Quantum wavepacket ab initio molecular dynamics: an approach for computing dynamically averaged vibrational spectra including critical nuclear quantum effects.

PubMed

Sumner, Isaiah; Iyengar, Srinivasan S

2007-10-18

We have introduced a computational methodology to study vibrational spectroscopy in clusters inclusive of critical nuclear quantum effects. This approach is based on the recently developed quantum wavepacket ab initio molecular dynamics method that combines quantum wavepacket dynamics with ab initio molecular dynamics. The computational efficiency of the dynamical procedure is drastically improved (by several orders of magnitude) through the utilization of wavelet-based techniques combined with the previously introduced time-dependent deterministic sampling procedure measure to achieve stable, picosecond length, quantum-classical dynamics of electrons and nuclei in clusters. The dynamical information is employed to construct a novel cumulative flux/velocity correlation function, where the wavepacket flux from the quantized particle is combined with classical nuclear velocities to obtain the vibrational density of states. The approach is demonstrated by computing the vibrational density of states of [Cl-H-Cl]-, inclusive of critical quantum nuclear effects, and our results are in good agreement with experiment. A general hierarchical procedure is also provided, based on electronic structure harmonic frequencies, classical ab initio molecular dynamics, computation of nuclear quantum-mechanical eigenstates, and employing quantum wavepacket ab initio dynamics to understand vibrational spectroscopy in hydrogen-bonded clusters that display large degrees of anharmonicities.

On the limiting characteristics of quantum random number generators at various clusterings of photocounts

NASA Astrophysics Data System (ADS)

Molotkov, S. N.

2017-03-01

Various methods for the clustering of photocounts constituting a sequence of random numbers are considered. It is shown that the clustering of photocounts resulting in the Fermi-Dirac distribution makes it possible to achieve the theoretical limit of the random number generation rate.

Free-energy landscapes from adaptively biased methods: Application to quantum systems

NASA Astrophysics Data System (ADS)

Calvo, F.

2010-10-01

Several parallel adaptive biasing methods are applied to the calculation of free-energy pathways along reaction coordinates, choosing as a difficult example the double-funnel landscape of the 38-atom Lennard-Jones cluster. In the case of classical statistics, the Wang-Landau and adaptively biased molecular-dynamics (ABMD) methods are both found efficient if multiple walkers and replication and deletion schemes are used. An extension of the ABMD technique to quantum systems, implemented through the path-integral MD framework, is presented and tested on Ne38 against the quantum superposition method.

pyCTQW: A continuous-time quantum walk simulator on distributed memory computers

NASA Astrophysics Data System (ADS)

Izaac, Josh A.; Wang, Jingbo B.

2015-01-01

In the general field of quantum information and computation, quantum walks are playing an increasingly important role in constructing physical models and quantum algorithms. We have recently developed a distributed memory software package pyCTQW, with an object-oriented Python interface, that allows efficient simulation of large multi-particle CTQW (continuous-time quantum walk)-based systems. In this paper, we present an introduction to the Python and Fortran interfaces of pyCTQW, discuss various numerical methods of calculating the matrix exponential, and demonstrate the performance behavior of pyCTQW on a distributed memory cluster. In particular, the Chebyshev and Krylov-subspace methods for calculating the quantum walk propagation are provided, as well as methods for visualization and data analysis.

Nanoscale patterning of colloidal quantum dots on transparent and metallic planar surfaces.

PubMed

Park, Yeonsang; Roh, Young-Geun; Kim, Un Jeong; Chung, Dae-Young; Suh, Hwansoo; Kim, Jineun; Cheon, Sangmo; Lee, Jaesoong; Kim, Tae-Ho; Cho, Kyung-Sang; Lee, Chang-Won

2012-09-07

The patterning of colloidal quantum dots with nanometer resolution is essential for their application in photonics and plasmonics. Several patterning approaches, such as the use of polymer composites, molecular lock-and-key methods, inkjet printing and microcontact printing of quantum dots have been recently developed. Herein, we present a simple method of patterning colloidal quantum dots for photonic nanostructures such as straight lines, rings and dot patterns either on transparent or metallic substrates. Sub-10 nm width of the patterned line could be achieved with a well-defined sidewall profile. Using this method, we demonstrate a surface plasmon launcher from a quantum dot cluster in the visible spectrum.

Quantum cluster variational method and message passing algorithms revisited

NASA Astrophysics Data System (ADS)

Domínguez, E.; Mulet, Roberto

2018-02-01

We present a general framework to study quantum disordered systems in the context of the Kikuchi's cluster variational method (CVM). The method relies in the solution of message passing-like equations for single instances or in the iterative solution of complex population dynamic algorithms for an average case scenario. We first show how a standard application of the Kikuchi's CVM can be easily translated to message passing equations for specific instances of the disordered system. We then present an "ad hoc" extension of these equations to a population dynamic algorithm representing an average case scenario. At the Bethe level, these equations are equivalent to the dynamic population equations that can be derived from a proper cavity ansatz. However, at the plaquette approximation, the interpretation is more subtle and we discuss it taking also into account previous results in classical disordered models. Moreover, we develop a formalism to properly deal with the average case scenario using a replica-symmetric ansatz within this CVM for quantum disordered systems. Finally, we present and discuss numerical solutions of the different approximations for the quantum transverse Ising model and the quantum random field Ising model in two-dimensional lattices.

Thermalization as an invisibility cloak for fragile quantum superpositions

NASA Astrophysics Data System (ADS)

Hahn, Walter; Fine, Boris V.

2017-07-01

We propose a method for protecting fragile quantum superpositions in many-particle systems from dephasing by external classical noise. We call superpositions "fragile" if dephasing occurs particularly fast, because the noise couples very differently to the superposed states. The method consists of letting a quantum superposition evolve under the internal thermalization dynamics of the system, followed by a time-reversal manipulation known as Loschmidt echo. The thermalization dynamics makes the superposed states almost indistinguishable during most of the above procedure. We validate the method by applying it to a cluster of spins ½.

Thermal helium clusters at 3.2 Kelvin in classical and semiclassical simulations

NASA Astrophysics Data System (ADS)

Schulte, J.

1993-03-01

The thermodynamic stability of4He4-13 at 3.2 K is investigated with the classical Monte Carlo method, with the semiclassical path-integral Monte Carlo (PIMC) method, and with the semiclassical all-order many-body method. In the all-order many-body simulation the dipole-dipole approximation including short-range correction is used. The resulting stability plots are discussed and related to recent TOF experiments by Stephens and King. It is found that with classical Monte Carlo of course the characteristics of the measured mass spectrum cannot be resolved. With PIMC, switching on more and more quantum mechanics. by raising the number of virtual time steps results in more structure in the stability plot, but this did not lead to sufficient agreement with the TOF experiment. Only the all-order many-body method resolved the characteristic structures of the measured mass spectrum, including magic numbers. The result shows the influence of quantum statistics and quantum mechanics on the stability of small neutral helium clusters.

Method for discovering relationships in data by dynamic quantum clustering

DOEpatents

Weinstein, Marvin; Horn, David

2017-05-09

Data clustering is provided according to a dynamical framework based on quantum mechanical time evolution of states corresponding to data points. To expedite computations, we can approximate the time-dependent Hamiltonian formalism by a truncated calculation within a set of Gaussian wave-functions (coherent states) centered around the original points. This allows for analytic evaluation of the time evolution of all such states, opening up the possibility of exploration of relationships among data-points through observation of varying dynamical-distances among points and convergence of points into clusters. This formalism may be further supplemented by preprocessing, such as dimensional reduction through singular value decomposition and/or feature filtering.

Method for discovering relationships in data by dynamic quantum clustering

DOEpatents

Weinstein, Marvin; Horn, David

2014-10-28

Data clustering is provided according to a dynamical framework based on quantum mechanical time evolution of states corresponding to data points. To expedite computations, we can approximate the time-dependent Hamiltonian formalism by a truncated calculation within a set of Gaussian wave-functions (coherent states) centered around the original points. This allows for analytic evaluation of the time evolution of all such states, opening up the possibility of exploration of relationships among data-points through observation of varying dynamical-distances among points and convergence of points into clusters. This formalism may be further supplemented by preprocessing, such as dimensional reduction through singular value decomposition and/or feature filtering.

Methanol in its own gravy. A PCM study for simulation of vibrational spectra.

PubMed

Billes, Ferenc; Mohammed-Ziegler, Ildikó; Mikosch, Hans

2011-05-07

For studying both hydrogen bond and dipole-dipole interactions between methanol molecules (self-association) the geometry of clusters of increasing numbers of methanol molecules (n = 1,2,3) were optimized and also their vibrational frequencies were calculated with quantum chemical methods. Beside these B3LYP/6-311G** calculations, PCM calculations were also done for all systems with PCM at the same quantum chemical method and basis set, for considering the effect of the liquid continuum on the cluster properties. Comparing the results, the measured and calculated infrared spectra are in good accordance. This journal is © the Owner Societies 2011

Quantum criticality of one-dimensional multicomponent Fermi gas with strongly attractive interaction

NASA Astrophysics Data System (ADS)

He, Peng; Jiang, Yuzhu; Guan, Xiwen; He, Jinyu

2015-01-01

Quantum criticality of strongly attractive Fermi gas with SU(3) symmetry in one dimension is studied via the thermodynamic Bethe ansatz (TBA) equations. The phase transitions driven by the chemical potential μ , effective magnetic field H1, H2 (chemical potential biases) are analyzed at the quantum criticality. The phase diagram and critical fields are analytically determined by the TBA equations in the zero temperature limit. High accurate equations of state, scaling functions are also obtained analytically for the strong interacting gases. The dynamic exponent z=2 and correlation length exponent ν =1/2 read off the universal scaling form. It turns out that the quantum criticality of the three-component gases involves a sudden change of density of states of one cluster state, two or three cluster states. In general, this method can be adapted to deal with the quantum criticality of multicomponent Fermi gases with SU(N) symmetry.

Random Walk Quantum Clustering Algorithm Based on Space

NASA Astrophysics Data System (ADS)

Xiao, Shufen; Dong, Yumin; Ma, Hongyang

2018-01-01

In the random quantum walk, which is a quantum simulation of the classical walk, data points interacted when selecting the appropriate walk strategy by taking advantage of quantum-entanglement features; thus, the results obtained when the quantum walk is used are different from those when the classical walk is adopted. A new quantum walk clustering algorithm based on space is proposed by applying the quantum walk to clustering analysis. In this algorithm, data points are viewed as walking participants, and similar data points are clustered using the walk function in the pay-off matrix according to a certain rule. The walk process is simplified by implementing a space-combining rule. The proposed algorithm is validated by a simulation test and is proved superior to existing clustering algorithms, namely, Kmeans, PCA + Kmeans, and LDA-Km. The effects of some of the parameters in the proposed algorithm on its performance are also analyzed and discussed. Specific suggestions are provided.

The Feigin Tetrahedron

NASA Astrophysics Data System (ADS)

Rupel, Dylan

2015-03-01

The first goal of this note is to extend the well-known Feigin homomorphisms taking quantum groups to quantum polynomial algebras. More precisely, we define generalized Feigin homomorphisms from a quantum shuffle algebra to quantum polynomial algebras which extend the classical Feigin homomorphisms along the embedding of the quantum group into said quantum shuffle algebra. In a recent work of Berenstein and the author, analogous extensions of Feigin homomorphisms from the dual Hall-Ringel algebra of a valued quiver to quantum polynomial algebras were defined. To relate these constructions, we establish a homomorphism, dubbed the quantum shuffle character, from the dual Hall-Ringel algebra to the quantum shuffle algebra which relates the generalized Feigin homomorphisms. These constructions can be compactly described by a commuting tetrahedron of maps beginning with the quantum group and terminating in a quantum polynomial algebra. The second goal in this project is to better understand the dual canonical basis conjecture for skew-symmetrizable quantum cluster algebras. In the symmetrizable types it is known that dual canonical basis elements need not have positive multiplicative structure constants, while this is still suspected to hold for skew-symmetrizable quantum cluster algebras. We propose an alternate conjecture for the symmetrizable types: the cluster monomials should correspond to irreducible characters of a KLR algebra. Indeed, the main conjecture of this note would establish this ''KLR conjecture'' for acyclic skew-symmetrizable quantum cluster algebras: that is, we conjecture that the images of rigid representations under the quantum shuffle character give irreducible characters for KLR algebras. We sketch a proof in the symmetric case giving an alternative to the proof of Kimura-Qin that all non-initial cluster variables in an acyclic skew-symmetric quantum cluster algebra are contained in the dual canonical basis. With these results in mind we interpret the cluster mutations directly in terms of the representation theory of the KLR algebra.

Quantum trajectories for time-dependent adiabatic master equations

NASA Astrophysics Data System (ADS)

Yip, Ka Wa; Albash, Tameem; Lidar, Daniel A.

2018-02-01

We describe a quantum trajectories technique for the unraveling of the quantum adiabatic master equation in Lindblad form. By evolving a complex state vector of dimension N instead of a complex density matrix of dimension N2, simulations of larger system sizes become feasible. The cost of running many trajectories, which is required to recover the master equation evolution, can be minimized by running the trajectories in parallel, making this method suitable for high performance computing clusters. In general, the trajectories method can provide up to a factor N advantage over directly solving the master equation. In special cases where only the expectation values of certain observables are desired, an advantage of up to a factor N2 is possible. We test the method by demonstrating agreement with direct solution of the quantum adiabatic master equation for 8-qubit quantum annealing examples. We also apply the quantum trajectories method to a 16-qubit example originally introduced to demonstrate the role of tunneling in quantum annealing, which is significantly more time consuming to solve directly using the master equation. The quantum trajectories method provides insight into individual quantum jump trajectories and their statistics, thus shedding light on open system quantum adiabatic evolution beyond the master equation.

Adapting the traveling salesman problem to an adiabatic quantum computer

NASA Astrophysics Data System (ADS)

Warren, Richard H.

2013-04-01

We show how to guide a quantum computer to select an optimal tour for the traveling salesman. This is significant because it opens a rapid solution method for the wide range of applications of the traveling salesman problem, which include vehicle routing, job sequencing and data clustering.

Quantum cluster algebras and quantum nilpotent algebras.

PubMed

Goodearl, Kenneth R; Yakimov, Milen T

2014-07-08

A major direction in the theory of cluster algebras is to construct (quantum) cluster algebra structures on the (quantized) coordinate rings of various families of varieties arising in Lie theory. We prove that all algebras in a very large axiomatically defined class of noncommutative algebras possess canonical quantum cluster algebra structures. Furthermore, they coincide with the corresponding upper quantum cluster algebras. We also establish analogs of these results for a large class of Poisson nilpotent algebras. Many important families of coordinate rings are subsumed in the class we are covering, which leads to a broad range of applications of the general results to the above-mentioned types of problems. As a consequence, we prove the Berenstein-Zelevinsky conjecture [Berenstein A, Zelevinsky A (2005) Adv Math 195:405-455] for the quantized coordinate rings of double Bruhat cells and construct quantum cluster algebra structures on all quantum unipotent groups, extending the theorem of Geiß et al. [Geiß C, et al. (2013) Selecta Math 19:337-397] for the case of symmetric Kac-Moody groups. Moreover, we prove that the upper cluster algebras of Berenstein et al. [Berenstein A, et al. (2005) Duke Math J 126:1-52] associated with double Bruhat cells coincide with the corresponding cluster algebras.

Quantum cluster algebras and quantum nilpotent algebras

PubMed Central

Goodearl, Kenneth R.; Yakimov, Milen T.

2014-01-01

A major direction in the theory of cluster algebras is to construct (quantum) cluster algebra structures on the (quantized) coordinate rings of various families of varieties arising in Lie theory. We prove that all algebras in a very large axiomatically defined class of noncommutative algebras possess canonical quantum cluster algebra structures. Furthermore, they coincide with the corresponding upper quantum cluster algebras. We also establish analogs of these results for a large class of Poisson nilpotent algebras. Many important families of coordinate rings are subsumed in the class we are covering, which leads to a broad range of applications of the general results to the above-mentioned types of problems. As a consequence, we prove the Berenstein–Zelevinsky conjecture [Berenstein A, Zelevinsky A (2005) Adv Math 195:405–455] for the quantized coordinate rings of double Bruhat cells and construct quantum cluster algebra structures on all quantum unipotent groups, extending the theorem of Geiß et al. [Geiß C, et al. (2013) Selecta Math 19:337–397] for the case of symmetric Kac–Moody groups. Moreover, we prove that the upper cluster algebras of Berenstein et al. [Berenstein A, et al. (2005) Duke Math J 126:1–52] associated with double Bruhat cells coincide with the corresponding cluster algebras. PMID:24982197

Degradation of Perfluorinated Ether Lubricants on Pure Aluminum Surfaces: Semiempirical Quantum Chemical Modeling

NASA Technical Reports Server (NTRS)

Slaby, Scott M.; Ewing, David W.; Zehe, Michael J.

1997-01-01

The AM1 semiempirical quantum chemical method was used to model the interaction of perfluoroethers with aluminum surfaces. Perfluorodimethoxymethane and perfluorodimethyl ether were studied interacting with aluminum surfaces, which were modeled by a five-atom cluster and a nine-atom cluster. Interactions were studied for edge (high index) sites and top (low index) sites of the clusters. Both dissociative binding and nondissociative binding were found, with dissociative binding being stronger. The two different ethers bound and dissociated on the clusters in different ways: perfluorodimethoxymethane through its oxygen atoms, but perfluorodimethyl ether through its fluorine atoms. The acetal linkage of perfluorodimeth-oxymethane was the key structural feature of this molecule in its binding and dissociation on the aluminum surface models. The high-index sites of the clusters caused the dissociation of both ethers. These results are consistent with the experimental observation that perfluorinated ethers decompose in contact with sputtered aluminum surfaces.

Collaborative Simulation Grid: Multiscale Quantum-Mechanical/Classical Atomistic Simulations on Distributed PC Clusters in the US and Japan

NASA Technical Reports Server (NTRS)

Kikuchi, Hideaki; Kalia, Rajiv; Nakano, Aiichiro; Vashishta, Priya; Iyetomi, Hiroshi; Ogata, Shuji; Kouno, Takahisa; Shimojo, Fuyuki; Tsuruta, Kanji; Saini, Subhash;

Compensated Crystal Assemblies for Type-II Entangled Photon Generation in Quantum Cluster States

DTIC Science & Technology

2010-03-01

in quantum computational architectures that operate by principles entirely distinct from any based on classical physics. In contrast with other...of the SPDC spectral function, to enable applications in regions that have not been accessible with other methods. Quantum Information and Computation ...Eliminating frequency and space-time correlations in multi-photon states, PRA 64, 063815, 2001 [2]A. Zeilinger et.al. Experimental One-way computing

Why are para-hydrogen clusters superfluid? A quantum theorem of corresponding states study.

PubMed

Sevryuk, Mikhail B; Toennies, J Peter; Ceperley, David M

2010-08-14

The quantum theorem of corresponding states is applied to N=13 and N=26 cold quantum fluid clusters to establish where para-hydrogen clusters lie in relation to more and less quantum delocalized systems. Path integral Monte Carlo calculations of the energies, densities, radial and pair distributions, and superfluid fractions are reported at T=0.5 K for a Lennard-Jones (LJ) (12,6) potential using six different de Boer parameters including the accepted value for hydrogen. The results indicate that the hydrogen clusters are on the borderline to being a nonsuperfluid solid but that the molecules are sufficiently delocalized to be superfluid. A general phase diagram for the total and kinetic energies of LJ (12,6) clusters encompassing all sizes from N=2 to N=infinity and for the entire range of de Boer parameters is presented. Finally the limiting de Boer parameters for quantum delocalization induced unbinding ("quantum unbinding") are estimated and the new results are found to agree with previous calculations for the bulk and smaller clusters.

Anharmonic effects in the quantum cluster equilibrium method

NASA Astrophysics Data System (ADS)

von Domaros, Michael; Perlt, Eva

2017-03-01

The well-established quantum cluster equilibrium (QCE) model provides a statistical thermodynamic framework to apply high-level ab initio calculations of finite cluster structures to macroscopic liquid phases using the partition function. So far, the harmonic approximation has been applied throughout the calculations. In this article, we apply an important correction in the evaluation of the one-particle partition function and account for anharmonicity. Therefore, we implemented an analytical approximation to the Morse partition function and the derivatives of its logarithm with respect to temperature, which are required for the evaluation of thermodynamic quantities. This anharmonic QCE approach has been applied to liquid hydrogen chloride and cluster distributions, and the molar volume, the volumetric thermal expansion coefficient, and the isobaric heat capacity have been calculated. An improved description for all properties is observed if anharmonic effects are considered.

Scalability of a Low-Cost Multi-Teraflop Linux Cluster for High-End Classical Atomistic and Quantum Mechanical Simulations

NASA Technical Reports Server (NTRS)

Kikuchi, Hideaki; Kalia, Rajiv K.; Nakano, Aiichiro; Vashishta, Priya; Shimojo, Fuyuki; Saini, Subhash

2003-01-01

Scalability of a low-cost, Intel Xeon-based, multi-Teraflop Linux cluster is tested for two high-end scientific applications: Classical atomistic simulation based on the molecular dynamics method and quantum mechanical calculation based on the density functional theory. These scalable parallel applications use space-time multiresolution algorithms and feature computational-space decomposition, wavelet-based adaptive load balancing, and spacefilling-curve-based data compression for scalable I/O. Comparative performance tests are performed on a 1,024-processor Linux cluster and a conventional higher-end parallel supercomputer, 1,184-processor IBM SP4. The results show that the performance of the Linux cluster is comparable to that of the SP4. We also study various effects, such as the sharing of memory and L2 cache among processors, on the performance.

Greedy bases in rank 2 quantum cluster algebras

PubMed Central

Lee, Kyungyong; Li, Li; Rupel, Dylan; Zelevinsky, Andrei

2014-01-01

We identify a quantum lift of the greedy basis for rank 2 coefficient-free cluster algebras. Our main result is that our construction does not depend on the choice of initial cluster, that it builds all cluster monomials, and that it produces bar-invariant elements. We also present several conjectures related to this quantum greedy basis and the triangular basis of Berenstein and Zelevinsky. PMID:24982182

Implementation of a quantum random number generator based on the optimal clustering of photocounts

NASA Astrophysics Data System (ADS)

Balygin, K. A.; Zaitsev, V. I.; Klimov, A. N.; Kulik, S. P.; Molotkov, S. N.

2017-10-01

To implement quantum random number generators, it is fundamentally important to have a mathematically provable and experimentally testable process of measurements of a system from which an initial random sequence is generated. This makes sure that randomness indeed has a quantum nature. A quantum random number generator has been implemented with the use of the detection of quasi-single-photon radiation by a silicon photomultiplier (SiPM) matrix, which makes it possible to reliably reach the Poisson statistics of photocounts. The choice and use of the optimal clustering of photocounts for the initial sequence of photodetection events and a method of extraction of a random sequence of 0's and 1's, which is polynomial in the length of the sequence, have made it possible to reach a yield rate of 64 Mbit/s of the output certainly random sequence.

Relaxation channels of multi-photon excited xenon clusters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Serdobintsev, P. Yu.; Melnikov, A. S.; Department of Physics, St. Petersburg State University, Saint Petersburg 198904

2015-09-21

The relaxation processes of the xenon clusters subjected to multi-photon excitation by laser radiation with quantum energies significantly lower than the thresholds of excitation of atoms and ionization of clusters were studied. Results obtained by means of the photoelectron spectroscopy method showed that desorption processes of excited atoms play a significant role in the decay of two-photon excited xenon clusters. A number of excited states of xenon atoms formed during this process were discovered and identified.

Multifrequency multi-qubit entanglement based on plasmonic hot spots

PubMed Central

Ren, Jun; Wu, Tong; Zhang, Xiangdong

2015-01-01

The theoretical method to study strong coupling between an ensemble of quantum emitters (QEs) and surface plasmons excited by the nanoparticle cluster has been presented by using a rigorous first-principles electromagnetic Green’s tensor technique. We have demonstrated that multi-qubit entanglements for two-level QEs can be produced at different coupling resonance frequencies, when they locate in the hot spots of the metallic nanoparticle cluster. The duration of quantum beats for such an entanglement can reach two orders longer than that for the entanglement in a photonic cavity. The phenomenon originates from collective coupling resonance excitation of the cluster. At the frequency of single scattering resonance, the entanglement cannot be produced although the single QE spontaneous decay rate is very big. PMID:26350051

Quantifying Complexity in Quantum Phase Transitions via Mutual Information Complex Networks

NASA Astrophysics Data System (ADS)

Valdez, Marc Andrew; Jaschke, Daniel; Vargas, David L.; Carr, Lincoln D.

2017-12-01

We quantify the emergent complexity of quantum states near quantum critical points on regular 1D lattices, via complex network measures based on quantum mutual information as the adjacency matrix, in direct analogy to quantifying the complexity of electroencephalogram or functional magnetic resonance imaging measurements of the brain. Using matrix product state methods, we show that network density, clustering, disparity, and Pearson's correlation obtain the critical point for both quantum Ising and Bose-Hubbard models to a high degree of accuracy in finite-size scaling for three classes of quantum phase transitions, Z2, mean field superfluid to Mott insulator, and a Berzinskii-Kosterlitz-Thouless crossover.

First principles study of edge carboxylated graphene quantum dots

NASA Astrophysics Data System (ADS)

Abdelsalam, Hazem; Elhaes, Hanan; Ibrahim, Medhat A.

2018-05-01

The structure stability and electronic properties of edge carboxylated hexagonal and triangular graphene quantum dots are investigated using density functional theory. The calculated binding energies show that the hexagonal clusters with armchair edges have the highest stability among all the quantum dots. The binding energy of carboxylated graphene quantum dots increases by increasing the number of carboxyl groups. Our study shows that the total dipole moment significantly increases by adding COOH with the highest value observed in triangular clusters. The edge states in triangular graphene quantum dots with zigzag edges produce completely different energy spectrum from other dots: (a) the energy gap in triangular zigzag is very small as compared to other clusters and (b) the highest occupied molecular orbital is localized at the edges which is in contrast to other clusters where it is distributed over the cluster surface. The enhanced reactivity and the controllable energy gap by shape and edge termination make graphene quantum dots ideal for various nanodevice applications such as sensors. The infrared spectra are presented to confirm the stability of the quantum dots.

Fast reconstruction of high-qubit-number quantum states via low-rate measurements

NASA Astrophysics Data System (ADS)

Li, K.; Zhang, J.; Cong, S.

2017-07-01

Due to the exponential complexity of the resources required by quantum state tomography (QST), people are interested in approaches towards identifying quantum states which require less effort and time. In this paper, we provide a tailored and efficient method for reconstructing mixed quantum states up to 12 (or even more) qubits from an incomplete set of observables subject to noises. Our method is applicable to any pure or nearly pure state ρ and can be extended to many states of interest in quantum information processing, such as a multiparticle entangled W state, Greenberger-Horne-Zeilinger states, and cluster states that are matrix product operators of low dimensions. The method applies the quantum density matrix constraints to a quantum compressive sensing optimization problem and exploits a modified quantum alternating direction multiplier method (quantum-ADMM) to accelerate the convergence. Our algorithm takes 8 ,35 , and 226 seconds, respectively, to reconstruct superposition state density matrices of 10 ,11 ,and12 qubits with acceptable fidelity using less than 1 % of measurements of expectation. To our knowledge it is the fastest realization that people can achieve using a normal desktop. We further discuss applications of this method using experimental data of mixed states obtained in an ion trap experiment of up to 8 qubits.

Blind Quantum Signature with Controlled Four-Particle Cluster States

NASA Astrophysics Data System (ADS)

Li, Wei; Shi, Jinjing; Shi, Ronghua; Guo, Ying

2017-08-01

A novel blind quantum signature scheme based on cluster states is introduced. Cluster states are a type of multi-qubit entangled states and it is more immune to decoherence than other entangled states. The controlled four-particle cluster states are created by acting controlled-Z gate on particles of four-particle cluster states. The presented scheme utilizes the above entangled states and simplifies the measurement basis to generate and verify the signature. Security analysis demonstrates that the scheme is unconditional secure. It can be employed to E-commerce systems in quantum scenario.

Minimal Model of Quantum Kinetic Clusters for the Energy-Transfer Network of a Light-Harvesting Protein Complex.

PubMed

Wu, Jianlan; Tang, Zhoufei; Gong, Zhihao; Cao, Jianshu; Mukamel, Shaul

2015-04-02

The energy absorbed in a light-harvesting protein complex is often transferred collectively through aggregated chromophore clusters. For population evolution of chromophores, the time-integrated effective rate matrix allows us to construct quantum kinetic clusters quantitatively and determine the reduced cluster-cluster transfer rates systematically, thus defining a minimal model of energy-transfer kinetics. For Fenna-Matthews-Olson (FMO) and light-havrvesting complex II (LCHII) monomers, quantum Markovian kinetics of clusters can accurately reproduce the overall energy-transfer process in the long-time scale. The dominant energy-transfer pathways are identified in the picture of aggregated clusters. The chromophores distributed extensively in various clusters can assist a fast and long-range energy transfer.

A Novel Quantum Blind Signature Scheme with Four-Particle Cluster States

NASA Astrophysics Data System (ADS)

Fan, Ling

2016-03-01

In an arbitrated quantum signature scheme, the signer signs the message and the receiver verifies the signature's validity with the assistance of the arbitrator. We present an arbitrated quantum blind signature scheme by measuring four-particle cluster states and coding. By using the special relationship of four-particle cluster states, we cannot only support the security of quantum signature, but also guarantee the anonymity of the message owner. It has a wide application to E-payment system, E-government, E-business, and etc.

Phase space theory of evaporation in neon clusters: the role of quantum effects.

PubMed

Calvo, F; Parneix, P

2009-12-31

Unimolecular evaporation of neon clusters containing between 14 and 148 atoms is theoretically investigated in the framework of phase space theory. Quantum effects are incorporated in the vibrational densities of states, which include both zero-point and anharmonic contributions, and in the possible tunneling through the centrifugal barrier. The evaporation rates, kinetic energy released, and product angular momentum are calculated as a function of excess energy or temperature in the parent cluster and compared to the classical results. Quantum fluctuations are found to generally increase both the kinetic energy released and the angular momentum of the product, but the effects on the rate constants depend nontrivially on the excess energy. These results are interpreted as due to the very few vibrational states available in the product cluster when described quantum mechanically. Because delocalization also leads to much narrower thermal energy distributions, the variations of evaporation observables as a function of canonical temperature appear much less marked than in the microcanonical ensemble. While quantum effects tend to smooth the caloric curve in the product cluster, the melting phase change clearly keeps a signature on these observables. The microcanonical temperature extracted from fitting the kinetic energy released distribution using an improved Arrhenius form further suggests a backbending in the quantum Ne(13) cluster that is absent in the classical system. Finally, in contrast to delocalization effects, quantum tunneling through the centrifugal barrier does not play any appreciable role on the evaporation kinetics of these rather heavy clusters.

Quantum soldering of individual quantum dots.

PubMed

Roy, Xavier; Schenck, Christine L; Ahn, Seokhoon; Lalancette, Roger A; Venkataraman, Latha; Nuckolls, Colin; Steigerwald, Michael L

2012-12-07

Making contact to a quantum dot: Single quantum-dot electronic circuits are fabricated by wiring atomically precise metal chalcogenide clusters with conjugated molecular connectors. These wired clusters can couple electronically to nanoscale electrodes and be tuned to control the charge-transfer characteristics (see picture). Copyright © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Cluster-state quantum computing enhanced by high-fidelity generalized measurements.

PubMed

Biggerstaff, D N; Kaltenbaek, R; Hamel, D R; Weihs, G; Rudolph, T; Resch, K J

2009-12-11

We introduce and implement a technique to extend the quantum computational power of cluster states by replacing some projective measurements with generalized quantum measurements (POVMs). As an experimental demonstration we fully realize an arbitrary three-qubit cluster computation by implementing a tunable linear-optical POVM, as well as fast active feedforward, on a two-qubit photonic cluster state. Over 206 different computations, the average output fidelity is 0.9832+/-0.0002; furthermore the error contribution from our POVM device and feedforward is only of O(10(-3)), less than some recent thresholds for fault-tolerant cluster computing.

Magnetic Properties of Strongly Correlated Hubbard Model and Quantum Spin-One Ferromagnets with Arbitrary Crystal-Field Potential: Linked Cluster Series Expansion Approach

NASA Astrophysics Data System (ADS)

Pan, Kok-Kwei

We have generalized the linked cluster expansion method to solve more many-body quantum systems, such as quantum spin systems with crystal-field potentials and the Hubbard model. The technique sums up all connected diagrams to a certain order of the perturbative Hamiltonian. The modified multiple-site Wick reduction theorem and the simple tau dependence of the standard basis operators have been used to facilitate the evaluation of the integration procedures in the perturbation expansion. Computational methods are developed to calculate all terms in the series expansion. As a first example, the perturbation series expansion of thermodynamic quantities of the single-band Hubbard model has been obtained using a linked cluster series expansion technique. We have made corrections to all previous results of several papers (up to fourth order). The behaviors of the three dimensional simple cubic and body-centered cubic systems have been discussed from the qualitative analysis of the perturbation series up to fourth order. We have also calculated the sixth-order perturbation series of this model. As a second example, we present the magnetic properties of spin-one Heisenberg model with arbitrary crystal-field potential using a linked cluster series expansion. The calculation of the thermodynamic properties using this method covers the whole range of temperature, in both magnetically ordered and disordered phases. The series for the susceptibility and magnetization have been obtained up to fourth order for this model. The method sums up all perturbation terms to certain order and estimates the result using a well -developed and highly successful extrapolation method (the standard ratio method). The dependence of critical temperature on the crystal-field potential and the magnetization as a function of temperature and crystal-field potential are shown. The critical behaviors at zero temperature are also shown. The range of the crystal-field potential for Ni(2+) compounds is roughly estimated based on this model using known experimental results.

Flexible resources for quantum metrology

NASA Astrophysics Data System (ADS)

Friis, Nicolai; Orsucci, Davide; Skotiniotis, Michalis; Sekatski, Pavel; Dunjko, Vedran; Briegel, Hans J.; Dür, Wolfgang

2017-06-01

Quantum metrology offers a quadratic advantage over classical approaches to parameter estimation problems by utilising entanglement and nonclassicality. However, the hurdle of actually implementing the necessary quantum probe states and measurements, which vary drastically for different metrological scenarios, is usually not taken into account. We show that for a wide range of tasks in metrology, 2D cluster states (a particular family of states useful for measurement-based quantum computation) can serve as flexible resources that allow one to efficiently prepare any required state for sensing, and perform appropriate (entangled) measurements using only single qubit operations. Crucially, the overhead in the number of qubits is less than quadratic, thus preserving the quantum scaling advantage. This is ensured by using a compression to a logarithmically sized space that contains all relevant information for sensing. We specifically demonstrate how our method can be used to obtain optimal scaling for phase and frequency estimation in local estimation problems, as well as for the Bayesian equivalents with Gaussian priors of varying widths. Furthermore, we show that in the paradigmatic case of local phase estimation 1D cluster states are sufficient for optimal state preparation and measurement.

Photoabsorption spectra of small HeN+ clusters (N = 3, 4, 10). A quantum Monte Carlo modeling

NASA Astrophysics Data System (ADS)

Ćosić, Rajko; Karlický, František; Kalus, René

2018-05-01

Photoabsorption cross-sections have been calculated for HeN+ clusters of selected sizes (N = 3, 4, 10) over a broad range of photon energies (Ephot = 2 - 14 eV) and compared with available experimental data. Semiempirical electronic Hamiltonians derived from the diatomics-in-molecules approach have been used for electronic structure calculations and a quantum, path-integral Monte Carlo method has been employed to model the delocalization of helium nuclei. While a quantitative agreement has been achieved between the theory and experiment for He3+ and He4+, only qualitative correspondence is seen for He10+ .

Quantum mean-field approximation for lattice quantum models: Truncating quantum correlations and retaining classical ones

NASA Astrophysics Data System (ADS)

Malpetti, Daniele; Roscilde, Tommaso

2017-02-01

The mean-field approximation is at the heart of our understanding of complex systems, despite its fundamental limitation of completely neglecting correlations between the elementary constituents. In a recent work [Phys. Rev. Lett. 117, 130401 (2016), 10.1103/PhysRevLett.117.130401], we have shown that in quantum many-body systems at finite temperature, two-point correlations can be formally separated into a thermal part and a quantum part and that quantum correlations are generically found to decay exponentially at finite temperature, with a characteristic, temperature-dependent quantum coherence length. The existence of these two different forms of correlation in quantum many-body systems suggests the possibility of formulating an approximation, which affects quantum correlations only, without preventing the correct description of classical fluctuations at all length scales. Focusing on lattice boson and quantum Ising models, we make use of the path-integral formulation of quantum statistical mechanics to introduce such an approximation, which we dub quantum mean-field (QMF) approach, and which can be readily generalized to a cluster form (cluster QMF or cQMF). The cQMF approximation reduces to cluster mean-field theory at T =0 , while at any finite temperature it produces a family of systematically improved, semi-classical approximations to the quantum statistical mechanics of the lattice theory at hand. Contrary to standard MF approximations, the correct nature of thermal critical phenomena is captured by any cluster size. In the two exemplary cases of the two-dimensional quantum Ising model and of two-dimensional quantum rotors, we study systematically the convergence of the cQMF approximation towards the exact result, and show that the convergence is typically linear or sublinear in the boundary-to-bulk ratio of the clusters as T →0 , while it becomes faster than linear as T grows. These results pave the way towards the development of semiclassical numerical approaches based on an approximate, yet systematically improved account of quantum correlations.

A Hardware-Accelerated Quantum Monte Carlo framework (HAQMC) for N-body systems

NASA Astrophysics Data System (ADS)

Gothandaraman, Akila; Peterson, Gregory D.; Warren, G. Lee; Hinde, Robert J.; Harrison, Robert J.

2009-12-01

Interest in the study of structural and energetic properties of highly quantum clusters, such as inert gas clusters has motivated the development of a hardware-accelerated framework for Quantum Monte Carlo simulations. In the Quantum Monte Carlo method, the properties of a system of atoms, such as the ground-state energies, are averaged over a number of iterations. Our framework is aimed at accelerating the computations in each iteration of the QMC application by offloading the calculation of properties, namely energy and trial wave function, onto reconfigurable hardware. This gives a user the capability to run simulations for a large number of iterations, thereby reducing the statistical uncertainty in the properties, and for larger clusters. This framework is designed to run on the Cray XD1 high performance reconfigurable computing platform, which exploits the coarse-grained parallelism of the processor along with the fine-grained parallelism of the reconfigurable computing devices available in the form of field-programmable gate arrays. In this paper, we illustrate the functioning of the framework, which can be used to calculate the energies for a model cluster of helium atoms. In addition, we present the capabilities of the framework that allow the user to vary the chemical identities of the simulated atoms. Program summaryProgram title: Hardware Accelerated Quantum Monte Carlo (HAQMC) Catalogue identifier: AEEP_v1_0 Program summary URL:http://cpc.cs.qub.ac.uk/summaries/AEEP_v1_0.html Program obtainable from: CPC Program Library, Queen's University, Belfast, N. Ireland Licensing provisions: Standard CPC licence, http://cpc.cs.qub.ac.uk/licence/licence.html No. of lines in distributed program, including test data, etc.: 691 537 No. of bytes in distributed program, including test data, etc.: 5 031 226 Distribution format: tar.gz Programming language: C/C++ for the QMC application, VHDL and Xilinx 8.1 ISE/EDK tools for FPGA design and development Computer: Cray XD1 consisting of a dual-core, dualprocessor AMD Opteron 2.2 GHz with a Xilinx Virtex-4 (V4LX160) or Xilinx Virtex-II Pro (XC2VP50) FPGA per node. We use the compute node with the Xilinx Virtex-4 FPGA Operating system: Red Hat Enterprise Linux OS Has the code been vectorised or parallelized?: Yes Classification: 6.1 Nature of problem: Quantum Monte Carlo is a practical method to solve the Schrödinger equation for large many-body systems and obtain the ground-state properties of such systems. This method involves the sampling of a number of configurations of atoms and averaging the properties of the configurations over a number of iterations. We are interested in applying the QMC method to obtain the energy and other properties of highly quantum clusters, such as inert gas clusters. Solution method: The proposed framework provides a combined hardware-software approach, in which the QMC simulation is performed on the host processor, with the computationally intensive functions such as energy and trial wave function computations mapped onto the field-programmable gate array (FPGA) logic device attached as a co-processor to the host processor. We perform the QMC simulation for a number of iterations as in the case of our original software QMC approach, to reduce the statistical uncertainty of the results. However, our proposed HAQMC framework accelerates each iteration of the simulation, by significantly reducing the time taken to calculate the ground-state properties of the configurations of atoms, thereby accelerating the overall QMC simulation. We provide a generic interpolation framework that can be extended to study a variety of pure and doped atomic clusters, irrespective of the chemical identities of the atoms. For the FPGA implementation of the properties, we use a two-region approach for accurately computing the properties over the entire domain, employ deep pipelines and fixed-point for all our calculations guaranteeing the accuracy required for our simulation.

Gate sequence for continuous variable one-way quantum computation

PubMed Central

Su, Xiaolong; Hao, Shuhong; Deng, Xiaowei; Ma, Lingyu; Wang, Meihong; Jia, Xiaojun; Xie, Changde; Peng, Kunchi

2013-01-01

Measurement-based one-way quantum computation using cluster states as resources provides an efficient model to perform computation and information processing of quantum codes. Arbitrary Gaussian quantum computation can be implemented sufficiently by long single-mode and two-mode gate sequences. However, continuous variable gate sequences have not been realized so far due to an absence of cluster states larger than four submodes. Here we present the first continuous variable gate sequence consisting of a single-mode squeezing gate and a two-mode controlled-phase gate based on a six-mode cluster state. The quantum property of this gate sequence is confirmed by the fidelities and the quantum entanglement of two output modes, which depend on both the squeezing and controlled-phase gates. The experiment demonstrates the feasibility of implementing Gaussian quantum computation by means of accessible gate sequences.

Nonperturbative light-front Hamiltonian methods

NASA Astrophysics Data System (ADS)

Hiller, J. R.

2016-09-01

We examine the current state-of-the-art in nonperturbative calculations done with Hamiltonians constructed in light-front quantization of various field theories. The language of light-front quantization is introduced, and important (numerical) techniques, such as Pauli-Villars regularization, discrete light-cone quantization, basis light-front quantization, the light-front coupled-cluster method, the renormalization group procedure for effective particles, sector-dependent renormalization, and the Lanczos diagonalization method, are surveyed. Specific applications are discussed for quenched scalar Yukawa theory, ϕ4 theory, ordinary Yukawa theory, supersymmetric Yang-Mills theory, quantum electrodynamics, and quantum chromodynamics. The content should serve as an introduction to these methods for anyone interested in doing such calculations and as a rallying point for those who wish to solve quantum chromodynamics in terms of wave functions rather than random samplings of Euclidean field configurations.

Efficient red luminescence from organic-soluble Au25 clusters by ligand structure modification

NASA Astrophysics Data System (ADS)

Mathew, Ammu; Varghese, Elizabeth; Choudhury, Susobhan; Pal, Samir Kumar; Pradeep, T.

2015-08-01

An efficient method to enhance visible luminescence in a visibly non-luminescent organic-soluble 4-(tert butyl)benzyl mercaptan (SBB)-stabilized Au25 cluster has been developed. This method relies mainly on enhancing the surface charge density on the cluster by creating an additional shell of thiolate on the cluster surface, which enhances visible luminescence. The viability of this method has been demonstrated by imparting red luminescence to various ligand-protected quantum clusters (QCs), observable to the naked eye. The bright red luminescent material derived from Au25SBB18 clusters was characterized using UV-vis and luminescence spectroscopy, TEM, SEM/EDS, XPS, TG, ESI and MALDI mass spectrometry, which collectively proposed an uncommon molecular formula of Au29SBB24S, suggested to be due to different stapler motifs protecting the Au25 core. The critical role of temperature on the emergence of luminescence in QCs has been studied. The restoration of the surface ligand shell on the Au25 cluster and subsequent physicochemical modification to the cluster were probed by various mass spectral and spectroscopic techniques. Our results provide fundamental insights into the ligand characteristics determining luminescence in QCs.An efficient method to enhance visible luminescence in a visibly non-luminescent organic-soluble 4-(tert butyl)benzyl mercaptan (SBB)-stabilized Au25 cluster has been developed. This method relies mainly on enhancing the surface charge density on the cluster by creating an additional shell of thiolate on the cluster surface, which enhances visible luminescence. The viability of this method has been demonstrated by imparting red luminescence to various ligand-protected quantum clusters (QCs), observable to the naked eye. The bright red luminescent material derived from Au25SBB18 clusters was characterized using UV-vis and luminescence spectroscopy, TEM, SEM/EDS, XPS, TG, ESI and MALDI mass spectrometry, which collectively proposed an uncommon molecular formula of Au29SBB24S, suggested to be due to different stapler motifs protecting the Au25 core. The critical role of temperature on the emergence of luminescence in QCs has been studied. The restoration of the surface ligand shell on the Au25 cluster and subsequent physicochemical modification to the cluster were probed by various mass spectral and spectroscopic techniques. Our results provide fundamental insights into the ligand characteristics determining luminescence in QCs. Electronic supplementary information (ESI) available: Additional data on characterization of red luminescent Au29 QC and comparison with parent Au25SBB18 are given. See DOI: 10.1039/c5nr03457d

Experimental demonstration of a measurement-based realisation of a quantum channel

NASA Astrophysics Data System (ADS)

McCutcheon, W.; McMillan, A.; Rarity, J. G.; Tame, M. S.

2018-03-01

We introduce and experimentally demonstrate a method for realising a quantum channel using the measurement-based model. Using a photonic setup and modifying the basis of single-qubit measurements on a four-qubit entangled cluster state, representative channels are realised for the case of a single qubit in the form of amplitude and phase damping channels. The experimental results match the theoretical model well, demonstrating the successful performance of the channels. We also show how other types of quantum channels can be realised using our approach. This work highlights the potential of the measurement-based model for realising quantum channels which may serve as building blocks for simulations of realistic open quantum systems.

Quantum structural fluctuation in para-hydrogen clusters revealed by the variational path integral method

NASA Astrophysics Data System (ADS)

Miura, Shinichi

2018-03-01

In this paper, the ground state of para-hydrogen clusters for size regime N ≤ 40 has been studied by our variational path integral molecular dynamics method. Long molecular dynamics calculations have been performed to accurately evaluate ground state properties. The chemical potential of the hydrogen molecule is found to have a zigzag size dependence, indicating the magic number stability for the clusters of the size N = 13, 26, 29, 34, and 39. One-body density of the hydrogen molecule is demonstrated to have a structured profile, not a melted one. The observed magic number stability is examined using the inherent structure analysis. We also have developed a novel method combining our variational path integral hybrid Monte Carlo method with the replica exchange technique. We introduce replicas of the original system bridging from the structured to the melted cluster, which is realized by scaling the potential energy of the system. Using the enhanced sampling method, the clusters are demonstrated to have the structured density profile in the ground state.

