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Optics Letters

Degenerate four-wave mixing spectroscopy based on two-dimensional femtosecond pulse shaping

Thomas Hornung, Joshua C. Vaughan, Thomas Feurer, Keith Adam Nelson

Published Sep 1, 2004• 55 citations
Publisher

Abstract

We report noncollinear, degenerate four-wave mixing experiments that employ a new device based on two-dimensional femtosecond pulse shaping that delays and modulates all incident fields. Heterodyne detection is easily implemented due to the full phase stability of the device.
DOI
10.1364/ol.29.002052

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We present a time-resolved study of the diffracted pulse in degenerate four-wave mixing experiments with short-response-time materials. The first step is the validation of a theoretical model that takes into account the temporal characteristics of the energy level (relaxation time T1 and dephasing time T2) and of the incident pulse (duration and spectral phase) in a simple particular case. Two methods are used for characterizing the diffracted beam: the amplitude correlation with the reference pulse and the spectrum intensity measurements. We discuss the experimental results, which show good agreement with the theoretical model and evidence the strong influence of the incident pulse characteristics.
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.
Multiple-quantum two-dimensional Fourier transform optical (2D FTOPT) spectroscopy was developed and conducted on GaAs quantum wells. Spatiotemporal femtosecond pulse shaping was used to control the optical phases and time delays of ultrashort pulses in multiple non-collinear beams so that fully coherent four-wave and higher-order mixing measurements could be conducted without delay stages, multiple interferometers, or any active phase control. Coherences of biexcitons, unbound but correlated exciton pairs, and excitons undergoing rephasing were observed directly.