Two-dimensional action spectroscopy of excitonic systems: Explicit simulation using a phase-modulation technique

Fikeraddis A. Damtie, Andreas Wacker, Tõnu Pullerits, and Khadga J. Karki
Phys. Rev. A 96, 053830 – Published 13 November 2017

Abstract

Two-dimensional (2D) spectroscopy has been intensively used to study electronic and vibronic coherences in biological systems and semiconductors. This technique studies coherent as well as incoherent signals that arise from the nonlinear interaction of a sequence of laser pulses. In this paper we present a direct evaluation of the 2D signal based on elementary quantum kinetics in order to compare with the common approximate diagrammatic approaches. Here we consider incoherent action signals such as fluorescence or photocurrent as the observable, which is easily accessible in a measurement. These observables are calculated by solving the time evolution of the density matrix in the Lindblad form, which can take into account all possible decoherence processes. The phase modulation technique is used to separate the relevant nonlinear signals from the other possible interaction pathways. The approach can be used to calculate 2D spectra of any quantum system. For our model system we find a good agreement for the quantum beating between the coupled states.

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  • Received 18 July 2017

DOI:https://doi.org/10.1103/PhysRevA.96.053830

©2017 American Physical Society

Physics Subject Headings (PhySH)

Atomic, Molecular & Optical

Authors & Affiliations

Fikeraddis A. Damtie* and Andreas Wacker

  • Mathematical Physics and NanoLund, Lund University, Box 118, 22100 Lund, Sweden

Tõnu Pullerits and Khadga J. Karki§

  • Chemical Physics and NanoLund, Lund University, Box 124, 22100 Lund, Sweden

  • *Fikeraddis.Damtie@teorfys.lu.se
  • Andreas.Wacker@fysik.lu.se
  • Tonu.Pullerits@chemphys.lu.se
  • §Khadga.Karki@chemphys.lu.se

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Issue

Vol. 96, Iss. 5 — November 2017

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