Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Nonlinear optical processes and the nearest neighbor distribution in rubidium vapor

Thomas M. Spinka

Published Aug 20, 2010• 2 citations
OpenAlex

Abstract

Nonlinear optical processes, with a particular emphasis on parametric four-wave mixing (PFWM), are studied in rubidium vapor. A theoretical framework is introduced that enables accurate calculations of nonlinear light-matter interactions, and calculations of these interactions using this framework are performed for a broad range of excitation conditions. In particular, the effects of femtosecond pulse parameters such as pulse duration, pulse energy, center wavelength, and chirp are investigated. Simulation results provide insight into the light-matter interactions in rubidium vapor for these conditions. The effects of pump pulse parameters on the production and evolution of atomic wavepackets in the nonlinear medium are investigated. A number of femtosecond-scale phenomena that were elusive or previously unknown are observed, including the observation of quantum beating at pump-probe time delays exceeding 500 ps, quantum beating on the 7s1/2 - 5d3/2 energy defect at 611 cm-1, and the effects of pump pulse chirp on the amplitude and temporal dynamics of quantum beating. Toward the goal of using the nonlinear optical process of PFWM to interrogate the nearest neighbor distribution (NND), a new analytical derivation for the NND in the non-interacting particle approximation is presented, along with the results of molecular dynamics simulations of the NND in rubidium vapor for realistic pair interaction potentials.

Related papers

Study of wavepacket dynamics in rubidium vapor by means of time-frequency analysis

Andrey A. Senin

Wavepackets are excited in rubidium vapor by intense ultrashort (∼100 fs) pulses centered at a wavelength of 620 nm or 770 nm. The generated atomic wavepackets are optically detected via a pump-probe experiment based on axially phase-matched parametric four-wave mixing (FWM). This nonlinear process results in coherent ultraviolet (UV) or violet emission that carries information about the relative number densities of the excited states. The frequency spectrum of the UV/violet signal intensity, recorded while varying the pump-probe time delay, shows the presence of quantum beats between energy levels involved in the FWM process. The time-frequency analysis of that temporal UV/violet data is done by means of the short-time Fourier transform that leads to retrieval of the temporal evolution of amplitude and phase of the quantum beats. The observed dynamics suggest that not only atomic but also molecular ( Rb*2 ) wavepackets are generated, and that the temporal history of the amplitude of the quantum beats reflects the production of the excited atomic fragments of Rb*2 dissociation. More precisely, changes in the Rb excited state number densities alter the third-order nonlinear susceptibility chi(3) of the Rb vapor, which affects generation of the output signal wave by FWM. Dissociation into several product states is detected, and their branching ratios are estimated. Thus, atomic wavepackets, combined with FWM, appear to be a sensitive new multichannel spectroscopic means to study the fundamental process of molecular dissociation.

•Jan 1, 2003•0 citations

Many-Body Dipole-Dipole Interactions between Excited Rb Atoms Probed by Wave Packets and Parametric Four-Wave Mixing

F. Shen, Ju Gao, Andrey A. Senin +5 more

Dipole-dipole interactions between excited Rb atoms at long range (approximately 300a0-2150a0) have been observed with molecular wave packets and a coherent nonlinear optical process. Fourier analysis of the parametric four-wave mixing (PFWM) signal wave intensity produced in femtosecond pump-probe experiments demonstrates the appearance of sidebands associated with the Rb 7s-5d(5/2) quantum beating frequency of approximately 18.3 THz. Calculations show that the observed sideband splittings and Fourier domain profiles result from multiple atom, dipole-dipole interactions, and ensembles comprising five or fewer Rb (7s, 6p) atoms account for virtually all of the data.

Physical Review Letters•Oct 5, 2007•41 citations

Quantum beat observations in rubidium vapor

Brian J. Ricconi

Probing the interactions between a mode-locked laser pulse and saturated rubidium vapor with a pump–probe technique has resulted in observations of coherences within the atom that persist longer than 150 ps. Quantum beats due to the interference between the 7S and 5D_{5/2} energy states were observed by a four-wave mixing process. The difference frequency between the 5D–5P_{3/2} and the 5P_{3/2}–5S transitions was also observed for interpulse delays up to 180 ps. The temporal evolution of the beat amplitude indicates the existence of a superfluorescent process and a scattering process detected simultaneously with the four-wave mixing process. A model was developed to explain the processes and was used to predict the range of pulse parameters for which the scattering process and four-wave mixing could be simultaneously detected.

