Laser induced temperature-jump time resolved IR spectroscopy of zeolites

Hawkins, Alexander P.; Edmeades, Amy E.; Hutchison, Christopher D. M.; Towrie, Michael; Howe, Russell F.; Greetham, Gregory M.; Donaldson, Paul M.

doi:10.1039/d3sc06128k

Chem. Sci.

2024

DOI: 10.1039/d3sc06128k

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Laser induced temperature-jump time resolved IR spectroscopy of zeolites

Alexander P. Hawkins,

Amy E. Edmeades,

Christopher D. M. Hutchison

et al.

Abstract: Laser heating of zeolites in combination with time-resolved IR spectroscopy is introduced as a means of studying chemical processes in heterogeneous catalysts from nanoseconds to seconds.

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Cited by 3 publications

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New approaches to vibrational spectroscopy of zeolite catalysts: a perspective

Howe

2024

Front. Chem. Sci. Eng.

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New approaches to vibrational spectroscopy of zeolite catalysts: a perspective

Howe

2024

Front. Chem. Sci. Eng.

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Mitigation of thermal artifacts in 100 kHz ultrafast 2D IR spectroscopy

Esterly,

Shivani,

Farrell

et al. 2024

The Journal of Chemical Physics

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Ytterbium lasers make possible shot-to-shot data collection of two-dimensional infrared (2D IR) spectra at 100 kHz and higher repetition rates. At those rates, the power absorbed by the sample is appreciable and creates a steady state temperature rise and an accumulated thermal grating artifact in the spectra that can obscure weak or low concentration IR chromophores. We report the magnitude of the temperature rise, the pulse ordering by which it is created, and ways to mitigate it. Using a calibrant molecule, we measured a steady-state temperature up to 32.5 and 45 °C for laser light at 4 µm in H2O and 6 µm in D2O, respectively, for a typical optical density used in 2D IR experiments. The temperature reached a steady state in ∼60 s. The temperature rise scales with the integrated optical density of the sample across the laser spectrum. By cooling the sample cell, we returned the steady state temperature to room temperature within the laser focus. For samples that undergo rotation, the accumulated thermal grating artifact is removed using a perpendicular ⟨XXYY⟩ polarization because the permuted time-orderings of the thermal grating artifact has the orientational response ⟨XYXY⟩, which decays to zero during the delay between consecutive laser pulses. The procedure described in this study can be used to characterize and minimize the thermal effects in experiments where repetition rate and/or pulse energy cause an appreciable temperature rise.

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Ultrafast Spectroscopy at the Central Laser Facility

Donaldson,

Sazanovich,

Malakar

et al. 2024

Johnson Matthey Technology Review

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In this article, we will examine ultrafast spectroscopy techniques and applications, covering time-resolved infrared (TR-IR) spectroscopy, time resolved visible (TA) spectroscopy, two-dimensional infrared (2D-IR) spectroscopy, Kerr-gated Raman spectroscopy, time-resolved Raman and surface sum-frequency generation (SSFG) spectroscopy. In addition to introducing each technique, we will cover some basics, such as what kinds of lasers are used and discuss how these techniques are applied to study a diversity of chemical problems such as photocatalysis, photochemistry, electrocatalysis, battery electrode characterisation, zeolite characterisation and protein structural dynamics.

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Laser induced temperature-jump time resolved IR spectroscopy of zeolites

Abstract: Laser heating of zeolites in combination with time-resolved IR spectroscopy is introduced as a means of studying chemical processes in heterogeneous catalysts from nanoseconds to seconds.

Cited by 3 publications

References 47 publications

New approaches to vibrational spectroscopy of zeolite catalysts: a perspective

New approaches to vibrational spectroscopy of zeolite catalysts: a perspective

Mitigation of thermal artifacts in 100 kHz ultrafast 2D IR spectroscopy

Ultrafast Spectroscopy at the Central Laser Facility

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