| Title: |
Intense-field interaction regime with weak laser pulses and localized plasmonic enhancement: Reference-free demonstration by 3rd- and 5th-order infrared spectroscopies |
| Authors: |
Mackin, Robert T.; Cohn, Bar; Chuntonov, Lev; Rubtsov, Igor V. |
| Contributors: |
National Science Foundation; United States-Israel Binational Science Foundation; Israel Science Foundation |
| Source: |
The Journal of Chemical Physics ; volume 151, issue 12 ; ISSN 0021-9606 1089-7690 |
| Publisher Information: |
AIP Publishing |
| Publication Year: |
2019 |
| Description: |
In bulk materials, intense field interaction is accompanied by undesired nonresonant processes. Plasmonic nanostructures localize enhanced fields exclusively in their vicinity. We report a 4-fold vibrational population inversion between all the excited and the ground states in the molecular monolayer on the surface of gold nanoantennas. Excited population assessment relies on a novel reference-sample-free evaluation of the field enhancement with 5th- and 3rd-order nonlinear infrared spectroscopies and on quantitative modeling of coherent excitation dynamics. This study opens opportunities for precise population control utilizing population inversion for vibrational transitions using weak fields. |
| Document Type: |
article in journal/newspaper |
| Language: |
English |
| DOI: |
10.1063/1.5120531 |
| DOI: |
10.1063/1.5120531/15563804/121103_1_online.pdf |
| Availability: |
https://doi.org/10.1063/1.5120531; http://aip.scitation.org/doi/am-pdf/10.1063/1.5120531; https://pubs.aip.org/aip/jcp/article-pdf/doi/10.1063/1.5120531/15563804/121103_1_online.pdf |
| Rights: |
https://publishing.aip.org/authors/rights-and-permissions |
| Accession Number: |
edsbas.82E7E3A0 |
| Database: |
BASE |