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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Nonlinear optical processes in Rydberg atoms systems

Eduard A. Manykin

Published May 30, 2002• 1 citation
Publisher

Abstract

The interaction between Rydberg systems [Rydberg atoms (RA) gas or Rydberg matter (RM)] and coherent light in various frequency bands is considered. It is shown why Rydberg systems possess a greater polarizabilities and, accordingly, linear and nonlinear susceptibilities and strong sensitive to high-1 (circular) Rydberg states in RA and RM. Quantum theory of physical and chemical properties of RA and RM are related with recent obtained results on the optical spectroscopy. The experimental data of Raman processes, wave mixing effects in gas of RA, and their clusters of RM are analyzed. Problem of blueshifts and stimulated electronic laser Raman processes, as well as four wave mixing in RM are discussed.

DOI
10.1117/12.468941

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The interaction between Rydberg systems [Rydberg atoms (RA) gas or Rydberg matter (RM)] and coherent light in various frequency bands is considered. It is shown why Rydberg systems possess a greater polarizabilities and, accordingly, linear and nonlinear susceptibilities and strong sensitive to high-1 (circular) Rydberg states in RA and RM. Quantum theory of physical and chemical properties of RA and RM are related with recent obtained results on the optical spectroscopy. The experimental data of Raman processes, wave mixing effects in gas of RA, and their clusters of RM are analyzed. Problem of blueshifts and stimulated electronic laser Raman processes, as well as four wave mixing in RM are discussed.
A brief state-of-art review of the research into the interaction of laser radiation with Rydberg atoms and clusters of Rydberg atoms is provided. The dynamics of various Rydberg species in a high-frequency optical field is described with the use of the quantum-mechanical approach. Experimental data indicating the existence of Rydberg-state species (Rydberg clusters and Rydberg matter) are analyzed. A special emphasis is placed on Raman processes in Rydberg atoms and Rydberg matter created on solid surfaces.
Wave-number blueshifts of single-mode laser light in low-density Rydberg matter are found to be due to stimulated Raman processes. The Rydberg matter is mainly formed from Rydberg states of K atoms. The lasers used are mW continuous-wave lasers in the ir, lead-salt tunable diode lasers. Of special significance is the blueshifting observed as shifts of Fabry-Perot etalon fringes of the order of 0.05 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$. This blueshifting is explained as due to complete conversion to anti-Stokes radiation through higher-order stimulated Raman shifting by extremely small quanta from the near continuum of energy levels in the metallic Rydberg matter phase. Complicated strong shifts of intensity to larger wave numbers in the laser modes are also observed, due to coupling of laser side modes to the anti-Stokes waves. The high efficiency of the stimulated Raman process is partly due to the weak coupling to other degrees of freedom.
Abstract Rydberg atoms, characterized by their giant polarizability and strong long-range interactions, provide an ideal platform for exploring optical nonlinearities. By coupling light to ensembles of Rydberg atoms, one can map the strong and nonlocal interactions between Rydberg atoms and light fields. A particularly important scheme for realizing such nonlinearity is electromagnetically induced transparency (EIT). This article presents a review of the research progress in nonlinear optics based on Rydberg-EIT systems, particularly nonlinear light propagation in Rydberg atomic gases. We first introduce the fundamental properties of Rydberg atoms and the physical mechanism of EIT-enhanced nonlinearity, emphasizing how the Rydberg blockade effect endows the system with a giant nonlocal Kerr nonlinearity. Subsequently, we discuss some typical nonlinear optical phenomena in such a system with focusing and defocusing nonlocal nonlinearities. In the focusing regime, we discuss spatial solitons, vortex solitons, soliton cloning, soliton molecules, optical bullets, and self-induced transparency solitons. Other topics are also discussed. In the defocusing regime, we analyze pattern formation and shock wave dynamics. Finally, we provide an outlook on the future development of this field toward quantum control, hybrid-system integration, and novel functional devices.
We present experimental results on nondegenerate four-wave mixing in a thermal vapor cell of rubidium atoms via highly excited Rydberg states. We observe sub-Doppler spectral features and a large sensitivity of the mixed light mode to small electric fields due to the large polarizabilities of the involved Rydberg state. We observe a saturation of the optical response due to the nonlinear four-level physics. The strong interaction between Rydberg atoms and the associated Rydberg blockade could potentially increase the nonlinearity dramatically.
Subject of this thesis is the theoretical investigation of ensembles of atoms that are coherently laser-excited to a Rydberg state. Rydberg excited atoms interact with each other over large distances, which leads to strongly correlated many-body dynamics, demanding powerful numerical tools for their modeling. The first part of the thesis deals with effective two-level atoms consisting of a ground and a Rydberg state only. For resonant laser excitation a modified scaling behavior of the excitation number is observed, which is caused by effects of finite system size and coarse graining of the medium due to the finite atomic density. For off-resonant excitation, ordered structures arise out of an initially homogeneous gas, which are reflected in strongly peaked spatial correlations and modified excitation statistics. In the second part a fast decaying intermediate level is additionally taken into account. In this situation the phenomenon of electromagnetically induced transparency (EIT) is encountered. This effect is suppressed in the presence of strong interactions between the Rydberg atoms leading to an optical nonlinearity. A model predicting the properties of a cloud of Rydberg atoms in EIT configuration is developed. In both parts the models are validated by comparing their predictions to recent experimental observations.