arXiv subjects

Michael Spanner

Publications and source records attributed to Michael Spanner.

At least 19 recordsLinked to original sources

arXiv2023

Quantum Relativity

Starting with a consideration of the implication of Bell inequalities in quantum mechanics, a new quantum postulate is suggested in order to restore classical locality and causality to quantum physics: only the relative coordinates between detected quantum events are valid observables. This postulate supports the EPR view that quantum mechanics is incomplete, while also staying compatible to the Bohr view that nothing exists beyond the quantum. The new postulate follows from a more general principle of quantum relativity, which states that only correlations between experimental detections of quantum events have a real classical existence. Quantum relativity provides a framework to differentiate the quantum and classical world.

physics.gen-ph↗

arXiv2022

General Time-Dependent Configuration-Interaction Singles I: The Molecular Case

We present a grid-based implementation of the time-dependent configuration-interaction singles method suitable for computing the strong-field ionization of small gas-phase molecules. After outlining the general equations of motion used in our treatment of this method, we present example calculations of strong-field ionization of helium, lithium hydride, water, and ethylene that demonstrate the utility of our implementation. The following companion paper specializes to the case of spherical symmetry, which is applied to various atoms.

physics.chem-ph↗

arXiv2021

Simulation of many-body dynamics using Rydberg excitons

The recent observation of high-lying Rydberg states of excitons in semiconductors with relatively high binding energy motivates exploring their applications in quantum nonlinear optics and quantum information processing. Here, we study Rydberg excitation dynamics of a mesoscopic array of excitons to demonstrate its application in simulation of quantum many-body dynamics. We show that the $\mathbb{Z}_2$-ordered phase can be reached using physical parameters available for cuprous oxide (Cu$_2$O) by optimizing driving laser parameters such as duration, intensity, and frequency. In an example, we study the application of our proposed system to solving the Maximum Independent Set (MIS) problem based on the Rydberg blockade effect.

quant-ph↗

arXiv2021

Strong Field Ionization of Water II: Electronic and Nuclear Dynamics En Route to Double Ionization

We investigate the role of nuclear motion and strong-field-induced electronic couplings during the double ionization of deuterated water using momentum-resolved coincidence spectroscopy. By examining the three-body dicationic dissociation channel, D$^{+}$/D$^{+}$/O, for both few- and multi-cycle laser pulses, strong evidence for intra-pulse dynamics is observed. The extracted angle- and energy-resolved double ionization yields are compared to classical trajectory simulations of the dissociation dynamics occurring from different electronic states of the dication. In contrast with measurements of single photon double ionization, pronounced departure from the expectations for vertical ionization is observed, even for pulses as short as 10~fs in duration. We outline numerous mechanisms by which the strong laser field can modify the nuclear wavefunction en-route to final states of the dication where molecular fragmentation occurs. Specifically, we consider the possibility of a coordinate-dependence to the strong-field ionization rate, intermediate nuclear motion in monocation states prior to double ionization, and near-resonant laser-induced dipole couplings in the ion. These results highlight the fact that, for small and light molecules such as D$_2$O, a vertical-transition treatment of the ionization dynamics is not sufficient to reproduce the features seen experimentally in the strong field coincidence double-ionization data.

physics.atom-ph↗

arXiv2020

N$_2^+$ Lasing: Gain and Absorption in the Presence of Rotational Coherence

We simulate the pump-probe experiments of lasing in molecular nitrogen ions with particular interest on the effects of rotational wave-packet dynamics. Our computations demonstrate that the coherent preparation of rotational wave packets in N$_2^+$ by an intense short non-resonant pulse results in a modulation of the subsequent emission from $B^2\Sigma_u^+ \rightarrow X^2\Sigma_g^+$ transitions induced by a resonant seed pulse. We model the dynamics of such pumping and emission using density matrix theory to describe the N$_2^+$ dynamics and the Maxwell wave equation to model the seed pulse propagation. We show that the gain and absorption of a delayed seed pulse is dependent on the pump-seed delay, that is, the rotational coherences excited by the pump pulse can modulate the gain and absorption of the delayed seed pulse. Further, we demonstrate that the coherent rotational dynamics of the nitrogen ions can cause lasing without electronic inversion.

