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  103. %%%TITLE, AUTHORS AND ABSTRACT%%%
  104. \twocolumn[
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  109. \includegraphics{head_foot/DOI} & \noindent\LARGE{\textbf{Photo-generated Electron-Hole Plasma-Induced Symmetry Breaking in Spherical Silicon Nanoparticles}} \\%Article title goes here instead of the text "This is the title"
  110. \vspace{0.3cm} & \vspace{0.3cm} \\
  111. & \noindent\large{Anton Rudenko,$^{\ast}$\textit{$^{a}$} Konstantin Ladutenko,\textit{$^{b}$} Sergey Makarov\textit{$^{b}$} and Tatiana E. Itina\textit{$^{a}$$^{b}$}
  112. \textit{$^{a}$~Laboratoire Hubert Curien, UMR CNRS 5516, University of Lyon/UJM, 42000, Saint-Etienne, France }
  113. \textit{$^{b}$~ITMO University, Kronverksiy pr. 49, St. Petersburg, Russia}
  114. } \\%Author names go here instead of "Full name", etc.
  115. \includegraphics{head_foot/dates} & \noindent\normalsize {The concept
  116. of nonlinear all-dielectric nanophotonics based on high refractive
  117. index (e.g., silicon) nanoparticles supporting magnetic optical
  118. response has recently emerged as a powerful tool for ultrafast
  119. all-optical modulation at nanoscale. A strong modulation can be
  120. achieved via photo-generation of dense electron-hole plasma in the
  121. regime of simultaneous excitation of electric and magnetic optical
  122. resonances, resulting in an effective transient reconfiguration of
  123. nanoparticle scattering properties. Because only homogeneous plasma generation was previously considered in the photo-excited nanoparticle, a possibility of symmetry breaking, however, remain unexplored. To examine these effects, numerical modeling is performed. Based on the simulation results, we propose an original concept of a well-controlled deeply subwavelength
  124. ($\approx$$\lambda$$^3$/100) plasma-induced nanopatterning of
  125. spherical silicon nanoparticles. In particular, the revealed strong
  126. symmetry breaking in the initially symmetrical nanoparticle, which is observed during
  127. ultrafast photoexcitation near the magnetic dipole resonance, enables a considerable increase in the precision of laser-induced nanotreatment. Importantly, the proposed
  128. ultrafast manipulation of the nanoparticle inherent structure and symmetry
  129. paves a way to the novel principles that are also promising for nonlinear optical nanodevices.}
  130. \end{tabular}
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  132. ]%%%END OF TITLE, AUTHORS AND ABSTRACT%%%
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  136. %%%FOOTNOTES%%%
  137. \footnotetext{\textit{$^{a}$~Univ Lyon, UJM-St-Etienne, CNRS UMR 5516,
  138. F-42000, Saint-Etienne, France}} \footnotetext{\textit{$^{b}$~ITMO
  139. University, Kronverksiy pr. 49, St. Petersburg, Russia}}
  140. % Please use \dag to cite the ESI in the main text of the article.
  141. % If you article does not have ESI please remove the the \dag symbol
  142. % from the title and the footnotetext below.
  143. % \footnotetext{\dag~Electronic Supplementary Information (ESI)
  144. % available: [details of any supplementary information available
  145. % should be included here]. See DOI:10.1039/b000000x/} %additional
  146. % addresses can be cited as above using the lower-case letters, c, d,
  147. % e... If all authors are from the same address, no letter is required
  148. % \footnotetext{\ddag~Additional footnotes to the title and authors can
  149. % be included \emph{e.g.}\ `Present address:' or `These authors
  150. % contributed equally to this work' as above using the symbols: \ddag,
  151. % \textsection, and \P. Please place the appropriate symbol next to the
  152. % author's name and include a \texttt{\textbackslash footnotetext} entry
  153. % in the the correct place in the list.}
  154. %%%END OF FOOTNOTES%%%
  155. %%%MAIN TEXT%%%%
  156. \section{Introduction}
  157. All-dielectric nonlinear nanophotonics based on high refractive index
  158. dielectric has become prospective paradigm in modern optics, owing to
  159. recent advances in harmonics generation~\cite{shcherbakov2014enhanced,
  160. yang2015nonlinear, makarov2016self, shorokhov2016multifold} and
  161. ultrafast all-optical modulation~\cite{iyer2015reconfigurable,
  162. makarov2015tuning, shcherbakov2015ultrafast, yang2015nonlinear,
  163. baranov2016nonlinear, baranov2016tuning}. In fact, all-dielectric
  164. nanoantennas and metasurfaces possess much smaller parasitic Joule
  165. losses at high intensities as compared with their plasmonic
  166. counterparts, whereas their nonlinear properties are comparable. More
  167. importantly, the unique properties of the nonlinear all-dielectric
  168. nanodevices are due to existing of both electric and magnetic optical
  169. resonances in visible and near IR
  170. ranges~\cite{kuznetsov2016optically}. For instance, even slight
  171. variation of dielectric permittivity around magnetic dipole resonance
  172. leads to significant changes of optical properties (transmittance or
  173. reflectance) of all-dielectric nanoantennas~\cite{makarov2015tuning,
  174. baranov2016nonlinear, baranov2016tuning} and
  175. metasurfaces~\cite{iyer2015reconfigurable, shcherbakov2015ultrafast,
  176. yang2015nonlinear}.
