Manipulation of two-dimensional spectra of excitonically coupled molecules by narrow-bandwidth laser pulses

被引：31

作者：

Abramavicius, D. ^{[1
,2
]}

Butkus, V. ^{[1
]}

Bujokas, J. ^{[1
]}

Valkunas, L. ^{[1
,2
]}

机构：

[1] Vilnius Univ, Dept Theoret Phys, Fac Phys, LT-10222 Vilnius, Lithuania

[2] Inst Phys, LT-02300 Vilnius, Lithuania

来源：

CHEMICAL PHYSICS | 2010年 / 372卷 / 1-3期

关键词：

Optical two-dimensional spectroscopy; Laser pulse shaping and manipulation; ELECTRONIC SPECTROSCOPY; OPTICAL SPECTROSCOPY; COHERENCE; DYNAMICS; SYSTEMS; COMPLEX;

D O I：

10.1016/j.chemphys.2010.04.015

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Complete expressions within the response function theory are derived for a coherent two-dimensional (2D) signal covering the finite-bandwidth and pulse-overlap effects. Ideal time domain, frequency domain as well as mixed regime are considered. Conditions for the strong pulse-overlap effects are also described and analyzed. As demonstrated for the excitonically coupled dimer, certain configurations of central frequencies allow to extract various peaks in the 2D signal, resembling certain physical processes. In the case of weakly overlapping pulses, the scheme for generating both ultra-broad-bandwidth time-domain signal and frequency-domain spectra from a set of narrow-bandwidth multi-color measurements is presented. Possibility of reconstructing microscopic parameters such as inter-molecular couplings and transition dipole orientations from high-resolution crosspeaks is discussed. (C) 2010 Elsevier B. V. All rights reserved.

引用

页码：22 / 32

页数：11

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