Laser Pulse Induced Second- and Third-Harmonic Generation of Gold Nanorods with Real-Time Time-Dependent Density Functional Tight Binding (RT-TDDFTB) Method

Fuente: arXiv
Gespeichert in:
Bibliographische Detailangaben
Hauptverfasser: Giri, Sajal Kumar, Schatz, George C.
Format: Preprint
Veröffentlicht: 2024
Schlagworte:
Online-Zugang:
Tags: Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
_version_ 1866929501110272000
author Giri, Sajal Kumar
Schatz, George C.
author_facet Giri, Sajal Kumar
Schatz, George C.
contents In this study, we investigate second- and third-harmonic generation processes in Au nanorod systems using the real-time time-dependent density functional tight binding method. Our study focuses on the computation of nonlinear signals based on the time dependent dipole response induced by linearly polarized laser pulses interacting with nanoparticles. We systematically explore the influence of various laser parameters, including pump intensity, duration, frequency, and polarization directions, on harmonic generation. We demonstrate all the results using Au nanorod dimer systems arranged in end-to-end configurations, and disrupting the spatial symmetry of regular single nanorod systems is crucial for second-harmonic generation processes. Furthermore, we study the impact of nanorod lengths, which lead to variable plasmon energies, on harmonic generation, and estimates of polarizabilities and hyper-polarizabilities are provided.
format Preprint
id arxiv_https___arxiv_org_abs_2405_00913
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Laser Pulse Induced Second- and Third-Harmonic Generation of Gold Nanorods with Real-Time Time-Dependent Density Functional Tight Binding (RT-TDDFTB) Method
Giri, Sajal Kumar
Schatz, George C.
Optics
Classical Physics
In this study, we investigate second- and third-harmonic generation processes in Au nanorod systems using the real-time time-dependent density functional tight binding method. Our study focuses on the computation of nonlinear signals based on the time dependent dipole response induced by linearly polarized laser pulses interacting with nanoparticles. We systematically explore the influence of various laser parameters, including pump intensity, duration, frequency, and polarization directions, on harmonic generation. We demonstrate all the results using Au nanorod dimer systems arranged in end-to-end configurations, and disrupting the spatial symmetry of regular single nanorod systems is crucial for second-harmonic generation processes. Furthermore, we study the impact of nanorod lengths, which lead to variable plasmon energies, on harmonic generation, and estimates of polarizabilities and hyper-polarizabilities are provided.
title Laser Pulse Induced Second- and Third-Harmonic Generation of Gold Nanorods with Real-Time Time-Dependent Density Functional Tight Binding (RT-TDDFTB) Method
topic Optics
Classical Physics
url https://arxiv.org/abs/2405.00913