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@@ -226,13 +226,7 @@ reflectance) of all-dielectric nanoantennas~\cite{makarov2015tuning,
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metasurfaces~\cite{iyer2015reconfigurable, shcherbakov2015ultrafast,
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metasurfaces~\cite{iyer2015reconfigurable, shcherbakov2015ultrafast,
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yang2015nonlinear, shcherbakov2017ultrafast}.
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yang2015nonlinear, shcherbakov2017ultrafast}.
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-In previous works on all-dielectric nonlinear nanostructures, the
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-building blocks (nanoparticles) were considered as objects with
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-dielectric permittivity \textit{homogeneously} distributed over
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-nanoparticle (NP). Therefore, in order to manipulate the propagation
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-angle of the transmitted light it was proposed to use complicated
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-nanostructures with reduced symmetry~\cite{albella2015switchable,
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- baranov2016tuning, shibanuma2016unidirectional}.
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+
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\begin{figure}[t] \centering
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\begin{figure}[t] \centering
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\includegraphics[width=0.75\linewidth]{Concept.pdf}
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\includegraphics[width=0.75\linewidth]{Concept.pdf}
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@@ -241,24 +235,20 @@ distributions in silicon nanoparticle around a magnetic resonance.}
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\label{fgr:concept}
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\label{fgr:concept}
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\end{figure}
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\end{figure}
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-Recently, plasma explosion imaging technique has been used to
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-observe electron-hole plasma (EHP), produced by femtosecond lasers,
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-inside NPs~\cite{Hickstein2014}. Particularly, a strongly
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-localized EHP in the front side\footnote{The incident wave propagates
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- in positive direction of $z$ axis. For the NP with
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- geometric center located at $z=0$ front side corresponds to the
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- volume $z>0$ and back side for $z<0$} of NaCl nanocrystals of
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-$R = 100$~nm was revealed. The forward ejection of ions was attributed in this case to a nanolensing effect inside the NP and to intensity enhancement as low as $10\%$ on the far side of the
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-NP. Much stronger enhancements can be achieved near electric
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-and magnetic dipole resonances excited in single semiconductor
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-NPs, such as silicon (Si), germanium (Ge) etc.
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-
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-In this Letter, we show that ultra-short laser-based EHP
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-photo-excitation in a spherical semiconductor (e.g., silicon) NP leads
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-to a strongly inhomogeneous carrier distribution. To reveal and study
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-this effect, we perform a full-wave numerical simulation. We consider
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+In previous works on all-dielectric nonlinear nanostructures, the
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+building blocks (nanoparticles) were considered as objects with
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+dielectric permittivity \textit{homogeneously} distributed over
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+nanoparticle (NP). Therefore, in order to manipulate the propagation
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+angle of the transmitted light it was proposed to use complicated
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+nanostructures with reduced symmetry~\cite{albella2015switchable,
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+ baranov2016tuning, shibanuma2016unidirectional}. On the other hand, plasma explosion imaging technique~\cite{Hickstein2014} revealed \textit{in situ} strongly asymmetrical electron-hole plasma (EHP) distribution in various dielectric NPs during their pumping by femtosecond laser pulses. Therefore, local permittivity in the strongly photoexcited NPs can be significantly inhomogeneous, and symmetry of nanoparticles can be reduced.
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+
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+%The forward ejection of ions was attributed in this case to a nanolensing effect inside the NP and to intensity enhancement as low as $10\%$ on the far side of the NP. Much stronger enhancements can be achieved near electric and magnetic dipole resonances excited in single semiconductor NPs, such as silicon (Si), germanium (Ge) etc.
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+
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+In this Letter, we show theoretically that ultra-fast photo-excitation in a spherical silicon NP leads
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+to a strongly inhomogeneous EHP distribution, as schematically shown in Fig.~\ref{fgr:concept}. To reveal and analyze this effect, we perform a full-wave numerical simulation. We consider
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an intense femtosecond (\textit{fs}) laser pulse to interact with a
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an intense femtosecond (\textit{fs}) laser pulse to interact with a
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-silicon NP supporting Mie resonances and two-photon free carrier
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+silicon NP supporting Mie resonances and two-photon EHP
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generation. In particular, we couple finite-difference time-domain
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generation. In particular, we couple finite-difference time-domain
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(FDTD) method used to solve three-dimensional Maxwell equations with
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(FDTD) method used to solve three-dimensional Maxwell equations with
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kinetic equations describing nonlinear EHP generation.
