اشترك بالحزمة الذهبية واحصل على وصول غير محدود شمرا أكاديميا
تسجيل مستخدم جديدNonlinear Raman Shift Induced by Exciton-to-Trion Transformation in Suspended Trilayer MoS2
115
0
0.0
(
0
)
اسأل ChatGPT حول البحث
ﻻ يوجد ملخص باللغة العربية
Layered two-dimensional (2D) semiconductors such as molybdenum disulfide (MoS2) have recently attracted remarkable attention because of their unique physical properties. Here, we use photoluminescence (PL) and Raman spectroscopy to study the formation of the so- called trions in a synthesized freestanding trilayer MoS2. A trion is a charged quasi-particle formed by adding one electron or hole to a neutral exciton (a bound electron-hole pair). We demonstrate accurate control over the transformation of excitons to trions by tuning the power of the optical pump (laser). Increasing the power of the excitation laser beyond a certain threshold (~ 4 mW) allows modulation of trion-to-exciton PL intensity ratio as well as the spectral linewidth of both trions and excitons. Via a systematic and complementary Raman analysis we disclose a strong coupling between laser induced exciton-to-trion transformation and the characteristic phononic vibrations of MoS2. The onset of such an optical transformation corresponds to the onset of a previously unknown nonlinear Raman shift of the in-plane (E12g) and out-of-plane (A1g) vibrational modes. This coupling directly affects the well-known linear red-shift of the A1g and E12g vibrations due to heating at low laser powers, and changes it to a nonlinear and non-monotonic dependence with a blue-shift in the high laser power regime. Local reduction of the electron density upon exciton-to-trion transformation is found to be the underlying mechanism for the blue-shift at high laser powers. Our findings enrich our knowledge about the strong coupling of photonic and phononic properties in 2D semiconductors, and enable reliable interpretation of PL and Raman spectra in the high laser power regimes.
قيم البحث
اقرأ أيضاً
We report on scattering induced valley polarization enhancement in monolayer molybdenum disulfide. With thermally activated and charge doping introduced scattering, our sample exhibits seven? and twelve-folds of improvements respectively. This counte
r-intuitive effect is attributed to disruptions to valley pseudospin precession caused by rapid modulation of exciton momentum and concomitant local exchange interaction field, at time scales much shorter than the precession period. In contrast, the valley coherence is improved by thermally activated scattering, but not by charge doping induced scattering. We propose that this is due to anisotropic pseudospin scattering and generalize the Maialle-Silva-Sham model to quantitatively explain our experimental results. Our work illustrates that cleaner samples with minimal scattering, such as those carefully suspended or protected by hexagonal boron nitride, do not necessarily lead to good valley polarization. Well-controlled scattering can in fact provide an interesting approach for improving valleytronic devices.
Optical excitation typically enhances electrical conduction and low-frequency radiation absorption in semiconductors. We have, however, observed a pronounced transient decrease of conductivity in doped monolayer molybdenum disulfide (MoS2), a two-dim
ensional (2D) semiconductor, under femtosecond laser excitation. In particular, the conductivity is reduced dramatically down to only 30% of its equilibrium value with high pump fluence. This anomalous phenomenon arises from the strong many-body interactions in the system, where photoexcited electron-hole pairs join the doping-induced charges to form trions, bound states of two electrons and one hole. The resultant increase of the carrier effective mass substantially diminishes the carrier conductivity.
We demonstrate that the temperature and doping dependencies of the photoluminescence (PL) spectra of a doped MoS2 monolayer have several peculiar characteristics defined by trion radiative decay. While only zero-momentum exciton states are coupled to
light, radiative recombination of non-zero momentum trions is also allowed. This leads to an asymmetric broadening of the trion spectral peak and redshift of the emitted light with increasing temperature. The lowest energy trion state is dark, which is manifested by the sharply non-monotonic temperature dependence of the PL intensity. Our calculations combine the Dirac model for the single-particle states, the parameters for which are obtained from the first principle calculations, and the direct solution of the three-particle problem within the Tamm-Dancoff approximation. The numerical results are well captured by a simple model that yields analytical expressions for the temperature dependencies of the PL spectra.
We investigate second harmonic generation (SHG) from hexagonal periodic arrays of triangular nano-holes of aluminum using a self-consistent methodology based on the hydrodynamics-Maxwell-Bloch approach. It is shown that angular polarization patterns
of the far-field second harmonic response abide to three-fold symmetry constraints on tensors. When a molecular layer is added to the system and its parameters are adjusted to achieve the strong coupling regime between a localized plasmon mode and molecular excitons, Rabi splitting is observed from occurrence of both single- and two-photon transition peaks within the SHG power spectrum. It is argued that the splitting observed for both transitions results from direct transitions between lower and upper polaritonic states of the strongly coupled system. This interpretation can be accounted by a tailored three-level quantum model, with results in agreement with the unbiased numerical approach. Our results suggest the hybrid states formed in strongly coupled systems directly contribute to the nonlinear dynamics. This opens new directions in designing THz sources and nonlinear frequency converters.
Optoelectronic excitations in monolayer MoS2 manifest from a hierarchy of electrically tunable, Coulombic free-carrier and excitonic many-body phenomena. Investigating the fundamental interactions underpinning these phenomena - critical to both many-
body physics exploration and device applications - presents challenges, however, due to a complex balance of competing optoelectronic effects and interdependent properties. Here, optical detection of bound- and free-carrier photoexcitations is used to directly quantify carrier-induced changes of the quasiparticle band gap and exciton binding energies. The results explicitly disentangle the competing effects and highlight longstanding theoretical predictions of large carrier-induced band gap and exciton renormalization in 2D semiconductors.
سجل دخول لتتمكن من نشر تعليقات
التعليقات
جاري جلب التعليقات
سجل دخول لتتمكن من متابعة معايير البحث التي قمت باختيارها
