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

TY - JOUR

T1 - Two-dimensional action spectroscopy of excitonic systems

T2 - Explicit simulation using a phase-modulation technique

AU - Damtie, Fikeraddis A.

AU - Wacker, Andreas

AU - Pullerits, Tõnu

AU - Karki, Khadga J.

N1 - Publisher Copyright: © 2017 American Physical Society.

PY - 2017/11/13

Y1 - 2017/11/13

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=85036611691&partnerID=8YFLogxK

U2 - 10.1103/PhysRevA.96.053830

DO - 10.1103/PhysRevA.96.053830

M3 - 文章

AN - SCOPUS:85036611691

SN - 2469-9926

VL - 96

JO - Physical Review A

JF - Physical Review A

IS - 5

M1 - 053830

ER -