Abstract

Ultrafast transient absorption spectroscopy is a powerful tool to reveal excited state dynamics in various materials. Conventionally, probe pulses are generated via bulk supercontinuum generation or (noncollinear) optical parametric amplifiers whilst pump pulses are generated separately using (noncollinear) optical parametric amplifiers. These systems are limited by either their spectral density, stability, spectral range, and/or temporal compressibility. Recently, a new intense broadband light source is being developed, the multi-plate compression, which promises to overcome these limitations. In this paper, we analyze the supercontinuum generated by a single Multiple Plate Compression system to set a benchmark for its use in the field of ultrafast pump-probe spectroscopy. We have compressed the supercontinuum to 3.3 fs using chirp mirrors alone, making it an excellent candidate for pump-probe experiments requiring high temporal resolution. Furthermore, the single light source can be used to generate both probe and pump pulses due to its high spectral density (>14.5 nJ/nm) between 490 and 890 nm. The intensity has an average shot-to-shot relative standard deviation of 4.6 % over 490 to 890 nm, calculated over 2,000 sequential shots. By using only 1,000 shot pairs, a Delta T/T noise level of 2.6times 10^{-4} RMS is achieved. Finally, as a proof of concept, the transient absorption spectrum of a methylammonium lead iodide perovskite film is taken, showing great signal to noise with only 1,000 shot pairs. These results show great potential for the employment of this technique in other spectroscopic techniques such as coherent multidimensional spectroscopy.

Highlights

  • Ultrafast transient absorption spectroscopy is a powerful tool to reveal excited state dynamics in various materials

  • The first option is a compressed broadband pump to obtain high temporal resolution, whilst the second option is a wavelength tuneable narrowband excitation to resonate with specific electronic transitions

  • We will demonstrate the feasibility of using a novel single light source, the Multiple Plate Compression (MPC), in the field of ultrafast pump-probe spectroscopy

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Summary

Introduction

Ultrafast transient absorption spectroscopy is a powerful tool to reveal excited state dynamics in various materials. Transient Absorption Spectroscopy (TAS) is an often used and powerful tool to examine excited state dynamics in materials such as charge ­transfer[1], charge and exciton ­diffusion[2,3] and hot carrier ­cooling[4,5] This spectroscopic technique utilizes a probe and a pump pulse, overlapping at the sample position. We will demonstrate the feasibility of using a novel single light source, the Multiple Plate Compression (MPC), in the field of ultrafast pump-probe spectroscopy This MPC system, where pulses are focused onto a series of thin plates, makes use of the high nonlinear coefficient of solid-state materials while avoiding destructive mechanisms. The high photon count allows for both the pump and probe to be generated by a single MPC setup, vastly reducing the experimental complexity of the TAS system

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