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Manipulation of atomic and molecular motion with pulsed lasers

Pasi Ryytty

Published Sep 29, 2000• 0 citations
OpenAlex

Abstract

In this thesis, the use of pulsed laser fields to control the center-of-mass motion of neutral atoms and molecules is studied both numerically and experimentally. In particular, we consider the use of a pulsed standing wave for the deflection of atomic beams, and develop novel types of mirrors for applications in atom and molecule optics. The research work shows that pulsed laser fields can be applied to form efficient mirrors for neutral particles regardless of the details of their internal energy-level structure. Moreover, it is shown that pulsed standing waves can also be utilized to efficiently deflect atomic beams. In the first part of the thesis, we study the effects of phase fluctuations of the laser field on the momentum distribution of atoms after interaction with a standing wave. Our numerical simulations show that the coherence properties of the laser field play a major role in diffraction of atoms, especially when using pulsed lasers. It turns out that the effects caused by the limited coherence time of the optical field are clearly observable as a transfer of atoms in momentum space to the region around zero momentum rather than to high momentum states. The numerical analysis of the pulsed standing-wave diffraction was complemented by experimental measurements of the deflection profiles of a beam of thermal sodium atoms. The experimental distributions were measured for a value of the coherence time intermediate between the Rabi period and the interaction time. A comparison of the results with an expected distribution calculated for a fully coherent interaction shows that the phase fluctuations of the light field drastically affect the achievable transverse momentum values. Based on our theoretical and experimental analysis of the diffraction profiles, we conclude that large deflection angles can be reached only when laser pulses with a Fourier-limited bandwidth are applied. The second part of the thesis concentrates on the development of pulsed mirrors for neutral atoms and molecules. In particular, we consider the use of an evanescent wave, formed in total internal reflection of light on a vacuum-dielectric interface, and of a standing wave as possible mirror configurations. Our numerical simulations of the pulsed evanescent-wave mirror show that atoms with initial velocities up to several tens of meters per second can be reflected already at the moderate field intensities of a few tens of MW/cm2. This allows pulsed evanescent waves to be applied in a compact setup to control the motion of thermal atomic beams, for which the traditional atom mirrors are suited only at grazing incidence. However, since the effective interaction volume of the atomic beam and the laser field is limited by the short decay length of the evanescent wave, only a relatively small number of atoms can be reflected with a single laser pulse. Furthermore, the reflection is always inelastic, since the force exerted on the atoms varies as a function of the initial position of the particles. To solve the above problem we consider the use of a standing wave as a pulsed mirror for atoms. Our numerical simulations show that with a proper choice of the pulse duration and field intensity, each period of the standing-wave pattern functions as an elastic mirror for particles with an initial kinetic energy below the depth of the standing-wave potential. Hence, the standing-wave pattern acts as a long row of independent atom mirrors, which provides a novel route to controlling large volumes of fast atoms even with a single laser pulse. As a second application for the pulsed standing-wave mirror we consider the reflection of slow molecules, for which no efficient mirror configuration previously has been available. It is shown that pulsed standing waves of nonresonant frequencies can be used to efficiently manipulate large volumes of rotationally cold molecules. With a suitable choice of the parameter values, the molecules can be reflected nearly elastically, or with a tailored momentum distribution. This opens up a possibility to use the pulsed standing-wave mirror to control the motion of particles in various applications of atomic and molecular physics. Such a mirror could be applied, for example, to steer and image molecular beams, separate molecular species, and to form pulsed molecular beams.

Related papers

Pulsed Standing-Wave Mirror for Neutral Atoms and Molecules

Pasi Ryytty, M. Kaivola

Reflection of neutral atoms and molecules by a pulsed standing wave with a duration on the order of nanoseconds is studied. It is shown that, with a suitable choice of the laser parameter values, each period of the standing-wave pattern functions as an independent mirror, thus providing a novel way to manipulate large samples of neutral gas-phase particles even with a single laser pulse. At moderate field intensities, the pulsed standing-wave mirror would be directly applicable, e.g., for the manipulation of buffer-gas cooled molecules.