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kinetic equations describing nonlinear EHP generation.
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@@ -269,7 +259,7 @@ nanostructures by using single photo-excited spherical silicon
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NPs. Moreover, we show that a dense EHP can be generated at deeply
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NPs. Moreover, we show that a dense EHP can be generated at deeply
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subwavelength scale ($< \lambda / 10$) supporting the formation of
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subwavelength scale ($< \lambda / 10$) supporting the formation of
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small metalized parts inside the NP. In fact, such effects transform
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small metalized parts inside the NP. In fact, such effects transform
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-an all-dielectric NP to a hybrid metall-dielectric one strongly
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+a dielectric NP to a hybrid metall-dielectric one strongly
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extending functionality of the ultrafast optical nanoantennas.
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extending functionality of the ultrafast optical nanoantennas.
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@@ -307,8 +297,8 @@ the critical density and above, silicon acquires metallic properties
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($Re(\epsilon) < 0$) and contributes to the EHP reconfiguration during
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($Re(\epsilon) < 0$) and contributes to the EHP reconfiguration during
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ultrashort laser irradiation.
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ultrashort laser irradiation.
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-The process of three-dimensional photo-generation of the EHP in
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-silicon NPs has not been modeled before in time-domain. Therefore,
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+The process of three-dimensional photo-generation and temporal evolution of EHP in
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+silicon NPs has not been modeled before. Therefore,
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herein we propose a model considering ultrashort laser interactions
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herein we propose a model considering ultrashort laser interactions
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with a resonant silicon sphere, where the EHP is generated via one-
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with a resonant silicon sphere, where the EHP is generated via one-
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and two-photon absorption processes. Importantly, we also consider
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and two-photon absorption processes. Importantly, we also consider
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@@ -324,9 +314,7 @@ scale.
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\subsection{Light propagation}
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\subsection{Light propagation}
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-Ultra-short laser interaction and light propagation inside the silicon
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-NP are modeled by solving the system of three-dimensional Maxwell's equations
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-written in the following way
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+The incident wave propagates in positive direction of $z$ axis, the NP geometric center located at $z=0$ front side corresponds to the volume $z>0$ and back side for $z<0$, as shown in Fig.~\ref{fgr:concept}. Ultra-short laser interaction and light propagation inside the silicon NP are modeled by solving the system of three-dimensional Maxwell's equations written in the following way
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\begin{align} \begin{cases} \label{Maxwell}$$
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\begin{align} \begin{cases} \label{Maxwell}$$
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\displaystyle{\frac{\partial{\vec{E}}}{\partial{t}}=\frac{\nabla\times\vec{H}}{\epsilon_0\epsilon}-\frac{1}{\epsilon_0\epsilon}(\vec{J}_p+\vec{J}_{Kerr})} \\
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\displaystyle{\frac{\partial{\vec{E}}}{\partial{t}}=\frac{\nabla\times\vec{H}}{\epsilon_0\epsilon}-\frac{1}{\epsilon_0\epsilon}(\vec{J}_p+\vec{J}_{Kerr})} \\
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\displaystyle{\frac{\partial{\vec{H}}}{\partial{t}}=-\frac{\nabla\times\vec{E}}{\mu_0}},
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\displaystyle{\frac{\partial{\vec{H}}}{\partial{t}}=-\frac{\nabla\times\vec{E}}{\mu_0}},
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@@ -360,7 +348,7 @@ method \cite{Rudenko2016}, based on the finite-difference time-domain
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(FDTD) \cite{Yee1966} and auxiliary-differential methods for
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(FDTD) \cite{Yee1966} and auxiliary-differential methods for
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dispersive media \cite{Taflove1995}. At the edges of the grid, we
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dispersive media \cite{Taflove1995}. At the edges of the grid, we
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apply the absorbing boundary conditions related to convolutional
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apply the absorbing boundary conditions related to convolutional
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-perfectly matched layers (CPML) to avoid nonphysical reflections
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+perfectly matched layers to avoid nonphysical reflections
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\cite{Roden2000}. The initial electric field is introduced as a
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\cite{Roden2000}. The initial electric field is introduced as a
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Gaussian slightly focused beam as follows
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Gaussian slightly focused beam as follows
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\begin{align}
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\begin{align}
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@@ -420,14 +408,14 @@ length will be around 10$\,$--15~nm for $N_e$ close to $N_{cr}$.
