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Symmetry-Breaking in the Multi-Photon Ionization Dynamics of Oriented Atoms

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Symmetry-Breaking in the Multi-Photon Ionization Dynamics of Oriented Atoms Scholars' Mine Doctoral Dissertations Student Theses and Dissertations Summer 2020 Symmetry-breaking in the multi-photon ionization dynamics of oriented atoms Aruma Handi Nishshanka Chandrajith De Silva Follow this and additional works at: https://scholarsmine.mst.edu/doctoral_dissertations Part of the Physics Commons Department: Physics Recommended Citation De Silva, Aruma Handi Nishshanka Chandrajith, "Symmetry-breaking in the multi-photon ionization dynamics of oriented atoms" (2020). Doctoral Dissertations. 2911. https://scholarsmine.mst.edu/doctoral_dissertations/2911 This thesis is brought to you by Scholars' Mine, a service of the Missouri S&T Library and Learning Resources. This work is protected by U. S. Copyright Law. Unauthorized use including reproduction for redistribution requires the permission of the copyright holder. For more information, please contact [email protected]. SYMMETRY-BREAKING IN THE MULTI-PHOTON IONIZATION DYNAMICS OF ORIENTED ATOMS by ARUMA HANDI NISHSHANKA CHANDRAJITH DE SILVA A DISSERTATION Presented to the Graduate Faculty of the MISSOURI UNIVERSITY OF SCIENCE AND TECHNOLOGY In Partial Fulfillment of the Requirements for the Degree DOCTOR OF PHILOSOPHY in PHYSICS 2020 Approved by: Daniel Fischer, Adviser Michael Schulz Jerry L. Peacher Don Madison V. A. Samaranayake ©2020 Aruma Handi Nishshanka Chandrajith de Silva All Rights Reserved iii ABSTRACT Laser cooling and trapping, femtosecond light creation, and coincident electron and ion momentum imaging was combined in a world-wide unique experimental setup. These state-of-the-art techniques were used to control atomic systems and analyze the few-body quantum dynamics in multi-photon ionization of lithium. An all-optical, near-resonant laser atom trap (AOT) was developed to prepare a lithium gas at milli-Kelvin temperatures. The atoms can be resonantly excited to the state 22P3/2(m/ = +1) with a high degree of polarization and are used as a target to study atomic multi-photon ionization in the field of an intense laser source based on an optical parametric chirped pulse amplifier (OPCPA) that provides few femtosecond laser pulses with intensities of up to 1012W/cm2. The momenta of emitted electrons and Li+ ions are analyzed in a COLTRIMS spectrometer with excellent resolution. The fundamental scientific questions addressed with this setup relate to the initial state dependence of multi-photon ionization processes. The influence of relative polarizations of target and laser pulse was studied in the most fundamental conceivable chiral systems. We studied a symmetry breaking between left- and right­ handed circular laser polarization, so-called circular dichroism, in the ionization of the 22P3/2(m/ = +1). It was found that the polarization-dependent dressing of the atoms in the field causes significant Autler-Townes shifts resulting in a strong circular dichroism that affects not only the total ionization rate and the photo-electron angular distributions (PAD) but also the energy of the emitted photons. The measured energy spectra, PADs, and momentum distributions are in excellent agreement with a theoretical model solving the time-dependent Schrodinger equation in the single-active electron approximation. iv ACKNOWLEDGMENTS First, I would like to express my sincere thanks to my advisor, Dr. Daniel Fischer, for allowing me to continue to work with, and giving me an ample opportunity to breathe an enormous amount of exciting physics about the collisions in ultra-cold atomic physics and unorthodox experiences, and for teaching me data analysis and scientific diplomacy. The illumination shined on is universal and forever. I thank the other committee members for their invaluable effort and time. It is with great respect I thank Dr. Thomas Vojta for his kind advice at difficult times when I needed them most. I thank Dr. Klaus Bartschat for the theoretical contribution. I thank the post-doctoral scholars, Sachin Sharma, Santwana Dubey, and especially Thusitha Arthanayaka, for the fruitful discussions during development of data analysis and help with running the experiment during the several nights when I really needed help. I extend my thanks to other fellow graduate students in the Fischer’s lab, Kevin Romans, Bishnu Acharya, Kyle Foster, and Onyx Russ, for all their hard work, help and suggestions by proofreading the dissertation. I thank Andy Stubbs, Ron Woody, Pam Crabtree, and Janice Gargus for helping me in numerous ways. I thank my parents for spending all their lives for me to achieve this precious moment of my life. My thanks extend to my relatives, friends, and teachers. I thank my elder brother for being a role model and an ideal