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

Jollans, Thomas; Caldarola, Martín; Sivan, Yonatan; Orrit, Michel

doi:10.1021/acs.jpca.0c06671

Cited by 29 publications

(43 citation statements)

References 41 publications

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“…Orrit's group explained this subtlety in 2020, 36 and noticed, like others, 33 that within the range of AS energy shifts, the difference between one model or another is not dramatic, and both of them could be conveniently replaced with Boltzmann statistics, that is a simple exponential profile:…”

Section: Photoluminescence or Light Scattering?mentioning

confidence: 99%

“…It also fails when interband transitions enter into play, i.e., at large wave numbers, or when the excitation laser wavelength is not red-shifted enough (Figures 3c,f). 36 Variations of 40% have been observed, though, in the temperature estimation when replacing BE with FD statistics (see Supplemental Information of ref 5). In semi-log representation (Figure 2d), at small wave numbers, the FD statistics are concave whereas the BE statistics are convex.…”

Section: Photoluminescence or Light Scattering?mentioning

confidence: 99%

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Anti-Stokes Thermometry in Nanoplasmonics

Baffou

2021

ACS Nano

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Whereas heating nanoparticles with light is straightforward, measuring the resulting nanoscale temperature increase is intricate, and still a matter of active research in plasmonics, with envisioned applications in nanochemistry, biomedicine, and solar light harvesting, among others. Interestingly, this research line mostly belongs to the optics community today, because light is not only used for heating but also often for temperature probing. In this Perspective, I present and discuss recent advances in the search for efficient and reliable thermometry techniques for nanoplasmonic systems by the nanooptics community. I focus on the recently proposed approach based on the spectral measurement of anti-Stokes emission from the plasmonic nanoparticles themselves.Nanoscale heating is a fundamental concept that offers research opportunities in many scientific fields.The method of choice for achieving nanoscale heating has been the use of light to illuminate molecular dyes or absorbing nanoparticles. Nanoparticles have been the preferred light absorbers over molecules because they neither photo-nor thermo-bleach, and are thus more suited for applications requiring prolonged use. The best photothermal conversion efficiencies are reached using metal nanoparticles.Metals feature large electronic density, in comparison to semiconductors for example, which ensures much stronger interactions with light and subsequent absorption. In addition, metal nanoparticles can exhibit localized plasmonic resonances, which further enhance light absorption by several orders of magnitude, especially with noble metals. This picture led to the field of thermoplasmonics, 1 which is the use of metal nanoparticles under illumination as nanosources of heat. In this field, gold nanoparticles in particular have played a major role for the past two decades because they feature strong plasmonic resonances, are biocompatible, and their resonance can be adjusted from the visible to the infrared range, as a function of their morphology.The challenge in nanoscale heating research and applications is not in achieving nanoscale heating. This achievement is actually trivial, when using nanoparticles. Rather, the difficulty is in measuring the resulting nanoscale temperature increase. 2 After two decades, the lack of efficient and reliable nanoscale thermometry continues to cause problems in some applications of nanoplasmonics. In particular, in plasmonics-assisted chemistry, the possible occurrence of plasmonic heating has been disregarded for a decade, with some work recently questioning the interpretation of data from several impactful publications. 3,4 In this field, heating is not the target, but rather a side effect. Nevertheless, it is crucial to quantify temperature increases properly to ensure correct interpretations of the experimental observations. Thus, thermometry is not only the concern of applications where heating is the target, it is ubiquitous in plasmonics, whether the resultant heating is desired or not.

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Section: Photoluminescence or Light Scattering?mentioning

confidence: 99%

Section: Photoluminescence or Light Scattering?mentioning

confidence: 99%

Anti-Stokes Thermometry in Nanoplasmonics

Baffou

2021

ACS Nano

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“…Such gradients may strongly affect reaction rates, yet are many times un-accounted for. High resolution thermometry techniques have been developed [98][99][100][101][102][103][104] and implemented in the context of photocatalysis 84 , however, they are far from being sufficiently robust 104 . Indeed, similar difficulties to measure the temperature distribution were observed also in other contemporary problems in nanophotonics, in particular, in perovskite films, see [105 and 106] and the ongoing exchange.…”