Quantum structural fluctuation in para-hydrogen clusters revealed by the variational path integral method.

PubMed

Miura, Shinichi

2018-03-14

In this paper, the ground state of para-hydrogen clusters for size regime N ≤ 40 has been studied by our variational path integral molecular dynamics method. Long molecular dynamics calculations have been performed to accurately evaluate ground state properties. The chemical potential of the hydrogen molecule is found to have a zigzag size dependence, indicating the magic number stability for the clusters of the size N = 13, 26, 29, 34, and 39. One-body density of the hydrogen molecule is demonstrated to have a structured profile, not a melted one. The observed magic number stability is examined using the inherent structure analysis. We also have developed a novel method combining our variational path integral hybrid Monte Carlo method with the replica exchange technique. We introduce replicas of the original system bridging from the structured to the melted cluster, which is realized by scaling the potential energy of the system. Using the enhanced sampling method, the clusters are demonstrated to have the structured density profile in the ground state.

Fast Implementation of Quantum Phase Gates and Creation of Cluster States via Transitionless Quantum Driving

NASA Astrophysics Data System (ADS)

Zhang, Chun-Ling; Liu, Wen-Wu

2018-05-01

In this paper, combining transitionless quantum driving and quantum Zeno dynamics, we propose an efficient scheme to fast implement a two-qubit quantum phase gate which can be used to generate cluster state of atoms trapped in distant cavities. The influence of various of various error sources including spontaneous emission and photon loss on the fidelity is analyzed via numerical simulation. The results show that this scheme not only takes less time than adiabatic scheme but also is not sensitive to both error sources. Additionally, a creation of N-atom cluster states is put forward as a typical example of the applications of the phase gates.

Demonstration of Monogamy Relations for Einstein-Podolsky-Rosen Steering in Gaussian Cluster States.

PubMed

Deng, Xiaowei; Xiang, Yu; Tian, Caixing; Adesso, Gerardo; He, Qiongyi; Gong, Qihuang; Su, Xiaolong; Xie, Changde; Peng, Kunchi

2017-06-09

Understanding how quantum resources can be quantified and distributed over many parties has profound applications in quantum communication. As one of the most intriguing features of quantum mechanics, Einstein-Podolsky-Rosen (EPR) steering is a useful resource for secure quantum networks. By reconstructing the covariance matrix of a continuous variable four-mode square Gaussian cluster state subject to asymmetric loss, we quantify the amount of bipartite steering with a variable number of modes per party, and verify recently introduced monogamy relations for Gaussian steerability, which establish quantitative constraints on the security of information shared among different parties. We observe a very rich structure for the steering distribution, and demonstrate one-way EPR steering of the cluster state under Gaussian measurements, as well as one-to-multimode steering. Our experiment paves the way for exploiting EPR steering in Gaussian cluster states as a valuable resource for multiparty quantum information tasks.

Demonstration of Monogamy Relations for Einstein-Podolsky-Rosen Steering in Gaussian Cluster States

NASA Astrophysics Data System (ADS)

Deng, Xiaowei; Xiang, Yu; Tian, Caixing; Adesso, Gerardo; He, Qiongyi; Gong, Qihuang; Su, Xiaolong; Xie, Changde; Peng, Kunchi

2017-06-01

Understanding how quantum resources can be quantified and distributed over many parties has profound applications in quantum communication. As one of the most intriguing features of quantum mechanics, Einstein-Podolsky-Rosen (EPR) steering is a useful resource for secure quantum networks. By reconstructing the covariance matrix of a continuous variable four-mode square Gaussian cluster state subject to asymmetric loss, we quantify the amount of bipartite steering with a variable number of modes per party, and verify recently introduced monogamy relations for Gaussian steerability, which establish quantitative constraints on the security of information shared among different parties. We observe a very rich structure for the steering distribution, and demonstrate one-way EPR steering of the cluster state under Gaussian measurements, as well as one-to-multimode steering. Our experiment paves the way for exploiting EPR steering in Gaussian cluster states as a valuable resource for multiparty quantum information tasks.

Creating fractional quantum Hall states with atomic clusters using light-assisted insertion of angular momentum

NASA Astrophysics Data System (ADS)

Zhang, Junyi; Beugnon, Jerome; Nascimbene, Sylvain

We describe a protocol to prepare clusters of ultracold bosonic atoms in strongly interacting states reminiscent of fractional quantum Hall states. Our scheme consists in injecting a controlled amount of angular momentum to an atomic gas using Raman transitions carrying orbital angular momentum. By injecting one unit of angular momentum per atom, one realizes a single-vortex state, which is well described by mean-field theory for large enough particle numbers. We also present schemes to realize fractional quantum Hall states, namely, the bosonic Laughlin and Moore-Read states. We investigate the requirements for adiabatic nucleation of such topological states, in particular comparing linear Landau-Zener ramps and arbitrary ramps obtained from optimized control methods. We also show that this protocol requires excellent control over the isotropic character of the trapping potential. ERC-Synergy Grant UQUAM, ANR-10-IDEX-0001-02, DIM NanoK Atocirc project.

First-principles calculations of Ti and O NMR chemical shift tensors in ferroelectric perovskites

NASA Astrophysics Data System (ADS)

Pechkis, Daniel; Walter, Eric; Krakauer, Henry

2011-03-01

Complementary chemical shift calculations were carried out with embedded clusters, using quantum chemistry methods, and with periodic boundary conditions, using the GIPAW approach within the Quantum Espresso package. Compared to oxygen chemical shifts, δ̂ (O), cluster calculations for δ̂ (Ti) were found to be more sensitive to size effects, termination, and choice of gaussian-type atomic basis set, while GIPAW results were found to be more sensitive to the pseudopotential construction. The two approaches complemented each other in optimizing these factors. We show that the two approaches yield comparable chemical shifts for suitably converged simulations, and results are compared with available experimental measurements. Supported by ONR.

Fault-tolerant measurement-based quantum computing with continuous-variable cluster states.

PubMed

Menicucci, Nicolas C

2014-03-28

A long-standing open question about Gaussian continuous-variable cluster states is whether they enable fault-tolerant measurement-based quantum computation. The answer is yes. Initial squeezing in the cluster above a threshold value of 20.5 dB ensures that errors from finite squeezing acting on encoded qubits are below the fault-tolerance threshold of known qubit-based error-correcting codes. By concatenating with one of these codes and using ancilla-based error correction, fault-tolerant measurement-based quantum computation of theoretically indefinite length is possible with finitely squeezed cluster states.

Controller-Independent Bidirectional Direct Communication with Four-Qubit Cluster States

NASA Astrophysics Data System (ADS)

Cao, Yong; Zha, Xin-Wei; Wang, Shu-Kai

2018-03-01

We propose a feasible scheme for implementing bidirectional quantum direct communication protocol using four-qubit cluster states. In this scheme, the quantum channel between the sender Alice and the receiver Bob consists of an ordered sequence of cluster states which are prepared by Alice. After ensuring the security of quantum channel, according to the secret messages, the sender will perform the unitary operation and the receiver can obtain different secret messages in a deterministic way.

Communication: Finite size correction in periodic coupled cluster theory calculations of solids.

PubMed

Liao, Ke; Grüneis, Andreas

2016-10-14

We present a method to correct for finite size errors in coupled cluster theory calculations of solids. The outlined technique shares similarities with electronic structure factor interpolation methods used in quantum Monte Carlo calculations. However, our approach does not require the calculation of density matrices. Furthermore we show that the proposed finite size corrections achieve chemical accuracy in the convergence of second-order Møller-Plesset perturbation and coupled cluster singles and doubles correlation energies per atom for insulating solids with two atomic unit cells using 2 × 2 × 2 and 3 × 3 × 3 k-point meshes only.

A nonperturbative light-front coupled-cluster method

NASA Astrophysics Data System (ADS)

Hiller, J. R.

2012-10-01

The nonperturbative Hamiltonian eigenvalue problem for bound states of a quantum field theory is formulated in terms of Dirac's light-front coordinates and then approximated by the exponential-operator technique of the many-body coupled-cluster method. This approximation eliminates any need for the usual approximation of Fock-space truncation. Instead, the exponentiated operator is truncated, and the terms retained are determined by a set of nonlinear integral equations. These equations are solved simultaneously with an effective eigenvalue problem in the valence sector, where the number of constituents is small. Matrix elements can be calculated, with extensions of techniques from standard coupled-cluster theory, to obtain form factors and other observables.

Canonical partition functions: ideal quantum gases, interacting classical gases, and interacting quantum gases

NASA Astrophysics Data System (ADS)

Zhou, Chi-Chun; Dai, Wu-Sheng

2018-02-01

In statistical mechanics, for a system with a fixed number of particles, e.g. a finite-size system, strictly speaking, the thermodynamic quantity needs to be calculated in the canonical ensemble. Nevertheless, the calculation of the canonical partition function is difficult. In this paper, based on the mathematical theory of the symmetric function, we suggest a method for the calculation of the canonical partition function of ideal quantum gases, including ideal Bose, Fermi, and Gentile gases. Moreover, we express the canonical partition functions of interacting classical and quantum gases given by the classical and quantum cluster expansion methods in terms of the Bell polynomial in mathematics. The virial coefficients of ideal Bose, Fermi, and Gentile gases are calculated from the exact canonical partition function. The virial coefficients of interacting classical and quantum gases are calculated from the canonical partition function by using the expansion of the Bell polynomial, rather than calculated from the grand canonical potential.

Atomically manufactured nickel-silicon quantum dots displaying robust resonant tunneling and negative differential resistance

NASA Astrophysics Data System (ADS)

Cheng, Jian-Yih; Fisher, Brandon L.; Guisinger, Nathan P.; Lilley, Carmen M.

2017-12-01

Providing a spin-free host material in the development of quantum information technology has made silicon a very interesting and desirable material for qubit design. Much of the work and experimental progress has focused on isolated phosphorous atoms. In this article, we report on the exploration of Ni-Si clusters that are atomically manufactured via self-assembly from the bottom-up and behave as isolated quantum dots. These small quantum dot structures are probed at the atomic-scale with scanning tunneling microscopy and spectroscopy, revealing robust resonance through discrete quantized energy levels within the Ni-Si clusters. The resonance energy is reproducible and the peak spacing of the quantum dot structures increases as the number of atoms in the cluster decrease. Probing these quantum dot structures on degenerately doped silicon results in the observation of negative differential resistance in both I-V and dI/dV spectra. At higher surface coverage of nickel, a well-known √19 surface modification is observed and is essentially a tightly packed array of the clusters. Spatial conductance maps reveal variations in the local density of states that suggest the clusters are influencing the electronic properties of their neighbors. All of these results are extremely encouraging towards the utilization of metal modified silicon surfaces to advance or complement existing quantum information technology.

Atomically manufactured nickel–silicon quantum dots displaying robust resonant tunneling and negative differential resistance

DOE PAGES

Cheng, Jian -Yih; Fisher, Brandon L.; Guisinger, Nathan P.; ...

2017-05-22

Providing a spin-free host material in the development of quantum information technology has made silicon a very interesting and desirable material for qubit design. Much of the work and experimental progress has focused on isolated phosphorous atoms. In this article, we report on the exploration of Ni–Si clusters that are atomically manufactured via self-assembly from the bottom-up and behave as isolated quantum dots. These small quantum dot structures are probed at the atomic-scale with scanning tunneling microscopy and spectroscopy, revealing robust resonance through discrete quantized energy levels within the Ni–Si clusters. The resonance energy is reproducible and the peak spacingmore » of the quantum dot structures increases as the number of atoms in the cluster decrease. Probing these quantum dot structures on degenerately doped silicon results in the observation of negative differential resistance in both I–V and dI/dV spectra. At higher surface coverage of nickel, a well-known √19 surface modification is observed and is essentially a tightly packed array of the clusters. Spatial conductance maps reveal variations in the local density of states that suggest the clusters are influencing the electronic properties of their neighbors. Furthermore, all of these results are extremely encouraging towards the utilization of metal modified silicon surfaces to advance or complement existing quantum information technology.« less

Atomically manufactured nickel–silicon quantum dots displaying robust resonant tunneling and negative differential resistance

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cheng, Jian -Yih; Fisher, Brandon L.; Guisinger, Nathan P.

Providing a spin-free host material in the development of quantum information technology has made silicon a very interesting and desirable material for qubit design. Much of the work and experimental progress has focused on isolated phosphorous atoms. In this article, we report on the exploration of Ni–Si clusters that are atomically manufactured via self-assembly from the bottom-up and behave as isolated quantum dots. These small quantum dot structures are probed at the atomic-scale with scanning tunneling microscopy and spectroscopy, revealing robust resonance through discrete quantized energy levels within the Ni–Si clusters. The resonance energy is reproducible and the peak spacingmore » of the quantum dot structures increases as the number of atoms in the cluster decrease. Probing these quantum dot structures on degenerately doped silicon results in the observation of negative differential resistance in both I–V and dI/dV spectra. At higher surface coverage of nickel, a well-known √19 surface modification is observed and is essentially a tightly packed array of the clusters. Spatial conductance maps reveal variations in the local density of states that suggest the clusters are influencing the electronic properties of their neighbors. Furthermore, all of these results are extremely encouraging towards the utilization of metal modified silicon surfaces to advance or complement existing quantum information technology.« less

HF in clusters of molecular hydrogen. I. Size evolution of quantum solvation by parahydrogen molecules.

PubMed

Jiang, Hao; Bacić, Zlatko

2005-06-22

We present a theoretical study of the quantum solvation of the HF molecule by a small number of parahydrogen molecules, having n = 1-13 solvent particles. The minimum-energy cluster structures determined for n = 1-12 have all of the H(2) molecules in the first solvent shell. The first solvent shell closes at n = 12 and its geometry is icosahedral, with the HF molecule at the center. The quantum-mechanical ground-state properties of the clusters are calculated exactly using the diffusion Monte Carlo method. The zero-point energy of (p-H(2))(n)HF clusters is unusually large, amounting to 86% of the potential well depth for n > 7. The radial probability distribution functions (PDFs) confirm that the first solvent shell is complete for n = 12, and that the 13th p-H(2) molecule begins to fill the second solvent shell. The p-H(2) molecules execute large-amplitude motions and are highly mobile, making the solvent cage exceptionally fluxional. The anisotropy of the solvent, very pronounced for small clusters, decreases rapidly with increasing n, so that for n approximately 8-9 the solvent environment is practically isotropic. The analysis of the pair angular PDF reveals that for a given n, the parahydrogen solvent density around the HF is modulated in a pattern which clearly reflects the lowest-energy cluster configuration. The rigidity of the solvent clusters displays an interesting size dependence, increasing from n = 6 to 9, becoming floppier for n = 10, and increasing again up to n = 12, as the solvent shell is filled. The rigidity of the solvent cage appears to reach its maximum for n = 12, the point at which the first solvent shell is closed.

Intracellular distribution of nontargeted quantum dots after natural uptake and microinjection

PubMed Central

Damalakiene, Leona; Karabanovas, Vitalijus; Bagdonas, Saulius; Valius, Mindaugas; Rotomskis, Ricardas

2013-01-01

Background: The purpose of this study was to elucidate the mechanism of natural uptake of nonfunctionalized quantum dots in comparison with microinjected quantum dots by focusing on their time-dependent accumulation and intracellular localization in different cell lines. Methods: The accumulation dynamics of nontargeted CdSe/ZnS carboxyl-coated quantum dots (emission peak 625 nm) was analyzed in NIH3T3, MCF-7, and HepG2 cells by applying the methods of confocal and steady-state fluorescence spectroscopy. Intracellular colocalization of the quantum dots was investigated by staining with Lysotracker®. Results: The uptake of quantum dots into cells was dramatically reduced at a low temperature (4°C), indicating that the process is energy-dependent. The uptake kinetics and imaging of intracellular localization of quantum dots revealed three accumulation stages of carboxyl-coated quantum dots at 37°C, ie, a plateau stage, growth stage, and a saturation stage, which comprised four morphological phases: adherence to the cell membrane; formation of granulated clusters spread throughout the cytoplasm; localization of granulated clusters in the perinuclear region; and formation of multivesicular body-like structures and their redistribution in the cytoplasm. Diverse quantum dots containing intracellular vesicles in the range of approximately 0.5–8 μm in diameter were observed in the cytoplasm, but none were found in the nucleus. Vesicles containing quantum dots formed multivesicular body-like structures in NIH3T3 cells after 24 hours of incubation, which were Lysotracker-negative in serum-free medium and Lysotracker-positive in complete medium. The microinjected quantum dots remained uniformly distributed in the cytosol for at least 24 hours. Conclusion: Natural uptake of quantum dots in cells occurs through three accumulation stages via a mechanism requiring energy. The sharp contrast of the intracellular distribution after microinjection of quantum dots in comparison with incubation as well as the limited transfer of quantum dots from vesicles into the cytosol and vice versa support the endocytotic origin of the natural uptake of quantum dots. Quantum dots with proteins adsorbed from the culture medium had a different fate in the final stage of accumulation from that of the protein-free quantum dots, implying different internalization pathways. PMID:23429995

Sulfate radical oxidation of aromatic contaminants: a detailed assessment of density functional theory and high-level quantum chemical methods.

PubMed

Pari, Sangavi; Wang, Inger A; Liu, Haizhou; Wong, Bryan M

2017-03-22

Advanced oxidation processes that utilize highly oxidative radicals are widely used in water reuse treatment. In recent years, the application of sulfate radical (SO 4 ˙ - ) as a promising oxidant for water treatment has gained increasing attention. To understand the efficiency of SO 4 ˙ - in the degradation of organic contaminants in wastewater effluent, it is important to be able to predict the reaction kinetics of various SO 4 ˙ - -driven oxidation reactions. In this study, we utilize density functional theory (DFT) and high-level wavefunction-based methods (including computationally-intensive coupled cluster methods), to explore the activation energies of SO 4 ˙ - -driven oxidation reactions on a series of benzene-derived contaminants. These high-level calculations encompass a wide set of reactions including 110 forward/reverse reactions and 5 different computational methods in total. Based on the high-level coupled-cluster quantum calculations, we find that the popular M06-2X DFT functional is significantly more accurate for OH - additions than for SO 4 ˙ - reactions. Most importantly, we highlight some of the limitations and deficiencies of other computational methods, and we recommend the use of high-level quantum calculations to spot-check environmental chemistry reactions that may lie outside the training set of the M06-2X functional, particularly for water oxidation reactions that involve SO 4 ˙ - and other inorganic species.

Solid oxide fuel cell anode image segmentation based on a novel quantum-inspired fuzzy clustering

NASA Astrophysics Data System (ADS)

Fu, Xiaowei; Xiang, Yuhan; Chen, Li; Xu, Xin; Li, Xi

2015-12-01

High quality microstructure modeling can optimize the design of fuel cells. For three-phase accurate identification of Solid Oxide Fuel Cell (SOFC) microstructure, this paper proposes a novel image segmentation method on YSZ/Ni anode Optical Microscopic (OM) images. According to Quantum Signal Processing (QSP), the proposed approach exploits a quantum-inspired adaptive fuzziness factor to adaptively estimate the energy function in the fuzzy system based on Markov Random Filed (MRF). Before defuzzification, a quantum-inspired probability distribution based on distance and gray correction is proposed, which can adaptively adjust the inaccurate probability estimation of uncertain points caused by noises and edge points. In this study, the proposed method improves accuracy and effectiveness of three-phase identification on the micro-investigation. It provides firm foundation to investigate the microstructural evolution and its related properties.

Machine Learning for Discriminating Quantum Measurement Trajectories and Improving Readout.

PubMed

Magesan, Easwar; Gambetta, Jay M; Córcoles, A D; Chow, Jerry M

2015-05-22

Current methods for classifying measurement trajectories in superconducting qubit systems produce fidelities systematically lower than those predicted by experimental parameters. Here, we place current classification methods within the framework of machine learning (ML) algorithms and improve on them by investigating more sophisticated ML approaches. We find that nonlinear algorithms and clustering methods produce significantly higher assignment fidelities that help close the gap to the fidelity possible under ideal noise conditions. Clustering methods group trajectories into natural subsets within the data, which allows for the diagnosis of systematic errors. We find large clusters in the data associated with T1 processes and show these are the main source of discrepancy between our experimental and ideal fidelities. These error diagnosis techniques help provide a path forward to improve qubit measurements.

Ground and excited states of NH4: Electron propagator and quantum defect analysis

NASA Astrophysics Data System (ADS)

Ortiz, J. V.; Martín, I.; Velasco, A. M.; Lavín, C.

2004-05-01

Vertical excitation energies of the Rydberg radical NH4 are inferred from ab initio electron propagator calculations on the electron affinities of NH4+. The adiabatic ionization energy of NH4 is evaluated with coupled-cluster calculations. These predictions provide optimal parameters for the molecular-adapted quantum defect orbital method, which is used to determine Einstein emission coefficients and radiative lifetimes. Comparisons with spectroscopic data and previous calculations are discussed.

Critical behavior of a quantum chain with four-spin interactions in the presence of longitudinal and transverse magnetic fields.

PubMed

Boechat, B; Florencio, J; Saguia, A; de Alcantara Bonfim, O F

2014-03-01

We study the ground-state properties of a spin-1/2 model on a chain containing four-spin Ising-like interactions in the presence of both transverse and longitudinal magnetic fields. We use entanglement entropy and finite-size scaling methods to obtain the phase diagrams of the model. Our numerical calculations reveal a rich variety of phases and the existence of multicritical points in the system. We identify phases with both ferromagnetic and antiferromagnetic orderings. We also find periodically modulated orderings formed by a cluster of like spins followed by another cluster of opposite like spins. The quantum phases in the model are found to be separated by either first- or second-order transition lines.

Quantum clustering and network analysis of MD simulation trajectories to probe the conformational ensembles of protein-ligand interactions.

PubMed

Bhattacharyya, Moitrayee; Vishveshwara, Saraswathi

2011-07-01

In this article, we present a novel application of a quantum clustering (QC) technique to objectively cluster the conformations, sampled by molecular dynamics simulations performed on different ligand bound structures of the protein. We further portray each conformational population in terms of dynamically stable network parameters which beautifully capture the ligand induced variations in the ensemble in atomistic detail. The conformational populations thus identified by the QC method and verified by network parameters are evaluated for different ligand bound states of the protein pyrrolysyl-tRNA synthetase (DhPylRS) from D. hafniense. The ligand/environment induced re-distribution of protein conformational ensembles forms the basis for understanding several important biological phenomena such as allostery and enzyme catalysis. The atomistic level characterization of each population in the conformational ensemble in terms of the re-orchestrated networks of amino acids is a challenging problem, especially when the changes are minimal at the backbone level. Here we demonstrate that the QC method is sensitive to such subtle changes and is able to cluster MD snapshots which are similar at the side-chain interaction level. Although we have applied these methods on simulation trajectories of a modest time scale (20 ns each), we emphasize that our methodology provides a general approach towards an objective clustering of large-scale MD simulation data and may be applied to probe multistate equilibria at higher time scales, and to problems related to protein folding for any protein or protein-protein/RNA/DNA complex of interest with a known structure.

Protonation States of Homocitrate and Nearby Residues in Nitrogenase Studied by Computational Methods and Quantum Refinement.

PubMed

Cao, Lili; Caldararu, Octav; Ryde, Ulf

2017-09-07

Nitrogenase is the only enzyme that can break the triple bond in N 2 to form two molecules of ammonia. The enzyme has been thoroughly studied with both experimental and computational methods, but there is still no consensus regarding the atomic details of the reaction mechanism. In the most common form, the active site is a MoFe 7 S 9 C(homocitrate) cluster. The homocitrate ligand contains one alcohol and three carboxylate groups. In water solution, the triply deprotonated form dominates, but because the alcohol (and one of the carboxylate groups) coordinate to the Mo ion, this may change in the enzyme. We have performed a series of computational calculations with molecular dynamics (MD), quantum mechanical (QM) cluster, combined QM and molecular mechanics (QM/MM), QM/MM with Poisson-Boltzmann and surface area solvation, QM/MM thermodynamic cycle perturbations, and quantum refinement methods to settle the most probable protonation state of the homocitrate ligand in nitrogenase. The results quite conclusively point out a triply deprotonated form (net charge -3) with a proton shared between the alcohol and one of the carboxylate groups as the most stable at pH 7. Moreover, we have studied eight ionizable protein residues close to the active site with MD simulations and determined the most likely protonation states.

Chemical accuracy from quantum Monte Carlo for the benzene dimer.

PubMed

Azadi, Sam; Cohen, R E

2015-09-14

We report an accurate study of interactions between benzene molecules using variational quantum Monte Carlo (VMC) and diffusion quantum Monte Carlo (DMC) methods. We compare these results with density functional theory using different van der Waals functionals. In our quantum Monte Carlo (QMC) calculations, we use accurate correlated trial wave functions including three-body Jastrow factors and backflow transformations. We consider two benzene molecules in the parallel displaced geometry, and find that by highly optimizing the wave function and introducing more dynamical correlation into the wave function, we compute the weak chemical binding energy between aromatic rings accurately. We find optimal VMC and DMC binding energies of -2.3(4) and -2.7(3) kcal/mol, respectively. The best estimate of the coupled-cluster theory through perturbative triplets/complete basis set limit is -2.65(2) kcal/mol [Miliordos et al., J. Phys. Chem. A 118, 7568 (2014)]. Our results indicate that QMC methods give chemical accuracy for weakly bound van der Waals molecular interactions, comparable to results from the best quantum chemistry methods.

Phase diagram and quench dynamics of the cluster-XY spin chain

NASA Astrophysics Data System (ADS)

Montes, Sebastián; Hamma, Alioscia

2012-08-01

We study the complete phase space and the quench dynamics of an exactly solvable spin chain, the cluster-XY model. In this chain, the cluster term and the XY couplings compete to give a rich phase diagram. The phase diagram is studied by means of the quantum geometric tensor. We study the time evolution of the system after a critical quantum quench using the Loschmidt echo. The structure of the revivals after critical quantum quenches presents a nontrivial behavior depending on the phase of the initial state and the critical point.

Phase diagram and quench dynamics of the cluster-XY spin chain.

PubMed

Montes, Sebastián; Hamma, Alioscia

2012-08-01

We study the complete phase space and the quench dynamics of an exactly solvable spin chain, the cluster-XY model. In this chain, the cluster term and the XY couplings compete to give a rich phase diagram. The phase diagram is studied by means of the quantum geometric tensor. We study the time evolution of the system after a critical quantum quench using the Loschmidt echo. The structure of the revivals after critical quantum quenches presents a nontrivial behavior depending on the phase of the initial state and the critical point.

Graph-theoretic quantum system modelling for neuronal microtubules as hierarchical clustered quantum Hopfield networks

NASA Astrophysics Data System (ADS)

Srivastava, D. P.; Sahni, V.; Satsangi, P. S.

2014-08-01

Graph-theoretic quantum system modelling (GTQSM) is facilitated by considering the fundamental unit of quantum computation and information, viz. a quantum bit or qubit as a basic building block. Unit directional vectors "ket 0" and "ket 1" constitute two distinct fundamental quantum across variable orthonormal basis vectors, for the Hilbert space, specifying the direction of propagation of information, or computation data, while complementary fundamental quantum through, or flow rate, variables specify probability parameters, or amplitudes, as surrogates for scalar quantum information measure (von Neumann entropy). This paper applies GTQSM in continuum of protein heterodimer tubulin molecules of self-assembling polymers, viz. microtubules in the brain as a holistic system of interacting components representing hierarchical clustered quantum Hopfield network, hQHN, of networks. The quantum input/output ports of the constituent elemental interaction components, or processes, of tunnelling interactions and Coulombic bidirectional interactions are in cascade and parallel interconnections with each other, while the classical output ports of all elemental components are interconnected in parallel to accumulate micro-energy functions generated in the system as Hamiltonian, or Lyapunov, energy function. The paper presents an insight, otherwise difficult to gain, for the complex system of systems represented by clustered quantum Hopfield network, hQHN, through the application of GTQSM construct.

Quantum phase transition between cluster and antiferromagnetic states

NASA Astrophysics Data System (ADS)

Son, W.; Amico, L.; Fazio, R.; Hamma, A.; Pascazio, S.; Vedral, V.

2011-09-01

We study a Hamiltonian system describing a three-spin-1/2 cluster-like interaction competing with an Ising-like exchange. We show that the ground state in the cluster phase possesses symmetry protected topological order. A continuous quantum phase transition occurs as result of the competition between the cluster and Ising terms. At the critical point the Hamiltonian is self-dual. The geometric entanglement is also studied and used to investigate the quantum phase transition. Our findings in one dimension corroborate the analysis of the two-dimensional generalization of the system, indicating, at a mean-field level, the presence of a direct transition between an antiferromagnetic and a valence bond solid ground state.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Azadi, Sam, E-mail: s.azadi@ucl.ac.uk; Cohen, R. E.

We report an accurate study of interactions between benzene molecules using variational quantum Monte Carlo (VMC) and diffusion quantum Monte Carlo (DMC) methods. We compare these results with density functional theory using different van der Waals functionals. In our quantum Monte Carlo (QMC) calculations, we use accurate correlated trial wave functions including three-body Jastrow factors and backflow transformations. We consider two benzene molecules in the parallel displaced geometry, and find that by highly optimizing the wave function and introducing more dynamical correlation into the wave function, we compute the weak chemical binding energy between aromatic rings accurately. We find optimalmore » VMC and DMC binding energies of −2.3(4) and −2.7(3) kcal/mol, respectively. The best estimate of the coupled-cluster theory through perturbative triplets/complete basis set limit is −2.65(2) kcal/mol [Miliordos et al., J. Phys. Chem. A 118, 7568 (2014)]. Our results indicate that QMC methods give chemical accuracy for weakly bound van der Waals molecular interactions, comparable to results from the best quantum chemistry methods.« less

Combination of Wavefunction and Density Functional Approximations for Describing Electronic Correlation

NASA Astrophysics Data System (ADS)

Garza, Alejandro J.

Perhaps the most important approximations to the electronic structure problem in quantum chemistry are those based on coupled cluster and density functional theories. Coupled cluster theory has been called the ``gold standard'' of quantum chemistry due to the high accuracy that it achieves for weakly correlated systems. Kohn-Sham density functionals based on semilocal approximations are, without a doubt, the most widely used methods in chemistry and material science because of their high accuracy/cost ratio. The root of the success of coupled cluster and density functionals is their ability to efficiently describe the dynamic part of the electron correlation. However, both traditional coupled cluster and density functional approximations may fail catastrophically when substantial static correlation is present. This severely limits the applicability of these methods to a plethora of important chemical and physical problems such as, e.g., the description of bond breaking, transition states, transition metal-, lanthanide- and actinide-containing compounds, and superconductivity. In an attempt to tackle this problem, nonstandard (single-reference) coupled cluster-based techniques that aim to describe static correlation have been recently developed: pair coupled cluster doubles (pCCD) and singlet-paired coupled cluster doubles (CCD0). The ability to describe static correlation in pCCD and CCD0 comes, however, at the expense of important amounts of dynamic correlation so that the high accuracy of standard coupled cluster becomes unattainable. Thus, the reliable and efficient description of static and dynamic correlation in a simultaneous manner remains an open problem for quantum chemistry and many-body theory in general. In this thesis, different ways to combine pCCD and CCD0 with density functionals in order to describe static and dynamic correlation simultaneously (and efficiently) are explored. The combination of wavefunction and density functional methods has a long history in quantum chemistry (practical implementations have appeared in the literature since the 1970s). However, this kind of techniques have not achieved widespread use due to problems such as double counting of correlation and the symmetry dilemma--the fact that wavefunction methods respect the symmetries of Hamiltonian, while modern functionals are designed to work with broken symmetry densities. Here, particular mathematical features of pCCD and CCD0 are exploited to avoid these problems in an efficient manner. The two resulting families of approximations, denoted as pCCD+DFT and CCD0+DFT, are shown to be able to describe static and dynamic correlation in standard benchmark calculations. Furthermore, it is also shown that CCD0+DFT lends itself to combination with correlation from the direct random phase approximation (dRPA). Inclusion of dRPA in the long-range via the technique of range-separation allows for the description of dispersion correlation, the remaining part of the correlation. Thus, when combined with the dRPA, CCD0+DFT can account for all three-types of electron correlation that are necessary to accurately describe molecular systems. Lastly, applications of CCD0+DFT to actinide chemistry are considered in this work. The accuracy of CCD0+DFT for predicting equilibrium geometries and vibrational frequencies of actinide molecules and ions is assessed and compared to that of well-established quantum chemical methods. For this purpose, the f0 actinyl series (UO2 2+, NpO 23+, PuO24+, the isoelectronic NUN, and Thorium (ThO, ThO2+) and Nobelium (NoO, NoO2) oxides are studied. It is shown that the CCD0+DFT description of these species agrees with available experimental data and is comparable with the results given by the highest-level calculations that are possible for such heavy compounds while being, at least, an order of magnitude lower in computational cost.

Multiple exciton generation in cluster-free alloy Cd(x)Hg(1-x)Te colloidal quantum dots synthesized in water.

PubMed

Kershaw, Stephen V; Kalytchuk, Sergii; Zhovtiuk, Olga; Shen, Qing; Oshima, Takuya; Yindeesuk, Witoon; Toyoda, Taro; Rogach, Andrey L

2014-12-21

A number of different composition CdxHg1-xTe alloy quantum dots have been synthesized using a modified aqueous synthesis and ion exchange method. The benefits of good stoichiometric control and high emission quantum yield were retained whilst also ensuring that the tendency to form gel-like clusters and adsorb excess cations in the stabilizing ligand shells was mitigated using a sequestering method to remove excess ionic material during and after the synthesis. This was highly desirable for ultrafast carrier dynamics measurements, avoiding strong photocharging effects which may mask fundamental carrier signals. Transient grating measurements revealed a composition dependent carrier multiplication process which competes with phonon mediated carrier cooling to deplete the initial hot carrier population. The interplay between these two mechanisms is strongly dependent on the electron effective mass which in these alloys has a marked composition dependence and may be considerably lower than the hole effective mass. For a composition x = 0.52 we measured a maximum carrier multiplication quantum yield of 199 ± 19% with pump photon energy 3 times the bandgap energy, Eg, whilst the threshold energy is calculated to be just 2.15Eg. There is some evidence to suggest an impact ionization process analogous to the inverse Auger S mechanism seen in bulk CdxHg1-xTe.

Strange Bedfellows: Quantum Mechanics and Data Mining

NASA Astrophysics Data System (ADS)

Weinstein, Marvin

2010-02-01

Last year, in 2008, I gave a talk titled Quantum Calisthenics. This year I am going to tell you about how the work I described then has spun off into a most unlikely direction. What I am going to talk about is how one maps the problem of finding clusters in a given data set into a problem in quantum mechanics. I will then use the tricks I described to let quantum evolution lets the clusters come together on their own.

Quantum Image Steganography and Steganalysis Based On LSQu-Blocks Image Information Concealing Algorithm

NASA Astrophysics Data System (ADS)

A. AL-Salhi, Yahya E.; Lu, Songfeng

2016-08-01

Quantum steganography can solve some problems that are considered inefficient in image information concealing. It researches on Quantum image information concealing to have been widely exploited in recent years. Quantum image information concealing can be categorized into quantum image digital blocking, quantum image stereography, anonymity and other branches. Least significant bit (LSB) information concealing plays vital roles in the classical world because many image information concealing algorithms are designed based on it. Firstly, based on the novel enhanced quantum representation (NEQR), image uniform blocks clustering around the concrete the least significant Qu-block (LSQB) information concealing algorithm for quantum image steganography is presented. Secondly, a clustering algorithm is proposed to optimize the concealment of important data. Finally, we used Con-Steg algorithm to conceal the clustered image blocks. Information concealing located on the Fourier domain of an image can achieve the security of image information, thus we further discuss the Fourier domain LSQu-block information concealing algorithm for quantum image based on Quantum Fourier Transforms. In our algorithms, the corresponding unitary Transformations are designed to realize the aim of concealing the secret information to the least significant Qu-block representing color of the quantum cover image. Finally, the procedures of extracting the secret information are illustrated. Quantum image LSQu-block image information concealing algorithm can be applied in many fields according to different needs.

Continuous Variable Cluster State Generation over the Optical Spatial Mode Comb

DOE PAGES

Pooser, Raphael C.; Jing, Jietai

2014-10-20

One way quantum computing uses single qubit projective measurements performed on a cluster state (a highly entangled state of multiple qubits) in order to enact quantum gates. The model is promising due to its potential scalability; the cluster state may be produced at the beginning of the computation and operated on over time. Continuous variables (CV) offer another potential benefit in the form of deterministic entanglement generation. This determinism can lead to robust cluster states and scalable quantum computation. Recent demonstrations of CV cluster states have made great strides on the path to scalability utilizing either time or frequency multiplexingmore » in optical parametric oscillators (OPO) both above and below threshold. The techniques relied on a combination of entangling operators and beam splitter transformations. Here we show that an analogous transformation exists for amplifiers with Gaussian inputs states operating on multiple spatial modes. By judicious selection of local oscillators (LOs), the spatial mode distribution is analogous to the optical frequency comb consisting of axial modes in an OPO cavity. We outline an experimental system that generates cluster states across the spatial frequency comb which can also scale the amount of quantum noise reduction to potentially larger than in other systems.« less

Hole localization in Fe2O3 from density functional theory and wave-function-based methods

NASA Astrophysics Data System (ADS)

Ansari, Narjes; Ulman, Kanchan; Camellone, Matteo Farnesi; Seriani, Nicola; Gebauer, Ralph; Piccinin, Simone

2017-08-01

Hematite (α -Fe2O3 ) is a promising photocatalyst material for water splitting, where photoinduced holes lead to the oxidation of water and the release of molecular oxygen. In this work, we investigate the properties of holes in hematite using density functional theory (DFT) calculations with hybrid functionals. We find that holes form small polarons and, depending on the fraction of exact exchange included in the PBE0 functional, the site where the holes localize changes from Fe to O. We find this result to be independent of the size and structure of the system: small Fe2O3 clusters with tetrahedral coordination, larger clusters with octahedral coordination, Fe2O3 (001) surfaces in contact with water, and bulk Fe2O3 display a very similar behavior in terms of hole localization as a function of the fraction of exact exchange. We then use wave-function-based methods such as coupled cluster with single and double excitations and Møller-Plesset second-order perturbation theory applied on a cluster model of Fe2O3 to shed light on which of the two solutions is correct. We find that these high-level quantum chemistry methods suggest holes in hematite are localized on oxygen atoms. We also explore the use of the DFT +U approach as a computationally convenient way to overcome the known limitations of generalized gradient approximation functionals and recover a gap in line with experiments and hole localization on oxygen in agreement with quantum chemistry methods.

Cluster Quantum Chemical Study of the Grignard Reagent Formation

NASA Astrophysics Data System (ADS)

Tulub, A. V.; Porsev, V. V.

The main stages of the Grignard reagent formation are described in a framework of quantum chemical cluster model. We have established two kinds of the adsorption of CH3Hal on Mgn clusters, one of which leads to radical formation and the second is responsible for radical free dissociate adsorption. The charge redistribution in cluster CH3MgnHal result to the strong electrostatic interaction with ether and Grignard reagent formation without any activation barrier.

Quantum Computational Universality of the 2D Cai-Miyake-D"ur-Briegel Quantum State

NASA Astrophysics Data System (ADS)

Wei, Tzu-Chieh; Raussendorf, Robert; Kwek, Leong Chuan

2012-02-01

Universal quantum computation can be achieved by simply performing single-qubit measurements on a highly entangled resource state, such as cluster states. Cai, Miyake, D"ur, and Briegel recently constructed a ground state of a two-dimensional quantum magnet by combining multiple Affleck-Kennedy-Lieb-Tasaki quasichains of mixed spin-3/2 and spin-1/2 entities and by mapping pairs of neighboring spin-1/2 particles to individual spin-3/2 particles [Phys. Rev. A 82, 052309 (2010)]. They showed that this state enables universal quantum computation by constructing single- and two-qubit universal gates. Here, we give an alternative understanding of how this state gives rise to universal measurement-based quantum computation: by local operations, each quasichain can be converted to a one-dimensional cluster state and entangling gates between two neighboring logical qubits can be implemented by single-spin measurements. Furthermore, a two-dimensional cluster state can be distilled from the Cai-Miyake-D"ur-Briegel state.

Quantum computational universality of the Cai-Miyake-Duer-Briegel two-dimensional quantum state from Affleck-Kennedy-Lieb-Tasaki quasichains

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wei, Tzu-Chieh; C. N. Yang Institute for Theoretical Physics, State University of New York at Stony Brook, Stony Brook, New York 11794-3840; Raussendorf, Robert

2011-10-15

Universal quantum computation can be achieved by simply performing single-qubit measurements on a highly entangled resource state, such as cluster states. Cai, Miyake, Duer, and Briegel recently constructed a ground state of a two-dimensional quantum magnet by combining multiple Affleck-Kennedy-Lieb-Tasaki quasichains of mixed spin-3/2 and spin-1/2 entities and by mapping pairs of neighboring spin-1/2 particles to individual spin-3/2 particles [Phys. Rev. A 82, 052309 (2010)]. They showed that this state enables universal quantum computation by single-spin measurements. Here, we give an alternative understanding of how this state gives rise to universal measurement-based quantum computation: by local operations, each quasichain canmore » be converted to a one-dimensional cluster state and entangling gates between two neighboring logical qubits can be implemented by single-spin measurements. We further argue that a two-dimensional cluster state can be distilled from the Cai-Miyake-Duer-Briegel state.« less

Quantum Error Correction

NASA Astrophysics Data System (ADS)

Lidar, Daniel A.; Brun, Todd A.

2013-09-01

Prologue; Preface; Part I. Background: 1. Introduction to decoherence and noise in open quantum systems Daniel Lidar and Todd Brun; 2. Introduction to quantum error correction Dave Bacon; 3. Introduction to decoherence-free subspaces and noiseless subsystems Daniel Lidar; 4. Introduction to quantum dynamical decoupling Lorenza Viola; 5. Introduction to quantum fault tolerance Panos Aliferis; Part II. Generalized Approaches to Quantum Error Correction: 6. Operator quantum error correction David Kribs and David Poulin; 7. Entanglement-assisted quantum error-correcting codes Todd Brun and Min-Hsiu Hsieh; 8. Continuous-time quantum error correction Ognyan Oreshkov; Part III. Advanced Quantum Codes: 9. Quantum convolutional codes Mark Wilde; 10. Non-additive quantum codes Markus Grassl and Martin Rötteler; 11. Iterative quantum coding systems David Poulin; 12. Algebraic quantum coding theory Andreas Klappenecker; 13. Optimization-based quantum error correction Andrew Fletcher; Part IV. Advanced Dynamical Decoupling: 14. High order dynamical decoupling Zhen-Yu Wang and Ren-Bao Liu; 15. Combinatorial approaches to dynamical decoupling Martin Rötteler and Pawel Wocjan; Part V. Alternative Quantum Computation Approaches: 16. Holonomic quantum computation Paolo Zanardi; 17. Fault tolerance for holonomic quantum computation Ognyan Oreshkov, Todd Brun and Daniel Lidar; 18. Fault tolerant measurement-based quantum computing Debbie Leung; Part VI. Topological Methods: 19. Topological codes Héctor Bombín; 20. Fault tolerant topological cluster state quantum computing Austin Fowler and Kovid Goyal; Part VII. Applications and Implementations: 21. Experimental quantum error correction Dave Bacon; 22. Experimental dynamical decoupling Lorenza Viola; 23. Architectures Jacob Taylor; 24. Error correction in quantum communication Mark Wilde; Part VIII. Critical Evaluation of Fault Tolerance: 25. Hamiltonian methods in QEC and fault tolerance Eduardo Novais, Eduardo Mucciolo and Harold Baranger; 26. Critique of fault-tolerant quantum information processing Robert Alicki; References; Index.

A study of fullerene-quantum dot composite structure on substrates with a transparent electrode layer

NASA Astrophysics Data System (ADS)

Pavlov, S. I.; Kirilenko, D. A.; Nashchekin, A. V.; Sokolov, R. V.; Konnikov, S. G.

2015-02-01

We have studied the structure of films consisting of fullerene clusters and a related fullerene-based composite with incorporated quantum dots. The films were obtained by electrophoretic deposition from solution onto glass substrates with a transparent indium-doped tin oxide (ITO) electrode layer. The average cluster size, as measured by electron microscopy, amounts to 300 nm in pure fullerene films and 800 nm in the composite material. Electron diffraction measurements showed that pure fullerene clusters had an fcc lattice, while the introduction of quantum dots rendered the fullerene matrix predominantly amorphous.

Recent Trends in Quantum Chemical Modeling of Enzymatic Reactions.

PubMed

Himo, Fahmi

2017-05-24

The quantum chemical cluster approach is a powerful method for investigating enzymatic reactions. Over the past two decades, a large number of highly diverse systems have been studied and a great wealth of mechanistic insight has been developed using this technique. This Perspective reviews the current status of the methodology. The latest technical developments are highlighted, and challenges are discussed. Some recent applications are presented to illustrate the capabilities and progress of this approach, and likely future directions are outlined.

Ab initio quantum chemistry: methodology and applications.

PubMed

Friesner, Richard A

2005-05-10

This Perspective provides an overview of state-of-the-art ab initio quantum chemical methodology and applications. The methods that are discussed include coupled cluster theory, localized second-order Moller-Plesset perturbation theory, multireference perturbation approaches, and density functional theory. The accuracy of each approach for key chemical properties is summarized, and the computational performance is analyzed, emphasizing significant advances in algorithms and implementation over the past decade. Incorporation of a condensed-phase environment by means of mixed quantum mechanical/molecular mechanics or self-consistent reaction field techniques, is presented. A wide range of illustrative applications, focusing on materials science and biology, are discussed briefly.

Light clusters and pasta phases in warm and dense nuclear matter

NASA Astrophysics Data System (ADS)

Avancini, Sidney S.; Ferreira, Márcio; Pais, Helena; Providência, Constança; Röpke, Gerd

2017-04-01

The pasta phases are calculated for warm stellar matter in a framework of relativistic mean-field models, including the possibility of light cluster formation. Results from three different semiclassical approaches are compared with a quantum statistical calculation. Light clusters are considered as point-like particles, and their abundances are determined from the minimization of the free energy. The couplings of the light clusters to mesons are determined from experimental chemical equilibrium constants and many-body quantum statistical calculations. The effect of these light clusters on the chemical potentials is also discussed. It is shown that, by including heavy clusters, light clusters are present up to larger nucleonic densities, although with smaller mass fractions.

Psi4NumPy: An Interactive Quantum Chemistry Programming Environment for Reference Implementations and Rapid Development.

