Molecular structure retrieval directly from laboratory-frame photoelectron spectra in laser-induced electron diffraction

• URL: http://arxiv.org/abs/2107.00307v1
• Date: Thu, 1 Jul 2021 08:55:14 GMT
• Title: Molecular structure retrieval directly from laboratory-frame photoelectron spectra in laser-induced electron diffraction
• Authors: A. Sanchez, K. Amini, S.-J. Wang, T. Steinle, B. Belsa, J. Danek, A.T. Le, X. Liu, R. Moshammer, T. Pfeifer, M. Richter, J. Ullrich, S. Gr\"afe, C.D. Lin, J. Biegert
• Abstract summary: We introduce a simple molecular retrieval method based on the identification of critical points in the oscillating molecular interference scattering signal. We show that both methods correctly retrieve the asymmetrically stretched and bent field-dressed configuration of the asymmetric top molecule carbonyl sulfide.
• Score: 0.33256372159758324
• License: http://creativecommons.org/licenses/by/4.0/
• Abstract: Ubiquitous to most molecular scattering methods is the challenge to retrieve bond distance and angle from the scattering signals since this requires convergence of pattern matching algorithms or fitting methods. This problem is typically exacerbated when imaging larger molecules or for dynamic systems with little a priori knowledge. Here, we employ laser-induced electron diffraction (LIED) which is a powerful means to determine the precise atomic configuration of an isolated gas-phase molecule with picometre spatial and attosecond temporal precision. We introduce a simple molecular retrieval method, which is based only on the identification of critical points in the oscillating molecular interference scattering signal that is extracted directly from the laboratory-frame photoelectron spectrum. The method is compared with a Fourier-based retrieval method, and we show that both methods correctly retrieve the asymmetrically stretched and bent field-dressed configuration of the asymmetric top molecule carbonyl sulfide (OCS), which is confirmed by our quantum-classical calculations.

Related papers

• Time resolved quantum tomography in molecular spectroscopy by the Maximal Entropy Approach [1.7563879056963012]
  A fundamental question emerges: what role, if any, do quantum coherences between molecular electron states play in photochemical reactions? The Maximal Entropy (MaxEnt) based Quantum State Tomography (QST) approach offers unique advantages in studying molecular dynamics. We present two methodologies for constructing these operators: one leveraging Molecular Angular Distribution Moments (MADMs) which accurately capture the orientation-dependent vibronic dynamics of molecules. We achieve a groundbreaking milestone by constructing, for the first time, the entanglement entropy of the electronic subsystem: a metric that was previously inaccessible.
  arXiv  Detail & Related papers  (2024-07-23T16:43:01Z)
• Coherent multidimensional spectroscopy in polariton systems [0.0]
  Fast dynamics of molecular polaritonics is scrutinized theoretically through the implementation of two-dimensional spectroscopy protocols. We derive conceptually simple and computationally efficient formulas to calculate two-dimensional spectra for molecules. Our theoretical method provides a deeper insight in those processes that yield relevant signals in multidimensional molecular spectroscopy.
  arXiv  Detail & Related papers  (2024-03-07T18:37:52Z)
• Quantum control of ro-vibrational dynamics and application to light-induced molecular chirality [39.58317527488534]
  Achiral molecules can be made temporarily chiral by excitation with electric fields. We go beyond the assumption of molecular orientations to remain fixed during the excitation process.
  arXiv  Detail & Related papers  (2023-10-17T20:33:25Z)
• Photoemission Orbital Tomography Using Robust Sparse PhaseLift [2.624902795082451]
  Photoemission orbital tomography (POT) from photoelectron momentum maps (PMMs) has enabled detailed analysis of the shape and energy of molecular orbitals in the adsorbed state. This study proposes a new POT method based on the PhaseLift. Molecular orbitals, including three-dimensional phases, can be identified from a single PMM by actively providing atomic positions and basis.
  arXiv  Detail & Related papers  (2023-07-24T03:18:51Z)
• Bipolar single-molecule electroluminescence and electrofluorochromism [50.591267188664666]
  We investigate cationic and anionic fluorescence of individual zinc phthalocyanine (ZnPc) molecules adsorbed on ultrathin NaCl films on Ag (111) by using STML. They depend on the tip-sample bias polarity and appear at threshold voltages that are correlated with the onset energies of particular molecular orbitals.
  arXiv  Detail & Related papers  (2022-10-20T09:22:45Z)
• Predicting molecular vibronic spectra using time-domain analog quantum simulation [0.0]
  We introduce a method for scalable analog quantum simulation of molecular spectroscopy. Our approach can treat more complicated molecular models than previous ones, requires fewer approximations, and can be extended to open quantum systems. We experimentally demonstrate our algorithm on a trapped-ion device, exploiting both intrinsic electronic and motional degrees of freedom.
  arXiv  Detail & Related papers  (2022-09-14T11:32:55Z)
• Calculating non-linear response functions for multi-dimensional electronic spectroscopy using dyadic non-Markovian quantum state diffusion [68.8204255655161]
  We present a methodology for simulating multi-dimensional electronic spectra of molecular aggregates with coupling electronic excitation to a structured environment. A crucial aspect of our approach is that we propagate the NMQSD equation in a doubled system Hilbert space but with the same noise.
  arXiv  Detail & Related papers  (2022-07-06T15:30:38Z)
• Simulation of absorption spectra of molecular aggregates: a Hierarchy of Stochastic Pure States approach [68.8204255655161]
  hierarchy of pure states (HOPS) provides a formally exact solution based on local, trajectories. Exploiting the localization of HOPS for the simulation of absorption spectra in large aggregares requires a formulation in terms of normalized trajectories.
  arXiv  Detail & Related papers  (2021-11-01T16:59:54Z)
• Visualizing spinon Fermi surfaces with time-dependent spectroscopy [62.997667081978825]
  We propose applying time-dependent photo-emission spectroscopy, an established tool in solid state systems, in cold atom quantum simulators. We show in exact diagonalization simulations of the one-dimensional $t-J$ model that the spinons start to populate previously unoccupied states in an effective band structure. The dependence of the spectral function on the time after the pump pulse reveals collective interactions among spinons.
  arXiv  Detail & Related papers  (2021-05-27T18:00:02Z)
• Continuum-electron interferometry for enhancement of photoelectron circular dichroism and measurement of bound, free, and mixed contributions to chiral response [39.58317527488534]
  We develop photoelectron interferometry based on laser-assisted extreme ultraviolet ionization for flexible and robust control of photoelectron circular dichroism in randomly oriented chiral molecules. A comb of XUV photons ionizes a sample of chiral molecules in the presence of a time-delayed infrared or visible laser pulse promoting interferences between components of the XUV-ionized photoelectron wave packet.
  arXiv  Detail & Related papers  (2021-04-15T15:20:57Z)
• Nondestructive dispersive imaging of rotationally excited ultracold molecules [0.0]
  We present and theoretically analyze a general scheme for dispersive imaging of electronic ground-state molecules. Our technique relies on the intrinsic anisotropy of excited molecular rotational states to generate optical birefringence.
  arXiv  Detail & Related papers  (2020-06-05T14:36:10Z)

This list is automatically generated from the titles and abstracts of the papers in this site.

This site does not guarantee the quality of this site (including all information) and is not responsible for any consequences.