Ultrafast Intense Molecular Photonics-from Femto to Attosecond Laser Chemistry

基于三种基本偏微分方程组，S方程、含时薛定谔方程及其相对论版本的含时狄拉克方程和激光麦克斯韦方程，我们探索了新的非微扰模型和模拟。数值解涵盖了核飞秒(1fs=10**-15s)和电子阿秒(1asEC=10**-18s)。加拿大计算机公司S大内存计算机允许对超快激光在超快成像、物质可视化和物质控制应用中的新问题和非微扰问题进行数值实验。我们的研究将发展分子对新的ASEC的非线性响应的建模和模拟，如我们在1995年的论文[1]中所建议的那样。目前光子学中的强激光研究局限于线偏振。我们在1995年提出使用双色同向和反向旋转的圆脉冲来产生环形HHG(高次谐波产生)和“圆”极化的ASEC脉冲，在相干控制和量子信息中产生量子电子“圆电流”的相干叠加的新工具。分子与强圆极化脉冲的相互作用是科学上的一个新的“篇章”。我们将从理论和数值[1]探索和包括科里奥利相互作用、圆激光诱导电流在分子内部产生的强磁场、相对论效应，如增强自旋-轨道相互作用等，来更详细地研究作为圆形“ASEC”脉冲的新来源的圆形HHG。特别是三个新的研究方向：(1)手性--相反的激光场螺旋产生不同方向的电流，由于激光磁场很弱，电流很小。测量手性分子的几何形状需要更高的场强，这将产生强电流和它们自己的磁场，手性模型中从来没有考虑过这一点，将进行详细的研究。(2)我们将研究双色圆形脉冲产生的环形高次谐波随脉冲频率、形状和强度的变化，以优化循环极化X射线的产生。这种X射线将用于电离核-电子的新的超快化学反应。我们将研究添加强红外脉冲以促进相邻电离核之间的电荷迁移，这是一种以前从未探索过的新效应。(3)光子-电子-核动量交换，是一种新的非绝热分子现象。环形脉冲最强。我们正在开发中；在加拿大计算中，S使用我们自己的分裂算符方法编制了一个新的相对论分子TDDE程序，包括新的科学-阿托化学-电子自旋，多光子动量交换，[1]ADBandrauk，JGuo，KJ袁，JOpt，19,124016(2017)；[2]S.Cherkowski，AD.Bandrauk，PBCorkum，Phys Rev Lett 113,263005(2015)。

We explore new nonperturbative models and simulations which are based on 3 fundamental PDE,s(Partial Diff Eqns):TDSE(Time-Dependent Schroedinger Equation),its relativistic version TDDE(Time-Dependent Dirac Equation) and laser Maxwell equations.The numerical solutions cover nuclear femtoseconds(1fs=10**-15s) to,electron attoseconds(1 asec=10**-18s) .Compute Canada,s large memory computers allow to perform "numerical experiments" on new problems,nonperturbative issues in the applications of ultrafast intense lasers to ultrafast imaging ,visualization and control of matter on the above time scales. Our research will develop modelling and simulations of the nonlinear responses of molecules to new asec "circularly" polarized pulses as proposed in our 1995 paper cited below in [1].Currently intense laser research in Photonics is limited to linear polarization.We have proposed in 1995 using bichromatic co and counter -rotating circular pulses to generate circular HHG(High Order Harmonic Generation) and "circularly" polarized asec pulses , new tools for generating coherent superpositions of quantum electron "circular currents" as opposed to stationary quantum states in Coherent Control and Quantum Information.The interaction of molecules with intense circularly polarized pulses is a new "chapter" in science Our original proposal to enhance circular HHG as new sources of circular "asec "pulses will be investigated in more detail theoretically,and numerically[1] to explore and include Coriolis interactions, intense magnetic fields generated inside molecules from circular laser induced currents ,relativistic effects such as enhancement of spin-orbit interactions. In particular 3 new research directions will be focused on:(1)-Chirality- opposite laser field helicities produce different direction currents which are very small due to weak laser magnetic fields. Measuring chiral molecular geometries requires higher field intensities which will generate strong currents and their own magnetic fields and has never been considered in chirality models and will be investigated in detail. (2)- Circular XRays-Circular HHG from bichromatic circular pulses will be investigated as a function of pulse frequencies ,shapes and intensities to optimize circularly polarize XRay.generation.Such XRays will serve to ionize core-electrons for new ultrafast chemical reactions.The addition of intense IR pulses will be investigated to promote charge migration between neighboring ionized cores ,a new effect never explored before (3)-exchange of photon-electron-nuclear momenta,is a new nonadiabatic molecular phenomenon.strongest with circular pulses[2].We are developping ;in Compute Canada,s programs a new relativistic molecular TDDE code using our own Split-Operator methods to include in the new science-Attochemistry -electron spin,multiphoton momentum exchange,[1]ADBandrauk,JGuo,KJYuan,,JOpt,19,124016(2017);[2]S.Chelkowski,AD.Bandrauk,PBCorkum,Phys Rev Lett 113,263005(2015).