Linear and Non-Linear Population Retrieval with Femtosecond Optical Pumping of Molecular Crystals for the Generalised Uniaxial and Biaxial Systems

Femtosecond optical measurements of photoexcitable molecular crystals carry ultrafast dynamics information with structural sensitivity. The creation and detection of transient dynamics depend on the optical parameters, as well as the explicit molecular structure, crystal symmetry, crystal orientatio...

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Main Authors: Christopher D. M. Hutchison, Alisia Fadini, Jasper J. van Thor
Format: Article
Language:English
Published: MDPI AG 2022-04-01
Series:Applied Sciences
Subjects:
Online Access:https://www.mdpi.com/2076-3417/12/9/4309
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author Christopher D. M. Hutchison
Alisia Fadini
Jasper J. van Thor
author_facet Christopher D. M. Hutchison
Alisia Fadini
Jasper J. van Thor
author_sort Christopher D. M. Hutchison
collection DOAJ
description Femtosecond optical measurements of photoexcitable molecular crystals carry ultrafast dynamics information with structural sensitivity. The creation and detection of transient dynamics depend on the optical parameters, as well as the explicit molecular structure, crystal symmetry, crystal orientation, polarisation of the photoexciting beam, and interaction geometry. In order to retrieve the linear and non-linear population transfer in photoexcited crystals, excitation theory is combined here with the calculation of birefringence decomposition and is shown for both the generalised uniaxial and biaxial systems. A computational tool was constructed based on this treatment to allow modelling of electric field decomposition, dipole projections, and non-linear excitation population levels. This is available open source and with a GUI for ease of use. Such work has applications in two areas of ultrafast science: multidimensional optical crystallography and femtosecond time-resolved X-ray crystallography.
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spelling doaj.art-8cf88a2f77de42d1841a7bb376cc27a22023-11-23T07:47:13ZengMDPI AGApplied Sciences2076-34172022-04-01129430910.3390/app12094309Linear and Non-Linear Population Retrieval with Femtosecond Optical Pumping of Molecular Crystals for the Generalised Uniaxial and Biaxial SystemsChristopher D. M. Hutchison0Alisia Fadini1Jasper J. van Thor2Department of Life Sciences, Faculty of Natural Sciences, Imperial College London, London SW7 2AZ, UKDepartment of Life Sciences, Faculty of Natural Sciences, Imperial College London, London SW7 2AZ, UKDepartment of Life Sciences, Faculty of Natural Sciences, Imperial College London, London SW7 2AZ, UKFemtosecond optical measurements of photoexcitable molecular crystals carry ultrafast dynamics information with structural sensitivity. The creation and detection of transient dynamics depend on the optical parameters, as well as the explicit molecular structure, crystal symmetry, crystal orientation, polarisation of the photoexciting beam, and interaction geometry. In order to retrieve the linear and non-linear population transfer in photoexcited crystals, excitation theory is combined here with the calculation of birefringence decomposition and is shown for both the generalised uniaxial and biaxial systems. A computational tool was constructed based on this treatment to allow modelling of electric field decomposition, dipole projections, and non-linear excitation population levels. This is available open source and with a GUI for ease of use. Such work has applications in two areas of ultrafast science: multidimensional optical crystallography and femtosecond time-resolved X-ray crystallography.https://www.mdpi.com/2076-3417/12/9/4309SFXTR-SFXcrystallographyXFEL2DESbirefringence
spellingShingle Christopher D. M. Hutchison
Alisia Fadini
Jasper J. van Thor
Linear and Non-Linear Population Retrieval with Femtosecond Optical Pumping of Molecular Crystals for the Generalised Uniaxial and Biaxial Systems
Applied Sciences
SFX
TR-SFX
crystallography
XFEL
2DES
birefringence
title Linear and Non-Linear Population Retrieval with Femtosecond Optical Pumping of Molecular Crystals for the Generalised Uniaxial and Biaxial Systems
title_full Linear and Non-Linear Population Retrieval with Femtosecond Optical Pumping of Molecular Crystals for the Generalised Uniaxial and Biaxial Systems
title_fullStr Linear and Non-Linear Population Retrieval with Femtosecond Optical Pumping of Molecular Crystals for the Generalised Uniaxial and Biaxial Systems
title_full_unstemmed Linear and Non-Linear Population Retrieval with Femtosecond Optical Pumping of Molecular Crystals for the Generalised Uniaxial and Biaxial Systems
title_short Linear and Non-Linear Population Retrieval with Femtosecond Optical Pumping of Molecular Crystals for the Generalised Uniaxial and Biaxial Systems
title_sort linear and non linear population retrieval with femtosecond optical pumping of molecular crystals for the generalised uniaxial and biaxial systems
topic SFX
TR-SFX
crystallography
XFEL
2DES
birefringence
url https://www.mdpi.com/2076-3417/12/9/4309
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