Prof. Luca Argenti, University of Central Florida

ASTRA: A Transition-Density-Matrix Approach to Time-Resolved Molecular Ionization

Attosecond science, which investigates the time-resolved correlated motion of electrons in atoms, molecules, and solids, is rapidly advancing toward larger molecular systems and more complex processes, such as multiple ionization and molecular fragmentation. Theoretical methods capable of addressing both multiple excitations and photofragment entanglement are essential to capture these phenomena. Among the most promising theoretical approaches are ab initio wave-function-based close-coupling (CC) methods, increasingly adopted by the AMO community.

Despite significant progress from codes like XCHEM [1,2], tRecX [3], RMT [4], and UKRmol+ [5], scaling remains a major challenge – whether in handling ionic correlation, accounting for many atoms, or for distant fragments. To address these limitations, we developed ASTRA [6] (AttoSecond TRAnsitions), an ab initio CC molecular ionization code based on high-order transition density matrices between correlated ionic states of arbitrary multiplicity [7], and hybrid Gaussian-B-spline integrals [5,9]. ASTRA integrates multiple state-of-the-art codes, such as DALTON [8], a general-purpose quantum chemistry code, LUCIA [7], a large-scale CI code, and GBTOlib [5], a hybrid integral library suited for slow photoelectrons and comparatively small molecules.

ASTRA has successfully reproduced total and partial photoionization cross sections, photoemission asymmetry parameters, and molecular-frame photoelectron angular distributions for molecules such as N ₂ , CO, H ₂ CO, and Pyrazine, showing excellent agreement with existing benchmarks. Currently, ASTRA is being applied to study attosecond transient absorption spectra of CO and O ₂ , as well as sequential XUV-pump IR-probe ionization of C ₂ H ₄ . Its formalism naturally extends to molecular double ionization and can efficiently model electron exchange between multiple disjoint molecular fragments − relevant for describing ionization in weakly bound clusters like (H ₂ O) _n .

Looking ahead, continued integration with tools tailored to high-energy photoemission, non-adiabatic nuclear dynamics, and strong fields ionization will be critical for addressing emerging challenges in ultrafast many-body dynamics. Free-electron lasers enable time-resolved studies of core ionization, while table-top attosecond pump-probe experiments are targeting increasingly larger molecules, monitoring both electron dynamics and nuclear rearrangements throughout chemical reactions with intense probe pulses [10]. To reproduce these complex experiments, we are collaborating with NIST to replace GBTOlib with a more efficient hybrid library capable of handling larger molecules and higher orbital angular momenta. We are also pairing ASTRA with surface-hopping methods [11], where multiphoton ionization is typically not available. Additionally, to track the asymptotic evolution of weakly coupled photofragments under strong light fields − without incurring prohibitive computational costs − we are considering integrating separate optimized propagators for each fragment, which will open the door for us to simulate strong-field multichannel molecular-ionization processes.

[1] M. Klinker et al., J. Phys. Chem. Lett. 9, 756 (2018).

[2] V. J. Borràs et al., Science Advances 9, eade3855 (2023).

[3] A. Scrinzi, Comput. Phys. Commun. 270, 108146 (2022).

[4] A. C. Brown et al., Comput. Phys. Commun. 250, 107062 (2020).

[5] Z. Masin et al., Comp. Phys. Commun. 249, 107092 (2020).

[6] J. M. Randazzo et al., Phys. Rev. Res. 5, 043115 (2023).

[7] J. Olsen et al., J. Chem. Phys. 89, 2185 (1988); ibid. 104, 8007 (1996).

[8] K. Aidas et al., Comp. Mol. Sci. 4, 269 (2014).

[9] H. Gharibnejad et al., Comp. Phys. Commun. 263, 107889 (2021).

[10] F. Vismarra et al., Nature Chemistry (2024).

[11] L. Fransén et al., J. Phys. Chem. A 128, 1457 (2024).

