Two-electron interference in two-photon attosecond double ionization of neon DOI
S. Chattopadhyay, Carlos Marante, Barry I. Schneider

et al.

Physical review. A/Physical review, A, Journal Year: 2024, Volume and Issue: 110(1)

Published: July 2, 2024

The pump-probe experiments enabled by x-ray free-electron lasers (XFEL) will allow us to directly observe correlated electronic motion with attosecond time resolution detecting photoelectron pairs in coincidence. In helium, the transition between nonsequential and sequential regime two-photon double ionization (TPDI) is well explained a virtual-sequential model. Much less known, however, about TPDI process more complex atoms. Recently, we extended model arbitrary light pulses [Chattopadhyay et al. Phys. Rev. A 108, 013114 (2023)]. This extension employs multichannel scattering states for single of both neutral ionized target, which initially applied helium. present study, show that our reproduces qualitative features angularly integrated observables available experimental results neon, considerably target. We an intriguing feature inverted two-particle interference joint-energy distribution $\mathrm{Ne}$ compared $\mathrm{He}$. phenomenon, attributable presence final doubly state triplet symmetry coupled two photoelectrons, should be observable current technologies.

Language: Английский

Selecting Initial Conditions for Trajectory-Based Nonadiabatic Simulations DOI Creative Commons
Jiří Janoš, Petr Slavı́ček, Basile F. E. Curchod

et al.

Accounts of Chemical Research, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 9, 2025

ConspectusPhotochemical reactions have always been the source of a great deal mystery. While classified as type chemical reaction, no doubts are allowed that general tenets ground-state chemistry do not directly apply to photochemical reactions. For typical understanding critical points potential (free) energy surface and embedding them in thermodynamics framework is often enough infer reaction yields or characteristic time scales. A working principle profile along minimum paths provides key information characterize reaction. These well-developed concepts, unfortunately, rarely stretch processes involving formation nonstationary state for molecular system after light absorption.Upon photoexcitation, molecule likely undergo internal conversion processes, is, changes electronic states mediated by couplings between nuclear motion, precisely what celebrated Born–Oppenheimer approximation neglects. coupled electron–nuclear coined nonadiabatic allow decay from one other nonradiatively. Understanding intricate dynamics pivotal rationalizing predicting outcome photoexcitation providing insights experiments conducted, example, advanced sources such free-electron lasers.Nowadays, most simulations based on approximations invoke near-classical depiction nuclei. This reliance due practical constraints, classical equations motion nuclei must be supplemented techniques hopping account transitions states. but overlooked aspect these selection initial conditions, specifically choice positions momenta dynamics, which can significantly influence how well mimic real quantum systems across various experimental scenarios. The conventional approach generating conditions typically maps onto phase space using Wigner quasiprobability function within harmonic approximation, followed second where undergoes sudden excitation.In this Account, we aim warn experienced user about possible limitations strategy initial-condition generation its inability accurately describe molecule. More specifically, argue phase-space distribution more represented through thermostat. method offers robust applied large, flexible, even solvated systems. Furthermore, reliability benchmarked against rigorous approaches path integral dynamics. Additionally, commonly used assumes vertical excitation molecule, reflects triggered laser pulses actual spectroscopic experiments. We discuss here generate any pulse. also strategies tackle continuous-wave laser.

Language: Английский

Citations

1
Fragmentation in Coulomb explosion of hydrocarbon molecules DOI
Samuel S. Taylor, K. Varga, Károly Mogyorósi

et al.

Physical review. A/Physical review, A, Journal Year: 2025, Volume and Issue: 111(1)

Published: Jan. 16, 2025

Language: Английский

Citations

1
Opportunities for gas-phase science at short-wavelength free-electron lasers with undulator-based polarization control DOI Creative Commons

Markus Ilchen,

E. Allaria, Primož Rebernik Ribič

et al.

Physical Review Research, Journal Year: 2025, Volume and Issue: 7(1)

Published: Jan. 27, 2025

Free-electron lasers (FELs) are the world's most brilliant light sources with rapidly evolving technological capabilities in terms of ultrabright and ultrashort pulses over a large range photon energies. Their revolutionary innovative developments have opened new fields science regarding nonlinear light-matter interaction, investigation ultrafast processes from specific observer sites, approaches to imaging matter atomic resolution. A core aspect FEL is study isolated prototypical systems gas phase possibility addressing well-defined electronic transitions or particular sites molecules. Notably for polarization-controlled short-wavelength FELs, offers avenues investigations phenomena spin-orientated systems, decoding function chiral building blocks life as well steering reactions particle emission dynamics otherwise inaccessible ways. This roadmap comprises descriptions facilities worldwide, diagnostics instrumentation, recent scientific highlights, novel methodology, mathematical modeling. The experimental theoretical landscape using polarization controllable FELs dichroic interaction will be discussed comprehensively outlined stimulate strengthen global collaborative efforts all disciplines. Published by American Physical Society 2025

Language: Английский

Citations

1
Including Photoexcitation Explicitly in Trajectory-Based Nonadiabatic Dynamics at No Cost DOI Creative Commons
Jiří Janoš, Petr Slavı́ček, Basile F. E. Curchod

et al.

The Journal of Physical Chemistry Letters, Journal Year: 2024, Volume and Issue: 15(42), P. 10614 - 10622

Published: Oct. 15, 2024

Over the last decades, theoretical photochemistry has produced multiple techniques to simulate nonadiabatic dynamics of molecules. Surprisingly, much less effort been devoted adequately describing first step a photochemical or photophysical process: photoexcitation. Here, we propose formalism include effect laser pulse in trajectory-based at level initial conditions, with no additional cost. The promoted density approach (PDA) decouples excitation from by defining new set which an time. PDA surface hopping leads simulations excellent agreement quantum using explicit and highlights strong impact on resulting photodynamics limits (sudden) vertical excitation. Combining methods is possible for any arbitrary-sized molecules code provided this work.

