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首页> 外文会议>Nonlinear Optics and Its Applications VIII; and Quantum Optics III >Engaging new dimensions in nonlinear optical spectroscopy using auxiliary beams of light
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Engaging new dimensions in nonlinear optical spectroscopy using auxiliary beams of light

机译：使用辅助光束在非线性光谱学中开拓新的领域

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By applying a sufficiently intense beam of off-resonant light, simultaneously with a conventional excitation source beam, the efficiencies of one- and two-photon absorption processes may be significantly modified. The nonlinear mechanism that is responsible, known as laser modified absorption, is fully described by a quantum electrodynamical analysis. The origin of the process, which involves stimulated forward Rayleigh-scattering of the auxiliary beam, relates to higher order terms which are secured by a time-dependent perturbation treatment. These terms, usually inconsequential when a single beam of light is present, become prominent under the secondary optical stimulus - even with levels of intensity that are moderate by today's standards. Distinctive kinds of behaviour may be observed for chromophores fixed in a static arrangement, or for solution- or gas-phase molecules whose response is tempered by a rotational average of orientations. In each case the results exhibit an interplay of factors involving the beam polarisations and the molecular electronic response. Special attention is given to interesting metastable states that are symmetry forbidden by one- or two-photon absorption. Such states may be accessible, and thus become populated, on input of the auxiliary beam. For example, in the one-photon absorption case, terms arise that are more usually associated with three-photon processes, corresponding to very different selection rules. Other kinds of metastable state also arise in the two-photon process, and measuring the effect of applying the stimulus beam to absorbances of such character adds a new dimension to the information content of the associated spectroscopy. Finally, based on these novel forms of optical nonlinearity, there may be new possibilities for quantum non-demolition measurements.
机译：通过与常规激发源光束同时施加足够强的非共振光束，可以显着改善单光子吸收过程和双光子吸收过程的效率。通过量子电动力学分析充分描述了负责的非线性机制，即激光修正吸收。该过程的起源涉及到辅助光束的前向瑞利散射，涉及到高阶项，这些项通过基于时间的扰动处理得到保证。这些术语在出现单光束时通常不重要，在次级光学刺激下会变得显着-即使其强度水平符合当今的标准。对于固定在静态排列中的发色团，或者对于其响应受取向旋转平均值调节的溶液或气相分子，可以观察到不同的行为。在每种情况下，结果都显示出涉及光束极化和分子电子响应的因素之间的相互作用。特别注意有趣的亚稳态，该状态被一或两个光子吸收所禁止。在辅助光束的输入下，这样的状态可能是可访问的，并因此被填充。例如，在单光子吸收的情况下，出现的术语通常与三光子过程相关，对应于非常不同的选择规则。在双光子过程中还会出现其他类型的亚稳态，并且测量将刺激光束应用于此类特征的吸光度的效果将为关联光谱的信息内容增加新的维度。最后，基于光学非线性的这些新颖形式，可能会有量子非爆破测量的新可能性。

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