Femtosecond nonlinear refraction of 2D semi-metallic redox exfoliated ZrTe2 at 800 nm

Maldonado, Mauricio; Neto, Manoel L. da Silva; Vianna, Pilar G.; Ribeiro, Henrique B.; Araújo, Cid B. de; Matos, Christiano J. S. de; Seixas, Leandro; Jawaid, Ali; Busch, Robert; Ritter, Allyson J.; Vaia, Richard A.; Gomes, Anderson S. L.

doi:10.1063/5.0031649

Cited by 14 publications

(13 citation statements)

References 28 publications

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“…To obtain scattering profiles of the dispersions, the measured extinction and absorption profiles were subtracted: E(λ) – A(λ) = S(λ). Complete morphological, compositional, and statistical analysis of these materials can be found in previous manuscripts. ,, …”

Section: Methodsmentioning

confidence: 99%

“…Complete morphological, compositional, and statistical analysis of these materials can be found in previous manuscripts. 20,37,48 CW, High-Repetition-Rate, Linearly or Circularly Polarized Light Experiments. The samples were excited with different wavelengths (790 and 532 nm), operation modes of laser (ML-CW and CW), and polarization states (linear and circular).…”

Section: ■ Conclusionmentioning

confidence: 99%

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Intensity-Dependent Thermally Induced Nonlinear Optical Response of Two-Dimensional Layered Transition-Metal Dichalcogenides in Suspension

et al. 2023

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We report experimental studies of spatial self-phase modulation (SSPM) in liquid suspensions of semiconducting MoS 2 , MoSe 2 , MoTe 2 , WS 2 , semimetallic ZrTe 2 , WTe 2 , and metallic NbS 2 , NbSe 2 using linearly and circularly polarized light with CW or CWmode-locked (ML) excitation lasers. For the semiconducting suspension of nanoflakes, excitation above and below the bandgap was performed. The results show that the intensity-dependent changes in the refractive index responsible for SSPM and associated ring formation are explained as arising from thermal origin. Measured values of the effective thermal nonlinear coefficient, n 2,th , range from ∼4.3 × 10 −7 to ∼4.2 × 10 −5 cm 2 /W, depending on the absorption strength of the suspension, and are independent of the optical excitation regime (polarization and laser mode of operation). The use of circularly polarized light to obtain the same results as seen with linearly polarized light is fundamental to complement the results, demonstrating that at the spectro-temporal regimes studied, thermal nonlinearity explains well the ring formation, in addition to providing the original SSPM results for NbS 2 , ZrTe 2 , and WTe 2 .

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Section: Methodsmentioning

confidence: 99%

Section: ■ Conclusionmentioning

confidence: 99%

Intensity-Dependent Thermally Induced Nonlinear Optical Response of Two-Dimensional Layered Transition-Metal Dichalcogenides in Suspension

et al. 2023

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“…Two-dimensional (2D) transition metal dichalcogenides (TMDCs) are amenable to large scale liquid phase exfoliation and exhibit distinct quantum optical properties compared to bulk analogs (i.e., bulk optical properties being observed at ≥10 layers 1 ). Exemplary 2D TMDC optical interactions include excitonic effects [2][3][4][5] , exciton quantum confinement 1,6,7 , charge transfer effects 8 , electric field screening 9 , quantum nonlinear effects [10][11][12][13] , and dopant-induced screening offering tailorable optical properties 14 . These representative phenomena constitute fundamental implications toward the pending design and development of lowdimensional high-performance nanophotonic devices such as perfect absorbers, tunable mirrors, and single-photon emitters or detectors.…”

