Vibrational Exciton Decay in Uranyl Crystals by Picosecond Coherent Raman Scattering: Energy Bottlenecks and High Order Relaxation Mechanisms

摘要: Anharmonicity in the crystal potential leads to phonon interactions which result vibrational relaxation and dephasing. For many systems a satisfactory description of is obtained by considering first anharmonic correction potential, namely cubic interaction. However, recent results on vibrationally sparse have shown that next higher order term (i.e quartic) necessary account for observed thermally induced dephasing [1–3]. In this work we focus importance mechanisms creating large energy gap. One expects mode immediately above gap an increased lifetime relative other modes molecule due absence any decay channels.