Physical Review Letters•May 29, 2000•14 citations

Reflection of atoms from a pulsed evanescent wave

Pasi Ryytty, M. Kaivola, C.G. Aminoff

Atomic motion in a pulsed evanescent wave, with a pulse duration on the order of the lifetime of the excited state, is calculated using the semiclassical Bloch-equation approach. The equations for the internal atomic motion are solved using two approximations based on high laser intensity and on slow atomic velocity. The center-of-mass motion in the field under the effect of the dipole force is subsequently determined by numerical integration. As an example, the calculations show that the maximum normally incident velocity allowing a sodium atom to be reflected is approximately 35 m/s when using a 10 MW/cm 2 laser pulse of 7 ns duration. Our results also demonstrate that the velocity distribution of the reflected atoms may considerably differ from the distribution of the incident atoms due to different deceleration and acceleration times in a short laser pulse. This effect may lead to an average slowing-down of the reflected part of a thermal particle beam.

Europhysics Letters (EPL)•Nov 10, 1996•1 citation

Atom optics with standing wave fields.

Jayson Leonard Cohen

This dissertation explores the spatial patterns that evolve dynamically in atomic clouds and beams after they interact with one or more standing wave fields, typically formed by laser beams. The main systems under study are ensembles of free atoms, but a model Bose-Einstein condensate and the harmonic oscillator are considered as well. Focused atomic patterns with features much smaller than the wave length of the light fields are possible owing to the nonlinear atom-field interaction and are emphasized. The quantitative results combine numerical simulations and analytical expressions. Computer algorithms were developed from known methods in partial differential equations to perform the numerical simulations. The analytical results relied on standard and newly contrived techniques in quantum physics. The analytical expressions were evaluated by computer in order to extract valuable quantitative information and to compare different analytical methods with one another and with the numerical simulations. The thesis is written as a self-contained piece, and as such, develops specific examples of atom-field configurations and atomic patterns of interest from a general theory of the atoms interacting with a spatially varying light field that influences the subsequent center-of-mass motion. Beyond those already published by our group and expanded upon in the thesis, significant advances are made in: the link between transient interactions in the time- and spatial-domains; an understanding of the Raman-Nath approximation, its range of validity, and its corrections; atomic focusing by pulsed adiabatic interactions between an atom and a single standing wave light field; the differences between classical and quantum free motion after periodic interactions; the distinctions between free motion after amplitude and phase gratings; harmonic oscillator ground states kicked by spatially varying pulses; and quasiperiodic echo effects. The general theoretical structure that was detailed can be applied effectively, as intended from the outset, to other problems in atom optics.

•Aug 1, 2000•0 citations

Optics for Neutral Atomic Beams: Reflection and Diffraction of Sodium Atoms by Evanescent Laser Light Fields

K. G. H. Baldwin, Joseph V. Hajnal, Peter Fisk +2 more

Realization of the analogues of optical components for the manipulation of atomic de Broglie waves has recently become possible through the use of laser-based techniques. The strong fields generated by laser light have already been used to reflect atoms using travelling evanescent waves, and to diffract atomic beams through small angles using transmission gratings formed by a standing laser light wave in vacuo. Present experiments aim to combine these techniques to produce a reflection diffraction grating formed by a standing evanescent laser-light field, and to exploit the larger diffraction angles made possible theoretically by such a scheme.

