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arXiv:quant-ph/0701179 · Physical Review A

Polarizability measurements of a molecule via a near-field matter-wave interferometer

Martin Berninger, André Stefanov, Sarayut Deachapunya, Markus Arndt

Published Jul 9, 2007• 80 citations

Abstract

We present a method for measuring the scalar polarizability of molecules by means of near-field matter-wave interferometry. This technique is applicable to a wide range of complex neutral molecules. A key feature of our experiment is the combination of good transmission and high spatial resolution, gained by imprinting a submicrometer spatial modulation onto a wide molecular beam. Our method significantly improves the measurement sensitivity of the polarizability-dependent shifts. We have successfully performed measurements on fullerenes and report the polarizability to be $\ensuremath{\alpha}=88.9\ifmmode\pm\else\textpm\fi{}0.9\ifmmode\pm\else\textpm\fi{}5.1\phantom{\rule{0.3em}{0ex}}{\mathrm{\AA{}}}^{3}$ for ${\mathrm{C}}_{60}$ and $\ensuremath{\alpha}=108.5\ifmmode\pm\else\textpm\fi{}2.0\ifmmode\pm\else\textpm\fi{}6.2\phantom{\rule{0.3em}{0ex}}{\mathrm{\AA{}}}^{3}$ for ${\mathrm{C}}_{70}$.

DOI: 10.1103/physreva.76.013607

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We present a method for measuring the scalar polarizability of molecules by means of near-field matter-wave interferometry. This technique is applicable to a wide range of complex neutral molecules. A key feature of our experiment is the combination of good transmission and high spatial resolution, gained by imprinting a submicrometer spatial modulation onto a wide molecular beam. Our method significantly improves the measurement sensitivity of the polarizability-dependent shifts. We have successfully performed measurements on fullerenes and report the polarizability to be

\ensuremath{\alpha}=88.9\ifmmode\pm\else\textpm\fi{}0.9\ifmmode\pm\else\textpm\fi{}5.1\phantom{\rule{0.3em}{0ex}}{\mathrm{\AA{}}}^{3}

for

{\mathrm{C}}_{60}

and

\ensuremath{\alpha}=108.5\ifmmode\pm\else\textpm\fi{}2.0\ifmmode\pm\else\textpm\fi{}6.2\phantom{\rule{0.3em}{0ex}}{\mathrm{\AA{}}}^{3}

for

{\mathrm{C}}_{70}

.

We review the concept of matter-wave assisted molecule metrology and present the most recent experiments which exploit the capability of universal matter-wave interferometers to measure forces as small as 10-26 N via shifts of the interference fringes in the presence of well-controlled fields. This technique allows us to compare, in the same instrument, a variety of electronic and magnetic properties for a large range of atoms and molecules. We exemplify this here with precision measurements of the static polarizability of cesium atoms and the fullerenes C60 and C70 as well as dynamically-induced susceptibilities of tailored tripeptides. We also present measurements of magnetic properties such as the diamagnetic susceptibility of ground-state atoms and aromatic and non-aromatic hydrocarbons.

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.

We demonstrate a near-field Talbot-Lau interferometer for C70 fullerene molecules. Such interferometers are particularly suitable for larger masses. Using three free-standing gold gratings of 1 microm period and a transversally incoherent but velocity-selected molecular beam, we achieve an interference fringe visibility of 40% with high count rate. Both the high visibility and its velocity dependence are in good agreement with a quantum simulation that takes into account the van der Waals interaction of the molecules with the gratings and are in striking contrast to a classical moiré model.

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.