Publications | Max Planck Institute for Intelligent Systems

Nonlinear optical spectroscopy of chiral molecules

Fischer, P., Hache, F.

CHIRALITY, 17(8):421-437, 2005 (article)

Abstract

We review nonlinear optical processes that are specific to chiral molecules in solution and on surfaces. In contrast to conventional natural optical activity phenomena, which depend linearly on the electric field strength of the optical field, we discuss how optical processes that are nonlinear (quadratic, cubic, and quartic) functions of the electromagnetic field strength may probe optically active centers and chiral vibrations. We show that nonlinear techniques open entirely new ways of exploring chirality in chemical and biological systems: The cubic processes give rise to nonlinear circular dichroism and nonlinear optical rotation and make it possible to observe dynamic chiral processes at ultrafast time scales. The quadratic second-harmonic and sum-frequency-generation phenomena and the quartic processes may arise entirely in the electric-dipole approximation and do not require the use of circularly polarized light to detect chirality: They provide surface selectivity and their observables can be relatively much larger than in linear optical activity. These processes also give rise to the generation of light at a new color, and in liquids this frequency conversion only occurs if the solution is optically active. We survey recent chiral nonlinear optical experiments and give examples of their application to problems of biophysical interest. (C) 2005 Wiley-Liss, Inc.

pf Fischer, P., Hache, F. Nonlinear optical spectroscopy of chiral molecules CHIRALITY, 17(8):421-437, 2005 (article)

Negative refraction at optical frequencies in nonmagnetic two-component molecular media

Chen, Y., Fischer, P., Wise, F.

PHYSICAL REVIEW LETTERS, 95(6), 2005 (article)

Abstract

There is significant motivation to develop media with negative refractive indices at optical frequencies, but efforts in this direction are hampered by the weakness of the magnetic response at such frequencies. We show theoretically that a nonmagnetic medium with two atomic or molecular constituents can exhibit a negative refractive index. A negative index is possible even when the real parts of both the permittivity and permeability are positive. This surprising result provides a route to isotropic negative-index media at optical frequencies.

pf Chen, Y., Fischer, P., Wise, F. Negative refraction at optical frequencies in nonmagnetic two-component molecular media PHYSICAL REVIEW LETTERS, 95(6), 2005 (article)

A dynamical systems approach to learning: a frequency-adaptive hopper robot

Buchli, J., Righetti, L., Ijspeert, A.

In Proceedings of the VIIIth European Conference on Artificial Life ECAL 2005, pages: 210-220, Springer Verlag, 2005 (inproceedings)

mg Buchli, J., Righetti, L., Ijspeert, A. A dynamical systems approach to learning: a frequency-adaptive hopper robot In Proceedings of the VIIIth European Conference on Artificial Life ECAL 2005, pages: 210-220, Springer Verlag, 2005 (inproceedings)

From Dynamic Hebbian Learning for Oscillators to Adaptive Central Pattern Generators

Righetti, L., Buchli, J., Ijspeert, A.

In Proceedings of 3rd International Symposium on Adaptive Motion in Animals and Machines – AMAM 2005, Verlag ISLE, Ilmenau, 2005 (inproceedings)

mg Righetti, L., Buchli, J., Ijspeert, A. From Dynamic Hebbian Learning for Oscillators to Adaptive Central Pattern Generators In Proceedings of 3rd International Symposium on Adaptive Motion in Animals and Machines – AMAM 2005, Verlag ISLE, Ilmenau, 2005 (inproceedings)

2004

Operating system support for interface virtualisation of reconfigurable coprocessors

Vuletic, M., Righetti, L., Pozzi, L., Ienne, P.

In In Proceedings of the Design, Automation and Test in Europe Conference and Exhibition, pages: 748-749, IEEE, Paris, France, 2004 (inproceedings)

Abstract

Reconfigurable systems-on-chip (SoC) consist of large field programmable gate arrays (FPGAs) and standard processors. The reconfigurable logic can be used for application-specific coprocessors to speedup execution of applications. The widespread use is limited by the complexity of interfacing software applications with coprocessors. We present a virtualization layer that lowers the interfacing complexity and improves the portability. The layer shifts the burden of moving data between processor and coprocessor from the programmer to the operating system (OS). A reconfigurable SoC running Linux is used to prove the concept.

