Two-Step Relaxation of Non-Equilibrium Electrons in Graphene: The Key to Understanding Pump–Probe Experiments

In the majority of experiments targeting nonlinear optical phenomena, the application of high-intensity pulses drives electrons in graphene into a strongly non-equilibrium state. Under these conditions, conventional perturbation theory falls short in explaining graphene’s intricate optical response...

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Main Authors: Diogo F. P. Cunha, Rui Dias, Manuel J. L. F. Rodrigues, Mikhail I. Vasilevskiy
Format: Article
Language:English
Published: MDPI AG 2024-02-01
Series:Applied Sciences
Subjects:
Online Access:https://www.mdpi.com/2076-3417/14/3/1250
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author Diogo F. P. Cunha
Rui Dias
Manuel J. L. F. Rodrigues
Mikhail I. Vasilevskiy
author_facet Diogo F. P. Cunha
Rui Dias
Manuel J. L. F. Rodrigues
Mikhail I. Vasilevskiy
author_sort Diogo F. P. Cunha
collection DOAJ
description In the majority of experiments targeting nonlinear optical phenomena, the application of high-intensity pulses drives electrons in graphene into a strongly non-equilibrium state. Under these conditions, conventional perturbation theory falls short in explaining graphene’s intricate optical response because of significant deviations in electron distribution over energy states from the equilibrium Fermi-Dirac one. In this work, we present a two-step relaxation model capable of predicting the transient dynamics of graphene’s carriers out of equilibrium, from the generation of spectrally narrow populations of non-thermalized electrons and holes to the establishment of a hot-electron gas and its subsequent cooling toward equilibrium with the crystal lattice. By comparing our model calculations to experimental results, we demonstrate its reliability and relevance to pump–probe experiments, providing insights into the pivotal role of hot electrons in comprehending ultrafast dynamics in graphene.
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spelling doaj.art-b5ea18377dc44935b15d6a733c40b0002024-02-09T15:08:23ZengMDPI AGApplied Sciences2076-34172024-02-01143125010.3390/app14031250Two-Step Relaxation of Non-Equilibrium Electrons in Graphene: The Key to Understanding Pump–Probe ExperimentsDiogo F. P. Cunha0Rui Dias1Manuel J. L. F. Rodrigues2Mikhail I. Vasilevskiy3Centre of Physics—CF-UM-UP and Laboratório de Física para Materiais e Tecnologias Emergentes (LaPMET), University of Minho, Campus of Gualtar, 4710-374 Braga, PortugalCentre of Physics—CF-UM-UP and Laboratório de Física para Materiais e Tecnologias Emergentes (LaPMET), University of Minho, Campus of Gualtar, 4710-374 Braga, PortugalCentre of Physics—CF-UM-UP and Laboratório de Física para Materiais e Tecnologias Emergentes (LaPMET), University of Minho, Campus of Gualtar, 4710-374 Braga, PortugalCentre of Physics—CF-UM-UP and Laboratório de Física para Materiais e Tecnologias Emergentes (LaPMET), University of Minho, Campus of Gualtar, 4710-374 Braga, PortugalIn the majority of experiments targeting nonlinear optical phenomena, the application of high-intensity pulses drives electrons in graphene into a strongly non-equilibrium state. Under these conditions, conventional perturbation theory falls short in explaining graphene’s intricate optical response because of significant deviations in electron distribution over energy states from the equilibrium Fermi-Dirac one. In this work, we present a two-step relaxation model capable of predicting the transient dynamics of graphene’s carriers out of equilibrium, from the generation of spectrally narrow populations of non-thermalized electrons and holes to the establishment of a hot-electron gas and its subsequent cooling toward equilibrium with the crystal lattice. By comparing our model calculations to experimental results, we demonstrate its reliability and relevance to pump–probe experiments, providing insights into the pivotal role of hot electrons in comprehending ultrafast dynamics in graphene.https://www.mdpi.com/2076-3417/14/3/1250graphenehot electronspump–probe spectroscopynonlinear optics
spellingShingle Diogo F. P. Cunha
Rui Dias
Manuel J. L. F. Rodrigues
Mikhail I. Vasilevskiy
Two-Step Relaxation of Non-Equilibrium Electrons in Graphene: The Key to Understanding Pump–Probe Experiments
Applied Sciences
graphene
hot electrons
pump–probe spectroscopy
nonlinear optics
title Two-Step Relaxation of Non-Equilibrium Electrons in Graphene: The Key to Understanding Pump–Probe Experiments
title_full Two-Step Relaxation of Non-Equilibrium Electrons in Graphene: The Key to Understanding Pump–Probe Experiments
title_fullStr Two-Step Relaxation of Non-Equilibrium Electrons in Graphene: The Key to Understanding Pump–Probe Experiments
title_full_unstemmed Two-Step Relaxation of Non-Equilibrium Electrons in Graphene: The Key to Understanding Pump–Probe Experiments
title_short Two-Step Relaxation of Non-Equilibrium Electrons in Graphene: The Key to Understanding Pump–Probe Experiments
title_sort two step relaxation of non equilibrium electrons in graphene the key to understanding pump probe experiments
topic graphene
hot electrons
pump–probe spectroscopy
nonlinear optics
url https://www.mdpi.com/2076-3417/14/3/1250
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AT manueljlfrodrigues twosteprelaxationofnonequilibriumelectronsingraphenethekeytounderstandingpumpprobeexperiments
AT mikhailivasilevskiy twosteprelaxationofnonequilibriumelectronsingraphenethekeytounderstandingpumpprobeexperiments