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@@ -513,7 +513,7 @@ license.
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size resonance value, corresponding to $R \approx 105$~nm. In
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size resonance value, corresponding to $R \approx 105$~nm. In
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contrast, for larger sizes, the intensity is enhanced in the back
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contrast, for larger sizes, the intensity is enhanced in the back
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side of the NP as demonstrated in Fig.~\ref{mie-fdtd}(d). In fact,
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side of the NP as demonstrated in Fig.~\ref{mie-fdtd}(d). In fact,
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- very similar EHP distributions can be obtained by applying Maxwell's
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+ rather similar EHP distributions can be obtained by applying Maxwell's
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equations coupled with the rate equation for relatively weak
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equations coupled with the rate equation for relatively weak
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excitation with EHP concentration of $N_e \approx 10^{20}$~cm$^{-3}$,
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excitation with EHP concentration of $N_e \approx 10^{20}$~cm$^{-3}$,
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see Fig.~\ref{mie-fdtd}(e,f). The optical properties do not change
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see Fig.~\ref{mie-fdtd}(e,f). The optical properties do not change
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@@ -540,7 +540,7 @@ license.
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evolution stages during pulse duration. Typical change of the
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evolution stages during pulse duration. 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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Fig.~\ref{plasma-grid}. For better visual representation of time
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- scale of the whole incident pulse and its single optical cycle we put a
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+ scale of a single optical cycle we put a
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squared electric field profile on all plots in
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squared electric field profile on all plots in
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Fig.~\ref{time-evolution} in gray color as a backgroud image (note
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Fig.~\ref{time-evolution} in gray color as a backgroud image (note
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linear time scale on the left column and logarithmic scale on the
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linear time scale on the left column and logarithmic scale on the
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@@ -563,14 +563,14 @@ license.
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electric one (\textit{a1}) has $Q \approx 4$. The larger particle
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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 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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20~\textit{fs} for the MD, and about 100~\textit{fs} for the MQ.
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20~\textit{fs} for the MD, and about 100~\textit{fs} for the MQ.
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According to these considerations, after few optical cycles taking
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According to these considerations, after few optical cycles taking
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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 of NP, which results
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- into a very similar field distribution for all size 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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initial penetration of electromagnetic field into the NP during the
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initial penetration of electromagnetic field into the NP during the
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@@ -597,9 +597,9 @@ license.
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the stationary intensity pattern corresponding to the Mie-based
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the stationary intensity pattern corresponding to the Mie-based
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intensity distribution at the \textit{'Stage~3'} (see
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intensity distribution at the \textit{'Stage~3'} (see
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Fig.~\ref{plasma-grid}). The EHP density for the most volume of NP is
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Fig.~\ref{plasma-grid}). The EHP density for the most volume of NP is
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- still relatively small to affect the EHP evolution or for diffusion,
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+ still relatively small to affect the EHP evolution,
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but is already high enough to change the local optical
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but is already high enough to change the local optical
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- properties. Below the MD resonance $R \approx 100$~nm, the EHP is
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+ properties. Below the MD resonance ($R = 75$~nm), the EHP is
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mostly localized in the front side of the NP as shown in
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mostly localized in the front side of the NP as shown in
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Fig.~\ref{plasma-grid}(c). The highest quasi-stationary asymmetry factor
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Fig.~\ref{plasma-grid}(c). The highest quasi-stationary asymmetry factor
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$G_{N_e} \approx 0.5$--$0.6$ is achieved in this case. At the MD
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$G_{N_e} \approx 0.5$--$0.6$ is achieved in this case. At the MD
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@@ -609,12 +609,12 @@ license.
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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 presence of continous pumping the Stage~3 is
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Once again, due to presence of continous pumping the Stage~3 is
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- superposed with Stage~1 field pattern, resulting in the EHP localized
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- in the front side. This can be seen when comparing result from the
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- Mie theory in Fig.~\ref{mie-fdtd}(d) and result of full 3D simulation
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- in Fig.~\ref{mie-fdtd}(f). Note that pumping of NP significantly
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- changes during a single optical cycle, this leads to a large
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- variation of asymmetry factor $G_{N_e}$ at first stage. This
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+ superposed with Stage~1 field pattern, resulting in the additional
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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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+ full 3D simulation in Fig.~\ref{mie-fdtd}(f). Note that pumping of NP
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+ significantly changes during a single optical cycle, this leads to a
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+ large variation of asymmetry factor $G_{N_e}$ at first stage. This
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variation stedialy decrease as it goes to Stage~3.