mentioning

confidence: 99%

“…The comprehensive critical studies published over the last year or so (see [41,53,54,[56][57][58][59][60][61]) and the vibrant ongoing discussion in the field seem to have re-directed the study of plasmon-assisted photocatalysis into a more reliable, quantitative scientific routine. Detailed thermal calculations are becoming more com-mon and accessible (e.g., [41, 47, 55, 58, and 74]) and the awareness to the characteristics of the temperature distribution 41,47,55 and to proper temperature measurements has grown 50,71,84,98,103,104,112,113 . Advanced techniques are being developed and the use of fluorescence and Raman techniques is becoming more abundant in the context of plasmon-assisted photocatalysis 76,99,104,110,114,115 .…”

mentioning

confidence: 99%

“…Detailed thermal calculations are becoming more com-mon and accessible (e.g., [41, 47, 55, 58, and 74]) and the awareness to the characteristics of the temperature distribution 41,47,55 and to proper temperature measurements has grown 50,71,84,98,103,104,112,113 . Advanced techniques are being developed and the use of fluorescence and Raman techniques is becoming more abundant in the context of plasmon-assisted photocatalysis 76,99,104,110,114,115 . Indeed, several convincing demonstrations of "hot" electron-driven reactions with proper thermal control have been reported 47,50,74,80 .…”

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confidence: 99%

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Recent developments in plasmon-assisted photocatalysis -- a personal perspective

Sivan,

Dubi

2020

Preprint

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It has been known for many years that metallic nanoparticles can catalyse various chemical reactions, both in the dark and under illumination, through different mechanisms. In the last decade or so, many claims of plasmon-assisted "hot" electron driven catalysis of bond-dissociation reactions have been put forward. These claims were challenged in a recent series of papers, where both the underlying theory of "hot" electron generation and the use of specific experimental setups to discover them in chemical reactions were examined in detail. The conclusion that arose from these works is that as long as temperature gradients exist inside the system (as for typical experimental setups) a quantification of non-thermal effects is close to impossible. Instead, a standard thermal theory was shown to be capable of explaining the experimental findings quite accurately. Here, we review the central lines of thought that led to these conclusions, from a personal perspective. We lay out the key aspects of the theory, and point to the specific caveats one must be aware of in performing photo-catalysis experiments. Finally, we provide some future directions of study.Metal nanoparticles (NPs) are known to exhibit unusual optical properties, in particular, for having absorption and scattering cross-sections that exceed their physical size. This was predicted to enable a long list of potential applications in diverse fields 1 . Unfortunately, however, the strong absorption in the metal severely limits many of these applications 2,3 . Since the energy absorbed in the metal gets converted to heat almost in its entirety 4,5 , in more recent years, attention was diverted into applications that exploit the absorption, like high temperature chemistry, thermal treatment of cancer, water purification etc. [6][7][8][9][10] .Adding to these, one of the most promising such applications was predicted to be the speeding up of chemical reactions, usually referred to as plasmon-assisted photocatalysis. In particular, it was envisioned that the absorption of photons promotes the generation of a non-equilibrium (also known as non-thermal, or "hot") carrier distribution such that electrons in the high-energy tail of this distribution can tunnel out of the metal into high-energy orbitals of the surrounding molecules, and then catalyse the chemical reaction. This was usually referred to as the "hot carrier mechanism" (or "indirect" plasmon-assisted photocatalysis [11][12][13] ). We note that the term "hot carriers" is somewhat unfortunate, as it implies that the carriers are in thermal equilibrium (i.e. their distribution is Fermi-like) albeit with a temperature higher than the ambient (such that the system in general is out of equilibrium). Yet, the common practice in the field refers to "hot electrons" as having a distribution which is different than a thermal distribution with the ambient temperature (see, e.g., the title of Ref. [14]). Hereafter, we use the terms "non-thermal" and "hot" intermittently, as is accustomed in the literature.The "hot" ...

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A review on short and ultrashort pulsed laser microdrilling: materials, mechanism, methods, and applications

Deepu,

Jagadesh

2024

J Braz. Soc. Mech. Sci. Eng.

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

Cited by 29 publications

References 41 publications

Anti-Stokes Thermometry in Nanoplasmonics

Anti-Stokes Thermometry in Nanoplasmonics

Recent developments in plasmon-assisted photocatalysis -- a personal perspective

A review on short and ultrashort pulsed laser microdrilling: materials, mechanism, methods, and applications

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