Nitrogen molecules illuminated by an intense femtosecond pulse in the near-infrared or mid-infrared regime give rise to coherent forward emission at a series of wavelengths,including 391.4,427.8,357.8 nm,etc [
Acta Photonica Sinica, Volume. 52, Issue 4, 0414001(2023)
Erasing of the Free Induction Decay by Incoherent Ionization Injection
Strong field physics is an important frontier of current physics research. In recent years, the rapid development of ultrafast laser technology has enabled researchers to obtain laser sources with shorter pulse width, higher pulse energy, and wider tunable range. With the advancing of the research on the interaction between strong laser and matter from the traditional perturbation regime to the non-perturbative region, rich strong field physical phenomena such as tunneling ionization and high-order harmonics have been observed. When the high-intensity femtosecond laser propagates in in a transparent medium, it can form a light-plasma filament due to nonlinear optical effects including Kerr effect and plasma generation. In particular, the study of “air lasing” radiation produced by interaction of intense femtosecond laser pulses with air molecules has attracted many attentions in recent 10 years. Air lasing has the characteristics of bidirectional emission, high intensity, high coherence and remote generation, and holds potential application in the field of optical remote sensing. Traditional optical remote sensing collects scattered signals or fluorescent signals of lasers on the atmospheric targets. These optical signals do not have directionality, which poses challenges to the sensitivity of ground collection devices and limits detection accuracy and sensitivity. As a new concept light source, air lasing is expected to greatly improve the signal strength of optical remote detection due to its capacity of emitting coherent beams from the remote atmosphere to the ground. In recent years, several important progress have been achieved as to the understanding of the air lasing signal generated by the interaction of strong-field laser and the most important component of air, nitrogen. Regarding the underlying mechanism of the coherent emission of neutral nitrogen molecule, it is now accepted that the emission at 337.4 nm is Amplified Spontaneous Emission (ASE). In contrast, the lasing mechanism of N
0 Introduction
Nitrogen molecules illuminated by an intense femtosecond pulse in the near-infrared or mid-infrared regime give rise to coherent forward emission at a series of wavelengths,including 391.4,427.8,357.8 nm,etc [
When tunable MIR femtosecond pulses were employed as the pump laser,it has been observed that coherent forward emission at a series of wavelengths including 391.4,427.8 nm superposed on the third or fifth harmonics of the pump laser[
In this work,we injected a delayed 800 nm pulse into the plasma after the main mid-infrared pump pulse and observed an erasing effect of the free-induction decay emission. It was found that the erasing effect lasts for a couple of picoseconds for the pump wavelengths of 1 250 and 1 550 nm. In particular,for the pump pulse at 1 550 nm,a significant enhancement of the emission around temporal overlapping of the pump and control pulses was observed,while for the 1 250 nm pump pulse such enhancement was not found. Furthermore,this erasing effect was studied for different gas pressures and control pulse energies. We attribute this erasing effect to the incoherent ionization injection of 800 nm control pulse and the change of ρBX coherence in the system caused by the 800 nm pulse. This erasing effect provides a simple method for temporal characterization of the weak FID emission in case it overlaps with the harmonics in the spectral domain.
