Temperature Dependence of Raman Scattering in Silicon
TL;DR: In this article, the authors measured the linewidth and the frequency of the q = 0 optical phonon in silicon over the temperature range of 20-770, and deduced an absolute halfwidth of 2.1
Abstract: We have measured the linewidth and the frequency of the q=0 optical phonon in silicon over the temperature range of 20-770\ifmmode^\circ\else\textdegree\fi{}K. The temperature dependence of the linewidth has been interpreted as arising from the decay of the optical phonon to two LA phonons at half the optical frequency. From the observed temperature variation, we deduce an absolute half-width $\ensuremath{\Gamma}$ of 2.1 ${\mathrm{cm}}^{\ensuremath{-}1}$ at 0\ifmmode^\circ\else\textdegree\fi{}K. This value is considerably smaller than that obtained theoretically by Cowley on the basis of numerical calculations which include decay to phonons throughout the Brillouin zone. His numerical calculations also predict a temperature dependence of the linewidth which does not agree with experiment. However, the observed change in frequency with temperature correlates very well with Cowley's theory. We have also studied the relative intensities of Stokes and anti-Stokes components of Raman spectra. The observed temperature dependence of the relative intensities is compared with that predicted on the basis of the Bose-Einstein population factor for the optical phonon.
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TL;DR: In this paper, a relaxation in the q-vector selection rule for the excitation of the Raman active optical phonons was proposed to increase the red shift and broadening of the signal from microcrystalline silicon films.
2,059 citations
TL;DR: A unified theoretical platform that not only can be used for understanding the underlying physics but should also provide guidance toward new and useful applications is provided.
Abstract: Several kinds of nonlinear optical effects have been observed in recent years using silicon waveguides, and their device applications are attracting considerable attention. In this review, we provide a unified theoretical platform that not only can be used for understanding the underlying physics but should also provide guidance toward new and useful applications. We begin with a description of the third-order nonlinearity of silicon and consider the tensorial nature of both the electronic and Raman contributions. The generation of free carriers through two-photon absorption and their impact on various nonlinear phenomena is included fully within the theory presented here. We derive a general propagation equation in the frequency domain and show how it leads to a generalized nonlinear Schrodinger equation when it is converted to the time domain. We use this equation to study propagation of ultrashort optical pulses in the presence of self-phase modulation and show the possibility of soliton formation and supercontinuum generation. The nonlinear phenomena of cross-phase modulation and stimulated Raman scattering are discussed next with emphasis on the impact of free carriers on Raman amplification and lasing. We also consider the four-wave mixing process for both continuous-wave and pulsed pumping and discuss the conditions under which parametric amplification and wavelength conversion can be realized with net gain in the telecommunication band.
877 citations
TL;DR: In this paper, the temperature dependence of the first-order Raman scattering by phonons in Si, Ge, and $\ensuremath{\alpha}\ensureMath{-}\mathrm{S} n} was measured.
Abstract: We have measured the temperature dependence of the first-order Raman scattering by phonons in Si, Ge, and $\ensuremath{\alpha}\ensuremath{-}\mathrm{S}\mathrm{n}$. The full widths at half maximum of the Raman lines, extrapolated to zero temperature, are 1.24\ifmmode\pm\else\textpm\fi{}0.07, 0.75\ifmmode\pm\else\textpm\fi{}0.03, and 0.81\ifmmode\pm\else\textpm\fi{}0.15 ${\mathrm{cm}}^{\ensuremath{-}1}$ for Si, Ge, and $\ensuremath{\alpha}\ensuremath{-}\mathrm{S}\mathrm{n}$, respectively. The reliability of the data obtained allows a critical examination of the theoretical calculations published so far. We show that the model assuming the decay of the Raman phonon into two acoustical phonons belonging to the same branch, first proposed by Klemens, does not represent adequately the temperature dependence of the Raman linewidth. The most important decay channels are shown to be combinations of optical and acoustical phonons. However, the more complete calculation by Cowley, which involves all possible decay channels, gives very large zero-temperature linewidths. We show that this arises mainly from the poor description of the phonon dispersion curves by the shell model used by Cowley, and that a better agreement between theory and experiment is to be expected by repeating the calculation with Weber's adiabatic bond-charge model.
619 citations
TL;DR: In this paper, the authors measured nonresonant and resonant Raman-scattering spectra from ZnO nanocrystals with an average diameter of 20nm.
Abstract: We have measured nonresonant and resonant Raman-scattering spectra from ZnO nanocrystals with an average diameter of 20nm. Based on our experimental data and comparison with the recently developed theory, we show that the observed shifts of the polar optical-phonon peaks in the resonant Raman spectra are not related to the spatial phonon confinement. The very weak dispersion of the polar optical phonons in ZnO nanocrystals does not lead to any noticeable redshift of the phonon peaks for 20-nm nanocrystals. The observed phonon shifts have been attributed to the local heating effects. We have demonstrated that even the low-power ultraviolet laser excitation, required for the resonant Raman spectroscopy, can lead to the strong local heating of ZnO nanocrystals. The latter causes significant (up to 14cm−1) redshift of the optical-phonon peaks compared to their position in bulk crystals. Nonresonant Raman excitation does not produce noticeable local heating. The obtained results can be used for identification ...
559 citations
TL;DR: In this paper, the temperature-dependent Raman spectra of exfoliated, monolayer molybdenum disulfide (MoS2) in the range of 100-320 K were analyzed.
Abstract: Atomically thin molybdenum disulfide (MoS2) offers potential for advanced devices and an alternative to graphene due to its unique electronic and optical properties. The temperature-dependent Raman spectra of exfoliated, monolayer MoS2 in the range of 100–320 K are reported and analyzed. The linear temperature coefficients of the in-plane E2g1 and the out-of-plane A1g modes for both suspended and substrate-supported monolayer MoS2 are measured. These data, when combined with the first-order coefficients from laser power-dependent studies, enable the thermal conductivity to be extracted. The resulting thermal conductivity κ = (34.5 ± 4) W/mK at room temperature agrees well with the first-principles lattice dynamics simulations. However, this value is significantly lower than that of graphene. The results from this work provide important input for the design of MoS2-based devices where thermal management is critical.
528 citations