arXiv subjects

Thomas Weinacht

Publications and source records attributed to Thomas Weinacht.

12 recordsLinked to original sources

arXiv2026

Coherent quantum control of dark excitons in hybrid metal organic chalchogenolates

Artificial atom-like systems are a promising candidate for next generation quantum processing. Among them, dark excitons exhibit one of the longest lifetimes at high temperatures. Here, we demonstrate coherent control of dark excitonic states in metal-organic chalcogenolates (MOChas) by using an ultrafast pulse shaper at room temperature. These dark exciton states are optically accessed via two-photon absorption and directly read out with a four-wave mixing process. The system is described by a non-perturbative, two-photon Hamiltonian based on well-known atomic physics and applied to a three level system comprised of two dark excitons. Empirical and theoretical state specific optical access is shown via a simple optical pulse shape. The developed Hamiltonian-based description is a first step towards a quantum processing platform using three-level systems and two photon transitions, one example being dark excitons in the MOCha silver benzeneselenolate (mithrene). Simple conditions for gate operations are laid out and described.

quant-ph↗

arXiv2026

Molecular Attoscope: Pulse Shape Spectroscopy of Electronic Coherence

Tracking the coupled motion of electrons and nuclei on their intrinsic timescales is essential to understanding and controlling photochemical transformations. While attosecond techniques have provided unprecedented insight into electronic dynamics, they have largely been restricted to ionic systems, with nuclear motion often neglected or indirectly inferred. Here, we demonstrate a ``molecular attoscope", which uses shaped laser pulses in the deep ultraviolet to perform a coherent measurement of electronic and nuclear dynamics in an entangled wave packet in neutral benzene. This enables us to trace both the 856-attosecond-period electronic motion and the 36-femtosecond-period nuclear motion. We observe electronic coherence persisting over hundreds of optical cycles, modulated by nuclear dynamics. Our holographic approach is general, and lays the groundwork for coherent measurements capable of visualizing the evolution of the coupled electronic-nuclear wave function in real time.

quant-ph↗

arXiv2026

Remote dispersion scan: transformer-network retrieval of ultrafast pulses after non-linear propagation

Accurate and rapid characterization of broadband electric fields is essential for all ultrafast applications and remains an active field of research. In this work, we introduce remote dispersion scan, a transformer neural network enabled dispersion scan based pulse characterization method that can characterize femtosecond laser pulses. A local scan of the non-linear spectral phase before several linear and nonlinear processes, including amplification, compression, and self phase modulation, allows for the field retrieval remotely at the interaction region. We show that the reconstruction accuracy obtained from a single measurement of the fundamental and second harmonic is comparable to that of a full two dimensional scan. We confirm the technique experimentally by compressing a 300 W, 1.3 ps, 1030 nm pulse in a hollow core fiber to 100 fs and measuring the fundamental and second harmonic spectra while scanning the second order phase in a pulse shaper before power amplification. These results establish a simple, robust, alignment insensitive live-view pulse reconstruction modality.

physics.optics↗

arXiv2025

Delay in electronic vortex states created by multiphoton ionization with single elliptically polarized laser pulses

We show experimentally and theoretically that vortex-shaped structures in the photoelectron momentum distribution can be observed for atoms interacting with a single intense elliptically polarized laser pulse. Our analysis reveals that these spiral structures are the result of destructive interference of two dominant photoelectron vortex states, which are released into the continuum by strong-field ionization. An electron born into one of those states is temporarily delayed near the atomic core by the combined atomic and laser potential, leading to fast changes in the phase delay with energy for photoelectrons in these vortex states. Our results open the door to studying electron dynamics of vortex states in strong-field ionization.

physics.atom-ph↗

arXiv2023

Direct Observation of Entangled Electronic-Nuclear Wave Packets

We present momentum resolved covariance measurements of entangled electronic-nuclear wave packets created and probed with octave spanning phaselocked ultrafast pulses. We launch vibrational wave packets on multiple electronic states via multi-photon absorption, and probe these wave packets via strong field double ionization using a second phaselocked pulse. Momentum resolved covariance mapping of the fragment ions highlights the nuclear motion, while measurements of the yield as a function of the relative phase between pump and probe pulses highlight the electronic coherence. The combined measurements allow us to directly visualize the entanglement between the electronic and nuclear degrees of freedom and follow the evolution of the complete wavefunction.

quant-ph↗

arXiv2023

Long Lived Electronic Coherences in Molecular Wave Packets Probed with Pulse Shape Spectroscopy

