Physical Sciences and Mathematics Commons^™

Temporal Coherent Control Of Resonant Two-Photon Double Ionization Of The Hydrogen Molecule Via Doubly Excited States, Jean Marcel Ngoko Djiokap, Anthony F. Starace

Anthony F. Starace Publications

We use time-delayed, counter-rotating, circularly polarized few-cycle attosecond nonoverlapping pulses to study the temporal coherent control of the resonant process of two-photon double ionization (TPDI) of hydrogen molecule via doubly excited states for pulse propagation direction along ˆk either parallel or perpendicular to the molecular axis ˆR. For ˆk ‖ ˆR and a pulse carrier frequency of 36 eV resonantly populating the Q₂ 1∏ ⁺ _u (1) doubly excited state as well as other 1∏ ⁺ _u doubly excited states, we find that the indirect ionization pathway through these doubly excited states changes the character of the kinematical vortex-shaped …

Attosecond-Pulse Metrology Based On High-Order Harmonic Generation, T. S. Sarantseva, M. V. Frolov, N. L. Manakov, A. A. Silaev, A. A. Romanov, N. V. Vvedenskii, Anthony F. Starace

Anthony F. Starace Publications

An all-optical method to retrieve the temporal intensity profile of an extreme ultraviolet (XUV) attosecond pulse is proposed based on XUV-assisted high-order harmonic generation (HHG) by an intense infrared (IR) pulse. For a harmonic located on the XUV-induced high-energy plateau (beyond the IR HHG plateau), the measured harmonic yield as a function of the time delay between the XUV and IR pulses is shown to accurately map the temporal intensity profile of the XUV pulse. Single-color and two-color orthogonal, linearly polarized IR pulses are used to demonstrate the method.

Minimizing The Duration Of Isolated Attosecond Pulses, Dian Peng, Anthony F. Starace, Hua-Chieh Shao, Jean Marcel Ngoko Djiokap

Anthony F. Starace Publications

We investigate theoretically how the duration of an isolated attosecond pulse (IAP) can be minimized by carefully selecting frequencies of high-order harmonic generation (HHG) spectra produced by ultrashort driving laser pulses. Based on numerical calculations of HHG by solving the time-dependent Schrödinger equation for a single H atom, we provide three strategies for generating shorter IAPs. First, when the high-frequency region of an HHG plateau is selected one should use frequencies below the cutoff. Second, for a wide HHG plateau the low-frequency region can produce shorter IAPs than the high-frequency region. Third, we propose a method of producing IAPs with …

Origin Of The Multiphoton-Regime Harmonic-Generation Plateau Structure, Jean Marcel Ngoko Djiokap, Anthony F. Starace

Anthony F. Starace Publications

A physical interpretation is provided for the formation of the multiphoton-regime plateau feature in the spectra of nonlinear and correlated process of high-order harmonic generation (HHG) of two-active-electron atoms interacting with an intense linearly polarized laser field [Phys. Rev. A 88, 053412 (2013) for beryllium]. While in the strong-field tunneling regime the plateau feature is well known to be due to rescattering effects of the freed electron, its counterpart in the multiphoton regime is due to atomic resonance effects involving both singly excited states and doubly excited states. Here, we propose a strategy to uncover which kind of these states …

Obituary: Anthony Starace (1945-2019)

Anthony F. Starace Publications

Anthony Starace, George Holmes University Professor of physics, died Sept. 5 from complications related to pancreatitis. He was 74.

Starace was born July 24, 1945, in the Queens borough of New York City. He graduated from Stuyvesant High School and earned his bachelor’s degree from Columbia University in 1966 before moving west to the University of Chicago, where he earned his doctorate under adviser Ugo Fano in 1971. It was in Chicago that he met Katherine Fritz of Beatrice, Nebraska, his wife of 51 years.

