Sub-10 fs Time-Resolved Vibronic Optical Microscopy

Christoph Schnedermann, Jong Min Lim, Torsten Wende, Alex S. Duarte, Limeng Ni, Qifei Gu, Aditya Sadhanala, Akshay Rao, Philipp Kukura

Research output: Contribution to journalArticlepeer-review

45 Scopus citations

Abstract

We introduce femtosecond wide-field transient absorption microscopy combining sub-10 fs pump and probe pulses covering the complete visible (500-650 nm) and near-infrared (650-950 nm) spectrum with diffraction-limited optical resolution. We demonstrate the capabilities of our system by reporting the spatially- and spectrally-resolved transient electronic response of MAPbI3-xClx perovskite films and reveal significant quenching of the transient bleach signal at grain boundaries. The unprecedented temporal resolution enables us to directly observe the formation of band-gap renormalization, completed in 25 fs after photoexcitation. In addition, we acquire hyperspectral Raman maps of TIPS pentacene films with sub-400 nm spatial and sub-15 cm-1 spectral resolution covering the 100-2000 cm-1 window. Our approach opens up the possibility of studying ultrafast dynamics on nanometer length and femtosecond time scales in a variety of two-dimensional and nanoscopic systems.

Original languageEnglish
Pages (from-to)4854-4859
Number of pages6
JournalJournal of Physical Chemistry Letters
Volume7
Issue number23
DOIs
StatePublished - 1 Dec 2016

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