We explore long lived electronic coherences in molecules using shaped ultrafast laser pulses to launch and probe entangled nuclear-electronic wave packets. We find that under certain conditions, the electronic phase remains well defined despite vibrational motion along many degrees of freedom. The experiments are interpreted with the help of electronic structure calculations which corroborate our interpretation of the measurements

quant-ph↗

arXiv2023

High Repetition-Rate Pulse Shaping of a Spectrally Broadened Yb Femtosecond Laser

We demonstrate compression and shaping of few cycle pulses from a high average power Ytterbium laser system. The pulses from a commercial 20 W, 100 kHz Yb laser system are spectrally broadened in two-stages using gas-filled, stretched hollow-core fibers and then compressed and shaped in an acousto-optic modulator-based pulse-shaper. The pulse-shaper allows for compression, characterization, and shaping all in one system, producing ~10 fs pulses with 50 uJ of energy

physics.optics↗

arXiv2022

A plano-convex thick-lens velocity map imaging apparatus for direct, high resolution 3D momentum measurements of photoelectrons with ion time-of-flight coincidence

Since its inception, velocity map imaging (VMI) has been a powerful tool for measuring the 2D momentum distribution of photoelectrons generated by strong laser fields. There has been continued interest in expanding it into 3D measurements either through reconstructive or direct methods. Recently much work has been devoted to the latter of these, particularly by relating the electron time-of-flight (TOF) to the third momentum component. The technical challenge here is having timing resolution sufficient to resolve structure in the narrow (< 10 ns) electron TOF spread. Here we build upon work in the fields of VMI lens design and 3D VMI measurement by using a plano-convex thick-lens VMI in conjunction with an event-driven camera (TPX3CAM) providing TOF information for high resolution 3D electron momentum measurements. We perform simulations to show that, with the addition of a mesh electrode to the thick-lens VMI geometry, a plano-convex electrostatic field is formed which extends the detectable electron cutoff energy range while retaining high resolution. Further, the thick-lens also extends the electron TOF range which allows for better resolution of the momentum along this axis. We experimentally demonstrate these capabilities by examining above-threshold ionization in Xenon where the apparatus is shown to collect electrons of energy up to $\sim$7 eV with a TOF spread of $\sim$30 ns, both of which are improvements on previous work by factors of $\sim$1.4 and $\sim$3.75 respectively. Finally, the PCTL-VMI is equipped with a coincident ion TOF spectrometer which is shown to effectively extract unique 3D momentum distributions for different ionic species within a gas mixture. These techniques have potential to lend themselves to more advanced measurements, particularly involving systems where the electron momentum distributions possess non-trivial symmetries and require high resolution.

physics.ins-det↗

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↗

arXiv2017

Coincidence velocity map imaging using Tpx3Cam, a time stamping optical camera with 1.5 ns timing resolution

We demonstrate a coincidence velocity map imaging apparatus equipped with a novel time stamping fast optical camera, Tpx3Cam, whose high sensitivity and ns timing resolution allow for simultaneous position and time-of-flight detection. This single detector design is simple, flexible and capable of highly differential measurements. We show detailed characterization of the camera and its application in strong field ionization experiments.

physics.ins-det↗

arXiv2016

Nonadiabatic dynamics and multiphoton resonances in strong field molecular ionization with few cycle laser pulses

We study strong field molecular ionization using few- (four to ten) cycle laser pulses. Employing a supercontinuum light source, we are able to tune the optical laser wavelength (photon energy) over a range of about $\sim$200 nm (500 meV). We measure the photoelectron spectrum for a series of different molecules as a function of laser intensity, frequency, and bandwidth and illustrate how the ionization dynamics vary with these parameters. We find that multiphoton resonances and nonadiabatic dynamics (internal conversion) play an important role and result in ionization to different ionic continua. Interestingly, while nuclear dynamics can be "frozen" for sufficiently short laser pulses, we find that resonances strongly influence the photoelectron spectrum and final cationic state of the molecule regardless of pulse duration -- even for pulses that are less than four cycles in duration.

physics.chem-ph↗

arXiv2016

Strong Field Molecular Ionization in the Impulsive Limit: Freezing Vibrations with Short Pulses

We study strong-field molecular ionization as a function of pulse duration. Experimental measurements of the photoelectron yield for a number of molecules reveal competition between different ionization continua (cationic states) which depends strongly on pulse duration. Surprisingly, in the limit of short pulse duration, we find that a single ionic continuum dominates the yield, whereas multiple continua are produced for longer pulses. Using calculations which take vibrational dynamics into account, we interpret our results in terms of nuclear motion and non-adiabatic dynamics during the ionization process.

physics.chem-ph↗