Prof. Bryce Gadway, Penn State

Synthetic Dimensions in Rydberg Atom Array

Arrays of dipolar-interacting spins - magnetic atoms, polar molecules, and Rydberg atoms - represent powerful and versatile platforms for analog quantum simulation experiments. The internal state dynamics in these dipolar arrays provide a natural setting to explore problems of equilibrium and non-equilibrium quantum magnetism. The presence of many internal states of the atoms and molecules further enables studies of large-spin magnetism, but also holds promise for more general quantum simulation studies. Here we describe how the simple addition of multi-frequency microwave fields to Rydberg arrays enables highly controllable studies of few- and many-body dynamics along an internal-state “synthetic” dimension. I’ll discuss several early studies in the Rydberg synthetic dimension platform, touching on interaction-driven phenomena relevant to topology, artificial gauge fields, and disorder-induced localization. Looking forward, such microwave manipulation opens up several new directions for exploring complex, driven quantum matter in dipolar arrays.

Prof. Wenchao Ge, University of Rhode Island

How to Make a Faster Trapped-Ion Quantum Computer?

Trapped ions offer a pristine platform for quantum computation, but enhancing the interactions without compromising the qubits remains a crucial challenge. In this talk, I will present a strategy to enhance the interaction strengths in trapped-ion systems via parametric amplification of the ions’ motion, thereby suppressing the relative importance of decoherence. We illustrate the power of this approach by showing how it can improve the speed and fidelity of two-qubit gates in multi-ion systems and how it can enhance collective spin states useful for quantum metrology. Our proposal has been further demonstrated in the experiment, confirming the enhancement. Our results open a new avenue of phonon modulation in trapped ions and are directly relevant to numerous other physical platforms in which spin interactions are mediated by bosons.

Jake Lewitt, Cortex Fusion, New York, NY

Nuclear fusion in molecules using lasers

Cortex Fusion Systems, Inc. uses shaped ultrafast laser pulses to catalyze fusion reactions in molecules. Our work comprises (1) designing transiently confining effective one-electron potentials in field-dressed molecules, (2) performing quantum chemistry calculations to validate the enhancement of nuclear tunneling by laser-modified electron screening dynamics, and (3) testing pulse shapes in the laser lab by coupling ultrafast spectroscopy techniques with nuclear radiation detection and spectrometry. In this regard, “quantum-controlled fusion” is a coherent, under-the-barrier process that does not require plasma ignition. Our goal is to repurpose the modern suite of commercial femtosecond laser amplifiers and pulse-shaping techniques to achieve compact and scalable fusion generators using quantum control.

Dr. Zeyang Li, Stanford University

Applying Cavity QED to Quantum Information Science

Abstract TBA

Dr. Esteban Goetz, Department of Physics, University of Connecticut

Interferometric Harmonic Spectroscopy for Electron Dynamics Imaging and Attosecond Pulse Train Phase Characterization

The advent of ultrashort light pulses has opened the possibility of investigating atomic and molecular processes on their natural time scales. In particular, Attosecond Transient Absorption Spectroscopy (ATAS) [1], a technique that allows to time-resolve the quantum dynamics of electrons by monitoring the absorption of extreme ultraviolet (XUV) radiation by an atomic or molecular system when the latter is dressed by an infrared (IR) laser source.

Motivated by recent experimental advances in self-referenced interferometric harmonic spectroscopy [2], we theoretically investigate an alternative approach to ATAS for electron dynamics imaging and attosecond pulse train (APT) phase characterization. In contrast to ATAS, which gives access to the imaginary part of the refractive index through an absorption measurement, an interferometric phase measurement gives information of its real part. In this talk, I will discuss the link between the XUV phase measurements of Ref. [2] and the different photoexcitation pathways occurring at the atomic level which are imprinted in the real part of the macroscopic refractive index. As an application, we show how such an interferometric approach can be used for phase retrieval of attosecond pulse trains based on two-arm harmonic spectroscopy and an optimization algorithm. Finally, I will highlight the impact of spin-orbit couplings and macroscopic and field propagation effects on the phase measurements and APT phase retrieval. Our theoretical description is based on numerical solution of the scalar Maxwell equations beyond Beer’s Law for the macroscopic field propagation coupled to the time-dependent Schroedinger equation for the quantum dynamics.

