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Register a new userCharge Trapping Dynamics in PbS Colloidal Quantum Dot Photovoltaic Devices
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The efficiency of solution-processed colloidal quantum dot (QD) based solar cells is limited by poor charge transport in the active layer of the device, which originates from multiple trapping sites provided by QD surface defects. We apply a recently developed ultrafast electro-optical technique, pump-push photocurrent spectroscopy, to elucidate the charge trapping dynamics in PbS colloidal-QD photovoltaic devices at working conditions. We show that IR photo-induced absorption of QD in the 0.2-0.5 eV region is partly associated with immobile charges, which can be optically de-trapped in our experiment. Using this absorption as a probe, we observe that the early trapping dynamics strongly depend on the nature of the ligands used for QD passivation while it depends only slightly on the nature of the electron-accepting layer. We find that weakly bound states, with a photon-activation energy of 0.2 eV, are populated instantaneously upon photoexcitation. This indicates that the photogenerated states show an intrinsically bound-state character, arguably similar to charge-transfer states formation in organic photovoltaic materials. Sequential population of deeper traps (activation energy 0.3-0.5 eV) is observed on the ~0.1-10 ns time scales, indicating that most of carrier trapping occurs only after substantial charge relaxation/transport. The reported study disentangles fundamentally different contributions to charge trapping dynamics in the nanocrystal-based optoelectronic devices and can serve as a useful tool for QD solar cell development.
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The formation of bound electron-hole pairs, also called charge-transfer (CT) states, in organic-based photovoltaic devices is one of the dominant loss mechanisms hindering performance. While CT state dynamics following electron transfer from donor to acceptor have been widely studied, there is not much known about the dynamics of bound CT states produced by hole transfer from the acceptor to the donor. In this letter, we compare the dynamics of CT states formed in the different charge-transfer pathways in a range of model systems. We show that the nature and dynamics of the generated CT states are similar in the case of electron and hole transfer. However the yield of bound and free charges is observed to be strongly dependent on the HOMOD-HOMOA and LUMOD-LUMOA energy differences of the material system. We propose a qualitative model in which the effects of static disorder and sampling of states during the relaxation determine the probability of accessing CT states favourable for charge separation.
We develop quantum dots in a single layered MOS structure using an undoped Si/SiGe wafer. By applying a positive bias on the surface gates, electrons are accumulated in the Si channel. Clear Coulomb diamond and double dot charge stability diagrams are measured. The temporal fluctuation of the current is traced, to which we apply the Fourier transform analysis. The power spectrum of the noise signal is inversely proportional to the frequency, and is different from the inversely quadratic behavior known for quantum dots made in doped wafers. Our results indicate that the source of charge noise for the doped wafers is related to the 2DEG dopant.
The dynamics of charge qubit in a double quantum dot coupled to phonons is investigated theoretically in terms of a perturbation treatment based on a unitary transformation. The dynamical tunneling current is obtained explicitly. The result is compared with the standard perturbation theory at Born-Markov approximation. The decoherence induced by acoustic phonons is analyzed at length. It is shown that the contribution from deformation potential coupling is comparable to that from piezoelectric coupling in small dot size and large tunneling rate case. A possible decoupling mechanism is predicted.
We propose a random matrix theory to describe the influence of a time-dependent external field on electron transport through open quantum dots. We describe the generation of the current by an oscillating field for the dot, connected to two leads with equal chemical potentials. For low frequency fields our results correspond to adiabatic charge pumping. Finite current can be produced if the system goes along a closed loop in parameter space, which covers a finite area. At high frequency finite current is produced even if the loop is a line in parameter space. This result can be explained in the same way as adiabatic pumping but considering the evolution of the system in phase space rather than in parametric space.
A double quantum dot device is a tunable two-level system for electronic energy states. A dc electron current directly measures the rates for elastic and inelastic transitions between the two levels. For inelastic transitions energy is exchanged with bosonic degrees of freedom in the environment. The inelastic transition rates are well described by the Einstein coefficients, relating absorption with stimulated and spontaneous emission. The most effectively coupled bosons in the specific environment of our semiconductor device are acoustic phonons. The experiments demonstrate the importance of vacuum fluctuations in the environment for little circuits of coherent quantum devices.
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