title: Sub-10 fs Time-Resolved Vibronic Optical Microscopy.
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-xClxperovskite 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-1spectral resolution covering the 100-2000 cm-1window. 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.
authors.affiliation: Physical and Theoretical Chemistry Laboratory, University of Oxford , South Parks Road, Oxford OX1 3QZ, United Kingdom.
authors.forename: Christoph
authors.initials: C
authors.lastname: Schnedermann
authors.affiliation: Physical and Theoretical Chemistry Laboratory, University of Oxford , South Parks Road, Oxford OX1 3QZ, United Kingdom.
authors.forename: Jong Min
authors.initials: JM
authors.lastname: Lim
authors.affiliation: Physical and Theoretical Chemistry Laboratory, University of Oxford , South Parks Road, Oxford OX1 3QZ, United Kingdom.
authors.forename: Torsten
authors.initials: T
authors.lastname: Wende
authors.affiliation: Physical and Theoretical Chemistry Laboratory, University of Oxford , South Parks Road, Oxford OX1 3QZ, United Kingdom.
authors.forename: Alex S
authors.initials: AS
authors.lastname: Duarte
authors.affiliation: Cavendish Laboratory, University of Cambridge , JJ Thomson Avenue, Cambridge CB3 0HE, United Kingdom.
authors.forename: Limeng
authors.initials: L
authors.lastname: Ni
authors.affiliation: Cavendish Laboratory, University of Cambridge , JJ Thomson Avenue, Cambridge CB3 0HE, United Kingdom.
authors.forename: Qifei
authors.initials: Q
authors.lastname: Gu
authors.affiliation: Cavendish Laboratory, University of Cambridge , JJ Thomson Avenue, Cambridge CB3 0HE, United Kingdom.
authors.forename: Aditya
authors.initials: A
authors.lastname: Sadhanala
authors.affiliation: Cavendish Laboratory, University of Cambridge , JJ Thomson Avenue, Cambridge CB3 0HE, United Kingdom.
authors.forename: Akshay
authors.initials: A
authors.lastname: Rao
authors.affiliation: Physical and Theoretical Chemistry Laboratory, University of Oxford , South Parks Road, Oxford OX1 3QZ, United Kingdom.
authors.forename: Philipp
authors.initials: P
authors.lastname: Kukura