  177. In all this works on all-dielectric nonlinear nanostructures, the
  178. building blocks (nanoparticles) were considered as objects with
  179. dielectric permittivity homogeneously distributed over
  180. nanoparticle. Therefore, in order to manipulate by propagation angle
  181. of transmitted light it is necessary to use complicated nanostructures
  182. with reduced symmetry~\cite{albella2015switchable, baranov2016tuning,
  183. shibanuma2016unidirectional}.
  184. \begin{figure}[t] \centering
  185. \includegraphics[width=0.75\linewidth]{Concept}
  186. \caption{Schematic illustration of electron-hole plasma 2D and 1D
  187. distributions in silicon nanoparticle around a magnetic resonance.}
  188. \label{fgr:concept}
  189. \end{figure}
  190. Recently, femtosecond lasers have been used to ionize nanoparticles locally and to produce electron-hole plasmas (EHP) inside them, which have been directly observed by using plasma explosion imaging\cite{Hickstein2014}. Interestingly, inhomogeneous resonant scattering patterns have been experimentally revealed inside a single silicon nanoparticle\cite{Valuckas2017}.
  191. In this Letter, we show that ultra-short laser-based EHP photo-excitation in
  192. a spherical semiconductor (e.g., silicon) nanoparticle leads to a strongly
  193. inhomogeneous carrier distribution. To reveal and study this effect, we
  194. perform a full-wave numerical simulation of the intense
  195. femtosecond (fs) laser pulse interaction with a silicon
  196. nanoparticle supporting Mie resonances and two-photon free carrier generation. In particular, we couple finite-difference time-domain (FDTD)
  197. method used to solve Maxwell equations with kinetic equations describing
  198. nonlinear EHP generation. Three-dimensional transient variation of the material dielectric permittivity is calculated for nanoparticles of several sizes. The obtained results propose a novel strategy to create
  199. complicated non-symmetrical nanostructures by using photo-excited
  200. single spherical silicon nanoparticles. Moreover, we show that dense EHP can
  201. be generated at deeply subwavelength scale
  202. ($\approx$$\lambda$$^3$/100) supporting formation of small metalized
  203. parts inside the nanoparticle, which transforms all-dielectric
  204. nanoparticle to a hybrid one that extends functionality of the ultrafast
  205. optical nanoantennas.
  206. %Plan:
  207. %\begin{itemize}
  208. %\item Fig.1: Beautiful conceptual picture
  209. %\item Fig.2: Temporal evolution of EHP in NP with different diameters
  210. %at fixed intensity, in order to show that we have the highest
  211. %asymmetry around magnetic dipole (MD) resonance. This would be really
  212. %nice!
  213. %\item Fig.3: Temporal evolution of EHP in NP with fixed diameter (at
  214. %MD) at different intensities, in order to show possible regimes of
  215. %plasma-patterning of NP volume. It would be nice, if we will show
  216. %power patterns decencies on intensity for side probe pulse to show beam steering due to symmetry breaking.
  217. %\item Fig.4: (a) Dependence on pulse duration is also interesting. We
  218. %have to show at which duration the asymmetry factor is saturated. (b)
  219. %2D map of asymmetry factor in false colors, where x-axis and y-axis correspond to intensity and NP diameter.