Following a postdoctoral appointment at Imperial College London, Starace moved to Lincoln as an assistant …

Performance Of Plastic Electron Optics Components Fabricated Using A 3d Printer, Phillip Wiebe, Peter Beierle, Hua-Chieh Shao, Bret Gergely, Anthony F. Starace, Herman Batelaan

Anthony F. Starace Publications

We show images produced by an electron beam deflector, a quadrupole lens and a einzel lens fabricated from conducting and non-conducting plastic using a 3D printer. Despite the difficulties associated with the use of plastics in vacuum, such as outgassing, poor conductivity, and print defects, the devices were used successfully in vacuum to steer, stretch and focus electron beams to millimeter diameters. Simulations indicate that much smaller focus spot sizes might be possible for such 3D-printed plastic electron lenses taking into account some possible surface defects. This work was motivated by our need to place electron optical components in difficult-to-access …

Analytic Generalized Description Of A Perturbative Nonparaxial Elegant Laguerre-Gaussian Phasor For Ultrashort Pulses In The Time Domain, Andrew Vikartofsky, Ethan C. Jahns, Anthony F. Starace

Anthony F. Starace Publications

An analytic expression for a polychromatic phasor representing an arbitrarily short elegant Laguerre-Gauss (eLG) laser pulse of any spot size and LG mode is presented in the time domain as a nonrecursive, closed-form perturbative expansion valid to any order of perturbative correction. This phasor enables the calculation of the complex electromagnetic fields for such beams without requiring the evaluation of any Fourier integrals. It is thus straightforward to implement in analytical or numerical applications involving eLG pulses.

Analytic Description Of High-Order Harmonic Generation In The Adiabatic Limit With Application To An Initial S State In An Intense Bicircular Laser Pulse, M. V. Frolov, N. L. Manakov, A. A. Minina, A. A. Silaev, N. V. Vvedenskii, M. Yu. Ivanov, Anthony F. Starace

Anthony F. Starace Publications

An analytic description of high-order harmonic generation (HHG) is proposed in the adiabatic (low-frequency) limit for an initial s state and a laser field having an arbitrary wave form. The approach is based on the two-state time-dependent effective range theory and is extended to the case of neutral atoms and positively charged ions by introducing ad hoc the Coulomb corrections for HHG. The resulting closed analytical form for the HHG amplitude is discussed in terms of real classical trajectories. The accuracy of the results of our analytic model is demonstrated by comparison with numerical solutions of the time-dependent Schrödinger equation …

Violation Of Centrosymmetry In Time-Resolved Coherent X-Ray Diffraction From Rovibrational States Of Diatomic Molecules, Hua-Chieh Shao, Anthony F. Starace

Anthony F. Starace Publications

Owing to increasing applications of time-resolved coherent x-ray scattering for the investigation of molecular reaction dynamics, we develop a theoretical model for time-dependent x-ray diffraction from molecular and/or electronic motion in molecules. Our model shows that the violation of centrosymmetry (VOC) is a general phenomenon in time-resolved diffraction patterns. We employ our theoretical model to illustrate the VOC in time-resolved coherent x-ray diffraction from two oriented diatomic molecules undergoing rovibrational motion: lithium hydride (LiD) and hydrogen (HD). Our simulations show asymmetric x-ray diffraction images that reflect the directions of the molecular motions.

Molecular Symmetry-Mixed Dichroism In Double Photoionization Of H2, Jean Marcel Ngoko Djiokap, Alexei V. Meremianin, N. L. Manakov, L. B. Madsen, S. X. Hu, Anthony F. Starace

Anthony F. Starace Publications

Dichroism in double photoionization of H₂ molecules by elliptically polarized extreme ultraviolet pulses is formulated analytically as a sum of atomiclike dichroism (AD) and molecular symmetry-mixed dichroism (MSMD) terms. The MSMD originates from an interplay of ¹Σ⁺_u and ¹Π⁺_u continuum molecular ionization amplitudes. For detection geometries in which the AD vanishes, numerical results for the sixfold differential probabilities for opposite pulse helicities show that the MSMD is significant in the electron momentum and angular distributions and is controllable by the ellipticity.

Dynamical Electron Vortices In Attosecond Double Photoionization Of H2, Jean Marcel Ngoko Djiokap, A. V. Meremianin, N. L. Manakov, L. B. Madsen, S. X. Hu, Anthony F. Starace

Anthony F. Starace Publications

We study electron momentum vortices in single-photon double ionization of H2 by time-delayed, counterrotating, elliptically polarized attosecond pulses propagating along kˆ either parallel or perpendicular to the molecular axis R. For kˆ | R, kinematical vortices occur similar to those found for He. For kˆ ⊥ R, we find dynamical vortex structures originating from an ellipticity-dependent interplay of ¹∑⁺_u and ¹∏⁺_u continuum amplitudes. We propose a complete experiment to determine the magnitudes and relative phase of these amplitudes by varying pulse ellipticities and time delays.

Perturbative Representation Of Ultrashort Nonparaxial Elegant Laguerre-Gaussian Fields, Andrew Vikartofsky, Anthony F. Starace, Liang-Wen Pi

Anthony F. Starace Publications

An analytical method for calculating the electromagnetic fields of a nonparaxial elegant Laguerre-Gaussian (LG) vortex beam is presented for arbitrary pulse duration, spot size, and LG mode. This perturbative approach provides a numerically tractable model for the calculation of arbitrarily high radial and azimuthal LG modes in the nonparaxial regime, without requiring integral representations of the fields. A key feature of this perturbative model is its use of a Poisson-like frequency spectrum, which allows for the proper description of pulses of arbitrarily short duration. This model is thus appropriate for simulating laser-matter interactions, including those involving short laser pulses.

Control Of Harmonic Generation By The Time Delay Between Two-Color, Bicircular Few-Cycle Mid-Ir Laser Pulses, M. V. Frolov, N. L. Manakov, A. A. Minina, N. V. Vvedenskii, A. A. Silaev, M. Yu. Ivanov, Anthony F. Starace

Anthony F. Starace Publications

We study control of high-order harmonic generation (HHG) driven by time-delayed, few-cycle ω and 2ω counterrotating mid-IR pulses. Our numerical and analytical study shows that the time delay between the two-color pulses allows control of the harmonic positions, both those allowed by angular momentum conservation and those seemingly forbidden by it. Moreover, the helicity of any particular harmonic is tunable from left to right circular without changing the driving pulse helicity. The highest HHG yield occurs for a time delay comparable to the fundamental period T = 2π/ω.

Enhancing High-Order Harmonic Generation By Sculpting Waveforms With Chirp, Dian Peng, M. V. Frolov, Liang-Wen Pi, Anthony F. Starace

Anthony F. Starace Publications

We present a theoretical analysis showing how chirp can be used to sculpt two-color driving laser field waveforms in order to enhance high-order harmonic generation (HHG) and/or extend HHG cutoff energies. Specifically, we consider driving laser field waveforms composed of two ultrashort pulses having different carrier frequencies in each of which a linear chirp is introduced. Two pairs of carrier frequencies of the component pulses are considered: (ω, 2ω) and (ω, 3ω). Our results show how changing the signs of the chirps in each of the two component pulses leads to drastic changes in the HHG spectra. Our theoretical analysis …

Time-Resolved Electron (E,2E) Momentum Spectroscopy: Application To Laser-Driven Electron Population Transfer In Atoms, Hua-Chieh Shao, Anthony F. Starace

Anthony F. Starace Publications

Owing to its ability to provide unique information on electron dynamics, time-resolved electron momentum spectroscopy (EMS) is used to study theoretically a laser-driven electronic motion in atoms. Specifically, a chirped laser pulse is used to adiabatically transfer the populations of lithium atoms from the ground state to the first excited state. During this process, impact ionization near the Bethe ridge by time-delayed ultrashort, high-energy electron pulses is used to image the instantaneous momentum density of this electronic population transfer. Simulations with 100 fs and 1 fs pulse durations demonstrate the capability of EMS to image the time-varying momentum density, including …

Xuv-Assisted High-Order-Harmonic-Generation Spectroscopy, T. S. Sarantseva, M. V. Frolov, N. L. Manakov, A. A. Silaev, N. V. Vvedenskii, Anthony F. Starace

Anthony F. Starace Publications

Using the analytic time-dependent effective range theory, we study two-color high-order harmonic generation (HHG) involving a weak extreme ultraviolet (XUV) pulse and an intense infrared laser field. Our analysis shows that XUV-assisted HHG spectra contain multiple additional plateau structures originating from absorption of one or more XUV photons at the photorecombination step of HHG. We show also that the HHG rate corresponding to the nth plateau can be presented in a factorized form involving the XUV-assisted (multiphoton) photorecombination cross section (PRCS) corresponding to absorption of n XUV photons of energy Ω and emission of a harmonic of energy Ω_{h …}

Doubly-Excited State Effects On Two-Photon Double Ionization Of Helium By Time-Delayed, Oppositely Circularly-Polarized Attosecond Pulses, Jean Marcel Ngoko Djiokap, Anthony F. Starace

Anthony F. Starace Publications

We study two-photon double ionization (TPDI) of helium by a pair of time-delayed (non-overlapping), oppositely circularly-polarized attosecond pulses whose carrier frequencies are resonant with ¹P^o doubly-excited states. All of our TPDI results are obtained by numerical solution of the two-electron time-dependent Schrödinger equation for the six-dimensional case of circularly-polarized attosecond pulses, and they are analyzed using perturbation theory (PT). As compared with the corresponding nonresonant TPDI process, we find that the doubly-excited states change the character of vortex patterns in the two-electron momentum distributions for the case of back-to-back detection of the two ionized electrons in the polarization …

Imaging Electronic Motions By Ultrafast Electron Diffraction, Hua-Chieh Shao, Anthony F. Starace

Anthony F. Starace Publications

Recently ultrafast electron diffraction and microscopy have reached unprecedented temporal resolution, and transient structures with atomic precision have been observed in various reactions. It is anticipated that these extraordinary advances will soon allow direct observation of electronic motions during chemical reactions. We therefore performed a series of theoretical investigations and simulations to investigate the imaging of electronic motions in atoms and molecules by ultrafast electron diffraction. Three prototypical electronic motions were considered for hydrogen atoms. For the case of a breathing mode, the electron density expands and contracts periodically, and we show that the time-resolved scattering intensities reflect such changes …

Energy-Resolved Coherent Diffraction From Laser-Driven Electronic Motion In Atoms, Hua-Chieh Shao, Anthony F. Starace

Anthony F. Starace Publications

We investigate theoretically the use of energy-resolved ultrafast electron diffraction to image laser-driven electronic motion in atoms. A chirped laser pulse is used to transfer the valence electron of the lithium atom from the ground state to the first excited state. During this process, the electronic motion is imaged by 100-fs and 1-fs electron pulses in energy-resolved diffraction measurements. Simulations show that the angle-resolved spectra reveal the time evolution of the energy content and symmetry of the electronic state. The time-dependent diffraction patterns are further interpreted in terms of the momentum transfer. For the case of incident 1-fs electron pulses, …

Ionization Enhancement And Suppression By Phase-Locked Ultrafast Pulse Pairs, David B. Foote, Y. Lin, Liang-Wen Pi, Jean Marcel Ngoko Djiokap, Anthony F. Starace, W. T. Hill

Anthony F. Starace Publications

We present the results of a study of ionization of Xe atoms by a pair of phase-locked pulses, which is characterized by interference produced by the twin peaks. Two types of interference are considered: ordinary optical interference, which changes the intensity of the composite pulse and thus the ion yield, and a quantum interference, in which the excited electron wave packets interfere. We use the measured Xe+ yield as a function of the temporal delay and/or relative phase between the peaks to monitor the interferences and compare their relative strengths. We model the interference with a pulse intensity function and …

