Abstract
Our theoretical model of forced dipole oscillation demonstrates that when the amplitude of the forcing field is changing fast, the oscillations of the bound electron in the atom or molecule initially proceed at two frequencies: the frequency of the natural electron oscillations and the frequency of the forcing field. Particularly, applied to the science of scattering, this model of transient forced atomic and molecular oscillations suggests that accurate interpretation of the laser scattering experiments using short laser pulses must include both the conventionally known scattering at the laser frequency (Rayleigh) and the predicted by our theoretical spectral emission that corresponds to the natural frequency of the electronic oscillations. This article presents the results of numerical simulations using our model performed for the hydrogen atom. The characteristics of the components of scattered radiation, their polarization, and Doppler thermal broadening are discussed.
© 2020 Optical Society of America under the terms of the OSA Open Access Publishing Agreement
1. Introduction
Study of Rayleigh scattering of light by atoms and molecules has a long history. Currently, Rayleigh scattering of laser radiation is widely used for diagnostics of gases and weakly ionized plasma [1]. Considering the long history of research one would assume that the fundamentals of the classical theory of Rayleigh scattering are well established and the science is settled. However, it appears that one important issue was omitted from the fundamentals of Rayleigh scattering theory - the transient (time-dependent) model of light scattering. The current scattering theory is solely based on the Lorentz’s model that considers temporally established forced oscillator [2]. It is commonly understood that, for the typical atomic and molecular oscillators the time to reach established (repeatable) forced oscillations is determined by the characteristic damping time of the natural oscillation of the optical electrons. Then simple estimates based on the available data for light attenuation in gases due to scattering show that the time required to reach established electron oscillations is ranging from tens of picoseconds to nanoseconds. Such time scale was in the realm of pure fiction during the period from the 17th to the 19th century when the foundations of the modern optics were developed. Hence, the established atomic oscillation model seemed to be well suited. In the middle of the 20th century, after the invention of lasers, sub-nanosecond time scale became a common reality. However, the basic assumptions of the foundational paradigm of the optics remained unchanged. Struggling with the temptation to significantly deviate for the topic, we still would like to state that, both the electrodynamics and quantum mechanics theories while applied for the needs of optics, describe the light-matter interaction utilizing the same antique paradigm of slowly changing and established forced oscillations of optical electrons. Returning to the topic of this publication: we suggest that under the conditions typical for a pulsed laser interaction, the forced atomic oscillations of optical electrons could occur in a transient mode during which the optical electron oscillations contain component that has a frequency close to the natural oscillation frequency.
We described the transient atomic oscillation in a recent paper [3] by considering scattering of a relatively short pulse of electromagnetic radiation. This theoretical work predicted that, when the dipole approximation is valid, the re-radiated optical field contains at least two components: one at the frequency of the incident electromagnetic wave, ${\boldsymbol{\omega }_{\boldsymbol{L}}}$, the other corresponds to the frequency $\boldsymbol{\omega ^{\prime}} \approx {\boldsymbol{\omega }_0}$, where ${\boldsymbol{\omega }_0}$ is the natural frequency electron oscillations. The former component is known as scattering and the latter component, that we called “pinging” emission, is previously unknown and yet not observed. Our work showed that the “pinging” emission is predicted to occur regardless of which oscillator model is used to describe the interaction of an optical electron with an electromagnetic wave: a classical Lorentzian oscillator [2] or an oscillator with realistic nonlinear potential [35]. Considering the widespread prevalence of laser diagnostic methods based on Rayleigh scattering, it is necessary to keep in mind when interpreting these experiments that for relatively short pulses the total cross-section of Rayleigh scattering can be very different from that obtained for a long pulse or stationary radiation.