Language: Английский

Citations

4
Time‐Dependent Vibrational Coupled Cluster Theory With Static and Dynamic Basis Functions DOI
Mads Greisen Højlund, Alberto Zoccante, Andreas Buchgraitz Jensen

et al.

Wiley Interdisciplinary Reviews Computational Molecular Science, Journal Year: 2025, Volume and Issue: 15(1)

Published: Jan. 1, 2025

ABSTRACT In recent decades, coupled cluster theory has proven valuable in accurately describing correlation many‐body systems, particularly time‐independent computations of molecular electronic structure and vibrations. This review describes advancements using parameterizations for time‐dependent wave functions the efficient computation quantum dynamics associated with motion nuclei. It covers vibrational (TDVCC) modal (TDMVCC), which employ static adaptive basis sets, respectively. We discuss theoretical foundation, including many‐mode second quantization, bivariational principles, various bases. Additionally, we highlight key features that make TDMVCC promising future dynamical simulations. These include fast configuration‐space convergence, use a compact set, possibility implementations computational cost scales only polynomially system size.

Language: Английский

Citations

0
Quantum effects of Coulomb explosion simulations revealed by time-dependent density-functional theory DOI
Samuel S. Taylor,

Cody Covington,

K. Varga

et al.

Physical review. A/Physical review, A, Journal Year: 2025, Volume and Issue: 111(3)

Published: March 12, 2025

Language: Английский

Citations

0
Assessing the performance of coupled-trajectory schemes on full-dimensional two-state linear vibronic coupling models DOI
Peter Schürger, Lea M. Ibele, David Lauvergnat

et al.

The Journal of Chemical Physics, Journal Year: 2025, Volume and Issue: 162(10)

Published: March 14, 2025

We investigate the performance of coupled-trajectory methods for nonadiabatic molecular dynamics in simulating photodynamics 4-(dimethylamino)benzonitrile (DMABN) and fulvene, with electronic structure provided by linear vibrational coupling models. focus on mixed quantum-classical (CTMQC) algorithm (combined) Tully surface hopping [(C)CTTSH] comparison to independent-trajectory approaches, such as multi-trajectory Ehrenfest hopping. Our analysis includes not only populations but also additional nuclear properties position momentum space. For both DMABN recently developed CCTTSH successfully resolves internal inconsistencies Instead, we find that highlights a significant weakness CTMQC, which arises when trajectories remain long time vicinity region strong nonadiabaticity.

Language: Английский

Citations

0
Multi-Beam-Energy Control Unit Based on Triple-Bend Achromats DOI Creative Commons
Lin Wu, Zihan Zhu,

Bingyang Yan

et al.

Photonics, Journal Year: 2025, Volume and Issue: 12(3), P. 275 - 275

Published: March 17, 2025

X-ray free electron lasers (XFELs) are the new generation of particle accelerator-based light sources, capable producing tunable, high-power pulses that increasingly vital across various scientific disciplines. Recently, continuous-wave (CW) XFELs driven by superconducting linear accelerators have garnered significant attention due to their ability enhance availability supporting multiple undulator lines simultaneously. In this paper, we introduce a novel delay system comprising four triple-bend achromats (TBAs). This was combined with fast kickers and can be employed generate beams on bunch-to-bunch basis in CW-XFEL facility. Based parameters Shanghai High-Repetition-Rate XFEL Extreme Light Facility, start-to-end simulations demonstrate TBA-based achieves excellent beam qualities while providing wide beam-energy-tuning range from 1.39 8 GeV.

Language: Английский

Citations

0
A single-crystal platform for unveiling ultrafast and complex photochemical cascade reactions DOI
Jian‐Ping Lang, Qiaoqiao Zhang, Yun‐Hu Deng

et al.

Research Square (Research Square), Journal Year: 2025, Volume and Issue: unknown

Published: April 25, 2025

Abstract Developing versatile crystalline platforms can significantly enhance the utility of time-resolved X-ray crystallography for observing diverse reaction mechanisms 1–6 . However, it is often limited by its inability to handle ultrafast and complex reactions. Here we propose a coordination polymer single-crystal platform that incorporates flexible cluster nodes integrated substrates. This advanced features enhanced diffraction capabilities adaptability substrate changes, enabling observation ultrafast, highly dynamic reactions involving multiple pathways intermediates. By combining this with cryo-assisted strategy, investigate complicated photochemical cycloaddition five transient intermediates three distinct routes, which are rationalized through theoretical calculations. Our findings underscore feasibility employing unravel elusive mechanisms, presenting promising approach broad applicability.

Language: Английский

Citations

0
Robust Inversion of Time-Resolved Data via Forward-Optimization in a Trajectory Basis DOI Creative Commons

Kyle Acheson,

Adam Kirrander

Journal of Chemical Theory and Computation, Journal Year: 2023, Volume and Issue: 19(10), P. 2721 - 2734

Published: May 2, 2023

An inversion method for time-resolved data from ultrafast experiments is introduced, based on forward-optimization in a trajectory basis. The applied to experimental X-ray scattering of the photochemical ring-opening reaction 1,3-cyclohexadiene and electron diffraction photodissociation CS2. In each case, yields model that reproduces data, identifies main dynamic motifs, agrees with independent observations. Notably, explicitly accounts continuity constraints robust even noisy data.

Language: Английский

Citations

9