Adiabatic-Limit Coulomb Factors For Photoelectron And High-Order-Harmonic Spectra, M. V. Frolov, N. L. Manakov, A. A. Minina, S. V. Popruzhenko, Anthony F. Starace

Anthony F. Starace Publications

A momentum-dependent Coulomb factor in the probability for nonlinear ionization of atoms by a strong low-frequency laser field is calculated analytically in the adiabatic approximation. Expressions for this Coulomb factor, valid for an arbitrary laser pulse waveform, are obtained and analyzed in detail for the cases of linear and circular polarizations. The dependence of the Coulomb factor on the photoelectron momentum is shown to be significant in both cases. Using a similar technique, the Coulomb factor for emission of high-order harmonics by an atom in a bichromatic laser field is also calculated. In contrast to the case of a single-frequency …

Kinematical Vortices In Double Photoionization Of Helium By Attosecond Pulses, Jean Marcel Ngoko Djiokap, A. V. Meremianin, N. L. Manakov, S. X. Hu, L. B. Madsen, Anthony F. Starace

Anthony F. Starace Publications

Two-armed helical vortex structures are predicted in the two-electron momentum distributions produced in double photoionization (DPI) of the He atom by a pair of time-delayed elliptically polarized attosecond pulses with opposite helicities. These predictions are based upon both a first-order perturbation theory analysis and numerical solutions of the two-electron, time-dependent Schrödinger equation in six spatial dimensions. The helical vortex structures originate from Ramsey interference of a pair of ionized two-electron wave packets, each having a total angular momentum of unity, and appear in the sixfold differential DPI probability distribution for any energy partitioning between the two electrons. The vortex structures …

Discontinuities In The Electromagnetic Fields Of Vortex Beams In The Complex Source-Sink Model, Andrew Vikartofsky, Liang-Wen Pi, Anthony F. Starace

Anthony F. Starace Publications

An analytical discontinuity is reported in what was thought to be the discontinuity-free exact nonparaxial vortex beam phasor obtained within the complex source-sink model. This discontinuity appears for all odd values of the orbital angular momentum mode. Such discontinuities in the phasor lead to nonphysical discontinuities in the real electromagnetic field components. We identify the source of the discontinuities, and provide graphical evidence of the discontinuous real electric fields for the first and third orbital angular momentum modes. A simple means of avoiding these discontinuities is presented.

Enhancing High-Order-Harmonic Generation By Time Delays Between Two-Color, Few-Cycle Pulses, Dian Peng, Liang-Wen Pi, M. V. Frolov, Anthony F. Starace

Anthony F. Starace Publications

Use of time delays in high-order-harmonic generation (HHG) driven by intense two-color, few-cycle pulses is investigated in order to determine means of optimizing HHG intensities and plateau cutoff energies. Based upon numerical solutions of the time-dependent Schrõdinger equation for the H atom as well as analytical analyses, we show that introducing a time delay between the two-color, few-cycle pulses can result in an enhancement of the intensity of the HHG spectrum by an order of magnitude (or more) at the cost of a reduction in the HHG plateau cutoff energy. Results for both positive and negative time delays as well …

Imaging Population Transfer In Atoms With Ultrafast Electron Pulses, Hua-Chieh Shao, Anthony F. Starace

Anthony F. Starace Publications

We propose the use of ultrafast electron diffraction (UED) to image a controllable, laser-driven coherent electron population transfer in lithium atoms with currently available femtosecond electron pulses. Our simulations demonstrate the ability of ultrafast electrons to image such an electronic population transfer, thus validating UED as a direct means of investigating electron dynamics. Provided the incident electron pulses have sufficient temporal resolution, the diffraction images are shown to resolve also the relative phases of the target electronic wave functions.

