arXiv subjects

M. Spanner

Publications and source records attributed to M. Spanner.

6 recordsLinked to original sources

arXiv2021

Strong Field Ionization of Water: Nuclear Dynamics Revealed by Varying the Pulse Duration

Polyatomic molecules in strong laser fields can undergo substantial nuclear motion within tens of femtoseconds. Ion imaging methods based on dissociation or Coulomb explosion therefore have difficulty faithfully recording the geometry dependence of the field ionization that initiates the dissociation process. Here we compare the strong-field double ionization and subsequent dissociation of water (both H$_2$O and D$_2$O) in 10-fs and 40-fs 800-nm laser pulses. We find that 10-fs pulses turn off before substantial internuclear motion occurs, whereas rapid internuclear motion can take place during the double ionization process for 40-fs pulses. The short-pulse measurements are consistent with a simple tunnel ionization picture, whose predictions help interpret the motion observed in the long-pulse measurements.

physics.atom-ph↗

arXiv2020

Deep learning and high harmonic generation

Using machine learning, we explore the utility of various deep neural networks (NN) when applied to high harmonic generation (HHG) scenarios. First, we train the NNs to predict the time-dependent dipole and spectra of HHG emission from reduced-dimensionality models of di- and triatomic systems based of on sets of randomly generated parameters (laser pulse intensity, internuclear distance, and molecular orientation). These networks, once trained, are useful tools to rapidly generate the HHG spectra of our systems. Similarly, we have trained the NNs to solve the inverse problem - to determine the molecular parameters based on HHG spectra or dipole acceleration data. These types of networks could then be used as spectroscopic tools to invert HHG spectra in order to recover the underlying physical parameters of a system. Next, we demonstrate that transfer learning can be applied to our networks to expand the range of applicability of the networks with only a small number of new test cases added to our training sets. Finally, we demonstrate NNs that can be used to classify molecules by type: di- or triatomic, symmetric or asymmetric, wherein we can even rely on fairly simple fully connected neural networks. With outlooks toward training with experimental data, these NN topologies offer a novel set of spectroscopic tools that could be incorporated into HHG experiments.

physics.optics↗

arXiv2015

Optical quantum memory for ultrafast photons using molecular alignment

The absorption of broadband photons in atomic ensembles requires either an effective broadening of the atomic transition linewidth, or an off-resonance Raman interaction. Here we propose a scheme for a quantum memory capable of storing and retrieving ultrafast photons in an ensemble of two-level atoms by using a propagation medium with a time-dependent refractive index generated from aligning an ensemble of gas-phase diatomic molecules. The refractive index dynamics generates an effective longitudinal inhomogeneous broadening of the two-level transition. We numerically demonstrate this scheme for storage and retrieval of a weak pulse as short as 50 fs, with a storage time of up to 20 ps. With additional optical control of the molecular alignment dynamics, the storage time can be extended about one nanosecond leading to time-bandwidth products of order $10^4$. This scheme could in principle be achieved using either a hollow-core fiber or a high-pressure gas cell, in a gaseous host medium comprised of diatomic molecules and a two-level atomic vapor at room temperature.

quant-ph↗

arXiv2012

Probing Asymmetric Molecules with High Harmonic Generation. [Original manuscript as prepared on 22/05/2011]

Asymmetric molecules look different when viewed from one side or the other. This difference influences the electronic structure of the valence electrons, thereby giving stereo sensitivity to chemistry and biology. We show that attosecond and re-collision science provides a detailed and sensitive probe of electronic asymmetry. On each 1/2 cycle of an intense light pulse, laser-induced tunnelling extracts an electron wave packet from the molecule. When the electron wave packet recombines, alternately from one side of the molecule or the other, its amplitude and phase asymmetry determines the even and odd harmonics radiation that it generates. This harmonic spectrum encodes three manifestations of asymmetry; an amplitude and phase asymmetry in electron tunneling; an asymmetry in the phase that the electron wave packet accumulates relative to the ion between the moment of ionization and recombination; and an asymmetry in the amplitude and phase of the transition moment. We report the first measurement of high harmonics from oriented gas samples. We determine the phase asymmetry of the attosecond XUV pulses emitted when an electron recollides from opposite sides of the CO molecule, and the phase asymmetry of the recollision electron just before recombination. We discuss how the various contributions to asymmetry can be isolated in future experiments.

physics.atom-ph↗

arXiv2012

Oriented rotational wave-packet dynamics studies via high harmonic generation

We produce oriented rotational wave packets in CO and measure their characteristics via high harmonic generation. The wavepacket is created using an intense, femtosecond laser pulse and its second harmonic. A delayed 800 nm pulse probes the wave packet, generating even-order high harmonics that arise from the broken symmetry induced by the orientation dynamics. The even-order harmonic radiation that we measure appears on a zero background, enabling us to accurately follow the temporal evolution of the wave packet. Our measurements reveal that, for the conditions optimum for harmonic generation, the orientation is produced by preferential ionization which depletes the sample of molecules of one orientation.

physics.atom-ph↗

arXiv2006

Observation of high-order quantum resonances in the kicked rotor

Quantum resonances in the kicked rotor are characterized by a dramatically increased energy absorption rate, in stark contrast to the momentum localization generally observed. These resonances occur when the scaled Planck's constant hbar=(r/s)*4pi, for any integers r and s. However only the hbar=r*2pi resonances are easily observable. We have observed high-order quantum resonances (s>2) utilizing a sample of low temperature, non-condensed atoms and a pulsed optical standing wave. Resonances are observed for hbar=(r/16)*4pi r=2-6. Quantum numerical simulations suggest that our observation of high-order resonances indicates a larger coherence length than expected from an initially thermal atomic sample.

quant-ph↗