PubMed

Smith, Daniel G A; Burns, Lori A; Sirianni, Dominic A; Nascimento, Daniel R; Kumar, Ashutosh; James, Andrew M; Schriber, Jeffrey B; Zhang, Tianyuan; Zhang, Boyi; Abbott, Adam S; Berquist, Eric J; Lechner, Marvin H; Cunha, Leonardo A; Heide, Alexander G; Waldrop, Jonathan M; Takeshita, Tyler Y; Alenaizan, Asem; Neuhauser, Daniel; King, Rollin A; Simmonett, Andrew C; Turney, Justin M; Schaefer, Henry F; Evangelista, Francesco A; DePrince, A Eugene; Crawford, T Daniel; Patkowski, Konrad; Sherrill, C David

2018-06-11

Psi4NumPy demonstrates the use of efficient computational kernels from the open-source Psi4 program through the popular NumPy library for linear algebra in Python to facilitate the rapid development of clear, understandable Python computer code for new quantum chemical methods, while maintaining a relatively low execution time. Using these tools, reference implementations have been created for a number of methods, including self-consistent field (SCF), SCF response, many-body perturbation theory, coupled-cluster theory, configuration interaction, and symmetry-adapted perturbation theory. Furthermore, several reference codes have been integrated into Jupyter notebooks, allowing background, underlying theory, and formula information to be associated with the implementation. Psi4NumPy tools and associated reference implementations can lower the barrier for future development of quantum chemistry methods. These implementations also demonstrate the power of the hybrid C++/Python programming approach employed by the Psi4 program.

Control of Wannier orbitals for generating tunable Ising interactions of ultracold atoms in an optical lattice

DOE Office of Scientific and Technical Information (OSTI.GOV)

Inaba, Kensuke; Tamaki, Kiyoshi; Igeta, Kazuhiro

2014-12-04

In this study, we propose a method for generating cluster states of atoms in an optical lattice. By utilizing the quantum properties of Wannier orbitals, we create an tunable Ising interaction between atoms without inducing the spin-exchange interactions. We investigate the cause of errors that occur during entanglement generations, and then we propose an error-management scheme, which allows us to create high-fidelity cluster states in a short time.

Quantum chemical study of the structure, spectroscopy and reactivity of NO+.(H2O)n=1-5 clusters

NASA Astrophysics Data System (ADS)

Linton, Kirsty A.; Wright, Timothy G.; Besley, Nicholas A.

2018-03-01

Quantum chemical methods including Møller-Plesset perturbation (MP2) theory and density functional theory (DFT) have been used to study the structure, spectroscopy and reactivity of NO+.(H2O)n=1-5 clusters. MP2/6-311++G** calculations are shown to describe the structure and spectroscopy of the clusters well. DFT calculations with exchange-correlation functionals with a low fraction of Hartree-Fock exchange give a binding energy of NO+.(H2O) that is too high and incorrectly predict the lowest energy structure of NO+.(H2O)2, and this error may be associated with a delocalization of charge onto the water molecule directly binding to NO+. Ab initio molecular dynamics (AIMD) simulations were performed to study the NO+.(H2O)5 H+.(H2O)4 + HONO reaction to investigate the formation of HONO from NO+.(H2O)5. Whether an intracluster reaction to form HONO is observed depends on the level of electronic structure theory used. Of note is that methods that accurately describe the relative energies of the product and reactant clusters did not show reactions on the timescales studied. This suggests that in the upper atmosphere the reaction may occur owing to the energy present in the NO+.(H2O)5 complex following its formation. This article is part of the theme issue `Modern theoretical chemistry'.

Theoretical investigation of the He4Br2 conformers.

PubMed

Valdés, Álvaro; Prosmiti, Rita; Villarreal, Pablo; Delgado-Barrio, Gerardo

2012-07-05

Full dimensional quantum dynamics calculations of the three lowest isomers of the He(4)Br(2) van der Waals molecule in its ground electronic state are reported. The calculations are performed using the multiconfiguration time-dependent Hartree (MCTDH) method and a realistic potential form that includes the sum of three body ab initio coupled-cluster single double triple [CCSD(T)] He-Br(2) interactions plus the He-He and Br-Br interactions. This potential exhibits several multiple minima, with the three lowest ones lying very close in energy, just within 2 cm(-1). Such small differences are also found in the calculated binding energies of the three most stable conformers, indicating the floppiness of the system and, thus, the need of accurate potential forms and quantum full dynamics methods to treat this kind of complexes. The 12 dimensional results reported in this work present benchmark data and, thus, can serve to evaluate approximate methods aiming to describe higher order rare gas-dihalogen (N > 4) complexes. A comparison with previous studies using different potential forms and approaches to the energetics for the He(4)Br(2) cluster is also presented.

Bidirectional Quantum Teleportation by Using Five-qubit Cluster State

NASA Astrophysics Data System (ADS)

Sang, Ming-huang

2016-03-01

We propose a scheme for bidirectional quantum teleportation by using a five-qubit cluster state. In our scheme, Alice can transmit an arbitrary two-qubit entangled state to Bob and at the same time Bob can teleport an arbitrary single-qubit state to Alice.

Fully accelerating quantum Monte Carlo simulations of real materials on GPU clusters

NASA Astrophysics Data System (ADS)

Esler, Kenneth

2011-03-01

Quantum Monte Carlo (QMC) has proved to be an invaluable tool for predicting the properties of matter from fundamental principles, combining very high accuracy with extreme parallel scalability. By solving the many-body Schrödinger equation through a stochastic projection, it achieves greater accuracy than mean-field methods and better scaling with system size than quantum chemical methods, enabling scientific discovery across a broad spectrum of disciplines. In recent years, graphics processing units (GPUs) have provided a high-performance and low-cost new approach to scientific computing, and GPU-based supercomputers are now among the fastest in the world. The multiple forms of parallelism afforded by QMC algorithms make the method an ideal candidate for acceleration in the many-core paradigm. We present the results of porting the QMCPACK code to run on GPU clusters using the NVIDIA CUDA platform. Using mixed precision on GPUs and MPI for intercommunication, we observe typical full-application speedups of approximately 10x to 15x relative to quad-core CPUs alone, while reproducing the double-precision CPU results within statistical error. We discuss the algorithm modifications necessary to achieve good performance on this heterogeneous architecture and present the results of applying our code to molecules and bulk materials. Supported by the U.S. DOE under Contract No. DOE-DE-FG05-08OR23336 and by the NSF under No. 0904572.

Efficient electronic structure theory via hierarchical scale-adaptive coupled-cluster formalism: I. Theory and computational complexity analysis

NASA Astrophysics Data System (ADS)

Lyakh, Dmitry I.

2018-03-01

A novel reduced-scaling, general-order coupled-cluster approach is formulated by exploiting hierarchical representations of many-body tensors, combined with the recently suggested formalism of scale-adaptive tensor algebra. Inspired by the hierarchical techniques from the renormalisation group approach, H/H2-matrix algebra and fast multipole method, the computational scaling reduction in our formalism is achieved via coarsening of quantum many-body interactions at larger interaction scales, thus imposing a hierarchical structure on many-body tensors of coupled-cluster theory. In our approach, the interaction scale can be defined on any appropriate Euclidean domain (spatial domain, momentum-space domain, energy domain, etc.). We show that the hierarchically resolved many-body tensors can reduce the storage requirements to O(N), where N is the number of simulated quantum particles. Subsequently, we prove that any connected many-body diagram consisting of a finite number of arbitrary-order tensors, e.g. an arbitrary coupled-cluster diagram, can be evaluated in O(NlogN) floating-point operations. On top of that, we suggest an additional approximation to further reduce the computational complexity of higher order coupled-cluster equations, i.e. equations involving higher than double excitations, which otherwise would introduce a large prefactor into formal O(NlogN) scaling.

Atomically precise cluster catalysis towards quantum controlled catalysts

PubMed Central

Watanabe, Yoshihide

2014-01-01

Catalysis of atomically precise clusters supported on a substrate is reviewed in relation to the type of reactions. The catalytic activity of supported clusters has generally been discussed in terms of electronic structure. Several lines of evidence have indicated that the electronic structure of clusters and the geometry of clusters on a support, including the accompanying cluster-support interaction, are strongly correlated with catalytic activity. The electronic states of small clusters would be easily affected by cluster–support interactions. Several studies have suggested that it is possible to tune the electronic structure through atomic control of the cluster size. It is promising to tune not only the number of cluster atoms, but also the hybridization between the electronic states of the adsorbed reactant molecules and clusters in order to realize a quantum-controlled catalyst. PMID:27877723

High-Threshold Fault-Tolerant Quantum Computation with Analog Quantum Error Correction

NASA Astrophysics Data System (ADS)

Fukui, Kosuke; Tomita, Akihisa; Okamoto, Atsushi; Fujii, Keisuke

2018-04-01

To implement fault-tolerant quantum computation with continuous variables, the Gottesman-Kitaev-Preskill (GKP) qubit has been recognized as an important technological element. However, it is still challenging to experimentally generate the GKP qubit with the required squeezing level, 14.8 dB, of the existing fault-tolerant quantum computation. To reduce this requirement, we propose a high-threshold fault-tolerant quantum computation with GKP qubits using topologically protected measurement-based quantum computation with the surface code. By harnessing analog information contained in the GKP qubits, we apply analog quantum error correction to the surface code. Furthermore, we develop a method to prevent the squeezing level from decreasing during the construction of the large-scale cluster states for the topologically protected, measurement-based, quantum computation. We numerically show that the required squeezing level can be relaxed to less than 10 dB, which is within the reach of the current experimental technology. Hence, this work can considerably alleviate this experimental requirement and take a step closer to the realization of large-scale quantum computation.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Weinstein, Marvin; /SLAC

Last year, in 2008, I gave a talk titled Quantum Calisthenics. This year I am going to tell you about how the work I described then has spun off into a most unlikely direction. What I am going to talk about is how one maps the problem of finding clusters in a given data set into a problem in quantum mechanics. I will then use the tricks I described to let quantum evolution lets the clusters come together on their own.

Spectral functions of strongly correlated extended systems via an exact quantum embedding

NASA Astrophysics Data System (ADS)

Booth, George H.; Chan, Garnet Kin-Lic

2015-04-01

Density matrix embedding theory (DMET) [Phys. Rev. Lett. 109, 186404 (2012), 10.1103/PhysRevLett.109.186404], introduced an approach to quantum cluster embedding methods whereby the mapping of strongly correlated bulk problems to an impurity with finite set of bath states was rigorously formulated to exactly reproduce the entanglement of the ground state. The formalism provided similar physics to dynamical mean-field theory at a tiny fraction of the cost but was inherently limited by the construction of a bath designed to reproduce ground-state, static properties. Here, we generalize the concept of quantum embedding to dynamic properties and demonstrate accurate bulk spectral functions at similarly small computational cost. The proposed spectral DMET utilizes the Schmidt decomposition of a response vector, mapping the bulk dynamic correlation functions to that of a quantum impurity cluster coupled to a set of frequency-dependent bath states. The resultant spectral functions are obtained on the real-frequency axis, without bath discretization error, and allows for the construction of arbitrary dynamic correlation functions. We demonstrate the method on the one- (1D) and two-dimensional (2D) Hubbard model, where we obtain zero temperature and thermodynamic limit spectral functions, and show the trivial extension to two-particle Green's functions. This advance therefore extends the scope and applicability of DMET in condensed-matter problems as a computationally tractable route to correlated spectral functions of extended systems and provides a competitive alternative to dynamical mean-field theory for dynamic quantities.

Quantum computational universality of the Cai-Miyake-Dür-Briegel two-dimensional quantum state from Affleck-Kennedy-Lieb-Tasaki quasichains

NASA Astrophysics Data System (ADS)

Wei, Tzu-Chieh; Raussendorf, Robert; Kwek, Leong Chuan

2011-10-01

Universal quantum computation can be achieved by simply performing single-qubit measurements on a highly entangled resource state, such as cluster states. Cai, Miyake, Dür, and Briegel recently constructed a ground state of a two-dimensional quantum magnet by combining multiple Affleck-Kennedy-Lieb-Tasaki quasichains of mixed spin-3/2 and spin-1/2 entities and by mapping pairs of neighboring spin-1/2 particles to individual spin-3/2 particles [Phys. Rev. APLRAAN1050-294710.1103/PhysRevA.82.052309 82, 052309 (2010)]. They showed that this state enables universal quantum computation by single-spin measurements. Here, we give an alternative understanding of how this state gives rise to universal measurement-based quantum computation: by local operations, each quasichain can be converted to a one-dimensional cluster state and entangling gates between two neighboring logical qubits can be implemented by single-spin measurements. We further argue that a two-dimensional cluster state can be distilled from the Cai-Miyake-Dür-Briegel state.

Superradiant Quantum Heat Engine.

PubMed

Hardal, Ali Ü C; Müstecaplıoğlu, Özgür E

2015-08-11

Quantum physics revolutionized classical disciplines of mechanics, statistical physics, and electrodynamics. One branch of scientific knowledge however seems untouched: thermodynamics. Major motivation behind thermodynamics is to develop efficient heat engines. Technology has a trend to miniaturize engines, reaching to quantum regimes. Development of quantum heat engines (QHEs) requires emerging field of quantum thermodynamics. Studies of QHEs debate whether quantum coherence can be used as a resource. We explore an alternative where it can function as an effective catalyst. We propose a QHE which consists of a photon gas inside an optical cavity as the working fluid and quantum coherent atomic clusters as the fuel. Utilizing the superradiance, where a cluster can radiate quadratically faster than a single atom, we show that the work output becomes proportional to the square of the number of the atoms. In addition to practical value of cranking up QHE, our result is a fundamental difference of a quantum fuel from its classical counterpart.

Self-consistent phonons revisited. I. The role of thermal versus quantum fluctuations on structural transitions in large Lennard-Jones clusters.

PubMed

Georgescu, Ionuţ; Mandelshtam, Vladimir A

2012-10-14

The theory of self-consistent phonons (SCP) was originally developed to address the anharmonic effects in condensed matter systems. The method seeks a harmonic, temperature-dependent Hamiltonian that provides the "best fit" for the physical Hamiltonian, the "best fit" being defined as the one that optimizes the Helmholtz free energy at a fixed temperature. The present developments provide a scalable O(N) unified framework that accounts for anharmonic effects in a many-body system, when it is probed by either thermal (ℏ → 0) or quantum fluctuations (T → 0). In these important limits, the solution of the nonlinear SCP equations can be reached in a manner that requires only the multiplication of 3N × 3N matrices, with no need of diagonalization. For short range potentials, such as Lennard-Jones, the Hessian, and other related matrices are highly sparse, so that the scaling of the matrix multiplications can be reduced from O(N(3)) to ~O(N). We investigate the role of quantum effects by continuously varying the de-Boer quantum delocalization parameter Λ and report the N-Λ (T = 0), and also the classical N-T (Λ = 0) phase diagrams for sizes up to N ~ 10(4). Our results demonstrate that the harmonic approximation becomes inadequate already for such weakly quantum systems as neon clusters, or for classical systems much below the melting temperatures.

Comment on "Quantum Teleportation of Eight-Qubit State via Six-Qubit Cluster State"

NASA Astrophysics Data System (ADS)

Sisodia, Mitali; Pathak, Anirban

2018-04-01

Recently, Zhao et al. (Int. J. Theor. Phys. 57, 516-522 2018) have proposed a scheme for quantum teleportation of an eight-qubit quantum state using a six qubit cluster state. In this comment, it's shown that the quantum resource (multi-partite entangled state used as the quantum channel) used by Zhao et al., is excessively high and the task can be performed using any two Bell states as the task can be reduced to the teleportation of an arbitrary two qubit state. Further, a trivial conceptual mistake made by Zhao et al., in the description of the quantum channel has been pointed out. It's also mentioned that recently a trend of proposing teleportation schemes with excessively high quantum resources has been observed and the essence of this comment is applicable to all such proposals.

Measurement-based quantum computation on two-body interacting qubits with adiabatic evolution.

PubMed

Kyaw, Thi Ha; Li, Ying; Kwek, Leong-Chuan

2014-10-31

A cluster state cannot be a unique ground state of a two-body interacting Hamiltonian. Here, we propose the creation of a cluster state of logical qubits encoded in spin-1/2 particles by adiabatically weakening two-body interactions. The proposal is valid for any spatial dimensional cluster states. Errors induced by thermal fluctuations and adiabatic evolution within finite time can be eliminated ensuring fault-tolerant quantum computing schemes.

Picking a Fight with Water, and Water Lost ... an Electron

NASA Astrophysics Data System (ADS)

Herr, Jonathan D.

The global need for energy is increasing, as is the importance of producing energy by green and renewable methodologies. This document outlines a research program dedicated to investigating a possible source for this form of energy generation and storage: solar fuels. The photon-induced splitting of water into molecular hydrogen and oxygen is currently hindered by large overpotentials from the oxidation half-reaction of water-splitting. This study concentrated on fundamental models of water-spitting chemistry, using a physical and computational chemistry analysis. The oxidation was first explored via ab initio electronic structure calculations of bare cationic water clusters, comprised of 2 to 21 molecules, in order to determine key electronic interactions that facilitate oxidation. Deeper understanding of these interactions could serve as guides for the development of viable water oxidation catalysts (WOC) designed to reduce overpotentials. The cationic water cluster study was followed by an investigation into hydrated copper (I) clusters, which acted as precursor models for real WOCs. Analyzing how the copper ion perturbed the properties of water clusters led to important electronic considerations for the development of WOCs, such as copper-water interactions that go beyond simple electrostatics. The importance of diagnostic thermodynamic properties, as well as anharmonic characteristics being persistent throughout oxidized water clusters, necessitated the use of quantum and classical molecular dynamics (MD) routines. Therefore, two new methods for accelerating computationally demanding classical and quantum MD methods were developed to increase their accessibility. The first method utilized a new form of electronic extrapolation - a linear prediction routine incorporating a Burg minimization - to decrease the iterations required for solving the electronic equations throughout the dynamics. The second method utilized a multiple-timestepping description of the potential energy term in the path integral molecular dynamics (PIMD) formalism. This method led to reductions of computational time by allowing the use of less computationally laborious methods for portions of the simulation and resulted in negligible increase of error. The determination of the fundamental driving forces within water oxidation and the development of acceleration techniques for important electronic structure methods will help drive progress into fully solar-initiated water oxidation.

High-speed linear optics quantum computing using active feed-forward.

PubMed

Prevedel, Robert; Walther, Philip; Tiefenbacher, Felix; Böhi, Pascal; Kaltenbaek, Rainer; Jennewein, Thomas; Zeilinger, Anton

2007-01-04

As information carriers in quantum computing, photonic qubits have the advantage of undergoing negligible decoherence. However, the absence of any significant photon-photon interaction is problematic for the realization of non-trivial two-qubit gates. One solution is to introduce an effective nonlinearity by measurements resulting in probabilistic gate operations. In one-way quantum computation, the random quantum measurement error can be overcome by applying a feed-forward technique, such that the future measurement basis depends on earlier measurement results. This technique is crucial for achieving deterministic quantum computation once a cluster state (the highly entangled multiparticle state on which one-way quantum computation is based) is prepared. Here we realize a concatenated scheme of measurement and active feed-forward in a one-way quantum computing experiment. We demonstrate that, for a perfect cluster state and no photon loss, our quantum computation scheme would operate with good fidelity and that our feed-forward components function with very high speed and low error for detected photons. With present technology, the individual computational step (in our case the individual feed-forward cycle) can be operated in less than 150 ns using electro-optical modulators. This is an important result for the future development of one-way quantum computers, whose large-scale implementation will depend on advances in the production and detection of the required highly entangled cluster states.

Cooling the Motion of Diamond Nanocrystals in a Magneto-Gravitational Trap in High Vacuum.

PubMed

Hsu, Jen-Feng; Ji, Peng; Lewandowski, Charles W; D'Urso, Brian

2016-07-22

Levitated diamond nanocrystals with nitrogen-vacancy (NV) centres in high vacuum have been proposed as a unique system for experiments in fundamental quantum mechanics, including the generation of large quantum superposition states and tests of quantum gravity. This system promises extreme isolation from its environment while providing quantum control and sensing through the NV centre spin. While optical trapping has been the most explored method of levitation, recent results indicate that excessive optical heating of the nanodiamonds under vacuum may make the method impractical with currently available materials. Here, we study an alternative magneto-gravitational trap for diamagnetic particles, such as diamond nanocrystals, with stable levitation from atmospheric pressure to high vacuum. Magnetic field gradients from permanent magnets confine the particle in two dimensions, while confinement in the third dimension is gravitational. We demonstrate that feedback cooling of the centre-of-mass motion of a trapped nanodiamond cluster results in cooling of one degree of freedom to less than 1 K.

Cooling the motion of diamond nanocrystals in a magneto-gravitational trap in high vacuum

DOE PAGES

Hsu, Jen -Feng; Ji, Peng; Lewandowski, Charles W.; ...

2016-07-22

Levitated diamond nanocrystals with nitrogen-vacancy (NV) centres in high vacuum have been proposed as a unique system for experiments in fundamental quantum mechanics, including the generation of large quantum superposition states and tests of quantum gravity. This system promises extreme isolation from its environment while providing quantum control and sensing through the NV centre spin. While optical trapping has been the most explored method of levitation, recent results indicate that excessive optical heating of the nanodiamonds under vacuum may make the method impractical with currently available materials. Here, we study an alternative magneto-gravitational trap for diamagnetic particles, such as diamondmore » nanocrystals, with stable levitation from atmospheric pressure to high vacuum. Magnetic field gradients from permanent magnets confine the particle in two dimensions, while confinement in the third dimension is gravitational. Furthermore, we demonstrate that feedback cooling of the centre-of-mass motion of a trapped nanodiamond cluster results in cooling of one degree of freedom to less than 1 K.« less

Cooling the Motion of Diamond Nanocrystals in a Magneto-Gravitational Trap in High Vacuum

PubMed Central

Hsu, Jen-Feng; Ji, Peng; Lewandowski, Charles W.; D’Urso, Brian

2016-01-01

Levitated diamond nanocrystals with nitrogen-vacancy (NV) centres in high vacuum have been proposed as a unique system for experiments in fundamental quantum mechanics, including the generation of large quantum superposition states and tests of quantum gravity. This system promises extreme isolation from its environment while providing quantum control and sensing through the NV centre spin. While optical trapping has been the most explored method of levitation, recent results indicate that excessive optical heating of the nanodiamonds under vacuum may make the method impractical with currently available materials. Here, we study an alternative magneto-gravitational trap for diamagnetic particles, such as diamond nanocrystals, with stable levitation from atmospheric pressure to high vacuum. Magnetic field gradients from permanent magnets confine the particle in two dimensions, while confinement in the third dimension is gravitational. We demonstrate that feedback cooling of the centre-of-mass motion of a trapped nanodiamond cluster results in cooling of one degree of freedom to less than 1 K. PMID:27444654

Quantum mechanical force field for hydrogen fluoride with explicit electronic polarization.

PubMed

Mazack, Michael J M; Gao, Jiali

2014-05-28

The explicit polarization (X-Pol) theory is a fragment-based quantum chemical method that explicitly models the internal electronic polarization and intermolecular interactions of a chemical system. X-Pol theory provides a framework to construct a quantum mechanical force field, which we have extended to liquid hydrogen fluoride (HF) in this work. The parameterization, called XPHF, is built upon the same formalism introduced for the XP3P model of liquid water, which is based on the polarized molecular orbital (PMO) semiempirical quantum chemistry method and the dipole-preserving polarization consistent point charge model. We introduce a fluorine parameter set for PMO, and find good agreement for various gas-phase results of small HF clusters compared to experiments and ab initio calculations at the M06-2X/MG3S level of theory. In addition, the XPHF model shows reasonable agreement with experiments for a variety of structural and thermodynamic properties in the liquid state, including radial distribution functions, interaction energies, diffusion coefficients, and densities at various state points.

N multipartite GHZ states in quantum networks

NASA Astrophysics Data System (ADS)

Caprara Vivoli, Valentina; Wehner, Stephanie

Nowadays progress in experimental quantum physics has brought to a significant control on systems like nitrogen-vacancy centres, ion traps, and superconducting qubit clusters. These systems can constitute the key cells of future quantum networks, where tasks like quantum communication at large scale and quantum cryptography can be achieved. It is, though, still not clear which approaches can be used to generate such entanglement at large distances using only local operations on or between at most two adjacent nodes. Here, we analyse three protocols that are able to generate genuine multipartite entanglement between an arbitrary large number of parties. In particular, we focus on the generation of the Greenberger-Horne-Zeilinger state. Moreover, the performances of the three methods are numerically compared in the scenario of a decoherence model both in terms of fidelity and entanglement generation rate. V.C.V. is founded by a NWO Vidi Grant, and S.W. is founded by STW Netherlands.

Generation of high-fidelity four-photon cluster state and quantum-domain demonstration of one-way quantum computing.

PubMed

Tokunaga, Yuuki; Kuwashiro, Shin; Yamamoto, Takashi; Koashi, Masato; Imoto, Nobuyuki

2008-05-30

We experimentally demonstrate a simple scheme for generating a four-photon entangled cluster state with fidelity over 0.860+/-0.015. We show that the fidelity is high enough to guarantee that the produced state is distinguished from Greenberger-Horne-Zeilinger, W, and Dicke types of genuine four-qubit entanglement. We also demonstrate basic operations of one-way quantum computing using the produced state and show that the output state fidelities surpass classical bounds, which indicates that the entanglement in the produced state essentially contributes to the quantum operation.

He-Ion Microscopy as a High-Resolution Probe for Complex Quantum Heterostructures in Core-Shell Nanowires.

PubMed

Pöpsel, Christian; Becker, Jonathan; Jeon, Nari; Döblinger, Markus; Stettner, Thomas; Gottschalk, Yeanitza Trujillo; Loitsch, Bernhard; Matich, Sonja; Altzschner, Marcus; Holleitner, Alexander W; Finley, Jonathan J; Lauhon, Lincoln J; Koblmüller, Gregor

2018-06-13

Core-shell semiconductor nanowires (NW) with internal quantum heterostructures are amongst the most complex nanostructured materials to be explored for assessing the ultimate capabilities of diverse ultrahigh-resolution imaging techniques. To probe the structure and composition of these materials in their native environment with minimal damage and sample preparation calls for high-resolution electron or ion microscopy methods, which have not yet been tested on such classes of ultrasmall quantum nanostructures. Here, we demonstrate that scanning helium ion microscopy (SHeIM) provides a powerful and straightforward method to map quantum heterostructures embedded in complex III-V semiconductor NWs with unique material contrast at ∼1 nm resolution. By probing the cross sections of GaAs-Al(Ga)As core-shell NWs with coaxial GaAs quantum wells as well as short-period GaAs/AlAs superlattice (SL) structures in the shell, the Al-rich and Ga-rich layers are accurately discriminated by their image contrast in excellent agreement with correlated, yet destructive, scanning transmission electron microscopy and atom probe tomography analysis. Most interestingly, quantitative He-ion dose-dependent SHeIM analysis of the ternary AlGaAs shell layers and of compositionally nonuniform GaAs/AlAs SLs reveals distinct alloy composition fluctuations in the form of Al-rich clusters with size distributions between ∼1-10 nm. In the GaAs/AlAs SLs the alloy clustering vanishes with increasing SL-period (>5 nm-GaAs/4 nm-AlAs), providing insights into critical size dimensions for atomic intermixing effects in short-period SLs within a NW geometry. The straightforward SHeIM technique therefore provides unique benefits in imaging the tiniest nanoscale features in topography, structure and composition of a multitude of diverse complex semiconductor nanostructures.

Sampling Molecular Conformers in Solution with Quantum Mechanical Accuracy at a Nearly Molecular-Mechanics Cost.

PubMed

Rosa, Marta; Micciarelli, Marco; Laio, Alessandro; Baroni, Stefano

2016-09-13

We introduce a method to evaluate the relative populations of different conformers of molecular species in solution, aiming at quantum mechanical accuracy, while keeping the computational cost at a nearly molecular-mechanics level. This goal is achieved by combining long classical molecular-dynamics simulations to sample the free-energy landscape of the system, advanced clustering techniques to identify the most relevant conformers, and thermodynamic perturbation theory to correct the resulting populations, using quantum-mechanical energies from density functional theory. A quantitative criterion for assessing the accuracy thus achieved is proposed. The resulting methodology is demonstrated in the specific case of cyanin (cyanidin-3-glucoside) in water solution.

Anionic water pentamer and hexamer clusters: An extensive study of structures and energetics

NASA Astrophysics Data System (ADS)

Ünal, Aslı; Bozkaya, Uǧur

2018-03-01

An extensive study of structures and energetics for anionic pentamer and hexamer clusters is performed employing high level ab initio quantum chemical methods, such as the density-fitted orbital-optimized linearized coupled-cluster doubles (DF-OLCCD), coupled-cluster singles and doubles (CCSD), and coupled-cluster singles and doubles with perturbative triples [CCSD(T)] methods. In this study, sixteen anionic pentamer clusters and eighteen anionic hexamer clusters are reported. Relative, binding, and vertical detachment energies (VDE) are presented at the complete basis set limit (CBS), extrapolating energies of aug4-cc-pVTZ and aug4-cc-pVQZ custom basis sets. The largest VDE values obtained at the CCSD(T)/CBS level are 9.9 and 11.2 kcal mol-1 for pentamers and hexamers, respectively, which are in very good agreement with the experimental values of 9.5 and 11.1 kcal mol-1. Our binding energy results, at the CCSD(T)/CBS level, indicate strong bindings in anionic clusters due to hydrogen bond interactions. The average binding energy per water molecules is -5.0 and -5.3 kcal mol-1 for pentamers and hexamers, respectively. Furthermore, our results demonstrate that the DF-OLCCD method approaches to the CCSD(T) quality for anionic clusters. The inexpensive analytic gradients of DF-OLCCD compared to CCSD or CCSD(T) make it very attractive for high-accuracy studies.

Anionic water pentamer and hexamer clusters: An extensive study of structures and energetics.

PubMed

Ünal, Aslı; Bozkaya, Uğur

2018-03-28

An extensive study of structures and energetics for anionic pentamer and hexamer clusters is performed employing high level ab initio quantum chemical methods, such as the density-fitted orbital-optimized linearized coupled-cluster doubles (DF-OLCCD), coupled-cluster singles and doubles (CCSD), and coupled-cluster singles and doubles with perturbative triples [CCSD(T)] methods. In this study, sixteen anionic pentamer clusters and eighteen anionic hexamer clusters are reported. Relative, binding, and vertical detachment energies (VDE) are presented at the complete basis set limit (CBS), extrapolating energies of aug4-cc-pVTZ and aug4-cc-pVQZ custom basis sets. The largest VDE values obtained at the CCSD(T)/CBS level are 9.9 and 11.2 kcal mol -1 for pentamers and hexamers, respectively, which are in very good agreement with the experimental values of 9.5 and 11.1 kcal mol -1 . Our binding energy results, at the CCSD(T)/CBS level, indicate strong bindings in anionic clusters due to hydrogen bond interactions. The average binding energy per water molecules is -5.0 and -5.3 kcal mol -1 for pentamers and hexamers, respectively. Furthermore, our results demonstrate that the DF-OLCCD method approaches to the CCSD(T) quality for anionic clusters. The inexpensive analytic gradients of DF-OLCCD compared to CCSD or CCSD(T) make it very attractive for high-accuracy studies.

Closed-cage tungsten oxide clusters in the gas phase.

PubMed

Singh, D M David Jeba; Pradeep, T; Thirumoorthy, Krishnan; Balasubramanian, Krishnan

2010-05-06

During the course of a study on the clustering of W-Se and W-S mixtures in the gas phase using laser desorption ionization (LDI) mass spectrometry, we observed several anionic W-O clusters. Three distinct species, W(6)O(19)(-), W(13)O(29)(-), and W(14)O(32)(-), stand out as intense peaks in the regular mass spectral pattern of tungsten oxide clusters suggesting unusual stabilities for them. Moreover, these clusters do not fragment in the postsource decay analysis. While trying to understand the precursor material, which produced these clusters, we found the presence of nanoscale forms of tungsten oxide. The structure and thermodynamic parameters of tungsten clusters have been explored using relativistic quantum chemical methods. Our computed results of atomization energy are consistent with the observed LDI mass spectra. The computational results suggest that the clusters observed have closed-cage structure. These distinct W(13) and W(14) clusters were observed for the first time in the gas phase.

Investigation of electronic structure of tri- and tetranuclear molybdenum clusters by X-ray photoelectron and emission spectroscopies and quantum chemical methods

NASA Astrophysics Data System (ADS)

Kryuchkova, Natalya A.; Syrokvashin, Mikhail M.; Gushchin, Artem L.; Korotaev, Evgeniy V.; Kalinkin, Alexander V.; Laricheva, Yuliya A.; Sokolov, Maxim N.

2018-02-01

Charge state studies of compounds [Mo3S4(tu)8(H2O)]Cl4·4H2O (1), [Mo3S4Cl3(dbbpy)3]Cl·5H2O (2), [Mo3S4(CuCl)Cl3(dbbpy)3][CuCl2] (3), containing {Mo3S4}4+ and {Mo3CuS4}5+ cluster cores bearing terminal thiourea (tu) or 4,4‧-di-tert-butyl-2,2‧-bipyridine (dbbpy) ligands, have been performed by X-ray photoelectron and X-ray emission spectroscopies combined with quantum chemical calculations. The best agreement between theory and experiments has been obtained using the B3LYP method. According to the experimental and calculated data, the Mo atoms are in the oxidation state 4+ for all compounds. The energies and shapes of the Cu2p lines indicate formal oxidation states of Cu as 1+. The coordination of Cu(I) to the cluster {Mo3S4} in 3 does not lead to significant changes in the charge state of the molybdenum atoms and the {Mo3S4} unit can be considered as a tridentate metallothia crown ether.

Quantum mechanics capacitance molecular mechanics modeling of core-electron binding energies of methanol and methyl nitrite on Ag(111) surface.

PubMed

Löytynoja, T; Li, X; Jänkälä, K; Rinkevicius, Z; Ågren, H

2016-07-14

We study a newly devised quantum mechanics capacitance molecular mechanics (QMCMM) method for the calculation of core-electron binding energies in the case of molecules adsorbed on metal surfaces. This yet untested methodology is applied to systems with monolayer of methanol/methyl nitrite on an Ag(111) surface at 100 K temperature. It was found out that the studied C, N, and O 1s core-hole energies converge very slowly as a function of the radius of the metallic cluster, which was ascribed to build up of positive charge on the edge of the Ag slab. Further analysis revealed that an extrapolation process can be used to obtain binding energies that deviated less than 0.5 eV against experiments, except in the case of methanol O 1s where the difference was as large as 1.8 eV. Additional QM-cluster calculations suggest that the latter error can be connected to the lack of charge transfer over the QM-CMM boundary. Thus, the results indicate that the QMCMM and QM-cluster methods can complement each other in a holistic picture of molecule-adsorbate core-ionization studies, where all types of intermolecular interactions are considered.

Quantum mechanics capacitance molecular mechanics modeling of core-electron binding energies of methanol and methyl nitrite on Ag(111) surface

NASA Astrophysics Data System (ADS)

Löytynoja, T.; Li, X.; Jänkälä, K.; Rinkevicius, Z.; Ågren, H.

2016-07-01

We study a newly devised quantum mechanics capacitance molecular mechanics (QMCMM) method for the calculation of core-electron binding energies in the case of molecules adsorbed on metal surfaces. This yet untested methodology is applied to systems with monolayer of methanol/methyl nitrite on an Ag(111) surface at 100 K temperature. It was found out that the studied C, N, and O 1s core-hole energies converge very slowly as a function of the radius of the metallic cluster, which was ascribed to build up of positive charge on the edge of the Ag slab. Further analysis revealed that an extrapolation process can be used to obtain binding energies that deviated less than 0.5 eV against experiments, except in the case of methanol O 1s where the difference was as large as 1.8 eV. Additional QM-cluster calculations suggest that the latter error can be connected to the lack of charge transfer over the QM-CMM boundary. Thus, the results indicate that the QMCMM and QM-cluster methods can complement each other in a holistic picture of molecule-adsorbate core-ionization studies, where all types of intermolecular interactions are considered.

Critical behavior of the quantum spin- {1}/{2} anisotropic Heisenberg model

NASA Astrophysics Data System (ADS)

Sousa, J. Ricardo de

A two-step renormalization group approach - a decimation followed by an effective field renormalization group (EFRG) - is proposed in this work to study the critical behavior of the quantum spin- {1}/{2} anisotropic Heisenberg model. The new method is illustrated by employing approximations in which clusters with one, two and three spins are used. The values of the critical parameter and critical exponent, in two- and three-dimensional lattices, for the Ising and isotropic Heisenberg limits are calculated and compared with other renormalization group approaches and exact (or series) results.

The quantum structure of anionic hydrogen clusters

NASA Astrophysics Data System (ADS)

Calvo, F.; Yurtsever, E.

2018-03-01

A flexible and polarizable interatomic potential has been developed to model hydrogen clusters interacting with one hydrogen anion, (H2)nH-, in a broad range of sizes n = 1-54 and parametrized against coupled cluster quantum chemical calculations. Using path-integral molecular dynamics simulations at 1 K initiated from the putative classical global minima, the equilibrium structures are found to generally rely on icosahedral shells with the hydrogen molecules pointing toward the anion, producing geometric magic numbers at sizes n = 12, 32, and 44 that are in agreement with recent mass spectrometry measurements. The energetic stability of the clusters is also connected with the extent of vibrational delocalization, measured here by the fluctuations among inherent structures hidden in the vibrational wave function. As the clusters grow, the outer molecules become increasingly free to rotate, and strong finite size effects are also found between magic numbers, associated with more prominent vibrational delocalization. The effective icosahedral structure of the 44-molecule cluster is found to originate from quantum nuclear effects as well, the classical structure showing no particular symmetry.

Kelvin-Helmholtz instability in a single-component atomic superfluid

NASA Astrophysics Data System (ADS)

Baggaley, A. W.; Parker, N. G.

2018-05-01

We demonstrate an experimentally feasible method for generating the classical Kelvin-Helmholtz instability in a single-component atomic Bose-Einstein condensate. By progressively reducing a potential barrier between two counterflowing channels, we seed a line of quantized vortices, which precede to form progressively larger clusters, mimicking the classical roll-up behavior of the Kelvin-Helmholtz instability. This cluster formation leads to an effective superfluid shear layer, formed through the collective motion of many quantized vortices. From this we demonstrate a straightforward method to measure the effective viscosity of a turbulent quantum fluid in a system with a moderate number of vortices, within the range of current experimental capabilities.

Quantum chemical study of the structure, spectroscopy and reactivity of NO+.(H2O) n=1-5 clusters.

PubMed

Linton, Kirsty A; Wright, Timothy G; Besley, Nicholas A

2018-03-13

Quantum chemical methods including Møller-Plesset perturbation (MP2) theory and density functional theory (DFT) have been used to study the structure, spectroscopy and reactivity of NO + (H 2 O) n =1-5 clusters. MP2/6-311++G** calculations are shown to describe the structure and spectroscopy of the clusters well. DFT calculations with exchange-correlation functionals with a low fraction of Hartree-Fock exchange give a binding energy of NO + (H 2 O) that is too high and incorrectly predict the lowest energy structure of NO + (H 2 O) 2 , and this error may be associated with a delocalization of charge onto the water molecule directly binding to NO + Ab initio molecular dynamics (AIMD) simulations were performed to study the NO + (H 2 O) 5 [Formula: see text] H + (H 2 O) 4 + HONO reaction to investigate the formation of HONO from NO + (H 2 O) 5 Whether an intracluster reaction to form HONO is observed depends on the level of electronic structure theory used. Of note is that methods that accurately describe the relative energies of the product and reactant clusters did not show reactions on the timescales studied. This suggests that in the upper atmosphere the reaction may occur owing to the energy present in the NO + (H 2 O) 5 complex following its formation.This article is part of the theme issue 'Modern theoretical chemistry'. © 2018 The Author(s).

Perspective: Quantum mechanical methods in biochemistry and biophysics.

PubMed

Cui, Qiang

2016-10-14

In this perspective article, I discuss several research topics relevant to quantum mechanical (QM) methods in biophysical and biochemical applications. Due to the immense complexity of biological problems, the key is to develop methods that are able to strike the proper balance of computational efficiency and accuracy for the problem of interest. Therefore, in addition to the development of novel ab initio and density functional theory based QM methods for the study of reactive events that involve complex motifs such as transition metal clusters in metalloenzymes, it is equally important to develop inexpensive QM methods and advanced classical or quantal force fields to describe different physicochemical properties of biomolecules and their behaviors in complex environments. Maintaining a solid connection of these more approximate methods with rigorous QM methods is essential to their transferability and robustness. Comparison to diverse experimental observables helps validate computational models and mechanistic hypotheses as well as driving further development of computational methodologies.

Quantum chemistry of the minimal CdSe clusters

NASA Astrophysics Data System (ADS)

Yang, Ping; Tretiak, Sergei; Masunov, Artëm E.; Ivanov, Sergei

2008-08-01

Colloidal quantum dots are semiconductor nanocrystals (NCs) which have stimulated a great deal of research and have attracted technical interest in recent years due to their chemical stability and the tunability of photophysical properties. While internal structure of large quantum dots is similar to bulk, their surface structure and passivating role of capping ligands (surfactants) are not fully understood to date. We apply ab initio wavefunction methods, density functional theory, and semiempirical approaches to study the passivation effects of substituted phosphine and amine ligands on the minimal cluster Cd2Se2, which is also used to benchmark different computational methods versus high level ab initio techniques. Full geometry optimization of Cd2Se2 at different theory levels and ligand coverage is used to understand the affinities of various ligands and the impact of ligands on cluster structure. Most possible bonding patterns between ligands and surface Cd/Se atoms are considered, including a ligand coordinated to Se atoms. The degree of passivation of Cd and Se atoms (one or two ligands attached to one atom) is also studied. The results suggest that B3LYP/LANL2DZ level of theory is appropriate for the system modeling, whereas frequently used semiempirical methods (such as AM1 and PM3) produce unphysical results. The use of hydrogen atom for modeling of the cluster passivating ligands is found to yield unphysical results as well. Hence, the surface termination of II-VI semiconductor NCs with hydrogen atoms often used in computational models should probably be avoided. Basis set superposition error, zero-point energy, and thermal corrections, as well as solvent effects simulated with polarized continuum model are found to produce minor variations on the ligand binding energies. The effects of Cd-Se complex structure on both the electronic band gap (highest occupied molecular orbital-lowest unoccupied molecular orbital energy difference) and ligand binding energies are systematically examined. The role played by positive charges on ligand binding is also explored. The calculated binding energies for various ligands L are found to decrease in the order OPMe3>OPH3>NH2Me>=NH3>=NMe3>PMe3>PH3 for neutral clusters and OPMe3>OPH3>PMe3>=NMe3>=NH2Me>=NH3>PH3 and OPMe3>OPH3>NH2Me>=NMe3>=PMe3>=NH3>PH3 for single and double ligations of positively charged Cd2Se22+ cluster, respectively.

Quantum chemical calculations in the structural analysis of phloretin

NASA Astrophysics Data System (ADS)

Gómez-Zavaglia, Andrea

2009-07-01

In this work, a conformational search on the molecule of phloretin [2',4',6'-Trihydroxy-3-(4-hydroxyphenyl)-propiophenone] has been performed. The molecule of phloretin has eight dihedral angles, four of them taking part in the carbon backbone and the other four, related with the orientation of the hydroxyl groups. A systematic search involving a random variation of the dihedral angles has been used to generate input structures for the quantum chemical calculations. Calculations at the DFT(B3LYP)/6-311++G(d,p) level of theory permitted the identification of 58 local minima belonging to the C 1 symmetry point group. The molecular structures of the conformers have been analyzed using hierarchical cluster analysis. This method allowed us to group conformers according to their similarities, and thus, to correlate the conformers' stability with structural parameters. The dendrogram obtained from the hierarchical cluster analysis depicted two main clusters. Cluster I included all the conformers with relative energies lower than 25 kJ mol -1 and cluster II, the remaining conformers. The possibility of forming intramolecular hydrogen bonds resulted the main factor contributing for the stability. Accordingly, all conformers depicting intramolecular H-bonds belong to cluster I. These conformations are clearly favored when the carbon backbone is as planar as possible. The values of the νC dbnd O and νOH vibrational modes were compared among all the conformers of phloretin. The redshifts associated with intramolecular H-bonds were correlated with the H-bonds distances and energies.

Singlet-paired coupled cluster theory for open shells

NASA Astrophysics Data System (ADS)

Gomez, John A.; Henderson, Thomas M.; Scuseria, Gustavo E.

2016-06-01

Restricted single-reference coupled cluster theory truncated to single and double excitations accurately describes weakly correlated systems, but often breaks down in the presence of static or strong correlation. Good coupled cluster energies in the presence of degeneracies can be obtained by using a symmetry-broken reference, such as unrestricted Hartree-Fock, but at the cost of good quantum numbers. A large body of work has shown that modifying the coupled cluster ansatz allows for the treatment of strong correlation within a single-reference, symmetry-adapted framework. The recently introduced singlet-paired coupled cluster doubles (CCD0) method is one such model, which recovers correct behavior for strong correlation without requiring symmetry breaking in the reference. Here, we extend singlet-paired coupled cluster for application to open shells via restricted open-shell singlet-paired coupled cluster singles and doubles (ROCCSD0). The ROCCSD0 approach retains the benefits of standard coupled cluster theory and recovers correct behavior for strongly correlated, open-shell systems using a spin-preserving ROHF reference.

Quantum lattice model solver HΦ

NASA Astrophysics Data System (ADS)

Kawamura, Mitsuaki; Yoshimi, Kazuyoshi; Misawa, Takahiro; Yamaji, Youhei; Todo, Synge; Kawashima, Naoki

2017-08-01

HΦ [aitch-phi ] is a program package based on the Lanczos-type eigenvalue solution applicable to a broad range of quantum lattice models, i.e., arbitrary quantum lattice models with two-body interactions, including the Heisenberg model, the Kitaev model, the Hubbard model and the Kondo-lattice model. While it works well on PCs and PC-clusters, HΦ also runs efficiently on massively parallel computers, which considerably extends the tractable range of the system size. In addition, unlike most existing packages, HΦ supports finite-temperature calculations through the method of thermal pure quantum (TPQ) states. In this paper, we explain theoretical background and user-interface of HΦ. We also show the benchmark results of HΦ on supercomputers such as the K computer at RIKEN Advanced Institute for Computational Science (AICS) and SGI ICE XA (Sekirei) at the Institute for the Solid State Physics (ISSP).

Improvements of Quantum Private Comparison Protocol Based on Cluster States

NASA Astrophysics Data System (ADS)

Zhou, Ming-Kuai

2018-01-01

Quantum private comparison aims to determine whether the secrets from two different users are equal or not by utilizing the laws of quantum mechanics. Recently, Sun and Long put forward a quantum private comparison (QPC) protocol by using four-particle cluster states (Int. J. Theor. Phys. 52, 212-218, 2013). In this paper, we investigate this protocol in depth, and suggest the corresponding improvements. Compared with the original protocol, the improved protocol has the following advantages: 1) it can release the requirements of authenticated classical channels and unitary operations; 2) it can prevent the malicious attack from the genuine semi-honest TP; 3) it can enhance the qubit efficiency.