Journal of Modern Optics•Nov 1, 1990•8 citations

Atomic motion in a high-intensity standing wave laser field

L.F. Saez Ramdohr

This work discusses the effect of a high-intensity standing wave laser field on the motion of neutral atoms moving with a relatively high velocity. The analysis involves a detailed calculation of the force acting on the atoms and the calculation of the diffusion tensor associated with the fluctuations of the quantum force operator. The high-intensity laser field limit corresponds to a Rabi frequency much greater than the natural rate of the atom. The general results are valid for any atomic velocity. Results are then specialized to the case of slow and fast atoms where the Doppler shift of the laser frequency due to the atomic motion is either smaller or larger than the natural decay rate of the atom. The results obtained for the force and diffusion tensor are applied to a particular ideal experiment that studies the evolution of a fast atomic beam crossing a high-intensity laser beam. The theories developed previously, for a similar laser configuration, discuss only the low atomic velocities case and not the more realistic case of fast atoms. Here, an approximate solution of the equation for the distribution is obtained. Starting from the approximate distribution function, the deflection angle and dispersion angle for themore » atomic beam with respect to the free motion are calculated.« less

•Jan 1, 1987•0 citations

Atomic raman diffraction: Theoretical perspectives from semi-classical to second quantized frameworks

Hartmann, Sabrina

This cumulative thesis consists of four publications [1-4], presented as three contributions (I) - (III), where the second one (II) consists of the joint publications [2,3]. All publications were written during the author's research activities at the Institute of Quantum Physics under the supervision of Prof. Dr. W. P. Schleich. All of the presented publications consider light-matter interactions and their potential application in atom interferometry, a comparatively young and rapidly evolving technique. Atom interferometers find application in high-precision measurements, the determination of physical constants, the testing of fundamental physics, and the provision of gravimeters and gyroscopes. The advancement of technology and science has led to significant improvements in performance and the development of ambitious mobile and space-based devices. The recent success of several experiments has led to the proposal of further experiments with the aim of opening up new frontiers. However, the construction of future devices necessitates a decision regarding the employed diffraction mechanism and geometry, depending on the specific technical and scientific requirements. Furthermore, it is necessary to enhance the sensitivity of future devices. The contributions in this dissertation address these issues. The first contribution (I) focuses on the diffraction of atoms by laser pulses which can be employed to generate atom-optical diffraction elements like beam splitters and mirrors. These diffraction elements can be combined to construct atom interferometers, which have been successfully employed for precision measurements regarding fundamental physics as well as practical applications. The article presents a numerical comparison of two distinct diffraction mechanisms (Bragg and Raman) and diffraction geometries (single and double diffraction) in microgravity. It discusses the fundamental differences between the mechanisms and geometries with respect to the diffraction efficiency, taking into account the width of the initial wave function and the duration of the light pulse. Additionally, it explores the transition between the two diffraction geometries when starting from an atom initially at rest and increasing its momentum. The results may serve as a reference for experimentalists in selecting the most suitable configuration, based on their aims and requirements in the realization of more advanced atom interferometers. The second contribution (II) is a follow-up to the previous one, but focuses exclusively on a single diffraction type in microgravity, namely the so-called double Raman diffraction. In contrast to the previous article, where we only discussed single two-photon processes, we consider in this article a six-photon process, also known as third-order diffraction, as well as three subsequent two-photon processes, which both lead to the same amount of transferred momentum and can both be used to realize large-momentum transfer (LMT). We demonstrate that third-order double Raman diffraction is a viable and advantageous method for the diffraction of small momentum distributions like Bose-Einstein condensates (BECs) compared to a sequence of three two-photon processes. Furthermore, we show that third-order Raman pulses can be successfully applied to create higher-order Raman atom interferometers. Third-order diffraction can be perfectly combined with other LMT techniques and, moreover, allows for a reduction in the overall duration of the diffraction process and the complexity of the experimental set-up, as only two distinct laser frequencies are required. Moreover, we present a third-order Mach-Zehnder interferometer with spurious paths being disregarded. As demonstrated later on in [3], this interferometer generates optimal contrast and a substantial amplitude. The third contribution (III) extends the semi-classical λ-scheme of single Raman diffraction, as discussed in detail in contribution (I), into a fully quantized multi-atom multi-λ configuration with center-of-mass motion inside a cavity. Therefore, the incorporation of an internal structure allows for a more realistic modeling of the atoms, which is relevant for multi-photon interaction or cooling processes. We use for our analysis the framework of second quantization, i.e., we take into account the field-theoretical nature of the multi-particle atomic field as well as of the diffracting light field. We reduce this model with a Hamiltonian averaging theory applied to the atomic field operators and obtain an effective Hamiltonian, which determines the time evolution of the system. We demonstrate the efficiency of our model by the application of a typical initial state. Moreover, for a specific input state, we obtain the Hong-Ou-Mandel effect simultaneously in the atomic and the optical system. Our many-body formalism is perfectly suited to theoretically describe contemporary high-precision atom interferometric experiments based on entanglement between the atoms, that aim to surpass the shot-noise limit.

