Archive 2016

Perovskite materials with stoichiometry ABX₃ are a rich family of ionic compounds with many technological interesting properties. They can be traditional inorganic, metal per- ovskites or hybrid perovskites with one organic cation. In this talk I want to discuss some results of a special modification of the latter kind, the so-called layered perovskites. This family of structures is currently rediscovered, and we report on the geometrical and electronic structure of one promising candidate ((C₆H₅C₂H₄NH₃)₂PbI₄) with phenethylammonium cations on the A-site and compare the differences towards the benchmark case of three-dimensional (3D) hybrid perovskites, CH₃PbI₃. The influence of varying the cation as well as changing the dimensionality from 3D to 2D systems is discussed by comparing bulk and monolayer structures of both systems. In addition, insight into the optical behavior and the observed electron-phonon coupling will be given. [more]

Working within the Nonequilibrium Green's Function formalism, a formula for the two-time current correlation function is derived for the case of transport through a nanojunction in response to an arbitrary time-dependent bias. The one-particle Hamiltonian and the wide band limit approximation are assumed, enabling us to extract all necessary Green's functions and self-energies for the system, extending the analytic work presented previously [Ridley et al. Phys. Rev. B (2015)]. [more]

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Phenomena that are connected to quantum mechanics, such as magnetism, transport, and the effect of impurity atoms and disorder, and their relation to material design and energy needs are important for almost every branch of the industry. Density functional theory (DFT) was successful at making accurate Predictions for many materials, in particular compounds which have a metallic behaviour. DFT combines high accuracy and moderate computational cost, but the computational effort of performing calculations with conventional DFT approaches is still non negligible and scales with the cube of the number of atoms. A recent optimised implementation of DFT was however shown to scale linearly with the number of atoms (ONETEP), and opened the route to large scale DFT calculations for molecules and nano-structures. Nonetheless, one bottleneck of DFT and ONETEP, is that it fails at describing well some of the compounds where strong correlations are present, in particular because the computational scheme has to capture both the band-like character of the uncorrelated part of the compound and the Mott-like features emerging from the local strongly correlated centres. A recent progress has been made in this direction by the dynamical mean-field theory (DMFT), that allows to describe the two limits (metal and insulator) in a remarkable precise way when combined with DFT. The ONETEP+DMFT implementation and strategies to overcome the main bottlenecks of this type of calculations will be discussed, and its applications illustrated by a few case of studies, such as the role of quantum entanglement in Myoglobin and heme systems. [more]

The possibility to manipulate the electrical properties of matter with very short opticalpulses is a fascinating field of research with possible far reaching applications inmany relevant technological fields. The first step towards the realization of this goal is to understand the ultrafast dynamics at the basis of light-matter interaction. Short and intense pulses allowed us to investigate a very interesting regime where the photon energy becomes comparable to the cycle-averaged kinetic energy of the electrons in the field. As the optical response of the material transitions from a classical to quantum-mechanical description many intriguing effects co-exist in this regime and the importance of inter- versus intra-band transitions is still debated. We used attosecond transient absorption spectroscopy (ATAS) to study the optical response of polycrystalline diamond driven by few-femtosecond, intense (IIR ~1012 W/cm²) infrared (IR) pulses. We monitored the system response by looking at the induced change in the absorbance with a 250-as pulse centred around 40 eV. We observed the appearance of oscillating features which modulate at twice the IR frequency, ωIR, and fully recover after the interaction. Simultaneous photoelectron acquisition from a gas nozzle placed in front of the diamond target allowed us to study the phase relation of the oscillating features and the pumping IR field. We found that the timing of the diamond response changes significantly with the probing energy and does not always follow the IR field adiabatically. Ab initio calculations performed by coupling time-dependent density functional theory (TDDFT) in real time with Maxwell’s equations reproduced the experimental observations. Further comparison with a numerical two-band model allowed us to conclude that intra-band motion dominates over inter-band transitions, thus identifying the dynamical Franz- Keldysh effect as the dominant mechanism in this regime. Our analysis constitutes an important step towards a full understanding of the optical properties of dielectrics in the Petahertz regime. [more]

Flexural and in-plane thermal fluctuations in crystalline membranes affect the band structure of the carriers, which has an effect on transport properties as well as carrier density of states of 2D systems. I consider a specific example of one-layer black phosphorus, which is a highly anisotropic material, and present our recent results on intrinsic carrier mobility. In contrast to graphene, where the mobility is determined by two-phonon (flexural) scattering, in black phosphorus one-phonon (in-plane) processes dominate. I also will show the results on DOS tail for holes in black phosphorus that have quasi-one-dimensional dispersion (my /mx » 1) and, as a result, an enhanced Van Hove singularity at the valence band top. Interaction with flexural phonons results in smearing of this singularity and to an appearing of a tail in DOS in the gap. The material parameters are determined by ab initio GW calculations and then are used for quantitative estimation of the above-mentioned effects. [more]

