Modeling generation and characterization of attosecond pulses

Generation of high-order harmonics has emerged as a powerful technique for the generation of broadband coherent radiation in the EUV regime. This has lead to the development of table-top EUV sources that can produce attosecond pulses. These pulses can serve as a probe to resolve atomic attosecond dynamics and image atomic orbitals and molecular motion. Due to high spatial and temporal coherence, high-order harmonic radiation can also be used to seed free electron lasers, which allow the generation of high-intensity X-ray radiation that can be used for imaging biomolecules. Since the first observation of high-order harmonics, effort has been made to accurately model both the generation and the characterization of attosecond pulses. Work on the modeling of high harmonic generation can be divided into two parts: (a) description of the interaction between the JR pulse and atoms that leads to emission of attosecond pulses (the single atom response) and (b) modeling of the propagation of attosecond pulses by accounting for macroscopic phase matching effects. In this work, we will focus on the single atom response which can be calculated either by numerically solving the time dependent Schrodinger equation (TDSE) or through the semi-classical three step model (TSM). In Chapter 2, the theory of light-atom interaction will be reviewed with the focus on the calculation of the dipole trasition matrix element (DTME) in the strong field formalism. It will be shown that the choice of the basis states - Volkov states and Coulomb Volkov states - to describe electrons in the continuum is crucial to the accuracy of DTME calculation. In Chapter 3, the TSM will be derived from the Schrodinger equation by using the saddle point approximation. Through this derivation, the quantum mechanical laser-atom interaction is reduced to a semi-classical model comprising of ionization, propagation and recombination . The numerical scheme for solving the TDSE will be discussed. It will then be used to demonstrate the generation of isolated attosecond pulses from non-sinusoidal sub-cycle pulses. The results of ADK and non-adiabatic ionization models will be compared with that from numerical TDSE, and then used to calculate the harmonic spectra in the tunneling and multi-photon ionization regimes. The recombination step of the TSM, which plays a crucial role in determining the qualitative shape of the high-order harmonic spectrum, will be investigated in Chapter 4. A commonly observed feature of Argon's high-order harmonic spectrum is the presence of a minimum at around 50 eV called the Cooper minimum. The minimum in the high-order harmonic spectrum has been attributed to the minimum in the recombination amplitude. The recombination amplitude will be calculated - in the strong field formalism - using length and acceleration form for two choices of continuum electron wavefunction description (Volkov and Coulomb-Volkov). Attosecond pulse characterization techniques, which are an extension of the subpicosecond pulse characterization technique like FROG…

[1]  A. Starace Theory of Atomic Photoionization , 1982 .

[2]  L. A. Lompré,et al.  Multiple-harmonic conversion of 1064 nm radiation in rare gases , 1988 .

[3]  D. J. Kane,et al.  Recent progress toward real-time measurement of ultrashort laser pulses , 1999 .

[4]  J. Toivanen,et al.  Solution of time-independent Schrödinger equation by the imaginary time propagation method , 2007, J. Comput. Phys..

[5]  C. C. Wang,et al.  Nonlinear optics. , 1966, Applied optics.

[6]  John Arents,et al.  Atomic Structure Calculations , 1964 .

[7]  D. Zeidler,et al.  High harmonic generation and the role of atomic orbital wave functions. , 2007, Physical review letters.

[8]  Liam P. Barry,et al.  Autocorrelation of ultrashort pulses at 1.5 /spl mu/m based on nonlinear response of silicon photodiodes , 1996 .

[9]  A. Becker,et al.  Intense-field many-body S-matrix theory , 2005 .

[10]  James A. R. Samson,et al.  Precision measurements of the total photoionization cross-sections of He, Ne, Ar, Kr, and Xe , 2002 .

[11]  Ivanov,et al.  Theory of high-harmonic generation by low-frequency laser fields. , 1994, Physical review. A, Atomic, molecular, and optical physics.

[12]  F. Quéré,et al.  Temporal characterization of attosecond XUV fields , 2005 .

[13]  J. Cooper,et al.  Photo-Ionization in the Soft x-Ray Range: 1 Z Dependence in a Central-Potential Model , 1968 .

[14]  Andrew D. Shiner,et al.  Probing collective multi-electron dynamics in xenon with high-harmonic spectroscopy , 2011 .

[15]  C. M. Lee,et al.  Relativistic Random-Phase Approximation , 1980 .

[16]  F. Kärtner,et al.  Scaling of high harmonic generation conversion efficiency , 2011 .

