Bouakline Foudhil
Institut für Chemie , Universität Potsdam , Karl-Liebknecht-Str. 24-25 , D-14476 Potsdam-Golm , Germany.
J Phys Chem Lett. 2018 May 3;9(9):2271-2277. doi: 10.1021/acs.jpclett.8b00607. Epub 2018 Apr 18.
We report strong evidence of Berry phase effects in intense laser dissociation of D molecules, manifested as Aharonov-Bohm-like oscillations in the photofragment angular distribution (PAD). Our calculations show that this interference pattern strongly depends on the parity of the diatom initial rotational state, (-1) . Indeed, the PAD local maxima (minima) observed in one case ( j odd) correspond to local minima (maxima) in the other case ( j even). Using simple topological arguments, we clearly show that such interference conversion is a direct signature of the Berry phase. The sole effect of the latter on the rovibrational wave function is a sign change of the relative phase between two interfering components, which wind in opposite senses around a light-induced conical intersection (LICI). Therefore, encirclement of the LICI leads to constructive ( j odd) or destructive ( j even) self-interference of the initial nuclear wavepacket in the dissociative limit. To corroborate our theoretical findings, we suggest an experiment of strong-field indirect dissociation of D molecules, comparing the PAD of the ortho and para molecular species in directions nearly perpendicular to the laser polarization axis.
我们报告了在D分子的强激光解离中存在贝里相位效应的有力证据,其表现为光碎片角分布(PAD)中类似阿哈罗诺夫 - 玻姆的振荡。我们的计算表明,这种干涉图样强烈依赖于双原子初始转动状态的宇称,即(-1)^j 。实际上,在一种情况(j为奇数)中观察到的PAD局部最大值(最小值)对应于另一种情况(j为偶数)中的局部最小值(最大值)。通过简单的拓扑论证,我们清楚地表明这种干涉转换是贝里相位的直接特征。后者对振转波函数的唯一影响是两个干涉分量之间相对相位的符号变化,这两个分量围绕光诱导锥形交叉点(LICI)以相反方向缠绕。因此,在解离极限下,LICI的环绕导致初始核波包的相长干涉(j为奇数)或相消干涉(j为偶数)。为了证实我们的理论发现,我们建议进行一个D分子的强场间接解离实验,比较正、仲分子种类在几乎垂直于激光偏振轴方向上的PAD。