  220. %\end{itemize} %Additionally, if you will manage to calculate
  221. %evolution of scattering power pattern and show considerable effect of
  222. % beam steering, we can try Nanoscale or LPR, because the novelty will
  223. % be very high.
  224. \section{Modeling details}
  225. We focus out attention on silicon because this material is promising
  226. for the implementation of numerous nonlinear photonic devices. This advantage is based on a broad
  227. range of optical nonlinearities, strong two-photon absorption, as well as a possibility of the photo-induced EHP
  228. excitation~\cite{leuthold2010nonlinear}. Furthermore, silicon
  229. nanoantennas demonstrate a sufficiently high damage threshold due to
  230. the large melting temperature ($\approx$1690~K), whereas its nonlinear
  231. optical properties have been extensively studied during last
  232. decays~\cite{Van1987, Sokolowski2000, leuthold2010nonlinear}. High silicon melting point typically preserves structures formed from this material up to the EHP densities on the order of the critical value $n_{cr} \approx 5\cdot{10}^{21}$ cm$^{-3}$ \cite{Korfiatis2007}. At the critical density and above, silicon acquires metallic properties ($Re(\epsilon) < 0$) and contributes to the EHP reconfiguration during ultrashort laser irradiation.
  233. The process of three-dimensional photo-generation of the EHP in silicon
  234. nanoparticles has not been modeled before in time-domain. Therefore, herein we propose a model considering ultrashort laser interactions with a resonant silicon
  235. sphere, where the EHP is generated via one- and two-photon absorption
  236. processes. Importantly, we
  237. also consider nonlinear feedback of the material by taking into
  238. account the intraband light absorption on the generated free carriers. To simplify our model, we neglect free carrier diffusion at the considered short time scales. In fact, the aim of the present work is to study the EHP dynamics \textit{during} ultra-short laser interaction with the nanoparticle. The created electron-hole plasma then will recombine, however, as its existence modifies both laser-particle interaction and, hence, the following particle evolution.
  239. \subsection{Light propagation}
  240. Ultra-short laser interaction and light propagation inside the silicon nanoparticle are modeled by solving the system of Maxwell's equations written in the following way
  241. \begin{align} \begin{cases} \label{Maxwell}$$
  242. \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})} \\
  243. \displaystyle{\frac{\partial{\vec{H}}}{\partial{t}}=-\frac{\nabla\times\vec{E}}{\mu_0}},
  244. $$ \end{cases} \end{align}
  245. where $\vec{E}$ is the electric field, $\vec{H}$ is the magnetizing field, $\epsilon_0$ is the free space permittivity, $\mu_0$ is the permeability of free space, $\epsilon = n^2 = 3.681^2$ is the permittivity of non-excited silicon at $800$ nm wavelength \cite{Green1995}, $\vec{J}_p$ and $\vec{J}_{Kerr}$ are the nonlinear currents, which include the contribution due to Kerr effect $\vec{J}_{Kerr} = \epsilon_0\epsilon_\infty\chi_3\frac{\partial\left(\left|\vec{E}\right|^2\vec{E}\right)}{\partial{t}}$, where $\chi_3 =4\cdot{10}^{-20}$ m$^2$/V$^2$ for laser wavelength $\lambda = 800$nm \cite{Bristow2007}, and heating of the conduction band, described by the differential equation derived from the Drude model
  246. \begin{equation} \label{Drude} \displaystyle{\frac{\partial{\vec{J_p}}}{\partial{t}} = - \nu_e\vec{J_p} + \frac{e^2n_e(t)}{m_e^*}\vec{E}}, \end{equation}