[17]  M. Amusia Rearrangement effects in photoionization. , 1980, Applied optics.

[18]  Nirit Dudovich,et al.  High harmonic interferometry of multi-electron dynamics in molecules , 2009, Nature.

[19]  R. Kosloff,et al.  Absorbing boundaries for wave propagation problems , 1986 .

[20]  L. Collins,et al.  Intense laser-induced recombination: The inverse above-threshold ionization process , 2004 .

[21]  C. L. Cocke,et al.  Attosecond pulse characterization. , 2013, Optics express.

[22]  B. Eggleton,et al.  High-energy pulse synthesis with sub-cycle waveform control for strong-field physics , 2011 .

[23]  Zenghu Chang,et al.  Characterizing ultrabroadband attosecond lasers. , 2010, Optics express.

[24]  P. Villoresi,et al.  Nonadiabatic three-dimensional model of high-order harmonic generation in the few-optical-cycle regime , 2000 .

[25]  L. Chipperfield,et al.  Ideal waveform to generate the maximum possible electron recollision energy for any given oscillation period. , 2009, Physical review letters.

[26]  J. West,et al.  Absolute photoionization cross-section tables for helium, neon, argon, and krypton in the VUV spectral regions , 1976 .

[27]  K.-N. Huang,et al.  Theoretical photoionization parameters for the noble gases argon, krypton, and xenon , 1981 .

[28]  J. Levesque,et al.  Tomographic imaging of molecular orbitals , 2004, Nature.

[29]  Richard L. Fork,et al.  LOCKING OF He–Ne LASER MODES INDUCED BY SYNCHRONOUS INTRACAVITY MODULATION , 1964 .

[30]  Eleftherios Goulielmakis,et al.  The accurate FROG characterization of attosecond pulses from streaking measurements , 2008 .

[31]  W. Johnson,et al.  Photoionization of the outer shells of neon, argon, krypton, and xenon using the relativistic random-phase approximation , 1979 .

[32]  J G Fujimoto,et al.  Sub-two-cycle pulses from a Kerr-lens mode-locked Ti:sapphire laser. , 1999, Optics letters.

[33]  P. Balcou,et al.  Observation of a Train of Attosecond Pulses from High Harmonic Generation , 2001, Science.

[34]  M. Spanner,et al.  Coulomb and polarization effects in sub-cycle dynamics of strong-field ionization , 2006 .

[35]  Stephen R. Leone,et al.  Real-time observation of valence electron motion , 2010, Nature.

[36]  R. Lucchese,et al.  Quantitative rescattering theory for high-order harmonic generation from molecules , 2009, 0903.5354.

[37]  S. Pabst,et al.  Impact of multichannel and multipole effects on the Cooper minimum in the high-order-harmonic spectrum of argon , 2012, 1202.4855.

[38]  J. Cooper,et al.  Photoionization from Outer Atomic Subshells. A Model Study , 1962 .

[39]  S. Chu,et al.  Generalized pseudospectral methods with mappings for bound and resonance state problems , 1993 .

[40]  Ahmed H. Zewail,et al.  Femtochemistry: Atomic-Scale Dynamics of the Chemical Bond† , 2000 .

[41]  Ariel Gordon,et al.  Numerical solver of the time-dependent Schrödinger equation with Coulomb singularities , 2006 .

[42]  P. Corkum,et al.  Following a chemical reaction using high-harmonic interferometry , 2010, Nature.

[43]  K. Taylor,et al.  R-matrix theory of photoionization. Application to neon and argon , 1975 .

[44]  S. V. Bulanov,et al.  Optics in the relativistic regime , 2006 .

[45]  D. Bondar Instantaneous multiphoton ionization rate and initial distribution of electron momentum , 2008, 0805.1890.

[46]  N. Tzoar,et al.  Compton scattering in the presence of coherent electromagnetic radiation , 1978 .

[47]  Shih-I Chu,et al.  Theoretical study of multiple high-order harmonic generation by intense ultrashort pulsed laser fields: A new generalized pseudospectral time-dependent method , 1997 .

[48]  Jon P. Davis,et al.  Nonadiabatic transitions induced by a time‐dependent Hamiltonian in the semiclassical/adiabatic limit: The two‐state case , 1976 .

[49]  F. Kärtner,et al.  Quantitative modeling of single atom high harmonic generation. , 2005, Physical review letters.

