Directional coherent light via intensity-induced sideband emission
Andrew J. Traverso, Chris O’Brien, Brett H. Hokr, Jonathan V. Thompson, Luqi Yuan, Charles W. Ballmann, Anatoly A. Svidzinsky, Georgi I. Petrov, Marlan O. Scully, Vladislav V. Yakovlev
We introduce a unique technique for generating directional coherent emissions that could be utilized to create coherent sources in a wide range of frequencies from the extreme ultraviolet (XUV) to the deep infrared. This is accomplished without population inversion by pumping a two-level system with a far-detuned strong optical field that induces the splitting of the two-level system. A nonlinear process of four-wave mixing then occurs across the split system, driving coherent emission at sidebands both red- and blue-detuned from the pump frequency, and propagates both forward and backward along the pump beam path. We observed this phenomenon in dense rubidium vapor along both the D1 and D2 transitions. The sideband emission exhibits a short pulse duration (<1 ns) with threshold-like behavior dependent on both the pump intensity and Rb vapor density. This technique offers a new capability for manipulating the emission frequency simply through intensity-induced atomic modulation that can be scaled to most frequency regimes using various atomic/molecular ensembles and pump energies. A scheme for generating coherent directional emission without the need for population inversion could be a valuable alternative to the laser. Developed by scientists at Texas A&M University in the USA, the approach can in principle be applied anywhere in the electromagnetic spectrum—from the extreme ultraviolet to the far infrared. It involves pumping a two-level system with a strong detuned optical signal, which induces transient AC Stark splitting of the energy levels and four-wave mixing. Initial tests with a dense rubidium vapour indicated that the near-infrared sidebands generated in the process are coherent pulses that are less than 1 nanosecond in duration. The approach should work with other atomic and molecular systems at other wavelengths and may be an attractive way for generating coherent extreme ultraviolet or X-ray radiation as well as a novel approach for remote sensing.
We introduce a unique technique for generating directional coherent emissions that could be utilized to create coherent sources in a wide range of frequencies from the extreme ultraviolet (XUV) to the deep infrared. This is accomplished without population inversion by pumping a two-level system with a far-detuned strong optical field that induces the splitting of the two-level system. A nonlinear process of four-wave mixing then occurs across the split system, driving coherent emission at sidebands both red- and blue-detuned from the pump frequency, and propagates both forward and backward along the pump beam path. We observed this phenomenon in dense rubidium vapor along both the D1 and D2 transitions. The sideband emission exhibits a short pulse duration (<1 ns) with threshold-like behavior dependent on both the pump intensity and Rb vapor density. This technique offers a new capability for manipulating the emission frequency simply through intensity-induced atomic modulation that can be scaled to most frequency regimes using various atomic/molecular ensembles and pump energies. A scheme for generating coherent directional emission without the need for population inversion could be a valuable alternative to the laser. Developed by scientists at Texas A&M University in the USA, the approach can in principle be applied anywhere in the electromagnetic spectrum—from the extreme ultraviolet to the far infrared. It involves pumping a two-level system with a strong detuned optical signal, which induces transient AC Stark splitting of the energy levels and four-wave mixing. Initial tests with a dense rubidium vapour indicated that the near-infrared sidebands generated in the process are coherent pulses that are less than 1 nanosecond in duration. The approach should work with other atomic and molecular systems at other wavelengths and may be an attractive way for generating coherent extreme ultraviolet or X-ray radiation as well as a novel approach for remote sensing.
