, necessitating the operator form of observables specific to the performed measurements. We present two methodologies for constructing these operators one leveraging Molecular Angular Distribution Moments (MADMs) which accurately capture the orientation-dependent vibronic dynamics of molecules and another utilizing Angular Momentum Coherence Operators to construct measurement operators for the full rovibronic density matrix in the symmetric top basis. A key revelation of our study is the direct link between Lagrange multipliers in the MaxEnt formalism and the unique set of MADMs. Additionally, we visualize the electron density within the molecular frame, demonstrating charge migration across the molecule. Furthermore, we achieve a groundbreaking milestone by constructing, for the first time, the entanglement entropy of the electronic subsystem─a metric that was previously inaccessible. The entropy vividly reveals and quantifies the effects of coupling between the excited electron and nuclear degrees of freedom. Consequently, our findings open new avenues for research in ultrafast molecular spectroscopy within the broader domain of quantum information science, offering profound implications for the study of molecular systems under excitation using quantum tomographic schemes.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Phys Chem Lett Año: 2024 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
Buscar en Google

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: J Phys Chem Lett Año: 2024 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos