Manipulating optical nonlinearities of molecular polaritons by delocalization
Manipulating optical nonlinearities of molecular polaritons by delocalization
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DOI：
10.1126/sciadv.aax5196
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发表时间：
2019-09-01
期刊：
影响因子：
13.6
通讯作者：
Xiong, Wei
中科院分区：
文献类型：
--
作者：
Xiang, Bo;Ribeiro, Raphael F.;Xiong, Wei
光学非线性是当代光子学工具箱中的关键资源，与量子门操作和全光开关有关。化学改性通常用于在微观水平上控制材料的非线性响应，但对这种响应的动态操作具有挑战性。中红外（IR）光学非线性的可调性更不发达，阻碍了其在化学传感或红外光子电路中的应用。在这里，我们报告了通过操纵宏观参数如腔纵向长度或分子浓度来控制振动极化子相干非线性。进一步的二维红外研究表明，非线性消相是观测到的超快极化子非线性的主要来源。所报道的现象源于微观分子激发与宏观光子腔模式之间的强耦合所引起的非线性宏观极化。
Optical nonlinearities are key resources in the contemporary photonics toolbox, relevant to quantum gate operations and all-optical switches. Chemical modification is often used to control the nonlinear response of materials at the microscopic level, but on-the-fly manipulation of such response is challenging. Tunability of optical nonlinearities in the mid-infrared (IR) is even less developed, hindering its applications in chemical sensing or IR photonic circuitry. Here, we report control of vibrational polariton coherent nonlinearities by manipulation of macroscopic parameters such as cavity longitudinal length or molecular concentration. Further two-dimensional IR investigations reveal that nonlinear dephasing provides the dominant source of the observed ultrafast polariton nonlinearities. The reported phenomena originate from the nonlinear macroscopic polarization stemming from strong coupling between microscopic molecular excitations and a macroscopic photonic cavity mode.