Polarization-controlled optimal scatter suppression in transient absorption spectroscopy

P. Malý, J. Ravensbergen, J.T.M. Kennis, R. van Grondelle, Roberta Croce, T Mančal, Bart van Oort

Research output: Contribution to JournalArticleAcademicpeer-review

Abstract

Ultrafast transient absorption spectroscopy is a powerful technique to study fast photo-induced processes, such as electron, proton and energy transfer, isomerization and molecular dynamics, in a diverse range of samples, including solid state materials and proteins. Many such experiments suffer from signal distortion by scattered excitation light, in particular close to the excitation (pump) frequency. Scattered light can be effectively suppressed by a polarizer oriented perpendicular to the excitation polarization and positioned behind the sample in the optical path of the probe beam. However, this introduces anisotropic polarization contributions into the recorded signal. We present an approach based on setting specific polarizations of the pump and probe pulses, combined with a polarizer behind the sample. Together, this controls the signal-to-scatter ratio (SSR), while maintaining isotropic signal. We present SSR for the full range of polarizations and analytically derive the optimal configuration at angles of 40.5° between probe and pump and of 66.9° between polarizer and pump polarizations. This improves SSR by 33 52 ≈. (or 3 compared to polarizer parallel to probe). The calculations are validated by transient absorption experiments on the common fluorescent dye Rhodamine B. This approach provides a simple method to considerably improve the SSR in transient absorption spectroscopy.
Original languageEnglish
Article number10.1038/srep43484
Pages (from-to)43484
Number of pages7
JournalScientific Reports
Volume7
DOIs
Publication statusPublished - 6 Mar 2017

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absorption spectroscopy
retarding
polarizers
polarization
pumps
probes
excitation
signal distortion
rhodamine
optical paths
isomerization
electron transfer
dyes
energy transfer
molecular dynamics
solid state
proteins
protons
configurations
pulses

Cite this

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title = "Polarization-controlled optimal scatter suppression in transient absorption spectroscopy",
abstract = "Ultrafast transient absorption spectroscopy is a powerful technique to study fast photo-induced processes, such as electron, proton and energy transfer, isomerization and molecular dynamics, in a diverse range of samples, including solid state materials and proteins. Many such experiments suffer from signal distortion by scattered excitation light, in particular close to the excitation (pump) frequency. Scattered light can be effectively suppressed by a polarizer oriented perpendicular to the excitation polarization and positioned behind the sample in the optical path of the probe beam. However, this introduces anisotropic polarization contributions into the recorded signal. We present an approach based on setting specific polarizations of the pump and probe pulses, combined with a polarizer behind the sample. Together, this controls the signal-to-scatter ratio (SSR), while maintaining isotropic signal. We present SSR for the full range of polarizations and analytically derive the optimal configuration at angles of 40.5° between probe and pump and of 66.9° between polarizer and pump polarizations. This improves SSR by 33 52 ≈. (or 3 compared to polarizer parallel to probe). The calculations are validated by transient absorption experiments on the common fluorescent dye Rhodamine B. This approach provides a simple method to considerably improve the SSR in transient absorption spectroscopy.",
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Polarization-controlled optimal scatter suppression in transient absorption spectroscopy. / Malý, P.; Ravensbergen, J.; Kennis, J.T.M.; van Grondelle, R.; Croce, Roberta; Mančal, T; van Oort, Bart.

In: Scientific Reports, Vol. 7, 10.1038/srep43484, 06.03.2017, p. 43484.

Research output: Contribution to JournalArticleAcademicpeer-review

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AU - Malý, P.

AU - Ravensbergen, J.

AU - Kennis, J.T.M.

AU - van Grondelle, R.

AU - Croce, Roberta

AU - Mančal, T

AU - van Oort, Bart

PY - 2017/3/6

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AB - Ultrafast transient absorption spectroscopy is a powerful technique to study fast photo-induced processes, such as electron, proton and energy transfer, isomerization and molecular dynamics, in a diverse range of samples, including solid state materials and proteins. Many such experiments suffer from signal distortion by scattered excitation light, in particular close to the excitation (pump) frequency. Scattered light can be effectively suppressed by a polarizer oriented perpendicular to the excitation polarization and positioned behind the sample in the optical path of the probe beam. However, this introduces anisotropic polarization contributions into the recorded signal. We present an approach based on setting specific polarizations of the pump and probe pulses, combined with a polarizer behind the sample. Together, this controls the signal-to-scatter ratio (SSR), while maintaining isotropic signal. We present SSR for the full range of polarizations and analytically derive the optimal configuration at angles of 40.5° between probe and pump and of 66.9° between polarizer and pump polarizations. This improves SSR by 33 52 ≈. (or 3 compared to polarizer parallel to probe). The calculations are validated by transient absorption experiments on the common fluorescent dye Rhodamine B. This approach provides a simple method to considerably improve the SSR in transient absorption spectroscopy.

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