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@@ -139,7 +139,6 @@
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\includegraphics{head_foot/dates}
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\includegraphics{head_foot/dates}
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& \noindent\normalsize
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& \noindent\normalsize
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-
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{The concept of nonlinear all-dielectric nanophotonics based on high
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{The concept of nonlinear all-dielectric nanophotonics based on high
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refractive index (e.g., silicon) nanoparticles supporting magnetic
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refractive index (e.g., silicon) nanoparticles supporting magnetic
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optical response has recently emerged as a powerful tool for ultrafast
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optical response has recently emerged as a powerful tool for ultrafast
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@@ -243,7 +242,7 @@ distributions in silicon nanoparticle around a magnetic resonance.}
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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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Recently, plasma explosion imaging technique has been used to
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-observe electron-hole plasmas (EHP), produced by femtosecond lasers,
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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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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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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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in positive direction of $z$ axis. For the NP with
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@@ -259,8 +258,8 @@ NPs, such as silicon (Si), germanium (Ge) etc.
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In this Letter, we show that ultra-short laser-based EHP
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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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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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to a strongly inhomogeneous carrier distribution. To reveal and study
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-this effect, we perform a full-wave numerical simulation of the
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-intense femtosecond (\textit{fs}) laser pulse interaction with a
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+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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silicon NP supporting Mie resonances and two-photon free carrier
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silicon NP supporting Mie resonances and two-photon free carrier
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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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@@ -270,20 +269,15 @@ permittivity is calculated for NPs of several sizes. The obtained
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results propose a novel strategy to create complicated non-symmetrical
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results propose a novel strategy to create complicated non-symmetrical
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nanostructures by using single photo-excited spherical silicon
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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
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-($\approx$$\lambda$$^3$/100) supporting the formation of small
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-metalized parts inside the NP. In fact, such effects transform an
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-all-dielectric NP to a hybrid one strongly extending functionality of
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-the ultrafast optical nanoantennas.
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+subwavelength scale ($< \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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+an all-dielectric NP to a hybrid metall-dielectric one strongly
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+extending functionality of the ultrafast optical nanoantennas.
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%Plan:
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%Plan:
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%\begin{itemize}
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%\begin{itemize}
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-%\item Fig.1: Beautiful conceptual picture
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-%\item Fig.2: Temporal evolution of EHP in NP with different diameters
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-%at fixed intensity, in order to show that we have the highest
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-%asymmetry around magnetic dipole (MD) resonance. This would be really
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-%nice!
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+
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%\item Fig.3: Temporal evolution of EHP in NP with fixed diameter (at
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%\item Fig.3: Temporal evolution of EHP in NP with fixed diameter (at
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%MD) at different intensities, in order to show possible regimes of
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%MD) at different intensities, in order to show possible regimes of
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%plasma-patterning of NP volume. It would be nice, if we will show
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%plasma-patterning of NP volume. It would be nice, if we will show
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@@ -316,19 +310,19 @@ the critical density and above, silicon acquires metallic properties
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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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The process of three-dimensional photo-generation of the EHP in
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-silicon NPs has not been modeled before in
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-time-domain. Therefore, herein we propose a model considering
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-ultrashort laser interactions with a resonant silicon sphere, where
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-the EHP is generated via one- and two-photon absorption processes.
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-Importantly, we also consider nonlinear feedback of the material by
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-taking into account the intraband light absorption on the generated
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-free carriers. To simplify our model, we neglect free carrier
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-diffusion at the considered short time scales. In fact, the aim of the
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-present work is to study the EHP dynamics \textit{during} ultra-short
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-laser interaction with the NP. The created electron-hole
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-plasma then will recombine, however, as its existence modifies both
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+silicon NPs has not been modeled before in time-domain. Therefore,
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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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+and two-photon absorption processes. Importantly, we also consider
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+nonlinear feedback of the material by taking into account the
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+intraband light absorption on the generated free carriers. To simplify
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+our model, we neglect free carrier diffusion due to the considered
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+short time scales. In fact, the aim of the present work is to study
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+the EHP dynamics \textit{during} ultra-short (\textit{fs}) laser
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+interaction with the NP. The created electron-hole modifies both
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laser-particle interaction and, hence, the following particle
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laser-particle interaction and, hence, the following particle
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-evolution.
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+evolution. However, the plasma then will recombine at picosecond time
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+scale.
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\subsection{Light propagation}
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\subsection{Light propagation}
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@@ -395,21 +389,6 @@ To account for the material ionization that is induced by a
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sufficiently intense laser field inside the particle, we couple
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sufficiently intense laser field inside the particle, we couple
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Maxwell's equations with the kinetic equation for the electron-hole
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Maxwell's equations with the kinetic equation for the electron-hole
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plasma as described below.
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plasma as described below.
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-% \begin{figure*}[ht!]
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-% \centering
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-% \includegraphics[width=120mm]{fig2.png}
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-% \caption{\label{fig2} Free carrier density snapshots of electron
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-% plasma evolution inside Si NP taken a) $30\:f\!s$ b) $10\:f\!s$
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-% before the pulse peak, c) at the pulse peak, d) $10\:f\!s$ e)
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-% $30\:f\!s$ after the pulse peak. Pulse duration $50\:f\!s$
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-% (FWHM). Wavelength $800$~nm in air. Radius of the NP
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-% $R \approx 105$~nm, corresponding to the resonance condition. Graph
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-% shows the dependence of the asymmetric parameter of electron plasma
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-% density on the average electron density in the front half of the NP.
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-% $n_{cr} = 5\cdot{10}^{21}$~cm$^{-3}$ is the critical plasma
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-% resonance electron density for silicon.}
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-% \end{figure*}
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-
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The time-dependent conduction-band carrier density evolution is
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The time-dependent conduction-band carrier density evolution is
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described by a rate equation that was proposed by van Driel
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described by a rate equation that was proposed by van Driel
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@@ -438,7 +417,7 @@ Einstein formula $D = k_B T_e \tau/m^* \approx (1\div2)\cdot{10}^{-3}$ m$^2$/s
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$\tau=1$~\textit{fs} is the collision time, $m^* = 0.18 m_e$ is the effective
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$\tau=1$~\textit{fs} is the collision time, $m^* = 0.18 m_e$ is the effective
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mass), where $T_e \approx 2*{10}^4$ K for $N_e$ close to $N_{cr}$ \cite{Ramer2014}. It
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mass), where $T_e \approx 2*{10}^4$ K for $N_e$ close to $N_{cr}$ \cite{Ramer2014}. It
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means that during the pulse duration ($\approx 50$~\textit{fs}) the diffusion
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means that during the pulse duration ($\approx 50$~\textit{fs}) the diffusion
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-length will be around $5\div10$~nm for $N_e$ close to $N_{cr}$.
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+length will be around $5--10$~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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@@ -454,35 +433,6 @@ length will be around $5\div10$~nm for $N_e$ close to $N_{cr}$.
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$\vec{E}$ is along $X$ axis.}
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$\vec{E}$ is along $X$ axis.}
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\end{figure}
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\end{figure}
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-%\begin{figure*}[ht!] \label{EHP}
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-%\centering
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-%\begin{tabular*}{0.76\textwidth}{ c@{\extracolsep{\fill}} c@{\extracolsep{\fill}} c@{\extracolsep{\fill}} c@{\extracolsep{\fill}} c}
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-%$-80\:f\!s$&$-60\:f\!s$&$-30\:f\!s$&$ -20\:f\!s$&$ -10\:f\!s$\\
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-%\end{tabular*}
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-%{\setlength\topsep{-1pt}
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-%\begin{flushleft}
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-%$R=75$~nm
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-%\end{flushleft}}
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-%\includegraphics[width=0.9\textwidth]{2nm_75}
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-%{\setlength\topsep{-1pt}
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-%\begin{flushleft}
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-%$R=100$~nm
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-%\end{flushleft}}
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-%\includegraphics[width=0.9\textwidth]{2nm_100}
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-%{\setlength\topsep{-1pt}
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-%\begin{flushleft}
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-%$R=115$~nm
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-%\end{flushleft}}
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-%\includegraphics[width=0.9\textwidth]{2nm_115}
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-%\caption{\label{plasma-105nm} Evolution of electron density $n_e$
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- % (using $10^{\,20} \ {\rm cm}^{-3}$ units) for
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- %(a$\,$--$\,$e)~$R=75$~nm, (f$\,$--$\,$j$\,$)~$R=100$~nm, and
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- %($\,$k$\,$--$\,$o)~$R=115$~nm. Gaussian pulse duration $80\:f\!s$,
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- %snapshots are taken before the pulse maxima, the corresponding
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- %time-shifts are shown in the top of each column. Laser irradiation
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- %fluences are (a-e) $0.12$~J/cm$^2$, (f-o) $0.16$~J/cm$^2$.}
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-%\end{figure*}
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-
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The changes of the real and imaginary parts of the permittivity
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The changes of the real and imaginary parts of the permittivity
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associated with the time-dependent free carrier response
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associated with the time-dependent free carrier response
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\cite{Sokolowski2000} can be derived from equations (\ref{Maxwell},
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\cite{Sokolowski2000} can be derived from equations (\ref{Maxwell},
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@@ -513,17 +463,17 @@ license.
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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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- \caption{\label{fig3} Temporal EHP (a, c, e) and asymmetry factor
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- $G_{N_e}$ (b, d, f) evolution for different Si nanoparticle radii
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- (a, b) $R = 75$~nm, (c, d) $R = 100$~nm, (e, f) $R = 115$~nm. Pulse
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+ \caption{\label{time-evolution} Temporal EHP (a, c, e) and asymmetry factor
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+ $G_{N_e}$ (b, d, f) evolution for different Si nanoparticle radii of
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+ (a, b) $R = 75$~nm, (c, d) $R = 100$~nm, and (e, f) $R = 115$~nm. Pulse
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duration $50$~\textit{fs} (FWHM). Wavelength $800$~nm in air. (b,
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duration $50$~\textit{fs} (FWHM). Wavelength $800$~nm in air. (b,
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- d, f) Different stages of EHP evolution shown in Fig.~\ref{fig2}
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+ d, f) Different stages of EHP evolution shown in Fig.~\ref{plasma-grid}
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are indicated. The temporal evolution of Gaussian beam intensity is
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are indicated. The temporal evolution of Gaussian beam intensity is
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also shown. Peak laser fluence is fixed to be $0.125$~J/cm$^2$.}
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also shown. Peak laser fluence is fixed to be $0.125$~J/cm$^2$.}
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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{fig2} 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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$1-4$: (1) first optical cycle, (2) extremum at few optical cycles,
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@@ -574,8 +524,8 @@ license.
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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 revealing the EHP evolution stages during pulse duration
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modeling revealing the EHP evolution stages during pulse duration
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- shown in Fig.~\ref{fig2} and the temporal/EHP dependent evolution of
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- the asymmetry factor $G_{N_e}$ in Fig.~\ref{fig3}.
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+ shown in Fig.~\ref{plasma-grid} and the temporal/EHP dependent evolution of
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+ the asymmetry factor $G_{N_e}$ in Fig.~\ref{time-evolution}.
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% Fig. \ref{Mie} demonstrates the temporal evolution of the EHP
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% Fig. \ref{Mie} demonstrates the temporal evolution of the EHP
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% generated inside the silicon NP of $R \approx 105$~nm. Here,
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% generated inside the silicon NP of $R \approx 105$~nm. Here,
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@@ -588,7 +538,7 @@ license.
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% asymmetry parameter, $G$, which is defined as a relation between the
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% asymmetry parameter, $G$, which is defined as a relation between the
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% average electron density generated in the front side of the
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% average electron density generated in the front side of the
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% NP and the average electron density in the back side, as
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% NP and the average electron density in the back side, as
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-% shown in Fig. \ref{fig2}. During the femtosecond pulse interaction,
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+% shown in Fig. \ref{plasma-grid}. During the femtosecond pulse interaction,
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% this parameter significantly varies.
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% this parameter significantly varies.
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@@ -617,10 +567,10 @@ license.
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of the low-\textit{Q} electric dipole resonance independently on the
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of the low-\textit{Q} electric dipole resonance independently on the
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exact size of NPs and with the EHP concentration mostly on the front
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exact size of NPs and with the EHP concentration mostly on the front
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side of the NPs. We address to this phenomena as \textit{'Stage 1'},
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side of the NPs. We address to this phenomena as \textit{'Stage 1'},
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- as shown in Figs.~\ref{fig2} and~\ref{fig2}. The first stage at the
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+ as shown in Figs.~\ref{plasma-grid} and~\ref{plasma-grid}. The first stage at the
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first optical cycle demonstrates the dominant electric dipole
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first optical cycle demonstrates the dominant electric dipole
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resonance effect on the intensity/EHP density distribution inside the
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resonance effect on the intensity/EHP density distribution inside the
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- NPs in Fig.~\ref{fig2}(a,e,j) and~\ref{fig3}. The larger the NPs size
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+ NPs in Fig.~\ref{plasma-grid}(a,e,j) and~\ref{time-evolution}. The larger the NPs size
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is, the higher the NP asymmetry $G_{N_e}$ is achieved.
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is, the higher the NP asymmetry $G_{N_e}$ is achieved.
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\textit{'Stage 2'} corresponds to further electric field oscillations
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\textit{'Stage 2'} corresponds to further electric field oscillations
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@@ -634,11 +584,11 @@ license.
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A number of optical cycles ($>$10 or $t>$25~\textit{fs}) is necessary
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A number of optical cycles ($>$10 or $t>$25~\textit{fs}) is necessary
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to achieve the stationary intensity pattern corresponding to the
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to achieve the stationary intensity pattern corresponding to the
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Mie-based intensity distribution at the \textit{'Stage $3$'} (see
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Mie-based intensity distribution at the \textit{'Stage $3$'} (see
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- Fig.~\ref{fig3}). The EHP density is still relatively small to affect
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+ Fig.~\ref{time-evolution}). The EHP density is still relatively small to affect
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the EHP evolution or for diffusion, but is already high enough to
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the EHP evolution or for diffusion, but is already high enough to
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change the local optical properties. Below the magnetic dipole
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change the local optical properties. Below the magnetic dipole
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resonance $R \approx 100$~nm, the EHP is mostly localized in the
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resonance $R \approx 100$~nm, the EHP is mostly localized in the
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- front side of the NP as shown in Fig.~\ref{fig2}(c). The highest
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+ front side of the NP as shown in Fig.~\ref{plasma-grid}(c). The highest
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stationary asymmetry factor $G_{N_e} \approx 0.5\div0.6$ is achieved
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stationary asymmetry factor $G_{N_e} \approx 0.5\div0.6$ is achieved
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in this case. At the magnetic dipole resonance conditions, the EHP
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in this case. At the magnetic dipole resonance conditions, the EHP
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distribution has a toroidal shape and is much closer to the
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distribution has a toroidal shape and is much closer to the
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@@ -652,13 +602,13 @@ license.
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contributes to the forward shifting of EHP density
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contributes to the forward shifting of EHP density
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maximum. Therefore, EHP is localized in the front part of the NP,
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maximum. Therefore, EHP is localized in the front part of the NP,
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influencing the asymmetry factor $G_{N_e}$ in
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influencing the asymmetry factor $G_{N_e}$ in
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- Fig.~\ref{fig3}. Approximately at the pulse peak, the critical
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+ Fig.~\ref{time-evolution}. Approximately at the pulse peak, the critical
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electron density $N_{cr} = 5\cdot{10}^{21}$~cm$^{-3}$ for silicon,
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electron density $N_{cr} = 5\cdot{10}^{21}$~cm$^{-3}$ for silicon,
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which corresponds to the transition to quasi-metallic state
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which corresponds to the transition to quasi-metallic state
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$Re(\epsilon) \approx 0$ and to the electron plasma resonance, is
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$Re(\epsilon) \approx 0$ and to the electron plasma resonance, is
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overcome. Further irradiation leads to a decrease in the asymmetry
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overcome. Further irradiation leads to a decrease in the asymmetry
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parameter down to $G_{N_e} = 0$ for higher EHP densities, as one can
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parameter down to $G_{N_e} = 0$ for higher EHP densities, as one can
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- observe in Fig.~\ref{fig2}(d, h, l).
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+ observe in Fig.~\ref{plasma-grid}(d, h, l).
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As the EHP acquires quasi-metallic properties at stronger excitation
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As the EHP acquires quasi-metallic properties at stronger excitation
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$N_e > 5\cdot{10}^{21}$~cm$^{-3}$, the EHP distribution evolves
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$N_e > 5\cdot{10}^{21}$~cm$^{-3}$, the EHP distribution evolves
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@@ -672,7 +622,7 @@ license.
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deeply subwavelength EHP regions due to high field localization. The
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deeply subwavelength EHP regions due to high field localization. The
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smallest EHP localization and the larger asymmetry factor are
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smallest EHP localization and the larger asymmetry factor are
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achieved below the magnetic dipole resonant conditions for $R < 100$~nm.
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achieved below the magnetic dipole resonant conditions for $R < 100$~nm.
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- Thus, the EHP distribution in Fig.~\ref{fig2}(c) is optimal for
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+ Thus, the EHP distribution in Fig.~\ref{plasma-grid}(c) is optimal for
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symmetry breaking in Si NP, as it results in the larger asymmetry
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symmetry breaking in Si NP, as it results in the larger asymmetry
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factor $G_{N_e}$ and higher electron densities $N_e$. We stress here
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factor $G_{N_e}$ and higher electron densities $N_e$. We stress here
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that such regime could be still safe for NP due to the very small
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that such regime could be still safe for NP due to the very small
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@@ -682,8 +632,8 @@ license.
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% factor on scattering directions}
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% factor on scattering directions}
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% \begin{figure}[ht] \centering
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% \begin{figure}[ht] \centering
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-% \includegraphics[width=90mm]{fig3.png}
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-% \caption{\label{fig3} a) Scattering efficiency factor $Q_{sca}$
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+% \includegraphics[width=90mm]{time-evolution.png}
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+% \caption{\label{time-evolution} a) Scattering efficiency factor $Q_{sca}$
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% dependence on the radius $R$ of non-excited silicon NP
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% dependence on the radius $R$ of non-excited silicon NP
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% calculated by Mie theory; b) Parameter of forward/backward scattering
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% calculated by Mie theory; b) Parameter of forward/backward scattering
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% dependence on the radius $R$ calculated by Mie theory for non-excited
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% dependence on the radius $R$ calculated by Mie theory for non-excited
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@@ -698,7 +648,7 @@ license.
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% evolution during ultrashort laser irradiation. A brief analysis of
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% evolution during ultrashort laser irradiation. A brief analysis of
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% the initial intensity distribution inside the NP given by
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% the initial intensity distribution inside the NP given by
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% the classical Mie theory for homogeneous spherical particles
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% the classical Mie theory for homogeneous spherical particles
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-% \cite{Mie1908} can be useful in this case. Fig. \ref{fig3}(a, b)
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+% \cite{Mie1908} can be useful in this case. Fig. \ref{time-evolution}(a, b)
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% shows the scattering efficiency and the asymmetry parameter for
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% shows the scattering efficiency and the asymmetry parameter for
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% forward/backward scattering for non-excited silicon NPs of
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% forward/backward scattering for non-excited silicon NPs of
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% different radii calculated by Mie theory \cite{Mie1908}. Scattering
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% different radii calculated by Mie theory \cite{Mie1908}. Scattering
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@@ -730,7 +680,7 @@ license.
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% $n_{cr} = 5\cdot{10}^{21}~cm^{-3}$, and $G$ is asymmetry of EHP,
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% $n_{cr} = 5\cdot{10}^{21}~cm^{-3}$, and $G$ is asymmetry of EHP,
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% defined previously. The calculation results for different radii of
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% defined previously. The calculation results for different radii of
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% silicon NPs and electron densities are presented in
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% silicon NPs and electron densities are presented in
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-% Fig. \ref{fig3}(c). One can see, that the maximum value are achieved
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+% Fig. \ref{time-evolution}(c). One can see, that the maximum value are achieved
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% for the NPs, that satisfy both initial maximum forward
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% for the NPs, that satisfy both initial maximum forward
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% scattering and not far from the first resonant condition. For larger
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% scattering and not far from the first resonant condition. For larger
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% NPs, lower values of EHP asymmetry factor are obtained, as
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% NPs, lower values of EHP asymmetry factor are obtained, as
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