首页> 外文OA文献 >Nonlinear optical response in condensed phases: A microscopic theory using the multipolar Hamiltonian
【2h】

Nonlinear optical response in condensed phases: A microscopic theory using the multipolar Hamiltonian

机译:凝聚相中的非线性光学响应:使用多极哈密顿量的微观理论

摘要

A general scheme is presented for calculating the nonlinear optical response in condensed phases that provides a unified picture of excitons, polaritons, retardation, and local-field effects in crystals and in disordered systems. A fully microscopic starting point is taken by considering the evolution of the quantized radiation-matter system described by the multipolar (µ•D┴) Hamiltonian. For a molecular system with localized electronic states we derive equations of motion in which the instantaneous intermolecular interactions are explicitly recovered and the interaction with the Maxwell electric field is of the µ•E┴ type. It is shown that with total neglect of retardation, these equations lead to the usual expressions for nonlinear optical susceptibilities in terms of equilibrium correlation functions of the polarization field of the molecular system. A mean-field approximation for these equations of motion yields the commonly used local-field expression. Finally, a procedure is proposed for calculating the optical response that fully accounts for retardation, based on a hierarchy of equations of motion for polaritons.
机译:提出了一种用于计算凝聚相中非线性光学响应的​​通用方案,该方案可提供晶体和无序系统中激子,极化子,延迟和局部场效应的统一图像。通过考虑由多极(µ•D┴)哈密顿量描述的量化辐射物质系统的演化,可以得出一个完全微观的起点。对于具有局部电子态的分子系统,我们导出运动方程,其中瞬时分子间相互作用被明确恢复,并且与麦克斯韦电场的相互作用为μ•E┴型。结果表明,在完全忽略延迟的情况下,这些方程式根据分子系统极化场的平衡相关函数得出了非线性光学磁化率的常用表达式。这些运动方程的平均场近似产生了常用的局部场表达式。最后,根据极化子运动方程的层次,提出了一种计算光学响应的​​程序,该程序可完全解决延迟问题。

著录项

相似文献

  • 外文文献
  • 中文文献
  • 专利

客服邮箱:kefu@zhangqiaokeyan.com

京公网安备:11010802029741号 ICP备案号:京ICP备15016152号-6 六维联合信息科技 (北京) 有限公司©版权所有
  • 客服微信

  • 服务号