Mapping atomic motions with ultrabright electrons: Towards fundamental limits in space-time resolution

Stephanie Manz, Albert Casandruc, Dongfang Zhang, Yinpeng Zhong, Rolf A. Loch, Alexander Marx, Taisuke Hasegawa, Lai Chung Liu, Shima Bayesteh, Hossein Delsim-Hashemi, Matthias Hoffmann, Matthias Felber, Max Hachmann, Frank Mayet, Julian Hirscht, Sercan Keskin, Masaki Hada, Sascha W. Epp, Klaus Flöttmann, R. J Dwayne Miller

Research output: Contribution to journalReview article

48 Citations (Scopus)

Abstract

The long held objective of directly observing atomic motions during the defining moments of chemistry has been achieved based on ultrabright electron sources that have given rise to a new field of atomically resolved structural dynamics. This class of experiments requires not only simultaneous sub-atomic spatial resolution with temporal resolution on the 100 femtosecond time scale but also has brightness requirements approaching single shot atomic resolution conditions. The brightness condition is in recognition that chemistry leads generally to irreversible changes in structure during the experimental conditions and that the nanoscale thin samples needed for electron structural probes pose upper limits to the available sample or "film" for atomic movies. Even in the case of reversible systems, the degree of excitation and thermal effects require the brightest sources possible for a given space-time resolution to observe the structural changes above background. Further progress in the field, particularly to the study of biological systems and solution reaction chemistry, requires increased brightness and spatial coherence, as well as an ability to tune the electron scattering cross-section to meet sample constraints. The electron bunch density or intensity depends directly on the magnitude of the extraction field for photoemitted electron sources and electron energy distribution in the transverse and longitudinal planes of electron propagation. This work examines the fundamental limits to optimizing these parameters based on relativistic electron sources using re-bunching cavity concepts that are now capable of achieving 10 femtosecond time scale resolution to capture the fastest nuclear motions. This analysis is given for both diffraction and real space imaging of structural dynamics in which there are several orders of magnitude higher space-time resolution with diffraction methods. The first experimental results from the Relativistic Electron Gun for Atomic Exploration (REGAE) are given that show the significantly reduced multiple electron scattering problem in this regime, which opens up micron scale systems, notably solution phase chemistry, to atomically resolved structural dynamics. This journal is

Original languageEnglish
Pages (from-to)467-491
Number of pages25
JournalFaraday Discussions
Volume177
DOIs
Publication statusPublished - Apr 1 2015
Externally publishedYes

Fingerprint

Electron sources
dynamic structural analysis
electron sources
Structural dynamics
Electrons
chemistry
Luminance
brightness
Electron scattering
electron scattering
electrons
Diffraction
electron flux density
Electron guns
Multiple scattering
bunching
electron guns
Biological systems
temporal resolution
diffraction

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Medicine(all)

Cite this

Manz, S., Casandruc, A., Zhang, D., Zhong, Y., Loch, R. A., Marx, A., ... Miller, R. J. D. (2015). Mapping atomic motions with ultrabright electrons: Towards fundamental limits in space-time resolution. Faraday Discussions, 177, 467-491. https://doi.org/10.1039/c4fd00204k

Mapping atomic motions with ultrabright electrons : Towards fundamental limits in space-time resolution. / Manz, Stephanie; Casandruc, Albert; Zhang, Dongfang; Zhong, Yinpeng; Loch, Rolf A.; Marx, Alexander; Hasegawa, Taisuke; Liu, Lai Chung; Bayesteh, Shima; Delsim-Hashemi, Hossein; Hoffmann, Matthias; Felber, Matthias; Hachmann, Max; Mayet, Frank; Hirscht, Julian; Keskin, Sercan; Hada, Masaki; Epp, Sascha W.; Flöttmann, Klaus; Miller, R. J Dwayne.

In: Faraday Discussions, Vol. 177, 01.04.2015, p. 467-491.