[1] M. Holler et al., Phys. Rev. Lett. 106, 123601 (2011)

[2] G. R. Harrison et al., arXiv:2305.17263 (2023)

Graduate student Geoff Harrison, Department of Physics, University of Connecticut

ITAS: A Technique for Complete Quantum Measurements on a New Timescale

Transient absorption spectroscopy is a well-established technique used to study electron dynamics in atomic and molecular systems but typically can only measure the magnitude of the electronic wavefunction. We have integrated interferometric methods into this technique to allow complete quantum measurements of both the magnitude and phase of electronic wavefunctions. A spatial light modulator (SLM) is used to separate the interferometric arms in an extremely stable way, enabling the measurement of effects on the zeptosecond timescale (with a jitter of 3zs). In this talk, I’ll describe how we’ve utilized SLMs to make these measurements possible and share some initial data we’ve taken looking at phase effects in argon.

Graduate student Debadarshini Mishra, Department of Physics, University of Connecticut

Imaging ultrafast dynamics in molecular systems

Imaging electronic and molecular dynamics at the attosecond and femtosecond timescales is crucial for understanding the mechanisms of chemical reactions, a fundamental aspect in fields ranging from materials science to biochemistry. This in-depth understanding of chemical processes may allow for precise control over reaction dynamics, thereby paving the way for advancements in technology and medicine, for example, by guiding the development of efficient catalysis, innovative materials, and targeted drugs. In this talk, I will describe our work on imaging time-resolved molecular dynamics using two distinct and complementary techniques.

In the first part of my talk, I will discuss the use of coincident Coulomb explosion imaging for the direct visualization of roaming reactions. These reactions represent unconventional pathways that allow fragments to remain weakly bonded, leading to the formation of unexpected final products. Typically, the neutral character of the roaming fragment and its indeterminate trajectory make direct experimental identification challenging. However, I will demonstrate that by leveraging the power of coincidence imaging, we can reconstruct the momentum vector of the neutral roamer and thus identify an unambiguous signature for roaming.

In the second part of my talk, I will discuss the imaging of UV-induced ring-opening and dissociation dynamics using ultrafast electron diffraction. I will demonstrate that by harnessing the superior temporal and structural resolution of this technique, we can explore the competition among different molecular pathways as well as their wavelength-dependent behavior.

Dr. François Légaré, Institut national de la recherche scientifique, Energy Materials Télécommunications center

Ultrafast IR/mid-IR laser technologies and their applications at ALLS

The Advanced Laser Light Source (ALLS) is a unique user facility located at INRS-EMT (Varennes, Canada) counting on 40M CDN$ of investment since 2002. Since 2019, this facility has jointed the LaserNetUS network and is now funded as a national research infrastructure by the Canada Foundation for Innovation – Major Science Initiatives. These fundings ease access to the facility for academic and government users. In the first part of my talk, I will give an overview of the facility’s capabilities including the most powerful laser in Canada with 750 TW. In the second part, I will discuss novel approaches developed by my team for the generation of ultrashort pulses in the IR and mid-IR spectral range. This includes multidimensional solitary states in hollow core fibers [1,2] as well as using the frequency domain optical parametric amplification for the generation of tunable CEP stable mid-IR laser pulses [3,4]. Pulse characterization in the mid-IR spectral range will be presented [5]. Finally, I will present recent results on the generation of high-dose MeV electrons from tight focussing in air [6].

References

[1] R. Safaei, G. Fan, O. Kwon, K. Légaré, P. Lassonde, B. E. Schmidt, H. Ibrahim, and F. Légaré (2020), High-energy multidimensional solitary states in hollow core fiber, Nature Phot. 14, 733-739.