1 Experimental setup
In the experiment,a femtosecond laser system(Coherent Legend DUO)delivers 40 fs pulses with pulse energy of 12 mJ at a repetition rate of 1 kHz. A dielectric beam splitter separates the pulses into two beams of almost equal energy. One of the beams with 5 mJ pulse energy was employed to pump an Optical Parametric Amplification(OPA)system,which provides wavelength-tunable femtosecond pulses ranging from 1 100 nm to 2 600 nm. The other 800 nm beam was attenuated properly before it was combined with the MIR pump by a dichroic mirror. The experimental setup is schematically presented in
Figure 1.Experimental setup. Inset,energy-level diagram of neutral and ionic nitrogen molecule
2 Experimental results
2.1 Lasing emission at 391.4 nm from molecular nitrogen ion
In
Figure 2.Spectrum of the forward emission as a function of the pump laser wavelength
2.2 The erasing effect by 800 nm control pulses
In
Figure 3.Suppression of the emission obtained at different pump wavelength
The time-resolved results for pump laser wavelength of 1 250 nm and 1 550 nm are presented in
Figure 4.Experimental results of 1 250 nm pump wavelength
Figure 5.Experimental results of 1 550 nm pump wavelength
In
3 Discussion
How should we understand this erasing effect of the free induction decay radiation by the delayed 800 nm femtosecond laser pulse?It is known that the 391.4 nm emission in case of MIR pump is due to the macroscopic polarization formed between the B and X states which is resonantly excited by multiple photons[
Here,we speculate that the suppression of the radiation at 391.4 nm by the 800 nm pulse could be due to two reasons. The first reason lies in the fact that the control pulse also ionizes the neutral nitrogen molecules. Due to its limited pulse energy and low laser intensity,we expect that most of the produced nitrogen ions is populated in the electronic fundamental X state of the ions,and the additional population to the upper A and B levels is neglectable. Since the 800 nm control pulse is far away from the B-X resonance,the increased population in the X state due to the control pulse is incoherently added to the pre-formed nitrogen ions system by the MIR pump pulse,which can lead to decrease of the B-X coherence due to incoherent mixing. Second,we noticed that the 800 nm field is near resonant with the X(ν = 0)and A(ν = 2)transition. This field,in principle,could excite the ρAX,ρBA and ρBX coherences in such way that the latter is depleted,leading to radiation suppression. We modelled this effect with our 1D Maxwell-Bloch code DeepOne[
In these equations
To model the experiment we asume a 1 mm nitrogen plasma,at 50 mbar pressure and 10% ionization with an initial B-X coherence,(ρBX=0.001)We inject a 100 μJ,100 fs,IR pulse in resonance with the X-A transition(λ~800 nm)at different delays and compare the total energy of the UV radiation(λ=391 nm)emitted due to the initial ρBX coherence.
The results of our 1D Maxwell-Bloch modelling are shown in
Figure 6.Results of the 1D Maxwell-Bloch modelling
In view of these results,we can affirm that the two aforementioned mechanisms(further ionization by the IR control pulse and depletion of the ρBX coherence by the interaction of the IR control pulse and the ρBA coherence)play a role in the dynamics of the system.
4 Conclusion
We have demonstrated that the FID emission of nitrogen ions pumped by femtosecond MIR pulses can be substantially suppressed by a subsequent 800 nm control pulse. This erasing effect occurs universally for different pump laser wavelength,gas pressure and control pulse energy. In addition to the erasing effect,a significant enhancement of the spectral signal was also found for λp = 1 550 nm,where two-photon resonance between the B and A levels occurs. Based on the numerical simulation of the density matrix and Maxwell equation, we attribute this erasing effect to the further photoionization by the 800 nm pulse and the change of coherence between the B and X states of the nitrogen ions. Specifically, the 800 nm pulses directly leads to the change of coherence between the B and A states (ρBA). The further coupling of the ρBA with the 800 nm pulse results in the reduction of the coherence of the B and X states (ρBX), which gives rise to the corresponding suppression of the 391.4 nm radiation.This erasing effect provides a simple method for measurement of the temporal duration of the FID emission,which is particularly useful when the weak FID emission overlaps with the harmonics of the pump laser in the spectral domain.
[21] Xiang ZHANG, Qi LU, Yalei ZHU et al. Multiple-photon resonance enabled quantum interference in emission spectroscopy of N2+. arXiv preprint(2022).
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Haicheng MEI, Xiang ZHANG, Santiago LÓPEZ, Qi LU, Siyu QIN, Liang XU, Eduardo OLIVA, Yi LIU. Erasing of the Free Induction Decay by Incoherent Ionization Injection[J]. Acta Photonica Sinica, 2023, 52(4): 0414001
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Received: Jan. 18, 2023
Accepted: Feb. 20, 2023
Published Online: Jun. 21, 2023
The Author Email: LIU Yi (yi.liu@usst.edu.cn)