Atomic gases tightly trapped near the focus of an electromagnetic wave interact with photons that exhibit a complex structure, displaying strong gradients of field amplitude and local polarization that can lead to topological phase singularities. We illustrate the consequences of this structure on a paradigmatic nonlinear optical process: three-wave mixing. The process begins by proper selection of the pump field, whose spatial structure is tailored to present huge gradients of the EM field that enhance atomic excitations through forbidden transitions. Atoms can then be depopulated via two electric dipole decays in a cascade configuration, thus providing the three necessary waves. The properties of the down-converted photons are conditioned to those of the pump field through phase matching conditions. It is emphasized that the expression of the photons must incorporate both the structure of the vectorial EM modes and the spatial configuration of the atomic trap. Due to the three-dimensional focusing, the slowly varying envelope approximation becomes inadequate when describing the scattered EM field. We discuss an alternative using a Green function formalism valid for any configuration of the field that also allows to identify the phase matching conditions. Spherical vectorial waves exemplify most concepts here discussed, including the possibility of observing nonlinear quantum phenomena at the single photon level.
Atomic gases tightly trapped near the focus of an electromagnetic wave interact with photons that exhibit a complex structure, displaying strong gradients of field amplitude and local polarization that can lead to topological phase singularities. We illustrate the consequences of this structure on a paradigmatic nonlinear optical process: three-wave mixing. The process begins by proper selection of the pump field, whose spatial structure is tailored to present huge gradients of the EM field that enhance atomic excitations through forbidden transitions. Atoms can then be depopulated via two electric dipole decays in a cascade configuration, thus providing the three necessary waves. The properties of the down-converted photons are conditioned to those of the pump field through phase matching conditions. It is emphasized that the expression of the photons must incorporate both the structure of the vectorial EM modes and the spatial configuration of the atomic trap. Due to the three-dimensional focusing, the slowly varying envelope approximation becomes inadequate when describing the scattered EM field. We discuss an alternative using a Green function formalism valid for any configuration of the field that also allows to identify the phase matching conditions. Spherical vectorial waves exemplify most concepts here discussed, including the possibility of observing nonlinear quantum phenomena at the single photon level.
Structured light, when strongly focused, generates highly confined vectorial electromagnetic field distributions, which may feature a polarization component along the optical axis. Manipulating and detecting such 3D light fields is challenging, as conventional optical elements and detectors do not interact with the axial polarization component. Vector light can, however, be mapped onto atomic polarizations, making electric dipole transitions an ideal candidate to sense such 3D light configurations. Working in the hyperfine Paschen–Back regime, where the electric dipole transitions are spectrally resolved, we demonstrate direct evidence of the axial polarization component of strongly focused radial light. We investigate the influence of various input polarization states, including radial, azimuthal, and higher-order optical vortices, on atomic absorption profiles. Our results confirm a clear mapping between the 3D vector light and the atomic transition strength. This work provides insights into vectorial light–matter interaction and opens avenues for quantum sensing applications.
Structured light, when strongly focused, generates highly confined vectorial electromagnetic field distributions which may feature a polarization component along the optical axis. Manipulating and detecting such 3D light fields is challenging, as conventional optical elements and detectors do not interact with the axial polarization component. Vector light can, however, be mapped onto atomic polarizations, making electric dipole transitions an ideal candidate to sense such 3D light configurations. Working in the hyperfine Paschen-Back regime, where the electric dipole transitions are spectrally resolved, we demonstrate direct evidence of the axial polarization component of strongly focused radial light. We investigate the influence of various input polarization states, including radial, azimuthal, and higher-order optical vortices, on atomic absorption profiles. Our results confirm a clear mapping between the 3D vector light and the atomic transition strength. This work provides new insights into vectorial light-matter interaction, and opens avenues for novel quantum sensing applications.
Spatially-structured laser beams, eventually carrying orbital angular momentum, affect electronic transitions of atoms and their motional states in a complex way. We present a general framework, based on the spherical tensor decomposition of the interaction Hamiltonian, for computing atomic transition matrix elements for light fields of arbitrary spatial mode and polarization structures. We study both the bare electronic matrix elements, corresponding to transitions with no coupling to the atomic center-of-mass motion, as well as the matrix elements describing the coupling to the quantized atomic motion in the resolved side-band regime. We calculate the spatial dependence of electronic and motional matrix elements for tightly focused Hermite-Gaussian, Laguerre-Gaussian and for radially and azimuthally polarized beams. We show that near the diffraction limit, all these beams exhibit longitudinal fields and field gradients, which strongly affect the selection rules and could be used to tailor the light-matter interaction. The presented framework is useful for describing trapped atoms or ions in spatially-structured light fields and therefore for designing new protocols and setups in quantum optics, -sensing and -information processing. We provide open code to reproduce our results or to evaluate interaction matrix elements for different transition types, beam structures and interaction geometries.
