Pump–Probe Optical Response and Four-Wave Mixing in a Zinc–Phthalocyanine–Metal Nanoparticle Hybrid System
We investigate theoretically the optical response of a zinc–phthalocyanine molecular quantum system near a gold spherical nanoparticle with a radius of 80 nm. The quantum system is irradiated by a strong pump and a weak probe coherent electromagnetic field. Using the density matrix methodology, we o...
| Main Authors: | , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
MDPI AG
2023-09-01
|
| Series: | Micromachines |
| Subjects: | |
| Online Access: | https://www.mdpi.com/2072-666X/14/9/1735 |
| _version_ | 1797578786792800256 |
|---|---|
| author | Natalia Domenikou Spyridon G. Kosionis Ioannis Thanopulos Vassilios Yannopapas Emmanuel Paspalakis |
| author_facet | Natalia Domenikou Spyridon G. Kosionis Ioannis Thanopulos Vassilios Yannopapas Emmanuel Paspalakis |
| author_sort | Natalia Domenikou |
| collection | DOAJ |
| description | We investigate theoretically the optical response of a zinc–phthalocyanine molecular quantum system near a gold spherical nanoparticle with a radius of 80 nm. The quantum system is irradiated by a strong pump and a weak probe coherent electromagnetic field. Using the density matrix methodology, we obtain analytical expressions for the absorption, dispersion, and the four-wave-mixing coefficients. The influence of the nanoparticle on the spontaneous decay rate of the quantum system, as well as on the external fields, are obtained by an electromagnetic Green’s tensor method. The spectroscopic parameters of the molecule are also obtained by ab initio methods. For the studied optical spectra, we find that, below a critical distance between the molecule and the plasmonic nanoparticle, determined by the minimal value of the effective Rabi frequency, single-peaked spectra are observed. Above this critical distance, the spectra exhibit the characteristic Mollow-shaped profiles. The enhancement of the pump field detuning induces the shift of the sideband resonances away from the origin. Lastly, and most importantly, regardless of the value of the detuning, the optical response of the system is maximized for an intermediate value of the interparticle distance. |
| first_indexed | 2024-03-10T22:26:46Z |
| format | Article |
| id | doaj.art-2200cf3a9cba46038395a67fdd8e326b |
| institution | Directory Open Access Journal |
| issn | 2072-666X |
| language | English |
| last_indexed | 2024-03-10T22:26:46Z |
| publishDate | 2023-09-01 |
| publisher | MDPI AG |
| record_format | Article |
| series | Micromachines |
| spelling | doaj.art-2200cf3a9cba46038395a67fdd8e326b2023-11-19T11:59:55ZengMDPI AGMicromachines2072-666X2023-09-01149173510.3390/mi14091735Pump–Probe Optical Response and Four-Wave Mixing in a Zinc–Phthalocyanine–Metal Nanoparticle Hybrid SystemNatalia Domenikou0Spyridon G. Kosionis1Ioannis Thanopulos2Vassilios Yannopapas3Emmanuel Paspalakis4Materials Science Department, School of Natural Sciences, University of Patras, 26504 Patras, GreeceMaterials Science Department, School of Natural Sciences, University of Patras, 26504 Patras, GreeceMaterials Science Department, School of Natural Sciences, University of Patras, 26504 Patras, GreeceDepartment of Physics, School of Natural Sciences, National Technical University of Athens, 15780 Athens, GreeceMaterials Science Department, School of Natural Sciences, University of Patras, 26504 Patras, GreeceWe investigate theoretically the optical response of a zinc–phthalocyanine molecular quantum system near a gold spherical nanoparticle with a radius of 80 nm. The quantum system is irradiated by a strong pump and a weak probe coherent electromagnetic field. Using the density matrix methodology, we obtain analytical expressions for the absorption, dispersion, and the four-wave-mixing coefficients. The influence of the nanoparticle on the spontaneous decay rate of the quantum system, as well as on the external fields, are obtained by an electromagnetic Green’s tensor method. The spectroscopic parameters of the molecule are also obtained by ab initio methods. For the studied optical spectra, we find that, below a critical distance between the molecule and the plasmonic nanoparticle, determined by the minimal value of the effective Rabi frequency, single-peaked spectra are observed. Above this critical distance, the spectra exhibit the characteristic Mollow-shaped profiles. The enhancement of the pump field detuning induces the shift of the sideband resonances away from the origin. Lastly, and most importantly, regardless of the value of the detuning, the optical response of the system is maximized for an intermediate value of the interparticle distance.https://www.mdpi.com/2072-666X/14/9/1735pump–probe optical responsenonlinear optical responsefour-wave mixingtwo-level quantum systemzinc–phthalocyanine moleculemetallic nanoparticle |
| spellingShingle | Natalia Domenikou Spyridon G. Kosionis Ioannis Thanopulos Vassilios Yannopapas Emmanuel Paspalakis Pump–Probe Optical Response and Four-Wave Mixing in a Zinc–Phthalocyanine–Metal Nanoparticle Hybrid System Micromachines pump–probe optical response nonlinear optical response four-wave mixing two-level quantum system zinc–phthalocyanine molecule metallic nanoparticle |
| title | Pump–Probe Optical Response and Four-Wave Mixing in a Zinc–Phthalocyanine–Metal Nanoparticle Hybrid System |
| title_full | Pump–Probe Optical Response and Four-Wave Mixing in a Zinc–Phthalocyanine–Metal Nanoparticle Hybrid System |
| title_fullStr | Pump–Probe Optical Response and Four-Wave Mixing in a Zinc–Phthalocyanine–Metal Nanoparticle Hybrid System |
| title_full_unstemmed | Pump–Probe Optical Response and Four-Wave Mixing in a Zinc–Phthalocyanine–Metal Nanoparticle Hybrid System |
| title_short | Pump–Probe Optical Response and Four-Wave Mixing in a Zinc–Phthalocyanine–Metal Nanoparticle Hybrid System |
| title_sort | pump probe optical response and four wave mixing in a zinc phthalocyanine metal nanoparticle hybrid system |
| topic | pump–probe optical response nonlinear optical response four-wave mixing two-level quantum system zinc–phthalocyanine molecule metallic nanoparticle |
| url | https://www.mdpi.com/2072-666X/14/9/1735 |
| work_keys_str_mv | AT nataliadomenikou pumpprobeopticalresponseandfourwavemixinginazincphthalocyaninemetalnanoparticlehybridsystem AT spyridongkosionis pumpprobeopticalresponseandfourwavemixinginazincphthalocyaninemetalnanoparticlehybridsystem AT ioannisthanopulos pumpprobeopticalresponseandfourwavemixinginazincphthalocyaninemetalnanoparticlehybridsystem AT vassiliosyannopapas pumpprobeopticalresponseandfourwavemixinginazincphthalocyaninemetalnanoparticlehybridsystem AT emmanuelpaspalakis pumpprobeopticalresponseandfourwavemixinginazincphthalocyaninemetalnanoparticlehybridsystem |