Organometallic Complexes for Non-linear Optics. 49.* Third-Order Non-linear Optical Spectral Dependence Studies of Arylalkynylruthenium Dendrimers

2011 ◽  
Vol 64 (9) ◽  
pp. 1269 ◽  
Author(s):  
Marek Samoc ◽  
T. Christopher Corkery ◽  
Andrew M. McDonagh ◽  
Marie P. Cifuentes ◽  
Mark G. Humphrey

The cubic hyperpolarizabilities of 1,3,5-(trans-[RuCl(dppe)2(C≡CC6H4-4-C≡C)])3C6H3 (1), 1,3,5-(trans-[Ru(C≡CPh)(dppe)2(C≡CC6H4-4-C≡C)])3C6H3 (2), 1,3,5-(trans-[Ru(C≡CC6H4-4-NO2)(dppe)2(C≡CC6H4-4-C≡C)])3C6H3 (3), 1,3,5-{trans-[Ru(C≡C-3,5-(trans-[Ru(C≡CPh)(dppe)2(C≡CC6H4-4-C≡C)])2C6H3)(dppe)2(C≡CC6H4-4-C≡C)]}3C6H3 (4), and 1,3,5-{trans-[Ru(C≡C-3,5-(trans-[Ru(C≡CC6H4-4-NO2)(dppe)2(C≡CC6H4-4-C≡C)])2C6H3)(dppe)2(C≡CC6H4-4-C≡C)]}3C6H3 (5) have been assessed over the spectral range 520–1600 nm using the Z-scan technique and ~150 fs pulses. All complexes exhibit negative values of γreal (corresponding to self-defocusing behaviour) and significant positive values of γimag (corresponding to two-photon absorption) at short wavelengths (up to 1000 nm). The maximal values of γreal and γimag increase in magnitude on dendrimer generation increase (proceeding from 2 to 4 or 3 to 5). The open-aperture Z-scan results have been used to confirm and contrast the two-photon (2PA) and three-photon absorption (3PA) behaviour of 1–5, the data being consistent with the existence of 2PA at the short wavelength range, but with significant 3PA at longer wavelengths for 1–3 and 5, a record 3PA coefficient for an inorganic complex for 5 at 1180 nm, and appreciable 3PA at the telecommunications wavelength of 1300 nm.

2012 ◽  
Vol 65 (7) ◽  
pp. 834 ◽  
Author(s):  
Adam Barlow ◽  
Bandar Babgi ◽  
Marek Samoc ◽  
T. Christopher Corkery ◽  
Stijn van Cleuvenbergen ◽  
...  

The alkynes HC≡CC6H2-2,6-Et2-4-C≡CC6H4-4-NO2 (4) and HC≡CC6H4-4-C≡CC6H2-2,6-Et2-4-C≡CC6H4-4-NO2 (6) and gold alkynyl complexes Au{C≡CC6H2-2,5-(OEt)2-4-C≡CC6H4-4-NO2}(PPh3) (7), Au(C≡CC6H2-2,6-Et2-4-C≡CC6H4-4-NO2)(PPh3) (8), and Au(C≡CC6H4-4-C≡CC6H2-2,6-Et2-4-C≡CC6H4-4-NO2)(PPh3) (9) have been synthesized. The linear optical properties and quadratic optical non-linearities of 7–9 have been measured, the latter by hyper-Rayleigh scattering at 1064 nm, and compared with data for the previously reported complexes Au(C≡CC6H4-4-NO2)(PPh3) (10) and Au(C≡CC6H4-4-C≡CC6H4-4-NO2)(PPh3) (11). The optical absorption maximum red-shifts and the first hyperpolarizabilities increase on π-system lengthening and on introduction of electron-releasing substituents on the π-bridge ring adjacent to the metal centre. The cubic non-linear optical properties of 1,4-{(PCy3)Au(C≡C)}2C6H4 (12) and {(PCy3)Au(C≡C-4-C6H4C≡C)}6C6 (13) have been assessed by wide spectroscopic range femtosecond Z-scan studies; the maximal values of the imaginary component and the effective two-photon absorption cross-section increase markedly on proceeding from linear complex 12 to 6-fold-symmetric complex 13, an increase that is maintained when data are scaled by relative molecular weight.


Symmetry ◽  
2021 ◽  
Vol 13 (1) ◽  
pp. 153 ◽  
Author(s):  
Christophe Humbert ◽  
Thomas Noblet

To take advantage of the singular properties of matter, as well as to characterize it, we need to interact with it. The role of optical spectroscopies is to enable us to demonstrate the existence of physical objects by observing their response to light excitation. The ability of spectroscopy to reveal the structure and properties of matter then relies on mathematical functions called optical (or dielectric) response functions. Technically, these are tensor Green’s functions, and not scalar functions. The complexity of this tensor formalism sometimes leads to confusion within some articles and books. Here, we do clarify this formalism by introducing the physical foundations of linear and non-linear spectroscopies as simple and rigorous as possible. We dwell on both the mathematical and experimental aspects, examining extinction, infrared, Raman and sum-frequency generation spectroscopies. In this review, we thus give a personal presentation with the aim of offering the reader a coherent vision of linear and non-linear optics, and to remove the ambiguities that we have encountered in reference books and articles.


2002 ◽  
Vol 209 (4-6) ◽  
pp. 461-466 ◽  
Author(s):  
I. Fuks-Janczarek ◽  
J-M. Nunzi ◽  
B. Sahraoui ◽  
I.V. Kityk ◽  
J. Berdowski ◽  
...  

2018 ◽  
Vol 8 (10) ◽  
pp. 1810 ◽  
Author(s):  
Rihan Wu ◽  
Jack Collins ◽  
Leigh Canham ◽  
Andrey Kaplan

We present an experimental investigation into the third-order nonlinearity of conventional crystalline (c-Si) and porous (p-Si) silicon with Z-scan technique at 800-nm and 2.4- μ m wavelengths. The Gaussian decomposition method is applied to extract the nonlinear refractive index, n 2 , and the two-photon absorption (TPA) coefficient, β , from the experimental results. The nonlinear refractive index obtained for c-Si is 7 ± 2 × 10 − 6 cm 2 /GW and for p-Si is − 9 ± 3 × 10 − 5 cm 2 /GW. The TPA coefficient was found to be 2.9 ± 0.9 cm/GW and 1.0 ± 0.3 cm/GW for c-Si and p-Si, respectively. We show an enhancement of the nonlinear refraction and a suppression of TPA in p-Si in comparison to c-Si, and the enhancement gets stronger as the wavelength increases.


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