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Physical Review Letters

Nonlinear Optical Processes by Van der Waals Interaction during Collision

Stephen E. Harris, D. B. Lidow

Published Sep 16, 1974• 83 citations
Publisher

Abstract

We describe an optical process where off-diagonal optical excitation of a first atomic species is coupled during collision to a second species. This coupling leads to new types of nonlinear optical processes, and allows large cross sections for inelastic collision between atoms with nonresonant energy levels.
DOI
10.1103/physrevlett.33.674

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We discuss laser-dressed dipolar and van der Waals interactions between atoms and polar molecules, so that a cold atomic gas with laser admixed Rydberg levels acts as a designed reservoir for both elastic and inelastic collisional processes. The elastic scattering channel is characterized by large elastic scattering cross sections and repulsive shields to protect from close encounter collisions. In addition, we discuss a dissipative (inelastic) collision where a spontaneously emitted photon carries away (kinetic) energy of the collision partners, thus providing a significant energy loss in a single collision. This leads to the scenario of rapid thermalization and cooling of a molecule in the mK down to the μK regime by cold atoms.
We measure inelastic cross sections for atomic thorium (Th) and molecular thorium monoxide (ThO) in collisions with 3^33He at temperatures near 1 K. We determine the Zeeman relaxation cross section for Th (3^33F2_22​) to be sim2times10−17\\sim 2 \\times 10^{-17}sim2times10−17~cm−2^{-2}−2 at 800~mK. We study electronic inelastic processes in Th (3^33P0_00​) and find no quenching even after 10610^6106 collisions at 800~mK. We measure the vibrational quenching cross section for ThO~(X,~nu=1\\nu=1nu=1) to be (7.9pm2.7)times10−19(7.9 \\pm 2.7) \\times 10^{-19}(7.9pm2.7)times10−19~cm−2^{-2}−2 at 800~mK. Finally, we observe indirect evidence for ThO (X, nu=0\\nu=0nu=0)--3^33He van der Waals complex formation, and measure the 3-body recombination rate constant to be Gamma3=(8pm2)times10−33\\Gamma_3 = (8 \\pm 2) \\times 10^{-33}Gamma3​=(8pm2)times10−33~cm6^66s−1^{-1}−1 at 2.4~K. The stability of the ground Th (3^33F2_22​) state, metastable Th (3^33P0_00​) state, and vibrational excited ThO (X, nu=1\\nu=1nu=1) state provides data on anisotropic interactions in new systems and opens up the possibility for further studies and experiments, including trapping.
The effect of atomic collisions on the optical characteristics of an ensemble of excited atoms is well known [ 1 , 2 ]. The evolution of laser techniques and the resulting interest in various nonlinear-spectroscopy methods have suggested that atomic collisions have a significant effect on the lasing mode of gas lasers and the shape and width of various nonlinear signals. For a long time attention has been focused on the important role of elastic collisions, among other things, and various methods have been proposed for describing such collisions [ 3 ].
A two-level model of an atomic system is investigated in order to study the cross section for certain inelastic collision processes. An impact-parameter method is employed. The time-dependent Schr\"odinger equation has been integrated numerically for some simple interaction potentials. Cross sections for excitation have been determined and are presented as functions of the parameters describing the model. The results are compared with those obtained by certain approximate methods. The effects of inclusion of diagonal matrix elements in the interaction Hamiltonian are found to be large. For a fixed form of the interaction potential, two cross sections, which may differ quite substantially, are obtained, depending on the algebraic sign of the coupling parameters or the energy difference between the states.