4.8 Article

State-resolved attosecond reversible and irreversible dynamics in strong optical fields

期刊

NATURE PHYSICS
卷 13, 期 5, 页码 472-478

出版社

NATURE PUBLISHING GROUP
DOI: 10.1038/NPHYS4027

关键词

-

资金

  1. National Science Foundation (NSF) [CHE-1361226]
  2. US Army Research Office (ARO) [W911NF-14-1-0383]
  3. Ministry of Education [MOE2014-T2-2-052]
  4. Agency for Science, Technology and Research [1223600008, 1321202083]
  5. Alexander von Humboldt Foundation
  6. NSF
  7. Division Of Chemistry
  8. Direct For Mathematical & Physical Scien [1361226] Funding Source: National Science Foundation

向作者/读者索取更多资源

Strong-field ionization (SFI) is a key process for accessing real-time quantum dynamics of electrons on the attosecond timescale. The theoretical foundation of SFI was pioneered in the 1960s, and later refined by various analytical models. While asymptotic ionization rates predicted by these models have been tested to be in reasonable agreement for a wide range of laser parameters, predictions for SFI on the sub-laser-cycle timescale are either beyond the scope of the models or show strong qualitative deviations from full quantum-mechanical simulations. Here, using the unprecedented state specificity of attosecond transient absorption spectroscopy, we follow the real-time SFI process of the two valence spin-orbit states of xenon. The results reveal that the irreversible tunnelling contribution is accompanied by a reversible electronic population that exhibits an observable spin-orbit-dependent phase delay. A detailed theoretical analysis attributes this observation to transient ground-state polarization, an unexpected facet of SFI that cannot be captured by existing analytical models that focus exclusively on the production of asymptotic electron/ion yields.

作者

我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。

评论

主要评分

4.8
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

Article Biochemistry & Molecular Biology

Tree-Code Based Improvement of Computational Performance of the X-ray-Matter-Interaction Simulation Tool XMDYN

Michal Stransky, Zoltan Jurek, Robin Santra, Adrian P. Mancuso, Beata Ziaja

Summary: In this work, tree-algorithm based solvers were incorporated into the molecular dynamics code XMDYN for the first time, improving its performance and enabling computationally efficient simulations of X-ray irradiated large atomic assemblies.

MOLECULES (2022)

Article Optics

In situ characterization of few-femtosecond laser pulses by learning from first-principles calculations

Otfried Geffert, Daria Kolbasova, Andrea Trabattoni, Francesca Calegari, Robin Santra

Summary: The field of ultrafast spectroscopy relies on precise characterization of ultrashort laser pulses. This study proposes an in situ characterization scheme based on first-principles calculations and introduces a machine-learning algorithm to reconstruct the pulse length and spectral width from the autocorrelation pattern.

OPTICS LETTERS (2022)

Article Chemistry, Physical

Dynamics retrieval from stochastically weighted incomplete data by low-pass spectral analysis

Cecilia M. Casadei, Ahmad Hosseinizadeh, Gebhard F. X. Schertler, Abbas Ourmazd, Robin Santra

Summary: Time-resolved serial femtosecond crystallography (TR-SFX) allows for the study of protein dynamics with atomic resolution on sub-picosecond timescales. In this work, the authors propose a novel approach called low-pass spectral analysis (LPSA) to improve the analysis of TR-SFX data. LPSA projects the data onto a subspace defined by trigonometric functions, attenuating high-frequency features and facilitating the retrieval of underlying dynamics. The authors demonstrate the effectiveness of LPSA in reconstructing dynamics and compare it to other existing data analysis techniques.

STRUCTURAL DYNAMICS-US (2022)

Article Chemistry, Physical

Chemical effects on the dynamics of organic molecules irradiated with high intensity x rays

Sourav Banerjee, Zoltan Jurek, Malik Muhammad Abdullah, Robin Santra

Summary: This study aims to extend the XMDYN toolkit to treat chemical bonds and investigate the impact of charge rearrangement on the time evolution by simulating the interaction of a highly intense x-ray pulse with an amino acid. The discussion also addresses the capability of the classical MD based approach, XMDYN, to capture the charge-rearrangement-enhanced x-ray ionization of molecules effect.

