Hsieh Ming-Hsiu, Krotz Alex, Tempelaar Roel
Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois60208, United States.
J Phys Chem Lett. 2023 Feb 9;14(5):1253-1258. doi: 10.1021/acs.jpclett.2c03724. Epub 2023 Jan 31.
Mean-field mixed quantum-classical dynamics could provide a much-needed means to inexpensively model quantum electrodynamical phenomena by describing the optical field and its vacuum fluctuations classically. However, this approach is known to suffer from an unphysical transfer of energy out of the vacuum fluctuations when the light-matter coupling becomes strong. We highlight this issue for the case of an atom in an optical cavity and resolve it by introducing an additional set of classical coordinates to specifically represent vacuum fluctuations whose light-matter interaction is scaled by the instantaneous ground-state population of the atom. This not only rigorously prevents the aforementioned unphysical energy transfer but is also shown to yield a radically improved accuracy in terms of the atomic population and the optical field dynamics, generating results in excellent agreement with full quantum calculations. As such, the resulting method emerges as an attractive solution for the affordable modeling of strong light-matter coupling phenomena involving macroscopic numbers of optical modes.
平均场混合量子 - 经典动力学可以提供一种急需的方法,通过经典地描述光场及其真空涨落,以低成本对量子电动力学现象进行建模。然而,当光与物质的耦合变强时,这种方法会出现从真空涨落中无物理意义地转移能量的问题。我们针对光学腔中原子的情况突出了这个问题,并通过引入一组额外的经典坐标来解决它,这些坐标专门用于表示其与物质相互作用按原子瞬时基态布居数缩放的真空涨落。这不仅严格防止了上述无物理意义的能量转移,而且在原子布居数和光场动力学方面也显示出显著提高的精度,产生的结果与全量子计算非常吻合。因此,由此产生的方法成为一种有吸引力的解决方案,可用于对涉及大量光学模式的强光与物质耦合现象进行经济实惠的建模。