2. Theoretical model
As an example, in this paper we consider the classical approximation of interaction of a hydrogen atom with an electromagnetic wave, when the dipole approximation is valid. As in our previous works [3–5], the equation of motion for electron displacement from the stationary Bohr’s orbit of the s-state of a hydrogen atom is provided by the solution of the following equation of motion:
For a given pulse of electromagnetic radiation, one can find a solution to the Eq. (1) that satisfies the initial conditions
Let’s assume that the induced atomic dipole emission is observed by a sufficiently broadband spectrograph. The spectral power density of this re-emitted radiation is
As was shown in [4], the solution of Eq. (1) becomes very close to the solution described by the classical Lorentz oscillator for decreasing incident radiation intensity, with the exception of higher harmonics. That is, the spectrum contains the main harmonic at the laser frequency ${\boldsymbol{\omega }_{\boldsymbol{L}}}$ and the radiation component at the “pinging” frequency $\boldsymbol{\omega ^{\prime}} \approx {\boldsymbol{\omega }_0}$.
3. Results of simulations and discussion
The results of simulation of the re-emission produced by a forced atomic oscillator described by the Eq. (1) is shown in the Figs. 1–3 for a pulse shape given by the Eq. (8) and for laser wavelength ${\boldsymbol{\lambda }_{\boldsymbol{L}}} = $532 nm.
The corresponding reduced values of the dynamics of the amplitude of the perturbing electric field:
An example of calculation for a pulse with a FWHM of 54 fs that corresponds to the parameter ${\boldsymbol{t}_{\boldsymbol{p}}} = 35$ fs is shown in Fig. 1.
The presence of the “pinging” frequency is clearly demonstrated in the Fig. 1(b). After the end of the laser pulse depicted by the red line, the forced oscillation ends at approximately 55-th femtosecond and after that the electron continues small amplitude oscillation with the frequency of “pinging” $\boldsymbol{\omega ^{\prime}} \approx {\boldsymbol{\omega }_0} \approx 2\boldsymbol{\pi } \cdot 6.59 \cdot {10^{15}}\boldsymbol{\; }\textbf{rad}/\textbf{s}$. The spectral analysis shown in the Fig. 1(c) demonstrates the power content of the “pinging” frequency in the spectral power density distribution.
With an increase in the steepness of the pulse fronts, the relative amplitude of the “pinging” component in the re-radiation spectrum at the frequency $\boldsymbol{\omega ^{\prime}}$ increases and it could become comparable or even exceed the spectral power density component of scattered light at the laser frequency ${\boldsymbol{\omega }_{\boldsymbol{L}}}$. In confirmation of the above, Figs. 2 and 3 show examples of calculations of shorter (FWHM 31.4 fs) and longer (FWHM 78.54 fs) pulses with parameters ${\boldsymbol{t}_{\boldsymbol{p}}} = 20$ fs and ${\boldsymbol{t}_{\boldsymbol{p}}} = 50$ fs, respectively.
In the case of a low intensity of the incident radiation, when the nonlinearity of forced electron motion and related to that generation of higher harmonics can be neglected [5], we can assume that the dipole moment has two components corresponding to oscillations at the “driving” and “pinging” frequencies:
Previously we showed [4] that for a linear Lorentz oscillator, the “pinging” frequency of the re-radiation, $\boldsymbol{\omega ^{\prime}}$, is less than the natural frequency of the oscillator, ${\boldsymbol{\omega }_0}$,
For typical laser interaction conditions $\boldsymbol{\gamma } \ll {\boldsymbol{\omega }_{\boldsymbol{L}}},\boldsymbol{\omega ^{\prime}}$ and ${\boldsymbol{\omega }_{\boldsymbol{L}}} \ll \boldsymbol{\omega ^{\prime}}$, or ${\boldsymbol{\omega }_{\boldsymbol{L}}} \gg \boldsymbol{\omega ^{\prime}}$. Then the total power of Rayleigh and “pinging” scattering, averaged over a time $\Delta \boldsymbol{t} \ge \boldsymbol{max}\left\{ {\frac{{2\boldsymbol{\pi }}}{{{\boldsymbol{\omega }_{\boldsymbol{L}}}}},\boldsymbol{\; }\frac{{2\boldsymbol{\pi }}}{{\boldsymbol{\omega^{\prime}}}}} \right\}$, is
The diagnostics based on Rayleigh scattering use spectrally resolved measurements when the temperature of scattering medium is of interest. The shape of the spectral line of scattered laser light is used to determine temperature assuming Doppler broadening. Note that a narrow-band receiver tuned to the vicinity of the laser frequency ${\omega _L}$ would provide the correct Rayleigh scattering cross section, the value of which is not affected by “pinging” radiation. However, the density of scattered medium is usually measured using energy or power meters that provide spectrally integrated value. In this case, disregarding “pinging” component will lead to an error that would increase with decrease of the laser pulse duration. Recently, the demand is increasing to measure density of rarified medium when the scattered light has low intensity with large intensity background. This leads to increased use of short and ultrashort pulse lasers.
