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Register a new userPump-Probe Faraday Rotation and Ellipticity in an Ensemble of Singly Charged Quantum Dots
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A description of spin Faraday rotation, Kerr rotation and ellipticity signals for single- and multi-layer ensembles of singly charged quantum dots (QDs) is developed. The microscopic theory considers both the single pump-pulse excitation and the effect of a train of such pulses, which in the case of long resident-electron spin coherence time leads to a stationary distribution of the electron spin polarization. The calculations performed for single-color and two-color pump-probe setups show that the three experimental techniques: Faraday rotation, Kerr rotation and ellipticity measurements provide complementary information about an inhomogeneous ensemble of QDs. The microscopic theory developed for a three-dimensional ensemble of QDs is shown to agree with the phenomenological description of these effects. The typical time-dependent traces of pump-probe Faraday rotation, Kerr rotation and ellipticity signals are calculated for various experimental conditions.
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Photo-luminescence intermittency (blinking) in semiconductor nanocrystals (NCs), a phenomenon ubiquitous to single-emitters, is generally considered to be temporally random intensity fluctuations between bright (On) and dark (Off) states. However, individual quantum-dots (QDs) rarely exhibit such telegraphic signal, and yet, the vast majority of single-NC blinking data are analyzed using a single fixed threshold, which generates binary trajectories. Further, blinking dynamics can vary dramatically over NCs in the ensemble, and it is unclear whether the exponents (m) of single-particle On-/Off-time distributions (P(t)-On/Off), which are used to validate mechanistic models of blinking, are narrowly distributed or not. Here, we sub-classify an ensemble based on the emissivity of QDs, and subsequently compare the (sub)ensemble behaviors. To achieve this, we analyzed a large number (>1000) of intensity trajectories for a model system, Mn+2 doped ZnCdS QDs, which exhibits diverse blinking dynamics. An intensity histogram dependent thresholding method allowed us to construct distributions of relevant blinking parameters (such as m). Interestingly, we find that single QD P(t)-On/Off s follow either truncated power law or power law, and their relative proportion vary over sub-populations. Our results reveal a remarkable variation in m(On/Off) amongst as well as within sub-ensembles, which implies multiple blinking mechanisms being operational among various QDs. We further show that the m(On/Off) obtained via cumulative single-particle P(t)-On/Off is clearly distinct from the weighted mean value of all single-particle m(On/Off), an evidence for the lack of ergodicity. Thus, investigation and analyses of a large number of QDs, albeit for a limited time-span of few decades, is crucial to characterize possible blinking mechanisms and heterogeneity therein
Using the recently reported mode locking effect we demonstrate a highly robust control of electron spin coherence in an ensemble of (In,Ga)As quantum dots during the single spin coherence time. The spin precession in a transverse magnetic field can be fully controlled up to 25 K by the parameters of the exciting pulsed laser protocol such as the pulse train sequence, leading to adjustable quantum beat bursts in Faraday rotation. Flipping of the electron spin precession phase was demonstrated by inverting the polarization within a pulse doublet sequence.
The operation of quantum dots at highest possible temperatures is desirable for many applications. Capacitance-voltage spectroscopy (C(V)-spectroscopy) measurements are an established instrument to analyze the electronic structure and energy levels of self-assembled quantum dots (QDs). We perform C(V) in the dark and C(V) under the influence of non-resonant illumination, probing exciton states up to $X^{4+}$ on InAs QDs embedded in a GaAs matrix for temperatures ranging from 2.5 K to 120 K. While a small shift in the charging spectra resonance is observed for the two pure spin degenerate electron s-state charging voltages with increasing temperature, a huge shift is visible for the electron-hole excitonic states resonance voltages. The $s_2$-peak moves to slightly higher, the $s_1$-peak to slightly lower charging voltages. In contrast, the excitonic states are surprisingly charged at much lower voltages upon increasing temperature. We derive a rate-model allowing to attribute and value different contributions to these shifts. Resonant tunnelling, state degeneracy and hole generation rate in combination with the Fermi distribution function turn out to be of great importance for the observed effects. The differences in the shifting behavior is connected to different equilibria schemes for the peaks; s-peaks arise when tunneling-in- and out-rates become equal, while excitonic peaks occur, when electron tunneling-in- and hole-generation rates are balanced.
A theoretical frame for pump-probe photoemission is presented. The approach is based on a general formulation using the Keldysh formalism for the lesser Greens function to describe the real-time evolution of the electronic degrees of freedom in the initial state after a strong pump pulse that drives the system out of equilibrium. The final state is represented by a time-reversed low-energy electron diffraction state. Our one-step description is related to Pendrys original formulation of the photoemission process as close as possible. The formalism allows for a quantitative calculation of time-dependent photocurrent for simple metals where a picture of effectively independent electrons is assumed as reliable. The theory is worked out for valence- and core-electron excitations. It comprises the study of different relativistic effects as a function of the pump-probe delay.
Charged excitons, or X$^{pm}$-trions, in monolayer transition metal dichalcogenides have binding energies of several tens of meV. Together with the neutral exciton X$^0$ they dominate the emission spectrum at low and elevated temperatures. We use charge tunable devices based on WSe$_2$ monolayers encapsulated in hexagonal boron nitride, to investigate the difference in binding energy between X$^+$ and X$^-$ and the X$^-$ fine structure. We find in the charge neutral regime, the X$^0$ emission accompanied at lower energy by a strong peak close to the longitudinal optical (LO) phonon energy. This peak is absent in reflectivity measurements, where only the X$^0$ and an excited state of the X$^0$ are visible. In the $n$-doped regime, we find a closer correspondence between emission and reflectivity as the trion transition with a well-resolved fine-structure splitting of 6~meV for X$^-$ is observed. We present a symmetry analysis of the different X$^+$ and X$^-$ trion states and results of the binding energy calculations. We compare the trion binding energy for the $n$-and $p$-doped regimes with our model calculations for low carrier concentrations. We demonstrate that the splitting between the X$^+$ and X$^-$ trions as well as the fine structure of the X$^-$ state can be related to the short-range Coulomb exchange interaction between the charge carriers.
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