Header logo is


2012


Fourier-transform photocurrent spectroscopy using a supercontinuum light source
Fourier-transform photocurrent spectroscopy using a supercontinuum light source

Petermann, C., Beigang, R., Fischer, P.

APPLIED PHYSICS LETTERS, 100(6), 2012 (article)

Abstract
We demonstrate an implementation of frequency-encoded photocurrent spectroscopy using a super-continuum light source. The spectrally broad light is spatially dispersed and modulated with a special mechanical chopper design that permits a continuous wavelength-dependent modulation. After recombination, the light beam contains a frequency encoded spectrum which enables us to map the spectral response of a given sample in 60 ms and with a lateral resolution of 10 mu m. (C) 2012 American Institute of Physics.

DOI [BibTex]

2012

DOI [BibTex]


Eine neue Form von Cavity Enhanced Absorption Spectroscopy
Eine neue Form von Cavity Enhanced Absorption Spectroscopy

Petermann, C., Fischer, P.

DE Gruyter, 79(1), 2012, Best paper award OPTO 2011 (article)

Abstract
Wir stellen eine Kopplungsmethode für resonatorgestützte Absorptionsmessungen vor, bei der Licht durch einen im Resonator platzierten akustooptischen Modulator aktiv ein- und ausgekoppelt wird. Dies ermöglicht es Cavity-Ring-Down-Spektroskopie (CRDS) mit breitbandigen und zeitlich inkohärenten Lichtquellen niedriger spektraler Leistungsdichte durchzuführen. Das Verfahren wird zum ersten Mal mit einer breitbandigen Superkontinuum-Quelle demonstriert.

___________________________________________________________________________________________

A new coupling scheme for cavity enhanced absorption spectroscopy makes use of an intracavity acousto-optical modulator to actively switch light into (and out of) a resonator. This allows cavity ringdown spectroscopy (CRDS) to be implemented with broadband temporally incoherent light sources with low spectral power densities. The method is demonstrated for the first time using a broadband supercontinuum source. Best paper award OPTO 2011.

link (url) [BibTex]

link (url) [BibTex]

2002


Chirality-specific nonlinear spectroscopies in isotropic media
Chirality-specific nonlinear spectroscopies in isotropic media

Fischer, P., Albrecht, A.

BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN, 75(5):1119-1124, 2002, 10th International Conference on Time-Resolved Vibrational Spectroscopy (TRVS 2001), OKAZZAKI, JAPAN, MAY 21-25, 2001 (article)

Abstract
Sum or difference frequency generation (SFG or DFG) in isotropic media is in the electric-dipole approximation only symmetry allowed for optically active systems. The hyperpolarizability giving rise to these three-wave mixing processes features only one isotropic component. It factorizes into two terms, an energy (denominator) factor and a triple product of transition moments. These forbid degenerate SFG, i.e., second harmonic generation, as well as the existence of the linear electrooptic effect (Pockels effect) in isotropic media. This second order response also has no static limit, which leads to particularly strong resonance phenomena that are qualitatively different from those usually seen in the ubiquitous even-wave mixing spectroscopies. In particular, the participation of two (not the usual one) excited states is essential to achieve dramatic resonance enhancement, We report our first efforts to see such resonantly enhanced chirality specific SFG.

DOI [BibTex]

2002

DOI [BibTex]


The chiral specificity of sum-frequency generation in solutions
The chiral specificity of sum-frequency generation in solutions

Fischer, P., Beckwitt, K., Wise, F., Albrecht, A.

CHEMICAL PHYSICS LETTERS, 352(5-6):463-468, 2002 (article)

Abstract
Sum-frequency generation in isotropic media is in the electric-dipole approximation the only symmetry allowed for chiral systems. We demonstrate that the sum-frequency intensity from an optically active liquid depends quadratically on the difference in concentration of the two enantiomers. The dominant contribution to the signal is found to be due to the chirality specific electric-dipolar three-wave mixing nonlinearity. Selecting the polarization of all fields allows the chiral electric-dipolar contributions to the bulk sum-frequency signal to be discerned from any achiral magnetic-dipolar and electric-quadrupolar contributions. (C) 2002 Published by Elsevier Science B.V.

DOI [BibTex]

DOI [BibTex]


On optical rectification in isotropic media
On optical rectification in isotropic media

Fischer, P., Albrecht, A.

LASER PHYSICS, 12(8):1177-1181, 2002 (article)

Abstract
Coherent nonlinear optical processes at second-order are only electric-dipole allowed in isotropic media that are optically active. Sum-frequency generation in chiral liquids has recently been observed, and difference-frequency and optical rectification have been predicted to exist in isotropic chiral media. Both Rayleigh-Schrodinger perturbation theory and the density matrix approach are used to discuss the quantum-chemical basis of optical rectification in optically active liquids. For pinene we compute the corresponding orientationally averaged hyperpolarizability, and estimate the light-induced dc electric polarization and the consequent voltage across a measuring capacitor it may give rise to near resonance.

[BibTex]

[BibTex]

2000


Phenomenological damping in optical response tensors
Phenomenological damping in optical response tensors

Buckingham, A., Fischer, P.

PHYSICAL REVIEW A, 61(3), 2000 (article)

Abstract
Although perturbation theory applied to the optical response of a molecule or material system is only strictly valid far from resonances, it is often applied to ``near-resonance{''} conditions by means of complex energies incorporating damping. Inconsistent signs of the damping in optical response tensors have appeared in the recent literature, as have errors in the treatment of the perturbation by a static held. The ``equal-sign{''} convention used in a recent publication yields an unphysical material response, and Koroteev's intimation that linear electro-optical circular dichroism may exist in an optically active liquid under resonance conditions is also flawed. We show that the isotropic part of the Pockels tensor vanishes.

DOI [BibTex]

2000

DOI [BibTex]


Ab initio investigation of the sum-frequency hyperpolarizability of small chiral molecules
Ab initio investigation of the sum-frequency hyperpolarizability of small chiral molecules

Champagne, B., Fischer, P., Buckingham, A.

CHEMICAL PHYSICS LETTERS, 331(1):83-88, 2000 (article)

Abstract
Using a sum-over-states procedure based on configuration interaction singles /6-311++G{*}{*}, we have computed the sum-frequency hyperpolarizability beta (ijk)(-3 omega; 2 omega, omega) Of two small chiral molecules, R-monofluoro-oxirane and R-(+)-propylene oxide. Excitation energies were scaled to fit experimental UV-absorption data and checked with ab initio values from time-dependent density functional theory. The isotropic part of the computed hyperpolarizabilities, beta(-3 omega; 2 omega, omega), is much smaller than that reported previously from sum-frequency generation experiments on aqueous solutions of arabinose. Comparison is made with a single-centre chiral model. (C) 2000 Elsevier Science B.V. All rights reserved.

DOI [BibTex]

DOI [BibTex]


Three-wave mixing in chiral liquids
Three-wave mixing in chiral liquids

Fischer, P., Wiersma, D., Righini, R., Champagne, B., Buckingham, A.

PHYSICAL REVIEW LETTERS, 85(20):4253-4256, 2000 (article)

Abstract
Second-order nonlinear optical frequency conversion in isotropic systems is only dipole allowed for sum- and difference-frequency generation in chiral media. We develop a single-center chiral model of the three-wave mixing (sum:frequency generation) nonlinearity and estimate its magnitude. We also report results from ab initio calculations and from three- and four-wave mixing experiments in support of the theoretical estimates. We show that the second-order susceptibility in chiral liquids is much smaller than previously thought.

DOI [BibTex]

DOI [BibTex]