Multistart Spiral Electron Vortices In Ionization By Circularly Polarized Uv Pulses, Jean Marcel Ngoko Djiokap, Alexei V. Meremianin, N. L. Manakov, S. X. Hu, L. B. Madsen, Anthony F. Starace

Anthony F. Starace Publications

Multistart spiral vortex patterns are predicted for the electron momentum distributions in the polarization plane following ionization of the helium atom by two time-delayed circularly polarized ultrashort laser pulses. For two ultraviolet (UV) pulses having the same frequency (such that two photons are required for ionization), single-color two-photon interferometry with corotating or counter-rotating time-delayed pulses is found to lead respectively to zero-start or four-start spiral vortex patterns in the ionized electron momentum distributions in the polarization plane. In contrast, two-color one-photon plus two-photon interferometry with time-delayed corotating or counter-rotating UV pulses is found to lead respectively to one …

Atomic Photoionization Experiment By Harmonic-Generation Spectroscopy, M. V. Frolov, T. S. Sarantseva, N. L. Manakov, K. D. Fulfer, B. P. Wilson, J. Troß, X. Ren, Erwin D. Poliakoff, A. A. Silaev, N. V. Vvedenskii, Anthony F. Starace, C. A. Trallero-Herrero

Anthony F. Starace Publications

Measurements of the high-order-harmonic generation yield of the argon (Ar) atom driven by a strong elliptically polarized laser field are shown to completely determine the field-free differential photoionization cross section of Ar, i.e., the energy dependence of both the angle-integrated photoionization cross section and the angular distribution asymmetry parameter.

Control Of Threshold Enhancements In Harmonic Generation By Atoms In A Two-Color Laser Field With Orthogonal Polarizations, M. V. Frolov, N. L. Manakov, T. S. Sarantseva, A. A. Silaev, N. V. Vvedenskii, Anthony F. Starace

Anthony F. Starace Publications

Threshold phenomena (or channel-closing effects) are analyzed in high-order harmonic generation (HHG) by atoms in a two-color laser field with orthogonal linearly polarized components of a fundamental field and its second harmonic. We show that the threshold behavior of HHG rates for the case of a weak second harmonic component is sensitive to the parity of a closing multiphoton ionization channel and the spatial symmetry of the initial bound state of the target atom, while for the case of comparable intensities of both components, suppression of threshold phenomena is observed as the relative phase between the components of a two-color …

Electron Vortices In Photoionization By Circularly Polarized Attosecond Pulses, Jean Marcel Ngoko Djiokap, S. X. Hu, L. B. Madsen, N. L. Manakov, A. V. Meremianin, Anthony F. Starace

Anthony F. Starace Publications

Single ionization of He by two oppositely circularly polarized, time-delayed attosecond pulses is shown to produce photoelectron momentum distributions in the polarization plane having helical vortex structures sensitive to the time delay between the pulses, their relative phase, and their handedness. Results are obtained by both ab initio numerical solution of the two-electron time-dependent Schrödinger equation and by a lowest-order perturbation theory analysis. The energy, bandwidth, and temporal duration of attosecond pulses are ideal for observing these vortex patterns.

Scaling Laws For High-Order-Harmonic Generation With Midinfrared Laser Pulses, M. V. Frolov, N. L. Manakov, Wei-Hao Xiong, Liang-You Peng, J. Burgdörfer, Anthony F. Starace

Anthony F. Starace Publications

We derive an analytic expression for thewavelength scaling of the high-order-harmonic generation (HHG) yield induced by midinfrared driving laser fields. It is based on a quasiclassical description of the returning electron wave packet, which is shown to be largely independent of atomic properties. The accuracy of this analytic expression is confirmed by comparison with results of numerical solutions of the time-dependent Schr¨odinger equation for wavelengths in the range of 1.4 μm ≤ λ ≤ 4 μm. We verify the wavelength scaling of the HHG yield found numerically for midinfrared laser fields in a recent paper by Le et al. [