Coulomb-explosion imaging using a pixel-imaging mass-spectrometry camera

Slater, Craig S.; Blake, S.; Brouard, M.; Lauer, Alexandra; Vallance, Claire; Bohun, C. Sean; Christensen, Lars Rune; Nielsen, Jens Hedegaard; Johansson, Mikael P.; Stapelfeldt, Henrik

doi:10.1103/physreva.91.053424

Cited by 59 publications

(83 citation statements)

References 44 publications

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“…With the above in mind, timed Coulomb explosion imaging could be directly applied to more complex photochemistry, including the dissociation of large molecules, multichromophoric compounds, or isomerization reactions. By using covariance or coincidence conditions, ion correlations could potentially be extracted [45], and information about the structural dynamics and chirality of parent molecules could be established.…”

Section: Discussionmentioning

confidence: 99%

“…The latter allow imaging of single fragments, or small time windows of fragments, and consequently miss correlations between ions with different m/z. By contrast, the PImMS camera can be used for coincident and covariance imaging [45]. In the present experiment, the camera repetition rate was synchronized to the 10 Hz pump-probe laser system, and approximately 450 laser shots were taken per delay step.…”

Section: Methodsmentioning

confidence: 99%

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Coulomb-explosion imaging of concurrent CH2BrI photodissociation dynamics

Burt¹,

Boll²,

Lee³

et al. 2017

Phys. Rev. A

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The dynamics following laser-induced molecular photodissociation of gas-phase CH 2 BrI at 271.6 nm were investigated by time-resolved Coulomb explosion imaging using intense near-IR femtosecond laser pulses. The observed delay-dependent photofragment momenta reveal that CH 2 BrI undergoes C-I cleavage, depositing 65.6% of the available energy into internal product states, and that absorption of a second UV photon breaks the C-Br bond of CH 2 Br. Simulations confirm that this mechanism is consistent with previous data recorded at 248 nm, demonstrating the sensitivity of Coulomb explosion imaging as a real-time probe of chemical dynamics.2

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Section: Discussionmentioning

confidence: 99%

Section: Methodsmentioning

confidence: 99%

Coulomb-explosion imaging of concurrent CH2BrI photodissociation dynamics

Burt¹,

Boll²,

Lee³

et al. 2017

Phys. Rev. A

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“…, where and are number of ions measured at th laser shot. Covariance mapping has been successfully applied to treatment of few-atomic molecules [20,39,40,197,200], as well as large molecules [33,43,[203][204][205] and clusters [206][207][208][209].…”

Section: Covariance Mappingmentioning

confidence: 99%

“…As a result, the angular distributions of carbon and hydrogen ions closely coincide in the case of acetylene, while carbon ions are ejected perpendicularly with respect to the iodine ones. The trajectories of ions following Coulomb explosion can be simulated by numerically solving the classical equation of motion under the assumption that each fragment ion is treated as a point charge and the repulsive forces between fragment ions are all Coulombic [43].…”

Section: Introductionmentioning

confidence: 99%

Multiple ionization and Coulomb explosion of molecules, molecular complexes, clusters and solid surfaces

Yatsuhashi

Nakashima

2018

Journal of Photochemistry and Photobiology C: Photochemistry Re

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Intense femtosecond lasers as well as X-ray free electron lasers provide new means to produce multiply charged molecular cations. The fragmentation processes that these high energy species undergo, termed Coulomb explosion, are utilized to determine the static molecular structures as well as to trace the molecular dynamics of ultrafast chemical reactions. This review focuses on recent advances made in studies of Coulomb explosion imaging, highlighting the use of this process to determine the static structures of complex molecules, geometric isomers, chiral molecules and molecular complexes. Briefly, we summarize the recent time-resolved studies of surface electric fields and the controversy pertaining to the contribution of Coulomb explosion to the mechanism for ablation of solid surfaces.

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“…2, where each covariance image, cov(X + , Y + ), represents the recoil velocity distribution of a partner ion Y + with respect to the recoil direction of a reference ion X + . 27,28 To understand the potential for structural identification offered by the covariance images, assume that the only knowledge available from the mass spectra of the isomers is that they that F + ions are ejected at ∼±120 • with respect to I + . This implies that the molecule contains one or two F atoms in the 3 or 5 positions.…”

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confidence: 99%

Communication: Gas-phase structural isomer identification by Coulomb explosion of aligned molecules

Burt

Amini

Lee

et al. 2018

The Journal of Chemical Physics

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The gas-phase structures of four difluoroiodobenzene and two dihydroxybromobenzene isomers were identified by correlating the emission angles of atomic fragment ions created following femtosecond laser-induced Coulomb explosion. The structural determinations were facilitated by confining the most polarizable axis of each molecule to the detection plane prior to the Coulomb explosion event using one-dimensional laser-induced adiabatic alignment. For a molecular target consisting of two difluoroiodobenzene isomers, each constituent structure could additionally be singled out and distinguished. a) These authors contributed equally to this work. b) ElectronicLaser-induced molecular Coulomb explosion is the process whereby an intense femtosecond laser pulse detaches several electrons from a molecule, breaking it into cationic fragments. If the axial recoil approximation is satisfied, the created fragment ions recoil along the original bond axes of their parent molecule, allowing laser-induced Coulomb explosions to be used for two purposes: the first concerns how molecules are oriented in space at the instant the laser pulse arrives, and is measured by determining the emission directions of the fragment ions with respect to one or more fixed axes. This method has been used as a probe for a large number of laser-induced alignment and orientation experiments. 1-4 The second concerns molecular structures, which can be identified by correlating the measured fragment momenta. These latter experiments have revealed static molecular geometries and, with femtosecond pump-probe schemes, structural and reaction dynamics. [5][6][7][8][9][10][11][12][13][14][15][16][17][18][19] Coulomb explosion research on diatomic and triatomic molecules has demonstrated that covariance and coincidence analyses are efficient and powerful approaches for identifying the correlations between the emission directions of different fragment ions. 20-25 This is even more evident in studies of larger and more complex molecules, towards which interest has turned over the past decade. 10,16,26,27 Covariance analysis of Coulomb explosion fragments has also been applied to molecules that were pre-aligned by adiabatic laser pulses. [26][27][28] In these experiments, this alignment placed the molecules in well-defined spatial orientations with respect to the imaging detector, and thereby increased the structural information obtained from the recorded fragment momenta. The purpose of this work is to further develop Coulomb explosion imaging of pre-aligned targets as a method to determine the structures of polyatomic molecules. In particular, we demonstrate that four difluoroiodobenzene (DFIB) isomers can be unequivocally distinguished by analyzing the angular correlations of specific fragment ions. Furthermore, we show that for a mixture of two DFIB isomers the constituent structures can be singled out and identified. Finally, to demonstrate that our method is also capable of identifying isomers when only one substituent is a halogen atom, experiments were carr...

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Coulomb-explosion imaging using a pixel-imaging mass-spectrometry camera

Cited by 59 publications

References 44 publications

Coulomb-explosion imaging of concurrent CH2BrI photodissociation dynamics

Coulomb-explosion imaging of concurrent CH2BrI photodissociation dynamics

Multiple ionization and Coulomb explosion of molecules, molecular complexes, clusters and solid surfaces

Communication: Gas-phase structural isomer identification by Coulomb explosion of aligned molecules

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