example always in my life, and my younger brother for always believing in me more than I did myself, which made me come this far. Last, but the most, I thank my beautiful wife, Dinithi, for preventing my uncountable number of quitting attempts of the Ph.D. program and for all the encouragement. Thanks, to the kids, Deon, Sehansa, and Jemeth, for tolerating me so long in this torturing journey. v TABLE OF CONTENTS Page ABSTRACT.................................................................................................................................iii ACKNOWLEDGMENTS..........................................................................................................iv LIST OF FIGURES....................................................................................................................vii LIST OF TABLES........................................................................................................................ x NOMENCLATURE....................................................................................................................xi SECTION 1. INTRODUCTION................................................................................................................1 2. ALL-OPTICAL TRAP (AOT)...........................................................................................6 2.1. GENERAL LASER COOLING AND MAGNETO OPTICAL TRAPS...........6 2.2. PROPERTIES OF 6Li AND LASER COOLING SCHEME................................9 2.3. SETUP, TRAP CONFIGURATION, AND TUNING OF THE AOT...............11 2.4. CHARACTERIZATION OF THE A OT................................................................14 2.4.1. Atom Number and Density............................................................................15 2.4.2. Cloud Temperature.........................................................................................16 2.5. CONCLUSIONS AND OPEN QUESTIONS....................................................... 18 3. REACTION MICROSCOPE........................................................................................... 19 3.1. CONFIGURATION AND FUNCTION.................................................................19 3.2. MOTION OF CHARGED PARTICLES IN STATIC EM FIELDS..................21 3.3. RESOLUTION 22 vi 4. FEMTO-SECOND LASER SYSTEM........................................................................... 25 4.1. EVOLUTION OF ULTRA-SHORT LASER PULSES...................................... 25 4.2. TITAN-SAPPHIRE OSCILLATOR......................................................................26 4.3. HIGH POWER AMPLIFIER..................................................................................29 4.4. NON-COLLINEAR OPTICAL PARAMETRIC AMPLIFIER (NOPA)....... 30 4.5. OPERATION IN TUNABLE M OD E....................................................................33 4.6. OPTIMIZATION AND CHARACTERIZATION OF LASER BEAM PARAMETERS........................................................................................................ 35 5. MULTI-PHOTON IONIZATION.................................................................................. 38 5.1. FUNDAMENTALS OF MULTI-PHOTON IONIZATION...............................38 5.2. IONIZATION DYNAMICS WITH INTENSE LASER PULSES.....................41 5.3. CIRCULAR DICHROISM...................................................................................... 45 5.4. IONIZATION WITH NARROW BANDWIDTH PULSES...............................49 5.5. AUTLER-TOWNES SPLITTING......................................................................... 53 5.6. DISCUSSION AND COMPARISON TO THEORY..........................................55 6. CONCLUSION ................................................................................................................ 63 BIBLIOGRAPHY....................................................................................................................... 66 VITA 74 vii LIST OF FIGURES Figure Page 2.1 (Left) Atomic energy level scheme in one dimension for a quadrupole magnetic field created by (right) anti-Helmholtz coils for a magneto-optical trap M OT ...........8 2.2 Hyperfine splitting of ground and excited states of 6Li.................................................10 2.3 The ground 2S1/2 (F = 3/2) and the excited 2P3/2 levels of 6Li splitting with magnetic field (Zeeman splitting [49]) Sharma et al.................................................... 10 2.4 AOT at the intersection of the three pairs of laser beams and the large Helmholtz’s coils producing homogeneous magnetic field................................................................ 12 2.5 Experimental data and the fits for the loading and decay curves of AOT with two atom lo ss............................................................................................................................... 16 2.6 Ballistic expansion
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