Perturbation theory of the non-linear optical polarization of an isolated system

Orr, Brian J.; Ward, John F.

doi:10.1080/00268977100100481

Cited by 1,312 publications

(654 citation statements)

References 24 publications

Supporting

Mentioning

644

Contrasting

Unclassified

Order By: Relevance

“…where |g = |G |0 is the global ground state, |f is an excited state, Ω f g = ω f g − iΓ f is the complex frequency of the f ← g transition, defined in terms of the real transition frequency (ω f g ) and of the damping factor of the f state (Γ f ) 25 . The summation in the above equation runs on all excitations, including vibrational excitations (in the G-manifold) as well as vibronic excitations (in the E-manifold).…”

Section: Tpa Spectra Of the Da Dimer With Holstein Couplingmentioning

confidence: 99%

Vibronic contributions to resonant NLO responses: two-photon absorption in push–pull chromophores

Painelli

Freo

Terenziani

2001

Chemical Physics Letters

View full text Add to dashboard Cite

Section: Tpa Spectra Of the Da Dimer With Holstein Couplingmentioning

confidence: 99%

Vibronic contributions to resonant NLO responses: two-photon absorption in push–pull chromophores

Painelli

Freo

Terenziani

2001

Chemical Physics Letters

View full text Add to dashboard Cite

“…We now focus on the linear and nonlinear optical properties of H-silsesquioxanes and report the results of calculations based on a combination of the intermediate neglect of differential overlap (INDO) and the configuration interaction (CI) methods coupled with sum-overstates (SOS) method. 9,10 This approach is demonstrated to be successful in calculating the optical properties of organometallic compounds and inorganic solid compounds. 11,12 To our knowledge, however, experimental or theoretical investigations of optical properties have not yet been reported for this class of polymers.…”

Section: Introductionmentioning

confidence: 99%

Calculations of Linear and Nonlinear Optical Properties of H−Silsesquioxanes

et al. 2000

View full text Add to dashboard Cite

We report the frequency dependence of linear and nonlinear optical susceptibilities of H-silsesquioxanes of various cage sizes and conformations using the INDO/CI method coupled with the SOS method. The average dynamic refractive index of silsesquioxanes is found to decrease as the cage size increases, and its variation is very small for the different conformations of the same cage size at the same incident wavelength. The calculated second-order susceptibilities show that small cages have a larger magnitude which is comparable to that of crystalline R-quartz. It is suggested here that H-silsesquioxanes of a smaller cage size can be a good candidate materials for nonlinear optical applications having low absorption, wide transparency and adequate susceptibility in ultraviolet or vacuum ultraviolet region of the spectrum.

show abstract

“…We carried out sum-over-state calculations, [37] in combination with Thomas-Kuhn sum rules analysis [38,39] to estimate the relevant values of b(À2w,w,w) and g(À2w,w,w,0), where w is the photon frequency for JR1 and di-4-ANEPPS at the wavelength of our experiments (850 nm; see the Supporting Information). These two molecules have similar b values at 850 nm, whereas g is substantially larger in the porphyrin dye, thus giving calculated field sensitivities of DS/S of 5.5 % for Table 1.…”

Section: Methodsmentioning

confidence: 99%

Porphyrins for Probing Electrical Potential Across Lipid Bilayer Membranes by Second Harmonic Generation

et al. 2013

View full text Add to dashboard Cite

Neurons communicate by using electrical signals, mediated by transient changes in the voltage across the plasma membrane. Optical techniques for visualizing these transmembrane potentials could revolutionize the field of neurobiology by allowing the spatial profile of electrical activity to be imaged in real time with high resolution, along individual neurons or groups of neurons within their native networks. [1,2] Second harmonic generation (SHG) is one of the most promising methods for imaging membrane potential, although so far this technique has only been demonstrated with a narrow range of dyes. [3] Here we show that SHG from a porphyrin-based membrane probe gives a fast electro-optic response to an electric field which is about 5-10 times greater than that of conventional styryl dyes. Our results indicate that porphyrin dyes are promising probes for imaging membrane potential.Studies of excitable cells, such as neurons and cardiac myocytes, require new methods for mapping changes in membrane potential, ideally with a voltage resolution of about 1 mV, a time resolution of 1 ms, and a spatial resolution of 1 mm. [1,2] Microelectrodes can be used to measure transmembrane potentials with excellent sensitivity and temporal resolution, but they do not provide subcellular spatial resolution. Fluorescent calcium indicators are widely used to probe membrane potential indirectly, through the intracellular Ca 2+ concentration. However, changes in calcium concentration do not accurately reflect voltage transients. [4] Fluorescent voltage-sensitive dyes were first developed 30 years ago, [5] and recent advances in the molecular design of these dyes [6][7][8][9][10] have made it possible to track the spatial evolution of action potentials. [11][12][13][14] Compared with fluorescence, SHG imaging has several advantages as a technique for probing membrane potential: [3,[15][16][17][18][19][20][21] SHG has a greater intrinsic sensitivity to electric fields than fluorescence, [19][20][21] and it is only produced by noncentrosymmetric molecules in noncentrosymmetric environments, thus making it ideal for probing interfaces such as lipid bilayers. Similar to twophoton-excited fluorescence, SHG is a two-photon nonlinear optical effect, and it brings the advantages of depth penetration associated with multiphoton microscopy. [22] The main disadvantage of SHG is that it often gives lower intensity than fluorescence; there is a need for the design of brighter, more voltage-sensitive SHG dyes. [3,23] Styryl dyes and retinal chromophores have been shown to exhibit voltage-sensitive SHG when localized in plasma membranes, [15,24] and the voltage sensitivity of their SHG is greater than that of their fluorescence. [19][20][21] Recently we reported that amphiphilic porphyrins such as JR1 exhibit strong SHG when localized in lipid membranes. [25] Here we compare the voltage sensitivity of the SHG from JR1 with that from three widely studied styryl dyes (FM4-64, di-4-ANEPPS, and RH237) in hemispherical lipid bilayers (HLBs). [15,26,27] ...

show abstract

Perturbation theory of the non-linear optical polarization of an isolated system

Cited by 1,312 publications

References 24 publications

Vibronic contributions to resonant NLO responses: two-photon absorption in push–pull chromophores

Vibronic contributions to resonant NLO responses: two-photon absorption in push–pull chromophores

Calculations of Linear and Nonlinear Optical Properties of H−Silsesquioxanes

Porphyrins for Probing Electrical Potential Across Lipid Bilayer Membranes by Second Harmonic Generation

Contact Info

Product

Resources

About