Inhomogeneous Nuclear Spin Flips

We discuss a feedback mechanism between electronic states in a double quantum dot and the underlying nuclear spin bath. We analyze two pumping cycles for which this feedback provides a force for the Overhauser fields of the two dots to either equilibrate or diverge. Which of these effects is favored depends on the g-factor and Overhauser coupling constant A of the material. The strength of the effect increases with A/V_x, where V_x is the exchange matrix element, and also increases as the external magnetic field B_{ext} decreases.Comment: 5 pages, 4 figures (jpg

Interpretations of High-Order Transient Absorption Spectroscopies

Transient absorption (TA) spectroscopy has long been an invaluable tool for determining the energetics and dynamics of excited states in atomic, molecular, and solid-state systems. When pump pulse intensities are sufficiently high, the resulting TA spectra include both the generally desired third-order response of the studied material as well as responses that are higher order in the electric field amplitudes of the pulses. It has recently been shown that pump-intensity-dependent TA measurements allow separating the various orders of response of the TA signal, but the information content available in those higher orders has not been described. We give a general framework, intuition, and nomenclature for understanding the information contained in high-order TA spectra. Standard TA spectra are generally interpreted in terms of three fundamental processes: ground-state bleach (GSB), stimulated emission (SE), and excited state absorption (ESA), and we extend those concepts to higher order. Each order introduces two new processes: SE and ESA from highly excited states that were not accessible in lower orders. In addition, each order contain negations of lower-order processes, just as GSB is a negation of the linear absorption. We show the new spectral and dynamical information that is introduced at each order and show how the relative signs of the signals in different orders can be used to identify which processes are dominant.Comment: 15 pages, 7 figure

Estimating causal networks in biosphere–atmosphere interaction with the PCMCI approach

Local meteorological conditions and biospheric activity are tightly coupled. Understanding these links is an essential prerequisite for predicting the Earth system under climate change conditions. However, many empirical studies on the interaction between the biosphere and the atmosphere are based on correlative approaches that are not able to deduce causal paths, and only very few studies apply causal discovery methods. Here, we use a recently proposed causal graph discovery algorithm, which aims to reconstruct the causal dependency structure underlying a set of time series. We explore the potential of this method to infer temporal dependencies in biosphere-atmosphere interactions. Specifically we address the following questions: How do periodicity and heteroscedasticity influence causal detection rates, i.e. the detection of existing and non-existing links? How consistent are results for noise-contaminated data? Do results exhibit an increased information content that justifies the use of this causal-inference method? We explore the first question using artificial time series with well known dependencies that mimic real-world biosphere-atmosphere interactions. The two remaining questions are addressed jointly in two case studies utilizing observational data. Firstly, we analyse three replicated eddy covariance datasets from a Mediterranean ecosystem at half hourly time resolution allowing us to understand the impact of measurement uncertainties. Secondly, we analyse global NDVI time series (GIMMS 3g) along with gridded climate data to study large-scale climatic drivers of vegetation greenness. Overall, the results confirm the capacity of the causal discovery method to extract time-lagged linear dependencies under realistic settings. The violation of the method's assumptions increases the likelihood to detect false links. Nevertheless, we consistently identify interaction patterns in observational data. Our findings suggest that estimating a directed biosphere-atmosphere network at the ecosystem level can offer novel possibilities to unravel complex multi-directional interactions. Other than classical correlative approaches, our findings are constrained to a few meaningful set of relations which can be powerful insights for the evaluation of terrestrial ecosystem models

Dynamic Nuclear Polarization in Double Quantum Dots

We theoretically investigate the controlled dynamic polarization of lattice nuclear spins in GaAs double quantum dots containing two electrons. Three regimes of long-term dynamics are identified, including the build up of a large difference in the Overhauser fields across the dots, the saturation of the nuclear polarization process associated with formation of so-called "dark states," and the elimination of the difference field. We show that in the case of unequal dots, build up of difference fields generally accompanies the nuclear polarization process, whereas for nearly identical dots, build up of difference fields competes with polarization saturation in dark states. The elimination of the difference field does not, in general, correspond to a stable steady state of the polarization process.Comment: 4 pages, 2 figure

Methodology for vetting heavily doped semiconductors for intermediate band photovoltaics: A case study in sulfur-hyperdoped silicon

We present a methodology for estimating the efficiency potential for candidate impurity-band photovoltaic materials from empirical measurements. This methodology employs both Fourier transform infrared spectroscopy and low-temperature photoconductivity to calculate a “performance figure of merit” and to determine both the position and bandwidth of the impurity band. We evaluate a candidate impurity-band material, silicon hyperdoped with sulfur; we find that the figure of merit is more than one order of magnitude too low for photovoltaic devices that exceed the thermodynamic efficiency limit for single band gap materials.National Science Foundation (U.S.) (Energy, Power, and Adaptive Systems Grant Contract ECCS-1102050)National Science Foundation (U.S.) (United States. Dept. of Energy NSF CA EEC-1041895)Center for Clean Water and Clean Energy at MIT and KFUP

Spin polarized current generation from quantum dots without magnetic fields

An unpolarized charge current passing through a chaotic quantum dot with spin-orbit coupling can produce a spin polarized exit current without magnetic fields or ferromagnets. We use random matrix theory to estimate the typical spin polarization as a function of the number of channels in each lead in the limit of large spin-orbit coupling. We find rms spin polarizations up to 45% with one input channel and two output channels. Finite temperature and dephasing both suppress the effect, and we include dephasing effects using a new variation of the third lead model. If there is only one channel in the output lead, no spin polarization can be produced, but we show that dephasing lifts this restriction.Comment: 7 pages, 3 figures. Revised version with reference to Bardarson, Adagideli, and Jacquod, Phys Rev Lett 98, 196601 (2007), who performed an analogous calculation in a different geometr

Coherent Exciton Dynamics in Supramolecular Light-Harvesting Nanotubes Revealed by Ultrafast Quantum Process Tomography

Long-lived exciton coherences have been recently observed in photosynthetic complexes via ultrafast spectroscopy, opening exciting possibilities for the study and design of coherent exciton transport. Yet, ambiguity in the spectroscopic signals has led to arguments for interpreting them in terms of the exciton dynamics, demanding more stringent tests. We propose a novel strategy, Quantum Process Tomography (QPT) for ultrafast spectroscopy, to reconstruct the evolving quantum state of excitons in double-walled supramolecular light-harvesting nanotubes at room temperature. The protocol calls for eight transient grating experiments with varied pulse spectra. Our analysis reveals unidirectional energy transfer from the outer to the inner wall excitons, absence of nonsecular processes, and an unexpected coherence between those two states lasting about 150 femtoseconds, indicating weak electronic coupling between the walls. Our work constitutes the first experimental QPT in a “warm” and complex system, and provides an elegant scheme to maximize information from ultrafast spectroscopy experiments.Chemistry and Chemical BiologyPhysic