•Jan 1, 2025•0 citations
In this thesis, the use of pulsed laser fields to control the center-of-mass motion of neutral atoms and molecules is studied both numerically and experimentally. In particular, we consider the use of a pulsed standing wave for the deflection of atomic beams, and develop novel types of mirrors for applications in atom and molecule optics. The research work shows that pulsed laser fields can be applied to form efficient mirrors for neutral particles regardless of the details of their internal energy-level structure. Moreover, it is shown that pulsed standing waves can also be utilized to efficiently deflect atomic beams. In the first part of the thesis, we study the effects of phase fluctuations of the laser field on the momentum distribution of atoms after interaction with a standing wave. Our numerical simulations show that the coherence properties of the laser field play a major role in diffraction of atoms, especially when using pulsed lasers. It turns out that the effects caused by the limited coherence time of the optical field are clearly observable as a transfer of atoms in momentum space to the region around zero momentum rather than to high momentum states. The numerical analysis of the pulsed standing-wave diffraction was complemented by experimental measurements of the deflection profiles of a beam of thermal sodium atoms. The experimental distributions were measured for a value of the coherence time intermediate between the Rabi period and the interaction time. A comparison of the results with an expected distribution calculated for a fully coherent interaction shows that the phase fluctuations of the light field drastically affect the achievable transverse momentum values. Based on our theoretical and experimental analysis of the diffraction profiles, we conclude that large deflection angles can be reached only when laser pulses with a Fourier-limited bandwidth are applied. The second part of the thesis concentrates on the development of pulsed mirrors for neutral atoms and molecules. In particular, we consider the use of an evanescent wave, formed in total internal reflection of light on a vacuum-dielectric interface, and of a standing wave as possible mirror configurations. Our numerical simulations of the pulsed evanescent-wave mirror show that atoms with initial velocities up to several tens of meters per second can be reflected already at the moderate field intensities of a few tens of MW/cm2. This allows pulsed evanescent waves to be applied in a compact setup to control the motion of thermal atomic beams, for which the traditional atom mirrors are suited only at grazing incidence. However, since the effective interaction volume of the atomic beam and the laser field is limited by the short decay length of the evanescent wave, only a relatively small number of atoms can be reflected with a single laser pulse. Furthermore, the reflection is always inelastic, since the force exerted on the atoms varies as a function of the initial position of the particles. To solve the above problem we consider the use of a standing wave as a pulsed mirror for atoms. Our numerical simulations show that with a proper choice of the pulse duration and field intensity, each period of the standing-wave pattern functions as an elastic mirror for particles with an initial kinetic energy below the depth of the standing-wave potential. Hence, the standing-wave pattern acts as a long row of independent atom mirrors, which provides a novel route to controlling large volumes of fast atoms even with a single laser pulse. As a second application for the pulsed standing-wave mirror we consider the reflection of slow molecules, for which no efficient mirror configuration previously has been available. It is shown that pulsed standing waves of nonresonant frequencies can be used to efficiently manipulate large volumes of rotationally cold molecules. With a suitable choice of the parameter values, the molecules can be reflected nearly elastically, or with a tailored momentum distribution. This opens up a possibility to use the pulsed standing-wave mirror to control the motion of particles in various applications of atomic and molecular physics. Such a mirror could be applied, for example, to steer and image molecular beams, separate molecular species, and to form pulsed molecular beams.
Reflection of neutral atoms and molecules by a pulsed standing wave with a duration on the order of nanoseconds is studied. It is shown that, with a suitable choice of the laser parameter values, each period of the standing-wave pattern functions as an independent mirror, thus providing a novel way to manipulate large samples of neutral gas-phase particles even with a single laser pulse. At moderate field intensities, the pulsed standing-wave mirror would be directly applicable, e.g., for the manipulation of buffer-gas cooled molecules.
