Phonon Mean Free Path Spectroscopy By Raman Thermometry

Fuente: arXiv
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Main Authors: Dudde, Katharina, Elhajhasan, Mahmoud, Würsch, Guillaume, Themann, Julian, Lierath, Jana, Paul, Dwaipayan, Protik, Nakib H., Romano, Giuseppe, Callsen, Gordon
Format: Preprint
Published: 2025
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author Dudde, Katharina
Elhajhasan, Mahmoud
Würsch, Guillaume
Themann, Julian
Lierath, Jana
Paul, Dwaipayan
Protik, Nakib H.
Romano, Giuseppe
Callsen, Gordon
author_facet Dudde, Katharina
Elhajhasan, Mahmoud
Würsch, Guillaume
Themann, Julian
Lierath, Jana
Paul, Dwaipayan
Protik, Nakib H.
Romano, Giuseppe
Callsen, Gordon
contents In this work, we exemplify on a bulk silicon sample that Raman thermometry is capable of phonon mean free path (PMFP) spectroscopy. Our experimental approach is similar to the variation of different characteristic length scales $l_{c}$ during thermal reflectance measurements in the time or frequency domain and transient thermal grating spectroscopy. In place of $l_{c}$, we vary the laser focus spot size ($w_{e}$) and the light penetration depth ($h_α$) during one-laser Raman thermometry (1LRT) measurements. For our largest $w_{e}$ values, the derived effective thermal conductivities $κ_{eff}$ converge towards the bulk thermal conductivity $κ_{bulk}$ for silicon. However, towards smaller $w_{e}$ values, we observe a pronounced increase for the $κ_{eff}$ values, which amounts up to a factor of 5.3 at 293K and even 8.3 at 200K. We mainly assign this phenomenon to quasi-ballistic phonon transport. As a result, we can compare our measured $κ_{eff}(w_{e})$ trends with the thermal accumulation function $κ_{cum}$ and its dependence on the phonon mean free path $l_{ph}$, which we derive from ab initio solutions of the linearized phonon Boltzmann transport equation (BTE). Since the variation of $w_{e}$ can be experimentally cumbersome, we also suggest varying $h_α(λ)$ via the applied Raman laser wavelength $λ$ during 1LRT. In this regard, we present proof-of-principle 1LRT measurements, yielding a step-like $κ_{eff}(λ)$ trend for four different $λ$ values, which we also interpret in terms of quasi-ballistic phonon transport. Our results shall seed future PMFP spectroscopy based on 1LRT, which can directly be benchmarked against state-of-art theory by comparison of $κ_{\text{cum}}$ trends and not only $κ$ values, aiming to test our understanding of the intricate phonon transport physics.
format Preprint
id arxiv_https___arxiv_org_abs_2505_14506
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Phonon Mean Free Path Spectroscopy By Raman Thermometry
Dudde, Katharina
Elhajhasan, Mahmoud
Würsch, Guillaume
Themann, Julian
Lierath, Jana
Paul, Dwaipayan
Protik, Nakib H.
Romano, Giuseppe
Callsen, Gordon
Optics
Materials Science
In this work, we exemplify on a bulk silicon sample that Raman thermometry is capable of phonon mean free path (PMFP) spectroscopy. Our experimental approach is similar to the variation of different characteristic length scales $l_{c}$ during thermal reflectance measurements in the time or frequency domain and transient thermal grating spectroscopy. In place of $l_{c}$, we vary the laser focus spot size ($w_{e}$) and the light penetration depth ($h_α$) during one-laser Raman thermometry (1LRT) measurements. For our largest $w_{e}$ values, the derived effective thermal conductivities $κ_{eff}$ converge towards the bulk thermal conductivity $κ_{bulk}$ for silicon. However, towards smaller $w_{e}$ values, we observe a pronounced increase for the $κ_{eff}$ values, which amounts up to a factor of 5.3 at 293K and even 8.3 at 200K. We mainly assign this phenomenon to quasi-ballistic phonon transport. As a result, we can compare our measured $κ_{eff}(w_{e})$ trends with the thermal accumulation function $κ_{cum}$ and its dependence on the phonon mean free path $l_{ph}$, which we derive from ab initio solutions of the linearized phonon Boltzmann transport equation (BTE). Since the variation of $w_{e}$ can be experimentally cumbersome, we also suggest varying $h_α(λ)$ via the applied Raman laser wavelength $λ$ during 1LRT. In this regard, we present proof-of-principle 1LRT measurements, yielding a step-like $κ_{eff}(λ)$ trend for four different $λ$ values, which we also interpret in terms of quasi-ballistic phonon transport. Our results shall seed future PMFP spectroscopy based on 1LRT, which can directly be benchmarked against state-of-art theory by comparison of $κ_{\text{cum}}$ trends and not only $κ$ values, aiming to test our understanding of the intricate phonon transport physics.
title Phonon Mean Free Path Spectroscopy By Raman Thermometry
topic Optics
Materials Science
url https://arxiv.org/abs/2505.14506