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<p>In this work, we present an Optical-Pump Terahertz-Probe spectrometer specially tailored to address the ultrafast solvation dynamics in the librational band of liquid water (~ 9 to 27 THz) upon optical excitation of a solute. This spectrometer utilizes an optical pump at 400&#xa0;nm, generated by Second-Harmonic Generation of the fundamental 800&#xa0;nm wavelength. The probe pulse is generated by an Optical Parametric Amplifier followed by a Non-collinear Difference Frequency Generator enabling tunability from 21 to 86 THz (700–2869&#xa0;cm⁻<sup>1</sup>). In a given configuration, the system provides an instantaneous probe bandwidth of ~ 5 THz. The signal is detected by means of a Mercury Cadmium Telluride detector. To avoid any spurious signals from transmission cell windows, the pump and probe beams are collinearly overlapped in a free-flowing liquid flat-jet with an adjustable thickness of ~ 10–30&#xa0;µm. The experimental temporal resolution of the setup was determined to be ~ 350&#xa0;fs, and the wavelength was calibrated using a home-built Michelson interferometer. As a first demonstration, we use this setup to study spectroscopic changes in the librational band of water upon photoexcitation of the prototypical photoacid 8-hydroxy-1,3,6-pyrenetrisulfonate (HPTS) in aqueous solution.</p>

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Probing Dynamics in the Frequency Range of the Librational Band of Water by Optical-Pump Terahertz-Probe Spectroscopy

  • 期刊论文

  • 发表日期：

    2026年3月30日

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  • Meera Ramachandran,
  • Claudius Hoberg,
  • Fabio Novelli,
  • Martina Havenith

摘要

In this work, we present an Optical-Pump Terahertz-Probe spectrometer specially tailored to address the ultrafast solvation dynamics in the librational band of liquid water (~ 9 to 27 THz) upon optical excitation of a solute. This spectrometer utilizes an optical pump at 400 nm, generated by Second-Harmonic Generation of the fundamental 800 nm wavelength. The probe pulse is generated by an Optical Parametric Amplifier followed by a Non-collinear Difference Frequency Generator enabling tunability from 21 to 86 THz (700–2869 cm⁻1). In a given configuration, the system provides an instantaneous probe bandwidth of ~ 5 THz. The signal is detected by means of a Mercury Cadmium Telluride detector. To avoid any spurious signals from transmission cell windows, the pump and probe beams are collinearly overlapped in a free-flowing liquid flat-jet with an adjustable thickness of ~ 10–30 µm. The experimental temporal resolution of the setup was determined to be ~ 350 fs, and the wavelength was calibrated using a home-built Michelson interferometer. As a first demonstration, we use this setup to study spectroscopic changes in the librational band of water upon photoexcitation of the prototypical photoacid 8-hydroxy-1,3,6-pyrenetrisulfonate (HPTS) in aqueous solution.