Isolating Polaritonic 2D-IR Transmission Spectra
Isolating Polaritonic 2D-IR Transmission Spectra
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DOI：
10.1021/acs.jpclett.1c03198
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发表时间：
2021-11-25
影响因子：
5.7
通讯作者：
Kubarych, Kevin J.
中科院分区：
文献类型：
--
作者：
Duan, Rong;Mastron, Joseph N.;Kubarych, Kevin J.
共振光学微腔内分子振动跃迁之间的强耦合导致集体离域振动极化激元的形成。极化激元化学有许多潜在的应用，从修饰化学反应到量子信息处理。获得极化激元响应的一个挑战是去除由于产生普通2D-IR光谱的未耦合分子引起的背景贡献，所述普通2D-IR光谱的振幅被极化激元透射光谱过滤。我们发现，振动极化激元的2D-IR光谱中的大多数功能可以解释由这个背景信号和真正的极化激元响应的线性叠加。通过一个简单的校正程序，其中过滤裸分子2D-IR光谱从测量的腔响应中减去，我们恢复的极化激元光谱。
Strong coupling between vibrational transitions in molecules within a resonant optical microcavity leads to the formation of collective, delocalized vibrational polaritons. There are many potential applications of "polaritonic chemistry", ranging from modified chemical reactivity to quantum information processing. One challenge in obtaining the polaritonic response is removing a background contribution due to the uncoupled molecules that generate an ordinary 2D-IR spectrum whose amplitude is filtered by the polariton transmission spectrum. We show that most features in 2D-IR spectra of vibrational polaritons can be explained by a linear superposition of this background signal and the true polariton response. Through a straightforward correction procedure, in which the filtered bare-molecule 2D-IR spectrum is subtracted from the measured cavity response, we recover the polaritonic spectrum.