STRUCTURAL DYNAMICS-US (2022)

Article Chemistry, Physical

Low-pass spectral analysis of time-resolved serial femtosecond crystallography data

Cecilia M. Casadei, Ahmad Hosseinizadeh, Spencer Bliven, Tobias Weinert, Jorg Standfuss, Russell Fung, Gebhard F. X. Schertler, Robin Santra

Summary: Low-pass spectral analysis (LPSA) is an effective algorithm for retrieving dynamics in model data affected by incompleteness and weighting errors. In this study, LPSA is applied to experimental time-resolved crystallography data and the parametric sensitivity is analyzed. The presence of high-frequency contamination in dynamical modes is investigated using synthetic data with various uncertainties and errors. A method is proposed to handle missing observations and improved dynamics retrieval is achieved.

STRUCTURAL DYNAMICS-US (2023)

Article Multidisciplinary Sciences

Femtosecond proton transfer in urea solutions probed by X-ray spectroscopy

Zhong Yin, Yi-Ping Chang, Tadas Balciunas, Yashoj Shakya, Aleksa Djorovic, Geoffrey Gaulier, Giuseppe Fazio, Robin Santra, Ludger Inhester, Jean-Pierre Wolf, Hans Jakob Worner

Summary: Researchers have revealed the femtosecond proton-transfer dynamics in ionized urea dimers in aqueous solution using table-top water-window X-ray absorption spectroscopy. By combining quantum-mechanical and molecular-mechanics calculations, they were able to identify the subsequent rearrangement of the urea dimer and the associated change of the electronic structure with site selectivity. These findings highlight the potential of table-top X-ray absorption spectroscopy in elucidating ultrafast dynamics in biomolecular systems.

NATURE (2023)

Article Multidisciplinary Sciences

Water layer and radiation damage effects on the orientation recovery of proteins in single-particle imaging at an X-ray free-electron laser

E. Juncheng, Michal Stransky, Zhou Shen, Zoltan Jurek, Carsten Fortmann-Grote, Richard Bean, Robin Santra, Beata Ziaja, Adrian P. Mancuso

Summary: This study investigates the impact of water layer thickness and radiation damage on orientation recovery from diffraction patterns of the nitrogenase iron protein. The results show that while a water layer mitigates protein damage, the noise generated by the scattering from it can introduce challenges for orientation recovery and is anticipated to cause problems in the phase retrieval process.

SCIENTIFIC REPORTS (2023)

Article Optics

Capturing electronic decoherence in quantum-classical dynamics using the ring-polymer-surface-hopping-density-matrix approach

Yashoj Shakya, Ralph Welsch, Ludger Inhester, Robin Santra

Summary: Simulations of coupled electronic and nuclear dynamics in molecules are computationally challenging and limited to model systems or small molecules. The approach presented in this study combines Tully's fewest switches surface hopping (FSSH) with ring-polymer molecular dynamics (RPMD) to overcome the limitations of FSSH in describing electronic coherences and decoherence phenomena. By incorporating decoherence effects through an electronic density-matrix formulation, this method captures a crucial decoherence mechanism missing in FSSH and provides a superior description of electronic coherences compared to earlier attempts at combining RPMD and FSSH.

PHYSICAL REVIEW A (2023)

Article Physics, Multidisciplinary

Theory of high-energy correlated multiphoton x-ray diffraction for synchrotron-radiation sources

Arunangshu Debnath, Robin Santra

Summary: We present a theoretical formulation for interpreting high-energy x-ray diffraction measurements using synchrotron radiation sources. The formulation allows classification of physical resources contributing to the correlation signatures and provides a unique perspective for structural imaging studies. It also offers a framework necessary for theoretical developments of associated reconstruction algorithms.

