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Advanced Photonics Research

Holographic Storage of Ultrafast Photonic Qubit in Molecules

Alexis Voisine, Franck Billard, O. Faucher, Pierre Béjot, E. Hertz

Published Feb 9, 2024• 4 citations
Publisher

Abstract

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.

DOI
10.1002/adpr.202400008

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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.
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 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.
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 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.
Ultrafast optical imaging is demonstrated by ultrashort laser pulse induced impulsive molecular alignment, involving optical image storage in the created molecular wakes followed by periodic readout and display. For diatomic molecules in air, both raised and intagliated monochromatic images are demonstrated, which is field-free, periodically achievable, and works as an ultrafast buffer memory for the imprinted optical images. Analogous to the holographic imaging, the phase information of a three-dimensional object can be revealed at various time delays.
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.