Let’s assume that the incident radiation is plane-polarized. Due to the thermal motion of the atoms/molecules, each of the components of the scattered radiation is subject to doubled Doppler broadening. Full with half maximum (FWHM) of thermal Doppler broadening at the frequency of the disturbing field takes into account a double frequency shift and depends on the angle $\boldsymbol{\theta }$ between the initial direction of the laser radiation and the radiation scattered towards the detector [1]:
Thus, observation of the spectral characteristics of the “pinging” signal also allows one to obtain the same information about the gas temperature as Rayleigh scattering. However, since the “pinging” frequency is different and independent from the laser frequency, ${\boldsymbol{\omega }_{\boldsymbol{L}}}$, there is no need to use a filter for the center of the laser emission line as in the case of so-called filtered Rayleigh scattering [1]. An additional benefit of the “pinging” scattering diagnostics is due to the uniqueness of the natural electron oscillation frequency for each type of atoms and molecules. Thus, using “pinging” one could obtain information on the composition of a multicomponent gas and, with appropriate normalization, information on the concentrations of individual components of the mixture.
As we demonstrated above (see Eq. (13)) the frequency of the “pinging” component of laser forced re-radiation is very close to the natural oscillation frequency of the optical electron, ${\boldsymbol{\omega }_0}$, that is determined by the effective potential, ${\boldsymbol{U}_0}$, and the radius of the orbit, ${\boldsymbol{r}_0}$, of the optical electron. For the considered case of s-state of the hydrogen atom and assuming the parameters stated above, the “pinging” dipole re-radiation has the wavelength of $\boldsymbol{\lambda ^{\prime}} \approx 45.45$ nm and the quantum $\boldsymbol{\varepsilon ^{\prime}} \approx 27.3\boldsymbol{\; }\textbf{eV}$. The energy of the re-radiated “pinging” quanta is approximately twice larger than the ionization potential of hydrogen. Then the ionization of the surrounding atoms with the “pinging” photons could be an additional mechanism for the generation of the seed electrons for the laser optical breakdown since it requires significantly lower laser intensities that are required by the Keldysh mechanism of multiphoton or tunnel ionization [8].
Note that the “pinging” radiation wavelength was obtained based on the accepted values of the effective potential, ${\boldsymbol{U}_0}$, and the radius of the orbit, ${\boldsymbol{r}_0}$. Experimental observation of ‘pinging” radiation will answer the question of how valid the selected values of these parameters are.
4. Conclusions
Our recently developed theoretical model of forced atomic oscillator predicts that a pulse of electromagnetic radiation with fronts that are faster than the characteristic time of atomic radiation decay, ${\gamma ^{ - 1}}$, additionally to the re-emission of radiation at the forcing frequency known as the Rayleigh scattering, the re-emission will contain a component with the frequency that is slightly lower than the frequency of the natural oscillations of the optical electron on its stationary orbit. We call this newly predicted effect the “pinging” emission. If the “pinging” existence is experimentally verified, then the analysis of elastic scattering of short laser pulses on atoms and molecules must include the re-emission at the frequency that is close to the frequency of the natural oscillations of the optical electron that is independent of the irradiation frequency. Disregarding the component of scattering due to the “pinging” emission would lead to significant errors in determining the scattering cross-section.
Acknowledgment
M.N.S. acknowledges partial support by the Princeton Collaborative Research Facility (PCRF) supported by the US DOE under contract DE-AC02-09CH11466.
Disclosures
The authors declare no conflicts of interest.
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