Research output: Contribution to journalReview article

Manz, S, Casandruc, A, Zhang, D, Zhong, Y, Loch, RA, Marx, A, Hasegawa, T, Liu, LC, Bayesteh, S, Delsim-Hashemi, H, Hoffmann, M, Felber, M, Hachmann, M, Mayet, F, Hirscht, J, Keskin, S, Hada, M, Epp, SW, Flöttmann, K & Miller, RJD 2015, 'Mapping atomic motions with ultrabright electrons: Towards fundamental limits in space-time resolution', Faraday Discussions, vol. 177, pp. 467-491. https://doi.org/10.1039/c4fd00204k
Manz, Stephanie ; Casandruc, Albert ; Zhang, Dongfang ; Zhong, Yinpeng ; Loch, Rolf A. ; Marx, Alexander ; Hasegawa, Taisuke ; Liu, Lai Chung ; Bayesteh, Shima ; Delsim-Hashemi, Hossein ; Hoffmann, Matthias ; Felber, Matthias ; Hachmann, Max ; Mayet, Frank ; Hirscht, Julian ; Keskin, Sercan ; Hada, Masaki ; Epp, Sascha W. ; Flöttmann, Klaus ; Miller, R. J Dwayne. / Mapping atomic motions with ultrabright electrons : Towards fundamental limits in space-time resolution. In: Faraday Discussions. 2015 ; Vol. 177. pp. 467-491.
@article{f963dc40be364b778223fefaeb3347b8,
title = "Mapping atomic motions with ultrabright electrons: Towards fundamental limits in space-time resolution",
abstract = "The long held objective of directly observing atomic motions during the defining moments of chemistry has been achieved based on ultrabright electron sources that have given rise to a new field of atomically resolved structural dynamics. This class of experiments requires not only simultaneous sub-atomic spatial resolution with temporal resolution on the 100 femtosecond time scale but also has brightness requirements approaching single shot atomic resolution conditions. The brightness condition is in recognition that chemistry leads generally to irreversible changes in structure during the experimental conditions and that the nanoscale thin samples needed for electron structural probes pose upper limits to the available sample or {"}film{"} for atomic movies. Even in the case of reversible systems, the degree of excitation and thermal effects require the brightest sources possible for a given space-time resolution to observe the structural changes above background. Further progress in the field, particularly to the study of biological systems and solution reaction chemistry, requires increased brightness and spatial coherence, as well as an ability to tune the electron scattering cross-section to meet sample constraints. The electron bunch density or intensity depends directly on the magnitude of the extraction field for photoemitted electron sources and electron energy distribution in the transverse and longitudinal planes of electron propagation. This work examines the fundamental limits to optimizing these parameters based on relativistic electron sources using re-bunching cavity concepts that are now capable of achieving 10 femtosecond time scale resolution to capture the fastest nuclear motions. This analysis is given for both diffraction and real space imaging of structural dynamics in which there are several orders of magnitude higher space-time resolution with diffraction methods. The first experimental results from the Relativistic Electron Gun for Atomic Exploration (REGAE) are given that show the significantly reduced multiple electron scattering problem in this regime, which opens up micron scale systems, notably solution phase chemistry, to atomically resolved structural dynamics. This journal is",
author = "Stephanie Manz and Albert Casandruc and Dongfang Zhang and Yinpeng Zhong and Loch, {Rolf A.} and Alexander Marx and Taisuke Hasegawa and Liu, {Lai Chung} and Shima Bayesteh and Hossein Delsim-Hashemi and Matthias Hoffmann and Matthias Felber and Max Hachmann and Frank Mayet and Julian Hirscht and Sercan Keskin and Masaki Hada and Epp, {Sascha W.} and Klaus Fl{\"o}ttmann and Miller, {R. J Dwayne}",
year = "2015",
month = "4",
day = "1",
doi = "10.1039/c4fd00204k",
language = "English",
volume = "177",
pages = "467--491",
journal = "Faraday Discussions",
issn = "1359-6640",
publisher = "Royal Society of Chemistry",

}

TY - JOUR

T1 - Mapping atomic motions with ultrabright electrons

T2 - Towards fundamental limits in space-time resolution

AU - Manz, Stephanie

AU - Casandruc, Albert

AU - Zhang, Dongfang

AU - Zhong, Yinpeng

AU - Loch, Rolf A.