Atomic motion in a pulsed evanescent wave, with a pulse duration on the order of the lifetime of the excited state, is calculated using the semiclassical Bloch-equation approach. The equations for the internal atomic motion are solved using two approximations based on high laser intensity and on slow atomic velocity. The center-of-mass motion in the field under the effect of the dipole force is subsequently determined by numerical integration. As an example, the calculations show that the maximum normally incident velocity allowing a sodium atom to be reflected is approximately 35 m/s when using a 10 MW/cm 2 laser pulse of 7 ns duration. Our results also demonstrate that the velocity distribution of the reflected atoms may considerably differ from the distribution of the incident atoms due to different deceleration and acceleration times in a short laser pulse. This effect may lead to an average slowing-down of the reflected part of a thermal particle beam.
This dissertation explores the spatial patterns that evolve dynamically in atomic clouds and beams after they interact with one or more standing wave fields, typically formed by laser beams. The main systems under study are ensembles of free atoms, but a model Bose-Einstein condensate and the harmonic oscillator are considered as well. Focused atomic patterns with features much smaller than the wave length of the light fields are possible owing to the nonlinear atom-field interaction and are emphasized. The quantitative results combine numerical simulations and analytical expressions. Computer algorithms were developed from known methods in partial differential equations to perform the numerical simulations. The analytical results relied on standard and newly contrived techniques in quantum physics. The analytical expressions were evaluated by computer in order to extract valuable quantitative information and to compare different analytical methods with one another and with the numerical simulations. The thesis is written as a self-contained piece, and as such, develops specific examples of atom-field configurations and atomic patterns of interest from a general theory of the atoms interacting with a spatially varying light field that influences the subsequent center-of-mass motion. Beyond those already published by our group and expanded upon in the thesis, significant advances are made in: the link between transient interactions in the time- and spatial-domains; an understanding of the Raman-Nath approximation, its range of validity, and its corrections; atomic focusing by pulsed adiabatic interactions between an atom and a single standing wave light field; the differences between classical and quantum free motion after periodic interactions; the distinctions between free motion after amplitude and phase gratings; harmonic oscillator ground states kicked by spatially varying pulses; and quasiperiodic echo effects. The general theoretical structure that was detailed can be applied effectively, as intended from the outset, to other problems in atom optics.
Realization of the analogues of optical components for the manipulation of atomic de Broglie waves has recently become possible through the use of laser-based techniques. The strong fields generated by laser light have already been used to reflect atoms using travelling evanescent waves, and to diffract atomic beams through small angles using transmission gratings formed by a standing laser light wave in vacuo. Present experiments aim to combine these techniques to produce a reflection diffraction grating formed by a standing evanescent laser-light field, and to exploit the larger diffraction angles made possible theoretically by such a scheme.
This work discusses the effect of a high-intensity standing wave laser field on the motion of neutral atoms moving with a relatively high velocity. The analysis involves a detailed calculation of the force acting on the atoms and the calculation of the diffusion tensor associated with the fluctuations of the quantum force operator. The high-intensity laser field limit corresponds to a Rabi frequency much greater than the natural rate of the atom. The general results are valid for any atomic velocity. Results are then specialized to the case of slow and fast atoms where the Doppler shift of the laser frequency due to the atomic motion is either smaller or larger than the natural decay rate of the atom. The results obtained for the force and diffusion tensor are applied to a particular ideal experiment that studies the evolution of a fast atomic beam crossing a high-intensity laser beam. The theories developed previously, for a similar laser configuration, discuss only the low atomic velocities case and not the more realistic case of fast atoms. Here, an approximate solution of the equation for the distribution is obtained. Starting from the approximate distribution function, the deflection angle and dispersion angle for themore » atomic beam with respect to the free motion are calculated.« less