The talk will cover the resonance energy transfer in light-harvesting systems and entropy transfer in nanomechancial resonators.In the first part, I will present a classical formulation of the quantum multichromophoric theory of resonance energy transfer developed on the basis of classical electrodynamics. The theory allows for the identification of a variety of processes of different order in the interactions that contribute to the energy transfer in molecular aggregates with intracoupling in donors and acceptor chromophores. Enhanced rates in multichromophoric resonance energy transfer are shown to be well described by this theory. Specifically, in a coupling configuration between $N_A$ acceptors and $N_D$ donors, the theory correctly predicts an enhancement of the energy transfer rate dependent on the total number of donoracceptor pairs. As an example, the theory, applied to the transfer rate in light harvesting II, gives results in excellent agreement with experiment. Finally, it is explicitly shown that as long as linear response theory holds, the classical multichromophoric theory formally coincides with the quantum formulation.In the second part, I will present a sideband cooling strategy that incorporates (i) the dynamics induced by structured (non-Markovian) environments in the target and auxiliary systems and (ii) the optimally time-modulated interaction between them. For the context of cavity optomechanics, when non-Markovian dynamics are considered in the target system, ground state cooling is reached at much faster rates and at much lower phonon occupation number than previously reported. In contrast to similar current strategies, ground state cooling is reached here for coupling-strength rates that are experimentally accessible for the state-of-the-art implementations. After the ultrafast optimal-ground-state-cooling protocol is accomplished, an additional optimal control strategy is considered to maintain the phonon number as closer as possible to the one obtained in the cooling procedure. Contrary to the conventional expectation, when non-Markovian dynamics are considered in the auxiliary system, the efficiency of the cooling protocol is undermined. [more]

In this talk I will describe the evolution of our understanding on how to describe transport through strongly correlated systems in the framework of density functional theory (DFT).A first indication that DFT might be useful to tackle this situation came with the realization that the Kondo plateau in the zero-bias conductance may already be captured at the level of standard Landauer theory combined with DFT. Later it has been shown how the description of Coulomb blockade in the zero-bias limit can be achieved within DFT. In a more recent development we have proposed a DFT formalism to describe electronic transport in the steady state which uses the density on the junction and the steady current as basic variables. In a finite window around zero bias, a one-to-one map is established between the basic variables and both local potential on as well as bias across the junction. The resulting Kohn-Sham system features two exchange-correlation (xc) potentials, a local xc potential and an xc contribution to the bias. For weakly coupled junctions the xc potentials exhibit steps in the density-current plane which are shown to be crucial to describe the Coulomb blockade diamonds.Finally, I will present a recent parametrization of the xc potentials for the single-impurity Anderson model which correctly incorporates both the Kondo and Coulomb blockade regimes, i.e., both zero and finite temperature. This parametrization allows for calculation of currents and differential conductances at arbitrary bias and temperature at negligible numerical cost but with the accuracy of sophisticated renormalization group methods. [more]

Since 2000, we have been developing a real-time, real-space computationalmethod based on time-dependent density functional theory to describe electron dynamics in crystalline solids induced by light pulses. In a microscopic scale, we solve the time-dependent Kohn-Sham equation in a unit cell of solid treating the applied electric field is by the vector potential. We further combine the microscopic calculation with the dynamics of light electromagnetic field in a multiscale modeling, as describe in the figure. In my presentation, I first explain our method including some historical aspects. Then I will show some recent and on-going applications such as energy transfer from a femtosecond laser pulse to electrons in quartz and graphite, and ultrafast changes of dielectric properties of diamond by an intense laser pulse. [more]

Van der Waals heterostructures (vdWHs) represent a novel and largely unexplored class of materials. Since 2013, when Geim and Grigorieva first conceived the stacking of 2D (two-dimensional) materials to create artificial layered structures with tailored properties, a number of promising (opto)electronics devices, e.g. light emitting diodes, solar cells, ultra-fast photodetectors, transistors etc. have been successfully fabricated. It is well established that for isolated 2D semiconductors and vdWHs the optical response is governed by excitonic effects. A theoretical understanding of excitonic effects and of how the electronic screening is affected for the more complex case of multi-layer structures is still lacking due to the computational limitations of standard ab-initio methods. [more]

The progress in quantum optics utilizes a unique photon state configuration for engineering of the ultimate light-matter interactions with relatively simple material systems. It results in a broad range of photonic applications including radiation sources, quantum communication, information, computing and nanotechnology. The development of the ultrafast multidimensional nonlinear spectroscopy that has been enabled by progress in ultrafast optical technology provides a unique tool for probing complex molecules, semiconductors, nanomaterials by classical light fields. [more]

Spurred by recent progress in melting, enhancement and induction of electronic order out of equilibrium, a tantalizing prospect concerns instead accessing transient Floquet steady states via broad pump pulses, to affect electronic properties. [more]

