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arXiv:1608.07135 · Physical Review A

Multiphoton absorption in optical gratings for matter waves

Kai Walter, Stefan Nimmrichter, Klaus Hornberger

Published Oct 20, 2016• 4 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/physreva.94.043637

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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.
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.
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Two of the major classes of atom optical elements are microfabricated structures and light beams. For instance, a standing light wave can act as a phase grating for atoms, as each absorption and emission process is accompanied by a coherent atomic recoil. After a simple discussion of the mechanical effects of light on atoms, we use a band-theoretical approach to categorize the main resonances (Bragg and Doppleron) that can be exploited to operate such a grating effectively. We discuss the incoherent effects of spontaneous emission, showing when and how they lead from a diffractive to a diffusive regime of atom–field interactions. We turn next to the diffraction of atoms by quantized fields and show the sensitivity of the resulting atomic diffraction pattern to the field photon statistics. In this quantized regime, the atom–field interaction leaves the system in an entangled state. We conclude by reviewing some proposals that exploit this property to perform measurements on the field (atom) to prepare and/or monitor specific atomic (field) states.
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 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
We demonstrate that structures made of light can be used to coherently control the motion of complex molecules. In particular, we show diffraction of the fullerenes C(60) and C(70) at a thin grating based on a standing light wave. We prove experimentally that the principles of this effect, well known from atom optics, can be successfully extended to massive and large molecules which are internally in a thermodynamic mixed state and which do not exhibit narrow optical resonances. Our results will be important for the observation of quantum interference with even larger and more complex objects.