Investigation of the nonlinear refractive index of single-crystalline thin gold films and plasmonic nanostructures

Goetz, Sebastian; Razinskas, Gary; Krauss, Enno; Dreher, Christian; Wurdack, Matthias; Geisler, Peter; Pawłowska, Monika; Hecht, Bert; Brixner, Tobias

doi:10.1007/s00340-016-6370-7

Cited by 4 publications

(4 citation statements)

References 47 publications

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“…By inspecting the sample surface after laser irradiations, the damage threshold is estimated to be 15 kJ/m 2 . The estimated damage threshold is higher than a previously reported value of 0.286 kJ/m 2 where large number of laser pulses were used [13] ; but agrees with the damage threshold of a single laser pulse radiation [18] .…”

Section: Resultssupporting

confidence: 86%

“…, measured with a 130 fs, 800 nm laser below the damage threshold [13] . The real part of the nonlinear susceptibility could be calculated from the nonlinear refractive index: 4 And similarly, the nonlinear absorption, taking the region below 1kJ/m2 is calculated to be 5…”

Section: Classical Modelmentioning

confidence: 99%

“…The nonlinear optical properties of gold have been extensively studied at laser intensities below the sample damage threshold [13] . In this paper, we study the nonlinear optical properties of gold at a laser intensity above the damage threshold.…”

Section: Introductionmentioning

confidence: 99%

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Nonlinear Optical Properties of Gold with Intense Femtosecond Laser Excitations above the Damage Threshold

Wang

Kan

Shen

2023

Preprint

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The nonlinear optical properties of gold thin films have been studied under the irradiation of destructive laser pluses. The transmissivity and the reflectivity of a 100-nm-thick gold film are measured with femtosecond laser irradiations up to 106 J/m2 fluence, which is much higher than the damage threshold of gold. The nonlinearity is calculated with Fresnel loss equations. The real part of the complex refractive index is calculated to have a peak at ~ 10 kJ/m2, which is close to the damage threshold. The complex third-order nonlinear susceptibility χ3 is estimated to be (3.87−6.64𝑖)×10−21𝑚2/𝑉2, which agrees the trend in previous reports that it decreases as pulse duration decreases. This nonlinearity is further studied with a plasmon-photon exchange (PPE) model, where laser induced plasmons and absorbed photons are strongly correlated. The result of the simulation with the PPE model is in good agreement with the experimental transmissivity above the damage threshold. The model predicted an interaction time between photons and plasmons to be about 500 fs. This model is found to be essential in understanding such nonlinear optical processes under both extremely high and conventionally low laser irradiations.

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Section: Resultssupporting

confidence: 86%

Section: Classical Modelmentioning

confidence: 99%

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Nonlinear Optical Properties of Gold with Intense Femtosecond Laser Excitations above the Damage Threshold

Wang

Kan

Shen

2023

Preprint

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“…Additionally, practical applications in most cases require chemically and physically stable systems, severely limiting in situ tunability of the linear as well as nonlinear optical properties. Consequently, the most common plasmonic material is gold (Au), as it possesses favorable optical properties, while other materials have been used as well. , In the case of Au, it was in fact recently shown that its absorption associated with transitions between the d- and sp-band results in an increased nonlinear conversion if the energies of the higher harmonic match these absorption bands. − …”

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confidence: 99%

Switchable Optical Nonlinearity at the Metal to Insulator Transition in Magnesium Thin Films

et al. 2020

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We report resonantly enhanced and switchable third order nonlinearity in magnesium thin films. Utilizing an optical parametric oscillator as a tunable broadband light source, we find a highly wavelength dependent third harmonic conversion efficiency, exhibiting a 40-to 50-fold signal increase over the investigated wavelength range between 1300 and 1800 nm. We relate this unusually strong increase of the intrinsic magnesium material nonlinearity to resonant sp-interband transitions around 0.7 eV or 1770 nm in the fundamental wavelength range, multiplying their impact on the conversion efficiencies. Moreover, we make use of the drastic change in the optical properties of magnesium at the phase transition between metallic magnesium and dielectric magnesium hydride by in situ hydrogenation. We are able to cyclically switch the nonlinearity and the efficiency of the third harmonic conversion process. The time-dependence of the nonlinear signal is complex and is a consequence of several contributions, including the hydrogen concentration-dependent change in the intrinsic nonlinear susceptibility, the change in the surface morphology during hydrogenation and dehydrogenation, as well as the volume change of the material. While shedding new light on the structural and morphological changes in such magnesium thin films, we envision that the switchable and large resonant third-order nonlinearity in magnesium will find applications in nanostructured systems, unlocking additional degrees of freedom in design and implementation, such as wavelength dependency and switchable material nonlinearities.

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Nonlinear optical properties of gold with intense femtosecond laser excitations above the damage threshold

Wang,

Kan,

Shen

2023

AIP Advances

View full text Add to dashboard Cite

The nonlinear optical properties of gold thin films have been studied under the irradiation of destructive laser pluses. The transmissivity and the reflectivity of a 100-nm-thick gold film are measured with femtosecond laser irradiations up to 106 J/m2 fluence, which is much higher than the damage threshold of gold. The nonlinearity is calculated with Fresnel loss equations. The real part of the complex refractive index is calculated to have a peak at ∼10 kJ/m2, which is close to the damage threshold. The complex third-order nonlinear susceptibility χ3 is estimated to be (4.95 − 2.02i) × 10−21 m2/V2, which agrees with the trend in previous reports that it decreases as the pulse duration decreases. This nonlinearity is further studied with a plasmon-photon exchange (PPE) model, where laser induced plasmons and absorbed photons are strongly correlated. The result of the simulation with the PPE model is in good agreement with the experimental transmissivity above the damage threshold. The model predicted an interaction time between photons and plasmons to be about 500 fs. This model is found to be essential in understanding such nonlinear optical processes under both extremely high and conventionally low laser irradiations.

show abstract

Investigation of the nonlinear refractive index of single-crystalline thin gold films and plasmonic nanostructures

Cited by 4 publications

References 47 publications

Nonlinear Optical Properties of Gold with Intense Femtosecond Laser Excitations above the Damage Threshold

Nonlinear Optical Properties of Gold with Intense Femtosecond Laser Excitations above the Damage Threshold

Switchable Optical Nonlinearity at the Metal to Insulator Transition in Magnesium Thin Films

Nonlinear optical properties of gold with intense femtosecond laser excitations above the damage threshold

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