The new paradigm of topology in condensed matter physics does not only pertain to insulators and semimetals but also to superconductors. Topological superconductors are predicted to show many novel physical properties. [more]

Time evolution in ensembles of quantum emitters (atoms, molecules, ions, Rydberg atoms, quantum dots etc) at low vs. high densities is fundamentally different. As particles get closer together, strong environment-mediated interactions start playing an important role both in the coherent (such as dipole-dipole interactions) as well as in the incoherent evolution (super- /subradiance). [more]

Which features make the brain such a powerful and energy-efficient computing machine? Can we reproduce them in the solid state, and if so, what type of computing paradigm would we obtain? [more]

The particle-hole map (PHM) is a new visualization tool to analyze electronic excitations in molecules in the time- or frequency domain, to be used in conjunction with TDDFT or other ab initio methods [1–3]. The purpose of the PHM is to give detailed insight into electronic excitation processes which is not obtainable from local visualization methods such as transition densities, density differences, or natural transition orbitals. The PHM provides information on the origins, destinations, and coherences of charge fluctuations during an excitation process. In contrast with the transition density matrix, the PHM has a statistical interpretation involving joint probabilities of individual states and their transitions, and it is easier to read and interpret. [more]

The photoinduced charge-separation events occurring in photovoltaic and light harvesting systems have traditionally been interpreted in terms of the incoherent kinetics of optical excitations and of charge hopping. Although signatures of quantum coherence were recently observed in energy transfer in photosynthetic bacteria andalgae[1] still very little is known about the role of quantum coherence at room temperature in technologically relevant organic photovoltaic materials. Recent experiments found evidence for an ultrafast long-range charge separation in such systems but could not differentiate between coherent and incoherent charge-transfermodels.[2] [more]

Light-matter interactions have been extensively studied by physicist in quantum optics and condensed matter physics, [1] but there are only fewer attempts to understand this effect in molecular science. [2, 3] [more]

The coupling and mutual dependence of electronic and vibrational degrees of freedom is at the heart of microscopic as well as macroscopic phenomena in condensed matter. Ultrafast pump-probe techniques provide experimental access to these coupling and correlation effects by revealing the response of electrons and lattice to specific excitation of a material. [more]

Coupled cluster theory is the dominant method in wave function-based calculations in systems of small to moderate size. It provides exceptionally accurate predictions for a wide array of energetics and properties. Moreover, it is size extensive, meaning that it can fruitfully be applied to condensed systems, provided only that one has computational resources sufficient for the task. Unfortunately, coupled cluster theory often breaks down in the presence of strong correlations, such as those responsible for superconductivity or various magnetically-ordered states. [more]

Quantum transport is often discussed in the steady-state regime where the characteristics of the system are described in terms of the energy-dependent transmission or conductance. There is, however, no guarantee that this description would capture the essential physics in, say, atomic-scale junction operating at high frequencies. Therefore, we look for an accurate theory for describing the full time-dependence. The time-dependence also provides us with ''transient spectroscopy'' which can give detailed information about the nanosystems out of equilibrium. [more]

In this talk, I will first give an introduction to Majorana bound states (MBS), zero-energy modes predicted to appear in exotic spin-polarized p-wave superconductors. MBS satisfy non-Abelian statistics and, in addition, encode quantum information in a topologically protected manner, which makes them highly interesting for quantum computation applications. The required p-wave superconductivity seems to be hard to find in nature, but recent theoretical works have shown that it can instead be artificially engineered, for example in a semiconductor nanowire with strong spin-orbit coupling which is covered by a superconductor and exposed to a magnetic field. I will also discuss the recent experimental progress towards creating and detecting MBS. [more]

Competition between ordered phases, and their associated phase transitions, are significant in the study of strongly correlated systems. [more]

The workshop covers advances and challenges in the simulation of materials and the description of light-matter interactions in molecules and solids. [more]

The development of efficient ways to exploit the energy from the sun is an issue of major importance. Among possible solutions, the employment of solar energy to promote chemical reactions has the advantage of addressing the problems of harvesting, converting and storing energy at the same time. In this context, water splitting plays a central role both for direct hydrogen production and for the production of hydrocarbons. Therefore, great attention has been recently devoted to hydrogen production by means of photoelectrochemical (PEC) cells, via water splitting to molecular hydrogen and oxygen. The main challenge is to develop anode materials for these cells that can split water efficiently. [more]

The alkali-doped fullerides (A₃C₆₀, A = K, Rb, Cs) show a highest superconducting transition temperature (Tc) among molecular solids. In the phase diagram, s-wave superconductivity (SC) lies next to Mott insulating phase. This adjacency is similar to the cuprates (d-wave SC) but is more surprising because s-wave SC is believed to be severely suppressed by strong correlations. [more]

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