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Detecting, Distinguishing, and Spatiotemporally Tracking Photogenerated Charge and Heat at the Nanoscale

[Image: see text] Since dissipative processes are ubiquitous in semiconductors, characterizing how electronic and thermal energy transduce and transport at the nanoscale is vital for understanding and leveraging their fundamental properties. For example, in low-dimensional transition metal dichalcog...

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Autores principales: Weaver, Hannah L., Went, Cora M., Wong, Joeson, Jasrasaria, Dipti, Rabani, Eran, Atwater, Harry A., Ginsberg, Naomi S.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10569093/
https://www.ncbi.nlm.nih.gov/pubmed/37721430
http://dx.doi.org/10.1021/acsnano.3c04607
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author Weaver, Hannah L.
Went, Cora M.
Wong, Joeson
Jasrasaria, Dipti
Rabani, Eran
Atwater, Harry A.
Ginsberg, Naomi S.
author_facet Weaver, Hannah L.
Went, Cora M.
Wong, Joeson
Jasrasaria, Dipti
Rabani, Eran
Atwater, Harry A.
Ginsberg, Naomi S.
author_sort Weaver, Hannah L.
collection PubMed
description [Image: see text] Since dissipative processes are ubiquitous in semiconductors, characterizing how electronic and thermal energy transduce and transport at the nanoscale is vital for understanding and leveraging their fundamental properties. For example, in low-dimensional transition metal dichalcogenides (TMDCs), excess heat generation upon photoexcitation is difficult to avoid since even with modest injected exciton densities exciton–exciton annihilation still occurs. Both heat and photoexcited electronic species imprint transient changes in the optical response of a semiconductor, yet the distinct signatures of each are difficult to disentangle in typical spectra due to overlapping resonances. In response, we employ stroboscopic optical scattering microscopy (stroboSCAT) to simultaneously map both heat and exciton populations in few-layer MoS(2) on relevant nanometer and picosecond length- and time scales and with 100-mK temperature sensitivity. We discern excitonic contributions to the signal from heat by combining observations close to and far from exciton resonances, characterizing the photoinduced dynamics for each. Our approach is general and can be applied to any electronic material, including thermoelectrics, where heat and electronic observables spatially interplay, and it will enable direct and quantitative discernment of different types of coexisting energy without recourse to complex models or underlying assumptions.
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spelling pubmed-105690932023-10-13 Detecting, Distinguishing, and Spatiotemporally Tracking Photogenerated Charge and Heat at the Nanoscale Weaver, Hannah L. Went, Cora M. Wong, Joeson Jasrasaria, Dipti Rabani, Eran Atwater, Harry A. Ginsberg, Naomi S. ACS Nano [Image: see text] Since dissipative processes are ubiquitous in semiconductors, characterizing how electronic and thermal energy transduce and transport at the nanoscale is vital for understanding and leveraging their fundamental properties. For example, in low-dimensional transition metal dichalcogenides (TMDCs), excess heat generation upon photoexcitation is difficult to avoid since even with modest injected exciton densities exciton–exciton annihilation still occurs. Both heat and photoexcited electronic species imprint transient changes in the optical response of a semiconductor, yet the distinct signatures of each are difficult to disentangle in typical spectra due to overlapping resonances. In response, we employ stroboscopic optical scattering microscopy (stroboSCAT) to simultaneously map both heat and exciton populations in few-layer MoS(2) on relevant nanometer and picosecond length- and time scales and with 100-mK temperature sensitivity. We discern excitonic contributions to the signal from heat by combining observations close to and far from exciton resonances, characterizing the photoinduced dynamics for each. Our approach is general and can be applied to any electronic material, including thermoelectrics, where heat and electronic observables spatially interplay, and it will enable direct and quantitative discernment of different types of coexisting energy without recourse to complex models or underlying assumptions. American Chemical Society 2023-09-18 /pmc/articles/PMC10569093/ /pubmed/37721430 http://dx.doi.org/10.1021/acsnano.3c04607 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Weaver, Hannah L.
Went, Cora M.
Wong, Joeson
Jasrasaria, Dipti
Rabani, Eran
Atwater, Harry A.
Ginsberg, Naomi S.
Detecting, Distinguishing, and Spatiotemporally Tracking Photogenerated Charge and Heat at the Nanoscale
title Detecting, Distinguishing, and Spatiotemporally Tracking Photogenerated Charge and Heat at the Nanoscale
title_full Detecting, Distinguishing, and Spatiotemporally Tracking Photogenerated Charge and Heat at the Nanoscale
title_fullStr Detecting, Distinguishing, and Spatiotemporally Tracking Photogenerated Charge and Heat at the Nanoscale
title_full_unstemmed Detecting, Distinguishing, and Spatiotemporally Tracking Photogenerated Charge and Heat at the Nanoscale
title_short Detecting, Distinguishing, and Spatiotemporally Tracking Photogenerated Charge and Heat at the Nanoscale
title_sort detecting, distinguishing, and spatiotemporally tracking photogenerated charge and heat at the nanoscale
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10569093/
https://www.ncbi.nlm.nih.gov/pubmed/37721430
http://dx.doi.org/10.1021/acsnano.3c04607
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