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

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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

Funding

P.M. and R.v.G. were supported by the European Research Council (ERC) through an Advanced Investigator Grant (no. 267333, PHOTPROT) to R.v.G and by the Canadian Institute for Advanced Research (CIFAR). R.v.G. was further supported by the EU FP7 project PAPETS (GA 323901). J.R. was supported by the BioSolar Cells Programme of the Netherlands ministry of Economic Affairs, Agriculture and Innovation. J.T.M.K. was supported by the Netherlands Organization of Scientific Research (NWO) through a VICI grant and a Middelgroot investment grant of the NWO Chemical Sciences council (NWO-CW). R.C. was supported by the ERC through a Consolidator Grant (no. 281341, ASAP) and by NWO through a VICI grant. P. M. and T.M. were supported by the Czech Science Foundation GAÈR (grant no. 14-25752S). B.v.O. was supported by NWO through a VENI grant to B.v.O and a VICI grant to R.C.

FundersFunder number
NWO Chemical Sciences council
Netherlands ministry of Economic Affairs, Agriculture and Innovation
Canadian Institute for Advanced Research
Seventh Framework Programme267333, 323901, 281341
European Research Council
Grantová Agentura České Republiky14-25752S
Nederlandse Organisatie voor Wetenschappelijk Onderzoek

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