标题： 非马尔可夫效应在长程极化子介导的能量转移中的作用 显示英文标题

标题： Non-Markovian effects in long-range polariton-mediated energy transfer

摘要： 分子内能量转移由近场效应驱动，在生物物理、化学、纳米光学和量子通信等应用中起着重要作用。分子系统中强光-物质耦合的进展为控制能量转移开辟了新可能性。特别是，分子之间的远距离能量转移已被报道为它们相互耦合到腔光子模式的结果，并形成了混合极化子状态。除了对光的强耦合外，分子系统还表现出电子和振动模式之间的强相互作用。后者可以作为能量的储存库，以促进非共振跃迁，并因此促进不同能量的极化子态之间的能量弛豫。然而，这些模式的非马尔可夫性质使得准确模拟这些效应具有挑战性。在这里，我们通过过程张量矩阵乘积算子（PT-MPO）方法来捕捉这些效应，以精确描述分子的振动环境，并结合光-物质相互作用的平均场处理。特别是，我们研究了一个由两个空间分离的不同种类分子层耦合到共同光子模式的系统的发射动力学，并表明与振动浴的耦合强度在控制发射光的能量动力学中起着关键作用；在强振动耦合下，这种动力学表现出强烈的非马尔可夫效应，最终导致极化子的形成。我们的结果为极化子长程能量转移提供了见解，并进一步理解了与分子极化子学这一快速增长领域相关的振动模式的作用。 显示英文摘要

摘要： Intramolecular energy transfer driven by near-field effects plays an important role in applications ranging from biophysics and chemistry to nano-optics and quantum communications. Advances in strong light-matter coupling in molecular systems have opened new possibilities to control energy transfer. In particular, long-distance energy transfer between molecules has been reported as the result of their mutual coupling to cavity photon modes, and the formation of hybrid polariton states. In addition to strong coupling to light, molecular systems also show strong interactions between electronic and vibrational modes. The latter can act as a reservoir for energy to facilitate off-resonant transitions, and thus energy relaxation between polaritonic states at different energies. However, the non-Markovian nature of those modes makes it challenging to accurately simulate these effects. Here we capture them via process tensor matrix product operator (PT-MPO) methods, to describe exactly the vibrational environment of the molecules combined with a mean-field treatment of the light-matter interaction. In particular, we study the emission dynamics of a system consisting of two spatially separated layers of different species of molecules coupled to a common photon mode, and show that the strength of coupling to the vibrational bath plays a crucial role in governing the dynamics of the energy of the emitted light; at strong vibrational coupling this dynamics shows strongly non-Markovian effects, eventually leading to polaron formation. Our results shed light on polaritonic long-range energy transfer, and provide further understanding of the role of vibrational modes of relevance to the growing field of molecular polaritonics.