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Optics Letters

Compact phase-stable design for single- and double-quantum two-dimensional electronic spectroscopy

Alexandra Nemeth, Jaroslaw Sperling, Jürgen Hauer, Harald Friedrich Kauffmann, Franz Milota

Published Oct 21, 2009• 41 citations
Publisher

Abstract

We report a compact, easy to align, and passively phase-stabilized setup for recording two-dimensional (2D) electronic spectra in three different phase-matching directions in the boxcar geometry. Passive phase stabilization is achieved by a diffractive optical element, the use of refractive optics for introducing pulse delays, and the use of common optics for all pulses. Representative 2D spectra correlating single- and double-quantum coherences in a molecular aggregate are presented.

DOI
10.1364/ol.34.003301

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Optical two-dimensional photon-echo spectroscopy is realized with shaped excitation pulses, allowing coherent control of twodimensional spectra. This development enables probing of state-selective quantum decoherence and phase/time sensitive couplings between states. The coherently-controlled two-dimensional photon-echo spectrometer with two pulse shapers is based on a passively stabilized four-beam interferometer with diffractive optic, and allows heterodyne detection of signals with a long-term phase stability of approximately Lambda/100. The two-dimensional spectra of Rhodamine 101 in a methanol solution, measured with unshaped and shaped pulses, exhibit significant differences. We observe in particular, the appearance of fine structure in the spectra obtained using shaped excitation pulses.
Abstract Two-dimensional (2D) spectroscopy uses multiple electromagnetic pulses to infer the properties of a complex system. A paradigmatic class of target systems are molecular aggregates, for which one can obtain information on the eigenstates, various types of static and dynamic disorder and on relaxation processes. However, two-dimensional spectra can be difficult to interpret without precise knowledge of how the signal components relate to microscopic Hamiltonian parameters and system-bath interactions. Here we show that two-dimensional spectroscopy can be mapped in the microwave domain to highly controllable Rydberg quantum simulators. By porting 2D spectroscopy to Rydberg atoms, we firstly open the possibility of its experimental quantum simulation, in a case where parameters and interactions are very well known. Secondly, the technique may provide additional handles for experimental access to coherences between system states and the ability to discriminate different types of decoherence mechanisms in Rydberg gases. We investigate the requirements for a specific implementation utilizing multiple phase coherent microwave pulses and a phase cycling technique to isolate signal components.
Two-dimensional electronic spectroscopy (2DES) can be implemented with different geometries, e.g., BOXCARS, collinear, and pump-probe geometries. The pump-probe geometry has the advantage of overlapping only two beams and reducing phase cycling steps. However, its applications are typically limited to observing the dynamics with single-quantum coherence and population, leaving the challenge to measure the dynamics of the double-quantum (2Q) coherence, which reflects the many-body interactions. We demonstrate an experimental technique in 2DES under pump-probe geometry with a designed pulse sequence and the signal processing method to extract 2Q coherence. In the designed pulse sequence, with the probe pulse arriving earlier than the pump pulses, our measured signal includes the 2Q signal as well as the zero-quantum signal. With phase cycling and data processing using causality enforcement, we extract the 2Q signal. The proposal is demonstrated with rubidium atoms. We observe the collective resonances of two-body dipole-dipole interactions in both the D1 and D2 lines.
Double-quantum two-dimensional (2D) coherent spectroscopy (MDCS) is a powerful optical method that is used to study the optical properties of atomic and complex molecular systems and semiconductor materials. Double-quantum 2D spectra and particularly the peak line shapes on the spectra can also provide information about many-body interactions. We model 2D spectra by solving the optical Bloch equations and show the effects of correlation between coupled resonances, which also explains the discrepancies between the experimental results reported by multiple groups.