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Effective Electron Temperature Measurement Using Time-Resolved Anti-Stokes Photoluminescence.

ABSTRACT: Anti-Stokes photoluminescence of metal nanoparticles, in which emitted photons have a higher energy than the incident photons, is an indicator of the temperature prevalent within a nanoparticle. Previous work has shown how to extract the temperature from a gold nanoparticle under continuous-wave monochromatic illumination. We extend the technique to pulsed illumination and introduce pump-probe anti-Stokes spectroscopy. This new technique enables us not only to measure an effective electron temperature in a gold nanoparticle (?103 K under our conditions), but also to measure ultrafast dynamics of a pulse-excited electron population, through its effect on the photoluminescence, with subpicosecond time resolution. We measure the heating and cooling, all within picoseconds, of the electrons and find that, with our subpicosecond pulses, the highest apparent temperature is reached 0.6 ps before the maximum change in magnitude of the extinction signal.

SUBMITTER: Jollans T

PROVIDER: S-EPMC7457233 | biostudies-literature | 2020 Aug

REPOSITORIES: biostudies-literature

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Effective Electron Temperature Measurement Using Time-Resolved Anti-Stokes Photoluminescence.

Jollans Thomas T Caldarola Martín M Sivan Yonatan Y Orrit Michel M

The journal of physical chemistry. A 20200814 34

Anti-Stokes photoluminescence of metal nanoparticles, in which emitted photons have a higher energy than the incident photons, is an indicator of the temperature prevalent within a nanoparticle. Previous work has shown how to extract the temperature from a gold nanoparticle under continuous-wave monochromatic illumination. We extend the technique to pulsed illumination and introduce pump-probe anti-Stokes spectroscopy. This new technique enables us not only to measure an effective electron tempe ...[more]

PMID: 32787000

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Project description:INTRODUCTION:Microfluidic reactionware allows small volumes of reagents to be utilized for highly controlled flow chemistry applications. By integrating these microreactors with onboard analytical systems, the devices change from passive ones to active ones, increasing their functionality and usefulness. A pressing application for these active microreactors is the monitoring of reaction progress and intermediaries with respect to time, shedding light on important information about these real-time synthetic processes. OBJECTIVE:In this multi-disciplinary study the objective was to utilise advanced digital fabrication to research metallic, active microreactors with integrated fibre optics for reaction progress monitoring of solvent based liquids, incompatible with previously researched polymer devices, in combination with on-board Ultraviolet-visible spectroscopy for real-time reaction monitoring. METHOD:A solid-state, metal-based additive manufactured system (Ultrasonic Additive Manufacturing) combined with focussed ion beam milling, that permitted the accurate embedment of delicate sensory elements directly at the point of need within aluminium layers, was researched as a method to create active, metallic, flow reactors with on-board sensing. This outcome was then used to characterise and correctly identify concentrations of UV-active water-soluble B-vitamin nicotinamide and fluorescein. A dilution series was formed from 0.01-1.75 mM; which was pumped through the research device and monitored using UV-vis spectroscopy. RESULTS:The results uniquely showed the in-situ ion milling of ultrasonically embedded optical fibres resulted in a metallic microfluidic reaction and monitoring device capable of measuring solvent solutions from 18 ?M to 18 mM of nicotinamide and fluorescein, in real time. This level of accuracy highlights that the researched device and methods are capable of real-time spectrographic analysis of a range of chemical reactions outside of those possible with polymer devices.

Dataset Information

Effective Electron Temperature Measurement Using Time-Resolved Anti-Stokes Photoluminescence.

Publications

Effective Electron Temperature Measurement Using Time-Resolved Anti-Stokes Photoluminescence.

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