physics.optics↗

arXiv2020

Rotational Quantum Beat Lasing Without Inversion

In standard lasers, light amplification requires population inversion between an upper and a lower state to break the reciprocity between absorption and stimulated emission. However, in a medium prepared in a specific superposition state, quantum interference may fully suppress absorption while leaving stimulated emission intact, opening the possibility of lasing without inversion. Here we show that lasing without inversion arises naturally during propagation of intense femtosecond laser pulses in air. It is triggered by the combination of molecular ionization and molecular alignment, both unavoidable in intense light fields. The effect could enable inversionless amplification of broadband radiation in many molecular gases, opening unusual opportunities for remote sensing.

physics.optics↗

arXiv2019

Generation of doubly excited Rydberg states based on Rydberg antiblockade in a cold atomic ensemble

Interaction between Rydberg atoms can significantly modify Rydberg excitation dynamics. Under a resonant driving field the Rydberg-Rydberg interaction in high-lying states can induce shifts in the atomic resonance such that a secondary Rydberg excitation becomes unlikely leading to the Rydberg blockade effect. In a related effect, off-resonant coupling of light to Rydberg states of atoms contributes to the Rydberg anti-blockade effect where the Rydberg interaction creates a resonant condition that promotes a secondary excitation in a Rydberg atomic gas. Here, we study the light-matter interaction and dynamics of off-resonant two-photon excitations and include two- and three-atom Rydberg interactions and their effect on excited state dynamics in an ensemble of cold atoms. In an experimentally-motivated regime, we find the optimal physical parameters such as Rabi frequencies, two-photon detuning, and pump duration to achieve significant enhancement in the probability of generating doubly-excited collective atomic states. This results in large auto-correlation values due to the Rydberg anti-blockade effect and makes this system a potential candidate for a high-purity two-photon Fock state source.

physics.atom-ph↗

arXiv2019

Probing multiphoton light-induced molecular potentials

The strong coupling between intense laser fields and valence electrons in molecules causes a distortion of the potential energy hypersurfaces which determine the motion of nuclei in a molecule and influences possible reaction pathways. The coupling strength varies with the angle between the light electric field and valence orbital, and thereby adds another dimension to the effective molecular potential energy surface, allowing for the emergence of light-induced conical intersections. Here, we demonstrate in theory and experiment that the full complexity of such light-induced potential energy surfaces can be uncovered. In H$_2^+$, the simplest of molecules, we observe a strongly modulated angular distribution of protons which has escaped prior observation. These modulations directly result from ultrafast dynamics on the light-induced molecular potentials and can be modified by varying the amplitude, duration and phase of the mid-infrared dressing field. This opens new opportunities for manipulating the dissociation of small molecules using strong laser fields.

physics.chem-ph↗

arXiv2018

Electron correlations and pre-collision in the re-collision picture of high harmonic generation

We discuss the seminal three-step model and the recollision picture in the context of high harmonic generation in molecules. In particular, we stress the importance of multi-electron correlation during the first and the third of the three steps of the process: (1) the strong field ionization and (3) the recombination. We point out how accurate account for multi-electron correlations during the third, recombination, step allows one to gauge the importance of pre-collision: the term coined by J. H. Eberly to describe unusual pathways during the first, ionization, step.

physics.atom-ph↗

arXiv2017

Streak Camera for Strong-Field Ionization

Ionization of an atom or molecule by a strong laser field produces sub-optical cycle wave packets whose control has given rise to attosecond science. The final states of the wave packets depend on ionization and deflection by the laser field, which are convoluted in conventional experiments. Here, we demonstrate a technique enabling efficient electron deflection, separate from the field driving strong-field ionization. Using a mid-infrared deflection field permits one to distinguish electron wave packets generated at different field maxima of an intense few-cycle visible laser pulse. We utilize this capability to trace the scattering of low-energy electrons driven by the mid-infrared field. Our approach represents a general technique for studying and controlling strong-field ionization dynamics on the attosecond time scale.

physics.optics↗

arXiv2017

Time-bin to Polarization Conversion of Ultrafast Photonic Qubits

The encoding of quantum information in photonic time-bin qubits is apt for long distance quantum communication schemes. In practice, due to technical constraints such as detector response time, or the speed with which co-polarized time-bins can be switched, other encodings, e.g. polarization, are often preferred for operations like state detection. Here, we present the conversion of qubits between polarization and time-bin encodings using a method that is based on an ultrafast optical Kerr shutter and attain efficiencies of 97% and an average fidelity of 0.827+/-0.003 with shutter speeds near 1 ps. Our demonstration delineates an essential requirement for the development of hybrid and high-rate optical quantum networks.

