论文标题
激发态振动极化子介导的UV/VIS-TO-IR光子下调转换
UV/vis-to-IR Photonic Down Conversion Mediated by Excited State Vibrational Polaritons
论文作者
论文摘要
这项工作提出了一种新的光物理现象，通过该现象，涉及Franck-Condon（FC）主动振动的分子的UV/VIV/VIS激发可通过强耦合到光腔，从而产生红外（IR）发射。所得的UV/VIS-TO-IR光子下调转换过程是由电子激发状态电位中的振动极化子介导的。结果表明，仅在具有非零FC活性和激发态的IR活性的分子时，通过UV/VIS激发形成了这种激发态振动偏振子（ESVP）。密度功能理论的计算显示出具有该特性和ESVP动力学的候选分子1-甲基酸（PAA）的有效鉴定，并使用截短的Wigner近似进行建模。总体而言，这项工作提出了北极星化学的新途径，在光激发的驱动下，激发状态动力学受到振动偏振子的形成。随之而来的是，光子降低转化率在激发态振动和量子转导方案中都具有潜在有用。
This work proposes a new photophysical phenomenon whereby UV/vis excitation of a molecule involving a Franck-Condon (FC) active vibration yields infrared (IR) emission by strong coupling to an optical cavity. The resulting UV/vis-to-IR photonic down conversion process is mediated by vibrational polaritons in the electronic excited state potential. It is shown that the formation of such excited state vibrational polaritons (ESVP) via UV/vis excitation only occurs with molecules having vibrational modes with both a non-zero FC activity and IR activity in the excited state. Density functional theory calculations are shown to effectively identify a candidate molecule, 1-Pyreneacetic acid (PAA), with this property and the dynamics of ESVP are modeled using the truncated Wigner approximation. Overall, this work presents a new avenue of polariton chemistry where excited state dynamics, driven by photoexcitation, are influenced by the formation of vibrational polaritons. Along with this, the photonic down conversion is potentially useful in both the sensing of excited state vibrations and in quantum transduction schemes.
