Professor Puckett's Research Homepage

Dr. Jakob den Brok, Harvard Smithsonian Center for Astrophysics

Title and abstract TBA

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).

Madisyn Brooks, UConn

Title and abstract TBA

Adam Riess- Bloomberg Distinguished Professor and 2011 co-winner of the Nobel Prize in Physics, Johns Hopkins University

In 1929 Edwin Hubble discovered that our Universe is expanding. Eighty years later, the Space Telescope that bears his name is being used to study an even more surprising phenomenon: that the expansion is speeding up. The origin of this effect is not known, but is broadly attributed to a type of “dark energy” first posited to exist by Albert Einstein and now dominating the mass-energy budget of the Universe. Professor Riess will describe how his team discovered the acceleration of the Universe and why understanding the nature of dark energy presents one of the greatest remaining challenges in astrophysics and cosmology. He will also discuss recent evidence that the Universe continues to defy our best efforts to predict its behavior.

Adam Riess is a Bloomberg Distinguished Professor, the Thomas J. Barber Professor in Space Studies at the Krieger School of Arts and Sciences, a distinguished astronomer at the Space Telescope Science Institute and a member of the National Academy of Sciences.

He received his bachelor’s degree in physics from the Massachusetts Institute of Technology in 1992 and his PhD from Harvard University in 1996. His research involves measurements of the cosmological framework with supernovae (exploding stars) and Cepheids (pulsating stars). Currently, he leads the SHOES Team in efforts to improve the measurement of the Hubble Constant and the Higher-z Team to find and measure the most distant type Ia supernovae known to probe the origin of cosmic acceleration.

In 2011, he was named a co-winner of the Nobel Prize in Physics and was awarded the Albert Einstein Medal for his leadership in the High-z Supernova Search Team’s discovery that the expansion rate of the universe is accelerating, a phenomenon widely attributed to a mysterious, unexplained “dark energy” filling the universe. The discovery was named by Science magazine in 1998 as “the Breakthrough Discovery of the Year.”

His accomplishments have been recognized with a number of other awards, including a MacArthur Fellowship in 2008, the Gruber Foundation Cosmology Prize in 2007 (shared), and the Shaw Prize in Astronomy in 2006.

Reception at 3:00pm in the Gant Science Light Court

Prof. Lina Necib, Department of Physics, MIT

Title and abstract TBA