Semi-empirical quantum optics for mid-infrared molecular nanophotonics
Abstract
Nanoscale infrared (IR) resonators with sub-diffraction limited mode volumes and open geometries have emerged as new platforms for implementing cavity quantum electrodynamics at room temperature. The use of IR nanoantennas and tip nanoprobes to study strong light–matter coupling of molecular vibrations with the vacuum field can be exploited for IR quantum control with nanometer spatial and femtosecond temporal resolution. In order to advance the development of molecule-based quantum nanophotonics in the mid-IR, we propose a generally applicable semi-empirical methodology based on quantum optics to describe light–matter interaction in systems driven by mid-IR femtosecond laser pulses. The theory is shown to reproduce recent experiments on the acceleration of the vibrational relaxation rate in infrared nanostructures. It also provides physical insights on the implementation of coherent phase rotations of the near-field using broadband nanotips. We then apply the quantum framework to develop general tip-design rules for the experimental manipulation of vibrational strong coupling and Fano interference effects in open infrared resonators. We finally propose the possibility of transferring the natural anharmonicity of molecular vibrational levels to the resonator near-field in the weak coupling regime to implement intensity-dependent phase shifts of the coupled system response with strong pulses and develop a vibrational chirpingmore »
- Authors:
-
[1];
[3];
[4];
[3];
[3];
[5];
[3];
[6]
- University of Santiago (Chile)
- Universidad de Concepción (Chile)
- Univ. of Colorado, Boulder, CO (United States)
- Colgate University, Hamilton, NY (United States)
- Universidad de Concepción (Chile); Millennium Institute for Research in Optics of ANID (Chile)
- University of Santiago (Chile); Millennium Institute for Research in Optics of ANID (Chile)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); US Air Force Office of Scientific Research (AFOSR)
- OSTI Identifier:
- 1982371
- Grant/Contract Number:
- AC02-05CH11231; FA9550-21-1-0272
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 156; Journal Issue: 12; Journal ID: ISSN 0021-9606
- Publisher:
- American Institute of Physics (AIP)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; Maxwell equations; Antennas; Femtosecond lasers; Nanophotonics; Vibrational spectroscopy; Quantum control theory; Quantum information; Quantum optics; Quantum theory; Cavity quantum electrodynamics
Citation Formats
Triana, Johan F., Arias, Mauricio, Nishida, Jun, Muller, Eric A., Wilcken, Roland, Johnson, Samuel C., Delgado, Aldo, Raschke, Markus B., and Herrera, Felipe. Semi-empirical quantum optics for mid-infrared molecular nanophotonics. United States: N. p., 2022.
Web. doi:10.1063/5.0075894.
Triana, Johan F., Arias, Mauricio, Nishida, Jun, Muller, Eric A., Wilcken, Roland, Johnson, Samuel C., Delgado, Aldo, Raschke, Markus B., & Herrera, Felipe. Semi-empirical quantum optics for mid-infrared molecular nanophotonics. United States. https://doi.org/10.1063/5.0075894
Triana, Johan F., Arias, Mauricio, Nishida, Jun, Muller, Eric A., Wilcken, Roland, Johnson, Samuel C., Delgado, Aldo, Raschke, Markus B., and Herrera, Felipe. Fri .
"Semi-empirical quantum optics for mid-infrared molecular nanophotonics". United States. https://doi.org/10.1063/5.0075894. https://www.osti.gov/servlets/purl/1982371.
@article{osti_1982371,
title = {Semi-empirical quantum optics for mid-infrared molecular nanophotonics},
author = {Triana, Johan F. and Arias, Mauricio and Nishida, Jun and Muller, Eric A. and Wilcken, Roland and Johnson, Samuel C. and Delgado, Aldo and Raschke, Markus B. and Herrera, Felipe},
abstractNote = {Nanoscale infrared (IR) resonators with sub-diffraction limited mode volumes and open geometries have emerged as new platforms for implementing cavity quantum electrodynamics at room temperature. The use of IR nanoantennas and tip nanoprobes to study strong light–matter coupling of molecular vibrations with the vacuum field can be exploited for IR quantum control with nanometer spatial and femtosecond temporal resolution. In order to advance the development of molecule-based quantum nanophotonics in the mid-IR, we propose a generally applicable semi-empirical methodology based on quantum optics to describe light–matter interaction in systems driven by mid-IR femtosecond laser pulses. The theory is shown to reproduce recent experiments on the acceleration of the vibrational relaxation rate in infrared nanostructures. It also provides physical insights on the implementation of coherent phase rotations of the near-field using broadband nanotips. We then apply the quantum framework to develop general tip-design rules for the experimental manipulation of vibrational strong coupling and Fano interference effects in open infrared resonators. We finally propose the possibility of transferring the natural anharmonicity of molecular vibrational levels to the resonator near-field in the weak coupling regime to implement intensity-dependent phase shifts of the coupled system response with strong pulses and develop a vibrational chirping model to understand the effect. The semi-empirical quantum theory is equivalent to first-principles techniques based on Maxwell’s equations, but its lower computational cost suggests its use as a rapid design tool for the development of strongly coupled infrared nanophotonic hardware for applications ranging from quantum control of materials to quantum information processing.},
doi = {10.1063/5.0075894},
journal = {Journal of Chemical Physics},
number = 12,
volume = 156,
place = {United States},
year = {Fri Mar 25 00:00:00 EDT 2022},
month = {Fri Mar 25 00:00:00 EDT 2022}
}
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