Fluorescence-detected pump-probe spectroscopy

Transient absorption (TA) spectroscopy is a powerful tool for studying ultrafast electronic dynamics. However, it has limitations due to artefacts during pulse overlap. They hinder the interpretation of the signal at very early delay times. Additionally, non-transmissive or highly scattering samples are difficult to handle in standard TA. We overcome these limitations by changing from transmission to fluorescence as the primary spectroscopic signal. This leads to fluorescence-detected pump–probe (F-PP) spectroscopy. F-PP provides background-free detection and eliminates artefacts. The duration of the laser pulses defines the time resolution of F-PP. We adapt this method to study energy transfer dynamics in molecules and mono- or few-layered low-dimensional materials.

Involved group members

Hongxing Hao

hongxing.hao@tum.de

Yang Cui

yang.cui@tum.de

Erling Thyrhaug
erling.thyrhaug@tum.de


Further reading

Tekavec, P. F.; Lott, G. A.; Marcus, A. H. Fluorescence-detected two-dimensional electronic coherence spectroscopy by acousto-optic phase modulation. The Journal of Chemical Physics 2007, 127 (21), 214307. DOI: 10.1063/1.2800560.

Bakulin, A. A.; Silva, C.; Vella, E. Ultrafast Spectroscopy with Photocurrent Detection: Watching Excitonic Optoelectronic Systems at Work. The Journal of Physical Chemistry Letters 2016, 7 (2), 250-258. DOI: 10.1021/acs.jpclett.5b01955.