We study the behavior of electric fields in and around dielectric and metal nanoparticles, and prepare the ground for their applications to a variety of systems viz. photovoltaics, imaging and detection techniques, and molecular spectroscopy. We exploit the property of nanoparticles being able to focus the radiation field into small regions and study some of the interesting nonlinear, and quantum coherence and interference phenomena near them. The traditional approach to study the nonlinear light-matter interactions involves the use of the slowly varying amplitude approximation (SVAA) as it simplifies the theoretical analysis. However, SVVA cannot be used for systems which are of the order of the wavelength of the light. We use the exact solutions of the Maxwell's equations to obtain the fields created due to metal and dielectric nanoparticles, and study nonlinear and quantum optical phenomena near these nanoparticles. We begin with the theoretical description of the electromagnetic fields created due to the nonlinear wavemixing process, namely, second-order nonlinearity in an nonlinear sphere. The phase-matching condition has been revisited in such particles and we found that it is not satisfied in the sphere. We have suggested a way to obtain optimal conditions for any type and size of material medium. We have also studied the modifications of the electromagnetic fields in a collection of nanoparticles due to strong near field nonlinear interactions using the generalized Mie theory for the case of many particles applicable in photovoltaics (PV). We also consider quantum coherence phenomena such as modification of dark states, stimulated Raman adiabatic passage (STIRAP), optical pumping in 4-level atoms near nanoparticles by using rotating wave approximation to describe the Hamiltonian of the atomic system. We also considered the behavior of atomic and the averaged atomic polarization in 7-level atoms near nanoparticles. This could be used as a prototype to study any n−level atomic system experimentally in the presence of ensembles of quantum emitters. In the last chapter, we suggested a variant of a pulse-shaping technique applicable in stimulated Raman spectroscopy (SRS) for detection of atoms and molecules in multiscattering media. We used discrete-dipole approximation to obtain the fields created by the nanoparticles.
The physics of optical vortices, also known as twisted light, is now a well-established and a growing branch of optical physics with a number of important applications and significant interdisciplinary connections.Optical vortex fields of widely varying forms and degrees of complexity can be realised in the laboratory by a host of different means.The interference between such beams with designated orbital angular momenta and optical spins (the latter is associated with wave polarisations) can be structured to conform to various geometrical arrangements.The focus of this review is on how such tailored forms of light can exert a controllable influence on atoms with which they interact.The main physical effects involve atoms in motion due to application of optical forces.The now mature area of atom optics has had notable successes both of fundamental nature and in applications such as atom lasers, atom guides and Bose-Einstein condensates.The concepts in atom optics encompass not only atomic beams interacting with light, but atomic motion in general as influenced by optical and other fields.Our primary concern in this review is on atoms in structured light where, in particular, the twisted nature of the light is made highly complex with additional features due to wave polarisation.These features bring to the fore a variety of physical phenomena not realisable in the context of atomic motion in more conventional forms of laser light.Atoms near resonance with such structured light fields become subject to electromagnetic fields with complex polarisation and phase distributions, as well as intricately structured intensity gradients and radiative forces.From the combined effect of optical spin and orbital angular momenta, atoms may also experience forces and torques involving an interplay between the internal and centre of mass degrees of freedom.Such interactions lead to new forms of processes including scattering, trapping and rotation and, as a result, they exhibit characteristic new features at the micro-scale and below.A number of distinctive properties involving angular momentum exchange between the light and the atoms are highlighted, and prospective applications are discussed.Comparison is made between the theoretical predictions in this area and the corresponding experiments that have been reported to date.
We have studied nonlinear quantum optical effects in a doubly driven four-level atomic system in a homogeneously broadened regime. On application of two strong fields the system can be made to display double electromagnetically induced transparency (EIT) because of constructive quantum interference giving rise to nonlinear absorption at three-photon resonance condition. This fact may be used to obtain other phenomena like the effect of photon switching in a pulsed regime and large cross phase modulation (XPM) effect. We also show that the behaviour of spatial modulation of transparency of the weak probe beam in a three-level system interacted with a strong standing wave pump field can be dramatically changed in our four-level ladder type system. Here, strong coupling field acting on the uppermost transition is represented by a standing wave whereas strong pump and weak probe fields acting successively on the lower transitions are represented by travelling waves. The effect of double EIT on nonlinear light generation based on the four-wave-mixing (FWM) technique is also investigated. We have examined that the four wave mixing efficiency can be effectively controlled by varying the strength of the pump field.