The development of Laue techniques for single-pulse diffraction of chemical complexes: Time-resolved Laue diffraction on a binuclear rhodium metal-organic complex

Anna Makal; Elzbieta Trzop; Jesse Sokolow; Jaroslaw Kalinowski; Jason Benedict; Philip Coppens

doi:10.1107/S0108767311011883

The development of Laue techniques for single-pulse diffraction of chemical complexes: Time-resolved Laue diffraction on a binuclear rhodium metal-organic complex

Anna Makal
, Elzbieta Trzop
, Jesse Sokolow
, Jaroslaw Kalinowski
, Jason Benedict
, Philip Coppens

Chemistry

SUNY Buffalo

Research output: Contribution to journal › Article › peer-review

41 Scopus citations

Abstract

A modified Laue method is shown to produce excited-state structures at atomic resolution of a quality competitive with those from monochromatic experiments. The much faster data collection allows the use of only one or a few X-ray pulses per data frame, which minimizes crystal damage caused by laser exposure of the samples and optimizes the attainable time resolution. The method has been applied to crystals of the α-modification of Rh ₂(μ-PNP)₂(PNP)₂ (BPh₄) ₂ [PNP = CH₃N(P(OCH₃)₂)₂, Ph = phenyl]. The experimental results show a shortening of the Rh - Rh distance in the organometallic complex of 0.136 (8) Å on excitation and are quantitatively supported by quantum-mechanical (QM)/molecular-mechanics (MM) theoretical calculations which take into account the confining effect of the crystal environment, but not by theoretical results on the isolated complex, demonstrating the defining effect of the crystal matrix.

Original language	English
Pages (from-to)	319-326
Number of pages	8
Journal	Acta Crystallographica Section A: Foundations of Crystallography
Volume	67
Issue number	4
DOIs	https://doi.org/10.1107/S0108767311011883
State	Published - Jul 2011

Keywords

Laue techniques
QM/MM calculations
quantum-mechanical/molecular- mechanics calculations
single-pulse diffraction
time-resolved X-ray crystallography

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10.1107/S0108767311011883

Cite this

Makal, A., Trzop, E., Sokolow, J., Kalinowski, J., Benedict, J., & Coppens, P. (2011). The development of Laue techniques for single-pulse diffraction of chemical complexes: Time-resolved Laue diffraction on a binuclear rhodium metal-organic complex. Acta Crystallographica Section A: Foundations of Crystallography, 67(4), 319-326. https://doi.org/10.1107/S0108767311011883

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title = "The development of Laue techniques for single-pulse diffraction of chemical complexes: Time-resolved Laue diffraction on a binuclear rhodium metal-organic complex",

abstract = "A modified Laue method is shown to produce excited-state structures at atomic resolution of a quality competitive with those from monochromatic experiments. The much faster data collection allows the use of only one or a few X-ray pulses per data frame, which minimizes crystal damage caused by laser exposure of the samples and optimizes the attainable time resolution. The method has been applied to crystals of the α-modification of Rh 2(μ-PNP)2(PNP)2 (BPh4) 2 [PNP = CH3N(P(OCH3)2)2, Ph = phenyl]. The experimental results show a shortening of the Rh - Rh distance in the organometallic complex of 0.136 (8) {\AA} on excitation and are quantitatively supported by quantum-mechanical (QM)/molecular-mechanics (MM) theoretical calculations which take into account the confining effect of the crystal environment, but not by theoretical results on the isolated complex, demonstrating the defining effect of the crystal matrix.",

keywords = "Laue techniques, QM/MM calculations, quantum-mechanical/molecular- mechanics calculations, single-pulse diffraction, time-resolved X-ray crystallography",

author = "Anna Makal and Elzbieta Trzop and Jesse Sokolow and Jaroslaw Kalinowski and Jason Benedict and Philip Coppens",

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Makal, A, Trzop, E, Sokolow, J, Kalinowski, J, Benedict, J & Coppens, P 2011, 'The development of Laue techniques for single-pulse diffraction of chemical complexes: Time-resolved Laue diffraction on a binuclear rhodium metal-organic complex', Acta Crystallographica Section A: Foundations of Crystallography, vol. 67, no. 4, pp. 319-326. https://doi.org/10.1107/S0108767311011883

The development of Laue techniques for single-pulse diffraction of chemical complexes: Time-resolved Laue diffraction on a binuclear rhodium metal-organic complex. / Makal, Anna; Trzop, Elzbieta; Sokolow, Jesse et al.
In: Acta Crystallographica Section A: Foundations of Crystallography, Vol. 67, No. 4, 07.2011, p. 319-326.

Research output: Contribution to journal › Article › peer-review

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T1 - The development of Laue techniques for single-pulse diffraction of chemical complexes

T2 - Time-resolved Laue diffraction on a binuclear rhodium metal-organic complex

AU - Makal, Anna

AU - Trzop, Elzbieta

AU - Sokolow, Jesse

AU - Kalinowski, Jaroslaw

AU - Benedict, Jason

AU - Coppens, Philip

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N2 - A modified Laue method is shown to produce excited-state structures at atomic resolution of a quality competitive with those from monochromatic experiments. The much faster data collection allows the use of only one or a few X-ray pulses per data frame, which minimizes crystal damage caused by laser exposure of the samples and optimizes the attainable time resolution. The method has been applied to crystals of the α-modification of Rh 2(μ-PNP)2(PNP)2 (BPh4) 2 [PNP = CH3N(P(OCH3)2)2, Ph = phenyl]. The experimental results show a shortening of the Rh - Rh distance in the organometallic complex of 0.136 (8) Å on excitation and are quantitatively supported by quantum-mechanical (QM)/molecular-mechanics (MM) theoretical calculations which take into account the confining effect of the crystal environment, but not by theoretical results on the isolated complex, demonstrating the defining effect of the crystal matrix.

AB - A modified Laue method is shown to produce excited-state structures at atomic resolution of a quality competitive with those from monochromatic experiments. The much faster data collection allows the use of only one or a few X-ray pulses per data frame, which minimizes crystal damage caused by laser exposure of the samples and optimizes the attainable time resolution. The method has been applied to crystals of the α-modification of Rh 2(μ-PNP)2(PNP)2 (BPh4) 2 [PNP = CH3N(P(OCH3)2)2, Ph = phenyl]. The experimental results show a shortening of the Rh - Rh distance in the organometallic complex of 0.136 (8) Å on excitation and are quantitatively supported by quantum-mechanical (QM)/molecular-mechanics (MM) theoretical calculations which take into account the confining effect of the crystal environment, but not by theoretical results on the isolated complex, demonstrating the defining effect of the crystal matrix.

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KW - QM/MM calculations

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The development of Laue techniques for single-pulse diffraction of chemical complexes: Time-resolved Laue diffraction on a binuclear rhodium metal-organic complex

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