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Laser & Photonics Review

Molecular Quantum Interface for Storing and Manipulating Ultrashort Optical Vortex

Firas Trawi, Franck Billard, O. Faucher, Pierre Béjot, E. Hertz

Published Nov 18, 2022• 8 citations
Publisher

Abstract

Abstract Light beams carrying orbital angular momentum (OAM) have become over the past few years a subject of widespread interest with unprecedented applications in various fields such as optical communication, super‐resolution imaging, optical tweezers, or quantum processing. In the present work it is demonstrated that gas‐phase molecules can be used as a quantum interface to store an OAM carried by an ultrashort laser pulse. The interplay between spin angular momentum and OAM is exploited to encode the spatial phase information of light beams into rotational coherences of molecules. The embedded spatial structure is restored on‐demand with a reading beam by taking advantage of field‐free molecular alignment. The strategy is successfully demonstrated in CO2 molecules at room temperature. Apart from applications to broadband coherent buffer memory, this method opens new functionalities in terms of optical processing and versatile control of OAM fields as well as for a deeper understanding of their role on various molecular processes.

DOI
10.1002/lpor.202200525

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Abstract Light beams carrying orbital angular momentum (OAM) have become over the past few years a subject of widespread interest with unprecedented applications in various fields such as optical communication, super‐resolution imaging, optical tweezers, or quantum processing. In the present work it is demonstrated that gas‐phase molecules can be used as a quantum interface to store an OAM carried by an ultrashort laser pulse. The interplay between spin angular momentum and OAM is exploited to encode the spatial phase information of light beams into rotational coherences of molecules. The embedded spatial structure is restored on‐demand with a reading beam by taking advantage of field‐free molecular alignment. The strategy is successfully demonstrated in CO2 molecules at room temperature. Apart from applications to broadband coherent buffer memory, this method opens new functionalities in terms of optical processing and versatile control of OAM fields as well as for a deeper understanding of their role on various molecular processes.
We exploit gas-phase molecules as light-matter interface to store an orbital angular momentum (OAM) or a superposition of OAM states (OAM-based photonic qubits) carried by ultrashort laser pulses. The interplay between spin angular momentum and OAM is exploited to encode the amplitude and spatial phase information of light beams into rotational coherences of molecules. This last is restored on-demand over tens of picoseconds with a reading beam by taking advantage of field-free molecular alignment. The underlying mechanism at the origin of the storage can be interpreted by the spatial structuring of the molecular sample induced by the field. The excitation indeed produces an inhomogeneous spatial distribution of molecular alignment (amplitude & orientation) whose periodical revivals associated with the quantum beatings of the rotational wavepacket enables to restore the spatial beam structure on-demand. The strategy is successfully demonstrated in CO2 molecules at room temperature. Besides applicability as storage medium with THz bandwidth application, the use of molecules as light-matter interface opens new functionalities in terms of optical processing and versatile control of OAM fields.
Herein, it is demonstrated that ultrashort spatially structured beams can sculpt a sample of gas‐phase molecules like a 4D material to produce a spatial pattern of aligned molecules whose shape and temporal evolution allow to restore the spatial light information on a time‐delayed reading pulse. To do so, the spatial phase and amplitude information of ultrashort light beams are encoded into rotational coherences of molecules by exploiting the interplay between spin angular momentum and orbital angular momentum. The field‐free molecular alignment resulting from the interaction leads to an inhomogeneous spatial structuring of the sample allowing to transfer the encoded information into a time‐delayed probe beam. The demonstration is conducted in molecules. Besides applications in terms of THz bandwidth buffer memory, the strategy features interesting prospects for establishing versatile optical processing of orbital angular momentum (OAM) fields, for studying various molecular processes, or for designing new photonic devices enabling to impart superpositions of OAM modes to light beams.
We present an experimental study of molecular alignment echoes driven by ultrashort structured light fields carrying orbital angular momentum (OAM). By combining two time-delayed pump pulses with spatially varying polarization, we produce a molecular "q plate" in a gaseous CO_{2} sample that can be rephased in a controllable manner. This approach enables the storage of OAM information within the rotational coherences of molecules and its retrieval at adjustable times. The concept is validated using vortex beams of various topological charges ℓ=±1, 2. These results extend the mechanism of molecular alignment echoes to vector light fields and establish a new route for optical processing of ultrashort OAM pulses, advancing molecular-based quantum interfaces for structured light.
Orbital Angular Momentum In article number 2400008, Edouard Hertz and co-workers show how ultrashort spatially structured beams can sculpt a sample of gas-phase molecules in three dimensions so as to produce a spatial pattern of aligned molecules whose shape and temporal evolution allow to restore the spatial light information on a time-delayed reading pulse. This property can be exploited to establish versatile optical processing of orbital angular momentum fields or to design new photonic devices.
We report on the demonstration of a nonlinear optical memory (NOM) for storage and on-demand manipulation of orbital angular momentum (OAM) of light via higher-order nonlinear processes in cold cesium atoms. A spatially resolved phase-matching technique is used to select each order of the nonlinear susceptibility associated, respectively, with time-delayed four-, six-, and eight-wave mixing processes. For a specific configuration of the stored OAM of the incident beams, we demonstrated that the OAM of the retrieved beam can be manipulated according to the order of the nonlinear process chosen by the operator for reading out the NOM. This demonstration indicates new pathways for applications in classical and quantum information processing where OAM of light is used to encode optical information.
Light carrying orbital angular momentum (OAM) has exciting applications, including the studies of fundamental quantum physics, optical manipulation and trapping of particles, astrophysics, high-precision optical measurements and optical communication, etc. In quantum information field, a photon encoded with information in its OAM degrees of freedom enables networks to carry significantly more information and increase their capacity greatly due to the inherent infinite degrees of freedom for OAM. Therefore it is no surprise that many groups and researchers are active in building up a high-dimensional quantum network and many important progresses have been achieved during the past years. To realize a long-distance quantum communication, a quantum repeater has to be used to overcome the problem of communication fidelity decreasing exponentially with the channel length, where, quantum memories for photons, used for storing quantum information, which have been realized successfully during the past decade in many systems such as a cold/hot atomic system, a solid matter, a diamond, and others, are key components consisting of a quantum repeater. Photons acted as information candidates can connect different quantum repeaters. Long distance quantum communication requires the wavelengths of photons are situated in the low-loss communication windows, but most quantum memories currently being developed for use in a quantum repeater work at different wavelengths, only few memories can work in low-loss communication windows. Furthermore, the signal stored is an attenuated coherent light and has the Gaussian mode. Though the storage of photonic entanglement at telecom wavelength is realized in an erbium-doped optical fibre recently, the spatial mode used is Gaussian mode. Quantum memories for photons with OAM have recently been realized, but all work at different wavelengths. So a quantum interface to bridge the wavelength gap is necessary.