Quantum annealing for combinatorial clustering

NASA Astrophysics Data System (ADS)

Kumar, Vaibhaw; Bass, Gideon; Tomlin, Casey; Dulny, Joseph

2018-02-01

Clustering is a powerful machine learning technique that groups "similar" data points based on their characteristics. Many clustering algorithms work by approximating the minimization of an objective function, namely the sum of within-the-cluster distances between points. The straightforward approach involves examining all the possible assignments of points to each of the clusters. This approach guarantees the solution will be a global minimum; however, the number of possible assignments scales quickly with the number of data points and becomes computationally intractable even for very small datasets. In order to circumvent this issue, cost function minima are found using popular local search-based heuristic approaches such as k-means and hierarchical clustering. Due to their greedy nature, such techniques do not guarantee that a global minimum will be found and can lead to sub-optimal clustering assignments. Other classes of global search-based techniques, such as simulated annealing, tabu search, and genetic algorithms, may offer better quality results but can be too time-consuming to implement. In this work, we describe how quantum annealing can be used to carry out clustering. We map the clustering objective to a quadratic binary optimization problem and discuss two clustering algorithms which are then implemented on commercially available quantum annealing hardware, as well as on a purely classical solver "qbsolv." The first algorithm assigns N data points to K clusters, and the second one can be used to perform binary clustering in a hierarchical manner. We present our results in the form of benchmarks against well-known k-means clustering and discuss the advantages and disadvantages of the proposed techniques.

Description of an α-cluster tail in 8Be and 20Ne: Delocalization of the α cluster by quantum penetration

NASA Astrophysics Data System (ADS)

Kanada-En'yo, Yoshiko

2014-10-01

We analyze the α-cluster wave functions in cluster states of ^8Be and ^{20}Ne by comparing the exact relative wave function obtained by the generator coordinate method (GCM) with various types of trial functions. For the trial functions, we adopt the fixed range shifted Gaussian of the Brink-Bloch (BB) wave function, the spherical Gaussian with the adjustable range parameter of the spherical Tohsaki-Horiuchi-Schuck-Röpke (sTHSR), the deformed Gaussian of the deformed THSR (dTHSR), and a function with the Yukawa tail (YT). The quality of the description of the exact wave function with a trial function is judged by the squared overlap between the trial function and the GCM wave function. A better result is obtained with the sTHSR wave function than the BB wave function, and further improvement can be made with the dTHSR wave function because these wave functions can describe the outer tail better. The YT wave function gives almost an equal quality to or even better quality than the dTHSR wave function, indicating that the outer tail of α-cluster states is characterized by the Yukawa-like tail rather than the Gaussian tail. In weakly bound α-cluster states with small α separation energy and the low centrifugal and Coulomb barriers, the outer tail part is the slowly damping function described well by the quantum penetration through the effective barrier. This outer tail characterizes the almost zero-energy free α gas behavior, i.e., the delocalization of the cluster.

Five-wave-packet quantum error correction based on continuous-variable cluster entanglement

PubMed Central

Hao, Shuhong; Su, Xiaolong; Tian, Caixing; Xie, Changde; Peng, Kunchi

2015-01-01

Quantum error correction protects the quantum state against noise and decoherence in quantum communication and quantum computation, which enables one to perform fault-torrent quantum information processing. We experimentally demonstrate a quantum error correction scheme with a five-wave-packet code against a single stochastic error, the original theoretical model of which was firstly proposed by S. L. Braunstein and T. A. Walker. Five submodes of a continuous variable cluster entangled state of light are used for five encoding channels. Especially, in our encoding scheme the information of the input state is only distributed on three of the five channels and thus any error appearing in the remained two channels never affects the output state, i.e. the output quantum state is immune from the error in the two channels. The stochastic error on a single channel is corrected for both vacuum and squeezed input states and the achieved fidelities of the output states are beyond the corresponding classical limit. PMID:26498395

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nielsen, Michael A.; School of Information Technology and Electrical Engineering, University of Queensland, Brisbane, Queensland 4072; Dawson, Christopher M.

The one-way quantum computing model introduced by Raussendorf and Briegel [Phys. Rev. Lett. 86, 5188 (2001)] shows that it is possible to quantum compute using only a fixed entangled resource known as a cluster state, and adaptive single-qubit measurements. This model is the basis for several practical proposals for quantum computation, including a promising proposal for optical quantum computation based on cluster states [M. A. Nielsen, Phys. Rev. Lett. (to be published), quant-ph/0402005]. A significant open question is whether such proposals are scalable in the presence of physically realistic noise. In this paper we prove two threshold theorems which showmore » that scalable fault-tolerant quantum computation may be achieved in implementations based on cluster states, provided the noise in the implementations is below some constant threshold value. Our first threshold theorem applies to a class of implementations in which entangling gates are applied deterministically, but with a small amount of noise. We expect this threshold to be applicable in a wide variety of physical systems. Our second threshold theorem is specifically adapted to proposals such as the optical cluster-state proposal, in which nondeterministic entangling gates are used. A critical technical component of our proofs is two powerful theorems which relate the properties of noisy unitary operations restricted to act on a subspace of state space to extensions of those operations acting on the entire state space. We expect these theorems to have a variety of applications in other areas of quantum-information science.« less

INTERDISCIPLINARY PHYSICS AND RELATED AREAS OF SCIENCE AND TECHNOLOGY: Efficient One-Step Generation of Cluster State with Charge Qubits in Circuit QED

NASA Astrophysics Data System (ADS)

Wang, Yi-Min; Li, Cheng-Zu

2010-01-01

We propose theoretical schemes to generate highly entangled cluster state with superconducting qubits in a circuit QED architecture. Charge qubits are located inside a superconducting transmission line, which serves as a quantum data bus. We show that large clusters state can be efficiently generated in just one step with the long-range Ising-like unitary operators. The quantum operations which are generally realized by two coupling mechanisms: either voltage coupling or current coupling, depend only on global geometric features and are insensitive not only to the thermal state of the transmission line but also to certain random operation errors. Thus high-fidelity one-way quantum computation can be achieved.

Parallelized traveling cluster approximation to study numerically spin-fermion models on large lattices

NASA Astrophysics Data System (ADS)

Mukherjee, Anamitra; Patel, Niravkumar D.; Bishop, Chris; Dagotto, Elbio

2015-06-01

Lattice spin-fermion models are important to study correlated systems where quantum dynamics allows for a separation between slow and fast degrees of freedom. The fast degrees of freedom are treated quantum mechanically while the slow variables, generically referred to as the "spins," are treated classically. At present, exact diagonalization coupled with classical Monte Carlo (ED + MC) is extensively used to solve numerically a general class of lattice spin-fermion problems. In this common setup, the classical variables (spins) are treated via the standard MC method while the fermion problem is solved by exact diagonalization. The "traveling cluster approximation" (TCA) is a real space variant of the ED + MC method that allows to solve spin-fermion problems on lattice sizes with up to 103 sites. In this publication, we present a novel reorganization of the TCA algorithm in a manner that can be efficiently parallelized. This allows us to solve generic spin-fermion models easily on 104 lattice sites and with some effort on 105 lattice sites, representing the record lattice sizes studied for this family of models.

Coexpression of CdSe and CdSe/CdS quantum dots in live cells using molecular hyperspectral imaging technology

NASA Astrophysics Data System (ADS)

Li, Qingli; Peng, Hui; Wang, Jing; Wang, Yiting; Guo, Fangmin

2015-11-01

A direct spatial and spectral observation of CdSe and CdSe/CdS quantum dots (QDs) as probes in live cells is performed by using a custom molecular hyperspectral imaging (MHI) system. Water-soluble CdSe and CdSe/CdS QDs are synthesized in aqueous solution under the assistance of high-intensity ultrasonic irradiation and incubated with colon cancer cells for bioimaging. Unlike the traditional fluorescence microscopy methods, MHI technology can identify QD probes according to their spectral signatures and generate coexpression and stain titer maps by a clustering method. The experimental results show that the MHI method has potential to unmix biomarkers by their spectral information, which opens up a pathway of optical multiplexing with many different QD probes.

Semiconductor nanocrystals covalently bound to solid inorganic surfaces using self-assembled monolayers

DOEpatents

Alivisatos, A. Paul; Colvin, Vicki L.

1998-01-01

Methods are described for attaching semiconductor nanocrystals to solid inorganic surfaces, using self-assembled bifunctional organic monolayers as bridge compounds. Two different techniques are presented. One relies on the formation of self-assembled monolayers on these surfaces. When exposed to solutions of nanocrystals, these bridge compounds bind the crystals and anchor them to the surface. The second technique attaches nanocrystals already coated with bridge compounds to the surfaces. Analyses indicate the presence of quantum confined clusters on the surfaces at the nanolayer level. These materials allow electron spectroscopies to be completed on condensed phase clusters, and represent a first step towards synthesis of an organized assembly of clusters. These new products are also disclosed.

Few-Photon Model of the Optical Emission of Semiconductor Quantum Dots

NASA Astrophysics Data System (ADS)

Richter, Marten; Carmele, Alexander; Sitek, Anna; Knorr, Andreas

2009-08-01

The Jaynes-Cummings model provides a well established theoretical framework for single electron two level systems in a radiation field. Similar exactly solvable models for semiconductor light emitters such as quantum dots dominated by many particle interactions are not known. We access these systems by a generalized cluster expansion, the photon-probability cluster expansion: a reliable approach for few-photon dynamics in many body electron systems. As a first application, we discuss vacuum Rabi oscillations and show that their amplitude determines the number of electrons in the quantum dot.

Theory of few photon dynamics in light emitting quantum dot devices

NASA Astrophysics Data System (ADS)

Carmele, Alexander; Richter, Marten; Sitek, Anna; Knorr, Andreas

2009-10-01

We present a modified cluster expansion to describe single-photon emitters in a semiconductor environment. We calculate microscopically to what extent semiconductor features in quantum dot-wetting layer systems alter the exciton and photon dynamics in comparison to the atom-like emission dynamics. We access these systems by the photon-probability-cluster-expansion: a reliable approach for few photon dynamics in many body electron systems. As a first application, we show that the amplitude of vacuum Rabi flops determines the number of electrons in the quantum dot.

Two-step entanglement concentration for arbitrary electronic cluster state

NASA Astrophysics Data System (ADS)

Zhao, Sheng-Yang; Liu, Jiong; Zhou, Lan; Sheng, Yu-Bo

2013-12-01

We present an efficient protocol for concentrating an arbitrary four-electron less-entangled cluster state into a maximally entangled cluster state. As a two-step entanglement concentration protocol (ECP), it only needs one pair of less-entangled cluster state, which makes this ECP more economical. With the help of electronic polarization beam splitter (PBS) and the charge detection, the whole concentration process is essentially the quantum nondemolition (QND) measurement. Therefore, the concentrated maximally entangled state can be remained for further application. Moreover, the discarded terms in some traditional ECPs can be reused to obtain a high success probability. It is feasible and useful in current one-way quantum computation.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gomez, John A.; Henderson, Thomas M.; Scuseria, Gustavo E.

Restricted single-reference coupled cluster theory truncated to single and double excitations accurately describes weakly correlated systems, but often breaks down in the presence of static or strong correlation. Good coupled cluster energies in the presence of degeneracies can be obtained by using a symmetry-broken reference, such as unrestricted Hartree-Fock, but at the cost of good quantum numbers. A large body of work has shown that modifying the coupled cluster ansatz allows for the treatment of strong correlation within a single-reference, symmetry-adapted framework. The recently introduced singlet-paired coupled cluster doubles (CCD0) method is one such model, which recovers correct behavior formore » strong correlation without requiring symmetry breaking in the reference. Here, we extend singlet-paired coupled cluster for application to open shells via restricted open-shell singlet-paired coupled cluster singles and doubles (ROCCSD0). The ROCCSD0 approach retains the benefits of standard coupled cluster theory and recovers correct behavior for strongly correlated, open-shell systems using a spin-preserving ROHF reference.« less

A noniterative asymmetric triple excitation correction for the density-fitted coupled-cluster singles and doubles method: Preliminary applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bozkaya, Uğur, E-mail: ugrbzky@gmail.com

2016-04-14

An efficient implementation of the asymmetric triples correction for the coupled-cluster singles and doubles [ΛCCSD(T)] method [S. A. Kucharski and R. J. Bartlett, J. Chem. Phys. 108, 5243 (1998); T. D. Crawford and J. F. Stanton, Int. J. Quantum Chem. 70, 601 (1998)] with the density-fitting [DF-ΛCCSD(T)] approach is presented. The computational time for the DF-ΛCCSD(T) method is compared with that of ΛCCSD(T). Our results demonstrate that the DF-ΛCCSD(T) method provide substantially lower computational costs than ΛCCSD(T). Further application results show that the ΛCCSD(T) and DF-ΛCCSD(T) methods are very beneficial for the study of single bond breaking problems as wellmore » as noncovalent interactions and transition states. We conclude that ΛCCSD(T) and DF-ΛCCSD(T) are very promising for the study of challenging chemical systems, where the coupled-cluster singles and doubles with perturbative triples method fails.« less

Quantum Teleportation of a Three-qubit State using a Five-qubit Cluster State

NASA Astrophysics Data System (ADS)

Liu, Zhong-min; Zhou, Lin

2014-12-01

Recently Muralidharan and Panigrahi (Phys. Rev. A 78, 062333 2008) had shown that using a five-qubit cluster state as quantum channel, it is possible to teleport an arbitrary single-qubit state and an arbitrary two-qubit state. In this paper, we investigate this channel for the teleportation of a special form of three-qubit state.

Quantum teleportation and information splitting via four-qubit cluster state and a Bell state

NASA Astrophysics Data System (ADS)

Ramírez, Marlon David González; Falaye, Babatunde James; Sun, Guo-Hua; Cruz-Irisson, M.; Dong, Shi-Hai

2017-10-01

Quantum teleportation provides a "bodiless" way of transmitting the quantum state from one object to another, at a distant location, using a classical communication channel and a previously shared entangled state. In this paper, we present a tripartite scheme for probabilistic teleportation of an arbitrary single qubit state, without losing the information of the state being teleported, via a fourqubit cluster state of the form | ϕ>1234 = α|0000>+ β|1010>+ γ|0101>- η|1111>, as the quantum channel, where the nonzero real numbers α, β, γ, and η satisfy the relation j αj2 + | β|2 + | γ|2 + | η|2 = 1. With the introduction of an auxiliary qubit with state |0>, using a suitable unitary transformation and a positive-operator valued measure (POVM), the receiver can recreate the state of the original qubit. An important advantage of the teleportation scheme demonstrated here is that, if the teleportation fails, it can be repeated without teleporting copies of the unknown quantum state, if the concerned parties share another pair of entangled qubit. We also present a protocol for quantum information splitting of an arbitrary two-particle system via the aforementioned cluster state and a Bell-state as the quantum channel. Problems related to security attacks were examined for both the cases and it was found that this protocol is secure. This protocol is highly efficient and easy to implement.

Entanglement-Based Machine Learning on a Quantum Computer

NASA Astrophysics Data System (ADS)

Cai, X.-D.; Wu, D.; Su, Z.-E.; Chen, M.-C.; Wang, X.-L.; Li, Li; Liu, N.-L.; Lu, C.-Y.; Pan, J.-W.

2015-03-01

Machine learning, a branch of artificial intelligence, learns from previous experience to optimize performance, which is ubiquitous in various fields such as computer sciences, financial analysis, robotics, and bioinformatics. A challenge is that machine learning with the rapidly growing "big data" could become intractable for classical computers. Recently, quantum machine learning algorithms [Lloyd, Mohseni, and Rebentrost, arXiv.1307.0411] were proposed which could offer an exponential speedup over classical algorithms. Here, we report the first experimental entanglement-based classification of two-, four-, and eight-dimensional vectors to different clusters using a small-scale photonic quantum computer, which are then used to implement supervised and unsupervised machine learning. The results demonstrate the working principle of using quantum computers to manipulate and classify high-dimensional vectors, the core mathematical routine in machine learning. The method can, in principle, be scaled to larger numbers of qubits, and may provide a new route to accelerate machine learning.

One-step generation of continuous-variable quadripartite cluster states in a circuit QED system

NASA Astrophysics Data System (ADS)

Yang, Zhi-peng; Li, Zhen; Ma, Sheng-li; Li, Fu-li

2017-07-01

We propose a dissipative scheme for one-step generation of continuous-variable quadripartite cluster states in a circuit QED setup consisting of four superconducting coplanar waveguide resonators and a gap-tunable superconducting flux qubit. With external driving fields to adjust the desired qubit-resonator and resonator-resonator interactions, we show that continuous-variable quadripartite cluster states of the four resonators can be generated with the assistance of energy relaxation of the qubit. By comparison with the previous proposals, the distinct advantage of our scheme is that only one step of quantum operation is needed to realize the quantum state engineering. This makes our scheme simpler and more feasible in experiment. Our result may have useful application for implementing quantum computation in solid-state circuit QED systems.

Multi-party Measurement-Device-Independent Quantum Key Distribution Based on Cluster States

NASA Astrophysics Data System (ADS)

Liu, Chuanqi; Zhu, Changhua; Ma, Shuquan; Pei, Changxing

2018-03-01

We propose a novel multi-party measurement-device-independent quantum key distribution (MDI-QKD) protocol based on cluster states. A four-photon analyzer which can distinguish all the 16 cluster states serves as the measurement device for four-party MDI-QKD. Any two out of four participants can build secure keys after the analyzers obtains successful outputs and the two participants perform post-processing. We derive a security analysis for the protocol, and analyze the key rates under different values of polarization misalignment. The results show that four-party MDI-QKD is feasible over 280 km in the optical fiber channel when the key rate is about 10- 6 with the polarization misalignment parameter 0.015. Moreover, our work takes an important step toward a quantum communication network.

Final Technical Report for Quantum Embedding for Correlated Electronic Structure in Large Systems and the Condensed Phase

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chan, Garnet Kin-Lic

2017-04-30

This is the final technical report. We briefly describe some selected results below. Developments in density matrix embedding. DMET is a quantum embedding theory that we introduced at the beginning of the last funding period, around 2012-2013. Since the first DMET papers, which demonstrated proof-of- principle calculations on the Hubbard model and hydrogen rings, we have carried out a number of different developments, including: Extending the DMET technology to compute broken symmetry phases, including magnetic phases and super- conductivity (Pub. 13); Calibrating the accuracy of DMET and its cluster size convergence against other methods, and formulation of a dynamical clustermore » analog (Pubs. 4, 10) (see Fig. 1); Implementing DMET for ab-initio molecular calculations, and exploring different self-consistency criteria (Pubs. 9, 14); Using embedding to defi ne quantum classical interfaces Pub. 2; Formulating DMET for spectral functions (Pub. 7) (see Fig. 1); Extending DMET to coupled fermion-boson problems (Pub. 12). Together with these embedding developments, we have also implemented a wide variety of impurity solvers within our DMET framework, including DMRG (Pub. 3), AFQMC (Pub. 10), and coupled cluster theory (CC) (Pub. 9).« less

Computation of the asymptotic states of modulated open quantum systems with a numerically exact realization of the quantum trajectory method

NASA Astrophysics Data System (ADS)

Volokitin, V.; Liniov, A.; Meyerov, I.; Hartmann, M.; Ivanchenko, M.; Hänggi, P.; Denisov, S.

2017-11-01

Quantum systems out of equilibrium are presently a subject of active research, both in theoretical and experimental domains. In this work, we consider time-periodically modulated quantum systems that are in contact with a stationary environment. Within the framework of a quantum master equation, the asymptotic states of such systems are described by time-periodic density operators. Resolution of these operators constitutes a nontrivial computational task. Approaches based on spectral and iterative methods are restricted to systems with the dimension of the hosting Hilbert space dim H =N ≲300 , while the direct long-time numerical integration of the master equation becomes increasingly problematic for N ≳400 , especially when the coupling to the environment is weak. To go beyond this limit, we use the quantum trajectory method, which unravels the master equation for the density operator into a set of stochastic processes for wave functions. The asymptotic density matrix is calculated by performing a statistical sampling over the ensemble of quantum trajectories, preceded by a long transient propagation. We follow the ideology of event-driven programming and construct a new algorithmic realization of the method. The algorithm is computationally efficient, allowing for long "leaps" forward in time. It is also numerically exact, in the sense that, being given the list of uniformly distributed (on the unit interval) random numbers, {η1,η2,...,ηn} , one could propagate a quantum trajectory (with ηi's as norm thresholds) in a numerically exact way. By using a scalable N -particle quantum model, we demonstrate that the algorithm allows us to resolve the asymptotic density operator of the model system with N =2000 states on a regular-size computer cluster, thus reaching the scale on which numerical studies of modulated Hamiltonian systems are currently performed.

Computation of the asymptotic states of modulated open quantum systems with a numerically exact realization of the quantum trajectory method.

PubMed

Volokitin, V; Liniov, A; Meyerov, I; Hartmann, M; Ivanchenko, M; Hänggi, P; Denisov, S

2017-11-01

Quantum systems out of equilibrium are presently a subject of active research, both in theoretical and experimental domains. In this work, we consider time-periodically modulated quantum systems that are in contact with a stationary environment. Within the framework of a quantum master equation, the asymptotic states of such systems are described by time-periodic density operators. Resolution of these operators constitutes a nontrivial computational task. Approaches based on spectral and iterative methods are restricted to systems with the dimension of the hosting Hilbert space dimH=N≲300, while the direct long-time numerical integration of the master equation becomes increasingly problematic for N≳400, especially when the coupling to the environment is weak. To go beyond this limit, we use the quantum trajectory method, which unravels the master equation for the density operator into a set of stochastic processes for wave functions. The asymptotic density matrix is calculated by performing a statistical sampling over the ensemble of quantum trajectories, preceded by a long transient propagation. We follow the ideology of event-driven programming and construct a new algorithmic realization of the method. The algorithm is computationally efficient, allowing for long "leaps" forward in time. It is also numerically exact, in the sense that, being given the list of uniformly distributed (on the unit interval) random numbers, {η_{1},η_{2},...,η_{n}}, one could propagate a quantum trajectory (with η_{i}'s as norm thresholds) in a numerically exact way. By using a scalable N-particle quantum model, we demonstrate that the algorithm allows us to resolve the asymptotic density operator of the model system with N=2000 states on a regular-size computer cluster, thus reaching the scale on which numerical studies of modulated Hamiltonian systems are currently performed.

Coupled Cluster Method with Single and Double Excitations Tailored by Matrix Product State Wave Functions.

PubMed

Veis, Libor; Antalík, Andrej; Brabec, Jiří; Neese, Frank; Legeza, Örs; Pittner, Jiří

2016-10-03

In the past decade, the quantum chemical version of the density matrix renormalization group (DMRG) method has established itself as the method of choice for calculations of strongly correlated molecular systems. Despite its favorable scaling, it is in practice not suitable for computations of dynamic correlation. We present a novel method for accurate "post-DMRG" treatment of dynamic correlation based on the tailored coupled cluster (CC) theory in which the DMRG method is responsible for the proper description of nondynamic correlation, whereas dynamic correlation is incorporated through the framework of the CC theory. We illustrate the potential of this method on prominent multireference systems, in particular, N 2 and Cr 2 molecules and also oxo-Mn(Salen), for which we have performed the first post-DMRG computations in order to shed light on the energy ordering of the lowest spin states.

Domain and network aggregation of CdTe quantum rods within Langmuir Blodgett monolayers

NASA Astrophysics Data System (ADS)

Zimnitsky, Dmitry; Xu, Jun; Lin, Zhiqun; Tsukruk, Vladimir V.

2008-05-01

Control over the organization of quantum rods was demonstrated by changing the surface area at the air-liquid interface by means of the Langmuir-Blodgett (LB) technique. The LB isotherm of CdTe quantum rods capped with a mixture of alkylphosphines shows a transition point in the liquid-solid state, which is caused by the inter-rod reorganization. As we observed, at low surface pressure the quantum rods are assembled into round-shaped aggregates composed of a monolayer of nanorods packed in limited-size clusters with random orientation. The increase of the surface pressure leads to the rearrangement of these aggregates into elongated bundles composed of uniformly oriented nanorod clusters. Further compression results in denser packing of nanorods aggregates and in the transformation of monolayered domains into a continuous network of locally ordered quantum rods.

Light clusters in nuclear matter: Excluded volume versus quantum many-body approaches

NASA Astrophysics Data System (ADS)

Hempel, Matthias; Schaffner-Bielich, Jürgen; Typel, Stefan; Röpke, Gerd

2011-11-01

The formation of clusters in nuclear matter is investigated, which occurs, e.g., in low-energy heavy-ion collisions or core-collapse supernovae. In astrophysical applications, the excluded volume concept is commonly used for the description of light clusters. Here we compare a phenomenological excluded volume approach to two quantum many-body models, the quantum statistical model and the generalized relativistic mean-field model. All three models contain bound states of nuclei with mass number A≤4. It is explored to which extent the complex medium effects can be mimicked by the simpler excluded volume model, regarding the chemical composition and thermodynamic variables. Furthermore, the role of heavy nuclei and excited states is investigated by use of the excluded volume model. At temperatures of a few MeV the excluded volume model gives a poor description of the medium effects on the light clusters, but there the composition is actually dominated by heavy nuclei. At larger temperatures there is a rather good agreement, whereas some smaller differences and model dependencies remain.

Experimental and theoretical study of the microsolvation of sodium atoms in methanol clusters: differences and similarities to sodium-water and sodium-ammonia.

PubMed

Dauster, Ingo; Suhm, Martin A; Buck, Udo; Zeuch, Thomas

2008-01-07

Methanol clusters are generated in a continuous He-seeded supersonic expansion and doped with sodium atoms in a pick-up cell. By this method, clusters of the type Na(CH(3)OH)(n) are formed and subsequently photoionized by applying a tunable dye-laser system. The microsolvation process of the Na 3s electron is studied by determining the ionization potentials (IPs) of these clusters size-selectively for n = 2-40. A decrease is found from n = 2 to 6 and a constant value of 3.19 +/- 0.07 eV for n = 6-40. The experimentally-determined ionization potentials are compared with ionization potentials derived from quantum-chemical calculations, assuming limiting vertical and adiabatic processes. In the first case, energy differences are calculated between the neutral and the ionized cationic clusters of the same geometry. In the second case, the ionized clusters are used in their optimized relaxed geometry. These energy differences and relative stabilities of isomeric clusters vary significantly with the applied quantum-chemical method (B3LYP or MP2). The comparison with the experiment for n = 2-7 reveals strong variations of the ionization potential with the cluster structure indicating that structural diversity and non-vertical pathways give significant signal contributions at the threshold. Based on these findings, a possible explanation for the remarkable difference in IP evolutions of methanol or water and ammonia is presented: for methanol and water a rather localized surface or semi-internal Na 3s electron is excited to either high Rydberg or more localized states below the vertical ionization threshold. This excitation is followed by a local structural relaxation that couples to an autoionization process. For small clusters with n < 6 for methanol and n < 4 for water the addition of solvent molecules leads to larger solvent-metal-ion interaction energies, which consequently lead to lower ionization thresholds. For n = 6 (methanol) and n = 4 (water) this effect comes to a halt, which may be connected with the completion of the first cationic solvation shell limiting the release of local relaxation energy. For Na(NH(3))(n), a largely delocalized and internal electron is excited to autoionizing electronic states, a process that is no longer local and consequently may depend on cluster size up to very large n.

Explicitly Representing the Solvation Shell in Continuum Solvent Calculations

PubMed Central

Svendsen, Hallvard F.; Merz, Kenneth M.

2009-01-01

A method is presented to explicitly represent the first solvation shell in continuum solvation calculations. Initial solvation shell geometries were generated with classical molecular dynamics simulations. Clusters consisting of solute and 5 solvent molecules were fully relaxed in quantum mechanical calculations. The free energy of solvation of the solute was calculated from the free energy of formation of the cluster and the solvation free energy of the cluster calculated with continuum solvation models. The method has been implemented with two continuum solvation models, a Poisson-Boltzmann model and the IEF-PCM model. Calculations were carried out for a set of 60 ionic species. Implemented with the Poisson-Boltzmann model the method gave an unsigned average error of 2.1 kcal/mol and a RMSD of 2.6 kcal/mol for anions, for cations the unsigned average error was 2.8 kcal/mol and the RMSD 3.9 kcal/mol. Similar results were obtained with the IEF-PCM model. PMID:19425558

Synthesis and characterization of Mn quantum dots by bioreduction with water hyacinth.

PubMed

Rosano-Ortega, G; Schabes-Retchkiman, P; Zorrilla, C; Liu, H B; Canizal, G; Avila-Pérez, P; Ascencio, J A

2006-01-01

The bio-reduction method is reported as a part of a complimentary self-sustained technology, where bioremediation and metal particle production are related. The use of the characterization methods in this self sustainable technique open the expectative to be used for several other elements and with other plants, which will be discussed. However, the particular case of Mn nanoparticles involves an important option to generate nanoparticles in the range of 1-4 nanometers with a well controlled size and with a structure based on an fcc-like geometry for the smallest clusters and with more complex arrays for cluster greater than four shells, which involves magnetic moments significantly related to their atomistic configuration. At the same time, the use of the characterization methods establishes the dependence of the nanoparticle's size on the pH conditions used during the synthesis; small clusters in the range of 1-2 nm were generated using pH=5, and it was shown that for the smallest aggregates, simple polyhedron shapes are stable.

Qudit quantum computation on matrix product states with global symmetry

NASA Astrophysics Data System (ADS)

Wang, Dongsheng; Stephen, David; Raussendorf, Robert

Resource states that contain nontrivial symmetry-protected topological order are identified for universal measurement-based quantum computation. Our resource states fall into two classes: one as the qudit generalizations of the qubit cluster state, and the other as the higher-symmetry generalizations of the spin-1 Affleck-Kennedy-Lieb-Tasaki (AKLT) state, namely, with unitary, orthogonal, or symplectic symmetry. The symmetry in cluster states protects information propagation (identity gate), while the higher symmetry in AKLT-type states enables nontrivial gate computation. This work demonstrates a close connection between measurement-based quantum computation and symmetry-protected topological order.

Qudit quantum computation on matrix product states with global symmetry

NASA Astrophysics Data System (ADS)

Wang, Dong-Sheng; Stephen, David T.; Raussendorf, Robert

2017-03-01

Resource states that contain nontrivial symmetry-protected topological order are identified for universal single-qudit measurement-based quantum computation. Our resource states fall into two classes: one as the qudit generalizations of the one-dimensional qubit cluster state, and the other as the higher-symmetry generalizations of the spin-1 Affleck-Kennedy-Lieb-Tasaki (AKLT) state, namely, with unitary, orthogonal, or symplectic symmetry. The symmetry in cluster states protects information propagation (identity gate), while the higher symmetry in AKLT-type states enables nontrivial gate computation. This work demonstrates a close connection between measurement-based quantum computation and symmetry-protected topological order.

Resonantly enhanced spin-lattice relaxation of Mn2 + ions in diluted magnetic (Zn,Mn)Se/(Zn,Be)Se quantum wells

NASA Astrophysics Data System (ADS)

Debus, J.; Ivanov, V. Yu.; Ryabchenko, S. M.; Yakovlev, D. R.; Maksimov, A. A.; Semenov, Yu. G.; Braukmann, D.; Rautert, J.; Löw, U.; Godlewski, M.; Waag, A.; Bayer, M.

2016-05-01

The dynamics of spin-lattice relaxation in the magnetic Mn2 + ion system of (Zn,Mn)Se/(Zn,Be)Se quantum-well structures are studied using optical methods. Pronounced cusps are found in the giant Zeeman shift of the quantum-well exciton photoluminescence at specific magnetic fields below 10 T, when the Mn spin system is heated by photogenerated carriers. The spin-lattice relaxation time of the Mn ions is resonantly accelerated at the cusp magnetic fields. Our theoretical analysis demonstrates that a cusp occurs at a spin-level mixing of single Mn2 + ions and a quick-relaxing cluster of nearest-neighbor Mn ions, which can be described as intrinsic cross-relaxation resonance within the Mn spin system.

Research on Quantum Algorithms at the Institute for Quantum Information

DTIC Science & Technology

2009-10-17

accuracy threshold theorem for the one-way quantum computer. Their proof is based on a novel scheme, in which a noisy cluster state in three spatial...detected. The proof applies to independent stochastic noise but (in contrast to proofs of the quantum accuracy threshold theorem based on concatenated...proved quantum threshold theorems for long-range correlated non-Markovian noise, for leakage faults, for the one-way quantum computer, for postselected

Kramers degeneracy and relaxation in vanadium, niobium and tantalum clusters

NASA Astrophysics Data System (ADS)

Diaz-Bachs, A.; Katsnelson, M. I.; Kirilyuk, A.

2018-04-01

In this work we use magnetic deflection of V, Nb, and Ta atomic clusters to measure their magnetic moments. While only a few of the clusters show weak magnetism, all odd-numbered clusters deflect due to the presence of a single unpaired electron. Surprisingly, for the majority of V and Nb clusters an atomic-like behavior is found, which is a direct indication of the absence of spin–lattice interaction. This is in agreement with Kramers degeneracy theorem for systems with a half-integer spin. This purely quantum phenomenon is surprisingly observed for large systems of more than 20 atoms, and also indicates various quantum relaxation processes, via Raman two-phonon and Orbach high-spin mechanisms. In heavier, Ta clusters, the relaxation is always present, probably due to larger masses and thus lower phonon energies, as well as increased spin–orbit coupling.

Structure of Low-Lying Excited States of Guanine in DNA and Solution: Combined Molecular Mechanics and High-Level Coupled Cluster Studies

DOE PAGES

Kowalski, Karol; Valiev, Marat

2007-01-01

High-level ab-initio equation-of-motion coupled-cluster methods with singles, doubles, and noniterative triples are used, in conjunction with the combined quantum mechanical molecular mechanics approach, to investigate the structure of low-lying excited states of the guanine base in DNA and solvated environments. Our results indicate that while the excitation energy of the first excited state is barely changed compared to its gas-phase counterpart, the excitation energy of the second excited state is blue-shifted by 0.24 eV.

Semiconductor nanocrystals covalently bound to solid inorganic surfaces using self-assembled monolayers

DOEpatents

Alivisatos, A.P.; Colvin, V.L.

1998-05-12

Methods are described for attaching semiconductor nanocrystals to solid inorganic surfaces, using self-assembled bifunctional organic monolayers as bridge compounds. Two different techniques are presented. One relies on the formation of self-assembled monolayers on these surfaces. When exposed to solutions of nanocrystals, these bridge compounds bind the crystals and anchor them to the surface. The second technique attaches nanocrystals already coated with bridge compounds to the surfaces. Analyses indicate the presence of quantum confined clusters on the surfaces at the nanolayer level. These materials allow electron spectroscopies to be completed on condensed phase clusters, and represent a first step towards synthesis of an organized assembly of clusters. These new products are also disclosed. 10 figs.

Applying the Coupled-Cluster Ansatz to Solids and Surfaces in the Thermodynamic Limit

NASA Astrophysics Data System (ADS)

Gruber, Thomas; Liao, Ke; Tsatsoulis, Theodoros; Hummel, Felix; Grüneis, Andreas

2018-04-01

Modern electronic structure theories can predict and simulate a wealth of phenomena in surface science and solid-state physics. In order to allow for a direct comparison with experiment, such ab initio predictions have to be made in the thermodynamic limit, substantially increasing the computational cost of many-electron wave-function theories. Here, we present a method that achieves thermodynamic limit results for solids and surfaces using the "gold standard" coupled cluster ansatz of quantum chemistry with unprecedented efficiency. We study the energy difference between carbon diamond and graphite crystals, adsorption energies of water on h -BN, as well as the cohesive energy of the Ne solid, demonstrating the increased efficiency and accuracy of coupled cluster theory for solids and surfaces.

Self-assembled inorganic clusters of semiconducting quantum dots for effective solar hydrogen evolution.

PubMed

Gao, Yu-Ji; Yang, Yichen; Li, Xu-Bing; Wu, Hao-Lin; Meng, Shu-Lin; Wang, Yang; Guo, Qing; Huang, Mao-Yong; Tung, Chen-Ho; Wu, Li-Zhu

2018-05-08

Owing to promoted electron-hole separation, the catalytic activity of semiconducting quantum dots (QDs) towards solar hydrogen (H2) production has been significantly enhanced by forming self-assembled clusters with ZnSe QDs made ex situ. Taking advantage of the favored interparticle hole transfer to ZnSe QDs, the rate of solar H2 evolution of CdSe QDs can be increased to ∼30 000 μmol h-1 g-1 with ascorbic acid as the sacrificial reagent, ∼150-fold higher than that of bare CdSe QDs clusters under the same conditions.

Influence of GaAs surface termination on GaSb/GaAs quantum dot structure and band offsets

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zech, E. S.; Chang, A. S.; Martin, A. J.

2013-08-19

We have investigated the influence of GaAs surface termination on the nanoscale structure and band offsets of GaSb/GaAs quantum dots (QDs) grown by molecular-beam epitaxy. Transmission electron microscopy reveals both coherent and semi-coherent clusters, as well as misfit dislocations, independent of surface termination. Cross-sectional scanning tunneling microscopy and spectroscopy reveal clustered GaSb QDs with type I band offsets at the GaSb/GaAs interfaces. We discuss the relative influences of strain and QD clustering on the band offsets at GaSb/GaAs interfaces.

Surface passivation for tight-binding calculations of covalent solids.

PubMed

Bernstein, N

2007-07-04

Simulation of a cluster representing a finite portion of a larger covalently bonded system requires the passivation of the cluster surface. We compute the effects of an explicit hybrid orbital passivation (EHOP) on the atomic structure in a model bulk, three-dimensional, narrow gap semiconductor, which is very different from the wide gap, quasi-one-dimensional organic molecules where most passivation schemes have been studied in detail. The EHOP approach is directly applicable to minimal atomic orbital basis methods such as tight-binding. Each broken bond is passivated by a hybrid created from an explicitly expressed linear combination of basis orbitals, chosen to represent the contribution of the missing neighbour, e.g. a sp(3) hybrid for a single bond. The method is tested by computing the forces on atoms near a point defect as a function of cluster geometry. We show that, compared to alternatives such as pseudo-hydrogen passivation, the force on an atom converges to the correct bulk limit more quickly as a function of cluster radius, and that the force is more stable with respect to perturbations in the position of the cluster centre. The EHOP method also obviates the need for parameterizing the interactions between the system atoms and the passivating atoms. The method is useful for cluster calculations of non-periodic defects in large systems and for hybrid schemes that simulate large systems by treating finite regions with a quantum-mechanical model, coupled to an interatomic potential description of the rest of the system.

Surface passivation for tight-binding calculations of covalent solids

NASA Astrophysics Data System (ADS)

Bernstein, N.

2007-07-01

Simulation of a cluster representing a finite portion of a larger covalently bonded system requires the passivation of the cluster surface. We compute the effects of an explicit hybrid orbital passivation (EHOP) on the atomic structure in a model bulk, three-dimensional, narrow gap semiconductor, which is very different from the wide gap, quasi-one-dimensional organic molecules where most passivation schemes have been studied in detail. The EHOP approach is directly applicable to minimal atomic orbital basis methods such as tight-binding. Each broken bond is passivated by a hybrid created from an explicitly expressed linear combination of basis orbitals, chosen to represent the contribution of the missing neighbour, e.g. a sp3 hybrid for a single bond. The method is tested by computing the forces on atoms near a point defect as a function of cluster geometry. We show that, compared to alternatives such as pseudo-hydrogen passivation, the force on an atom converges to the correct bulk limit more quickly as a function of cluster radius, and that the force is more stable with respect to perturbations in the position of the cluster centre. The EHOP method also obviates the need for parameterizing the interactions between the system atoms and the passivating atoms. The method is useful for cluster calculations of non-periodic defects in large systems and for hybrid schemes that simulate large systems by treating finite regions with a quantum-mechanical model, coupled to an interatomic potential description of the rest of the system.

A Poisson nonnegative matrix factorization method with parameter subspace clustering constraint for endmember extraction in hyperspectral imagery

NASA Astrophysics Data System (ADS)

Sun, Weiwei; Ma, Jun; Yang, Gang; Du, Bo; Zhang, Liangpei

2017-06-01

A new Bayesian method named Poisson Nonnegative Matrix Factorization with Parameter Subspace Clustering Constraint (PNMF-PSCC) has been presented to extract endmembers from Hyperspectral Imagery (HSI). First, the method integrates the liner spectral mixture model with the Bayesian framework and it formulates endmember extraction into a Bayesian inference problem. Second, the Parameter Subspace Clustering Constraint (PSCC) is incorporated into the statistical program to consider the clustering of all pixels in the parameter subspace. The PSCC could enlarge differences among ground objects and helps finding endmembers with smaller spectrum divergences. Meanwhile, the PNMF-PSCC method utilizes the Poisson distribution as the prior knowledge of spectral signals to better explain the quantum nature of light in imaging spectrometer. Third, the optimization problem of PNMF-PSCC is formulated into maximizing the joint density via the Maximum A Posterior (MAP) estimator. The program is finally solved by iteratively optimizing two sub-problems via the Alternating Direction Method of Multipliers (ADMM) framework and the FURTHESTSUM initialization scheme. Five state-of-the art methods are implemented to make comparisons with the performance of PNMF-PSCC on both the synthetic and real HSI datasets. Experimental results show that the PNMF-PSCC outperforms all the five methods in Spectral Angle Distance (SAD) and Root-Mean-Square-Error (RMSE), and especially it could identify good endmembers for ground objects with smaller spectrum divergences.

The theory of variational hybrid quantum-classical algorithms

NASA Astrophysics Data System (ADS)

McClean, Jarrod R.; Romero, Jonathan; Babbush, Ryan; Aspuru-Guzik, Alán

2016-02-01

Many quantum algorithms have daunting resource requirements when compared to what is available today. To address this discrepancy, a quantum-classical hybrid optimization scheme known as ‘the quantum variational eigensolver’ was developed (Peruzzo et al 2014 Nat. Commun. 5 4213) with the philosophy that even minimal quantum resources could be made useful when used in conjunction with classical routines. In this work we extend the general theory of this algorithm and suggest algorithmic improvements for practical implementations. Specifically, we develop a variational adiabatic ansatz and explore unitary coupled cluster where we establish a connection from second order unitary coupled cluster to universal gate sets through a relaxation of exponential operator splitting. We introduce the concept of quantum variational error suppression that allows some errors to be suppressed naturally in this algorithm on a pre-threshold quantum device. Additionally, we analyze truncation and correlated sampling in Hamiltonian averaging as ways to reduce the cost of this procedure. Finally, we show how the use of modern derivative free optimization techniques can offer dramatic computational savings of up to three orders of magnitude over previously used optimization techniques.

Trajectory control of PbSe–γ-Fe2O3 nanoplatforms under viscous flow and an external magnetic field

PubMed Central

Etgar, Lioz; Nakhmani, Arie; Tannenbaum, Allen; Lifshitz, Efrat; Tannenbaum, Rina

2010-01-01

The flow behavior of nanostructure clusters, consisting of chemically bonded PbSe quantum dots and magnetic γ -Fe2O3 nanoparticles, has been investigated. The clusters are regarded as model nanoplatforms with multiple functionalities, where the γ -Fe2O3 magnets serve as transport vehicles, manipulated by an external magnetic field gradient, and the quantum dots act as fluorescence tags within an optical window in the near-infrared regime. The clusters’ flow was characterized by visualizing their trajectories within a viscous fluid (mimicking a blood stream), using an optical imaging method, while the trajectory pictures were analyzed by a specially developed processing package. The trajectories were examined under various flow rates, viscosities and applied magnetic field strengths. The results revealed a control of the trajectories even at low magnetic fields (<1 T), validating the use of similar nanoplatforms as active targeting constituents in personalized medicine. PMID:20368678

The accuracy of ab initio calculations without ab initio calculations for charged systems: Kriging predictions of atomistic properties for ions in aqueous solutions

NASA Astrophysics Data System (ADS)

Di Pasquale, Nicodemo; Davie, Stuart J.; Popelier, Paul L. A.

2018-06-01

Using the machine learning method kriging, we predict the energies of atoms in ion-water clusters, consisting of either Cl- or Na+ surrounded by a number of water molecules (i.e., without Na+Cl- interaction). These atomic energies are calculated following the topological energy partitioning method called Interacting Quantum Atoms (IQAs). Kriging predicts atomic properties (in this case IQA energies) by a model that has been trained over a small set of geometries with known property values. The results presented here are part of the development of an advanced type of force field, called FFLUX, which offers quantum mechanical information to molecular dynamics simulations without the limiting computational cost of ab initio calculations. The results reported for the prediction of the IQA components of the energy in the test set exhibit an accuracy of a few kJ/mol, corresponding to an average error of less than 5%, even when a large cluster of water molecules surrounding an ion is considered. Ions represent an important chemical system and this work shows that they can be correctly taken into account in the framework of the FFLUX force field.

Parallelized traveling cluster approximation to study numerically spin-fermion models on large lattices

DOE PAGES

Mukherjee, Anamitra; Patel, Niravkumar D.; Bishop, Chris; ...

2015-06-08

Lattice spin-fermion models are quite important to study correlated systems where quantum dynamics allows for a separation between slow and fast degrees of freedom. The fast degrees of freedom are treated quantum mechanically while the slow variables, generically referred to as the “spins,” are treated classically. At present, exact diagonalization coupled with classical Monte Carlo (ED + MC) is extensively used to solve numerically a general class of lattice spin-fermion problems. In this common setup, the classical variables (spins) are treated via the standard MC method while the fermion problem is solved by exact diagonalization. The “traveling cluster approximation” (TCA)more » is a real space variant of the ED + MC method that allows to solve spin-fermion problems on lattice sizes with up to 10 3 sites. In this paper, we present a novel reorganization of the TCA algorithm in a manner that can be efficiently parallelized. Finally, this allows us to solve generic spin-fermion models easily on 10 4 lattice sites and with some effort on 10 5 lattice sites, representing the record lattice sizes studied for this family of models.« less

Parallelized traveling cluster approximation to study numerically spin-fermion models on large lattices

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mukherjee, Anamitra; Patel, Niravkumar D.; Bishop, Chris

Lattice spin-fermion models are quite important to study correlated systems where quantum dynamics allows for a separation between slow and fast degrees of freedom. The fast degrees of freedom are treated quantum mechanically while the slow variables, generically referred to as the “spins,” are treated classically. At present, exact diagonalization coupled with classical Monte Carlo (ED + MC) is extensively used to solve numerically a general class of lattice spin-fermion problems. In this common setup, the classical variables (spins) are treated via the standard MC method while the fermion problem is solved by exact diagonalization. The “traveling cluster approximation” (TCA)more » is a real space variant of the ED + MC method that allows to solve spin-fermion problems on lattice sizes with up to 10 3 sites. In this paper, we present a novel reorganization of the TCA algorithm in a manner that can be efficiently parallelized. Finally, this allows us to solve generic spin-fermion models easily on 10 4 lattice sites and with some effort on 10 5 lattice sites, representing the record lattice sizes studied for this family of models.« less

Cluster expansion for ground states of local Hamiltonians

NASA Astrophysics Data System (ADS)

Bastianello, Alvise; Sotiriadis, Spyros

2016-08-01

A central problem in many-body quantum physics is the determination of the ground state of a thermodynamically large physical system. We construct a cluster expansion for ground states of local Hamiltonians, which naturally incorporates physical requirements inherited by locality as conditions on its cluster amplitudes. Applying a diagrammatic technique we derive the relation of these amplitudes to thermodynamic quantities and local observables. Moreover we derive a set of functional equations that determine the cluster amplitudes for a general Hamiltonian, verify the consistency with perturbation theory and discuss non-perturbative approaches. Lastly we verify the persistence of locality features of the cluster expansion under unitary evolution with a local Hamiltonian and provide applications to out-of-equilibrium problems: a simplified proof of equilibration to the GGE and a cumulant expansion for the statistics of work, for an interacting-to-free quantum quench.

