2020
DOI: 10.1103/physrevb.102.235408
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Dispersion of the nonlinear susceptibility of MoS2 and WS2 from second-harmonic scattering spectroscopy

Abstract: Dispersion of the absolute second-order susceptibility of both MoS 2 and WS 2 is assessed on a wide spectral excitation range (710-1300 nm) by using second-harmonic scattering spectroscopy (SHS). SHS is an accurate ensemble measurement here applied on well-dispersed suspensions of monodisperse liquid-exfoliated nanosheets showing a high monolayer content. The as-derived, high susceptibility values shed light on the discrepancies between available literature values while evidencing resonances associated with th… Show more

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Cited by 10 publications
(12 citation statements)
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“…To quantify the optical nonlinearity of the nanocomposite, we first calibrated the SHG response using a monolayer 2H-WS 2 sample as a reference (a highly noncentrosymmetric material with high second-order nonlinear optical susceptibility) . Here, single crystal WS 2 is mechanically exfoliated onto the SiO 2 /Si substrate, and the second-order nonlinear optical susceptibility |χ (2) | is calculated to be ∼1.2 nm/V, showing good agreement with the previous experimental result. , SHG yield of our h-BN/c-BN nanocomposite is comparable to that of the monolayer 2H-WS 2 (Figure b), with an SHG intensity ratio P c‑BN/h‑BN : P WS2 ∼ 1:2. The effective interaction length of forward-propagating SHG inside the sample is d = 1 Δ k = λ S H G 2 π false( n S H G n p u m p false) ∼ 300 nm, where Δ k is the phase mismatch due to the difference in refractive indices (RI) at the pump ( n pump ) and SHG ( n SHG ) frequencies. , Thus, we estimate that the lower bound of the effective second-order nonlinear susceptibility |χ (2) | in the composite is about of ∼3 pm/V.…”
supporting
confidence: 80%
See 1 more Smart Citation
“…To quantify the optical nonlinearity of the nanocomposite, we first calibrated the SHG response using a monolayer 2H-WS 2 sample as a reference (a highly noncentrosymmetric material with high second-order nonlinear optical susceptibility) . Here, single crystal WS 2 is mechanically exfoliated onto the SiO 2 /Si substrate, and the second-order nonlinear optical susceptibility |χ (2) | is calculated to be ∼1.2 nm/V, showing good agreement with the previous experimental result. , SHG yield of our h-BN/c-BN nanocomposite is comparable to that of the monolayer 2H-WS 2 (Figure b), with an SHG intensity ratio P c‑BN/h‑BN : P WS2 ∼ 1:2. The effective interaction length of forward-propagating SHG inside the sample is d = 1 Δ k = λ S H G 2 π false( n S H G n p u m p false) ∼ 300 nm, where Δ k is the phase mismatch due to the difference in refractive indices (RI) at the pump ( n pump ) and SHG ( n SHG ) frequencies. , Thus, we estimate that the lower bound of the effective second-order nonlinear susceptibility |χ (2) | in the composite is about of ∼3 pm/V.…”
supporting
confidence: 80%
“…45 Here, single crystal WS 2 is mechanically exfoliated onto the SiO 2 /Si substrate, and the second-order nonlinear optical susceptibility |χ (2) | is calculated to be ∼1.2 nm/V, showing good agreement with the previous experimental result. 45,46 SHG yield of our h-BN/c-BN nanocomposite is comparable to that of the monolayer 2H-WS 2 (Figure 3b), with an SHG intensity ratio P c-BN/h-BN :P WS2 ∼ 1:2. The effective interaction length of forward-propagating SHG inside the sample is d = ∼ 300 nm, where Δk is the phase mismatch due to the difference in refractive indices (RI) at the pump (n pump ) and SHG (n SHG ) frequencies.…”
mentioning
confidence: 53%
“…[ 262–265 ] These bound excitons influence nonlinear light matter interactions. [ 41,209,266–268 ] For example, in 1L MoS 2 , significant enhancement in SHG and THG is found when in resonance with an A‐exciton [ 269 ] and a similar trend is noted for an SHG investigation with WS 2 . [ 270 ] The strong exciton effects in 2D materials due to large density of states increase the efficiency of generating OHG.…”
Section: Tuning Of Optical Harmonic Generation In 2d Layered Materialsmentioning
confidence: 77%
“…Note that we only used diluted samples to limit the absorption of the fundamental beam and reabsorption of the generated 2ω photons within the suspension. Moreover, the incident power was limited to 50 mW to prevent the occurrence of thermal lensing, which could induce self-defocusing of the fundamental beam, thereby modifying its intensity . We addressed both of these concerns in the Supporting Information.…”
Section: Resultsmentioning
confidence: 99%