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Nature Communications

Coherence in the presence of absorption and heating in a molecule interferometer

Joseph P. Cotter, Sandra Eibenberger, Lukas Mairhofer, Xiaxi Cheng, Peter Asenbaum, Markus Arndt, K. Walter, Stefan Nimmrichter, Klaus Hornberger

Published Jun 11, 2015• 21 citations
Publisher

Abstract

Matter-wave interferometry can be used to probe the foundations of physics and to enable precise measurements of particle properties and fundamental constants. It relies on beam splitters that coherently divide the wave function. In atom interferometers, such elements are often realised using lasers by exploiting the dipole interaction or through photon absorption. It is intriguing to extend these ideas to complex molecules where the energy of an absorbed photon can rapidly be redistributed across many internal degrees of freedom. Here, we provide evidence that center-of-mass coherence can be maintained even when the internal energy and entropy of the interfering particle are substantially increased by absorption of photons from a standing light wave. Each photon correlates the molecular center-of-mass wave function with its internal temperature and splits it into a superposition with opposite momenta in addition to the beam-splitting action of the optical dipole potential.

DOI
10.1038/ncomms8336

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Matter-wave interferometry can be used to probe the foundations of physics and to enable precise measurements of particle properties and fundamental constants. It relies on beam splitters that coherently divide the wave function. In atom interferometers, such elements are often realised using lasers by exploiting the dipole interaction or through photon absorption. It is intriguing to extend these ideas to complex molecules where the energy of an absorbed photon can rapidly be redistributed across many internal degrees of freedom. Here, we provide evidence that center-of-mass coherence can be maintained even when the internal energy and entropy of the interfering particle are substantially increased by absorption of photons from a standing light wave. Each photon correlates the molecular center-of-mass wave function with its internal temperature and splits it into a superposition with opposite momenta in addition to the beam-splitting action of the optical dipole potential.
We discuss new de Broglie coherence experiments in a near-field molecule interferometer with a variety of large organic molecules. While de Broglie coherence is to first order only associated with the center-of-mass motion of the diffracted particle, we here investigate the question as to which extent the internal molecular property is relevant for, compatible with or detrimental for maintaining coherence in the translational degree of freedom. External perturbations, such as inhomogeneous external electric fields, may influence the delocalized molecules inside the matter wave interferometer and they allow us to access the molecular polarizabilities, permanent or even fluctuating electric dipole moments. We extract information about the molecular states from the interference phase shifts as well as from the observed dephasing in a Kapitza-Dirac Talbot-Lau-Stark-deflectometer. We discuss the relevance of our experiments with regard to both molecule metrology and the foundations of quantum mechanics, i.e. the preservation of coherence for highly complex particles in external fields.
The present thesis deals with two main topics. First, I study in detail the interaction of a delocalized molecular matter-wave with a standing-wave laser grating. Due to absorption of photons in an optical grating, molecules can get excited and numerous internal photophysical processes are induced. For the theoretical description of the molecule-light interaction I take three relevant internal molecular processes into account: intersystem crossing, fluorescence and internal conversion. Furthermore, the fact that molecules can change their optical properties because of the photoexcitation is shown to have a measurable effect on matter-wave interferometry. The second topic of this thesis is about collisions between a polar molecule and non-polar environmental gas atoms, and their effects on the coherence of the center-of-mass state. Because the scattering potential depends on the molecular orientation the molecular rotational state must also be considered. Assuming a slow rotation of the molecule compared to the scattering time and that the molecular mass fairly exceeds the mass of a gas atom, I present a master equation of collisional decoherence, which depends on the molecular orientation. Its predictions for matter-wave interferometry are discussed both in the near and far field.
We present a theory for the diffraction of large molecules or nanoparticles at a standing light wave. Such particles can act as a genuine photon absorbers due to their numerous internal degrees of freedom effecting fast internal energy conversion. Our theory incorporates the interplay of three light-induced properties: the coherent phase modulation due to the dipole interaction, a nonunitary absorption-induced amplitude modulation described as a generalized measurement, and a coherent recoil splitting that resembles a quantum random walk in steps of the photon momentum. We discuss how these effects show up in near-field and far-field interference schemes, and we confirm our effective description by a dynamic evaluation of the grating interaction, which accounts for the internal states.
We measure the absolute absorption cross section of molecules using a matter-wave interferometer. A nanostructured density distribution is imprinted onto a dilute molecular beam through quantum interference. As the beam crosses the light field of a probe laser some molecules will absorb a single photon. These absorption events impart a momentum recoil which shifts the position of the molecule relative to the unperturbed beam. Averaging over the shifted and unshifted components within the beam leads to a reduction of the fringe visibility, enabling the absolute absorption cross section to be extracted with high accuracy. This technique is independent of the molecular density, it is minimally invasive and successfully eliminates many problems related to photon cycling, state mixing, photobleaching, photoinduced heating, fragmentation, and ionization. It can therefore be extended to a wide variety of neutral molecules, clusters, and nanoparticles.
We show that matter-wave diffraction off a single standing laser wave can be used as an accurate measurement scheme for photophysical molecular parameters. These include state-dependent optical polarizabilities and photon-absorption cross sections, the relaxation rates for fluorescence, internal conversion, and intersystem crossing, as well as ionization or cleavage probabilities. We discuss how the different photophysical processes manifest as features of the interference pattern, and we determine the accuracy of molecular parameters estimated from a realistic measurement with finite particle numbers. The analysis is based on an analytic calculation in Wigner representation, which accounts for the laser-induced coherent and incoherent dynamics, for the finite longitudinal and transverse coherence in the matter-wave beam, the gravitational and Coriolis acceleration, and an imperfect standing laser wave. Published by the American Physical Society 2024
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.