Department of Chemistry, Washington State University, Pullman, WA 99164, USA.
Int J Mol Sci. 2023 Apr 19;24(8):7490. doi: 10.3390/ijms24087490.
Our understanding of molecules has stagnated at a single quantum system, with atoms as Newtonian particles and electrons as quantum particles. Here, however, we reveal that both atoms and electrons in a molecule are quantum particles, and their quantum-quantum interactions create a previously unknown, newfangled molecular property-supracence. Molecular supracence is a phenomenon in which the molecule transfers its potential energy from quantum atoms to photo-excited electrons so that the emitted photon has more energy than that of the absorbed one. Importantly, experiments reveal such quantum energy exchanges are independent of temperature. When quantum fluctuation results in absorbing low-energy photons, yet still emitting high-energy photons, supracence occurs. This report, therefore, reveals novel principles governing molecular supracence via experiments that were rationalized by full quantum (FQ) theory. This advancement in understanding predicts the super-spectral resolution of supracence, and molecular imaging confirms such innovative forecasts using closely emitting rhodamine 123 and rhodamine B in living cell imaging of mitochondria and endosomes.
我们对分子的理解一直停留在单个量子体系中，其中原子是牛顿粒子，电子是量子粒子。然而，在这里，我们揭示了分子中的原子和电子都是量子粒子，它们的量子-量子相互作用创造了一种以前未知的、新颖的分子特性——超激发。分子超激发是一种现象，其中分子将其势能从量子原子转移到光激发电子，从而使发射的光子具有比吸收的光子更高的能量。重要的是，实验表明这种量子能量交换与温度无关。当量子涨落导致吸收低能量光子，但仍发射高能量光子时，就会发生超激发。因此，本报告通过实验揭示了分子超激发的新原理，这些实验通过全量子（FQ）理论得到了合理化。这一理解上的进步预测了超激发的超光谱分辨率，分子成像通过在活细胞中线粒体和内体的 rhodamine 123 和 rhodamine B 的紧密发射证实了这一创新预测。