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\begin{figure}[ht!]
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\begin{figure}[ht!]
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\centering
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\centering
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\includegraphics[width=0.495\textwidth]{mie-fdtd-3}
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\includegraphics[width=0.495\textwidth]{mie-fdtd-3}
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-\caption{\label{mie-fdtd} (a, b) First four Lorentz-Mie coefficients
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- ($a_1$, $a_2$, $b_1$, $b_2$) and factors of asymmetry $G_I$,
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- $G_{I^2}$ according to Mie theory at fixed wavelength $800$~nm. (c,
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- d) Squared intensity distribution calculated by Mie theory and (e,
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- f) EHP distribution for low free carrier densities
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+\caption{\label{mie-fdtd} (a) First four Lorentz-Mie coefficients
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+ ($a_1$, $a_2$, $b_1$, $b_2$) and (b) factors of asymmetry $G_I$,
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+ $G_{I^2}$ according to the Mie theory at fixed wavelength $800$~nm. (c,
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+ d) Squared intensity distributions at different radii \textit{R} calculated by the Mie theory and (e,
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+ f) EHP distribution for low densities
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$N_e \approx 10^{20}$~cm$^{-3}$ by Maxwell's equations
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$N_e \approx 10^{20}$~cm$^{-3}$ by Maxwell's equations
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(\ref{Maxwell}, \ref{Drude}) coupled with EHP density equation
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(\ref{Maxwell}, \ref{Drude}) coupled with EHP density equation
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- (\ref{Dens}). (c-f) Incident light propagates from the left to the
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+ (\ref{Dens}). \red{Please, write $G_I$ and $G_{I^2}$ instead of \textit{G} as a title to axis-Y in (b)} (c-f) Incident light propagates from the left to the
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right along $Z$ axis, electric field polarization $\vec{E}$ is along
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right along $Z$ axis, electric field polarization $\vec{E}$ is along
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$X$ axis.}
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$X$ axis.}
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\end{figure}
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\end{figure}
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@@ -448,17 +436,19 @@ Mie theory~\cite{Bohren1983}. It is only valid in the absence of
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nonlinear optical response, thus we can compare it against
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nonlinear optical response, thus we can compare it against
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above-mentioned FDTD-EHP model only for small plasma densities, where
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above-mentioned FDTD-EHP model only for small plasma densities, where
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we can neglect EHP impact to the refractive index. Non-stationary
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we can neglect EHP impact to the refractive index. Non-stationary
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-nature of a~\textit{fs} pulse increase the complexity of the
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-analysis. A detailed discussion on the relation between Mie theory and
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+nature of a~\textit{fs} pulse increases the complexity of the
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+analysis. A detailed discussion on the relation between the Mie theory and
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FDTD-EHP model will be provided in the next section.
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FDTD-EHP model will be provided in the next section.
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-We used Scattnlay program to evaluate calculations of Mie coefficients
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-and near-field distribution~\cite{Ladutenko2017}. This program is
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+We used the Scattnlay program to evaluate calculations of Lorentz-Mie coefficients ($a_i$, $b_i$)
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+and near-field distribution~\cite{Ladutenko2017}. This program is
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available online at GitHub~\cite{Scattnlay-web} under open source
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available online at GitHub~\cite{Scattnlay-web} under open source
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license.
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license.
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\section{Results and discussion}
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\section{Results and discussion}
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+\subsection{Asymmetry factors}
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+
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\begin{figure*}[p]
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\begin{figure*}[p]
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\centering
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\centering
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\includegraphics[width=145mm]{time-evolution-I-no-NP.pdf}
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\includegraphics[width=145mm]{time-evolution-I-no-NP.pdf}
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@@ -468,20 +458,20 @@ license.
