Ultrafast Intense Molecular Photonics-from Femto to Attosecond Laser Chemistry

我们基于三个基本的PDE，s（部分差分方程）：TDSE（时变薛定谔方程），它的相对论版本TDDE（时变狄拉克方程）和激光麦克斯韦方程探索了新的非微扰模型和模拟。数值解涵盖核飞秒（1fs=10**-15s）到电子阿秒（1asec =10**-18s）。加拿大计算机公司的大存储计算机允许在新问题上进行“数值实验”，在超快强激光应用到超快成像、可视化和上述时间尺度上的物质控制中的非扰动问题。我们的研究将发展分子对新的asec“圆”极化脉冲的非线性响应的建模和模拟，这是我们在1995年的论文中提出的。目前在光子学领域的激光研究还局限于线偏振。我们在1995年提出了使用双色共和反旋转圆形脉冲来产生圆形HHG（高次谐波产生）和“圆形”极化asec脉冲的新工具，用于产生量子电子“圆电流”的相干叠加，而不是相干控制和量子信息中的固定量子态。我们最初提出的增强圆形HHG作为圆形“asec”脉冲的新来源的建议将在理论上进行更详细的研究，并在数值上探索和包括科里奥利相互作用，圆形激光感应电流在分子内部产生的强磁场，相对论效应，如自旋轨道相互作用的增强。特别是将重点研究3个新的方向：(1)-手性-相反的激光场螺旋度产生不同方向的电流，这些电流由于弱激光磁场而非常小。测量手性分子几何需要更高的场强，这将产生强电流和自身的磁场，这在手性模型中从未被考虑过，我们将对此进行详细的研究。(2)-圆形x射线-双色圆形脉冲的圆形HHG将作为脉冲频率，形状和强度的函数进行研究，以优化圆极化x射线的产生，这种x射线将用于电离核心电子，用于新的超快化学反应。强红外脉冲的加入将被研究以促进邻近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。圆形脉冲[2]最强。我们在发展；在计算加拿大，利用我们自己的分裂算子方法编制了一个新的相对论性分子TDDE代码，其中包括新科学-原子化学-电子自旋，多光子动量交换，[2]s . chelkowski，AD. (2017)；刘建军，刘建军，物理学报，33(5):444 - 444（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).