Ground and excited states of the Rydberg radical H3O: Electron propagator and quantum defect analysis

NASA Astrophysics Data System (ADS)

Melin, Junia; Ortiz, J. V.; Martín, I.; Velasco, A. M.; Lavín, C.

2005-06-01

Vertical excitation energies of the Rydberg radical H3O are inferred from ab initio electron propagator calculations on the electron affinities of H3O+. The adiabatic ionization energy of H3O is evaluated with coupled-cluster calculations. These predictions provide optimal parameters for the molecular-adapted quantum defect orbital method, which is used to determine oscillator strengths. Given that the experimental spectrum of H3O does not seem to be available, comparisons with previous calculations are discussed. A simple model Hamiltonian, suitable for the study of bound states with arbitrarily high energies is generated by these means.

Entangled quantum electronic wavefunctions of the Mn₄CaO₅ cluster in photosystem II.

PubMed

Kurashige, Yuki; Chan, Garnet Kin-Lic; Yanai, Takeshi

2013-08-01

It is a long-standing goal to understand the reaction mechanisms of catalytic metalloenzymes at an entangled many-electron level, but this is hampered by the exponential complexity of quantum mechanics. Here, by exploiting the special structure of physical quantum states and using the density matrix renormalization group, we compute near-exact many-electron wavefunctions of the Mn4CaO5 cluster of photosystem II, with more than 1 × 10(18) quantum degrees of freedom. This is the first treatment of photosystem II beyond the single-electron picture of density functional theory. Our calculations support recent modifications to the structure determined by X-ray crystallography. We further identify multiple low-lying energy surfaces associated with the structural distortion seen using X-ray crystallography, highlighting multistate reactivity in the chemistry of the cluster. Direct determination of Mn spin-projections from our wavefunctions suggests that current candidates that have been recently distinguished using parameterized spin models should be reassessed. Through entanglement maps, we reveal rich information contained in the wavefunctions on bonding changes in the cycle.

Rotational symmetry breaking toward a string-valence bond solid phase in frustrated J1 -J2 transverse field Ising model

NASA Astrophysics Data System (ADS)

Sadrzadeh, M.; Langari, A.

2018-06-01

We study the effect of quantum fluctuations by means of a transverse magnetic field (Γ) on the highly degenerate ground state of antiferromagnetic J1 -J2 Ising model on the square lattice, at the limit J2 /J1 = 0.5 . We show that harmonic quantum fluctuations based on single spin flips can not lift such degeneracy, however an-harmonic quantum fluctuations based on multi spin cluster flip excitations lift the degeneracy toward a unique ground state with string-valence bond solid (VBS) nature. A cluster operator formalism has been implemented to incorporate an-harmonic quantum fluctuations. We show that cluster-type excitations of the model lead not only to lower the excitation energy compared with a single-spin flip but also to lift the extensive degeneracy in favor of a string-VBS state, which breaks lattice rotational symmetry with only two fold degeneracy. The tendency toward the broken symmetry state is justified by numerical exact diagonalization. Moreover, we introduce a map to find the relation between the present model on the checkerboard and square lattices.

Fluorescence Imaging Assisted Photodynamic Therapy Using Photosensitizer-Linked Gold Quantum Clusters.

PubMed

Nair, Lakshmi V; Nazeer, Shaiju S; Jayasree, Ramapurath S; Ajayaghosh, Ayyappanpillai

2015-06-23

Fluorescence imaging assisted photodynamic therapy (PDT) is a viable two-in-one clinical tool for cancer treatment and follow-up. While the surface plasmon effect of gold nanorods and nanoparticles has been effective for cancer therapy, their emission properties when compared to gold nanoclusters are weak for fluorescence imaging guided PDT. In order to address the above issues, we have synthesized a near-infrared-emitting gold quantum cluster capped with lipoic acid (L-AuC with (Au)18(L)14) based nanoplatform with excellent tumor reduction property by incorporating a tumor-targeting agent (folic acid) and a photosensitizer (protoporphyrin IX), for selective PDT. The synthesized quantum cluster based photosensitizer PFL-AuC showed 80% triplet quantum yield when compared to that of the photosensitizer alone (63%). PFL-AuC having 60 μg (0.136 mM) of protoporphyrin IX was sufficient to kill 50% of the tumor cell population. Effective destruction of tumor cells was evident from the histopathology and fluorescence imaging, which confirm the in vivo PDT efficacy of PFL-AuC.

Development and application of QM/MM methods to study the solvation effects and surfaces

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dibya, Pooja Arora

2010-01-01

Quantum mechanical (QM) calculations have the advantage of attaining high-level accuracy, however QM calculations become computationally inefficient as the size of the system grows. Solving complex molecular problems on large systems and ensembles by using quantum mechanics still poses a challenge in terms of the computational cost. Methods that are based on classical mechanics are an inexpensive alternative, but they lack accuracy. A good trade off between accuracy and efficiency is achieved by combining QM methods with molecular mechanics (MM) methods to use the robustness of the QM methods in terms of accuracy and the MM methods to minimize themore » computational cost. Two types of QM combined with MM (QM/MM) methods are the main focus of the present dissertation: the application and development of QM/MM methods for solvation studies and reactions on the Si(100) surface. The solvation studies were performed using a discreet solvation model that is largely based on first principles called the effective fragment potential method (EFP). The main idea of combining the EFP method with quantum mechanics is to accurately treat the solute-solvent and solvent-solvent interactions, such as electrostatic, polarization, dispersion and charge transfer, that are important in correctly calculating solvent effects on systems of interest. A second QM/MM method called SIMOMM (surface integrated molecular orbital molecular mechanics) is a hybrid QM/MM embedded cluster model that mimics the real surface.3 This method was employed to calculate the potential energy surfaces for reactions of atomic O on the Si(100) surface. The hybrid QM/MM method is a computationally inexpensive approach for studying reactions on larger surfaces in a reasonably accurate and efficient manner. This thesis is comprised of four chapters: Chapter 1 describes the general overview and motivation of the dissertation and gives a broad background of the computational methods that have been employed in this work. Chapter 2 illustrates the methodology of the interface of the EFP method with the configuration interaction with single excitations (CIS) method to study solvent effects in excited states. Chapter 3 discusses the study of the adiabatic electron affinity of the hydroxyl radical in aqueous solution and in micro-solvated clusters using a QM/EFP method. Chapter 4 describes the study of etching and diffusion of oxygen atom on a reconstructed Si(100)-2 x 1 surface using a hybrid QM/MM embedded cluster model (SIMOMM). Chapter 4 elucidates the application of the EFP method towards the understanding of the aqueous ionization potential of Na atom. Finally, a general conclusion of this dissertation work and prospective future direction are presented in Chapter 6.« less

Study of CP(N-1) theta-vacua by cluster simulation of SU(N) quantum spin ladders.

PubMed

Beard, B B; Pepe, M; Riederer, S; Wiese, U-J

2005-01-14

D-theory provides an alternative lattice regularization of the 2D CP(N-1) quantum field theory in which continuous classical fields emerge from the dimensional reduction of discrete SU(N) quantum spins. Spin ladders consisting of n transversely coupled spin chains lead to a CP(N-1) model with a vacuum angle theta=npi. In D-theory no sign problem arises and an efficient cluster algorithm is used to investigate theta-vacuum effects. At theta=pi there is a first order phase transition with spontaneous breaking of charge conjugation symmetry for CP(N-1) models with N>2.

Bidirectional Controlled Quantum Information Transmission by Using a Five-Qubit Cluster State

NASA Astrophysics Data System (ADS)

Sang, Zhi-wen

2017-11-01

We demonstrate that an entangled five-qubit cluster state can be used to realize the deterministic bidirectional controlled quantum information transmission by performing only Bell-state measurement and single-qubit measurements. In our protocol, Alice can teleport an arbitrary unknown single-qubit state to Bob and at the same time Bob can remotely prepare an arbitrary known single-qubit state for Alice via the control of the supervisor Charlie.

Extending density functional embedding theory for covalently bonded systems.

PubMed

Yu, Kuang; Carter, Emily A

2017-12-19

Quantum embedding theory aims to provide an efficient solution to obtain accurate electronic energies for systems too large for full-scale, high-level quantum calculations. It adopts a hierarchical approach that divides the total system into a small embedded region and a larger environment, using different levels of theory to describe each part. Previously, we developed a density-based quantum embedding theory called density functional embedding theory (DFET), which achieved considerable success in metals and semiconductors. In this work, we extend DFET into a density-matrix-based nonlocal form, enabling DFET to study the stronger quantum couplings between covalently bonded subsystems. We name this theory density-matrix functional embedding theory (DMFET), and we demonstrate its performance in several test examples that resemble various real applications in both chemistry and biochemistry. DMFET gives excellent results in all cases tested thus far, including predicting isomerization energies, proton transfer energies, and highest occupied molecular orbital-lowest unoccupied molecular orbital gaps for local chromophores. Here, we show that DMFET systematically improves the quality of the results compared with the widely used state-of-the-art methods, such as the simple capped cluster model or the widely used ONIOM method.

Pure Gaussian state generation via dissipation: a quantum stochastic differential equation approach.

PubMed

Yamamoto, Naoki

2012-11-28

Recently, the complete characterization of a general Gaussian dissipative system having a unique pure steady state was obtained. This result provides a clear guideline for engineering an environment such that the dissipative system has a desired pure steady state such as a cluster state. In this paper, we describe the system in terms of a quantum stochastic differential equation (QSDE) so that the environment channels can be explicitly dealt with. Then, a physical meaning of that characterization, which cannot be seen without the QSDE representation, is clarified; more specifically, the nullifier dynamics of any Gaussian system generating a unique pure steady state is passive. In addition, again based on the QSDE framework, we provide a general and practical method to implement a desired dissipative Gaussian system, which has a structure of quantum state transfer.

Quantum influence in the criticality of the spin- {1}/{2} anisotropic Heisenberg model

NASA Astrophysics Data System (ADS)

Ricardo de Sousa, J.; Araújo, Ijanílio G.

1999-07-01

We study the spin- {1}/{2} anisotropic Heisenberg antiferromagnetic model using the effective field renormalization group (EFRG) approach. The EFRG method is illustrated by employing approximations in which clusters with one ( N'=1) and two ( N=2) spins are used. The dependence of the critical temperature Tc (ferromagnetic-F case) and TN (antiferromagnetic-AF case) and thermal critical exponent, Yt, are obtained as a function of anisotropy parameter ( Δ) on a simple cubic lattice. We find that, in our results, TN is higher than Tc for the quantum anisotropic Heisenberg limit and TN= Tc for the Ising and quantum XY limits. We have also shown that the thermal critical exponent Yt for the isotropic Heisenberg model shows a small dependence on the type of interaction (F or AF) due to finite size effects.

Understanding the evolution of luminescent gold quantum clusters in protein templates.

PubMed

Chaudhari, Kamalesh; Xavier, Paulrajpillai Lourdu; Pradeep, Thalappil

2011-11-22

We show that the time-dependent biomineralization of Au(3+) by native lactoferrin (NLf) and bovine serum albumin (BSA) resulting in near-infrared (NIR) luminescent gold quantum clusters (QCs) occurs through a protein-bound Au(1+) intermediate and subsequent emergence of free protein. The evolution was probed by diverse tools, principally, using matrix-assisted laser desorption ionization mass spectrometry (MALDI MS), X-ray photoelectron spectroscopy (XPS), and photoluminescence spectroscopy (PL). The importance of alkaline pH in the formation of clusters was probed. At neutral pH, a Au(1+)-protein complex was formed (starting from Au(3+)) with the binding of 13-14 gold atoms per protein. When the pH was increased above 12, these bound gold ions were further reduced to Au(0) and nucleation and growth of cluster commenced, which was corroborated by the beginning of emission; at this point, the number of gold atoms per protein was ~25, suggesting the formation of Au(25). During the cluster evolution, at certain time intervals, for specific molar ratios of gold and protein, occurrence of free protein was noticed in the mass spectra, suggesting a mixture of products and gold ion redistribution. By providing gold ions at specific time of the reaction, monodispersed clusters with enhanced luminescence could be obtained, and the available quantity of free protein could be utilized efficiently. Monodispersed clusters would be useful in obtaining single crystals of protein-protected noble metal quantum clusters where homogeneity of the system is of primary concern. © 2011 American Chemical Society

Internal proton transfer and H2 rotations in the H5(+) cluster: a marked influence on its thermal equilibrium state.

PubMed

de Tudela, Ricardo Pérez; Barragán, Patricia; Prosmiti, Rita; Villarreal, Pablo; Delgado-Barrio, Gerardo

2011-03-31

Classical and path integral Monte Carlo (CMC, PIMC) "on the fly" calculations are carried out to investigate anharmonic quantum effects on the thermal equilibrium structure of the H5(+) cluster. The idea to follow in our computations is based on using a combination of the above-mentioned nuclear classical and quantum statistical methods, and first-principles density functional (DFT) electronic structure calculations. The interaction energies are computed within the DFT framework using the B3(H) hybrid functional, specially designed for hydrogen-only systems. The global minimum of the potential is predicted to be a nonplanar configuration of C(2v) symmetry, while the next three low-lying stationary points on the surface correspond to extremely low-energy barriers for the internal proton transfer and to the rotation of the H2 molecules, around the C2 axis of H5(+), connecting the symmetric C(2v) minima in the planar and nonplanar orientations. On the basis of full-dimensional converged PIMC calculations, results on the quantum vibrational zero-point energy (ZPE) and state of H5(+) are reported at a low temperature of 10 K, and the influence of the above-mentioned topological features of the surface on its probability distributions is clearly demonstrated.

Quantum Tasks with Non-maximally Quantum Channels via Positive Operator-Valued Measurement

NASA Astrophysics Data System (ADS)

Peng, Jia-Yin; Luo, Ming-Xing; Mo, Zhi-Wen

2013-01-01

By using a proper positive operator-valued measure (POVM), we present two new schemes for probabilistic transmission with non-maximally four-particle cluster states. In the first scheme, we demonstrate that two non-maximally four-particle cluster states can be used to realize probabilistically sharing an unknown three-particle GHZ-type state within either distant agent's place. In the second protocol, we demonstrate that a non-maximally four-particle cluster state can be used to teleport an arbitrary unknown multi-particle state in a probabilistic manner with appropriate unitary operations and POVM. Moreover the total success probability of these two schemes are also worked out.

Identification of the low-energy excitations in a quantum critical system

NASA Astrophysics Data System (ADS)

Heitmann, Tom; Lamsal, Jagat; Watson, Shannon; Erwin, Ross; Chen, Wangchun; Zhao, Yang; Montfrooij, Wouter

2017-05-01

We have identified low-energy magnetic excitations in a doped quantum critical system by means of polarized neutron scattering experiments. The presence of these excitations could explain why Ce(Fe0.76Ru0.24)2Ge2 displays dynamical scaling in the absence of local critical behavior or long-range spin-density wave criticality. The low-energy excitations are associated with the reorientations of the superspins of fully ordered, isolated magnetic clusters that form spontaneously upon lowering the temperature. The system houses both frozen clusters and dynamic clusters, as predicted by Hoyos and Vojta [Phys. Rev. B 74, 140401(R) (2006)].

Self-consistent field for fragmented quantum mechanical model of large molecular systems.

PubMed

Jin, Yingdi; Su, Neil Qiang; Xu, Xin; Hu, Hao

2016-01-30

Fragment-based linear scaling quantum chemistry methods are a promising tool for the accurate simulation of chemical and biomolecular systems. Because of the coupled inter-fragment electrostatic interactions, a dual-layer iterative scheme is often employed to compute the fragment electronic structure and the total energy. In the dual-layer scheme, the self-consistent field (SCF) of the electronic structure of a fragment must be solved first, then followed by the updating of the inter-fragment electrostatic interactions. The two steps are sequentially carried out and repeated; as such a significant total number of fragment SCF iterations is required to converge the total energy and becomes the computational bottleneck in many fragment quantum chemistry methods. To reduce the number of fragment SCF iterations and speed up the convergence of the total energy, we develop here a new SCF scheme in which the inter-fragment interactions can be updated concurrently without converging the fragment electronic structure. By constructing the global, block-wise Fock matrix and density matrix, we prove that the commutation between the two global matrices guarantees the commutation of the corresponding matrices in each fragment. Therefore, many highly efficient numerical techniques such as the direct inversion of the iterative subspace method can be employed to converge simultaneously the electronic structure of all fragments, reducing significantly the computational cost. Numerical examples for water clusters of different sizes suggest that the method shall be very useful in improving the scalability of fragment quantum chemistry methods. © 2015 Wiley Periodicals, Inc.

Local resonances in STM manipulation of chlorobenzene on Si(111)-7×7: performance of different cluster models and density functionals

NASA Astrophysics Data System (ADS)

Utecht, Manuel; Klamroth, Tillmann

2018-07-01

Hot localised charge carriers on the Si(111)-7×7 surface are modelled by small charged clusters. Such resonances induce non-local desorption, i.e. more than 10 nm away from the injection site, of chlorobenzene in scanning tunnelling microscope experiments. We used such a cluster model to characterise resonance localisation and vibrational activation for positive and negative resonances recently. In this work, we investigate to which extent the model depends on details of the used cluster or quantum chemistry methods and try to identify the smallest possible cluster suitable for a description of the neutral surface and the ion resonances. Furthermore, a detailed analysis for different chemisorption orientations is performed. While some properties, as estimates of the resonance energy or absolute values for atomic changes, show such a dependency, the main findings are very robust with respect to changes in the model and/or the chemisorption geometry.

An investigation about the structures, thermodynamics and kinetics of the formic acid involved molecular clusters

NASA Astrophysics Data System (ADS)

Zhang, Rui; Jiang, Shuai; Liu, Yi-Rong; Wen, Hui; Feng, Ya-Juan; Huang, Teng; Huang, Wei

2018-05-01

Despite the very important role of atmospheric aerosol nucleation in climate change and air quality, the detailed aerosol nucleation mechanism is still unclear. Here we investigated the formic acid (FA) involved multicomponent nucleation molecular clusters including sulfuric acid (SA), dimethylamine (DMA) and water (W) through a quantum chemical method. The thermodynamics and kinetics analysis was based on the global minima given by Basin-Hopping (BH) algorithm coupled with Density Functional Theory (DFT) and subsequent benchmarked calculations. Then the interaction analysis based on ElectroStatic Potential (ESP), Topological and Atomic Charges analysis was made to characterize the binding features of the clusters. The results show that FA binds weakly with the other molecules in the cluster while W binds more weakly. Further kinetic analysis about the time evolution of the clusters show that even though the formic acid's weak interaction with other nucleation precursors, its effect on sulfuric acid dimer steady state concentration cannot be neglected due to its high concentration in the atmosphere.

Efficient Entanglement Concentration of Nonlocal Two-Photon Polarization-Time-Bin Hyperentangled States

NASA Astrophysics Data System (ADS)

Wang, Zi-Hang; Yu, Wen-Xuan; Wu, Xiao-Yuan; Gao, Cheng-Yan; Alzahrani, Faris; Hobiny, Aatef; Deng, Fu-Guo

2018-03-01

We present two different hyperentanglement concentration protocols (hyper-ECPs) for two-photon systems in nonlocal polarization-time-bin hyperentangled states with known parameters, including Bell-like and cluster-like states, resorting to the parameter splitting method. They require only one of two parties in quantum communication to operate her photon in the process of entanglement concentration, not two, and they have the maximal success probability. They work with linear optical elements and have good feasibility in experiment, especially in the case that there are a big number of quantum data exchanged as the parties can obtain the information about the parameters of the nonlocal hyperentangled states by sampling a subset of nonlocal hyperentangled two-photon systems and measuring them. As the quantum state of photons in the time-bin degree of freedom suffers from less noise in an optical-fiber channel, these hyper-ECPs may have good applications in practical long-distance quantum communication in the future.

Patching the Exchange-Correlation Potential in Density Functional Theory.

PubMed

Huang, Chen

2016-05-10

A method for directly patching exchange-correlation (XC) potentials in materials is derived. The electron density of a system is partitioned into subsystem densities by dividing its Kohn-Sham (KS) potential among the subsystems. Inside each subsystem, its projected KS potential is required to become the total system's KS potential. This requirement, together with the nearsightedness principle of electronic matters, ensures that the electronic structures inside subsystems can be good approximations to the total system's electronic structure. The nearsightedness principle also ensures that subsystem densities could be well localized in their regions, making it possible to use high-level methods to invert the XC potentials for subsystem densities. Two XC patching methods are developed. In the local XC patching method, the total system's XC potential is improved in the cluster region. We show that the coupling between a cluster and its environment is important for achieving a fast convergence of the electronic structure in the cluster region. In the global XC patching method, we discuss how to patch the subsystem XC potentials to construct the XC potential in the total system, aiming to scale up high-level quantum mechanics simulations of materials. Proof-of-principle examples are given.

Computational studies of atmospherically-relevant chemical reactions in water clusters and on liquid water and ice surfaces.

PubMed

Gerber, R Benny; Varner, Mychel E; Hammerich, Audrey D; Riikonen, Sampsa; Murdachaew, Garold; Shemesh, Dorit; Finlayson-Pitts, Barbara J

2015-02-17

CONSPECTUS: Reactions on water and ice surfaces and in other aqueous media are ubiquitous in the atmosphere, but the microscopic mechanisms of most of these processes are as yet unknown. This Account examines recent progress in atomistic simulations of such reactions and the insights provided into mechanisms and interpretation of experiments. Illustrative examples are discussed. The main computational approaches employed are classical trajectory simulations using interaction potentials derived from quantum chemical methods. This comprises both ab initio molecular dynamics (AIMD) and semiempirical molecular dynamics (SEMD), the latter referring to semiempirical quantum chemical methods. Presented examples are as follows: (i) Reaction of the (NO(+))(NO3(-)) ion pair with a water cluster to produce the atmospherically important HONO and HNO3. The simulations show that a cluster with four water molecules describes the reaction. This provides a hydrogen-bonding network supporting the transition state. The reaction is triggered by thermal structural fluctuations, and ultrafast changes in atomic partial charges play a key role. This is an example where a reaction in a small cluster can provide a model for a corresponding bulk process. The results support the proposed mechanism for production of HONO by hydrolysis of NO2 (N2O4). (ii) The reactions of gaseous HCl with N2O4 and N2O5 on liquid water surfaces. Ionization of HCl at the water/air interface is followed by nucleophilic attack of Cl(-) on N2O4 or N2O5. Both reactions proceed by an SN2 mechanism. The products are ClNO and ClNO2, precursors of atmospheric atomic chlorine. Because this mechanism cannot result from a cluster too small for HCl ionization, an extended water film model was simulated. The results explain ClNO formation experiments. Predicted ClNO2 formation is less efficient. (iii) Ionization of acids at ice surfaces. No ionization is found on ideal crystalline surfaces, but the process is efficient on isolated defects where it involves formation of H3O(+)-acid anion contact ion pairs. This behavior is found in simulations of a model of the ice quasi-liquid layer corresponding to large defect concentrations in crystalline ice. The results are in accord with experiments. (iv) Ionization of acids on wet quartz. A monolayer of water on hydroxylated silica is ordered even at room temperature, but the surface lattice constant differs significantly from that of crystalline ice. The ionization processes of HCl and H2SO4 are of high yield and occur in a few picoseconds. The results are in accord with experimental spectroscopy. (v) Photochemical reactions on water and ice. These simulations require excited state quantum chemical methods. The electronic absorption spectrum of methyl hydroperoxide adsorbed on a large ice cluster is strongly blue-shifted relative to the isolated molecule. The measured and calculated adsorption band low-frequency tails are in agreement. A simple model of photodynamics assumes prompt electronic relaxation of the excited peroxide due to the ice surface. SEMD simulations support this, with the important finding that the photochemistry takes place mainly on the ground state. In conclusion, dynamics simulations using quantum chemical potentials are a useful tool in atmospheric chemistry of water media, capable of comparison with experiment.

Efficient simultaneous dense coding and teleportation with two-photon four-qubit cluster states

NASA Astrophysics Data System (ADS)

Zhang, Cai; Situ, Haozhen; Li, Qin; He, Guang Ping

2016-08-01

We firstly propose a simultaneous dense coding protocol with two-photon four-qubit cluster states in which two receivers can simultaneously get their respective classical information sent by a sender. Because each photon has two degrees of freedom, the protocol will achieve a high transmittance. The security of the simultaneous dense coding protocol has also been analyzed. Secondly, we investigate how to simultaneously teleport two different quantum states with polarization and path degree of freedom using cluster states to two receivers, respectively, and discuss its security. The preparation and transmission of two-photon four-qubit cluster states is less difficult than that of four-photon entangled states, and it has been experimentally generated with nearly perfect fidelity and high generation rate. Thus, our protocols are feasible with current quantum techniques.

Improving the accuracy of Møller-Plesset perturbation theory with neural networks

NASA Astrophysics Data System (ADS)

McGibbon, Robert T.; Taube, Andrew G.; Donchev, Alexander G.; Siva, Karthik; Hernández, Felipe; Hargus, Cory; Law, Ka-Hei; Klepeis, John L.; Shaw, David E.

2017-10-01

Noncovalent interactions are of fundamental importance across the disciplines of chemistry, materials science, and biology. Quantum chemical calculations on noncovalently bound complexes, which allow for the quantification of properties such as binding energies and geometries, play an essential role in advancing our understanding of, and building models for, a vast array of complex processes involving molecular association or self-assembly. Because of its relatively modest computational cost, second-order Møller-Plesset perturbation (MP2) theory is one of the most widely used methods in quantum chemistry for studying noncovalent interactions. MP2 is, however, plagued by serious errors due to its incomplete treatment of electron correlation, especially when modeling van der Waals interactions and π-stacked complexes. Here we present spin-network-scaled MP2 (SNS-MP2), a new semi-empirical MP2-based method for dimer interaction-energy calculations. To correct for errors in MP2, SNS-MP2 uses quantum chemical features of the complex under study in conjunction with a neural network to reweight terms appearing in the total MP2 interaction energy. The method has been trained on a new data set consisting of over 200 000 complete basis set (CBS)-extrapolated coupled-cluster interaction energies, which are considered the gold standard for chemical accuracy. SNS-MP2 predicts gold-standard binding energies of unseen test compounds with a mean absolute error of 0.04 kcal mol-1 (root-mean-square error 0.09 kcal mol-1), a 6- to 7-fold improvement over MP2. To the best of our knowledge, its accuracy exceeds that of all extant density functional theory- and wavefunction-based methods of similar computational cost, and is very close to the intrinsic accuracy of our benchmark coupled-cluster methodology itself. Furthermore, SNS-MP2 provides reliable per-conformation confidence intervals on the predicted interaction energies, a feature not available from any alternative method.

Improving the accuracy of Møller-Plesset perturbation theory with neural networks.

PubMed

McGibbon, Robert T; Taube, Andrew G; Donchev, Alexander G; Siva, Karthik; Hernández, Felipe; Hargus, Cory; Law, Ka-Hei; Klepeis, John L; Shaw, David E

2017-10-28

Noncovalent interactions are of fundamental importance across the disciplines of chemistry, materials science, and biology. Quantum chemical calculations on noncovalently bound complexes, which allow for the quantification of properties such as binding energies and geometries, play an essential role in advancing our understanding of, and building models for, a vast array of complex processes involving molecular association or self-assembly. Because of its relatively modest computational cost, second-order Møller-Plesset perturbation (MP2) theory is one of the most widely used methods in quantum chemistry for studying noncovalent interactions. MP2 is, however, plagued by serious errors due to its incomplete treatment of electron correlation, especially when modeling van der Waals interactions and π-stacked complexes. Here we present spin-network-scaled MP2 (SNS-MP2), a new semi-empirical MP2-based method for dimer interaction-energy calculations. To correct for errors in MP2, SNS-MP2 uses quantum chemical features of the complex under study in conjunction with a neural network to reweight terms appearing in the total MP2 interaction energy. The method has been trained on a new data set consisting of over 200 000 complete basis set (CBS)-extrapolated coupled-cluster interaction energies, which are considered the gold standard for chemical accuracy. SNS-MP2 predicts gold-standard binding energies of unseen test compounds with a mean absolute error of 0.04 kcal mol -1 (root-mean-square error 0.09 kcal mol -1 ), a 6- to 7-fold improvement over MP2. To the best of our knowledge, its accuracy exceeds that of all extant density functional theory- and wavefunction-based methods of similar computational cost, and is very close to the intrinsic accuracy of our benchmark coupled-cluster methodology itself. Furthermore, SNS-MP2 provides reliable per-conformation confidence intervals on the predicted interaction energies, a feature not available from any alternative method.

Physical-depth architectural requirements for generating universal photonic cluster states

NASA Astrophysics Data System (ADS)

Morley-Short, Sam; Bartolucci, Sara; Gimeno-Segovia, Mercedes; Shadbolt, Pete; Cable, Hugo; Rudolph, Terry

2018-01-01

Most leading proposals for linear-optical quantum computing (LOQC) use cluster states, which act as a universal resource for measurement-based (one-way) quantum computation. In ballistic approaches to LOQC, cluster states are generated passively from small entangled resource states using so-called fusion operations. Results from percolation theory have previously been used to argue that universal cluster states can be generated in the ballistic approach using schemes which exceed the critical threshold for percolation, but these results consider cluster states with unbounded size. Here we consider how successful percolation can be maintained using a physical architecture with fixed physical depth, assuming that the cluster state is continuously generated and measured, and therefore that only a finite portion of it is visible at any one point in time. We show that universal LOQC can be implemented using a constant-size device with modest physical depth, and that percolation can be exploited using simple pathfinding strategies without the need for high-complexity algorithms.

Cluster State Quantum Computing

DTIC Science & Technology

2012-12-01

probability that the desired target gate ATar has been faithfully implemented on the computational modes given a successful measurement of the ancilla...modes: () = �(†)� 2 2(†) , (3) since Tr ( ATar † ATar )=2Mc for a properly normalized target gate. As we are interested...optimization method we have developed maximizes the success probability S for a given target transformation ATar , for given ancilla resources, and for a

Cluster State Quantum Computation

DTIC Science & Technology

2014-02-01

information of relevance to the transformation. We define the fidelity as the probability that the desired target gate ATar has been faithfully...implemented on the computational modes given a successful measurement of the ancilla modes: 2 , (3) since Tr ( ATar † ATar )=2Mc for a properly normalized...photonic gates The optimization method we have developed maximizes the success probability S for a given target transformation ATar , for given

Kinematics of the Doped Quantum Vortices in Superfluid Helium Droplets

NASA Astrophysics Data System (ADS)

Bernando, Charles; Vilesov, Andrey F.

2018-05-01

Recent observation of quantum vortices in superfluid 4He droplets measuring a few hundreds of nanometers in diameter involved decoration of vortex cores by clusters containing large numbers of Xe atoms, which served as X-ray contrast agents. Here, we report on the study of the kinematics of the combined vortex-cluster system in a cylinder and in a sphere. Equilibrium states, characterized by total angular momentum, L, were found by minimizing the total energy, E, which sums from the kinetic energy of the liquid due to the vortex and due to orbiting Xe clusters, as well as solvation energy of the cluster in the droplet. Calculations show that, at small mass of the cluster, the equilibrium displacement of the system from the rotation axis is close to that for the bare vortex. However, upon decrease in L beyond certain critical value, which is larger for heavier clusters, the displacement bifurcates toward the surface region, where the motion of the system is governed by the clusters. In addition, at even smaller L, bare orbiting clusters become energetically favorable, opening the possibility for the vortex to detach from the cluster and to annihilate at the droplet's surface.

Vibrational properties of gold nanoparticles obtained by green synthesis

NASA Astrophysics Data System (ADS)

Alvarez, Ramón A. B.; Cortez-Valadez, M.; Bueno, L. Oscar Neira; Britto Hurtado, R.; Rocha-Rocha, O.; Delgado-Beleño, Y.; Martinez-Nuñez, C. E.; Serrano-Corrales, Luis Ivan; Arizpe-Chávez, H.; Flores-Acosta, M.

2016-10-01

This study reports the synthesis and characterization of gold nanoparticles through an ecological method to obtain nanostructures from the extract of the plant Opuntia ficus-indica. Colloidal nanoparticles show sizes that vary between 10-20 nm, and present various geometric morphologies. The samples were characterized through optical absorption, Raman Spectroscopy and Transmission Electron Microscopy (TEM). Additionally, low energy metallic clusters of Aun (n=2-20 atoms) were modeled by computational quantum chemistry. The theoretical results were obtained with Density Functional Theory (DFT). The predicted results of Au clusters show a tendency and are correlated with the experimental results concerning the optical absorption bands and Raman spectroscopy in gold nanoparticles.

Solutions of the two-dimensional Hubbard model: Benchmarks and results from a wide range of numerical algorithms

DOE PAGES

LeBlanc, J. P. F.; Antipov, Andrey E.; Becca, Federico; ...

2015-12-14

Numerical results for ground-state and excited-state properties (energies, double occupancies, and Matsubara-axis self-energies) of the single-orbital Hubbard model on a two-dimensional square lattice are presented, in order to provide an assessment of our ability to compute accurate results in the thermodynamic limit. Many methods are employed, including auxiliary-field quantum Monte Carlo, bare and bold-line diagrammatic Monte Carlo, method of dual fermions, density matrix embedding theory, density matrix renormalization group, dynamical cluster approximation, diffusion Monte Carlo within a fixed-node approximation, unrestricted coupled cluster theory, and multireference projected Hartree-Fock methods. Comparison of results obtained by different methods allows for the identification ofmore » uncertainties and systematic errors. The importance of extrapolation to converged thermodynamic-limit values is emphasized. Furthermore, cases where agreement between different methods is obtained establish benchmark results that may be useful in the validation of new approaches and the improvement of existing methods.« less

Prediction of tautomer ratios by embedded-cluster integral equation theory

NASA Astrophysics Data System (ADS)

Kast, Stefan M.; Heil, Jochen; Güssregen, Stefan; Schmidt, K. Friedemann

2010-04-01

The "embedded cluster reference interaction site model" (EC-RISM) approach combines statistical-mechanical integral equation theory and quantum-chemical calculations for predicting thermodynamic data for chemical reactions in solution. The electronic structure of the solute is determined self-consistently with the structure of the solvent that is described by 3D RISM integral equation theory. The continuous solvent-site distribution is mapped onto a set of discrete background charges ("embedded cluster") that represent an additional contribution to the molecular Hamiltonian. The EC-RISM analysis of the SAMPL2 challenge set of tautomers proceeds in three stages. Firstly, the group of compounds for which quantitative experimental free energy data was provided was taken to determine appropriate levels of quantum-chemical theory for geometry optimization and free energy prediction. Secondly, the resulting workflow was applied to the full set, allowing for chemical interpretations of the results. Thirdly, disclosure of experimental data for parts of the compounds facilitated a detailed analysis of methodical issues and suggestions for future improvements of the model. Without specifically adjusting parameters, the EC-RISM model yields the smallest value of the root mean square error for the first set (0.6 kcal mol-1) as well as for the full set of quantitative reaction data (2.0 kcal mol-1) among the SAMPL2 participants.

An orientation analysis method for protein immobilized on quantum dot particles

NASA Astrophysics Data System (ADS)

Aoyagi, Satoka; Inoue, Masae

2009-11-01

The evaluation of orientation of biomolecules immobilized on nanodevices is crucial for the development of high performance devices. Such analysis requires ultra high sensitivity so as to be able to detect less than one molecular layer on a device. Time-of-flight secondary ion mass spectrometry (TOF-SIMS) has sufficient sensitivity to evaluate the uppermost surface structure of a single molecular layer. The objective of this study is to develop an orientation analysis method for proteins immobilized on nanomaterials such as quantum dot particles, and to evaluate the orientation of streptavidin immobilized on quantum dot particles by means of TOF-SIMS. In order to detect fragment ions specific to the protein surface, a monoatomic primary ion source (Ga +) and a cluster ion source (Au 3+) were employed. Streptavidin-immobilized quantum dot particles were immobilized on aminosilanized ITO glass plates at amino groups by covalent bonding. The reference samples streptavidin directly immobilized on ITO plates were also prepared. All samples were dried with a freeze dryer before TOF-SIMS measurement. The positive secondary ion spectra of each sample were obtained using TOF-SIMS with Ga + and Au 3+, respectively, and then they were compared so as to characterize each sample and detect the surface structure of the streptavidin immobilized with the biotin-immobilized quantum dots. The chemical structures of the upper surface of the streptavidin molecules immobilized on the quantum dot particles were evaluated with TOF-SIMS spectra analysis. The indicated surface side of the streptavidin molecules immobilized on the quantum dots includes the biotin binding site.

Route to the Smallest Doped Semiconductor: Mn(2+)-Doped (CdSe)13 Clusters.

PubMed

Yang, Jiwoong; Fainblat, Rachel; Kwon, Soon Gu; Muckel, Franziska; Yu, Jung Ho; Terlinden, Hendrik; Kim, Byung Hyo; Iavarone, Dino; Choi, Moon Kee; Kim, In Young; Park, Inchul; Hong, Hyo-Ki; Lee, Jihwa; Son, Jae Sung; Lee, Zonghoon; Kang, Kisuk; Hwang, Seong-Ju; Bacher, Gerd; Hyeon, Taeghwan

2015-10-14

Doping semiconductor nanocrystals with magnetic transition-metal ions has attracted fundamental interest to obtain a nanoscale dilute magnetic semiconductor, which has unique spin exchange interaction between magnetic spin and exciton. So far, the study on the doped semiconductor NCs has usually been conducted with NCs with larger than 2 nm because of synthetic challenges. Herein, we report the synthesis and characterization of Mn(2+)-doped (CdSe)13 clusters, the smallest doped semiconductors. In this study, single-sized doped clusters are produced in large scale. Despite their small size, these clusters have semiconductor band structure instead of that of molecules. Surprisingly, the clusters show multiple excitonic transitions with different magneto-optical activities, which can be attributed to the fine structure splitting. Magneto-optically active states exhibit giant Zeeman splittings up to elevated temperatures (128 K) with large g-factors of 81(±8) at 4 K. Our results present a new synthetic method for doped clusters and facilitate the understanding of doped semiconductor at the boundary of molecules and quantum nanostructure.

Surfactant-controlled polymerization of semiconductor clusters to quantum dots through competing step-growth and living chain-growth mechanisms.

PubMed

Evans, Christopher M; Love, Alyssa M; Weiss, Emily A

2012-10-17

This article reports control of the competition between step-growth and living chain-growth polymerization mechanisms in the formation of cadmium chalcogenide colloidal quantum dots (QDs) from CdSe(S) clusters by varying the concentration of anionic surfactant in the synthetic reaction mixture. The growth of the particles proceeds by step-addition from initially nucleated clusters in the absence of excess phosphinic or carboxylic acids, which adsorb as their anionic conjugate bases, and proceeds indirectly by dissolution of clusters, and subsequent chain-addition of monomers to stable clusters (Ostwald ripening) in the presence of excess phosphinic or carboxylic acid. Fusion of clusters by step-growth polymerization is an explanation for the consistent observation of so-called "magic-sized" clusters in QD growth reactions. Living chain-addition (chain addition with no explicit termination step) produces QDs over a larger range of sizes with better size dispersity than step-addition. Tuning the molar ratio of surfactant to Se(2-)(S(2-)), the limiting ionic reagent, within the living chain-addition polymerization allows for stoichiometric control of QD radius without relying on reaction time.

Cloud Quantum Computing of an Atomic Nucleus

NASA Astrophysics Data System (ADS)

Dumitrescu, E. F.; McCaskey, A. J.; Hagen, G.; Jansen, G. R.; Morris, T. D.; Papenbrock, T.; Pooser, R. C.; Dean, D. J.; Lougovski, P.

2018-05-01

We report a quantum simulation of the deuteron binding energy on quantum processors accessed via cloud servers. We use a Hamiltonian from pionless effective field theory at leading order. We design a low-depth version of the unitary coupled-cluster ansatz, use the variational quantum eigensolver algorithm, and compute the binding energy to within a few percent. Our work is the first step towards scalable nuclear structure computations on a quantum processor via the cloud, and it sheds light on how to map scientific computing applications onto nascent quantum devices.

Cloud Quantum Computing of an Atomic Nucleus

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dumitrescu, Eugene F.; McCaskey, Alex J.; Hagen, Gaute

Here, we report a quantum simulation of the deuteron binding energy on quantum processors accessed via cloud servers. We use a Hamiltonian from pionless effective field theory at leading order. We design a low-depth version of the unitary coupled-cluster ansatz, use the variational quantum eigensolver algorithm, and compute the binding energy to within a few percent. Our work is the first step towards scalable nuclear structure computations on a quantum processor via the cloud, and it sheds light on how to map scientific computing applications onto nascent quantum devices.

Cloud Quantum Computing of an Atomic Nucleus.

PubMed

Dumitrescu, E F; McCaskey, A J; Hagen, G; Jansen, G R; Morris, T D; Papenbrock, T; Pooser, R C; Dean, D J; Lougovski, P

2018-05-25

We report a quantum simulation of the deuteron binding energy on quantum processors accessed via cloud servers. We use a Hamiltonian from pionless effective field theory at leading order. We design a low-depth version of the unitary coupled-cluster ansatz, use the variational quantum eigensolver algorithm, and compute the binding energy to within a few percent. Our work is the first step towards scalable nuclear structure computations on a quantum processor via the cloud, and it sheds light on how to map scientific computing applications onto nascent quantum devices.

Cloud Quantum Computing of an Atomic Nucleus

DOE PAGES

Dumitrescu, Eugene F.; McCaskey, Alex J.; Hagen, Gaute; ...

2018-05-23

Here, we report a quantum simulation of the deuteron binding energy on quantum processors accessed via cloud servers. We use a Hamiltonian from pionless effective field theory at leading order. We design a low-depth version of the unitary coupled-cluster ansatz, use the variational quantum eigensolver algorithm, and compute the binding energy to within a few percent. Our work is the first step towards scalable nuclear structure computations on a quantum processor via the cloud, and it sheds light on how to map scientific computing applications onto nascent quantum devices.

Demonstration of measurement-only blind quantum computing

NASA Astrophysics Data System (ADS)

Greganti, Chiara; Roehsner, Marie-Christine; Barz, Stefanie; Morimae, Tomoyuki; Walther, Philip

2016-01-01

Blind quantum computing allows for secure cloud networks of quasi-classical clients and a fully fledged quantum server. Recently, a new protocol has been proposed, which requires a client to perform only measurements. We demonstrate a proof-of-principle implementation of this measurement-only blind quantum computing, exploiting a photonic setup to generate four-qubit cluster states for computation and verification. Feasible technological requirements for the client and the device-independent blindness make this scheme very applicable for future secure quantum networks.

On the importance of an accurate representation of the initial state of the system in classical dynamics simulations

NASA Astrophysics Data System (ADS)

García-Vela, A.

2000-05-01

A definition of a quantum-type phase-space distribution is proposed in order to represent the initial state of the system in a classical dynamics simulation. The central idea is to define an initial quantum phase-space state of the system as the direct product of the coordinate and momentum representations of the quantum initial state. The phase-space distribution is then obtained as the square modulus of this phase-space state. The resulting phase-space distribution closely resembles the quantum nature of the system initial state. The initial conditions are sampled with the distribution, using a grid technique in phase space. With this type of sampling the distribution of initial conditions reproduces more faithfully the shape of the original phase-space distribution. The method is applied to generate initial conditions describing the three-dimensional state of the Ar-HCl cluster prepared by ultraviolet excitation. The photodissociation dynamics is simulated by classical trajectories, and the results are compared with those of a wave packet calculation. The classical and quantum descriptions are found in good agreement for those dynamical events less subject to quantum effects. The classical result fails to reproduce the quantum mechanical one for the more strongly quantum features of the dynamics. The properties and applicability of the phase-space distribution and the sampling technique proposed are discussed.

QDENSITY—A Mathematica Quantum Computer simulation

NASA Astrophysics Data System (ADS)

Juliá-Díaz, Bruno; Burdis, Joseph M.; Tabakin, Frank

2006-06-01

This Mathematica 5.2 package is a simulation of a Quantum Computer. The program provides a modular, instructive approach for generating the basic elements that make up a quantum circuit. The main emphasis is on using the density matrix, although an approach using state vectors is also implemented in the package. The package commands are defined in Qdensity.m which contains the tools needed in quantum circuits, e.g., multiqubit kets, projectors, gates, etc. Selected examples of the basic commands are presented here and a tutorial notebook, Tutorial.nb is provided with the package (available on our website) that serves as a full guide to the package. Finally, application is made to a variety of relevant cases, including Teleportation, Quantum Fourier transform, Grover's search and Shor's algorithm, in separate notebooks: QFT.nb, Teleportation.nb, Grover.nb and Shor.nb where each algorithm is explained in detail. Finally, two examples of the construction and manipulation of cluster states, which are part of "one way computing" ideas, are included as an additional tool in the notebook Cluster.nb. A Mathematica palette containing most commands in QDENSITY is also included: QDENSpalette.nb. Program summaryTitle of program: QDENSITY Catalogue identifier: ADXH_v1_0 Program summary URL:http://cpc.cs.qub.ac.uk/summaries/ADXH_v1_0 Program available from: CPC Program Library, Queen's University of Belfast, N. Ireland Operating systems: Any which supports Mathematica; tested under Microsoft Windows XP, Macintosh OS X, and Linux FC4 Programming language used: Mathematica 5.2 No. of bytes in distributed program, including test data, etc.: 180 581 No. of lines in distributed program, including test data, etc.: 19 382 Distribution format: tar.gz Method of solution: A Mathematica package is provided which contains commands to create and analyze quantum circuits. Several Mathematica notebooks containing relevant examples: Teleportation, Shor's Algorithm and Grover's search are explained in detail. A tutorial, Tutorial.nb is also enclosed. QDENSITY is available at http://www.pitt.edu/~tabakin/QDENSITY.