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$R = 115$~nm. Pulse duration $130$~\textit{fs} (FWHM). Wavelength
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$R = 115$~nm. Pulse duration $130$~\textit{fs} (FWHM). Wavelength
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$800$~nm in air. (b, d, f) Different stages of EHP evolution shown
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$800$~nm in air. (b, d, f) Different stages of EHP evolution shown
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in Fig.~\ref{plasma-grid} are indicated. The temporal evolution of
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in Fig.~\ref{plasma-grid} are indicated. The temporal evolution of
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- Gaussian beam intensity is also shown. Peak laser fluence is fixed
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- to be $0.125$~J/cm$^2$.}
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+ Gaussian beam intensity is also shown. Peak laser intensity is fixed to
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+ be 10$^{12}$~W/cm$^2$. For better visual representation of time scale at a single optical cycle we put a squared electric field profile in all plots in Fig.~\ref{time-evolution} in gray color as a background image (note linear time scale on the left column and logarithmic scale on the right one). \red{Please, remove italic style of font for 't, fs' on titles of X-axises. Also, all fonts should be the same: please don't mix Times and Arial.}}
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\vspace*{\floatsep}
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\vspace*{\floatsep}
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\centering
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\centering
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\includegraphics[width=150mm]{plasma-grid.pdf}
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\includegraphics[width=150mm]{plasma-grid.pdf}
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\caption{\label{plasma-grid} EHP density snapshots inside Si nanoparticle of
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\caption{\label{plasma-grid} EHP density snapshots inside Si nanoparticle of
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radii $R = 75$~nm (a-d), $R = 100$~nm (e-h) and $R = 115$~nm (i-l)
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radii $R = 75$~nm (a-d), $R = 100$~nm (e-h) and $R = 115$~nm (i-l)
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taken at different times and conditions of excitation (stages
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taken at different times and conditions of excitation (stages
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- $1-4$: (1) first optical cycle, (2) extremum at few optical cycles,
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- (3) Mie theory, (4) nonlinear effects). $\Delta{Re(\epsilon)}$
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- indicates the real part change of the dielectric function defined
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- by Equation (\ref{Index}). Pulse duration $130$~\textit{fs}
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- (FWHM). Wavelength $800$~nm in air. Peak laser fluence is fixed to
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- be $0.125$~J/cm$^2$.}
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+ $1-4$: (1) first optical cycle, (2) maximum during few optical cycles,
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+ (3) quasi-stationary regime, (4) strongly nonlinear regime). $\Delta{Re(\epsilon)}$
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+ indicates the real part change of the local permittivity defined
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+ by Equation (\ref{Index}). Pulse duration 130~fs
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+ (FWHM). Wavelength 800~nm in air. Peak laser intensity is fixed to
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+ be 10$^{12}$~W/cm$^2$. }
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\end{figure*}
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\end{figure*}
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%\subsection{Effect of the irradiation intensity on EHP generation}
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%\subsection{Effect of the irradiation intensity on EHP generation}
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@@ -494,10 +484,10 @@ license.
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and magnetic dipole (ED and MD), while for sizes near
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and magnetic dipole (ED and MD), while for sizes near
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$R \approx 150$~nm a magnetic quadrupole (MQ) response turns to be
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$R \approx 150$~nm a magnetic quadrupole (MQ) response turns to be
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the main one. The superposition of multipoles defines the
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the main one. The superposition of multipoles defines the
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- distribution of electric field inside of the NP. We introduce $G_I$
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+ distribution of electric field inside the NP. We introduce $G_I$
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factor of asymmetry, corresponding to difference between the volume
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factor of asymmetry, corresponding to difference between the volume
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- integral of intensity in the front side of the NP to that in the back
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- side normalized to their sum:
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+ integral of squared electric field in the front side ($I^{front}$) of the NP to that in the back
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+ side ($I^{back}$) normalized to their sum:
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$G_I = (I^{front}-I^{back})/(I^{front}+I^{back})$, where
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$G_I = (I^{front}-I^{back})/(I^{front}+I^{back})$, where
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$I^{front}=\int_{(z>0)}|E|^2d{\mathrm{v}}$ and
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$I^{front}=\int_{(z>0)}|E|^2d{\mathrm{v}}$ and
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$I^{back}=\int_{(z<0)} |E|^2d{\mathrm{v}}$ are expressed via
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$I^{back}=\int_{(z<0)} |E|^2d{\mathrm{v}}$ are expressed via
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@@ -527,37 +517,30 @@ license.