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variation stedialy decrease as it goes to Stage~3.
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The explain this we need to consider time evolution of mean EHP
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The explain this we need to consider time evolution of mean EHP
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@@ -628,14 +628,50 @@ license.
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optical cycle of the incident wave. This delay causes a large value
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optical cycle of the incident wave. This delay causes a large value
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of the assymetry factor during first stage. However, as soon as mean
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of the assymetry factor during first stage. However, as soon as mean
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EHP density increases the contribution of this pumping steps to
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EHP density increases the contribution of this pumping steps to
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- resulting assymetry becomes smallar and the variation of $G_{N_e}$
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- synced with the period of incident light decreases.
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+ resulting assymetry becomes smallar and the synced with the period of
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+ incident light variation of $G_{N_e}$ decreases.
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%A bookmark by Kostya
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%A bookmark by Kostya
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- For the higher excitation conditions, the optical properties of
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- silicon change significantly according to the equations
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- (\ref{Index}). As a result, the we observe the forward shifting of
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+ Higher excitation conditions are followed with large values of
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+ electric field amplitude, which lead to apperance of high EHP
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+ densities causing a significant change of optical properties of
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+ silicon according to the equations (\ref{Index}). As it follows from
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+ 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 becomes strong enougth it leads to the
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+ reconfiguration of the electric field inside of NP and vice versa. We
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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 obligatory as
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+ far as the result from the Mie theory comes with the assumption of
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+ homogeneous optical properties in a spherical NP.
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+
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+ This way evolution of EHP density during Stage~4 depends on the
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+ result of multipole modes superposition in the end of Stage~3 and is
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+ quite different as we change the size of NP. For $R=75$~nm and
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+ $R=100$~nm we observe a front side asymmetry before Stage~4, however,
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+ the origin of it is quite different. The $R=75$~nm NP is out of
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+ resonance, moreover, Mie field pattern and the one which comes from
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+ Stage~1 are quite similar. As soon as EHP density becomes high enough
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+ to change optical properties the NP is still out of resonanse,
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+ however, presence of EHP increases absorption in accordance with
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+ (\ref{Index}). This effectively leads to a kind of screening, it
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+ becomes harder for incident wave to penetrate deep into EHP. Finally,
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+ this finishes spilling the NP`s volume with plasma reducing the
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+ asymmetry, see Fig.~\ref{plasma-grid}(d).
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+
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+ For $R=100$~nm the evolution to during the final stage goes in a
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+ similar way, with a notable exception regarding MD resonance. As
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+ soon as presence of EHP incresases the absorption, it suppresses the
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+ MD resonance with symmetric filed pattern, thus, the asymmetry factor
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+ can be increased. This was actualy observed in
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+ Fig.~\ref{time-evolution}(d) with a local maxima near 100~\textit{fs}
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+ mark.
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+
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+ The last NP with $R=115$~nm shows the most complex behavior during
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+ the Stage~4.
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+
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+ as a result, the we observe the forward shifting of
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EHP density maximum. Therefore, EHP is localized in the front part of
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EHP density maximum. Therefore, EHP is localized in the front part of
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the NP, influencing the asymmetry factor $G_{N_e}$ in
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the NP, influencing the asymmetry factor $G_{N_e}$ in
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Fig.~\ref{time-evolution}. Approximately at the pulse peak, the
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Fig.~\ref{time-evolution}. Approximately at the pulse peak, the
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@@ -652,7 +688,7 @@ license.
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induced transient optical response and the effect of newly formed
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induced transient optical response and the effect of newly formed
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EHP. This way, the distribution becomes more homogeneous and the
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EHP. This way, the distribution becomes more homogeneous and the
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effect is likely to be enhanced by electron diffusion inside Si
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effect is likely to be enhanced by electron diffusion inside Si
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- NPs. We refer to these nonlinear phenomena as \textit{'Stage~4'}.
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+ NPs.
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It is worth noting that it is possible to achieve a formation of
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It is worth noting that it is possible to achieve a formation of
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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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