Vortex clustering and universal scaling laws in two-dimensional quantum turbulence.

PubMed

Skaugen, Audun; Angheluta, Luiza

2016-03-01

We investigate numerically the statistics of quantized vortices in two-dimensional quantum turbulence using the Gross-Pitaevskii equation. We find that a universal -5/3 scaling law in the turbulent energy spectrum is intimately connected with the vortex statistics, such as number fluctuations and vortex velocity, which is also characterized by a similar scaling behavior. The -5/3 scaling law appearing in the power spectrum of vortex number fluctuations is consistent with the scenario of passive advection of isolated vortices by a turbulent superfluid velocity generated by like-signed vortex clusters. The velocity probability distribution of clustered vortices is also sensitive to spatial configurations, and exhibits a power-law tail distribution with a -5/3 exponent.

A homonuclear spin-pair filter for solid-state NMR based on adiabatic-passage techniques

NASA Astrophysics Data System (ADS)

Verel, René; Baldus, Marc; Ernst, Matthias; Meier, Beat H.

1998-05-01

A filtering scheme for the selection of spin pairs (and larger spin clusters) under fast magic-angle spinning is proposed. The scheme exploits the avoided level crossing in spin pairs during an adiabatic amplitude sweep through the so-called HORROR recoupling condition. The advantages over presently used double-quantum filters are twofold. (i) The maximum theoretical filter efficiency is, due to the adiabatic variation, 100% instead of 73% as for transient methods. (ii) Since the filter does not rely on the phase-cycling properties of the double-quantum coherence, there is no need to obtain the full double-quantum intensity for all spins in the sample at one single point in time. The only important requirement is that all coupled spins pass through a two-spin state during the amplitude sweep. This makes the pulse scheme robust with respect to rf-amplitude missetting, rf-field inhomogeneity and chemical-shift offset.

Quantum chemical modeling of enzymatic reactions: the case of 4-oxalocrotonate tautomerase.

PubMed

Sevastik, Robin; Himo, Fahmi

2007-12-01

The reaction mechanism of 4-oxalocrotonate tautomerase (4-OT) is studied using the density functional theory method B3LYP. This enzyme catalyzes the isomerisation of unconjugated alpha-keto acids to their conjugated isomers. Two different quantum chemical models of the active site are devised and the potential energy curves for the reaction are computed. The calculations support the proposed reaction mechanism in which Pro-1 acts as a base to shuttle a proton from the C3 to the C5 position of the substrate. The first step (proton transfer from C3 to proline) is shown to be the rate-limiting step. The energy of the charge-separated intermediate (protonated proline-deprotonated substrate) is calculated to be quite low, in accordance with measured pKa values. The results of the two models are used to evaluate the methodology employed in modeling enzyme active sites using quantum chemical cluster models.

Communication: A simplified coupled-cluster Lagrangian for polarizable embedding.

PubMed

Krause, Katharina; Klopper, Wim

2016-01-28

A simplified coupled-cluster Lagrangian, which is linear in the Lagrangian multipliers, is proposed for the coupled-cluster treatment of a quantum mechanical system in a polarizable environment. In the simplified approach, the amplitude equations are decoupled from the Lagrangian multipliers and the energy obtained from the projected coupled-cluster equation corresponds to a stationary point of the Lagrangian.

Communication: A simplified coupled-cluster Lagrangian for polarizable embedding

DOE Office of Scientific and Technical Information (OSTI.GOV)

Krause, Katharina; Klopper, Wim, E-mail: klopper@kit.edu

A simplified coupled-cluster Lagrangian, which is linear in the Lagrangian multipliers, is proposed for the coupled-cluster treatment of a quantum mechanical system in a polarizable environment. In the simplified approach, the amplitude equations are decoupled from the Lagrangian multipliers and the energy obtained from the projected coupled-cluster equation corresponds to a stationary point of the Lagrangian.

PREFACE: Advanced many-body and statistical methods in mesoscopic systems

NASA Astrophysics Data System (ADS)

Anghel, Dragos Victor; Sabin Delion, Doru; Sorin Paraoanu, Gheorghe

2012-02-01

It has increasingly been realized in recent times that the borders separating various subfields of physics are largely artificial. This is the case for nanoscale physics, physics of lower-dimensional systems and nuclear physics, where the advanced techniques of many-body theory developed in recent times could provide a unifying framework for these disciplines under the general name of mesoscopic physics. Other fields, such as quantum optics and quantum information, are increasingly using related methods. The 6-day conference 'Advanced many-body and statistical methods in mesoscopic systems' that took place in Constanta, Romania, between 27 June and 2 July 2011 was, we believe, a successful attempt at bridging an impressive list of topical research areas: foundations of quantum physics, equilibrium and non-equilibrium quantum statistics/fractional statistics, quantum transport, phases and phase transitions in mesoscopic systems/superfluidity and superconductivity, quantum electromechanical systems, quantum dissipation, dephasing, noise and decoherence, quantum information, spin systems and their dynamics, fundamental symmetries in mesoscopic systems, phase transitions, exactly solvable methods for mesoscopic systems, various extension of the random phase approximation, open quantum systems, clustering, decay and fission modes and systematic versus random behaviour of nuclear spectra. This event brought together participants from seventeen countries and five continents. Each of the participants brought considerable expertise in his/her field of research and, at the same time, was exposed to the newest results and methods coming from the other, seemingly remote, disciplines. The talks touched on subjects that are at the forefront of topical research areas and we hope that the resulting cross-fertilization of ideas will lead to new, interesting results from which everybody will benefit. We are grateful for the financial and organizational support from IFIN-HH, Ovidius University (where the conference took place), the Academy of Romanian Scientists and the Romanian National Authority for Scientific Research. This conference proceedings volume brings together some of the invited and contributed talks of the conference. The hope of the editors is that they will constitute reference material for applying many-body techniques to problems in mesoscopic and nuclear physics. We thank all the participants for their contribution to the success of this conference. D V Anghel and D S Delion IFIN-HH, Bucharest, Romania G S Paraoanu Aalto University, Finland Conference photograph

Protein-protected luminescent noble metal quantum clusters: an emerging trend in atomic cluster nanoscience

PubMed Central

Xavier, Paulrajpillai Lourdu; Chaudhari, Kamalesh; Baksi, Ananya; Pradeep, Thalappil

2012-01-01

Noble metal quantum clusters (NMQCs) are the missing link between isolated noble metal atoms and nanoparticles. NMQCs are sub-nanometer core sized clusters composed of a group of atoms, most often luminescent in the visible region, and possess intriguing photo-physical and chemical properties. A trend is observed in the use of ligands, ranging from phosphines to functional proteins, for the synthesis of NMQCs in the liquid phase. In this review, we briefly overview recent advancements in the synthesis of protein protected NMQCs with special emphasis on their structural and photo-physical properties. In view of the protein protection, coupled with direct synthesis and easy functionalization, this hybrid QC-protein system is expected to have numerous optical and bioimaging applications in the future, pointers in this direction are visible in the literature. PMID:22312454

Geometric construction of quantum hall clustering Hamiltonians

DOE PAGES

Lee, Ching Hua; Papić, Zlatko; Thomale, Ronny

2015-10-08

In this study, many fractional quantum Hall wave functions are known to be unique highest-density zero modes of certain “pseudopotential” Hamiltonians. While a systematic method to construct such parent Hamiltonians has been available for the infinite plane and sphere geometries, the generalization to manifolds where relative angular momentum is not an exact quantum number, i.e., the cylinder or torus, remains an open problem. This is particularly true for non-Abelian states, such as the Read-Rezayi series (in particular, the Moore-Read and Read-Rezayi Z 3 states) and more exotic nonunitary (Haldane-Rezayi and Gaffnian) or irrational (Haffnian) states, whose parent Hamiltonians involve complicatedmore » many-body interactions. Here, we develop a universal geometric approach for constructing pseudopotential Hamiltonians that is applicable to all geometries. Our method straightforwardly generalizes to the multicomponent SU(n) cases with a combination of spin or pseudospin (layer, subband, or valley) degrees of freedom. We demonstrate the utility of our approach through several examples, some of which involve non-Abelian multicomponent states whose parent Hamiltonians were previously unknown, and we verify the results by numerically computing their entanglement properties.« less

Energetics and solvation structure of a dihalogen dopant (I2) in (4)He clusters.

PubMed

Pérez de Tudela, Ricardo; Barragán, Patricia; Valdés, Álvaro; Prosmiti, Rita

2014-08-21

The energetics and structure of small HeNI2 clusters are analyzed as the size of the system changes, with N up to 38. The full interaction between the I2 molecule and the He atoms is based on analytical ab initio He-I2 potentials plus the He-He interaction, obtained from first-principle calculations. The most stable structures, as a function of the number of solvent He atoms, are obtained by employing an evolutionary algorithm and compared with CCSD(T) and MP2 ab initio computations. Further, the classical description is completed by explicitly including thermal corrections and quantum features, such as zero-point-energy values and spatial delocalization. From quantum PIMC calculations, the binding energies and radial/angular probability density distributions of the thermal equilibrium state for selected-size clusters are computed at a low temperature. The sequential formation of regular shell structures is analyzed and discussed for both classical and quantum treatments.

A high fat diet containing saturated but not unsaturated fatty acids enhances T cell receptor clustering on the nanoscale.

PubMed

Shaikh, Saame Raza; Boyle, Sarah; Edidin, Michael

2015-09-01

Cell culture studies show that the nanoscale lateral organization of surface receptors, their clustering or dispersion, can be altered by changing the lipid composition of the membrane bilayer. However, little is known about similar changes in vivo, which can be effected by changing dietary lipids. We describe the use of a newly developed method, k-space image correlation spectroscopy, kICS, for analysis of quantum dot fluorescence to show that a high fat diet can alter the nanometer-scale clustering of the murine T cell receptor, TCR, on the surface of naive CD4(+) T cells. We found that diets enriched primarily in saturated fatty acids increased TCR nanoscale clustering to a level usually seen only on activated cells. Diets enriched in monounsaturated or n-3 polyunsaturated fatty acids had no effect on TCR clustering. Also none of the high fat diets affected TCR clustering on the micrometer scale. Furthermore, the effect of the diets was similar in young and middle aged mice. Our data establish proof-of-principle that TCR nanoscale clustering is sensitive to the composition of dietary fat. Copyright © 2015 Elsevier Ltd. All rights reserved.

Ligand-protected gold clusters: the structure, synthesis and applications

NASA Astrophysics Data System (ADS)

Pichugina, D. A.; Kuz'menko, N. E.; Shestakov, A. F.

2015-11-01

Modern concepts of the structure and properties of atomic gold clusters protected by thiolate, selenolate, phosphine and phenylacetylene ligands are analyzed. Within the framework of the superatom theory, the 'divide and protect' approach and the structure rule, the stability and composition of a cluster are determined by the structure of the cluster core, the type of ligands and the total number of valence electrons. Methods of selective synthesis of gold clusters in solution and on the surface of inorganic composites based, in particular, on the reaction of Aun with RS, RSe, PhC≡C, Hal ligands or functional groups of proteins, on stabilization of clusters in cavities of the α-, β and γ-cyclodextrin molecules (Au15 and Au25) and on anchorage to a support surface (Au25/SiO2, Au20/C, Au10/FeOx) are reviewed. Problems in this field are also discussed. Among the methods for cluster structure prediction, particular attention is given to the theoretical approaches based on the density functional theory (DFT). The structures of a number of synthesized clusters are described using the results obtained by X-ray diffraction analysis and DFT calculations. A possible mechanism of formation of the SR(AuSR)n 'staple' units in the cluster shell is proposed. The structure and properties of bimetallic clusters MxAunLm (M=Pd, Pt, Ag, Cu) are discussed. The Pd or Pt atom is located at the centre of the cluster, whereas Ag and Cu atoms form bimetallic compounds in which the heteroatom is located on the surface of the cluster core or in the 'staple' units. The optical properties, fluorescence and luminescence of ligand-protected gold clusters originate from the quantum effects of the Au atoms in the cluster core and in the oligomeric SR(AuSR)x units in the cluster shell. Homogeneous and heterogeneous reactions catalyzed by atomic gold clusters are discussed in the context of the reaction mechanism and the nature of the active sites. The bibliography includes 345 references.

Hydrogen-vacancy-dislocation interactions in α-Fe

NASA Astrophysics Data System (ADS)

Tehranchi, A.; Zhang, X.; Lu, G.; Curtin, W. A.

2017-02-01

Atomistic simulations of the interactions between dislocations, hydrogen atoms, and vacancies are studied to assess the viability of a recently proposed mechanism for the formation of nanoscale voids in Fe-based steels in the presence of hydrogen. Quantum-mechanics/molecular-mechanics method calculations confirm molecular statics simulations based on embedded atom method (EAM) potential showing that individual vacancies on the compressive side of an edge dislocation can be transported with the dislocation as it glides. Molecular dynamics simulations based on EAM potential then show, however, that vacancy clusters in the glide plane of an approaching dislocation are annihilated or reduced in size by the creation of a double-jog/climb process that is driven by the huge reduction in energy accompanying vacancy annihilation. The effectiveness of annihilation/reduction processes is not reduced by the presence of hydrogen in the vacancy clusters because typical V-H cluster binding energies are much lower than the vacancy formation energy, except at very high hydrogen content in the cluster. Analysis of a range of configurations indicates that hydrogen plays no special role in stabilizing nanovoids against jog formation processes that shrink voids. Experimental observations of nanovoids on the fracture surfaces of steels must be due to as-yet undetermined processes.

Effective scheme for partitioning covalent bonds in density-functional embedding theory: From molecules to extended covalent systems.

PubMed

Huang, Chen; Muñoz-García, Ana Belén; Pavone, Michele

2016-12-28

Density-functional embedding theory provides a general way to perform multi-physics quantum mechanics simulations of large-scale materials by dividing the total system's electron density into a cluster's density and its environment's density. It is then possible to compute the accurate local electronic structures and energetics of the embedded cluster with high-level methods, meanwhile retaining a low-level description of the environment. The prerequisite step in the density-functional embedding theory is the cluster definition. In covalent systems, cutting across the covalent bonds that connect the cluster and its environment leads to dangling bonds (unpaired electrons). These represent a major obstacle for the application of density-functional embedding theory to study extended covalent systems. In this work, we developed a simple scheme to define the cluster in covalent systems. Instead of cutting covalent bonds, we directly split the boundary atoms for maintaining the valency of the cluster. With this new covalent embedding scheme, we compute the dehydrogenation energies of several different molecules, as well as the binding energy of a cobalt atom on graphene. Well localized cluster densities are observed, which can facilitate the use of localized basis sets in high-level calculations. The results are found to converge faster with the embedding method than the other multi-physics approach ONIOM. This work paves the way to perform the density-functional embedding simulations of heterogeneous systems in which different types of chemical bonds are present.

Quantum correlations and limit cycles in the driven-dissipative Heisenberg lattice

NASA Astrophysics Data System (ADS)

Owen, E. T.; Jin, J.; Rossini, D.; Fazio, R.; Hartmann, M. J.

2018-04-01

Driven-dissipative quantum many-body systems have attracted increasing interest in recent years as they lead to novel classes of quantum many-body phenomena. In particular, mean-field calculations predict limit cycle phases, slow oscillations instead of stationary states, in the long-time limit for a number of driven-dissipative quantum many-body systems. Using a cluster mean-field and a self-consistent Mori projector approach, we explore the persistence of such limit cycles as short range quantum correlations are taken into account in a driven-dissipative Heisenberg model.

Quantum Materials at the Nanoscale - Final Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cooper, Stephen Lance

The central aim of the Quantum Materials at the Nanoscale (QMN) cluster was to understand and control collective behavior involving the interplay of spins, orbitals, and charges, which governs many scientifically interesting and technologically important phenomena in numerous complex materials. Because these phenomena involve various competing interactions, and influence properties on many different length and energy scales in complex materials, tackling this important area of study motivated a collaborative effort that combined the diverse capabilities of QMN cluster experimentalists, the essential theoretical analysis provided by QMN cluster theorists, and the outstanding facilities and staff of the FSMRL. During the fundingmore » period 2007-2014, the DOE cluster grant for the Quantum Materials at the Nanoscale (QMN) cluster supported, at various times, 15 different faculty members (14 in Physics and 1 in Materials Science and Engineering), 7 postdoctoral research associates, and 57 physics and materials science PhD students. 41 of these PhD students have since graduated and have gone on to a variety of advanced technical positions at universities, industries, and national labs: 25 obtained postdoctoral positions at universities (14), industrial labs (2 at IBM), DOE national facilities (3 at Argonne National Laboratory, 1 at Brookhaven National Lab, 1 at Lawrence Berkeley National Lab, and 1 at Sandia National Lab), and other federal facilities (2 at NIST); 13 took various industrial positions, including positions at Intel (5), Quantum Design (1), Lasque Industries (1), Amazon (1), Bloomberg (1), and J.P. Morgan (1). Thus, the QMN grant provided the essential support for training a large number of technically advanced personnel who have now entered key national facilities, industries, and institutions. Additionally, during the period 2007-2015, the QMN cluster produced 159 publications (see pages 14-23), including 23 papers published in Physical Review Letters; 16 papers in Nature, Nature Physics, Nature Materials, or Nature Communications; 4 papers in Science, and 8 papers in Applied Physics Letters. In this report, we provide some key highlights of the collaborative projects in which the QMN cluster members have been involved since 2007.« less

Nuclear quantum effects in water clusters: the role of the molecular flexibility.

PubMed

González, Briesta S; Noya, Eva G; Vega, Carlos; Sesé, Luis M

2010-02-25

With the objective of establishing the importance of water flexibility in empirical models which explicitly include nuclear quantum effects, we have carried out path integral Monte Carlo simulations in water clusters with up to seven molecules. Two recently developed models have been used for comparison: the rigid TIP4PQ/2005 and the flexible q-TIP4P/F models, both inspired by the rigid TIP4P/2005 model. To obtain a starting configuration for our simulations, we have located the global minima for the rigid TIP4P/2005 and TIP4PQ/2005 models and for the flexible q-TIP4P/F model. All the structures are similar to those predicted by the rigid TIP4P potential showing that the charge distribution mainly determines the global minimum structure. For the flexible q-TIP4P/F model, we have studied the geometrical distortion upon isotopic substitution by studying tritiated water clusters. Our results show that tritiated water clusters exhibit an r(OT) distance shorter than the r(OH) distance in water clusters, not significant changes in the Phi(HOH) angle, and a lower average dipole moment than water clusters. We have also carried out classical simulations with the rigid TIP4PQ/2005 model showing that the rotational kinetic energy is greatly affected by quantum effects, but the translational kinetic energy is only slightly modified. The potential energy is also noticeably higher than in classical simulations. Finally, as a concluding remark, we have calculated the formation energies of water clusters using both models, finding that the formation energies predicted by the rigid TIP4PQ/2005 model are lower by roughly 0.6 kcal/mol than those of the flexible q-TIP4P/F model for clusters of moderate size, the origin of this difference coming mainly from the geometrical distortion of the water molecule in the clusters that causes an increase in the intramolecular potential energy.

LASER APPLICATIONS AND OTHER TOPICS IN QUANTUM ELECTRONICS: On gamma-ray spectra of metal nuclei in a metal-carbon cluster

NASA Astrophysics Data System (ADS)

Rivlin, Lev A.

2007-07-01

The resonance absorption and emission gamma-ray spectra are constructed for nuclear transitions in metals in large metal-carbon clusters. The possibilities of observing gamma lines with the natural linewidth in an isolated molecule and the suppression of the excess line broadening in an ensemble of molecules are estimated. The possibility of the appearance of the hidden population inversion of nuclear states and the quantum amplification of the type of coherent stimulated scattering is also analysed.

Exploring the atomic structure of 1.8nm monolayer-protected gold clusters with aberration-corrected STEM.

PubMed

Liu, Jian; Jian, Nan; Ornelas, Isabel; Pattison, Alexander J; Lahtinen, Tanja; Salorinne, Kirsi; Häkkinen, Hannu; Palmer, Richard E

2017-05-01

Monolayer-protected (MP) Au clusters present attractive quantum systems with a range of potential applications e.g. in catalysis. Knowledge of the atomic structure is needed to obtain a full understanding of their intriguing physical and chemical properties. Here we employed aberration-corrected scanning transmission electron microscopy (ac-STEM), combined with multislice simulations, to make a round-robin investigation of the atomic structure of chemically synthesised clusters with nominal composition Au 144 (SCH 2 CH 2 Ph) 60 provided by two different research groups. The MP Au clusters were "weighed" by the atom counting method, based on their integrated intensities in the high angle annular dark field (HAADF) regime and calibrated exponent of the Z dependence. For atomic structure analysis, we compared experimental images of hundreds of clusters, with atomic resolution, against a variety of structural models. Across the size range 123-151 atoms, only 3% of clusters matched the theoretically predicted Au 144 (SR) 60 structure, while a large proportion of the clusters were amorphous (i.e. did not match any model structure). However, a distinct ring-dot feature, characteristic of local icosahedral symmetry, was observed in about 20% of the clusters. Copyright © 2017. Published by Elsevier B.V.

Independent-Cluster Parametrizations of Wave Functions in Model Field Theories III. The Coupled-Cluster Phase Spaces and Their Geometrical Structure

NASA Astrophysics Data System (ADS)

Arponen, J. S.; Bishop, R. F.

1993-11-01

In this third paper of a series we study the structure of the phase spaces of the independent-cluster methods. These phase spaces are classical symplectic manifolds which provide faithful descriptions of the quantum mechanical pure states of an arbitrary system. They are "superspaces" in the sense that the full physical many-body or field-theoretic system is described by a point of the space, in contrast to "ordinary" spaces for which the state of the physical system is described rather by the whole space itself. We focus attention on the normal and extended coupled-cluster methods (NCCM and ECCM). Both methods provide parametrizations of the Hilbert space which take into account in increasing degrees of completeness the connectivity properties of the associated perturbative diagram structure. This corresponds to an increasing incorporation of locality into the description of the quantum system. As a result the degree of nonlinearity increases in the dynamical equations that govern the temporal evolution and determine the equilibrium state. Because of the nonlinearity, the structure of the manifold becomes geometrically complicated. We analyse the neighbourhood of the ground state of the one-mode anharmonic bosonic field theory and derive the nonlinear expansion beyond the linear response regime. The expansion is given in terms of normal-mode amplitudes, which provide the best local coordinate system close to the ground state. We generalize the treatment to other nonequilibrium states by considering the similarly defined normal coordinates around the corresponding phase space point. It is pointed out that the coupled-cluster method (CCM) maps display such features as (an)holonomy, or geometric phase. For example, a physical state may be represented by a number of different points on the CCM manifold. For this reason the whole phase spaces in the NCCM or ECCM cannot be covered by a single chart. To account for this non-Euclidean nature we introduce a suitable pseudo-Riemannian metric structure which is compatible with an important subset of all canonical transformations. It is then shown that the phase space of the configuration-interaction method is flat, namely the complex Euclidean space; that the NCCM manifold has zero curvature even though its Reimann tensor does not vanish; and that the ECCM manifold is intrinsically curved. It is pointed out that with the present metrization many of the dimensions of the ECCM phase space are effectively compactified and that the overall topological structure of the space is related to the distribution of the zeros of the Bargmann wave function.

SU-F-BRD-13: Quantum Annealing Applied to IMRT Beamlet Intensity Optimization

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nazareth, D; Spaans, J

Purpose: We report on the first application of quantum annealing (QA) to the process of beamlet intensity optimization for IMRT. QA is a new technology, which employs novel hardware and software techniques to address various discrete optimization problems in many fields. Methods: We apply the D-Wave Inc. proprietary hardware, which natively exploits quantum mechanical effects for improved optimization. The new QA algorithm, running on this hardware, is most similar to simulated annealing, but relies on natural processes to directly minimize the free energy of a system. A simple quantum system is slowly evolved into a classical system, representing the objectivemore » function. To apply QA to IMRT-type optimization, two prostate cases were considered. A reduced number of beamlets were employed, due to the current QA hardware limitation of ∼500 binary variables. The beamlet dose matrices were computed using CERR, and an objective function was defined based on typical clinical constraints, including dose-volume objectives. The objective function was discretized, and the QA method was compared to two standard optimization Methods: simulated annealing and Tabu search, run on a conventional computing cluster. Results: Based on several runs, the average final objective function value achieved by the QA was 16.9 for the first patient, compared with 10.0 for Tabu and 6.7 for the SA. For the second patient, the values were 70.7 for the QA, 120.0 for Tabu, and 22.9 for the SA. The QA algorithm required 27–38% of the time required by the other two methods. Conclusion: In terms of objective function value, the QA performance was similar to Tabu but less effective than the SA. However, its speed was 3–4 times faster than the other two methods. This initial experiment suggests that QA-based heuristics may offer significant speedup over conventional clinical optimization methods, as quantum annealing hardware scales to larger sizes.« less

Computational Role of Tunneling in a Programmable Quantum Annealer

NASA Technical Reports Server (NTRS)

Boixo, Sergio; Smelyanskiy, Vadim; Shabani, Alireza; Isakov, Sergei V.; Dykman, Mark; Amin, Mohammad; Mohseni, Masoud; Denchev, Vasil S.; Neven, Hartmut

2016-01-01

Quantum tunneling is a phenomenon in which a quantum state tunnels through energy barriers above the energy of the state itself. Tunneling has been hypothesized as an advantageous physical resource for optimization. Here we present the first experimental evidence of a computational role of multiqubit quantum tunneling in the evolution of a programmable quantum annealer. We developed a theoretical model based on a NIBA Quantum Master Equation to describe the multi-qubit dissipative cotunneling effects under the complex noise characteristics of such quantum devices.We start by considering a computational primitive, the simplest non-convex optimization problem consisting of just one global and one local minimum. The quantum evolutions enable tunneling to the global minimum while the corresponding classical paths are trapped in a false minimum. In our study the non-convex potentials are realized by frustrated networks of qubit clusters with strong intra-cluster coupling. We show that the collective effect of the quantum environment is suppressed in the critical phase during the evolution where quantum tunneling decides the right path to solution. In a later stage dissipation facilitates the multiqubit cotunneling leading to the solution state. The predictions of the model accurately describe the experimental data from the D-WaveII quantum annealer at NASA Ames. In our computational primitive the temperature dependence of the probability of success in the quantum model is opposite to that of the classical paths with thermal hopping. Specially, we provide an analysis of an optimization problem with sixteen qubits,demonstrating eight qubit cotunneling that increases success probabilities. Furthermore, we report results for larger problems with up to 200 qubits that contain the primitive as subproblems.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kira, M., E-mail: mackillo.kira@physik.uni-marburg.de

Atomic Bose–Einstein condensates (BECs) can be viewed as macroscopic objects where atoms form correlated atom clusters to all orders. Therefore, the presence of a BEC makes the direct use of the cluster-expansion approach–lucrative e.g. in semiconductor quantum optics–inefficient when solving the many-body kinetics of a strongly interacting Bose. An excitation picture is introduced with a nonunitary transformation that describes the system in terms of atom clusters within the normal component alone. The nontrivial properties of this transformation are systematically studied, which yields a cluster-expansion friendly formalism for a strongly interacting Bose gas. Its connections and corrections to the standard Hartree–Fock–Bogoliubov approachmore » are discussed and the role of the order parameter and the Bogoliubov excitations are identified. The resulting interaction effects are shown to visibly modify number fluctuations of the BEC. Even when the BEC has a nearly perfect second-order coherence, the BEC number fluctuations can still resolve interaction-generated non-Poissonian fluctuations. - Highlights: • Excitation picture expresses interacting Bose gas with few atom clusters. • Semiconductor and BEC many-body investigations are connected with cluster expansion. • Quantum statistics of BEC is identified in terms of atom clusters. • BEC number fluctuations show extreme sensitivity to many-body correlations. • Cluster-expansion friendly framework is established for an interacting Bose gas.« less

Fragmentation dynamics of ionized neon clusters (Ne(n), n=3-14) embedded in helium nanodroplets.

PubMed

Bonhommeau, David; Halberstadt, Nadine; Viel, Alexandra

2006-01-14

We report a theoretical study of the nonadiabatic fragmentation dynamics of ionized neon clusters embedded in helium nanodroplets for cluster sizes up to n=14 atoms. The dynamics of the neon atoms is modeled using the molecular dynamics with quantum transitions method of Tully [J. Chem. Phys. 93, 1061 (1990)] with the nuclei treated classically and transitions between electronic states quantum mechanically. The potential-energy surfaces are derived from a diatomics-in-molecules model to which induced dipole-induced dipole interactions are added. The effect of the spin-orbit interaction is also discussed. The helium environment is modeled by a friction force acting on charged atoms whose speed exceeds the critical Landau velocity. The dependence of the fragment size distribution on the friction strength and on the initial nanodroplet size is investigated. By comparing with the available experimental data obtained for Ne3+ and Ne4+, a reasonable value for the friction coefficient, the only parameter of the model, is deduced. This value is then used to predict the effect of the helium environment on the dissociation dynamics of larger neon clusters, n=5-14. The results show stabilization of larger fragments than in the gas phase, but fragmentation is not completely caged. In addition, two types of dynamics are characterized for Ne4+: fast and explosive, therefore leaving no time for friction to cool down the process when dynamics starts on one of the highest electronic states, and slower, therefore leading to some stabilization by helium when it starts on one of the lowest electronic states.

Exponential Potential versus Dark Matter

DTIC Science & Technology

1993-10-15

scale of the solar system. Galaxy, Dark matter , Galaxy cluster, Gravitation, Quantum gravity...A two parameter exponential potential explains the anomalous kinematics of galaxies and galaxy clusters without need for the myriad ad hoc dark ... matter models currently in vogue. It also explains much about the scales and structures of galaxies and galaxy clusters while being quite negligible on the

Guanidine: A Highly Efficient Stabilizer in Atmospheric New-Particle Formation.

PubMed

Myllys, Nanna; Ponkkonen, Tuomo; Passananti, Monica; Elm, Jonas; Vehkamäki, Hanna; Olenius, Tinja

2018-05-24

The role of a strong organobase, guanidine, in sulfuric acid-driven new-particle formation is studied using state-of-the-art quantum chemical methods and molecular cluster formation simulations. Cluster formation mechanisms at the molecular level are resolved, and theoretical results on cluster stability are confirmed with mass spectrometer measurements. New-particle formation from guanidine and sulfuric acid molecules occurs without thermodynamic barriers under studied conditions, and clusters are growing close to a 1:1 composition of acid and base. Evaporation rates of the most stable clusters are extremely low, which can be explained by the proton transfers and symmetrical cluster structures. We compare the ability of guanidine and dimethylamine to enhance sulfuric acid-driven particle formation and show that more than 2000-fold concentration of dimethylamine is needed to yield as efficient particle formation as in the case of guanidine. At similar conditions, guanidine yields 8 orders of magnitude higher particle formation rates compared to dimethylamine. Highly basic compounds such as guanidine may explain experimentally observed particle formation events at low precursor vapor concentrations, whereas less basic and more abundant bases such as ammonia and amines are likely to explain measurements at high concentrations.

Magnesium ferrite nanocrystal clusters for magnetorheological fluid with enhanced sedimentation stability

NASA Astrophysics Data System (ADS)

Wang, Guangshuo; Ma, Yingying; Li, Meixia; Cui, Guohua; Che, Hongwei; Mu, Jingbo; Zhang, Xiaoliang; Tong, Yu; Dong, Xufeng

2017-01-01

In this study, magnesium ferrite (MgFe2O4) nanocrystal clusters were synthesized using an ascorbic acid-assistant solvothermal method and evaluated as a candidate for magnetorheological (MR) fluid. The morphology, microstructure and magnetic properties of the MgFe2O4 nanocrystal clusters were investigated in detail by field emission scanning electron microscopy (FESEM), transmission electron microscope (TEM), thermogravimetric analyzer (TGA), X-ray diffraction (XRD) and superconducting quantum interference device (SQUID). The MgFe2O4 nanocrystal clusters were suspended in silicone oil to prepare MR fluid and the MR properties were tested using a Physica MCR301 rheometer fitted with a magneto-rheological module. The prepared MR fluid showed typical Bingham plastic behavior, changing from a liquid-like to a solid-like structure under an external magnetic field. Compared with the conventional carbonyl iron particles, MgFe2O4 nanocrystal clusters-based MR fluid demonstrated enhanced sedimentation stability due to the reduced mismatch in density between the particles and the carrier medium. In summary, the as-prepared MgFe2O4 nanocrystal clusters are regarded as a promising candidate for MR fluid with enhanced sedimentation stability.

Efficient quantum circuits for one-way quantum computing.

PubMed

Tanamoto, Tetsufumi; Liu, Yu-Xi; Hu, Xuedong; Nori, Franco

2009-03-13

While Ising-type interactions are ideal for implementing controlled phase flip gates in one-way quantum computing, natural interactions between solid-state qubits are most often described by either the XY or the Heisenberg models. We show an efficient way of generating cluster states directly using either the imaginary SWAP (iSWAP) gate for the XY model, or the sqrt[SWAP] gate for the Heisenberg model. Our approach thus makes one-way quantum computing more feasible for solid-state devices.

Gordon Research Conference on Crystal Growth (1990)

DTIC Science & Technology

1990-04-01

Labs, MH) 14. Cox Vapor Levitation Epitaxy of Quantum Wires and Wire-like Structures Using Laterally Propagating Surface Steps. (Bellcore, Red Bank) 15...introduced many new aspects of crystal growth, including strained layer superlattices, quantum cluster growth, and vertical zone melting of GaAs...Films 2. E. Bauser Semiconductor Liquid Phase Epitaxy: Growth and Properties of Layers and Heterostructures 3. M. L. Steigerwald Growth of Quantum

Building mechanical Greenberger-Horne-Zeilinger and cluster states by harnessing optomechanical quantum steerable correlations

NASA Astrophysics Data System (ADS)

Tan, Huatang; Wei, Yanghua; Li, Gaoxiang

2017-11-01

Greenberger-Horne-Zeilinger (GHZ) and cluster states are two typical kinds of multipartite entangled states and can respectively be used for realizing quantum networks and one-way computation. We propose a feasible scheme for generating Gaussian GHZ and cluster states of multiple mechanical oscillators by pulsed cavity optomechanics. In our scheme, each optomechanical cavity is driven by a blue-detuned pulse to establish quantum steerable correlations between the cavity output field and the mechanical oscillator, and the cavity outputs are combined at a beam-splitter array with given transmissivity and reflectivity for each beam splitter. We show that by harnessing the light-mechanical steerable correlations, the mechanical GHZ and cluster states can be realized via homodyne detection on the amplitude and phase quadratures of the output fields from the beam-splitter array. These achieved mechanical entangled states can be viewed as the output states of an effective mechanical beam-splitter array with the mechanical inputs prepared in squeezed states with the light-mechanical steering. The effects of detection efficiency and thermal noise on the achieved mechanical states are investigated. The present scheme does not require externally injected squeezing and it can also be applicable to other systems such as light-atomic-ensemble interface, apart from optomechanical systems.

Exploring the importance of quantum effects in nucleation: The archetypical Nen case

NASA Astrophysics Data System (ADS)

Unn-Toc, Wesley; Halberstadt, Nadine; Meier, Christoph; Mella, Massimo

2012-07-01

The effect of quantum mechanics (QM) on the details of the nucleation process is explored employing Ne clusters as test cases due to their semi-quantal nature. In particular, we investigate the impact of quantum mechanics on both condensation and dissociation rates in the framework of the microcanonical ensemble. Using both classical trajectories and two semi-quantal approaches (zero point averaged dynamics, ZPAD, and Gaussian-based time dependent Hartree, G-TDH) to model cluster and collision dynamics, we simulate the dissociation and monomer capture for Ne8 as a function of the cluster internal energy, impact parameter and collision speed. The results for the capture probability Ps(b) as a function of the impact parameter suggest that classical trajectories always underestimate capture probabilities with respect to ZPAD, albeit at most by 15%-20% in the cases we studied. They also do so in some important situations when using G-TDH. More interestingly, dissociation rates kdiss are grossly overestimated by classical mechanics, at least by one order of magnitude. We interpret both behaviours as mainly due to the reduced amount of kinetic energy available to a quantum cluster for a chosen total internal energy. We also find that the decrease in monomer dissociation energy due to zero point energy effects plays a key role in defining dissociation rates. In fact, semi-quantal and classical results for kdiss seem to follow a common "corresponding states" behaviour when the proper definition of internal and dissociation energies are used in a transition state model estimation of the evaporation rate constants.

First principles studies of electron tunneling in proteins

PubMed Central

Hayashi, Tomoyuki; Stuchebrukhov, Alexei A.

2014-01-01

A first principles study of electronic tunneling along the chain of seven Fe/S clusters in respiratory complex I, a key enzyme in the respiratory electron transport chain, is described. The broken-symmetry states of the Fe/S metal clusters calculated at both DFT and semi-empirical ZINDO levels were utilized to examine both the extremely weak electronic couplings between Fe/S clusters and the tunneling pathways, which provide a detailed atomistic-level description of the charge transfer process in the protein. One-electron tunneling approximation was found to hold within a reasonable accuracy, with only a moderate induced polarization of the core electrons. The method is demonstrated to be able to calculate accurately the coupling matrix elements as small as 10−4 cm−1. A distinct signature of the wave properties of electrons is observed as quantum interferences of multiple tunneling pathways. PMID:25383312

Initiating Molecular Growth in the Interstellar Medium via Dimeric Complexes of Observed Ions and Molecules

NASA Technical Reports Server (NTRS)

Bera, Partha P.; Head-Gordon, Martin; Lee, Timothy J.

2011-01-01

A feasible initiation step for particle growth in the interstellar medium (ISM) is simulated by means of ab quantum chemistry methods. The systems studied are dimer ions formed by pairing nitrogen containing small molecules known to exist in the ISM with ions of unsaturated hydrocarbons or vice versa. Complexation energies, structures of ensuing complexes and electronic excitation spectra of the encounter complexes are estimated using various quantum chemistry methods. Moller-Plesset perturbation theory (MP2, Z-averaged perturbation theory (ZAP2), coupled cluster singles and doubles with perturbative triples corrections (CCSD(T)), and density functional theory (DFT) methods (B3LYP) were employed along with the correlation consistent cc-pVTZ and aug-cc-pVTZ basis sets. Two types of complexes are predicted. One type of complex has electrostatic binding with moderate (7-20 kcal per mol) binding energies, that are nonetheless significantly stronger than typical van der Waals interactions between molecules of this size. The other type of complex develops strong covalent bonds between the fragments. Cyclic isomers of the nitrogen containing complexes are produced very easily by ion-molecule reactions. Some of these complexes show intense ultraviolet visible spectra for electronic transitions with large oscillator strengths at the B3LYP, omegaB97, and equations of motion coupled cluster (EOM-CCSD) levels. The open shell nitrogen containing carbonaceous complexes especially exhibit a large oscillator strength electronic transition in the visible region of the electromagnetic spectrum.

All-photonic quantum repeaters

PubMed Central

Azuma, Koji; Tamaki, Kiyoshi; Lo, Hoi-Kwong

2015-01-01

Quantum communication holds promise for unconditionally secure transmission of secret messages and faithful transfer of unknown quantum states. Photons appear to be the medium of choice for quantum communication. Owing to photon losses, robust quantum communication over long lossy channels requires quantum repeaters. It is widely believed that a necessary and highly demanding requirement for quantum repeaters is the existence of matter quantum memories. Here we show that such a requirement is, in fact, unnecessary by introducing the concept of all-photonic quantum repeaters based on flying qubits. In particular, we present a protocol based on photonic cluster-state machine guns and a loss-tolerant measurement equipped with local high-speed active feedforwards. We show that, with such all-photonic quantum repeaters, the communication efficiency scales polynomially with the channel distance. Our result paves a new route towards quantum repeaters with efficient single-photon sources rather than matter quantum memories. PMID:25873153

Will water act as a photocatalyst for cluster phase chemical reactions? Vibrational overtone-induced dehydration reaction of methanediol

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kramer, Zeb C.; Takahashi, Kaito; Skodje, Rex T.

2012-04-28

The possibility of water catalysis in the vibrational overtone-induced dehydration reaction of methanediol is investigated using ab initio dynamical simulations of small methanediol-water clusters. Quantum chemistry calculations employing clusters with one or two water molecules reveal that the barrier to dehydration is lowered by over 20 kcal/mol because of hydrogen-bonding at the transition state. Nevertheless, the simulations of the reaction dynamics following OH-stretch excitation show little catalytic effect of water and, in some cases, even show an anticatalytic effect. The quantum yield for the dehydration reaction exhibits a delayed threshold effect where reaction does not occur until the photon energymore » is far above the barrier energy. Unlike thermally induced reactions, it is argued that competition between reaction and the irreversible dissipation of photon energy may be expected to raise the dynamical threshold for the reaction above the transition state energy. It is concluded that quantum chemistry calculations showing barrier lowering are not sufficient to infer water catalysis in photochemical reactions, which instead require dynamical modeling.« less

Quantum Dynamics of Helium Clusters

DTIC Science & Technology

1993-03-01

the structure of both these and the HeN clusters in the body fixed frame by computing principal moments of inertia, thereby avoiding the...8217 of helium clusters, with the modification that we subtract 0.96 K from the computed values so that lor sufficiently large clusters we recover the...phonon spectrum of liquid He. To get a picture of these spectra one needs to compute the structure functions 51. Monte Carlo random walk simulations

Cluster-Continuum Calculations of Hydration Free Energies of Anions and Group 12 Divalent Cations.

PubMed

Riccardi, Demian; Guo, Hao-Bo; Parks, Jerry M; Gu, Baohua; Liang, Liyuan; Smith, Jeremy C

2013-01-08

Understanding aqueous phase processes involving group 12 metal cations is relevant to both environmental and biological sciences. Here, quantum chemical methods and polarizable continuum models are used to compute the hydration free energies of a series of divalent group 12 metal cations (Zn(2+), Cd(2+), and Hg(2+)) together with Cu(2+) and the anions OH(-), SH(-), Cl(-), and F(-). A cluster-continuum method is employed, in which gas-phase clusters of the ion and explicit solvent molecules are immersed in a dielectric continuum. Two approaches to define the size of the solute-water cluster are compared, in which the number of explicit waters used is either held constant or determined variationally as that of the most favorable hydration free energy. Results obtained with various polarizable continuum models are also presented. Each leg of the relevant thermodynamic cycle is analyzed in detail to determine how different terms contribute to the observed mean signed error (MSE) and the standard deviation of the error (STDEV) between theory and experiment. The use of a constant number of water molecules for each set of ions is found to lead to predicted relative trends that benefit from error cancellation. Overall, the best results are obtained with MP2 and the Solvent Model D polarizable continuum model (SMD), with eight explicit water molecules for anions and 10 for the metal cations, yielding a STDEV of 2.3 kcal mol(-1) and MSE of 0.9 kcal mol(-1) between theoretical and experimental hydration free energies, which range from -72.4 kcal mol(-1) for SH(-) to -505.9 kcal mol(-1) for Cu(2+). Using B3PW91 with DFT-D3 dispersion corrections (B3PW91-D) and SMD yields a STDEV of 3.3 kcal mol(-1) and MSE of 1.6 kcal mol(-1), to which adding MP2 corrections from smaller divalent metal cation water molecule clusters yields very good agreement with the full MP2 results. Using B3PW91-D and SMD, with two explicit water molecules for anions and six for divalent metal cations, also yields reasonable agreement with experimental values, due in part to fortuitous error cancellation associated with the metal cations. Overall, the results indicate that the careful application of quantum chemical cluster-continuum methods provides valuable insight into aqueous ionic processes that depend on both local and long-range electrostatic interactions with the solvent.

Statistical mechanics of the cluster Ising model

NASA Astrophysics Data System (ADS)

Smacchia, Pietro; Amico, Luigi; Facchi, Paolo; Fazio, Rosario; Florio, Giuseppe; Pascazio, Saverio; Vedral, Vlatko

2011-08-01

We study a Hamiltonian system describing a three-spin-1/2 clusterlike interaction competing with an Ising-like antiferromagnetic interaction. We compute free energy, spin-correlation functions, and entanglement both in the ground and in thermal states. The model undergoes a quantum phase transition between an Ising phase with a nonvanishing magnetization and a cluster phase characterized by a string order. Any two-spin entanglement is found to vanish in both quantum phases because of a nontrivial correlation pattern. Nevertheless, the residual multipartite entanglement is maximal in the cluster phase and dependent on the magnetization in the Ising phase. We study the block entropy at the critical point and calculate the central charge of the system, showing that the criticality of the system is beyond the Ising universality class.

Quantum Gibbs Samplers: The Commuting Case

NASA Astrophysics Data System (ADS)

Kastoryano, Michael J.; Brandão, Fernando G. S. L.

2016-06-01

We analyze the problem of preparing quantum Gibbs states of lattice spin Hamiltonians with local and commuting terms on a quantum computer and in nature. Our central result is an equivalence between the behavior of correlations in the Gibbs state and the mixing time of the semigroup which drives the system to thermal equilibrium (the Gibbs sampler). We introduce a framework for analyzing the correlation and mixing properties of quantum Gibbs states and quantum Gibbs samplers, which is rooted in the theory of non-commutative {mathbb{L}_p} spaces. We consider two distinct classes of Gibbs samplers, one of them being the well-studied Davies generator modelling the dynamics of a system due to weak-coupling with a large Markovian environment. We show that their spectral gap is independent of system size if, and only if, a certain strong form of clustering of correlations holds in the Gibbs state. Therefore every Gibbs state of a commuting Hamiltonian that satisfies clustering of correlations in this strong sense can be prepared efficiently on a quantum computer. As concrete applications of our formalism, we show that for every one-dimensional lattice system, or for systems in lattices of any dimension at temperatures above a certain threshold, the Gibbs samplers of commuting Hamiltonians are always gapped, giving an efficient way of preparing the associated Gibbs states on a quantum computer.

Error Sensitivity to Environmental Noise in Quantum Circuits for Chemical State Preparation.

PubMed

Sawaya, Nicolas P D; Smelyanskiy, Mikhail; McClean, Jarrod R; Aspuru-Guzik, Alán

2016-07-12

Calculating molecular energies is likely to be one of the first useful applications to achieve quantum supremacy, performing faster on a quantum than a classical computer. However, if future quantum devices are to produce accurate calculations, errors due to environmental noise and algorithmic approximations need to be characterized and reduced. In this study, we use the high performance qHiPSTER software to investigate the effects of environmental noise on the preparation of quantum chemistry states. We simulated 18 16-qubit quantum circuits under environmental noise, each corresponding to a unitary coupled cluster state preparation of a different molecule or molecular configuration. Additionally, we analyze the nature of simple gate errors in noise-free circuits of up to 40 qubits. We find that, in most cases, the Jordan-Wigner (JW) encoding produces smaller errors under a noisy environment as compared to the Bravyi-Kitaev (BK) encoding. For the JW encoding, pure dephasing noise is shown to produce substantially smaller errors than pure relaxation noise of the same magnitude. We report error trends in both molecular energy and electron particle number within a unitary coupled cluster state preparation scheme, against changes in nuclear charge, bond length, number of electrons, noise types, and noise magnitude. These trends may prove to be useful in making algorithmic and hardware-related choices for quantum simulation of molecular energies.

