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Ultrafast Molecular Frame Quantum Tomography.
Morrigan, Luna; Neville, Simon P; Gregory, Margaret; Boguslavskiy, Andrey E; Forbes, Ruaridh; Wilkinson, Iain; Lausten, Rune; Stolow, Albert; Schuurman, Michael S; Hockett, Paul; Makhija, Varun.
Afiliación
  • Morrigan L; Department of Chemistry and Physics, University of Mary Washington, Fredericksburg, Virginia 22401, USA.
  • Neville SP; National Research Council Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada.
  • Gregory M; Department of Chemistry and Physics, University of Mary Washington, Fredericksburg, Virginia 22401, USA.
  • Boguslavskiy AE; Department of Physics, University of Ottawa, 150 Louis Pasteur, Ottawa, Ontario K1N 6N5, Canada.
  • Forbes R; Department of Chemistry and Biomolecular Sciences, University of Ottawa, Ottawa, Ontario K1N 6N5, Canada.
  • Wilkinson I; Department of Physics, University of Ottawa, 150 Louis Pasteur, Ottawa, Ontario K1N 6N5, Canada.
  • Lausten R; Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA.
  • Stolow A; National Research Council Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada.
  • Schuurman MS; Institute for Electronic Structure Dynamics, Helmholtz-Zentrum für Materialien und Energie, Hahn-Meitner-Platz 1, 14109 Berlin, Germany.
  • Hockett P; National Research Council Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada.
  • Makhija V; National Research Council Canada, 100 Sussex Drive, Ottawa, Ontario K1A 0R6, Canada.
Phys Rev Lett ; 131(19): 193001, 2023 Nov 10.
Article en En | MEDLINE | ID: mdl-38000424
We develop and experimentally demonstrate a methodology for a full molecular frame quantum tomography (MFQT) of dynamical polyatomic systems. We exemplify this approach through the complete characterization of an electronically nonadiabatic wave packet in ammonia (NH_{3}). The method exploits both energy and time-domain spectroscopic data, and yields the lab frame density matrix (LFDM) for the system, the elements of which are populations and coherences. The LFDM fully characterizes electronic and nuclear dynamics in the molecular frame, yielding the time- and orientation-angle dependent expectation values of any relevant operator. For example, the time-dependent molecular frame electronic probability density may be constructed, yielding information on electronic dynamics in the molecular frame. In NH_{3}, we observe that electronic coherences are induced by nuclear dynamics which nonadiabatically drive electronic motions (charge migration) in the molecular frame. Here, the nuclear dynamics are rotational and it is nonadiabatic Coriolis coupling which drives the coherences. Interestingly, the nuclear-driven electronic coherence is preserved over longer timescales. In general, MFQT can help quantify entanglement between electronic and nuclear degrees of freedom, and provide new routes to the study of ultrafast molecular dynamics, charge migration, quantum information processing, and optimal control schemes.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Phys Rev Lett Año: 2023 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos
Texto completo
Añadir a Mi BVS
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Phys Rev Lett Año: 2023 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos