Linear and nonlinear spectroscopy from quantum master equations

The Journal of Chemical Physics
Jonathan H Fetherolf, Timothy C Berkelbach

Abstract

We investigate the accuracy of the second-order time-convolutionless (TCL2) quantum master equation for the calculation of linear and nonlinear spectroscopies of multichromophore systems. We show that even for systems with non-adiabatic coupling, the TCL2 master equation predicts linear absorption spectra that are accurate over an extremely broad range of parameters and well beyond what would be expected based on the perturbative nature of the approach; non-equilibrium population dynamics calculated with TCL2 for identical parameters are significantly less accurate. For third-order (two-dimensional) spectroscopy, the importance of population dynamics and the violation of the so-called quantum regression theorem degrade the accuracy of TCL2 dynamics. To correct these failures, we combine the TCL2 approach with a classical ensemble sampling of slow microscopic bath degrees of freedom, leading to an efficient hybrid quantum-classical scheme that displays excellent accuracy over a wide range of parameters. In the spectroscopic setting, the success of such a hybrid scheme can be understood through its separate treatment of homogeneous and inhomogeneous broadening. Importantly, the presented approach has the computational scaling of ...Continue Reading

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Citations

May 17, 2018·The Journal of Chemical Physics·Justin Provazza, David F Coker
Aug 3, 2019·The Journal of Chemical Physics·Seogjoo J Jang
Jul 22, 2019·The Journal of Chemical Physics·Kade Head-Marsden, David A Mazziotti
Jun 10, 2019·The Journal of Chemical Physics·Peter A Rose, Jacob J Krich
Jul 6, 2019·The Journal of Chemical Physics·Addison J Schile, David T Limmer
May 3, 2019·The Journal of Chemical Physics·Kritanjan Polley, Roger F Loring
Dec 12, 2018·The Journal of Chemical Physics·Addison J Schile, David T Limmer
Jan 28, 2021·The Journal of Chemical Physics·Peter A Rose, Jacob J Krich
Dec 3, 2020·The Journal of Chemical Physics·Kritanjan Polley, Roger F Loring
Sep 10, 2020·The Journal of Physical Chemistry. B·Lorenzo CupelliniJianshu Cao
Dec 17, 2020·Chemical Reviews·Kade Head-MarsdenPrineha Narang
Jul 10, 2021·The Journal of Chemical Physics·Kritanjan Polley, Roger F Loring
Aug 9, 2021·The Journal of Chemical Physics·Eric A ArsenaultGraham R Fleming
Oct 28, 2020·The Journal of Physical Chemistry. B·Kritanjan Polley, Roger F Loring
Oct 8, 2021·Journal of Chemical Theory and Computation·Yakov BraverAndrius Gelzinis

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