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asymmetry factor
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asymmetry factor
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$G_{N_e} = (N_e^{front}-N_e^{back})/(N_e^{front}+N_e^{back})$
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$G_{N_e} = (N_e^{front}-N_e^{back})/(N_e^{front}+N_e^{back})$
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indicating the relationship between the average EHP densities in the front and in the back halves of the NP, defined as $N_e^{front}=\frac{2}{V}\int_{(z>0)} {N_e}d{\mathrm{v}}$ and
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indicating the relationship between the average EHP densities in the front and in the back halves of the NP, defined as $N_e^{front}=\frac{2}{V}\int_{(z>0)} {N_e}d{\mathrm{v}}$ and
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- $N_e^{back}=\frac{2}{V}\int_{(z<0)} {N_e}d{\mathrm{v}}$, where $V = \frac{4}{3}\pi{R}^3$ is the volume of the nanosphere. In this way, $G_{N_e} = 0$ corresponds to the quasi-homogeneous case and the assumption of the
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- NP homogeneous EHP distribution can be made to investigate the
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+ $N_e^{back}=\frac{2}{V}\int_{(z<0)} {N_e}d{\mathrm{v}}$, where $V = \frac{4}{3}\pi{R}^3$ is the volume of the nanosphere. In this way, $G_{N_e} = 0$ corresponds to the symmetrical case and the assumption of the NP homogeneous EHP distribution can be made to investigate the
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optical response of the excited Si NP. When $G_{N_e}$ significantly
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optical response of the excited Si NP. When $G_{N_e}$ significantly
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differs from $0$, this assumption, however, could not be
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differs from $0$, this assumption, however, could not be
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justified. In what follows, we discuss the results of the numerical
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justified. In what follows, we discuss the results of the numerical
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- modeling (see Fig.~\ref{time-evolution}) of the temporal evolution of
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- EHP densities and the asymmetry factor $G_{N_e}$. It reveals the EHP
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- evolution stages during pulse duration. Typical change of the
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+ modeling of the temporal evolution of
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+ EHP densities and the asymmetry factors $G_{N_e}$ for different sizes of Si NP, as shown in Fig.~\ref{time-evolution}). Typical change of the
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permittivity corresponding to each stage is shown in
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permittivity corresponding to each stage is shown in
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- Fig.~\ref{plasma-grid}. For better visual representation of time
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- scale at a single optical cycle we put a
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- squared electric field profile in all plots in
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- Fig.~\ref{time-evolution} in gray color as a background image (note
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- linear time scale on the left column and logarithmic scale on the
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- right one).
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-
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- To describe all the stages of non-linear light interaction with Si
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+ Fig.~\ref{plasma-grid}. It reveals the EHP
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+ evolution stages during interaction of femtosecond laser pulse with the Si NPs.
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+
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+ \subsection{Stages of transient Si nanoparticle photoexcitation}
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+
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+To describe all the stages of non-linear light interaction with Si
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NP, we present the calculation results obtained by using Maxwell's
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NP, we present the calculation results obtained by using Maxwell's
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equations coupled with electron kinetics equations for different
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equations coupled with electron kinetics equations for different
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- radii for resonant and non-resonant conditions. In this case, the
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+ radii for resonant and non-resonant conditions at peak intensity 10$^{12}$~W/cm$^2$ and $\lambda = 800~nm$. In this case, the
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geometry of the EHP distribution can strongly deviate from the
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geometry of the EHP distribution can strongly deviate from the
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- intensity distribution given by Mie theory. Two main reasons cause
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+ intensity distribution given by the Mie theory. Two main reasons cause
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the deviation: (i) non-stationarity of interaction between
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the deviation: (i) non-stationarity of interaction between
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electromagnetic pulse and NP (ii) nonlinear effects, taking place due
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electromagnetic pulse and NP (ii) nonlinear effects, taking place due
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to transient optical changes in Si. The non-stationary intensity
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to transient optical changes in Si. The non-stationary intensity
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deposition during \textit{fs} pulse results in different time delays
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deposition during \textit{fs} pulse results in different time delays
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for exciting electric and magnetic resonances inside Si NP because of
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for exciting electric and magnetic resonances inside Si NP because of
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- different quality factors $Q$ of the resonances.
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-
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- In particular, MD resonance (\textit{b1}) has $Q \approx 8$, whereas
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- electric one (\textit{a1}) has $Q \approx 4$. The larger particle
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+ different quality factors $Q$ of the resonances. In particular, MD resonance (\textit{b1}) has $Q \approx 8$, whereas electric one (\textit{a1}) has $Q \approx 4$. The larger particle
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supporting MQ resonance (\textit{b2}) demonstrates $ Q \approx
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supporting MQ resonance (\textit{b2}) demonstrates $ Q \approx
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40$. As soon as the electromagnetic wave period at $\lambda = 800$~nm
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40$. As soon as the electromagnetic wave period at $\lambda = 800$~nm
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is $\approx 2.7$~\textit{fs}, one needs about 10~\textit{fs} to pump the ED,
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is $\approx 2.7$~\textit{fs}, one needs about 10~\textit{fs} to pump the ED,
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@@ -566,7 +549,7 @@ license.