2004

mg Vuletic, M., Righetti, L., Pozzi, L., Ienne, P. Operating system support for interface virtualisation of reconfigurable coprocessors In In Proceedings of the Design, Automation and Test in Europe Conference and Exhibition, pages: 748-749, IEEE, Paris, France, 2004 (inproceedings)

2003

New electro-optic effect: Sum-frequency generation from optically active liquids in the presence of a dc electric field

Fischer, P., Buckingham, A., Beckwitt, K., Wiersma, D., Wise, F.

PHYSICAL REVIEW LETTERS, 91(17), 2003 (article)

Abstract

We report the observation of sum-frequency signals that depend linearly on an applied electrostatic field and that change sign with the handedness of an optically active solute. This recently predicted chiral electro-optic effect exists in the electric-dipole approximation. The static electric field gives rise to an electric-field-induced sum-frequency signal (an achiral third-order process) that interferes with the chirality-specific sum-frequency at second order. The cross-terms linear in the electrostatic field constitute the effect and may be used to determine the absolute sign of second- and third-order nonlinear-optical susceptibilities in isotropic media.

2003

pf Fischer, P., Buckingham, A., Beckwitt, K., Wiersma, D., Wise, F. New electro-optic effect: Sum-frequency generation from optically active liquids in the presence of a dc electric field PHYSICAL REVIEW LETTERS, 91(17), 2003 (article)

Chiral and achiral contributions to sum-frequency generation from optically active solutions of binaphthol

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

JOURNAL OF PHYSICAL CHEMISTRY A, 107(40):8232-8238, 2003 (article)

Abstract

The nonlinear sum- and difference-frequency generation spectroscopies can be probes of molecular chirality in optically active systems. We present a tensorial analysis of the chirality-specific electric-dipolar sum-frequency-generation susceptibility and the achiral electric-quadrupolar and magnetic-dipolar nonlinearities at second order in isotropic media. The chiral and achiral contributions to the sum-frequency signal from the bulk of optically active solutions of 1,1'-bi-2-naphthol (2,2'-dehydroxy-1,1'-binaphthyl) can be distinguished, and the former dominates. Ab initio computations reveal the dramatic resonance enhancement that the isotropic component of the electric-dipolar three-wave mixing hyperpolarizability experiences. Away from resonance its magnitude rapidly decreases, as-unlike the vector component-it is zero in the static limit. The dispersion of the first hyperpolarizability is computed by a configuration interaction singles sum-over-states approach with explicit regard to the Franck-Condon active vibrational substructure for all resonant electronic states.

pf Fischer, P., Wise, F., Albrecht, A. Chiral and achiral contributions to sum-frequency generation from optically active solutions of binaphthol JOURNAL OF PHYSICAL CHEMISTRY A, 107(40):8232-8238, 2003 (article)

Evolution of Fault-tolerant Self-replicating Structures

Righetti, L., Shokur, S., Capcarre, M.

In Advances in Artificial Life, pages: 278-288, Lecture Notes in Computer Science, Springer Berlin Heidelberg, 2003 (inproceedings)

Abstract

Designed and evolved self-replicating structures in cellular automata have been extensively studied in the past as models of Artificial Life. However, CAs, unlike their biological counterpart, are very brittle: any faulty cell usually leads to the complete destruction of any emerging structures, let alone self-replicating structures. A way to design fault-tolerant structures based on error-correcting-code has been presented recently [1], but it required a cumbersome work to be put into practice. In this paper, we get back to the original inspiration for these works, nature, and propose a way to evolve self-replicating structures, faults here being only an idiosyncracy of the environment.

mg Righetti, L., Shokur, S., Capcarre, M. Evolution of Fault-tolerant Self-replicating Structures In Advances in Artificial Life, pages: 278-288, Lecture Notes in Computer Science, Springer Berlin Heidelberg, 2003 (inproceedings)