  247. where $e$ is the elementary charge, $m_e^* = 0.18m_e$ is the reduced electron-hole mass \cite{Sokolowski2000}, $n_e(t)$ is the time-dependent free carrier density and $\nu_e = 10^{15}$ s$^{-1}$ is the electron collision frequency \cite{Sokolowski2000}. Silicon nanoparticle is surrounded by vacuum, where the light propagation is calculated by Maxwell's equations with $\vec{J} = 0$ and $\epsilon = 1$. The system of Maxwell's equations coupled with electron density equation is solved by the finite-difference numerical method \cite{Rudenko2016}, based on the finite-difference time-domain (FDTD) \cite{Yee1966} and auxiliary-differential methods for dispersive media \cite{Taflove1995}. At the edges of the grid, we apply the absorbing boundary conditions related to convolutional perfectly matched layers (CPML) to avoid nonphysical reflections \cite{Roden2000}. The initial electric field is introduced as a Gaussian slightly focused beam as follows
  248. \begin{align}
  249. \begin{aligned}
  250. \label{Gaussian}
  251. {E_x}(t, r, z) = \frac{w_0}{w(z)}{exp}\left(i\omega{t} - \frac{r^2}{{w(z)}^2} - ikz - ik\frac{r^2}{2R(z)} + i\varsigma(z)\right)\\
  252. \times\;{exp}\left(-\frac{(t-t_0)^2}{\theta^2}\right),
  253. \end{aligned}
  254. \end{align}
  255. where $\theta$ is the temporal pulse width at the half maximum (FWHM), $t_0$ is a time delay, $w_0 = 3{\mu}m$ is the waist beam, $w(z) = {w_0}\sqrt{1+(\frac{z}{z_R})^2}$ is the Gaussian's beam spot size, $\omega = 2{\pi}c/{\lambda}$ is the angular frequency, $\lambda = 800 nm$ is the laser wavelength in air, $c$ is the speed of light, ${z_R} = \frac{\pi{{w_0}^2}n_0}{\lambda}$ is the Rayleigh length, $r = \sqrt{x^2 + y^2}$ is the radial distance from the beam's waist, $R_z = z\left(1+(\frac{z_R}{z})^2\right)$ is the radius of curvature of the wavelength comprising the beam, and $\varsigma(z) = {\arctan}(\frac{z}{z_R}) $ is the Gouy phase shift.
  256. \subsection{Material ionization}
  257. To account for the material ionization that is induced by a sufficiently intense laser field inside the particle, we couple Maxwell's equations with the kinetic equation for the electron-hole plasma as follows
  258. % \begin{figure*}[ht!]
  259. % \centering
  260. % \includegraphics[width=120mm]{fig2.png}
  261. % \caption{\label{fig2} Free carrier density snapshots of electron plasma evolution inside Si nanoparticle taken a) $30$ fs b) $10$ fs before the pulse peak, c) at the pulse peak, d) $10$ fs e) $30$ fs after the pulse peak. Pulse duration $50$ fs (FWHM). Wavelength $800$ nm in air. Radius of the nanoparticle $R \approx 105$ nm, corresponding to the resonance condition. Graph shows the dependence of the asymmetric parameter of electron plasma density on the average electron density in the front half of the nanoparticle. $n_{cr} = 5\cdot{10}^{21}$ cm$^{-3}$ is the critical plasma resonance electron density for silicon.}
  262. % \end{figure*}
  263. The time-dependent conduction-band carrier density evolution is described by a rate equation that was proposed by van Driel \cite{Van1987}. This equation takes into account such processes as photoionization, avalanche ionization and Auger recombination, and is written as
  264. \begin{equation} \label{Dens} \displaystyle{\frac{\partial{n_e}}{\partial t} = \frac{n_a-n_e}{n_a}\left(\frac{\sigma_1I}{\hbar\omega} + \frac{\sigma_2I^2}{2\hbar\omega}\right) + \alpha{I}n_e - \frac{C\cdot{n_e}^3}{C\tau_{rec}n_e^2+1},} \end{equation}
  265. where $I=\frac{n}{2}\sqrt{\frac{\epsilon_0}{\mu_0}}\left|\vec{E}\right|^2$ is the intensity, $\sigma_1 = 1.021\cdot{10}^3 cm^{-1}$ and $\sigma_2 = 0.1\cdot{10}^{-7}$ cm/W are the one-photon and two-photon interband cross-sections \cite{Choi2002, Bristow2007, Derrien2013}, $n_a = 5\cdot{10}^{22} cm^{-3}$ is the saturation particle density \cite{Derrien2013}, $C = 3.8\cdot{10}^{-31}$ cm$^6$/s is the Auger recombination rate \cite{Van1987}, $\tau_{rec} = 6\cdot{10}^{-12}$s is the minimum Auger recombination time \cite{Yoffa1980}, and $\alpha = 21.2$ cm$^2$/J is the avalanche ionization coefficient \cite{Pronko1998} at the wavelength $800$ nm in air. As we have noted, free carrier diffusion is neglected during and shortly after the laser excitation \cite{Van1987, Sokolowski2000}.
