Partial secular Bloch-Redfield master equation for incoherent excitation of multilevel quantum systems

The Journal of Chemical Physics
Timur V Tscherbul, Paul Brumer

Abstract

We present an efficient theoretical method for calculating the time evolution of the density matrix of a multilevel quantum system weakly interacting with incoherent light. The method combines the Bloch-Redfield theory with a partial secular approximation for one-photon coherences, resulting in a master equation that explicitly exposes the reliance on transition rates and the angles between transition dipole moments in the energy basis. The partial secular Bloch-Redfield master equation allows an unambiguous distinction between the regimes of quantum coherent vs. incoherent energy transfer under incoherent light illumination. The fully incoherent regime is characterized by orthogonal transition dipole moments in the energy basis, leading to a dynamical evolution governed by a coherence-free Pauli-type master equation. The coherent regime requires non-orthogonal transition dipole moments in the energy basis and leads to the generation of noise-induced quantum coherences and population-to-coherence couplings. As a first application, we consider the dynamics of excited state coherences arising under incoherent light excitation from a single ground state and observe population-to-coherence transfer and the formation of non-equilibr...Continue Reading

References

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Feb 25, 2014·The Journal of Chemical Physics·Zaheen S Sadeq, Paul Brumer
Apr 2, 2014·The Journal of Physical Chemistry. a·T V Tscherbul, P Brumer
Sep 27, 2014·Physical Review Letters·Timur V Tscherbul, Paul Brumer
Feb 16, 2015·The Journal of Chemical Physics·Jan JeskeJared H Cole
Feb 7, 2013·The Journal of Physical Chemistry Letters·Ivan KassalSaleh Rahimi-Keshari

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Citations

Sep 10, 2016·The Journal of Physical Chemistry Letters·Sima Baghbanzadeh, Ivan Kassal
Jan 5, 2017·The Journal of Chemical Physics·Amro DodinPaul Brumer
Sep 24, 2018·The Journal of Chemical Physics·Simon Axelrod, Paul Brumer
Apr 24, 2020·The Journal of Chemical Physics·Chern Chuang, Paul Brumer
Aug 17, 2018·Physical Review. E·Michael Kilgour, Dvira Segal
Sep 24, 2020·The Journal of Chemical Physics·Kenneth A Jung, Paul Brumer
Jan 1, 2021·The Journal of Chemical Physics·Veljko Janković, Tomáš Mančal
Jan 1, 2021·The Journal of Chemical Physics·Veljko Janković, Tomáš Mančal
May 16, 2018·The Journal of Physical Chemistry Letters·Paul Brumer

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