Spectroscopic accuracy directly from quantum chemistry: application to ground and excited states of beryllium dimer.

PubMed

Sharma, Sandeep; Yanai, Takeshi; Booth, George H; Umrigar, C J; Chan, Garnet Kin-Lic

2014-03-14

We combine explicit correlation via the canonical transcorrelation approach with the density matrix renormalization group and initiator full configuration interaction quantum Monte Carlo methods to compute a near-exact beryllium dimer curve, without the use of composite methods. In particular, our direct density matrix renormalization group calculations produce a well-depth of D(e) = 931.2 cm(-1) which agrees very well with recent experimentally derived estimates D(e) = 929.7±2 cm(-1) [J. M. Merritt, V. E. Bondybey, and M. C. Heaven, Science 324, 1548 (2009)] and D(e) = 934.6 cm(-1) [K. Patkowski, V. Špirko, and K. Szalewicz, Science 326, 1382 (2009)], as well the best composite theoretical estimates, D(e) = 938±15 cm(-1) [K. Patkowski, R. Podeszwa, and K. Szalewicz, J. Phys. Chem. A 111, 12822 (2007)] and D(e) = 935.1±10 cm(-1) [J. Koput, Phys. Chem. Chem. Phys. 13, 20311 (2011)]. Our results suggest possible inaccuracies in the functional form of the potential used at shorter bond lengths to fit the experimental data [J. M. Merritt, V. E. Bondybey, and M. C. Heaven, Science 324, 1548 (2009)]. With the density matrix renormalization group we also compute near-exact vertical excitation energies at the equilibrium geometry. These provide non-trivial benchmarks for quantum chemical methods for excited states, and illustrate the surprisingly large error that remains for 1 ¹Σ(g)⁻ state with approximate multi-reference configuration interaction and equation-of-motion coupled cluster methods. Overall, we demonstrate that explicitly correlated density matrix renormalization group and initiator full configuration interaction quantum Monte Carlo methods allow us to fully converge to the basis set and correlation limit of the non-relativistic Schrödinger equation in small molecules.

Psi4 1.1: An Open-Source Electronic Structure Program Emphasizing Automation, Advanced Libraries, and Interoperability.

PubMed

Parrish, Robert M; Burns, Lori A; Smith, Daniel G A; Simmonett, Andrew C; DePrince, A Eugene; Hohenstein, Edward G; Bozkaya, Uğur; Sokolov, Alexander Yu; Di Remigio, Roberto; Richard, Ryan M; Gonthier, Jérôme F; James, Andrew M; McAlexander, Harley R; Kumar, Ashutosh; Saitow, Masaaki; Wang, Xiao; Pritchard, Benjamin P; Verma, Prakash; Schaefer, Henry F; Patkowski, Konrad; King, Rollin A; Valeev, Edward F; Evangelista, Francesco A; Turney, Justin M; Crawford, T Daniel; Sherrill, C David

2017-07-11

Psi4 is an ab initio electronic structure program providing methods such as Hartree-Fock, density functional theory, configuration interaction, and coupled-cluster theory. The 1.1 release represents a major update meant to automate complex tasks, such as geometry optimization using complete-basis-set extrapolation or focal-point methods. Conversion of the top-level code to a Python module means that Psi4 can now be used in complex workflows alongside other Python tools. Several new features have been added with the aid of libraries providing easy access to techniques such as density fitting, Cholesky decomposition, and Laplace denominators. The build system has been completely rewritten to simplify interoperability with independent, reusable software components for quantum chemistry. Finally, a wide range of new theoretical methods and analyses have been added to the code base, including functional-group and open-shell symmetry adapted perturbation theory, density-fitted coupled cluster with frozen natural orbitals, orbital-optimized perturbation and coupled-cluster methods (e.g., OO-MP2 and OO-LCCD), density-fitted multiconfigurational self-consistent field, density cumulant functional theory, algebraic-diagrammatic construction excited states, improvements to the geometry optimizer, and the "X2C" approach to relativistic corrections, among many other improvements.

Comparison of memory thresholds for planar qudit geometries

NASA Astrophysics Data System (ADS)

Marks, Jacob; Jochym-O'Connor, Tomas; Gheorghiu, Vlad

2017-11-01

We introduce and analyze a new type of decoding algorithm called general color clustering, based on renormalization group methods, to be used in qudit color codes. The performance of this decoder is analyzed under a generalized bit-flip error model, and is used to obtain the first memory threshold estimates for qudit 6-6-6 color codes. The proposed decoder is compared with similar decoding schemes for qudit surface codes as well as the current leading qubit decoders for both sets of codes. We find that, as with surface codes, clustering performs sub-optimally for qubit color codes, giving a threshold of 5.6 % compared to the 8.0 % obtained through surface projection decoding methods. However, the threshold rate increases by up to 112% for large qudit dimensions, plateauing around 11.9 % . All the analysis is performed using QTop, a new open-source software for simulating and visualizing topological quantum error correcting codes.

Transport coefficients of Quark-Gluon plasma with full QCD potential

NASA Astrophysics Data System (ADS)

J. P., Prasanth; Bannur, Vishnu M.

2018-05-01

The shear viscosity η, bulk viscosity ζ and their ratio with the entropy density, η / s, ζ / s have been studied in a quark-gluon plasma (QGP) within the cluster expansion method. The cluster expansion method allows us to include the interaction between the partons in the deconfined phase and to calculate the equation of state of quark-gluon plasma. It has been argued that the interactions present in the equation of state, the modified Cornell potential significantly contributes to the viscosity. The results obtained within our approaches agree with lattice quantum chromodynamics (LQCD) equation of state. We obtained η / s ≈ 0 . 128 within the temperature range T /Tc ∈ [ 0 . 9 , 1 . 5 ] which is very close to the theoretical lower bound η / s ≥ 1 /(4 π) in Yang-Mills theory. We also demonstrate that the effects of ζ / s at freezeout are possibly large.

Bias-Free Chemically Diverse Test Sets from Machine Learning.

PubMed

Swann, Ellen T; Fernandez, Michael; Coote, Michelle L; Barnard, Amanda S

2017-08-14

Current benchmarking methods in quantum chemistry rely on databases that are built using a chemist's intuition. It is not fully understood how diverse or representative these databases truly are. Multivariate statistical techniques like archetypal analysis and K-means clustering have previously been used to summarize large sets of nanoparticles however molecules are more diverse and not as easily characterized by descriptors. In this work, we compare three sets of descriptors based on the one-, two-, and three-dimensional structure of a molecule. Using data from the NIST Computational Chemistry Comparison and Benchmark Database and machine learning techniques, we demonstrate the functional relationship between these structural descriptors and the electronic energy of molecules. Archetypes and prototypes found with topological or Coulomb matrix descriptors can be used to identify smaller, statistically significant test sets that better capture the diversity of chemical space. We apply this same method to find a diverse subset of organic molecules to demonstrate how the methods can easily be reapplied to individual research projects. Finally, we use our bias-free test sets to assess the performance of density functional theory and quantum Monte Carlo methods.

Electron correlation in the interacting quantum atoms partition via coupled-cluster lagrangian densities.

PubMed

Holguín-Gallego, Fernando José; Chávez-Calvillo, Rodrigo; García-Revilla, Marco; Francisco, Evelio; Pendás, Ángel Martín; Rocha-Rinza, Tomás

2016-07-15

The electronic energy partition established by the Interacting Quantum Atoms (IQA) approach is an important method of wavefunction analyses which has yielded valuable insights about different phenomena in physical chemistry. Most of the IQA applications have relied upon approximations, which do not include either dynamical correlation (DC) such as Hartree-Fock (HF) or external DC like CASSCF theory. Recently, DC was included in the IQA method by means of HF/Coupled-Cluster (CC) transition densities (Chávez-Calvillo et al., Comput. Theory Chem. 2015, 1053, 90). Despite the potential utility of this approach, it has a few drawbacks, for example, it is not consistent with the calculation of CC properties different from the total electronic energy. To improve this situation, we have implemented the IQA energy partition based on CC Lagrangian one- and two-electron orbital density matrices. The development presented in this article is tested and illustrated with the H2 , LiH, H2 O, H2 S, N2 , and CO molecules for which the IQA results obtained under the consideration of (i) the CC Lagrangian, (ii) HF/CC transition densities, and (iii) HF are critically analyzed and compared. Additionally, the effect of the DC in the different components of the electronic energy in the formation of the T-shaped (H2 )2 van der Waals cluster and the bimolecular nucleophilic substitution between F(-) and CH3 F is examined. We anticipate that the approach put forward in this article will provide new understandings on subjects in physical chemistry wherein DC plays a crucial role like molecular interactions along with chemical bonding and reactivity. © 2016 Wiley Periodicals, Inc. © 2016 Wiley Periodicals, Inc.

From Three-Photon Greenberger-Horne-Zeilinger States to Ballistic Universal Quantum Computation.

PubMed

Gimeno-Segovia, Mercedes; Shadbolt, Pete; Browne, Dan E; Rudolph, Terry

2015-07-10

Single photons, manipulated using integrated linear optics, constitute a promising platform for universal quantum computation. A series of increasingly efficient proposals have shown linear-optical quantum computing to be formally scalable. However, existing schemes typically require extensive adaptive switching, which is experimentally challenging and noisy, thousands of photon sources per renormalized qubit, and/or large quantum memories for repeat-until-success strategies. Our work overcomes all these problems. We present a scheme to construct a cluster state universal for quantum computation, which uses no adaptive switching, no large memories, and which is at least an order of magnitude more resource efficient than previous passive schemes. Unlike previous proposals, it is constructed entirely from loss-detecting gates and offers a robustness to photon loss. Even without the use of an active loss-tolerant encoding, our scheme naturally tolerates a total loss rate ∼1.6% in the photons detected in the gates. This scheme uses only 3 Greenberger-Horne-Zeilinger states as a resource, together with a passive linear-optical network. We fully describe and model the iterative process of cluster generation, including photon loss and gate failure. This demonstrates that building a linear-optical quantum computer needs to be less challenging than previously thought.

Entanglement percolation on a quantum internet with scale-free and clustering characters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu Liang; Zhu Shiqun

The applicability of entanglement percolation protocol to real Internet structure is investigated. If the current Internet can be used directly in the quantum regime, the protocol can provide a way to establish long-distance entanglement when the links are pure nonmaximally entangled states. This applicability is primarily due to the combination of scale-free degree distribution and a high level of clustering, both of which are widely observed in many natural and artificial networks including the current Internet. It suggests that the topology of real Internet may play an important role in entanglement establishment.

Entanglement percolation on a quantum internet with scale-free and clustering characters

NASA Astrophysics Data System (ADS)

Wu, Liang; Zhu, Shiqun

2011-11-01

The applicability of entanglement percolation protocol to real Internet structure is investigated. If the current Internet can be used directly in the quantum regime, the protocol can provide a way to establish long-distance entanglement when the links are pure nonmaximally entangled states. This applicability is primarily due to the combination of scale-free degree distribution and a high level of clustering, both of which are widely observed in many natural and artificial networks including the current Internet. It suggests that the topology of real Internet may play an important role in entanglement establishment.

Classical Optimal Control for Energy Minimization Based On Diffeomorphic Modulation under Observable-Response-Preserving Homotopy.

PubMed

Soley, Micheline B; Markmann, Andreas; Batista, Victor S

2018-06-12

We introduce the so-called "Classical Optimal Control Optimization" (COCO) method for global energy minimization based on the implementation of the diffeomorphic modulation under observable-response-preserving homotopy (DMORPH) gradient algorithm. A probe particle with time-dependent mass m( t;β) and dipole μ( r, t;β) is evolved classically on the potential energy surface V( r) coupled to an electric field E( t;β), as described by the time-dependent density of states represented on a grid, or otherwise as a linear combination of Gaussians generated by the k-means clustering algorithm. Control parameters β defining m( t;β), μ( r, t;β), and E( t;β) are optimized by following the gradients of the energy with respect to β, adapting them to steer the particle toward the global minimum energy configuration. We find that the resulting COCO algorithm is capable of resolving near-degenerate states separated by large energy barriers and successfully locates the global minima of golf potentials on flat and rugged surfaces, previously explored for testing quantum annealing methodologies and the quantum optimal control optimization (QuOCO) method. Preliminary results show successful energy minimization of multidimensional Lennard-Jones clusters. Beyond the analysis of energy minimization in the specific model systems investigated, we anticipate COCO should be valuable for solving minimization problems in general, including optimization of parameters in applications to machine learning and molecular structure determination.

Hybrid quantum and molecular mechanics embedded cluster models for chemistry on silicon and silicon carbide surfaces

NASA Astrophysics Data System (ADS)

Shoemaker, James Richard

Fabrication of silicon carbide (SiC) semiconductor devices are of interest for aerospace applications because of their high-temperature tolerance. Growth of an insulating SiO2 layer on SiC by oxidation is a poorly understood process, and sometimes produces interface defects that degrade device performance. Accurate theoretical models of surface chemistry, using quantum mechanics (QM), do not exist because of the huge computational cost of solving Schrodinger's equation for a molecular cluster large enough to represent a surface. Molecular mechanics (MM), which describes a molecule as a collection of atoms interacting through classical potentials, is a fast computational method, good at predicting molecular structure, but cannot accurately model chemical reactions. A new hybrid QM/MM computational method for surface chemistry was developed and applied to silicon and SiC surfaces. The addition of MM steric constraints was shown to have a large effect on the energetics of O atom adsorption on SiC. Adsorption of O atoms on Si-terminated SiC(111) favors above surface sites, in contrast to Si(111), but favors subsurface adsorption sites on C- terminated SiC(111). This difference, and the energetics of C atom etching via CO2 desorption, can explain the observed poor performance of SiC devices in which insulating layers were grown on C-terminated surfaces.

Particle-hole symmetry in many-body theories of electron correlation

NASA Astrophysics Data System (ADS)

Kats, Daniel; Usvyat, Denis; Manby, Frederick R.

2018-06-01

Second-quantised creation and annihilation operators for fermionic particles anticommute, but the same is true for the creation and annihilation operators for holes. This introduces a symmetry into the quantum theory of fermions that is absent for bosons. In ab initio electronic structure theory, it is common to classify methods by the number of electrons for which the method returns exact results: for example Hartree-Fock theory is exact for one-electron systems, whereas coupled-cluster theory with single and double excitations is exact for two-electron systems. Here, we discuss the generalisation: methods based on approximate wavefunctions that are exact for n-particle systems are also exact for n-hole systems. Novel electron correlation methods that attempt to improve on the coupled-cluster framework sometimes retain this property, and sometimes lose it. Here, we argue for retaining particle-hole symmetry as a desirable design criterion of approximate electron correlation methods. Dispensing with it might lead to loss of n-representability of density matrices, and this in turn can lead to spurious long-range behaviour in the correlation energy.

Electronic structure and orientation relationship of Li nanoclusters embedded in MgO studied by depth-selective positron annihilation two-dimensional angular correlation

NASA Astrophysics Data System (ADS)

Falub, C. V.; Mijnarends, P. E.; Eijt, S. W.; van Huis, M. A.; van Veen, A.; Schut, H.

2002-08-01

Quantum-confined positrons are sensitive probes for determining the electronic structure of nanoclusters embedded in materials. In this work, a depth-selective positron annihilation 2D-ACAR (two-dimensional angular correlation of annihilation radiation) method is used to determine the electronic structure of Li nanoclusters formed by implantation of 1016-cm-2 30-keV 6Li ions in MgO (100) and (110) crystals and by subsequent annealing at 950 K. Owing to the difference between the positron affinities of lithium and MgO, the Li nanoclusters act as quantum dots for positrons. 2D-ACAR distributions for different projections reveal a semicoherent fitting of the embedded metallic Li nanoclusters to the host MgO lattice. Ab initio Korringa-Kohn-Rostoker calculations of the momentum density show that the anisotropies of the experimental distributions are consistent with an fcc crystal structure of the Li nanoclusters. The observed reduction of the width of the experimental 2D-ACAR distribution is attributed to positron trapping in vacancies associated with Li clusters. This work proposes a method for studying the electronic structure of metallic quantum dots embedded in an insulating material.

Actinide chemistry using singlet-paired coupled cluster and its combinations with density functionals

NASA Astrophysics Data System (ADS)

Garza, Alejandro J.; Sousa Alencar, Ana G.; Scuseria, Gustavo E.

2015-12-01

Singlet-paired coupled cluster doubles (CCD0) is a simplification of CCD that relinquishes a fraction of dynamic correlation in order to be able to describe static correlation. Combinations of CCD0 with density functionals that recover specifically the dynamic correlation missing in the former have also been developed recently. Here, we assess the accuracy of CCD0 and CCD0+DFT (and variants of these using Brueckner orbitals) as compared to well-established quantum chemical methods for describing ground-state properties of singlet actinide molecules. The f0 actinyl series (UO22+, NpO23+, PuO24+), the isoelectronic NUN, and thorium (ThO, ThO2+) and nobelium (NoO, NoO2) oxides are studied.

Assessment of the Density Functional Tight Binding Method for Protic Ionic Liquids

PubMed Central

2015-01-01

Density functional tight binding (DFTB), which is ∼100–1000 times faster than full density functional theory (DFT), has been used to simulate the structure and properties of protic ionic liquid (IL) ions, clusters of ions and the bulk liquid. Proton affinities for a wide range of IL cations and anions determined using DFTB generally reproduce G3B3 values to within 5–10 kcal/mol. The structures and thermodynamic stabilities of n-alkyl ammonium nitrate clusters (up to 450 quantum chemical atoms) predicted with DFTB are in excellent agreement with those determined using DFT. The IL bulk structure simulated using DFTB with periodic boundary conditions is in excellent agreement with published neutron diffraction data. PMID:25328497

Effect of Coulomb Correlation on the Magnetic Properties of Mn Clusters.

PubMed

Huang, Chengxi; Zhou, Jian; Deng, Kaiming; Kan, Erjun; Jena, Puru

2018-05-03

In spite of decades of research, a fundamental understanding of the unusual magnetic behavior of small Mn clusters remains a challenge. Experiments show that Mn 2 is antiferromagnetic while small clusters containing up to five Mn atoms are ferromagnetic with magnetic moments of 5 μ B /atom and become ferrimagnetic as they grow further. Theoretical studies based on density functional theory (DFT), however, find Mn 2 to be ferromagnetic, with ferrimagnetic order setting in at different sizes that depend upon the computational methods used. While quantum chemical techniques correctly account for the antiferromagnetic ground state of Mn 2 , they are computationally too demanding to treat larger clusters, making it difficult to understand the evolution of magnetism. These studies clearly point to the importance of correlation and the need to find ways to treat it effectively for larger clusters and nanostructures. Here, we show that the DFT+ U method can be used to account for strong correlation. We determine the on-site Coulomb correlation, Hubbard U self-consistently by using the linear response theory and study its effect on the magnetic coupling of Mn clusters containing up to five atoms. With a calculated U value of 4.8 eV, we show that the ground state of Mn 2 is antiferromagnetic with a Mn-Mn distance of 3.34 Å, which agrees well with the electron spin resonance experiment. Equally important, we show that on-site Coulomb correlation also plays an important role in the evolution of magnetic coupling in larger clusters, as the results differ significantly from standard DFT calculations. We conclude that for a proper understanding of magnetism of Mn nanostructures (clusters, chains, and layers) one must take into account the effect of strong correlation.

Universal photonic quantum computation via time-delayed feedback

PubMed Central

Pichler, Hannes; Choi, Soonwon; Zoller, Peter; Lukin, Mikhail D.

2017-01-01

We propose and analyze a deterministic protocol to generate two-dimensional photonic cluster states using a single quantum emitter via time-delayed quantum feedback. As a physical implementation, we consider a single atom or atom-like system coupled to a 1D waveguide with a distant mirror, where guided photons represent the qubits, while the mirror allows the implementation of feedback. We identify the class of many-body quantum states that can be produced using this approach and characterize them in terms of 2D tensor network states. PMID:29073057

Theoretical investigation of the relative stability of Na{sup +}He{sub n} (n = 2–24) clusters: Many-body versus delocalization effects

DOE Office of Scientific and Technical Information (OSTI.GOV)

Issaoui, Noureddine, E-mail: issaoui-noureddine@yahoo.fr; Abdessalem, Kawther; Ghalla, Houcine

2014-11-07

The solvation of the Na{sup +} ion in helium clusters has been studied theoretically using optimization methods. A many-body empirical potential was developed to account for Na{sup +}–He and polarization interactions, and the most stable structures of Na{sup +}He{sub n} clusters were determined using the basin-hopping method. Vibrational delocalization was accounted for using zero-point energy corrections at the harmonic or anharmonic levels, the latter being evaluated from quantum Monte Carlo simulations for spinless particles. From the static perspective, many-body effects are found to play a minor role, and the structures obtained reflect homogeneous covering up to n = 10, followedmore » by polyicosahedral packing above this size, the cluster obtained at n = 12 appearing particularly stable. The cationic impurity binds the closest helium atoms sufficiently to negate vibrational delocalization at small sizes. However, this snowball effect is obliterated earlier than shell completion, the nuclear wavefunctions of {sup 4}He{sub n}Na{sup +} with n = 5–7, and n > 10 already exhibiting multiple inherent structures. The decrease in the snowball size due to many-body effects is consistent with recent mass spectrometry measurements.« less

Majorana-Based Fermionic Quantum Computation.

PubMed

O'Brien, T E; Rożek, P; Akhmerov, A R

2018-06-01

Because Majorana zero modes store quantum information nonlocally, they are protected from noise, and have been proposed as a building block for a quantum computer. We show how to use the same protection from noise to implement universal fermionic quantum computation. Our architecture requires only two Majorana modes to encode a fermionic quantum degree of freedom, compared to alternative implementations which require a minimum of four Majorana modes for a spin quantum degree of freedom. The fermionic degrees of freedom support both unitary coupled cluster variational quantum eigensolver and quantum phase estimation algorithms, proposed for quantum chemistry simulations. Because we avoid the Jordan-Wigner transformation, our scheme has a lower overhead for implementing both of these algorithms, allowing for simulation of the Trotterized Hubbard Hamiltonian in O(1) time per unitary step. We finally demonstrate magic state distillation in our fermionic architecture, giving a universal set of topologically protected fermionic quantum gates.

Majorana-Based Fermionic Quantum Computation

NASA Astrophysics Data System (ADS)

O'Brien, T. E.; RoŻek, P.; Akhmerov, A. R.

2018-06-01

Because Majorana zero modes store quantum information nonlocally, they are protected from noise, and have been proposed as a building block for a quantum computer. We show how to use the same protection from noise to implement universal fermionic quantum computation. Our architecture requires only two Majorana modes to encode a fermionic quantum degree of freedom, compared to alternative implementations which require a minimum of four Majorana modes for a spin quantum degree of freedom. The fermionic degrees of freedom support both unitary coupled cluster variational quantum eigensolver and quantum phase estimation algorithms, proposed for quantum chemistry simulations. Because we avoid the Jordan-Wigner transformation, our scheme has a lower overhead for implementing both of these algorithms, allowing for simulation of the Trotterized Hubbard Hamiltonian in O (1 ) time per unitary step. We finally demonstrate magic state distillation in our fermionic architecture, giving a universal set of topologically protected fermionic quantum gates.

Tug-of-war between classical and multicenter bonds in H-(Be)n-H species

NASA Astrophysics Data System (ADS)

Lundell, Katie A.; Boldyrev, Alexander I.

2018-05-01

Quantum chemical calculations were performed for beryllium homocatenated compounds [H-(Be)n-H]. Global minimum structures were found using machine searches (Coalescence Kick method) with density functional theory. Chemical bonding analysis was performed with the Adaptive Natural Density Partitioning method. It was found that H-(Be)2-H and H-(Be)3-H clusters are linear with classical two-center two-electron bonds, while for n > 3, three-dimensional structures are more stable with multicenter bonding. Thus, at n = 4, multicenter bonding wins the tug-of-war vs. the classical bonding.

Stepwise Assembly and Characterization of DNA Linked Two-Color Quantum Dot Clusters.

PubMed

Coopersmith, Kaitlin; Han, Hyunjoo; Maye, Mathew M

2015-07-14

The DNA-mediated self-assembly of multicolor quantum dot (QD) clusters via a stepwise approach is described. The CdSe/ZnS QDs were synthesized and functionalized with an amphiphilic copolymer, followed by ssDNA conjugation. At each functionalization step, the QDs were purified via gradient ultracentrifugation, which was found to remove excess polymer and QD aggregates, allowing for improved conjugation yields and assembly reactivity. The QDs were then assembled and disassembled in a stepwise manner at a ssDNA functionalized magnetic colloid, which provided a convenient way to remove unreacted QDs and ssDNA impurities. After assembly/disassembly, the clusters' optical characteristics were studied by fluorescence spectroscopy and the assembly morphology and stoichiometry was imaged via electron microscopy. The results indicate that a significant amount of QD-to-QD energy transfer occurred in the clusters, which was studied as a function of increasing acceptor-to-donor ratios, resulting in increased QD acceptor emission intensities compared to controls.

Spectroscopic studies of clusterization of methanol molecules isolated in a nitrogen matrix

NASA Astrophysics Data System (ADS)

Vaskivskyi, Ye.; Doroshenko, I.; Chernolevska, Ye.; Pogorelov, V.; Pitsevich, G.

2017-12-01

IR absorption spectra of methanol isolated in a nitrogen matrix are recorded at temperatures ranging from 9 to 34 K. The changes in the spectra with increasing matrix temperature are analyzed. Based on quantum-chemical calculations of the geometric and spectral parameters of different methanol clusters, the observed absorption bands are identified. The cluster composition of the sample is determined at each temperature. It is shown that as the matrix is heated there is a redistribution among the different cluster structures in the sample, from smaller to larger clusters.

Noise thresholds for optical quantum computers.

PubMed

Dawson, Christopher M; Haselgrove, Henry L; Nielsen, Michael A

2006-01-20

In this Letter we numerically investigate the fault-tolerant threshold for optical cluster-state quantum computing. We allow both photon loss noise and depolarizing noise (as a general proxy for all local noise), and obtain a threshold region of allowed pairs of values for the two types of noise. Roughly speaking, our results show that scalable optical quantum computing is possible for photon loss probabilities <3 x 10(-3), and for depolarization probabilities <10(-4).

On the inclusion of alkanes into the monolayer of aliphatic alcohols at the water/alkane vapor interface: a quantum chemical approach.

PubMed

Vysotsky, Yuri B; Fomina, Elena S; Belyaeva, Elena A; Fainerman, Valentin B; Vollhardt, Dieter

2013-02-14

In the framework of the quantum chemical semiempirical PM3 method thermodynamic and structural parameters of the formation and clusterization of aliphatic alcohols C(n)H(2n+1)OH (n(OH) = 8-16) at 298 K at the water/alkane vapor C(n)H(2n+2), (n(CH(3)) = 6-16) interface were calculated. The dependencies of enthalpy, entropy and Gibbs' energy of clusterization per one monomer molecule of 2D films on the alkyl chain length of corresponding alcohols and alkanes, the molar fraction of alkanes in the monolayers and the immersion degree of alcohol molecules into the water phase were shown to be linear or stepwise. The threshold of spontaneous clusterization of aliphatic alcohols at the water/alkane vapor interface was 10-11 carbon atoms at 298 K which is in line with experimental data at the air/water interface. It is shown that the presence of alkane vapor does not influence the process of alcohol monolayer formation. The structure of these monolayers is analogous to those obtained at the air/water interface in agreement with experimental data. The inclusion of alkane molecules into the amphiphilic monolayer at the water/alkane vapor interface is possible for amphiphiles with the spontaneous clusterization threshold at the air/water interface (n(s)(0)) of at least 16 methylene units in the alkyl chain, and it does not depend on the molar fraction of alkanes in the corresponding monolayer. The inclusion of alkanes from the vapor phase into the amphiphilic monolayer also requires that the difference between the alkyl chain lengths of alcohols and alkanes is not larger than n(s)(0) - 15 and n(s)(0) - 14 for the 2D film 1 and 2D film 2, respectively.

Atomic Cluster Ionization and Attosecond Generation at Long Wavelengths

DTIC Science & Technology

2015-10-31

fellowships for further studies in science, mathematics, engineering or technology fields: Student Metrics This section only applies to graduating...order to investigate this we use a modified Lewenstein quantum model in which the cluster is represented by a 1D Coulomb potential for the parent ion

Combined quantum mechanical and molecular mechanical method for metal-organic frameworks: proton topologies of NU-1000.

PubMed

Wu, Xin-Ping; Gagliardi, Laura; Truhlar, Donald G

2018-01-17

Metal-organic frameworks (MOFs) are materials with applications in catalysis, gas separations, and storage. Quantum mechanical (QM) calculations can provide valuable guidance to understand and predict their properties. In order to make the calculations faster, rather than modeling these materials as periodic (infinite) systems, it is useful to construct finite models (called cluster models) and use subsystem methods such as fragment methods or combined quantum mechanical and molecular mechanical (QM/MM) methods. Here we employ a QM/MM methodology to study one particular MOF that has been of widespread interest because of its wide pores and good solvent and thermal stability, namely NU-1000, which contains hexanuclear zirconium nodes and 1,3,6,8-tetrakis(p-benzoic acid)pyrene (TBAPy 4- ) linkers. A modified version of the Bristow-Tiana-Walsh transferable force field has been developed to allow QM/MM calculations on NU-1000; we call the new parametrization the NU1T force field. We consider isomeric structures corresponding to various proton topologies of the [Zr 6 (μ 3 -O) 8 O 8 H 16 ] 8+ node of NU-1000, and we compute their relative energies using a QM/MM scheme designed for the present kind of problem. We compared the results to full quantum mechanical (QM) energy calculations and found that the QM/MM models can reproduce the full QM relative energetics (which span a range of 334 kJ mol -1 ) with a mean unsigned deviation (MUD) of only 2 kJ mol -1 . Furthermore, we found that the structures optimized by QM/MM are nearly identical to their full QM optimized counterparts.

Molecular Interactions and Properties with Many-Body Methods

DTIC Science & Technology

1990-04-17

AFOSR have been identified in a book by Schaefer , Quantum Chemistry (Oxford, 1984), as being among the 149 most influential papers in the 50-year...Coupled Cluster Investigation of Isomerization Reactions: HCN*HNC, BH3CN-BH 3NC- and HCNBH3 *HNCBH3," J. Am. Chem. Soc. 110, 4926 (1988). 21. M. Rittby...Kucharski, J. Noga and R.J. Bartlett, J. Chem. Phys. 88, 1035 (1988). 49. H. Urban and R.J. Bartlett, J. Am. Chem. Soc. 110, 4926 (1988). 50. G.D

An accurate and linear-scaling method for calculating charge-transfer excitation energies and diabatic couplings

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pavanello, Michele; Van Voorhis, Troy; Visscher, Lucas

2013-02-07

Quantum-mechanical methods that are both computationally fast and accurate are not yet available for electronic excitations having charge transfer character. In this work, we present a significant step forward towards this goal for those charge transfer excitations that take place between non-covalently bound molecules. In particular, we present a method that scales linearly with the number of non-covalently bound molecules in the system and is based on a two-pronged approach: The molecular electronic structure of broken-symmetry charge-localized states is obtained with the frozen density embedding formulation of subsystem density-functional theory; subsequently, in a post-SCF calculation, the full-electron Hamiltonian and overlapmore » matrix elements among the charge-localized states are evaluated with an algorithm which takes full advantage of the subsystem DFT density partitioning technique. The method is benchmarked against coupled-cluster calculations and achieves chemical accuracy for the systems considered for intermolecular separations ranging from hydrogen-bond distances to tens of Angstroms. Numerical examples are provided for molecular clusters comprised of up to 56 non-covalently bound molecules.« less

An accurate and linear-scaling method for calculating charge-transfer excitation energies and diabatic couplings.

PubMed

Pavanello, Michele; Van Voorhis, Troy; Visscher, Lucas; Neugebauer, Johannes

2013-02-07

Quantum-mechanical methods that are both computationally fast and accurate are not yet available for electronic excitations having charge transfer character. In this work, we present a significant step forward towards this goal for those charge transfer excitations that take place between non-covalently bound molecules. In particular, we present a method that scales linearly with the number of non-covalently bound molecules in the system and is based on a two-pronged approach: The molecular electronic structure of broken-symmetry charge-localized states is obtained with the frozen density embedding formulation of subsystem density-functional theory; subsequently, in a post-SCF calculation, the full-electron Hamiltonian and overlap matrix elements among the charge-localized states are evaluated with an algorithm which takes full advantage of the subsystem DFT density partitioning technique. The method is benchmarked against coupled-cluster calculations and achieves chemical accuracy for the systems considered for intermolecular separations ranging from hydrogen-bond distances to tens of Ångstroms. Numerical examples are provided for molecular clusters comprised of up to 56 non-covalently bound molecules.

DNA-Mediated Patterning of Single Quantum Dot Nanoarrays: A Reusable Platform for Single-Molecule Control

NASA Astrophysics Data System (ADS)

Huang, Da; Freeley, Mark; Palma, Matteo

2017-03-01

We present a facile strategy of general applicability for the assembly of individual nanoscale moieties in array configurations with single-molecule control. Combining the programming ability of DNA as a scaffolding material with a one-step lithographic process, we demonstrate the patterning of single quantum dots (QDs) at predefined locations on silicon and transparent glass surfaces: as proof of concept, clusters of either one, two, or three QDs were assembled in highly uniform arrays with a 60 nm interdot spacing within each cluster. Notably, the platform developed is reusable after a simple cleaning process and can be designed to exhibit different geometrical arrangements.

Universal quantum computation with temporal-mode bilayer square lattices

NASA Astrophysics Data System (ADS)

Alexander, Rafael N.; Yokoyama, Shota; Furusawa, Akira; Menicucci, Nicolas C.

2018-03-01

We propose an experimental design for universal continuous-variable quantum computation that incorporates recent innovations in linear-optics-based continuous-variable cluster state generation and cubic-phase gate teleportation. The first ingredient is a protocol for generating the bilayer-square-lattice cluster state (a universal resource state) with temporal modes of light. With this state, measurement-based implementation of Gaussian unitary gates requires only homodyne detection. Second, we describe a measurement device that implements an adaptive cubic-phase gate, up to a random phase-space displacement. It requires a two-step sequence of homodyne measurements and consumes a (non-Gaussian) cubic-phase state.

Spin-driven structural effects in alkali doped (4)He clusters from quantum calculations.

PubMed

Bovino, S; Coccia, E; Bodo, E; Lopez-Durán, D; Gianturco, F A

2009-06-14

In this paper, we carry out variational Monte Carlo and diffusion Monte Carlo (DMC) calculations for Li(2)((1)Sigma(g) (+))((4)He)(N) and Li(2)((3)Sigma(u) (+))((4)He)(N) with N up to 30 and discuss in detail the results of our computations. After a comparison between our DMC energies with the "exact" discrete variable representation values for the species with one (4)He, in order to test the quality of our computations at 0 K, we analyze the structural features of the whole range of doped clusters. We find that both species reside on the droplet surface, but that their orientation is spin driven, i.e., the singlet molecule is perpendicular and the triplet one is parallel to the droplet's surface. We have also computed quantum vibrational relaxation rates for both dimers in collision with a single (4)He and we find them to differ by orders of magnitude at the estimated surface temperature. Our results therefore confirm the findings from a great number of experimental data present in the current literature and provide one of the first attempts at giving an accurate, fully quantum picture for the nanoscopic properties of alkali dimers in (4)He clusters.

Large-scale frequency- and time-domain quantum entanglement over the optical frequency comb (Conference Presentation)

NASA Astrophysics Data System (ADS)

Pfister, Olivier

2017-05-01

When it comes to practical quantum computing, the two main challenges are circumventing decoherence (devastating quantum errors due to interactions with the environmental bath) and achieving scalability (as many qubits as needed for a real-life, game-changing computation). We show that using, in lieu of qubits, the "qumodes" represented by the resonant fields of the quantum optical frequency comb of an optical parametric oscillator allows one to create bona fide, large scale quantum computing processors, pre-entangled in a cluster state. We detail our recent demonstration of 60-qumode entanglement (out of an estimated 3000) and present an extension to combining this frequency-tagged with time-tagged entanglement, in order to generate an arbitrarily large, universal quantum computing processor.

Quantum Monte Carlo Simulation of condensed van der Waals Systems

NASA Astrophysics Data System (ADS)

Benali, Anouar; Shulenburger, Luke; Romero, Nichols A.; Kim, Jeongnim; Anatole von Lilienfeld, O.

2012-02-01

Van der Waals forces are as ubiquitous as infamous. While post-Hartree-Fock methods enable accurate estimates of these forces in molecules and clusters, they remain elusive for dealing with many-electron condensed phase systems. We present Quantum Monte Carlo [1,2] results for condensed van der Waals systems. Interatomic many-body contributions to cohesive energies and bulk modulus will be discussed. Numerical evidence is presented for crystals of rare gas atoms, and compared to experiments and methods [3]. Sandia National Laboratories is a multiprogram laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. DoE's National Nuclear Security Administration under Contract No. DE-AC04-94AL85000.[4pt] [1] J. Kim, K. Esler, J. McMinis and D. Ceperley, SciDAC 2010, J. of Physics: Conference series, Chattanooga, Tennessee, July 11 2011 [0pt] [2] QMCPACK simulation suite, http://qmcpack.cmscc.org (unpublished)[0pt] [3] O. A. von Lillienfeld and A. Tkatchenko, J. Chem. Phys. 132 234109 (2010)

The Harvard Clean Energy Project: High-throughput screening of organic photovoltaic materials using cheminformatics, machine learning, and pattern recognition

NASA Astrophysics Data System (ADS)

Olivares-Amaya, Roberto; Hachmann, Johannes; Amador-Bedolla, Carlos; Daly, Aidan; Jinich, Adrian; Atahan-Evrenk, Sule; Boixo, Sergio; Aspuru-Guzik, Alán

2012-02-01

Organic photovoltaic devices have emerged as competitors to silicon-based solar cells, currently reaching efficiencies of over 9% and offering desirable properties for manufacturing and installation. We study conjugated donor polymers for high-efficiency bulk-heterojunction photovoltaic devices with a molecular library motivated by experimental feasibility. We use quantum mechanics and a distributed computing approach to explore this vast molecular space. We will detail the screening approach starting from the generation of the molecular library, which can be easily extended to other kinds of molecular systems. We will describe the screening method for these materials which ranges from descriptor models, ubiquitous in the drug discovery community, to eventually reaching first principles quantum chemistry methods. We will present results on the statistical analysis, based principally on machine learning, specifically partial least squares and Gaussian processes. Alongside, clustering methods and the use of the hypergeometric distribution reveal moieties important for the donor materials and allow us to quantify structure-property relationships. These efforts enable us to accelerate materials discovery in organic photovoltaics through our collaboration with experimental groups.

Cluster-model calculations of exotic decays from heavy nuclei

NASA Astrophysics Data System (ADS)

Buck, B.; Merchant, A. C.

1989-05-01

A cluster model employing a local, effective cluster-core potential is used to investigate exotic decay from heavy nuclei as a quantum tunneling phenomenon within a semiclassical approximation. Excellent agreement with all reported experimental measurements of the decay widths for 14C and 24Ne emission is obtained. As an added bonus, the width for alpha particle emission from 212Po is also calculated in good agreement with experiment.

Models of optical quantum computing

NASA Astrophysics Data System (ADS)

Krovi, Hari

2017-03-01

I review some work on models of quantum computing, optical implementations of these models, as well as the associated computational power. In particular, we discuss the circuit model and cluster state implementations using quantum optics with various encodings such as dual rail encoding, Gottesman-Kitaev-Preskill encoding, and coherent state encoding. Then we discuss intermediate models of optical computing such as boson sampling and its variants. Finally, we review some recent work in optical implementations of adiabatic quantum computing and analog optical computing. We also provide a brief description of the relevant aspects from complexity theory needed to understand the results surveyed.

Isotope exchange in reactions between D2O and size-selected ionic water clusters containing pyridine, H+ (pyridine)m(H2O)n.

PubMed

Ryding, Mauritz Johan; Zatula, Alexey S; Andersson, Patrik Urban; Uggerud, Einar

2011-01-28

Pyridine containing water clusters, H(+)(pyridine)(m)(H(2)O)(n), have been studied both experimentally by a quadrupole time-of-flight mass spectrometer and by quantum chemical calculations. In the experiments, H(+)(pyridine)(m)(H(2)O)(n) with m = 1-4 and n = 0-80 are observed. For the cluster distributions observed, there are no magic numbers, neither in the abundance spectra, nor in the evaporation spectra from size selected clusters. Experiments with size-selected clusters H(+)(pyridine)(m)(H(2)O)(n), with m = 0-3, reacting with D(2)O at a center-of-mass energy of 0.1 eV were also performed. The cross-sections for H/D isotope exchange depend mainly on the number of water molecules in the cluster and not on the number of pyridine molecules. Clusters having only one pyridine molecule undergo D(2)O/H(2)O ligand exchange, while H(+)(pyridine)(m)(H(2)O)(n), with m = 2, 3, exhibit significant H/D scrambling. These results are rationalized by quantum chemical calculations (B3LYP and MP2) for H(+)(pyridine)(1)(H(2)O)(n) and H(+)(pyridine)(2)(H(2)O)(n), with n = 1-6. In clusters containing one pyridine, the water molecules form an interconnected network of hydrogen bonds associated with the pyridinium ion via a single hydrogen bond. For clusters containing two pyridines, the two pyridine molecules are completely separated by the water molecules, with each pyridine being positioned diametrically opposite within the cluster. In agreement with experimental observations, these calculations suggest a "see-saw mechanism" for pendular proton transfer between the two pyridines in H(+)(pyridine)(2)(H(2)O)(n) clusters.

Cluster state generation in one-dimensional Kitaev honeycomb model via shortcut to adiabaticity

NASA Astrophysics Data System (ADS)

Kyaw, Thi Ha; Kwek, Leong-Chuan

2018-04-01

We propose a mean to obtain computationally useful resource states also known as cluster states, for measurement-based quantum computation, via transitionless quantum driving algorithm. The idea is to cool the system to its unique ground state and tune some control parameters to arrive at computationally useful resource state, which is in one of the degenerate ground states. Even though there is set of conserved quantities already present in the model Hamiltonian, which prevents the instantaneous state to go to any other eigenstate subspaces, one cannot quench the control parameters to get the desired state. In that case, the state will not evolve. With involvement of the shortcut Hamiltonian, we obtain cluster states in fast-forward manner. We elaborate our proposal in the one-dimensional Kitaev honeycomb model, and show that the auxiliary Hamiltonian needed for the counterdiabatic driving is of M-body interaction.

Percolation bounds for decoding thresholds with correlated erasures in quantum LDPC codes

NASA Astrophysics Data System (ADS)

Hamilton, Kathleen; Pryadko, Leonid

Correlations between errors can dramatically affect decoding thresholds, in some cases eliminating the threshold altogether. We analyze the existence of a threshold for quantum low-density parity-check (LDPC) codes in the case of correlated erasures. When erasures are positively correlated, the corresponding multi-variate Bernoulli distribution can be modeled in terms of cluster errors, where qubits in clusters of various size can be marked all at once. In a code family with distance scaling as a power law of the code length, erasures can be always corrected below percolation on a qubit adjacency graph associated with the code. We bound this correlated percolation transition by weighted (uncorrelated) percolation on a specially constructed cluster connectivity graph, and apply our recent results to construct several bounds for the latter. This research was supported in part by the NSF Grant PHY-1416578 and by the ARO Grant W911NF-14-1-0272.

Electron wavepacket dynamics in highly quasi-degenerate coupled electronic states: a theory for chemistry where the notion of adiabatic potential energy surface loses the sense.

PubMed

Yonehara, Takehiro; Takatsuka, Kazuo

2012-12-14

We develop a theory and the method of its application for chemical dynamics in systems, in which the adiabatic potential energy hyper-surfaces (PES) are densely quasi-degenerate to each other in a wide range of molecular geometry. Such adiabatic electronic states tend to couple each other through strong nonadiabatic interactions. Technically, therefore, it is often extremely hard to accurately single out the individual PES in those systems. Moreover, due to the mutual nonadiabatic couplings that may spread wide in space and due to the energy-time uncertainty relation, the notion of the isolated and well-defined potential energy surface should lose the sense. On the other hand, such dense electronic states should offer a very interesting molecular field in which chemical reactions to proceed in characteristic manners. However, to treat these systems, the standard theoretical framework of chemical reaction dynamics, which starts from the Born-Oppenheimer approximation and ends up with quantum nuclear wavepacket dynamics, is not very useful. We here explore this problem with our developed nonadiabatic electron wavepacket theory, which we call the phase-space averaging and natural branching (PSANB) method [T. Yonehara and K. Takatsuka, J. Chem. Phys. 129, 134109 (2008)], or branching-path representation, in which the packets are propagated in time along the non-Born-Oppenheimer branching paths. In this paper, after outlining the basic theory, we examine using a one-dimensional model how well the PSANB method works with such densely quasi-degenerate nonadiabatic systems. To do so, we compare the performance of PSANB with the full quantum mechanical results and those given by the fewest switches surface hopping (FSSH) method, which is known to be one of the most reliable and flexible methods to date. It turns out that the PSANB electron wavepacket approach actually yields very good results with far fewer initial sampling paths. Then we apply the electron wavepacket dynamics in path-branching representation and the so-called semiclassical Ehrenfest theory to a hydrogen molecule embedded in twelve membered boron cluster (B(12)) in excited states, which are densely quasi-degenerate due to the vacancy in 2p orbitals of boron atom [1s(2)2s(2)2p(1)]. Bond dissociation of the hydrogen molecule quickly takes place in the cluster and the resultant hydrogen atoms are squeezed out to the surface of the cluster. We further study collision dynamics between H(2) and B(12), which also gives interesting phenomena. The present study suggests an interesting functionality of the boron clusters.

Multi-bit dark state memory: Double quantum dot as an electronic quantum memory

NASA Astrophysics Data System (ADS)

Aharon, Eran; Pozner, Roni; Lifshitz, Efrat; Peskin, Uri

2016-12-01

Quantum dot clusters enable the creation of dark states which preserve electrons or holes in a coherent superposition of dot states for a long time. Various quantum logic devices can be envisioned to arise from the possibility of storing such trapped particles for future release on demand. In this work, we consider a double quantum dot memory device, which enables the preservation of a coherent state to be released as multiple classical bits. Our unique device architecture uses an external gating for storing (writing) the coherent state and for retrieving (reading) the classical bits, in addition to exploiting an internal gating effect for the preservation of the coherent state.