Section: Introductionmentioning

confidence: 99%

Exfoliation procedure-dependent optical properties of solution deposited MoS2 films

et al. 2023

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The development of high-precision large-area optical coatings and devices comprising low-dimensional materials hinges on scalable solution-based manufacturability with control over exfoliation procedure-dependent effects. As such, it is critical to understand the influence of technique-induced transition metal dichalcogenide (TMDC) optical properties that impact the design, performance, and integration of advanced optical coatings and devices. Here, we examine the optical properties of semiconducting MoS2 films from the exfoliation formulations of four prominent approaches: solvent-mediated exfoliation, chemical exfoliation with phase reconversion, redox exfoliation, and native redox exfoliation. The resulting MoS2 films exhibit distinct refractive indices (n), extinction coefficients (k), dielectric functions (ε1 and ε2), and absorption coefficients (α). For example, a large index contrast of Δn ≈ 2.3 is observed. These exfoliation procedures and related chemistries produce different exfoliated flake dimensions, chemical impurities, carrier doping, and lattice strain that influence the resulting optical properties. First-principles calculations further confirm the impact of lattice defects and doping characteristics on MoS2 optical properties. Overall, incomplete phase reconfiguration (from 1T to mixed crystalline 2H and amorphous phases), lattice vacancies, intraflake strain, and Mo oxidation largely contribute to the observed differences in the reported MoS2 optical properties. These findings highlight the need for controlled technique-induced effects as well as the opportunity for continued development of, and improvement to, liquid phase exfoliation methodologies. Such chemical and processing-induced effects present compelling routes to engineer exfoliated TMDC optical properties toward the development of next-generation high-performance mirrors, narrow bandpass filters, and wavelength-tailored absorbers.

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“…While most previous studies of these nonlinear optical properties have focused on TMDs prepared through bottom-up approaches, solution-phase preparation of TMDs offers the advantage of easy integration with existing manufacturing technologies. Redox-exfoliation of TMDs provides a low-cost, scalable method to generate colloidally stable few-layer and monolayer TMDs with generality and high yield. , However, few studies thus far have examined the linear and nonlinear optical properties of redox-exfoliated TMDs. − As we demonstrate in this study, the POM clusters produced during the redox-exfoliation process have a profound effect on the nonlinear optical properties of TMDs. As a result, redox-exfoliated TMDs of MoS 2 and WS 2 exhibit saturable SHG and high-order multiphoton photoluminescence (MPPL) as demonstrated in this work.…”

Section: Introductionmentioning

confidence: 99%

Tenth-Order Multiphoton Excitation and Saturable Second Harmonic Generation in Polyoxometalate-Exfoliated Molybdenum Disulfide

et al. 2022

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Nanomaterials are promising alternatives to traditional bulk crystals for nonlinear optics and energy conversion materials. In this study, we report the observation of saturable second harmonic generation and high-order (up to 10th) multiphoton photoluminescence in colloidal MoS2 nanoflakes prepared by redox exfoliation which generates polyoxometalate clusters. Fourier transform nonlinear optical spectroscopy enabled the resolution of these high-order signals through two-dimensional nonlinear excitation/detection correlation spectra. Complementary modeling of the nonlinear interferograms suggested mechanisms for the observed high-order signals, which involve saturation of transitions resonant with the harmonic energy and multiple competing orders of multiphoton absorption. The saturable second harmonic generation and high-order multiphoton photoluminescence, which were not observed in MoS2 prepared by chemical vapor deposition, are related to the formation of polyoxometalate clusters during the redox exfoliation process. Further studies demonstrated that polyoxometalates can induce high-order nonlinear optical effects in other colloidal semiconductors with resonances at the harmonic energy, suggesting a general route to drastically alter the nonlinear optical response of nanomaterials with molecular adsorbates. This response is due in part to the interfacial charge transfer between polyoxometalate species and the nanomaterial. Fourier transform nonlinear optical spectroscopy offers a route to resolving the effects of molecular adsorbates, which are obscured in traditional nonlinear optical measurements.

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Femtosecond nonlinear refraction of 2D semi-metallic redox exfoliated ZrTe2 at 800 nm

Cited by 14 publications

References 28 publications

Intensity-Dependent Thermally Induced Nonlinear Optical Response of Two-Dimensional Layered Transition-Metal Dichalcogenides in Suspension

Intensity-Dependent Thermally Induced Nonlinear Optical Response of Two-Dimensional Layered Transition-Metal Dichalcogenides in Suspension

Exfoliation procedure-dependent optical properties of solution deposited MoS2 films

Tenth-Order Multiphoton Excitation and Saturable Second Harmonic Generation in Polyoxometalate-Exfoliated Molybdenum Disulfide

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