[2] L. Arias, A. Longa, G. Jargot, A. Pomerleau, P. Lassonde, G. Fan, R. Safaei, P. Corkum, F. Boschini, H. Ibrahim, and F. Légaré, Few-cycle Yb laser source at 20 kHz using multidimensional solitary states in hollow-core fibers, Opt. Lett. 47, 3612-3615 (2022).

[3] A. Leblanc, G. Dalla-Barba, P. Lassonde, A. Laramée, B. Schmidt, E. Cormier, H. Ibrahim, and F. Légaré (2020), High-field mid-infrared pulses derived from frequency domain optical parametric amplification, Opt. Lett. 45, 2267-2270.

[4] G. Dalla-Barba, G. Jargot, P. Lassonde, S. Tóth, E. Haddad, F. Boschini, J. Delagnes, A. Leblanc, H. Ibrahim, E. Cormier, and F. Légaré, Mid-infrared frequency domain optical parametric amplifier, Opt. Express 31, 14954-14964 (2023).

[5] A. Leblanc, P. Lassonde, S. Petit, J.-C. Delagnes, E. Haddad, G. Ernotte, M. R. Bionta, V. Gruson, B. E. Schmidt, H. Ibrahim, E. Cormier, and F. Légaré (2019), Phase-matching-free pulse retrieval based on transient absorption in solids, Opt. Express 27, 28998.

[6] S. Vallières, J. Powell, T. Connell, M. Evans, M. Lytova, F. Fillion-Gourdeau, S. Fourmaux, S. Payeur, P. Lassonde, S. MacLean, and F. Légaré, High Dose-Rate MeV Electron Beam from a Tightly-Focused Femtosecond IR Laser in Ambient Air (2024), Laser Photonics Rev. 18, 2300078.

François Légaré is a chemical physicist who specializes in developing novel approaches for ultrafast science and technologies, as well as biomedical imaging with nonlinear optics (Ph.D. in chemistry, 2004 – co-supervised by Profs. André D. Bandrauk and Paul B. Corkum). Full professor (2013 - …) at the Energy Materials Telecommunications center of the Institut national de la recherche scientifique (INRS-EMT), he was the director of the Advanced Laser Light Source (ALLS) until 2023. Since 2022, he is the director of the INRS-EMT center and CEO of ALLS. Under his scientific leadership, INRS has received in 2017 a grant of 13.9M CDN$ from the Canada Foundation for Innovation and the Quebec government, with 11.9M CDN$ to upscale the ALLS facility with high average power Ytterbium laser systems and advanced instrumentation for time-resolved material characterization. He is a Fellow and senior member of OPTICA and Fellow of the American Physical Society. He is a member of The College of New Scholars, Artists and Scientists of the Royal Society of Canada (2017). He was awarded the Herzberg medal from the Canadian Association of Physics in 2015 and the Rutherford Memorial Medal in physics of the Royal Society of Canada in 2016. He has contributed to about 200 articles in peer reviewed journals including prestigious ones such as Nature, Science, Nature Photonics, Nature Physics, Nature Communications, and Physical Review Letters. According to Google Scholar, his h-index is 59 with more than 13,000 citations.

Dr. Thomas Weinacht, Stony Brook University

Long Lived Electronic Coherences in Molecules

I will discuss experiments and calculations that demonstrate long lived electronic coherences in molecules using a combination of measurements with shaped octave spanning ultrafast laser pulses, 3D velocity map imaging and calculations of the light matter interaction. Our pump-probe measurements prepare and interrogate entangled nuclear-electronic wave packets whose electronic phase remains well defined despite vibrational motion along many degrees of freedom. The experiments and calculations illustrate how coherences between excited electronic states survive even when coherence with the ground state is lost, and may have important implications for light harvesting, electronic transport and attosecond science.