quant-ph↗

arXiv2017

Deep learning and the Schr\"odinger equation

We have trained a deep (convolutional) neural network to predict the ground-state energy of an electron in four classes of confining two-dimensional electrostatic potentials. On randomly generated potentials, for which there is no analytic form for either the potential or the ground-state energy, the neural network model was able to predict the ground-state energy to within chemical accuracy, with a median absolute error of 1.49 mHa. We also investigate the performance of the model in predicting other quantities such as the kinetic energy and the first excited-state energy of random potentials.

cond-mat.mtrl-sci↗

arXiv2015

Ultrafast slow-light: Raman-induced delay of THz-bandwidth pulses

We propose and experimentally demonstrate a scheme to generate optically-controlled delays based on off-resonant Raman absorption. Dispersion in a transparency window between two neighboring, optically-activated Raman absorption lines is used to reduce the group velocity of broadband 765 nm pulses. We implement this approach in a potassium titanyl phosphate (KTP) waveguide at room temperature, and demonstrate Raman-induced delays of up to 140 fs for a 650-fs duration, 1.8-THz bandwidth, signal pulse; the available delay-bandwidth product is $\approx1$. Our approach is applicable to single photon signals, offers wavelength tunability, and is a step toward processing ultrafast photons.

quant-ph↗

arXiv2015

Comment on "Human Time-Frequency Acuity Beats the Fourier Uncertainty Principle"

In the initial article [Phys. Rev. Lett. 110, 044301 (2013), arXiv:1208.4611] it was claimed that human hearing can beat the Fourier uncertainty principle. In this Comment, we demonstrate that the experiment designed and implemented in the original article was ill-chosen to test Fourier uncertainty in human hearing.

q-bio.NC↗

arXiv2013

Transition between mechanisms of laser-induced field-free molecular orientation

The transition between two distinct mechanisms for the laser-induced field-free orientation of CO molecules is observed via measurements of orientation revival times and subsequent comparison to theoretical calculations. In the first mechanism, which we find responsible for the orientation of CO up to peak intensities of 8 x 10^13 W/cm^2, the molecules are impulsively oriented through the hyperpolarizability interaction. At higher intensities, asymmetric depletion through orientation-selective ionization is the dominant orienting mechanism. In addition to the clear identification of the two regimes of orientation, we propose that careful measurements of the onset of the orientation depletion mechanism as a function of the laser intensity will provide a relatively simple route to calibrate absolute rates of non-perturbative strong-field molecular ionization.

physics.chem-ph↗

arXiv2012

Mechanisms of two-color laser-induced field-free molecular orientation

Two mechanisms of two-color (ω+ 2ω) laser-induced field-free molecular orientation, based on the hyperpolarizability and ionization depletion, are explored and compared. The CO molecule is used as a computational example. While the hyperpolarizability mechanism generates small amounts of orientation at intensities below the ionization threshold, ionization depletion quickly becomes the dominant mechanism as soon as ionizing intensities are reached. Only the ionization mechanism leads to substantial orientation (e.g. on the order of | | > 0.1). For intensities typical of laser-induced molecular alignment and orientation experiments, the two mechanism lead to robust, characteristic timings of the field-free orientation wave-packet revivals relative to the the alignment revivals and the revival time. The revival timings can be used to detect the active orientation mechanism experimentally.

physics.atom-ph↗

arXiv2011

Multifaceted Faculty Network Design and Management: Practice and Experience Report

We report on our experience on multidimensional aspects of our faculty's network design and management, including some unique aspects such as campus-wide VLANs and ghosting, security and monitoring, switching and routing, and others. We outline a historical perspective on certain research, design, and development decisions and discuss the network topology, its scalability, and management in detail; the services our network provides, and its evolution. We overview the security aspects of the management as well as data management and automation and the use of the data by other members of the IT group in the faculty.

cs.NI↗

arXiv2009

One-Electron Ionization of Multielectron Systems in Strong Nonresonant Laser Fields

We present a novel approach to calculating strong field ionization dynamics of multielectron molecular targets. Adopting a multielectron wavefunction ansatz based on field-free ab initio neutral and ionic multielectron states, a set of coupled time-dependent single-particle Schroedinger equations describing the neutral amplitude and continuum electron are constructed. These equations, amenable to direct numerical solution or further analytical treatment, allow one to study multielectron effects during strong field ionization, recollision, and high harmonic generation. We apply the method to strong field ionization of CO_2, and suggest the importance of intermediate core excitation to explain previous failure of analytical models to reproduce experimental ionization yields for this molecule.

physics.atom-ph↗