This cumulative thesis consists of four publications [1-4], presented as three contributions (I) - (III), where the second one (II) consists of the joint publications [2,3]. All publications were written during the author's research activities at the Institute of Quantum Physics under the supervision of Prof. Dr. W. P. Schleich. All of the presented publications consider light-matter interactions and their potential application in atom interferometry, a comparatively young and rapidly evolving technique. Atom interferometers find application in high-precision measurements, the determination of physical constants, the testing of fundamental physics, and the provision of gravimeters and gyroscopes. The advancement of technology and science has led to significant improvements in performance and the development of ambitious mobile and space-based devices. The recent success of several experiments has led to the proposal of further experiments with the aim of opening up new frontiers. However, the construction of future devices necessitates a decision regarding the employed diffraction mechanism and geometry, depending on the specific technical and scientific requirements. Furthermore, it is necessary to enhance the sensitivity of future devices. The contributions in this dissertation address these issues. The first contribution (I) focuses on the diffraction of atoms by laser pulses which can be employed to generate atom-optical diffraction elements like beam splitters and mirrors. These diffraction elements can be combined to construct atom interferometers, which have been successfully employed for precision measurements regarding fundamental physics as well as practical applications. The article presents a numerical comparison of two distinct diffraction mechanisms (Bragg and Raman) and diffraction geometries (single and double diffraction) in microgravity. It discusses the fundamental differences between the mechanisms and geometries with respect to the diffraction efficiency, taking into account the width of the initial wave function and the duration of the light pulse. Additionally, it explores the transition between the two diffraction geometries when starting from an atom initially at rest and increasing its momentum. The results may serve as a reference for experimentalists in selecting the most suitable configuration, based on their aims and requirements in the realization of more advanced atom interferometers. The second contribution (II) is a follow-up to the previous one, but focuses exclusively on a single diffraction type in microgravity, namely the so-called double Raman diffraction. In contrast to the previous article, where we only discussed single two-photon processes, we consider in this article a six-photon process, also known as third-order diffraction, as well as three subsequent two-photon processes, which both lead to the same amount of transferred momentum and can both be used to realize large-momentum transfer (LMT). We demonstrate that third-order double Raman diffraction is a viable and advantageous method for the diffraction of small momentum distributions like Bose-Einstein condensates (BECs) compared to a sequence of three two-photon processes. Furthermore, we show that third-order Raman pulses can be successfully applied to create higher-order Raman atom interferometers. Third-order diffraction can be perfectly combined with other LMT techniques and, moreover, allows for a reduction in the overall duration of the diffraction process and the complexity of the experimental set-up, as only two distinct laser frequencies are required. Moreover, we present a third-order Mach-Zehnder interferometer with spurious paths being disregarded. As demonstrated later on in [3], this interferometer generates optimal contrast and a substantial amplitude. The third contribution (III) extends the semi-classical λ-scheme of single Raman diffraction, as discussed in detail in contribution (I), into a fully quantized multi-atom multi-λ configuration with center-of-mass motion inside a cavity. Therefore, the incorporation of an internal structure allows for a more realistic modeling of the atoms, which is relevant for multi-photon interaction or cooling processes. We use for our analysis the framework of second quantization, i.e., we take into account the field-theoretical nature of the multi-particle atomic field as well as of the diffracting light field. We reduce this model with a Hamiltonian averaging theory applied to the atomic field operators and obtain an effective Hamiltonian, which determines the time evolution of the system. We demonstrate the efficiency of our model by the application of a typical initial state. Moreover, for a specific input state, we obtain the Hong-Ou-Mandel effect simultaneously in the atomic and the optical system. Our many-body formalism is perfectly suited to theoretically describe contemporary high-precision atom interferometric experiments based on entanglement between the atoms, that aim to surpass the shot-noise limit.