Time-dependent density functional theory

Due to their bandgap engineering capabilities for optoelectronics applications, the study of nano-graphene has been a topic of interest to researchers in recent years. Using a first-principles study based on density functional theory (DFT) and thermal DFT, we investigated the electronic structures and optical properties of bilayer graphene quantum dots (GQDs). The dielectric tensors, absorption spectra, and the refractive indexes of the bilayer GQDs were obtained for both in-plane and out-of-plane polarization. In addition, we calculated the absorption spectra via time-dependent DFT (TD-DFT) in the linear response regime. The TDDFT results show that a blue shift occurs in the absorption spectrum, which is consistent with the experimental results. In this investigation, we consider triangular and hexagonal GQDs of various sizes with zigzag and armchair edges. Our simulations show that unlike monolayer GQDs, for which light absorption for out-of-plane polarization occurs in the ultraviolet wavelength range of 85-250 nm, the out-of-plane polarization light absorption peaks in the bilayer GQDs appear in the near-infrared range of 500-1600 nm, similar to those in bilayer graphene sheets. The out-of-plane polarization light absorption peaks in the near-infrared range make bilayer GQDs suitable for integrated optics and optical communication applications.

Das Verbundprojekt SIMULTAN erforscht die Früherkennung für Instabilität, Unruhe und Kollaps von Erdfällen. Der neuartige Forschungsansatz kombiniert strukturelle, geophysikalische, petrophysikalische und hydrologische Kartierungsmethoden, die von Sensorentwicklung und mulit-skaliger Überwachung flankiert werden, und umfasst eine Informationsplattform. Kollapsprozesse an Erdfällen finden generell in den obersten wenigen 100 Metern der Erdkruste statt. Individuelle Prozesskomponenten können einfach sein und verstanden werden. Aber es wechselwirken auch Prä-Kollapsprozesse und Vorläufer auf unterschiedlichen raum-zeitlichen Skalen und mit kleinen Variationen miteinander. Dies erfordert innovative, multi-skalige Beobachtungen, Analysen und integrierte Früherkennungskonzepte, besonders für urbane Bereiche, die bisher noch nicht vollständig entwickelt verfügbar sind und auch noch nicht als automatische operationelle Systeme arbeiten. Zur Identifizierung und Quantifizierung von Subrosionsbereichen zeigten sich bohrlochseismische Verfahren mit kombinierten P- und S-Wellen als zielführend. Als besonderer Indikator, der sich auch für Langzeitmonitoring eignet, hat sich dabei das ungewöhnliche Konversionsverhalten der Wellen in Subrosionszonen gezeigt. Neue Prozessingverfahren zur Detektion kleiner seismischer Ereignisse und für emergente Einsätze unterstützen den Ansatz von angepassten Arraymessungen. Geodätisch-gravimetrische Überwachungsnetze sind auch unter urbanen Bedingungen geeignet, durch Subrosion verursachte Oberflächendeformationen und Massenverlagerungen räumlich-zeitlich zu erfassen und zu überwachen. Nivellements liefern bezüglich der Oberflächendeformation höchste Genauigkeiten; zugleich sind sie vergleichsweise kostengünstig zu realisieren. Die Integration von GNSS hat in Verbindung mit dem Nivellement die räumliche Auflösung im Untersuchungsgebiet zusätzlich gestützt und hat das Potenzial, diese großräumig zu kontrollieren. Gravimetrische Messungen sind mit einem sehr hohen Aufwand verbunden. Die Kombination oberflächengeophysikalischer Verfahren mit einer vertikal hochaufgelösten direct push-basierten Erkundung im Raum mit einem maßgeschneiderten hydrogeologischen Monitoring bietet eine zuverlässige Grundlage für numerische Prozessmodellierungen und ermöglichen es, erdfallrelevante Prozesse abzubilden und zu erfassen. Karstaquifer- und geomechanische Modellierungen konnten die Prozesse in den Fokusgebieten erfolgreich abbilden, sobald diese mit realistischen Werten unterlegt wurden. Es zeigt sich somit insgesamt, dass sowohl flächenhafte Messungen und zeitlich wiederholte Kampagnen sehr vorteilhaft sind, da sie es erlauben, Fehler zu verringern und beanspruchte Bereiche einzugrenzen. Erst dieses integrierte Vorgehen ermöglicht es, potenzielle Wegsamkeiten im Untergrund hochauflösender als bisher abzubilden und zu bewerten. Als solches stellt es ein Instrumentarium zur Charakterisierung und angepassten Überwachung von Untergrundbereichen im Allgemeinen zur Verfügung. Diese Ergebnisse und Szenarien stehen der Öffentlichkeit auf einer Informationsplattform zur Verfügung (http://simultan.gfz-potsdam.de).

Abstract: {\tt yambo} is an {\it ab initio} code for calculating quasiparticle energies and optical properties of electronic systems within the framework of many-body perturbation theory and time-dependent density functional theory. Quasiparticle energies are calculated within the ...