  266. \begin{figure}[ht!]
  267. \centering
  268. \includegraphics[width=0.495\textwidth]{mie-fdtd-3}
  269. \caption{\label{mie-fdtd} Mie and FDTD comparison. (c-f) Incident light goes from the left.}
  270. \end{figure}
  271. \begin{figure*}[ht!]
  272. \centering
  273. \includegraphics[width=0.9\textwidth]{2nm_75}
  274. \includegraphics[width=0.9\textwidth]{2nm_115}
  275. \caption{\label{plasma-105nm} Split figure \ref{fig2} into two, this is first part.}
  276. \end{figure*}
  277. The changes of the real and imaginary parts of the permittivity associated with the time-dependent free carrier response \cite{Sokolowski2000} can be derived from equations (\ref{Maxwell}, \ref{Drude}) and are written as follows
  278. \begin{align} \begin{cases} \label{Index} $$
  279. \displaystyle{Re(\epsilon) = \epsilon -\frac{{e^2}n_e}{\epsilon_0m_e^*(\omega^2+{\nu_e}^2)}} \\
  280. \displaystyle{Im(\epsilon) = \frac{{e^2}n_e\nu_e}{\epsilon_0m_e^*\omega(\omega^2+{\nu_e}^2)}.}
  281. $$ \end{cases} \end{align}
  282. \section{Results and discussion}
  283. \subsection{Effect of the irradiation intensity on EHP generation}
  284. Fig. \ref{fig2} demonstrates the temporal evolution of the EHP generated inside the silicon
  285. nanoparticle of $R \approx 105$ nm. Here, irradiation by
  286. high-intensity, $I\approx $ from XXX to YYY (???), ultrashort laser Gaussian pulse is considered. Snapshots of free carrier density taken at different times correspond to different total amount of the deposited energy (different laser intensities).
  287. To better analyze the degree of inhomogeneity, we introduce the EHP asymmetry parameter, $G$, which is defined
  288. as a relation between the average electron density generated in the
  289. front side of the nanoparticle and the average electron density in the
  290. back side, as shown in Fig. \ref{fig2}. During the femtosecond pulse
  291. interaction, this parameter significantly varies.
  292. Far before the pulse peak shown in Fig. \ref{fig2}(a), the excitation
  293. processes follow the intensity distribution, generating a low-density
  294. electron plasma of a toroidal shape at magnetic dipole resonance
  295. conditions. For higher intensities, the optical properties of silicon
  296. change significantly according to the equations (\ref{Index}). As a result, the non-resonant electric dipole contributes to the forward shifting of EHP
  297. density maximum. Therefore, EHP is localized in the front part of the
  298. nanoparticle, increasing the asymmetry factor $G$ in
  299. Fig. \ref{fig2}(b). Approximately at the pulse peak, the critical
  300. electron density $n_{cr} = 5\cdot{10}^{21} cm^{-3}$ for silicon, which
  301. corresponds to the transition to quasi-metallic state $Re(\epsilon)
  302. \approx 0$ and to the electron plasma resonance (so-called "volume plasmons", and/or "localized plasmons" typical for metallic nanoparticles !??) \cite{Sokolowski2000}, is overcome.
  303. At the same time, $G$ factor
  304. reaches the maximum value close to $2.5$ in
  305. Fig. \ref{fig2}(c). Further irradiation leads to a decrease in the
  306. asymmetry parameter down to $1$ for higher electron densities, as one may observe in
  307. Fig. \ref{fig2}(d, e).
  308. It is worth noting that it is possible to achieve a formation of
  309. deeply subwavelength EHP regions due to high field localization. In
  310. particular, we observe very small EHP localization at magnetic dipole
  311. resonant conditions for $R \approx 105$ nm. The EHP distribution in
  312. Fig. \ref{fig2}(c) is optimal for symmetry breaking in silicon
  313. nanoparticle, as it results in the larger asymmetry factor $G$ and higher
  314. electron densities $n_e$. We stress here that such regime
  315. could be still safe for nanoparticle due to the very small volume where such high
  316. EHP density is formed.
  317. TODO: need to discuss this -
  318. Of cause, this plasma is expected to diffuse after the considered time and turn to the homogeneously distributed one over the nanoparticle volume with a smaller density. Part of the electrons can also be ejected/injected into the surrounding medium, the process known to depend on the Shottky barrier at the particle border.