PHYSICAL REVIEW RESEARCH (2023)

Article Optics

State-resolved ionization dynamics of a neon atom induced by x-ray free-electron-laser pulses

Laura Budewig, Sang-Kil Son, Robin Santra

Summary: We propose a theoretical framework to study the state-resolved ionization dynamics of neon atoms driven by ultraintense x-ray free-electron-laser pulses. By combining a state-resolved electronic-structure calculation with a Monte Carlo rate-equation method, we are able to investigate the dynamics based on time-dependent state populations. Our results show that both configuration-based and state-resolved calculations yield similar charge-state distributions, except when resonant excitations are involved. Furthermore, we analyze time-resolved spectra of ions, electrons, and photons to explore frustrated absorption during the ionization dynamics of neon atoms.

PHYSICAL REVIEW A (2023)

Article Physics, Multidisciplinary

Machine-learning calibration of intense x-ray free-electron-laser pulses using Bayesian optimization

Niels Breckwoldt, Sang-Kil Son, Tommaso Mazza, Aljoscha Roerig, Rebecca Boll, Michael Meyer, Aaron C. LaForge, Debadarshini Mishra, Nora Berrah, Robin Santra

Summary: X-ray free-electron lasers (XFELs) bring new possibilities for probing and manipulating atomic and molecular dynamics with unprecedented resolution. However, accurately comparing experimental results with theoretical simulations requires precise characterization of the spatial and temporal profile of the X-ray pulses. In this study, we propose a calibration scheme based on Bayesian optimization to accurately determine the pulse duration and spatial fluence distribution profile of intense XFEL pulses. This method can serve as a comprehensive tool for characterizing ultraintense and ultrafast X-ray pulses.

PHYSICAL REVIEW RESEARCH (2023)

Article Optics

Laser-pulse characterization using strong-field autocorrelation patterns and random-forest-based machine learning

Daria Kolbasova, Robin Santra

Summary: Building on a previous strategy, this study presents an efficient alternative approach for characterizing ultrashort low-frequency laser pulses in situ. By using quantum-mechanical calculations, the researchers simulate the ionization of rare-gas atoms in strong fields and generate autocorrelation patterns for femtosecond laser pulses. They investigate the nonperturbative and nonlinear dependence of these patterns on pulse characteristics and propose an analytical function to describe them. The function's parameters and supervised machine learning are then utilized to retrieve key pulse parameters from the autocorrelation patterns produced via strong-field ionization. This approach offers advantages for experimental data applications.

PHYSICAL REVIEW A (2023)

Article Optics

Nonsequential two-photon absorption in solid Ge irradiated by an intense x-ray free-electron-laser pulse

Stanislaw Wirok-Stoletow, Rui Jin, Daria Kolbasova, Sang-Kil Son, Andrew Aquila, Robin Santra

Summary: We theoretically investigate the formation of highly charged ions in a germanium solid driven by intense X-ray pulses and its effect on the cross sections for nonsequential two-photon absorption. Our study finds that the formation of charged ions in germanium is quick under the given experimental conditions, but the cross sections for nonsequential two-photon absorption are insensitive to different charge states.

PHYSICAL REVIEW A (2022)

Article Physics, Fluids & Plasmas

Plasma environmental effects in the atomic structure for simulating x-ray free-electron-laser-heated solid-density matter

Rui Jin, Zoltan Jurek, Robin Santra, Sang-Kil Son

Summary: This study incorporates a recently proposed treatment of transient ionization potential depression (IPD) into plasma dynamics simulations, and demonstrates the importance of the IPD effects in theoretical modeling of dense plasmas by comparing two simulations.

PHYSICAL REVIEW E (2022)

Article Chemistry, Physical

Ultrafast proton transfer of the aqueous phenol radical cation

Muhammad Shafiq Bin Mohd Yusof, Hongwei Song, Tushar Debnath, Bethany Lowe, Minghui Yang, Zhi-Heng Loh

Summary: Proton transfer reactions play a crucial role in chemical and biological processes. This study investigates the ultrafast proton transfer dynamics of the aqueous phenol radical cation using femtosecond spectroscopy and quantum dynamics calculations. The results suggest that proton transfer occurs on a very fast timescale of about 0.1 ps. These findings contribute to a better understanding of the ultrafast proton transfer triggered by photoionization.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2022)

暂无数据