The method developed recently for prediction of 1s electron spectra is now extended to the 2p spectra of SiH4, PH3, H2S, HCl, and Ar. The method for X-ray absorption spectra involves the use of ΔE for the excitation and ionization energies, and application of time-dependent density functional theory using the exchange-correlation potential known as statistical average of orbital potentials for the intensities. Additional assumptions and approximations are also made. The best exchange-correlation functional Exc for the earlier calculation of ΔE in 1s spectra of C to Ne (namely Perdew–Wang 1986 exchange, combined with Perdew–Wang 1991 correlation) is no longer used in this work on 2p spectra of Si to Ar. Instead, recently tested Exc good for 2p core-electron binding energies (known as OPTX) for exchange and LYP for correlation, plus scalar zeroth-order regular approximation is adopted here for the ΔE calculations. Our calculated X-ray absorption spectra are generally in good agreement with experiment. Although the predictions for the higher excitations suffer from basis set difficulties, our procedure should be helpful in the interpretation of absorption spectra of 2p electrons of Si to Ar. In addition, we report calculated results for other kinds of electron spectra for SiH4, PH3, H2S, HCl, and Ar, including valence electron ionizations and excitations as well as X-ray emission. © 2008 Wiley Periodicals, Inc. Int J Quantum Chem, 2008

A matrix-dynamical perspective on explicitly dependent quantum systems, this summary covers all main aspects of higher-dimensional groups on SU(3), elliptical symmetries, invariants, PDE calculus and hypergeometric matrix calculus. New group structures are developed and applied to exotic physical systems with particular application for the future development of fast processing and time optimal quantum logic on trit states.

We present the theoretical and technical foundations of the Amsterdam Density Functional (ADF) program with a survey of the characteristics of the code (numerical integration, density fitting for the Coulomb potential, and STO basis functions). Recent developments enhance the efficiency of ADF (e.g., parallelization, near order-N scaling, QM/MM) and its functionality (e.g., NMR chemical shifts, COSMO solvent effects, ZORA relativistic method, excitation energies, frequency-dependent (hyper)polarizabilities, atomic VDD charges). In the Applications section we discuss the physical model of the electronic structure and the chemical bond, i.e., the Kohn–Sham molecular orbital (MO) theory, and illustrate the power of the Kohn–Sham MO model in conjunction with the ADF-typical fragment approach to quantitatively understand and predict chemical phenomena. We review the “Activation-strain TS interaction” (ATS) model of chemical reactivity as a conceptual framework for understanding how activation barriers of various types of (competing) reaction mechanisms arise and how they may be controlled, for example, in organic chemistry or homogeneous catalysis. Finally, we include a brief discussion of exemplary applications in the field of biochemistry (structure and bonding of DNA) and of time-dependent density functional theory (TDDFT) to indicate how this development further reinforces the ADF tools for the analysis of chemical phenomena. © 2001 John Wiley & Sons, Inc. J Comput Chem 22: 931–967, 2001

The optical properties of two-dimensional (2D) materials are accurately described by many-body methods including specifically pronounced electron−electron and electron−hole effects. Such methods are, however, computationally demanding and applicable on small computational cells only. We provide approximate optical gaps for 2D materials from time-dependent (TD) density functional theory based on a set of specific screened hybrid functionals and show that this approach effectively accounts for all important physical effects including excitons. Optical gap values obtained from the TD-HSE06 approach for a broad gap range 1−6 eV of eight 2D materials are in agreement with both experimental optical gaps and accurate GW+BSE calculations. Further, we show that such an approach is eligible and practicable for van der Waals heterostructures containing incommensurate cells of different monolayers and enables detailed analysis of intra-and interlayer excitonic wave functions. TD-HSE06 is therefore a suitable method for a reliable description of the optical properties of extended periodic 2D systems.

A recently introduced formulation of time dependent linear response density functional theory within the plane-wave pseudopotential framework 􏰉J. Hutter, J. Chem. Phys. 118, 3928 􏰞2003􏰀􏰁 is
n→􏰛* electronic
applied to the study of solvent shift and intensity enhancement effects of the 1A
transition in acetone, treating solute and solvent at the same level of theory. We propose a suitable formalism for computing transition intensities based on the modern theory of polarization, which is applicable to condensed-phase and finite systems alike. The gain in intensity brought about by thermal fluctuations is studied in molecular acetone at room temperature, and in gas-phase ( CH3 ) 2 CO• ( H2 O) 2 at 25 K. The latter system is characterized by the appearance of relatively intense features in the low-energy region of the spectrum, attributable to spurious solvent →solute charge-transfer excitations created by deficiencies in the DFT methodology. The n→􏰛* transition can be partially isolated from the charge-transfer bands, yielding a blueshift of 0.17 eV with respect to gas-phase acetone. This analysis is then carried over to a solution of acetone in water, where further complications are encountered in the from of a solute→solvent charge transfer excitations overlapping with the n→􏰛* band. The optically active occupied states are found to be largely localized on either solute or solvent, and using this feature we were again able to isolate the physical n→􏰛* band and compute the solvatochromic shift. The result of 0.19 eV is in good agreement with experiment, as is the general increase in the mean oscillator strength of the transition. The unphysical charge transfers are interpreted in terms of degeneracies in the spectrum of orbital energies of the aqueous acetone solution.

This paper presents a solution to real-world delivery problems (RWDPs) for home delivery services where a large number of roads exist in cities and the traffic on the roads rapidly changes with time. The methodology for finding the shortest-travel-time tour includes a hybrid meta-heuristic that combines ant colony optimization (ACO) with Dijkstra's algorithm, a search technique that uses both real-time traffic and predicted traffic, and a way to use a real-world road map and measured traffic in Japan. We previously proposed a hybrid ACO for RWDPs that used a MAX-MIN Ant System (MMAS) and proposed a method to improve the search rate of MMAS. Since traffic on roads changes with time, the search rate is important in RWDPs. In the current work, we combine the hybrid ACO method with the improved MMAS. Experimental results using a map of central Tokyo and historical traffic data indicate that the proposed method can find a better solution than conventional methods.

Time-dependent density-functional theory in the projector augmented-wave method. [The Journal of Chemical Physics 128, 244101 (2008)]. Michael Walter, Hannu Häkkinen, Lauri Lehtovaara, Martti Puska, Jussi Enkovaara, Carsten Rostgaard, Jens Jørgen Mortensen. Abstract. ...