•Jun 27, 2012•1 citation

Ultrafast Dynamics and Nonlinear Interactions in Alkali Atoms and Diatomics

Pramod Charles John

Ultrafast laser pump-probe techniques have been used to study the rovibrational dynamics of the B, C, and D states of the Cesium dimer and to study atomic wavepackets and nonlinear effects in Rubidium and Potassium. Two color, pump-probe techniques have been used to probe the time evolution of wavepackets in the B, C, and D rovibrational levels of Cs$\sb2$. The temporal history of the wavepacket is inferred from the time and energy-integrated photoelectron signal produced when the excited state is photoionized by a time-delayed probe pulse. Oscillatory motion is observed in the photoionization signals, corresponding to the vibrational energy differences of the state begin studied. The period of oscillation ranges between 2.2 and 1.1 ps depending on the state. Quantum mechanical simulations of the wavepacket motion show excellent agreement with the experimental data. Experiments have been carried out in which atomic wavepackets interact with a four-wave mixing process in Rb and K to produce spatially and temporally coherent pulses of UV radiation. Wave packets are produced by coherently exciting an ensemble of states using the broad bandwidth of a femtosecond pulse. Oscillations corresponding to the energy differences between the levels in the wavepacket are superimposed on the UV signal when two identical pump and delayed probe pulses are introduced into the alkali vapor. Analyses of the UV emission line profiles show excellent agreement with the four-wave mixing process.

•Dec 1, 1997•0 citations

Study of four-wave mixing in the femtosecond laser pulse propagation near the resonance rubidium doublet

A. A. Preobrazhenskaya, Д. Ю. Преображенский, A. A. Pastor +1 more

In this paper, we investigated the coherent degenerate and nondegenerate four-wave interaction in the propagation of a femtosecond laser pulse in atomic rubidium vapor. In the case of degenerate four-wave interaction, the mechanism for optical switching in an optically dense resonant medium is considered. The third-order nonlinear interaction of the laser beams intersecting in the cell at a small angle leads to a nonlinear response in the form of a fourth beam, which occurs as a result of the interaction between the two pump beams and the third signal laser beam.

Russian Journal of Physical Chemistry B•Jul 1, 2015•0 citations

Dynamics of Interfering Wave Packets in Rubidium by High Resolution Quantum Beat Spectroscopy

William Goldshlag

High resolution quantum beat spectroscopy has been realized to study atomic wave packet dynamics. Wave packets comprising pairs of low quantum number (n = 5 - 8) electronic states were formed in Rb vapor with ultrafast laser pulses, and their dynamics was observed by an all-optical technique of parametric four wave mixing (PFWM). The experimental apparatus designed, constructed and automated for this work provided unprecedented signal intensity that enabled time-frequency-resolved analysis of wave packet dynamics with picosecond temporal resolution over the course of 1100 ps. Both time-resolved and non-time-resolved discrete Fourier methods were applied to measure the concurrent formation of multiple wave packets. Many novel effects and interactions have been measured either for the first time or with greatly improved signal-to-noise ratio. Among them were the formation of the 8S1/2 - 6D5/2 wave packet that was not directly excited by the ultrafast radiation, formation and relative dynamics of quantum beating harmonics up to 73 THz, and quantum beating revivals. The effects of vapor number density and temperature were analyzed experimentally. Interference between the 7S1/2 - 5D5/2 and 8S1/2 - 6D5/2 wave packets (frequencies of 18.225 THz and 10.73 THz, respectively) has been observed for the first time and will be described in detail.

