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Faraday Discussions

Coherent control of the motion of complex molecules and the coupling to internal state dynamics

Paul Venn, Hendrik Ulbricht

Published Jan 1, 2011• 0 citations
Publisher

Abstract

We discuss coherent control of the centre of mass motion of complex molecules by de Broglie interferometry. We describe an experiment to couple the dynamics of internal state population of complex molecules to their centre of mass motion. We discuss how this can be used to probe state population and transition, especially the photo-switching of flourinated di-azobenzene molecules between their cis- and trans-configuration. We propose an experiment to photo-isomerise complex di-azobenzene molecules in the gas-phase, including the selective detection of molecules in different conformations. In addition we discuss possible ways of optimising the conformation detection through cooling, and optical techiques.

DOI
10.1039/c1fd00066g

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We discuss coherent control of the centre of mass motion of complex molecules by de Broglie interferometry. We describe an experiment to couple the dynamics of internal state population of complex molecules to their centre of mass motion. We discuss how this can be used to probe state population and transition, especially the photo-switching of flourinated di-azobenzene molecules between their cis- and trans-configuration. We propose an experiment to photo-isomerise complex di-azobenzene molecules in the gas-phase, including the selective detection of molecules in different conformations. In addition we discuss possible ways of optimising the conformation detection through cooling, and optical techiques.
The optical switching of molecular ensembles in a dissipative environment is a subject of various fields of chemical physics and physical chemistry. Here we try to switch arrays of molecules from a stable collective ground state to a state in which all molecules have been transferred to another stable higher-energy configuration. In our model switching proceeds through electronically excited intermediates which are coherently coupled to each other through dipolar interactions, and which decay incoherently within a finite lifetime by coupling to a dissipative environment. The model is quite general, but parameters are chosen to roughly resemble the all-trans $\ensuremath{\rightarrow}$ all-cis isomerization of an array of azobenzene molecules on a surface. Using analytical and optimal control pulses and the concept of ``laser distillation,'' we demonstrate that for various aggregates (dimers up to hexamers), controlled and complete switching should be possible.
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We describe the state of the art in preparing, manipulating and detecting coherent molecular matter. We focus on experimental methods for handling the quantum motion of compound systems from diatomic molecules to clusters or biomolecules.Molecular quantum optics offers many challenges and innovative prospects: already the combination of two atoms into one molecule takes several well-established methods from atomic physics, such as for instance laser cooling, to their limits. The enormous internal complexity that arises when hundreds or thousands of atoms are bound in a single organic molecule, cluster or nanocrystal provides a richness that can only be tackled by combining methods from atomic physics, chemistry, cluster physics, nanotechnology and the life sciences.We review various molecular beam sources and their suitability for matter-wave experiments. We discuss numerous molecular detection schemes and give an overview over diffraction and interference experiments that have already been performed with molecules or clusters.Applications of de Broglie studies with composite systems range from fundamental tests of physics up to quantum-enhanced metrology in physical chemistry, biophysics and the surface sciences.Nanoparticle quantum optics is a growing field, which will intrigue researchers still for many years to come. This review can, therefore, only be a snapshot of a very dynamical process.
Optics and interferometry with matter waves is the art of coherently manipulating the translational motion of particles like neutrons, atoms and molecules. Coherent atom optics is an extension of techniques that were developed for manipulating \emph{internal} quantum states. Applying these ideas to translational motion required the development of techniques to localize atoms and transfer population coherently between distant localities. In this view position and momentum are (continuouse) quantum mechanical degree of freedom analogous to discrete internal quantum states. In our contribution we start with an introduction into matter-wave optics in section 1, discuss coherent atom optics and atom interferometry techniques for molecular beams in section 2 and for trapped atoms in section 3. In section 4 we then describe tools and experiments that allow us to probe the evolution of quantum states of many-body systems by atom interference.
Abstract Rather different problems can be lumped together under the general term 'laser control of atoms and molecules'. They include the laser selection of atomic and molecular velocities for the purpose of Doppler-free spectroscopy, laser control of the position and velocity of atoms (i.e. laser trapping and cooling of atoms), and laser control of atomic and molecular processes (ionization, dissociation) with a view of detecting single atoms and molecules and particularly separating isotopes and nuclear isomers. Over the last decades the principal problems posed have been successfully solved, and many of them have evolved remarkably in the subsequent investigations of the international research community. For example, the solution of the problem of laser cooling and trapping of atoms has given birth to the new field of the physics of ultracold matter, i.e. quantum atomic and molecular gases. The laser non-coherent control of uni-molecular processes has found an interesting extension in the field of laser coherent control of molecules. The concept of laser control of position has been successfully demonstrated with microparticles (optical tweezers), concurrently with investigations into atomic control. The laser photo-ionization of molecules on surfaces has led to the development of novel techniques of laser-assisted mass spectrometry of macromolecules, and so on. The aim of this book is to review these topics from a unified or 'coherent' point of view. It will be useful for many readers in various fields of laser science and its applications.
We investigate the influence of thermally activated internal molecular dynamics on the phase shifts of matter waves inside a molecule interferometer. While de Broglie physics generally describes only the center-of-mass motion of a quantum object, our experiment demonstrates that the translational quantum phase is sensitive to dynamic conformational state changes inside the diffracted molecules. The structural flexibility of tailor-made organic particles is sufficient to admit a mixture of strongly fluctuating dipole moments. These modify the electric susceptibility and through this the quantum interference pattern in the presence of an external electric field. Detailed molecular dynamics simulations combined with density-functional theory allow us to quantify the time-dependent structural reconfigurations and to predict the ensemble-averaged square of the dipole moment which is found to be in good agreement with the interferometric result. The experiment thus opens a different perspective on matter wave interferometry, as we demonstrate here that it is possible to collect structural information about molecules even if they are delocalized over more than 100 times their own diameter.