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place on a 10~\textit{fs} scale it results in the excitation of the
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place on a 10~\textit{fs} scale it results in the excitation of the
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low-\textit{Q} ED resonance, which dominates MD and MQ independently
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low-\textit{Q} ED resonance, which dominates MD and MQ independently
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on the exact size of NPs. Moreover, during the first optical cycle
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on the exact size of NPs. Moreover, during the first optical cycle
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- there is no multipole modes structure inside of NP, which results
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+ there is no multipole modes structure inside NP, which results
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into a very similar field distribution for all sizes of NP under
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into a very similar field distribution for all sizes of NP under
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consideration as shown in Fig.~\ref{plasma-grid}(a,e,i) . We address
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consideration as shown in Fig.~\ref{plasma-grid}(a,e,i) . We address
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to this phenomena as \textit{'Stage~1'}. This stage demonstrates the
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to this phenomena as \textit{'Stage~1'}. This stage demonstrates the
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@@ -585,7 +568,7 @@ license.
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in the front side of the Si NP. This effect dominates for the
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in the front side of the Si NP. This effect dominates for the
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smallest NP with $R=75$~nm in Fig.~\ref{plasma-grid}(b), where ED
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smallest NP with $R=75$~nm in Fig.~\ref{plasma-grid}(b), where ED
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mode is tuned far away from the resonance (see Fig.~\ref{mie-fdtd}(c)
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mode is tuned far away from the resonance (see Fig.~\ref{mie-fdtd}(c)
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- for field suppression inside of NP predicted by Mie theory). At this
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+ for field suppression inside NP predicted by the Mie theory). At this
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stage, the density of EHP ($N_e < 10^{20}$~cm$^2$) is still not high
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stage, the density of EHP ($N_e < 10^{20}$~cm$^2$) is still not high
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enough to significantly affect the optical properties of the NP.
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enough to significantly affect the optical properties of the NP.
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@@ -605,7 +588,7 @@ license.
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the MD resonant size for $R = 115$~nm the $G_{N_e} < 0$ due to
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the MD resonant size for $R = 115$~nm the $G_{N_e} < 0$ due to
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the fact that EHP is dominantly localized in the back side of the NP.
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the fact that EHP is dominantly localized in the back side of the NP.
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- Once again, due to the presence of a continuous pumping the Stage~3 is
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+ In other words, due to the presence of a quasi-stationary pumping the Stage~3 is
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superposed with the Stage~1 field pattern, resulting in an additional
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superposed with the Stage~1 field pattern, resulting in an additional
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EHP localized in the front side. This can be seen when comparing
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EHP localized in the front side. This can be seen when comparing
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result from the Mie theory in Fig.~\ref{mie-fdtd}(d) and result of
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result from the Mie theory in Fig.~\ref{mie-fdtd}(d) and result of
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@@ -630,10 +613,10 @@ license.
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Higher excitation conditions are followed by larger values of
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Higher excitation conditions are followed by larger values of
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electric field amplitude, which lead to the appearance of high EHP
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electric field amplitude, which lead to the appearance of high EHP
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densities causing a significant change in the optical properties of
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densities causing a significant change in the optical properties of
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- silicon according to the equations (\ref{Index}). From Mie theory, the initial (at the end of Stage~3) space pattern of
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+ silicon according to the equations (\ref{Index}). From the Mie theory, the initial (at the end of Stage~3) space pattern of
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optical properties is non-homogeneous. When non-homogeneity of
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optical properties is non-homogeneous. When non-homogeneity of
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optical properties becomes strong enough it leads to the
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optical properties becomes strong enough it leads to the
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- reconfiguration of the electric field inside of NP and vice versa. We
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+ reconfiguration of the electric field inside NP and vice versa. We
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refer to these strong nonlinear phenomena as \textit{'Stage~4'}. In
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refer to these strong nonlinear phenomena as \textit{'Stage~4'}. In
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general the reconfiguration of the electric field is unavoidable as
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general the reconfiguration of the electric field is unavoidable as
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far as the result from the Mie theory comes with the assumption of
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far as the result from the Mie theory comes with the assumption of
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