New approaches for generating coherent light are of keen interest to the scientific community due to the increasing demand for unique sources tailored to specific applications. In fields like microscopy, remote sensing, and soft X-ray/XUV lasers this interest is especially pronounced as novel techniques would have a profound impact. Here, we present new methods for generating coherent light by inducing collective coherence in the gain medium. In particular, we demonstrate coherent emission produced through four-wave mixing on a dressed state, stimulated Raman by inducing coherence between two vibrational levels via 2-photon coupling, and finally, a remote atmospheric coherent source via strong-oscillatory superfluorescence in atomic oxygen. Four-wave mixing on a dressed state could be used to generate XUV coherent radiation or remote atmospheric sensing, as it produces both a forward and backward propagating field. We observe this in Rb vapor with emission occurring at detunings of up to 30 nm from the transition. Similarly, 2-photon enhanced stimulated Raman could be implemented for XUV generation as well, due to the asymmetric gain observed on the anti-Stokes emission relative to the Stokes in Methane. It is also a great platform for microscopy as it is background-free unlike other conventional methods like CARS and CSRS. Atmospheric lasing via oxygen is a prime candidate for nextgeneration remote sensing techniques, and here we study its emission mechanisms in depth demonstrating that superfluorescence serves as the main driving process for the observed 845 nm generation. This intense strong-oscillatory emission lends itself for use in coherent Raman techniques. Furthermore, a dual Raman-Brillouin microscope is also presented and demonstrated, which could prove to be a powerful new tool in biomedical and material characterizations applications.
Extreme ultraviolet (XUV) light is a valuable frequency range for ultrafast optics experiments. The short wavelength is a requirement for ultrashort pulses, which are widely used to characterize fast dynamics. Additionally, the high photon energy enables quantum control of high frequency transitions in atoms. These transitions are of interest for ultrafast quantum control as the bandwidth of the control pulses needs to be less than the transition frequency. Presently, however, no good modulators exist for these frequencies, which significantly reduces the possible ultrafast optics experiments or applications in the XUV regime. This thesis addresses this problem and focuses on the control of XUV light in time and space. To enable control of XUV light a method is described which modulates the phase of XUV light emitted from a gas of noble atoms. The atoms are resonantly excited with a coherent XUV pulse generated through high order harmonic generation. After the excitation pulse has passed through the gas, the atoms will emit light in the absence of an external field, known as free induction. The phase of the emitted light is changed by shifting the resonance frequencies through the AC Stark shift with a non-resonant infrared control pulse. This phase-control of the emitting atoms also translates into a control of the phase of the emitted XUV field.With the method described in the previous paragraph, the direction of XUV light emitted from noble gases was controlled, and the temporal dynamics of the emission was studied. The redirection of the XUV emission, through the use of a spatially offset IR pulse, was found to change both with intensity of the control pulse and by changing the spatial offset between the pulses. By varying the delay between the excitation and the control pulse the time of redirection was controlled, which enabled high signal to noise study of the temporal dynamics of the emission. Furthermore, with two control pulses the emission was redirected twice, resulting in an XUV pulse shape with controlled duration emitted with a certain angle. Hopefully the presented work will result in more research into the development of this technique, to fully realize the possibility to shape the amplitude and phase of XUV pulses. Such a development would open the door for ultrafast XUV quantum control.
We report on an investigation of simultaneous generation of several narrow-bandwidth laser-like coherent emissions from nitrogen molecular ions ( ) produced in intense mid-infrared laser fields. With systematic examinations on the dependences of coherent emissions on gas pressure as well as several laser parameters including laser intensity, polarization and wavelength of the pump laser pulses, we reveal that the multiple coherent emission lines generated in originate from a series of nonlinear processes beginning with four-wave mixing, followed with stimulated Raman scattering. Our analyses further show that the observed nonlinear processes are greatly enhanced at the resonant wavelengths, giving rise to high conversion efficiencies from the infrared pump laser pulses to the coherent emission lines near the transition wavelengths between the different vibrational energy levels of ground X and that of the excited B states.
Abstract Ultrashort, coherent light pulses in the extreme ultraviolet (XUV) wavelength region are excellent tools for a wide range of experiments. These XUV pulses are in particular used to characterize electron dynamics. Additionally, the high photon energy enables quantum control of short-lived transitions in atoms. These transitions are of interest for ultrafast quantum control as the bandwidth of the control pulses needs to be less than the transition frequency. Coherent XUV pulses would be even more useful if the tools to control and manipulate them existed. Presently, however, no modulators exist for these frequencies, which significantly reduces the number of possible ultrafast optics experiments and applications in the XUV regime. This Ph.D. tutorial addresses this problem and focuses on the control of XUV light in time and space. To enable control of XUV light we have developed a method for opto-optical modulation (OOM), which modulates the phase of XUV light emitted from a gas of atoms. The atoms are resonantly excited with a coherent XUV pulse generated through high order harmonic generation and emit light after the excitation pulse passed. By shifting the resonance frequencies through the AC Stark shift with a non-resonant infrared control pulse, the phase of the emitted light, and therefore its wavefront, is controlled. With OOM the direction of XUV light emitted from noble gases has been controlled, and the temporal dynamics of the emission studied. By varying the delay between the excitation and the control pulse, the time of redirection was controlled, which enabled high signal to noise study of the temporal dynamics of the emission. Furthermore, a proof-of-principle experiment with two control pulses was performed, resulting in a shaped XUV pulse with controlled duration. The technique of OOM presented in this article is still at a very early stage and in order to obtain complete control of the amplitude and phase of the XUV pulses further development is necessary. Such development would present new opportunities for ultrafast XUV quantum control.