AU - Marx, Alexander

AU - Hasegawa, Taisuke

AU - Liu, Lai Chung

AU - Bayesteh, Shima

AU - Delsim-Hashemi, Hossein

AU - Hoffmann, Matthias

AU - Felber, Matthias

AU - Hachmann, Max

AU - Mayet, Frank

AU - Hirscht, Julian

AU - Keskin, Sercan

AU - Hada, Masaki

AU - Epp, Sascha W.

AU - Flöttmann, Klaus

AU - Miller, R. J Dwayne

PY - 2015/4/1

Y1 - 2015/4/1

N2 - The long held objective of directly observing atomic motions during the defining moments of chemistry has been achieved based on ultrabright electron sources that have given rise to a new field of atomically resolved structural dynamics. This class of experiments requires not only simultaneous sub-atomic spatial resolution with temporal resolution on the 100 femtosecond time scale but also has brightness requirements approaching single shot atomic resolution conditions. The brightness condition is in recognition that chemistry leads generally to irreversible changes in structure during the experimental conditions and that the nanoscale thin samples needed for electron structural probes pose upper limits to the available sample or "film" for atomic movies. Even in the case of reversible systems, the degree of excitation and thermal effects require the brightest sources possible for a given space-time resolution to observe the structural changes above background. Further progress in the field, particularly to the study of biological systems and solution reaction chemistry, requires increased brightness and spatial coherence, as well as an ability to tune the electron scattering cross-section to meet sample constraints. The electron bunch density or intensity depends directly on the magnitude of the extraction field for photoemitted electron sources and electron energy distribution in the transverse and longitudinal planes of electron propagation. This work examines the fundamental limits to optimizing these parameters based on relativistic electron sources using re-bunching cavity concepts that are now capable of achieving 10 femtosecond time scale resolution to capture the fastest nuclear motions. This analysis is given for both diffraction and real space imaging of structural dynamics in which there are several orders of magnitude higher space-time resolution with diffraction methods. The first experimental results from the Relativistic Electron Gun for Atomic Exploration (REGAE) are given that show the significantly reduced multiple electron scattering problem in this regime, which opens up micron scale systems, notably solution phase chemistry, to atomically resolved structural dynamics. This journal is

AB - The long held objective of directly observing atomic motions during the defining moments of chemistry has been achieved based on ultrabright electron sources that have given rise to a new field of atomically resolved structural dynamics. This class of experiments requires not only simultaneous sub-atomic spatial resolution with temporal resolution on the 100 femtosecond time scale but also has brightness requirements approaching single shot atomic resolution conditions. The brightness condition is in recognition that chemistry leads generally to irreversible changes in structure during the experimental conditions and that the nanoscale thin samples needed for electron structural probes pose upper limits to the available sample or "film" for atomic movies. Even in the case of reversible systems, the degree of excitation and thermal effects require the brightest sources possible for a given space-time resolution to observe the structural changes above background. Further progress in the field, particularly to the study of biological systems and solution reaction chemistry, requires increased brightness and spatial coherence, as well as an ability to tune the electron scattering cross-section to meet sample constraints. The electron bunch density or intensity depends directly on the magnitude of the extraction field for photoemitted electron sources and electron energy distribution in the transverse and longitudinal planes of electron propagation. This work examines the fundamental limits to optimizing these parameters based on relativistic electron sources using re-bunching cavity concepts that are now capable of achieving 10 femtosecond time scale resolution to capture the fastest nuclear motions. This analysis is given for both diffraction and real space imaging of structural dynamics in which there are several orders of magnitude higher space-time resolution with diffraction methods. The first experimental results from the Relativistic Electron Gun for Atomic Exploration (REGAE) are given that show the significantly reduced multiple electron scattering problem in this regime, which opens up micron scale systems, notably solution phase chemistry, to atomically resolved structural dynamics. This journal is

UR - http://www.scopus.com/inward/record.url?scp=84928136868&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=84928136868&partnerID=8YFLogxK

U2 - 10.1039/c4fd00204k

DO - 10.1039/c4fd00204k

M3 - Review article

C2 - 25631530

AN - SCOPUS:84928136868

VL - 177

SP - 467

EP - 491

JO - Faraday Discussions

JF - Faraday Discussions

SN - 1359-6640

ER -