  319. \subsection{Effects of nanoparticle size/scattering efficiency factor
  320. on scattering directions}
  321. % \begin{figure}[ht] \centering
  322. % \includegraphics[width=90mm]{fig3.png}
  323. % \caption{\label{fig3} a) Scattering efficiency factor $Q_{sca}$
  324. % dependence on the radius $R$ of non-excited silicon nanoparticle
  325. % calculated by Mie theory; b) Parameter of forward/backward scattering
  326. % dependence on the radius $R$ calculated by Mie theory for non-excited
  327. % silicon nanoparticle c) Optimization parameter $K$ dependence on the
  328. % average electron density $n_e^{front}$ in the front half of the
  329. % nanoparticle for indicated radii (1-7).}
  330. % \end{figure}
  331. We have discussed the EHP kinetics for a silicon nanoparticle of a fixed radius $R \approx 105$ nm. In what follows, we investigate the influence of the nanoparticle size on
  332. the EHP patterns and temporal evolution during ultrashort laser
  333. irradiation. A brief analysis of the initial intensity distribution
  334. inside the nanoparticle given by the classical Mie theory for
  335. homogeneous spherical particles \cite{Mie1908} can be useful in
  336. this case. Fig. \ref{fig3}(a, b) shows the scattering efficiency and
  337. the asymmetry parameter for forward/backward scattering for
  338. non-excited silicon nanoparticles of different radii calculated by Mie
  339. theory \cite{Mie1908}. Scattering efficiency dependence gives
  340. us the value of resonant sizes of nanoparticles, where the initial
  341. electric fields are significantly enhanced and, therefore, we can
  342. expect that the following conditions will result in a stronger
  343. electron density gradients. Additionally, in the case of maximum
  344. forward or backward scattering, the initial intensity distribution has
  345. the maximum of asymmetry. One can note, that for $R \approx 100$ nm
  346. and $R \approx 150$ nm both criteria are fulfilled: the intensity is
  347. enhanced $5-10$ times due to near-resonance conditions and its
  348. distribution has a strong asymmetry.
  349. In what follows, we present the calculation results obtained by using
  350. Maxwell's equations coupled with electron kinetics for different
  351. extremum radii for resonant and non-resonant conditions. One can note,
  352. that the maximum asymmetry factor of EHP $G$ does not guarantee the
  353. optimal asymmetry of intensity distribution, as the size of generated
  354. plasma and the value of the electron density equally contribute to the
  355. change of the modified nanoparticle optical response. For example, it
  356. is easier to localize high electron densities inside smaller
  357. nanoparticles, however, due to the negligible size of the generated
  358. EHP with respect to laser wavelength in media, the intensity
  359. distribution around the nanoparticle will not change
  360. considerably. Therefore, we propose to introduce the optimization
  361. factor $K = \frac{n_e(G-1)R^2}{n_{cr}G{R_0^2}}$, where $R_0 = 100$ nm,
  362. $n_{cr} = 5\cdot{10}^{21} cm^{-3}$, and $G$ is asymmetry of EHP,
  363. defined previously. The calculation results for different radii of
  364. silicon nanoparticles and electron densities are presented in
  365. Fig. \ref{fig3}(c). One can see, that the maximum value are achieved
  366. for the nanoparticles, that satisfy both initial maximum forward
  367. scattering and not far from the first resonant condition. For larger
  368. nanoparticles, lower values of EHP asymmetry factor are obtained, as
  369. the electron density evolves not only from the intensity patterns in
  370. the front side of the nanoparticle but also in the back side.
