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Physical Review A

All-optical processing in coherent nonlinear spectroscopy

Dan Oron, Nirit Dudovich, Yaron R. Silberberg

Published Aug 31, 2004• 35 citations
Publisher

Abstract

In spectroscopy, the fingerprint of a substance is usually comprised of a sequence of spectral lines with characteristic frequencies and strengths. Identification of substances often involves postprocessing, where the measured spectrum is compared with tabulated fingerprint spectra. Here we suggest a scheme for nonlinear spectroscopy, where, through coherent control of the nonlinear process, the information from the entire spectrum can be practically collected into a single coherent entity. We apply this for all-optical analysis of coherent Raman spectra and demonstrate enhanced detection and effective background suppression using coherent processing.

DOI
10.1103/physreva.70.023415

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In spectroscopy, the fingerprint of a substance is usually comprised of a sequence of spectral lines with characteristic frequencies and strengths. Identification of substances often involves postprocessing, where the measured spectrum is compared with tabulated fingerprint spectra. Here we suggest a scheme for nonlinear spectroscopy, where, through coherent control of the nonlinear process, the information from the entire spectrum can be practically collected into a single coherent entity. We apply this for all-optical analysis of coherent Raman spectra and demonstrate enhanced detection and effective background suppression using coherent processing.
Phase-and-polarization coherent control is applied to control the nonlinear response of a quantum system. We use it to obtain high-resolution background-free single-pulse coherent anti-Stokes Raman spectra. The ability to control both the spectral phase and the spectral polarization enables measurement of a specific off-diagonal susceptibility tensor element while exploiting the different spectral response of the resonant Raman signal and the nonresonant background to achieve maximal background suppression.
Optical multidimensional coherent spectroscopy is a powerful tool for studying structure and dynamics in complex systems, such as semiconductors. In optical two-dimensional coherent spectroscopy (2DCS), where the spectrum is presented in a two-dimensional (2D) plane with two frequency axes, an important advantage is the ability to isolate quantum pathways by unfolding a one-dimensional spectrum onto a 2D plane. For many systems, however, the quantum pathways are only partially separated in a 2D spectrum. In order to completely isolate the quantum pathways, we extend 2DCS into a third dimension to generate three-dimensional (3D) spectra in which the spectrum is further unfolded. A 3D spectrum provides complete and well-isolated information of the third-order optical response of the system. The information can be used to fully characterize the quantum pathways and to determine the system’s Hamiltonian. Quantitative knowledge of the Hamiltonian enables prediction and control of quantum processes. For instance, such information is essential for deterministic control and improved performance of coherent control schemes.
Nonlinear spectroscopic method based on degenerate four-wave mixing allows unusually sensitive measurement of isotopes and hyperfine profiles with sub-Doppler spectral resolution. Compared to other isotope capable methods including mass spectrometry, wave mixing offers a simple, more cost effective approach with minimal sample preparation steps. Since no two hyperfine profiles are alike, hyperfine-based isotope analysis offers unambiguous isotope information. Unlike mass-based methods such as mass spectrometry, frequency-based wave-mixing spectroscopy offers more information rich spectra. A non-planar 3-D wave-mixing optical setup generates a coherent signal beam in its own space and propagation direction. Hence, virtually 100% of the signal can be collected and detected conveniently. Using compact solid-state lasers and popular atomizers, a wave-mixing setup is relatively compact. Sub-Doppler spectral resolution can be further enhanced by using simple low-pressure atomizers. Ultrasensitive fingerprinting of important isotopes promises many potential applications.