Ultrafast Intense Molecular Photonics-from Femto to Attosecond Laser Chemistry

超快强分子光子学——从飞秒到阿秒激光化学

• 批准号: RGPIN-2019-05291
• 负责人: Bandrauk, Andre
• 金额: $ 2.62万
• 依托单位: Université de Sherbrooke
• 依托单位国家: 加拿大
• 项目类别: Discovery Grants Program - Individual
• 财政年份: 2022
• 资助国家: 加拿大
• 起止时间: 2022-01-01 至 2023-12-31
• 项目状态: 已结题
• 来源: https://www.nserc-crsng.gc.ca/ase-oro/Details-Detailles_eng.asp?id=748650
• 关键词: Ultrafast; Intense; Molecular; Photonics; Femto

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).

我们探索了新的非微扰模型和模拟，这些模型和模拟是基于三个基本偏微分方程：TDSE（含时薛定谔方程），它的相对论版本TDDE（含时狄拉克方程）和激光麦克斯韦方程。数值解涵盖了核飞秒（1 fs =10**-15 s）到电子阿秒（1 asec=10**-18 s）。计算加拿大的大容量计算机允许在上述时间尺度上对超快强激光应用于超快成像、可视化和控制物质的新问题、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“圆”偏振脉冲的非线性响应的建模和模拟，正如我们在1995年的论文中所提出的。目前光子学中的强激光研究仅限于线偏振。我们在1995年提出了利用双色同向和反向旋转的圆脉冲产生圆高次谐波。（高次谐波产生）和“圆”偏振asec脉冲，在相干控制和量子信息中，产生量子电子“圆电流”相干叠加的新工具，而不是静止量子态。分子与强圆偏振脉冲的相互作用是一个新的“篇章”。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和数值上进行更详细的研究[1]，以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，如增强自旋轨道相互作用。特别是三个新的研究方向将集中在：（1）-手性-相反的激光场螺旋产生不同方向的电流，这是非常小的，由于弱激光磁场。测量手性分子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，并且从未在手性模型中考虑过，并且将被详细研究。(2)-圆形X射线-来自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，以优化圆形HHG X射线的产生。这种X射线将用于为新的超快化学反应提供核心电子。将研究增加强IR脉冲以促进相邻电离核心之间的电荷迁移，（3）光子-电子-核动量交换是一种新的非绝热分子现象，在圆脉冲作用下最强[2]。在加拿大计算中，s使用我们自己的分裂算子方法编制了一个新的相对论分子TDDE代码，以包括在新的科学-原子化学-电子自旋中，多光子动量交换，[1]ADBandrauk，JGuo，KJYuan，，JOpt，19，124016（2017）;[2]S.Chelkowski，AD.Bandrauk，PBCorkum，Phys Rev Lett 113，263005（2015）。