Faithful Remote Information Concentration Based on the Optimal Universal 1→2 Telecloning of Arbitrary Two-Qubit States

NASA Astrophysics Data System (ADS)

Peng, Jia-Yin; Lei, Hong-Xuan; Mo, Zhi-Wen

2014-05-01

The previous protocols of remote quantum information concentration were focused on the reverse process of quantum telecloning of single-qubit states. We here investigate the reverse process of optimal universal 1→2 telecloning of arbitrary two-qubit states. The aim of this telecloning is to distribute respectively the quantum information to two groups of spatially separated receivers from a group of two senders situated at two different locations. Our scheme shows that the distributed quantum information can be remotely concentrated back to a group of two different receivers with 1 of probability by utilizing maximally four-particle cluster state and four-particle GHZ state as quantum channel.

A theoretical study of water equilibria: The cluster distribution versus temperature and pressure for (H2O)n, n=1-60, and ice

NASA Astrophysics Data System (ADS)

Lenz, Annika; Ojamäe, Lars

2009-10-01

The size distribution of water clusters at equilibrium is studied using quantum-chemical calculations in combination with statistical thermodynamics. The necessary energetic data is obtained by quantum-chemical B3LYP computations and through extrapolations from the B3LYP results for the larger clusters. Clusters with up to 60 molecules are included in the equilibrium computations. Populations of different cluster sizes are calculated using both an ideal gas model with noninteracting clusters and a model where a correction for the interaction energy is included analogous to the van der Waals law. In standard vapor the majority of the water molecules are monomers. For the ideal gas model at 1 atm large clusters [56-mer (0-120 K) and 28-mer (100-260 K)] dominate at low temperatures and separate to smaller clusters [21-22-mer (170-280 K) and 4-6-mer (270-320 K) and to monomers (300-350 K)] when the temperature is increased. At lower pressure the transition from clusters to monomers lies at lower temperatures and fewer cluster sizes are formed. The computed size distribution exhibits enhanced peaks for the clusters consisting of 21 and 28 water molecules; these sizes are for protonated water clusters often referred to as magic numbers. If cluster-cluster interactions are included in the model the transition from clusters to monomers is sharper (i.e., occurs over a smaller temperature interval) than when the ideal-gas model is used. Clusters with 20-22 molecules dominate in the liquid region. When a large icelike cluster is included it will dominate for temperatures up to 325 K for the noninteracting clusters model. Thermodynamic properties (Cp, ΔH) were calculated with in general good agreement with experimental values for the solid and gas phase. A formula for the number of H-bond topologies in a given cluster structure is derived. For the 20-mer it is shown that the number of topologies contributes to making the population of dodecahedron-shaped cluster larger than that of a lower-energy fused prism cluster at high temperatures.

A theoretical study of water equilibria: the cluster distribution versus temperature and pressure for (H2O)n, n = 1-60, and ice.

PubMed

Lenz, Annika; Ojamäe, Lars

2009-10-07

The size distribution of water clusters at equilibrium is studied using quantum-chemical calculations in combination with statistical thermodynamics. The necessary energetic data is obtained by quantum-chemical B3LYP computations and through extrapolations from the B3LYP results for the larger clusters. Clusters with up to 60 molecules are included in the equilibrium computations. Populations of different cluster sizes are calculated using both an ideal gas model with noninteracting clusters and a model where a correction for the interaction energy is included analogous to the van der Waals law. In standard vapor the majority of the water molecules are monomers. For the ideal gas model at 1 atm large clusters [56-mer (0-120 K) and 28-mer (100-260 K)] dominate at low temperatures and separate to smaller clusters [21-22-mer (170-280 K) and 4-6-mer (270-320 K) and to monomers (300-350 K)] when the temperature is increased. At lower pressure the transition from clusters to monomers lies at lower temperatures and fewer cluster sizes are formed. The computed size distribution exhibits enhanced peaks for the clusters consisting of 21 and 28 water molecules; these sizes are for protonated water clusters often referred to as magic numbers. If cluster-cluster interactions are included in the model the transition from clusters to monomers is sharper (i.e., occurs over a smaller temperature interval) than when the ideal-gas model is used. Clusters with 20-22 molecules dominate in the liquid region. When a large icelike cluster is included it will dominate for temperatures up to 325 K for the noninteracting clusters model. Thermodynamic properties (C(p), DeltaH) were calculated with in general good agreement with experimental values for the solid and gas phase. A formula for the number of H-bond topologies in a given cluster structure is derived. For the 20-mer it is shown that the number of topologies contributes to making the population of dodecahedron-shaped cluster larger than that of a lower-energy fused prism cluster at high temperatures.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Löytynoja, T., E-mail: tuomas.loytynoja@oulu.fi; Division of Theoretical Chemistry and Biology, School of Biotechnology, Royal Institute of Technology, SE-106 91 Stockholm; Li, X.

We study a newly devised quantum mechanics capacitance molecular mechanics (QMCMM) method for the calculation of core-electron binding energies in the case of molecules adsorbed on metal surfaces. This yet untested methodology is applied to systems with monolayer of methanol/methyl nitrite on an Ag(111) surface at 100 K temperature. It was found out that the studied C, N, and O 1s core-hole energies converge very slowly as a function of the radius of the metallic cluster, which was ascribed to build up of positive charge on the edge of the Ag slab. Further analysis revealed that an extrapolation process canmore » be used to obtain binding energies that deviated less than 0.5 eV against experiments, except in the case of methanol O 1s where the difference was as large as 1.8 eV. Additional QM-cluster calculations suggest that the latter error can be connected to the lack of charge transfer over the QM–CMM boundary. Thus, the results indicate that the QMCMM and QM-cluster methods can complement each other in a holistic picture of molecule-adsorbate core-ionization studies, where all types of intermolecular interactions are considered.« less

Simulations of defect spin qubits in piezoelectric semiconductors

NASA Astrophysics Data System (ADS)

Seo, Hosung

In recent years, remarkable advances have been reported in the development of defect spin qubits in semiconductors for solid-state quantum information science and quantum metrology. Promising spin qubits include the nitrogen-vacancy center in diamond, dopants in silicon, and the silicon vacancy and divacancy spins in silicon carbide. In this talk, I will highlight some of our recent efforts devoted to defect spin qubits in piezoelectric wide-gap semiconductors for potential applications in mechanical hybrid quantum systems. In particular, I will describe our recent combined theoretical and experimental study on remarkably robust quantum coherence found in the divancancy qubits in silicon carbide. We used a quantum bath model combined with a cluster expansion method to identify the microscopic mechanisms behind the unusually long coherence times of the divacancy spins in SiC. Our study indicates that developing spin qubits in complex crystals with multiple types of atom is a promising route to realize strongly coherent hybrid quantum systems. I will also discuss progress and challenges in computational design of new spin defects for use as qubits in piezoelectric crystals such as AlN and SiC, including a new defect design concept using large metal ion - vacancy complexes. Our first principles calculations include DFT computations using recently developed self-consistent hybrid density functional theory and large-scale many-body GW theory. This work was supported by the National Science Foundation (NSF) through the University of Chicago MRSEC under Award Number DMR-1420709.

Yoink: An interaction-based partitioning API.

PubMed

Zheng, Min; Waller, Mark P

2018-05-15

Herein, we describe the implementation details of our interaction-based partitioning API (application programming interface) called Yoink for QM/MM modeling and fragment-based quantum chemistry studies. Interactions are detected by computing density descriptors such as reduced density gradient, density overlap regions indicator, and single exponential decay detector. Only molecules having an interaction with a user-definable QM core are added to the QM region of a hybrid QM/MM calculation. Moreover, a set of molecule pairs having density-based interactions within a molecular system can be computed in Yoink, and an interaction graph can then be constructed. Standard graph clustering methods can then be applied to construct fragments for further quantum chemical calculations. The Yoink API is licensed under Apache 2.0 and can be accessed via yoink.wallerlab.org. © 2018 Wiley Periodicals, Inc. © 2018 Wiley Periodicals, Inc.

Scalable quantum information processing with atomic ensembles and flying photons

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mei Feng; Yu Yafei; Feng Mang

2009-10-15

We present a scheme for scalable quantum information processing with atomic ensembles and flying photons. Using the Rydberg blockade, we encode the qubits in the collective atomic states, which could be manipulated fast and easily due to the enhanced interaction in comparison to the single-atom case. We demonstrate that our proposed gating could be applied to generation of two-dimensional cluster states for measurement-based quantum computation. Moreover, the atomic ensembles also function as quantum repeaters useful for long-distance quantum state transfer. We show the possibility of our scheme to work in bad cavity or in weak coupling regime, which could muchmore » relax the experimental requirement. The efficient coherent operations on the ensemble qubits enable our scheme to be switchable between quantum computation and quantum communication using atomic ensembles.« less

Molecular Magnetic Quantum Cellular Automata

DTIC Science & Technology

2004-06-01

Folting K, Gatteschi D, Christou G, Hendrickson D N 1993a, High-Spin Molecules - [Mn12O12(O2CR)16(H2O)4], J. Am. Chem. Soc. 115 1804 Sessoli R... Gatteschi D, Caneschi A and Novak M A 1993b, Magnetic bistability in a metal-ion cluster, Nature 365 141 Twamely J 2003, Quantum-cellular-automata

Hierarchy of the Collective Effects in Water Clusters.

PubMed

Bakó, Imre; Mayer, István

2016-02-04

The results of dipole moment as well as of intra- and intermolecular bond order calculations indicate the big importance of collective electrostatic effects caused by the nonimmediate environment in liquid water models. It is also discussed how these collective effects are built up as consequences of the electrostatic and quantum chemical interactions in water clusters.

Random phase approximation and cluster mean field studies of hard core Bose Hubbard model

NASA Astrophysics Data System (ADS)

Alavani, Bhargav K.; Gaude, Pallavi P.; Pai, Ramesh V.

2018-04-01

We investigate zero temperature and finite temperature properties of the Bose Hubbard Model in the hard core limit using Random Phase Approximation (RPA) and Cluster Mean Field Theory (CMFT). We show that our RPA calculations are able to capture quantum and thermal fluctuations significantly better than CMFT.

A triple quantum dot based nano-electromechanical memory device

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pozner, R.; Lifshitz, E.; Solid State Institute, Technion-Israel Institute of Technology, Haifa 32000

Colloidal quantum dots (CQDs) are free-standing nano-structures with chemically tunable electronic properties. This tunability offers intriguing possibilities for nano-electromechanical devices. In this work, we consider a nano-electromechanical nonvolatile memory (NVM) device incorporating a triple quantum dot (TQD) cluster. The device operation is based on a bias induced motion of a floating quantum dot (FQD) located between two bound quantum dots (BQDs). The mechanical motion is used for switching between two stable states, “ON” and “OFF” states, where ligand-mediated effective interdot forces between the BQDs and the FQD serve to hold the FQD in each stable position under zero bias. Consideringmore » realistic microscopic parameters, our quantum-classical theoretical treatment of the TQD reveals the characteristics of the NVM.« less

Path-integral molecular dynamics simulations of hydrated hydrogen chloride cluster HCl(H 2O) 4 on a semiempirical potential energy surface

NASA Astrophysics Data System (ADS)

Takayanagi, Toshiyuki; Takahashi, Kenta; Kakizaki, Akira; Shiga, Motoyuki; Tachikawa, Masanori

2009-04-01

Path-integral molecular dynamics simulations for the HCl(H 2O) 4 cluster have been performed on the ground-state potential energy surface directly obtained on-the-fly from semiempirical PM3-MAIS molecular orbital calculations. It is found that the HCl(H 2O) 4 cluster has structural rearrangement above the temperature of 300 K showing a liquid-like behavior. Quantum mechanical fluctuation of hydrogen nuclei plays a significant role in structural arrangement processes in this cluster.

Novel schemes for measurement-based quantum computation.

PubMed

Gross, D; Eisert, J

2007-06-01

We establish a framework which allows one to construct novel schemes for measurement-based quantum computation. The technique develops tools from many-body physics-based on finitely correlated or projected entangled pair states-to go beyond the cluster-state based one-way computer. We identify resource states radically different from the cluster state, in that they exhibit nonvanishing correlations, can be prepared using nonmaximally entangling gates, or have very different local entanglement properties. In the computational models, randomness is compensated in a different manner. It is shown that there exist resource states which are locally arbitrarily close to a pure state. We comment on the possibility of tailoring computational models to specific physical systems.

Large-scale atomistic calculations of clusters in intense x-ray pulses

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ho, Phay J.; Knight, Chris

Here, we present the methodology of our recently developed Monte-Carlo/ Molecular-Dynamics method for studying the fundamental ultrafast dynamics induced by high-fluence, high-intensity x-ray free electron laser (XFEL) pulses in clusters. The quantum nature of the initiating ionization process is accounted for by a Monte Carlo method to calculate probabilities of electronic transitions, including photo absorption, inner-shell relaxation, photon scattering, electron collision and recombination dynamics, and thus track the transient electronic configurations explicitly. The freed electrons and ions are followed by classical particle trajectories using a molecular dynamics algorithm. These calculations reveal the surprising role of electron-ion recombination processes that leadmore » to the development of nonuniform spatial charge density profiles in x-ray excited clusters over femtosecond timescales. In the high-intensity limit, it is important to include the recombination dynamics in the calculated scattering response even for a 2- fs pulse. We also demonstrate that our numerical codes and algorithms can make e!cient use of the computational power of massively parallel supercomputers to investigate the intense-field dynamics in systems with increasing complexity and size at the ultrafast timescale and in non-linear x-ray interaction regimes. In particular, picosecond trajectories of XFEL clusters with attosecond time resolution containing millions of particles can be e!ciently computed on upwards of 262,144 processes.« less

Large-scale atomistic calculations of clusters in intense x-ray pulses

DOE PAGES

Ho, Phay J.; Knight, Chris

2017-04-28

Here, we present the methodology of our recently developed Monte-Carlo/ Molecular-Dynamics method for studying the fundamental ultrafast dynamics induced by high-fluence, high-intensity x-ray free electron laser (XFEL) pulses in clusters. The quantum nature of the initiating ionization process is accounted for by a Monte Carlo method to calculate probabilities of electronic transitions, including photo absorption, inner-shell relaxation, photon scattering, electron collision and recombination dynamics, and thus track the transient electronic configurations explicitly. The freed electrons and ions are followed by classical particle trajectories using a molecular dynamics algorithm. These calculations reveal the surprising role of electron-ion recombination processes that leadmore » to the development of nonuniform spatial charge density profiles in x-ray excited clusters over femtosecond timescales. In the high-intensity limit, it is important to include the recombination dynamics in the calculated scattering response even for a 2- fs pulse. We also demonstrate that our numerical codes and algorithms can make e!cient use of the computational power of massively parallel supercomputers to investigate the intense-field dynamics in systems with increasing complexity and size at the ultrafast timescale and in non-linear x-ray interaction regimes. In particular, picosecond trajectories of XFEL clusters with attosecond time resolution containing millions of particles can be e!ciently computed on upwards of 262,144 processes.« less

Intermolecular interactions in the condensed phase: Evaluation of semi-empirical quantum mechanical methods

NASA Astrophysics Data System (ADS)

Christensen, Anders S.; Kromann, Jimmy C.; Jensen, Jan H.; Cui, Qiang

2017-10-01

To facilitate further development of approximate quantum mechanical methods for condensed phase applications, we present a new benchmark dataset of intermolecular interaction energies in the solution phase for a set of 15 dimers, each containing one charged monomer. The reference interaction energy in solution is computed via a thermodynamic cycle that integrates dimer binding energy in the gas phase at the coupled cluster level and solute-solvent interaction with density functional theory; the estimated uncertainty of such calculated interaction energy is ±1.5 kcal/mol. The dataset is used to benchmark the performance of a set of semi-empirical quantum mechanical (SQM) methods that include DFTB3-D3, DFTB3/CPE-D3, OM2-D3, PM6-D3, PM6-D3H+, and PM7 as well as the HF-3c method. We find that while all tested SQM methods tend to underestimate binding energies in the gas phase with a root-mean-squared error (RMSE) of 2-5 kcal/mol, they overestimate binding energies in the solution phase with an RMSE of 3-4 kcal/mol, with the exception of DFTB3/CPE-D3 and OM2-D3, for which the systematic deviation is less pronounced. In addition, we find that HF-3c systematically overestimates binding energies in both gas and solution phases. As most approximate QM methods are parametrized and evaluated using data measured or calculated in the gas phase, the dataset represents an important first step toward calibrating QM based methods for application in the condensed phase where polarization and exchange repulsion need to be treated in a balanced fashion.

Error Correction using Quantum Quasi-Cyclic Low-Density Parity-Check(LDPC) Codes

NASA Astrophysics Data System (ADS)

Jing, Lin; Brun, Todd; Quantum Research Team

Quasi-cyclic LDPC codes can approach the Shannon capacity and have efficient decoders. Manabu Hagiwara et al., 2007 presented a method to calculate parity check matrices with high girth. Two distinct, orthogonal matrices Hc and Hd are used. Using submatrices obtained from Hc and Hd by deleting rows, we can alter the code rate. The submatrix of Hc is used to correct Pauli X errors, and the submatrix of Hd to correct Pauli Z errors. We simulated this system for depolarizing noise on USC's High Performance Computing Cluster, and obtained the block error rate (BER) as a function of the error weight and code rate. From the rates of uncorrectable errors under different error weights we can extrapolate the BER to any small error probability. Our results show that this code family can perform reasonably well even at high code rates, thus considerably reducing the overhead compared to concatenated and surface codes. This makes these codes promising as storage blocks in fault-tolerant quantum computation. Error Correction using Quantum Quasi-Cyclic Low-Density Parity-Check(LDPC) Codes.

The [(AI 2O 3) 2] - Anion Cluster: Electron Localization-Delocalization Isomerism

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sierka, Marek; Dobler, Jens; Sauer, Joachim

2009-10-05

Three-dimensional bulk alumina and its two-dimensional thin films show great structural diversity, posing considerable challenges to their experimental structural characterization and computational modeling. Recently, structural diversity has also been demonstrated for zerodimensional gas phase aluminum oxide clusters. Mass-selected clusters not only make systematic studies of the structural and electronic properties as a function of size possible, but lately have also emerged as powerful molecular models of complex surfaces and solid catalysts. In particular, the [(Al 2O 3) 3-5] + clusters were the first example of polynuclear maingroup metal oxide cluster that are able to thermally activate CH 4. Over themore » past decades gas phase aluminum oxide clusters have been extensively studied both experimentally and computationally, but definitive structural assignments were made for only a handful of them: the planar [Al 3O 3] - and [Al 5O 4] - cluster anions, and the [(Al 2O 3) 1-4(AlO)] + cluster cations. For stoichiometric clusters only the atomic structures of [(Al 2O 3) 4] +/0 have been nambiguously resolved. Here we report on the structures of the [(Al 2O 3) 2] -/0 clusters combining photoelectron spectroscopy (PES) and quantum chemical calculations employing a genetic algorithm as a global optimization technique. The [(Al 2O 3) 2] - cluster anion show energetically close lying but structurally distinct cage and sheet-like isomers which differ by delocalization/localization of the extra electron. The experimental results are crucial for benchmarking the different computational methods applied with respect to a proper description of electron localization and the relative energies for the isomers which will be of considerable value for future computational studies of aluminum oxide and related systems.« less

Constructing simple yet accurate potentials for describing the solvation of HCl/water clusters in bulk helium and nanodroplets.

PubMed

Boese, A Daniel; Forbert, Harald; Masia, Marco; Tekin, Adem; Marx, Dominik; Jansen, Georg

2011-08-28

The infrared spectroscopy of molecules, complexes, and molecular aggregates dissolved in superfluid helium clusters, commonly called HElium NanoDroplet Isolation (HENDI) spectroscopy, is an established, powerful experimental technique for extracting high resolution ro-vibrational spectra at ultra-low temperatures. Realistic quantum simulations of such systems, in particular in cases where the solute is undergoing a chemical reaction, require accurate solute-helium potentials which are also simple enough to be efficiently evaluated over the vast number of steps required in typical Monte Carlo or molecular dynamics sampling. This precludes using global potential energy surfaces as often parameterized for small complexes in the realm of high-resolution spectroscopic investigations that, in view of the computational effort imposed, are focused on the intermolecular interaction of rigid molecules with helium. Simple Lennard-Jones-like pair potentials, on the other hand, fall short in providing the required flexibility and accuracy in order to account for chemical reactions of the solute molecule. Here, a general scheme of constructing sufficiently accurate site-site potentials for use in typical quantum simulations is presented. This scheme employs atom-based grids, accounts for local and global minima, and is applied to the special case of a HCl(H(2)O)(4) cluster solvated by helium. As a first step, accurate interaction energies of a helium atom with a set of representative configurations sampled from a trajectory following the dissociation of the HCl(H(2)O)(4) cluster were computed using an efficient combination of density functional theory and symmetry-adapted perturbation theory, i.e. the DFT-SAPT approach. For each of the sampled cluster configurations, a helium atom was placed at several hundred positions distributed in space, leading to an overall number of about 400,000 such quantum chemical calculations. The resulting total interaction energies, decomposed into several energetic contributions, served to fit a site-site potential, where the sites are located at the atomic positions and, additionally, pseudo-sites are distributed along the lines joining pairs of atom sites within the molecular cluster. This approach ensures that this solute-helium potential is able to describe both undissociated molecular and dissociated (zwitter-) ionic configurations, as well as the interconnecting reaction pathway without re-adjusting partial charges or other parameters depending on the particular configuration. Test calculations of the larger HCl(H(2)O)(5) cluster interacting with helium demonstrate the transferability of the derived site-site potential. This specific potential can be readily used in quantum simulations of such HCl/water clusters in bulk helium or helium nanodroplets, whereas the underlying construction procedure can be generalized to other molecular solutes in other atomic solvents such as those encountered in rare gas matrix isolation spectroscopy.

Quantum Electron Tunneling in Respiratory Complex I1

PubMed Central

Hayashi, Tomoyuki; Stuchebrukhov, Alexei A.

2014-01-01

We have simulated the atomistic details of electronic wiring of all Fe/S clusters in complex I, a key enzyme in the respiratory electron transport chain. The tunneling current theory of many-electron systems is applied to the broken-symmetry (BS) states of the protein at the ZINDO level. One-electron tunneling approximation is found to hold in electron tunneling between the anti-ferromagnetic binuclear and tetranuclear Fe/S clusters with moderate induced polarization of the core electrons. Calculated tunneling energy is about 3 eV higher than Fermi level in the band gap of the protein, which supports that the mechanism of electron transfer is quantum mechanical tunneling, as in the rest of electron transport chain. Resulting electron tunneling pathways consist of up to three key contributing protein residues between neighboring Fe/S clusters. A distinct signature of the wave properties of electrons is observed as quantum interferences when multiple tunneling pathways exist. In N6a-N6b, electron tunnels along different pathways depending on the involved BS states, suggesting possible fluctuations of the tunneling pathways driven by the local protein environment. The calculated distance dependence of the electron transfer rates with internal water molecules included are in good agreement with a reported phenomenological relation. PMID:21495666

Tunable Quantum Spin Liquidity in Mo3O13 Cluster Mott Insulators

NASA Astrophysics Data System (ADS)

Akbari-Sharbaf, Arash; Ziat, Djamel; Verrier, Aime; Quilliam, Jeffrey A.; Sinclair, Ryan; Zhou, Haidong D.; Sun, Xuefeng F.

A study of a tunable quantum spin liquid (QSL) phase in the compound Li2In1- x ScxMo3O8 (x = 0.2, 0.4, 0.6, 0.8, 1) will be presented. Crystal structure of these compounds can be viewed as Mo ions arranged on an asymmetric Kagome lattice (KL), with two different Mo-Mo bond lengths, separated by nonmagnetic layers composed of Li, In, and Sc ions. Using X-ray diffraction spectroscopy, muon spin relaxation spectroscopy, bulk magnetic susceptibility and specific heat measurements we show that by changing the composition of the nonmagnetic layers we can drive the system from an ordered antiferromagnetic state to a quantum spin liquid state. The mechanism responsible for the tunability of the magnetic phase in this class of materials may be associated with the degree of asymmetry of the KL controlled by the composition of the nonmagnetic layers. For high degree of asymmetry the constraint on the electronic distribution leads to a configuration of Mo3O8 clusters with net spin-1/2 per cluster arrange on a triangular lattice and long range antiferromagnetic order. For low degree of asymmetry the electronic distribution leads to a magnetic phase with QSL character. We acknowledge support from NSERC and CFREF.

Quantum liquid droplets in a mixture of Bose-Einstein condensates

NASA Astrophysics Data System (ADS)

Cabrera, C. R.; Tanzi, L.; Sanz, J.; Naylor, B.; Thomas, P.; Cheiney, P.; Tarruell, L.

2018-01-01

Quantum droplets are small clusters of atoms self-bound by the balance of attractive and repulsive forces. Here, we report on the observation of droplets solely stabilized by contact interactions in a mixture of two Bose-Einstein condensates. We demonstrate that they are several orders of magnitude more dilute than liquid helium by directly measuring their size and density via in situ imaging. We show that the droplets are stablized against collapse by quantum fluctuations and that they require a minimum atom number to be stable. Below that number, quantum pressure drives a liquid-to-gas transition that we map out as a function of interaction strength. These ultradilute isotropic liquids remain weakly interacting and constitute an ideal platform to benchmark quantum many-body theories.

Local density variation of gold nanoparticles in aquatic environments

NASA Astrophysics Data System (ADS)

Hosseinzadeh, F.; Shirazian, F.; Shahsavari, R.; Khoei, A. R.

2016-10-01

Gold (Au) nanoparticles are widely used in diagnosing cancer, imaging, and identification of therapeutic methods due to their particular quantum characteristics. This research presents different types of aqueous models and potentials used in TIP3P, to study the effect of the particle size and density of Au clusters in aquatic environments; so it can be useful to facilitate future investigation of the interaction of proteins with Au nanoparticles. The EAM potential is used to model the structure of gold clusters. It is observed that in the systems with identical gold/water density and different cluster radii, gold particles are distributed in aqueous environment almost identically. Thus, Au particles have identical local densities, and the root mean square displacement (RMSD) increases with a constant slope. However in systems with constant cluster radii and different gold/water densities, Au particle dispersion increases with density; as a result, the local density decreases and the RMSD increases with a larger slope. In such systems, the larger densities result in more blunted second peaks in gold-gold radial distribution functions, owing to more intermixing of the clusters and less FCC crystalline features at longer range, a mechanism that is mediated by the competing effects of gold-water and gold-gold interactions.

Merging symmetry projection methods with coupled cluster theory: Lessons from the Lipkin model Hamiltonian

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wahlen-Strothman, J. M.; Henderson, T. H.; Hermes, M. R.

Coupled cluster and symmetry projected Hartree-Fock are two central paradigms in electronic structure theory. However, they are very different. Single reference coupled cluster is highly successful for treating weakly correlated systems, but fails under strong correlation unless one sacrifices good quantum numbers and works with broken-symmetry wave functions, which is unphysical for finite systems. Symmetry projection is effective for the treatment of strong correlation at the mean-field level through multireference non-orthogonal configuration interaction wavefunctions, but unlike coupled cluster, it is neither size extensive nor ideal for treating dynamic correlation. We here examine different scenarios for merging these two dissimilar theories.more » We carry out this exercise over the integrable Lipkin model Hamiltonian, which despite its simplicity, encompasses non-trivial physics for degenerate systems and can be solved via diagonalization for a very large number of particles. We show how symmetry projection and coupled cluster doubles individually fail in different correlation limits, whereas models that merge these two theories are highly successful over the entire phase diagram. Despite the simplicity of the Lipkin Hamiltonian, the lessons learned in this work will be useful for building an ab initio symmetry projected coupled cluster theory that we expect to be accurate in the weakly and strongly correlated limits, as well as the recoupling regime.« less

Influence of temperature on the molecular composition of ions and charged clusters during pure biogenic nucleation

NASA Astrophysics Data System (ADS)

Frege, Carla; Ortega, Ismael K.; Rissanen, Matti P.; Praplan, Arnaud P.; Steiner, Gerhard; Heinritzi, Martin; Ahonen, Lauri; Amorim, António; Bernhammer, Anne-Kathrin; Bianchi, Federico; Brilke, Sophia; Breitenlechner, Martin; Dada, Lubna; Dias, António; Duplissy, Jonathan; Ehrhart, Sebastian; El-Haddad, Imad; Fischer, Lukas; Fuchs, Claudia; Garmash, Olga; Gonin, Marc; Hansel, Armin; Hoyle, Christopher R.; Jokinen, Tuija; Junninen, Heikki; Kirkby, Jasper; Kürten, Andreas; Lehtipalo, Katrianne; Leiminger, Markus; Mauldin, Roy Lee; Molteni, Ugo; Nichman, Leonid; Petäjä, Tuukka; Sarnela, Nina; Schobesberger, Siegfried; Simon, Mario; Sipilä, Mikko; Stolzenburg, Dominik; Tomé, António; Vogel, Alexander L.; Wagner, Andrea C.; Wagner, Robert; Xiao, Mao; Yan, Chao; Ye, Penglin; Curtius, Joachim; Donahue, Neil M.; Flagan, Richard C.; Kulmala, Markku; Worsnop, Douglas R.; Winkler, Paul M.; Dommen, Josef; Baltensperger, Urs

2018-01-01

It was recently shown by the CERN CLOUD experiment that biogenic highly oxygenated molecules (HOMs) form particles under atmospheric conditions in the absence of sulfuric acid, where ions enhance the nucleation rate by 1-2 orders of magnitude. The biogenic HOMs were produced from ozonolysis of α-pinene at 5 °C. Here we extend this study to compare the molecular composition of positive and negative HOM clusters measured with atmospheric pressure interface time-of-flight mass spectrometers (APi-TOFs), at three different temperatures (25, 5 and -25 °C). Most negative HOM clusters include a nitrate (NO3-) ion, and the spectra are similar to those seen in the nighttime boreal forest. On the other hand, most positive HOM clusters include an ammonium (NH4+) ion, and the spectra are characterized by mass bands that differ in their molecular weight by ˜ 20 C atoms, corresponding to HOM dimers. At lower temperatures the average oxygen to carbon (O : C) ratio of the HOM clusters decreases for both polarities, reflecting an overall reduction of HOM formation with decreasing temperature. This indicates a decrease in the rate of autoxidation with temperature due to a rather high activation energy as has previously been determined by quantum chemical calculations. Furthermore, at the lowest temperature (-25 °C), the presence of C30 clusters shows that HOM monomers start to contribute to the nucleation of positive clusters. These experimental findings are supported by quantum chemical calculations of the binding energies of representative neutral and charged clusters.

Exact diagonalization library for quantum electron models

NASA Astrophysics Data System (ADS)

Iskakov, Sergei; Danilov, Michael

2018-04-01

We present an exact diagonalization C++ template library (EDLib) for solving quantum electron models, including the single-band finite Hubbard cluster and the multi-orbital impurity Anderson model. The observables that can be computed using EDLib are single particle Green's functions and spin-spin correlation functions. This code provides three different types of Hamiltonian matrix storage that can be chosen based on the model.

Note: The performance of new density functionals for a recent blind test of non-covalent interactions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mardirossian, Narbe; Head-Gordon, Martin

Benchmark datasets of non-covalent interactions are essential for assessing the performance of density functionals and other quantum chemistry approaches. In a recent blind test, Taylor et al. benchmarked 14 methods on a new dataset consisting of 10 dimer potential energy curves calculated using coupled cluster with singles, doubles, and perturbative triples (CCSD(T)) at the complete basis set (CBS) limit (80 data points in total). Finally, the dataset is particularly interesting because compressed, near-equilibrium, and stretched regions of the potential energy surface are extensively sampled.

Note: The performance of new density functionals for a recent blind test of non-covalent interactions

DOE PAGES

Mardirossian, Narbe; Head-Gordon, Martin

2016-11-09

Benchmark datasets of non-covalent interactions are essential for assessing the performance of density functionals and other quantum chemistry approaches. In a recent blind test, Taylor et al. benchmarked 14 methods on a new dataset consisting of 10 dimer potential energy curves calculated using coupled cluster with singles, doubles, and perturbative triples (CCSD(T)) at the complete basis set (CBS) limit (80 data points in total). Finally, the dataset is particularly interesting because compressed, near-equilibrium, and stretched regions of the potential energy surface are extensively sampled.

Ab initio simulations of scanning-tunneling-microscope images with embedding techniques and application to C58-dimers on Au(111).

PubMed

Wilhelm, Jan; Walz, Michael; Stendel, Melanie; Bagrets, Alexei; Evers, Ferdinand

2013-05-14

We present a modification of the standard electron transport methodology based on the (non-equilibrium) Green's function formalism to efficiently simulate STM-images. The novel feature of this method is that it employs an effective embedding technique that allows us to extrapolate properties of metal substrates with adsorbed molecules from quantum-chemical cluster calculations. To illustrate the potential of this approach, we present an application to STM-images of C58-dimers immobilized on Au(111)-surfaces that is motivated by recent experiments.

Multiconfiguration pair-density functional theory investigation of the electronic spectrum of MnO4-

NASA Astrophysics Data System (ADS)

Sharma, Prachi; Truhlar, Donald G.; Gagliardi, Laura

2018-03-01

The electronic spectrum of permanganate ions contains various highly multiconfigurational ligand-to-metal charge transfer states and is notorious for being one of the most challenging systems to be treated by quantum-chemical methods. Here we studied the lowest nine vertical excitation energies using restricted active space second-order perturbation theory (RASPT2) and multiconfiguration pair-density functional theory (MC-PDFT) to test and compare these two theories in computing such a challenging spectrum. The results are compared to literature data, including time-dependent density functional theory, completely renormalized equation-of-motion couple-cluster theory with single and double excitations, symmetry-adapted-cluster configuration interaction, and experimental spectra in the gas phase and solution. Our results show that MC-PDFT accurately predicts the spectrum at a significantly reduced cost as compared to RASPT2.

Multiconfiguration pair-density functional theory investigation of the electronic spectrum of MnO4.

PubMed

Sharma, Prachi; Truhlar, Donald G; Gagliardi, Laura

2018-03-28

The electronic spectrum of permanganate ions contains various highly multiconfigurational ligand-to-metal charge transfer states and is notorious for being one of the most challenging systems to be treated by quantum-chemical methods. Here we studied the lowest nine vertical excitation energies using restricted active space second-order perturbation theory (RASPT2) and multiconfiguration pair-density functional theory (MC-PDFT) to test and compare these two theories in computing such a challenging spectrum. The results are compared to literature data, including time-dependent density functional theory, completely renormalized equation-of-motion couple-cluster theory with single and double excitations, symmetry-adapted-cluster configuration interaction, and experimental spectra in the gas phase and solution. Our results show that MC-PDFT accurately predicts the spectrum at a significantly reduced cost as compared to RASPT2.

Asymmetric Bidirectional Controlled Teleportation by Using Six-qubit Cluster State

NASA Astrophysics Data System (ADS)

Li, Yuan-hua; Nie, Li-ping; Li, Xiao-lan; Sang, Ming-huang

2016-06-01

We propose a scheme for asymmetric bidirectional controlled teleportation by using a six-qubit cluster state as quantum channel. In our scheme, Alice can transmit an arbitrary two-qubit entangled state to Bob and at the same time Bob can teleport an arbitrary single-qubit state to Alice under the control of the supervisor Charlie.

A universal matter-wave interferometer with optical ionization gratings in the time-domain

PubMed Central

Haslinger, Philipp; Dörre, Nadine; Geyer, Philipp; Rodewald, Jonas; Nimmrichter, Stefan; Arndt, Markus

2015-01-01

Matter-wave interferometry with atoms1 and molecules2 has attracted a rapidly growing interest throughout the last two decades both in demonstrations of fundamental quantum phenomena and in quantum-enhanced precision measurements. Such experiments exploit the non-classical superposition of two or more position and momentum states which are coherently split and rejoined to interfere3-11. Here, we present the experimental realization of a universal near-field interferometer built from three short-pulse single-photon ionization gratings12,13. We observe quantum interference of fast molecular clusters, with a composite de Broglie wavelength as small as 275 fm. Optical ionization gratings are largely independent of the specific internal level structure and are therefore universally applicable to different kinds of nanoparticles, ranging from atoms to clusters, molecules and nanospheres. The interferometer is sensitive to fringe shifts as small as a few nanometers and yet robust against velocity-dependent phase shifts, since the gratings exist only for nanoseconds and form an interferometer in the time-domain. PMID:25983851

High-Resolution Infrared Spectroscopy of Imidazole Clusters in Helium Droplets Using Quantum Cascade Lasers

NASA Astrophysics Data System (ADS)

Mani, Devendra; Can, Cihad; Pal, Nitish; Schwaab, Gerhard; Havenith, Martina

2017-06-01

Imidazole ring is a part of many biologically important molecules and drugs. Imidazole monomer, dimer and its complexes with water have earlier been studied using infrared spectroscopy in helium droplets^{1,2} and molecular beams^{3}. These studies were focussed on the N-H and O-H stretch regions, covering the spectral region of 3200-3800 \\wn. We have extended the studies on imidazole clusters into the ring vibration region. The imidazole clusters were isolated in helium droplets and were probed using a combination of infrared spectroscopy and mass spectrometry. The spectra in the region of 1000-1100 \\wn and 1300-1460 \\wn were recorded using quantum cascade lasers. Some of the observed bands could be assigned to imidazole monomer and higher order imidazole clusters, using pickup curve analysis and ab initio calculations. Work is still in progress. The results will be discussed in detail in the talk. References: 1) M.Y. Choi and R.E. Miller, J. Phys. Chem. A, 110, 9344 (2006). 2) M.Y. Choi and R.E. Miller, Chem. Phys. Lett., 477, 276 (2009). 3) J. Zischang, J. J. Lee and M. Suhm, J. Chem. Phys., 135, 061102 (2011). Note: This work was supported by the Cluster of Excellence RESOLV (Ruhr-Universitat EXC1069) funded by the Deutsche Forschungsgemeinschaft.

Sorting Five Human Tumor Types Reveals Specific Biomarkers and Background Classification Genes.

PubMed

Roche, Kimberly E; Weinstein, Marvin; Dunwoodie, Leland J; Poehlman, William L; Feltus, Frank A

2018-05-25

We applied two state-of-the-art, knowledge independent data-mining methods - Dynamic Quantum Clustering (DQC) and t-Distributed Stochastic Neighbor Embedding (t-SNE) - to data from The Cancer Genome Atlas (TCGA). We showed that the RNA expression patterns for a mixture of 2,016 samples from five tumor types can sort the tumors into groups enriched for relevant annotations including tumor type, gender, tumor stage, and ethnicity. DQC feature selection analysis discovered 48 core biomarker transcripts that clustered tumors by tumor type. When these transcripts were removed, the geometry of tumor relationships changed, but it was still possible to classify the tumors using the RNA expression profiles of the remaining transcripts. We continued to remove the top biomarkers for several iterations and performed cluster analysis. Even though the most informative transcripts were removed from the cluster analysis, the sorting ability of remaining transcripts remained strong after each iteration. Further, in some iterations we detected a repeating pattern of biological function that wasn't detectable with the core biomarker transcripts present. This suggests the existence of a "background classification" potential in which the pattern of gene expression after continued removal of "biomarker" transcripts could still classify tumors in agreement with the tumor type.

Exploring the possibility to store the mixed oxygen-hydrogen cluster in clathrate hydrate in molar ratio 1:2 (O2+2H2).

PubMed

Qin, Yan; Du, Qi-Shi; Xie, Neng-Zhong; Li, Jian-Xiu; Huang, Ri-Bo

2017-05-01

An interesting possibility is explored: storing the mixture of oxygen and hydrogen in clathrate hydrate in molar ratio 1:2. The interaction energies between oxygen, hydrogen, and clathrate hydrate are calculated using high level quantum chemical methods. The useful conclusion points from this study are summarized as follows. (1) The interaction energies of oxygen-hydrogen mixed cluster are larger than the energies of pure hydrogen molecular cluster. (2) The affinity of oxygen molecules with water molecules is larger than that of the hydrogen molecules with water molecules. (3) The dimension of O 2 -2H 2 interaction structure is smaller than the dimension of CO 2 -2H 2 interaction structure. (4) The escaping energy of oxygen molecules from the hydrate cell is larger than that of the hydrogen molecules. (5) The high affinity of the oxygen molecules with both the water molecules and the hydrogen molecules may promote the stability of oxygen-hydrogen mixture in the clathrate hydrate. Therefore it is possible to store the mixed (O 2 +2H 2 ) cluster in clathrate hydrate. Copyright © 2017 Elsevier Inc. All rights reserved.

Local Response of Topological Order to an External Perturbation

NASA Astrophysics Data System (ADS)

Hamma, Alioscia; Cincio, Lukasz; Santra, Siddhartha; Zanardi, Paolo; Amico, Luigi

2013-05-01

We study the behavior of the Rényi entropies for the toric code subject to a variety of different perturbations, by means of 2D density matrix renormalization group and analytical methods. We find that Rényi entropies of different index α display derivatives with opposite sign, as opposed to typical symmetry breaking states, and can be detected on a very small subsystem regardless of the correlation length. This phenomenon is due to the presence in the phase of a point with flat entanglement spectrum, zero correlation length, and area law for the entanglement entropy. We argue that this kind of splitting is common to all the phases with a certain group theoretic structure, including quantum double models, cluster states, and other quantum spin liquids. The fact that the size of the subsystem does not need to scale with the correlation length makes it possible for this effect to be accessed experimentally.

Role of cationic size in the optical properties of the LiCl crystal surface: theoretical study.

PubMed

Abdel Halim, Wael Salah; Abdullah, Noha; Abdel-Aal, Safaa; Shalabi, A S

2012-06-01

The size of the cations (either Ca(2+), Sr(2+), Ga(+), or Au(+)) at the F(A1)-type color centers on the (100) surface of LiCl crystal plays an important role in the optical properties of this surface. In this work, double-well potentials at this surface were investigated using ab initio quantum mechanical methods. Quantum clusters were embedded in simulated Coulomb fields that closely approximate the Madelung fields of the host surface, and the ions that were the nearest neighbors to the F(A1) site were allowed to relax to equilibrium. The calculated Stokes-shifted optical transition bands, optical-optical conversion efficiency, and relaxed excited states of the defect-containing surface, as well as the orientational destruction of the color centers, recording sensitivity, exciton (energy) transfer, and the Glasner-Tompkins empirical relation were all found to be sensitive to the size of the dopant cation.

Flexible and Comprehensive Implementation of MD-PMM Approach in a General and Robust Code.

PubMed

Carrillo-Parramon, Oliver; Del Galdo, Sara; Aschi, Massimiliano; Mancini, Giordano; Amadei, Andrea; Barone, Vincenzo

2017-11-14

The Perturbed Matrix Method (PMM) approach to be used in combination with Molecular Dynamics (MD) trajectories (MD-PMM) has been recoded from scratch, improved in several aspects, and implemented in the Gaussian suite of programs for allowing a user-friendly and yet flexible tool to estimate quantum chemistry observables in complex systems in condensed phases. Particular attention has been devoted to a description of rigid and flexible quantum centers together with powerful essential dynamics and clustering approaches. The default implementation is fully black-box and does not require any external action concerning both MD and PMM sections. At the same time, fine-tuning of different parameters and use of external data are allowed in all the steps of the procedure. Two specific systems (Tyrosine and Uridine) have been reinvestigated with the new version of the code in order to validate the implementation, check the performances, and illustrate some new features.

Criticality of the low-frequency conductivity for the bilayer quantum Heisenberg model

NASA Astrophysics Data System (ADS)

Nishiyama, Yoshihiro

2018-04-01

The criticality of the low-frequency conductivity for the bilayer quantum Heisenberg model was investigated numerically. The dynamical conductivity (associated with the O(3) symmetry) displays the inductor σ( ω) = ( iωL)-1 and capacitor iωC behaviors for the ordered and disordered phases, respectively. Both constants, C and L, have the same scaling dimension as that of the reciprocal paramagnetic gap Δ -1. Then, there arose a question to fix the set of critical amplitude ratios among them. So far, the O(2) case has been investigated in the context of the boson-vortex duality. In this paper, we employ the exact diagonalization method, which enables us to calculate the paramagnetic gap Δ directly. Thereby, the set of critical amplitude ratios as to C, L and Δ are estimated with the finite-size-scaling analysis for the cluster with N ≤ 34 spins.

Magnetic anisotropy in the Kitaev model systems Na2IrO3 and RuCl3

NASA Astrophysics Data System (ADS)

Chaloupka, Jiří; Khaliullin, Giniyat

2016-08-01

We study the ordered moment direction in the extended Kitaev-Heisenberg model relevant to honeycomb lattice magnets with strong spin-orbit coupling. We utilize numerical diagonalization and analyze the exact cluster ground states using a particular set of spin-coherent states, obtaining thereby quantum corrections to the magnetic anisotropy beyond conventional perturbative methods. It is found that the quantum fluctuations strongly modify the moment direction obtained at a classical level and are thus crucial for a precise quantification of the interactions. The results show that the moment direction is a sensitive probe of the model parameters in real materials. Focusing on the experimentally relevant zigzag phases of the model, we analyze the currently available neutron-diffraction and resonant x-ray-diffraction data on Na2IrO3 and RuCl3 and discuss the parameter regimes plausible in these Kitaev-Heisenberg model systems.

Molecular interactions in ethyl acetate-chlorobenzene binary solution: Dielectric, spectroscopic studies and quantum chemical calculations.

PubMed

Karthick, N K; Kumbharkhane, A C; Joshi, Y S; Mahendraprabu, A; Shanmugam, R; Elangovan, A; Arivazhagan, G

2017-05-05

Dielectric studies using Time Domain Reflectometry method has been carried out on the binary solution of Ethyl acetate (EA) with Chlorobenzene (CBZ) over the entire composition range. Spectroscopic (FTIR and 13 C NMR) signatures of neat EA, CBZ and their equimolar binary solution have also been recorded. The results of the spectroscopic studies favour the presence of (CBZ) CH⋯OC (EA), (EA) methylene CH⋯π electrons (CBZ) and (EA) methyl CH⋯Cl (CBZ) contacts which have been validated using quantum chemical calculations. Dimerization of CBZ has been identified. Presence of β-clusters has been identified in all the solutions. Although EA and CBZ molecules have nearly equal molar volumes, CBZ molecules experience larger hindrance for the rotation than EA molecules. Very small excess dielectric constant (ε E ) values may be correlated with weak heteromolecular forces and/or closed heteromolecular association. Copyright © 2017 Elsevier B.V. All rights reserved.

Molecular interactions in ethyl acetate-chlorobenzene binary solution: Dielectric, spectroscopic studies and quantum chemical calculations

NASA Astrophysics Data System (ADS)

Karthick, N. K.; Kumbharkhane, A. C.; Joshi, Y. S.; Mahendraprabu, A.; Shanmugam, R.; