https://www.rowland.harvard.edu/rjf/fischer/images/chirality_17_421.pdf

Nonlinear optical spectroscopy of chiral molecules.

The past decade has witnessed the emergence of new measurement approaches and applications for chiral thin films and materials enabled by the observations of the high sensitivity of second-order nonlinear optical measurements to chirality. In thin films, the chiral response to second harmonic generation and sum frequency generation (SFG) from a single molecular monolayer is often comparable with the achiral response. The chiral specificity also allows for symmetry-allowed SFG in isotropic chiral media, confirming predictions made ∼50 years ago. With these experimental demonstrations in hand, an important challenge is the construction of intuitive predictive models that allow the measured chiral response to be meaningfully related back to molecular and macromolecular structure. This review defines and considers three distinct mechanisms for chiral effects in uniaxially oriented assemblies: orientational chirality, intrinsic chirality, and isotropic chirality. The role of each is discussed in experimental and computational studies of bacteriorhodopsin films, binaphthol, and collagen. Collectively, these three model systems support a remarkably simple framework for quantitatively recovering the measured chiral-specific activity.

Chirality in nonlinear optics.

We performed Hyper−Rayleigh Scattering (HRS) experiments to measure the second-order nonlinear optical response of the collagen triple helix and determine the physical origin of second harmonic signals observed in collagenous tissues. HRS experiments yielded a second-order hyperpolarizability of 1.25 × 10−27 esu for rat-tail type I collagen, a surprisingly large value considering that collagen presents no strong harmonophore in its amino acid sequence. Polarization-resolved experiments showed intramolecular coherent contributions to the HRS signal along with incoherent contributions that are the only contributions for molecules with dimensions much smaller than the excitation wavelength. We therefore modeled the effective second-order hyperpolarizability of the 290 nm long collagen triple helix by summing coherently the nonlinear response of well-aligned moieties along the triple helix axis. This model was confirmed by HRS measurements after denaturation of the collagen triple helix and for a collagen-lik...

Measurement of the Second-Order Hyperpolarizability of the Collagen Triple Helix and Determination of Its Physical Origin

The general failure of Kleinman symmetry in practical nonlinear optical applications

A very sensitive experimental setup for accurate wavelength-dependent hyper-Rayleigh scattering (HRS) measurements of the molecular first hyperpolarizability β in the broad fundamental wavelength range of 600 to 1800 nm is presented. The setup makes use of a stable continuously tunable picosecond optical parametric amplifier with kilohertz repetition rate. To correct for multi-photon fluorescence, a small spectral range around the second harmonic wavelength is detected in parallel using a spectrograph coupled to an intensified charge-coupled device. Reliable calibration against the pure solvent is possible over the full accessible spectral range. An extensive set of wavelength-dependent HRS calibration data for a wide range of solvents is presented, and very accurate measurements of the β dispersion of the well-known nonlinear optical chromophore Disperse Red 1 are demonstrated.

/pdf/highly-sensitive-setup-for-tunable-wavelength-hyper-rayleigh-20hfmo7jbj.pdf

Highly sensitive setup for tunable wavelength hyper-Rayleigh scattering with parallel detection and calibration data for various solvents

We describe improvements to a previously reported hyper-Rayleigh scattering technique [J. Opt. Soc. Am. B15, 289 (1998) ], for measuring all rotational invariants of the first hyperpolarizability tensor. The full hyper-Rayleigh scattering tensor is expressed in terms of its rotationally invariant components leading to a figures of merit corresponding to each of the rotationally invariant tensors. With elliptically polarized incident light, the polarization state and the intensity of the harmonic light are measured at a scattering angle of 45°. A new analytical fitting method is applied to the signal for two polarization measurements to yield the invariants. We have measured several chiral and nonchiral chromophores to determine the hyperpolarizability tensor with which to analyze the measurement accuracy, to reveal structure property relationships, and to assess the applicability of the chromophores as nonlinear optical materials. Results for a series of chiral chromophores and for Crystal Violet are presented.

Measurements of the hyperpolarizability tensor by means of hyper-Rayleigh scattering

Optimization of the molecular hyperpolarizability for second harmonic generation in chiral media

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Measurements of the hyperpolarizability tensor by means of hyper-Rayleigh scattering

Optimization of the molecular hyperpolarizability for second harmonic generation in chiral media