•Dec 8, 2017•0 citations
Nonlinear optical processes, with a particular emphasis on parametric four-wave mixing (PFWM), are studied in rubidium vapor. A theoretical framework is introduced that enables accurate calculations of nonlinear light-matter interactions, and calculations of these interactions using this framework are performed for a broad range of excitation conditions. In particular, the effects of femtosecond pulse parameters such as pulse duration, pulse energy, center wavelength, and chirp are investigated. Simulation results provide insight into the light-matter interactions in rubidium vapor for these conditions. The effects of pump pulse parameters on the production and evolution of atomic wavepackets in the nonlinear medium are investigated. A number of femtosecond-scale phenomena that were elusive or previously unknown are observed, including the observation of quantum beating at pump-probe time delays exceeding 500 ps, quantum beating on the 7s1/2 - 5d3/2 energy defect at 611 cm-1, and the effects of pump pulse chirp on the amplitude and temporal dynamics of quantum beating. Toward the goal of using the nonlinear optical process of PFWM to interrogate the nearest neighbor distribution (NND), a new analytical derivation for the NND in the non-interacting particle approximation is presented, along with the results of molecular dynamics simulations of the NND in rubidium vapor for realistic pair interaction potentials.
Wavepackets are excited in rubidium vapor by intense ultrashort (∼100 fs) pulses centered at a wavelength of 620 nm or 770 nm. The generated atomic wavepackets are optically detected via a pump-probe experiment based on axially phase-matched parametric four-wave mixing (FWM). This nonlinear process results in coherent ultraviolet (UV) or violet emission that carries information about the relative number densities of the excited states. The frequency spectrum of the UV/violet signal intensity, recorded while varying the pump-probe time delay, shows the presence of quantum beats between energy levels involved in the FWM process. The time-frequency analysis of that temporal UV/violet data is done by means of the short-time Fourier transform that leads to retrieval of the temporal evolution of amplitude and phase of the quantum beats. The observed dynamics suggest that not only atomic but also molecular ( Rb*2 ) wavepackets are generated, and that the temporal history of the amplitude of the quantum beats reflects the production of the excited atomic fragments of Rb*2 dissociation. More precisely, changes in the Rb excited state number densities alter the third-order nonlinear susceptibility chi(3) of the Rb vapor, which affects generation of the output signal wave by FWM. Dissociation into several product states is detected, and their branching ratios are estimated. Thus, atomic wavepackets, combined with FWM, appear to be a sensitive new multichannel spectroscopic means to study the fundamental process of molecular dissociation.
Dipole-dipole interactions between excited Rb atoms at long range (approximately 300a0-2150a0) have been observed with molecular wave packets and a coherent nonlinear optical process. Fourier analysis of the parametric four-wave mixing (PFWM) signal wave intensity produced in femtosecond pump-probe experiments demonstrates the appearance of sidebands associated with the Rb 7s-5d(5/2) quantum beating frequency of approximately 18.3 THz. Calculations show that the observed sideband splittings and Fourier domain profiles result from multiple atom, dipole-dipole interactions, and ensembles comprising five or fewer Rb (7s, 6p) atoms account for virtually all of the data.
Probing the interactions between a mode-locked laser pulse and saturated rubidium vapor with a pump–probe technique has resulted in observations of coherences within the atom that persist longer than 150 ps. Quantum beats due to the interference between the 7S and 5D_{5/2} energy states were observed by a four-wave mixing process. The difference frequency between the 5D–5P_{3/2} and the 5P_{3/2}–5S transitions was also observed for interpulse delays up to 180 ps. The temporal evolution of the beat amplitude indicates the existence of a superfluorescent process and a scattering process detected simultaneously with the four-wave mixing process. A model was developed to explain the processes and was used to predict the range of pulse parameters for which the scattering process and four-wave mixing could be simultaneously detected.
Ultrafast laser pump-probe techniques have been used to study the rovibrational dynamics of the B, C, and D states of the Cesium dimer and to study atomic wavepackets and nonlinear effects in Rubidium and Potassium. Two color, pump-probe techniques have been used to probe the time evolution of wavepackets in the B, C, and D rovibrational levels of Cs$\sb2$. The temporal history of the wavepacket is inferred from the time and energy-integrated photoelectron signal produced when the excited state is photoionized by a time-delayed probe pulse. Oscillatory motion is observed in the photoionization signals, corresponding to the vibrational energy differences of the state begin studied. The period of oscillation ranges between 2.2 and 1.1 ps depending on the state. Quantum mechanical simulations of the wavepacket motion show excellent agreement with the experimental data. Experiments have been carried out in which atomic wavepackets interact with a four-wave mixing process in Rb and K to produce spatially and temporally coherent pulses of UV radiation. Wave packets are produced by coherently exciting an ensemble of states using the broad bandwidth of a femtosecond pulse. Oscillations corresponding to the energy differences between the levels in the wavepacket are superimposed on the UV signal when two identical pump and delayed probe pulses are introduced into the alkali vapor. Analyses of the UV emission line profiles show excellent agreement with the four-wave mixing process.
In this paper, we investigated the coherent degenerate and nondegenerate four-wave interaction in the propagation of a femtosecond laser pulse in atomic rubidium vapor. In the case of degenerate four-wave interaction, the mechanism for optical switching in an optically dense resonant medium is considered. The third-order nonlinear interaction of the laser beams intersecting in the cell at a small angle leads to a nonlinear response in the form of a fourth beam, which occurs as a result of the interaction between the two pump beams and the third signal laser beam.
High resolution quantum beat spectroscopy has been realized to study atomic wave packet dynamics. Wave packets comprising pairs of low quantum number (n = 5 - 8) electronic states were formed in Rb vapor with ultrafast laser pulses, and their dynamics was observed by an all-optical technique of parametric four wave mixing (PFWM). The experimental apparatus designed, constructed and automated for this work provided unprecedented signal intensity that enabled time-frequency-resolved analysis of wave packet dynamics with picosecond temporal resolution over the course of 1100 ps. Both time-resolved and non-time-resolved discrete Fourier methods were applied to measure the concurrent formation of multiple wave packets. Many novel effects and interactions have been measured either for the first time or with greatly improved signal-to-noise ratio. Among them were the formation of the 8S1/2 - 6D5/2 wave packet that was not directly excited by the ultrafast radiation, formation and relative dynamics of quantum beating harmonics up to 73 THz, and quantum beating revivals. The effects of vapor number density and temperature were analyzed experimentally. Interference between the 7S1/2 - 5D5/2 and 8S1/2 - 6D5/2 wave packets (frequencies of 18.225 THz and 10.73 THz, respectively) has been observed for the first time and will be described in detail.