Coherent supercontinuum radiation in the extreme-ultraviolet (XUV) range is indispensable for synthesizing attosecond light pulses and for exploring transient atomic structures. Here, we report the striking observations of coherent XUV supercontinuum (XSC) extended from below to far above the ionization threshold, which exhibits completely different temporal and spatial properties comparing to the conventional rescattering induced high harmonic generation (HHG). We demonstrate that the strong-field created coherence among bound orbitals strongly distort the atomic transition energies during the pulse, leading to coherent emission spanning tens of electron-volts, in contrast to the line emission via free-induction decay occurring after the pulse. The supposed non-radiating bound dark states contribute as well by emitting dressed energy through dark-to-bright emission mechanism. All the processes modulated at sub-cycle time scale jointly form this new-type coherent XSC. This work achieves the strong-field attosecond control of the exotic atomic radiation dynamics and provides the means of simultaneous generation of separated attosecond sources, i.e., XSC and HHG, with potential advancing attosecond interferometry.
The four-wave mixing produced with two ultrashort phase-locked !-3! laser pulses propagating coherently in a two-level system in the infrared spectral region is shown to depend on the pulses relative phase. The Maxwell-Bloch equations are solved beyond the rotating-wave approximation to account for field frequencies which are largely detuned from the atomic resonance. The relative phase dominating the efficiency of the coupling to the 5! anti-Stokes Raman component is determined by sign of the total ac Stark shift induced in the system, in such a way that the phase influence disappears precisely where the ac Stark effect due to both pulses is compensated. This fundamental quantum interference effect can be the basis for nonlinear ultrafast optical spectroscopy techniques. Phenomena arising from the coherent control of nonlinear interactions are of importance in fields as diverse as optoelectronics and materials research, in high harmonic generation, in photoionization or molecular dissociation, and in biological applications such as spectroscopy and imaging, among others [1, 2, 3, 4, 5, 6, 7]. Optical quantum coherent control is based on the fact that the phases of interfering transition amplitudes in light-matter interactions can be controlled through the optical phase of coherent light sources that drive the interaction, in such a way that the transition rates to final states and the dynamics at various stages of the process can be modified [1]. In a recent paper [8], a theoretical investigation on the quantum coherent control of the optical transient four-wave mixing of two intense phase-locked femtosecond laser pulses of central angular frequencies ω and 3ω propagating in a two-level atom (TLA) was reported. It was shown how the nonlinear (χ (3) ) coupling to the antiStokes Raman field at frequency 5ω depends critically on the initial relative phase φ of the propagating pulses. In Ref. [8], the study was centered to intense pulses in the visible and ultraviolet spectral regions, with frequencies at resonance or lower than the atomic transition. The phenomena observed in [8], however, can be scaled to various laser and material parameters. In the infrared spectral range, for instance, experiments on ultrafast molecular dynamics are frequently performed by help of twocolor pump probe nonlinear spectroscopy techniques. In this type of studies, due to the high intensities inherent to ultrashort (subpicosecond) pulses, nonlinear effects such as stimulated Raman processes may become important and are often utilized as a complementary tool to gain information [9]. In this Letter, we address the conditions for quantum coherent control of transient four-wave mixing interactions with two phase-locked ω-3ω femtosecond laser pulses in the mid-IR spectral region. Our purpose is to reveal the basic physics for a strict two-level medium and to this end the Maxwell-Bloch TLA will be considered. We will study pulses with a duration of 300 fs (with a w 5w