[50]  J. West,et al.  Angular distribution and photoionization cross section measurements on the 3p and 3s subshells of argon , 1974 .

[51]  I. Lindau,et al.  Atomic subshell photoionization cross sections and asymmetry parameters: 1 ⩽ Z ⩽ 103 , 1985 .

[52]  Franz X Kärtner,et al.  Two-dimensional spectral shearing interferometry for few-cycle pulse characterization. , 2006, Optics letters.

[53]  H. Bethe,et al.  Ingoing Waves in Final State of Scattering Problems , 1954 .

[54]  J. Burgdorfer,et al.  Time-resolved photoemission by attosecond streaking: extraction of time information , 2011, 1102.1461.

[55]  J. West,et al.  Angular distribution and photoionization measurements on the 2p and 2s electrons in neon , 1976 .

[56]  Role of many-electron dynamics in high harmonic generation. , 2006, Physical review letters.

[57]  Interplay of mulitphoton and tunneling ionization in short-wavelength-driven high-order harmonic generation , 2011 .

[58]  G. L. Yudin,et al.  Nonadiabatic tunnel ionization: Looking inside a laser cycle , 2001 .

[59]  T. Maiman Stimulated Optical Radiation in Ruby , 1960, Nature.

[60]  K. Hong,et al.  Recombination-amplitude calculations of noble gases, in both length and acceleration forms, beyond the strong-field approximation , 2013, 1308.0968.

[61]  V. S. Popov,et al.  IONIZATION OF ATOMS IN AN ALTERNATING ELECTRIC FIELD , 1966 .

[62]  R. Holzwarth,et al.  Attosecond control of electronic processes by intense light fields , 2003, Nature.

[63]  Kulander Time-dependent Hartree-Fock theory of multiphoton ionization: Helium. , 1987, Physical review. A, General physics.

[64]  Jonathan A. Cooper,et al.  Spectral Distribution of Atomic Oscillator Strengths , 1968 .

[65]  D. Descamps,et al.  High-order harmonic spectroscopy of the Cooper minimum in argon: Experimental and theoretical study , 2010, 1012.2676.

[66]  C. Lin,et al.  Multichannel relativistic random-phase approximation for the photoionization of atoms , 1979 .

[67]  High-order harmonic generation in Xe, Kr, and Ar driven by a 2.1-μm source: High-order harmonic spectroscopy under macroscopic effects , 2012, 1209.1773.

[68]  L. Keldysh,et al.  IONIZATION IN THE FIELD OF A STRONG ELECTROMAGNETIC WAVE , 1964 .

[69]  Sang-Kil Son,et al.  Impact of hollow-atom formation on coherent x-ray scattering at high intensity , 2011, 1101.4932.

[70]  N. Karpowicz,et al.  Attosecond streaking enables the measurement of quantum phase. , 2010, Physical review letters.

[71]  S. Pabst Atomic and molecular dynamics triggered by ultrashort light pulses on the atto- to picosecond time scale , 2013, 1305.2508.

[72]  D. Kane,et al.  Single-shot measurement of the intensity and phase of an arbitrary ultrashort pulse by using frequency-resolved optical gating. , 1993, Optics letters.

[73]  B. Piraux,et al.  Phase-dependent harmonic emission with ultrashort laser pulses , 1998 .

[74]  Ivanov,et al.  Coulomb corrections and polarization effects in high-intensity high-harmonic emission. , 1996, Physical review. A, Atomic, molecular, and optical physics.

[75]  Shore,et al.  Calculations of multiple-harmonic conversion of 1064 nm radiation in Xe. , 1989, Physical review letters.

[76]  Henry C. Kapteyn,et al.  High-Harmonic Generation of Attosecond Pulses in the ``Single-Cycle'' Regime , 1997 .

[77]  Harald Friedrich,et al.  Theoretical Atomic Physics , 1991 .

[78]  Rick Trebino,et al.  Measuring ultrashort laser pulses in the time-frequency domain using frequency-resolved optical gating , 1997 .

[79]  P. Corkum,et al.  Observation of electronic structure minima in high-harmonic generation. , 2009, Physical review letters.

[80]  M. Scully,et al.  Advances in Atomic, Molecular, and Optical Physics , 2022, Advances In Atomic, Molecular, and Optical Physics.

[81]  I. A. Walmsley,et al.  Self-referencing spectral interferometry for measuring ultrashort optical pulses , 1999 .

[82]  A. Starace Trends in the theory of atomic photoionization. , 1980, Applied optics.