  371. TODO:
  372. Need to discuss agreement/differences between Mie and FDTD+rate. Anton ?!
  373. To demonstrate the effect of symmetry breaking, we calculate the
  374. intensity distribution around the nanoparticle for double-pulse
  375. experiment. The first pulse of larger pulse energy and polarization
  376. along $Ox$ generates asymmetric EHP inside silicon nanoparticle,
  377. whereas the second pulse of lower pulse energy and polarization
  378. $Oz$ interacts with EHP after the first pulse is gone. The minimum
  379. relaxation time of high electron density in silicon is $\tau_{rec} =
  380. 6\cdot{10}^{-12}$ s \cite{Yoffa1980}, therefore, the
  381. electron density will not have time to decrease significantly for
  382. subpicosecond pulse separations. In our simulations, we use $\delta{t}
  383. = 200$ fs pulse separation. The intensity distributions near the
  384. silicon nanoparticle of $R = 95$ nm, corresponding to maxima value of
  385. $K$ optimization factor, without plasma and with generated plasma are
  386. shown in Fig. \ref{fig4}. The intensity distribution is strongly
  387. asymmetric in the case of EHP presence. One can note, that the excited
  388. nanoparticle is out of quasi-resonant condition and the intensity
  389. enhancements in Fig. \ref{fig4}(c) are weaker than in
  390. Fig. \ref{fig4}(b). Therefore, the generated nanoplasma acts like a quasi-metallic nonconcentric nanoshell inside the nanoparticle, providing a symmetry reduction \cite{Wang2006}.
  391. % \begin{figure}[ht] \centering
  392. % \includegraphics[width=90mm]{fig4.png}
  393. % \caption{\label{fig4} a) Electron plasma distribution inside Si
  394. % nanoparticle $R \approx 95$ nm $50$ fs after the pulse peak; (Kostya: Is it scattering field intensity snapshot XXX fs after the second pulse maxima passed the particle?) Intensity
  395. % distributions around and inside the nanoparticle b) without plasma, c)
  396. % with electron plasma inside.}
  397. % \end{figure}
  398. %\begin{figure} %\centering
  399. % \includegraphics[height=0.7\linewidth]{Si-flow-R140-XYZ-Eabs}
  400. % \caption{EHP distributions for nonres., MD, ED, and MQ nanoparticles
  401. % at moderate photoexcitation. The aim is to show different possible
  402. % EHP patterns and how strong could be symmetry breaking.
  403. % \label{fgr:example}
  404. %\end{figure}
  405. \subsection{Asymmetry analysis: effects of pulse duration, intensity
  406. and size} It is important to optimize asymmetry by varying pulse
  407. duration, intensity and size.
  408. TODO Kostya: add some discusion on rise-on time for optical switching
  409. like this: Small size will give as a magnetic dipole b1 resonance with
  410. Q-factor (ratio of wavelength to the resonance width at half-height)
  411. of about 8, a1 Q approx 4, the larger particle will have b2 Q approx
  412. 40. For large particle we will have e.g. at R=238.4 second order b4
  413. resonance with Q approx 800. As soon as the period at WL=800nm is 2.6
  414. fs, we need about 25 fs pulse to pump dipole response, about 150 fs
  415. for quadrupole, and about 2000fs for b4. If we think of optical
  416. switching applications this is a rise-on time.
  417. TODO Kostya: Add discussion about mode selection due to the formation
  418. of the plasma.
  419. \section{Conclusions} We have considered ultra-short and sufficiently intense light interactions with a single
  420. semiconductor nanoparticle under different irradiation conditions and
  421. for various particle sizes. As a result of the presented
  422. self-consistent calculations, we have obtained spatio-temporal EHP
  423. evolution inside the particle for different laser intensities and temporal
  424. pulse widths. It has been demonstrated that the EHP generation strongly affects
  425. nanoparticle scattering and, in particular, changes the preferable
  426. scattering direction.
  427. In particular, the scattering efficiency factor
  428. is used to define the optimum nanoparticle size for preferential
  429. forward or backward scattering. Furthermore, a parameter has been
  430. introduced to describe the scattering asymmetry as a ratio of the EHP
  431. density in the front side to that in the back side of the
  432. nanoparticle. This parameter can be then used for two-dimensional
  433. scattering mapping, which is particularly important in numerous
  434. photonics applications. The observed plasma-induced breaking symmetry
  435. can be also useful for beam steering, or for the enhanced second
  436. harmonics generation.
  437. \section{Acknowledgments} We gratefully acknowledge support from The French
  438. Ministry of Science and Education, from the French Center of Scientific Research (CNRS) and from the PHC Kolmogorov project "FORMALAS".
  439. %%%END OF MAIN TEXT%%%
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  448. %%%REFERENCES%%%
  449. \bibliography{References.bib} %You need to replace "rsc" on this line
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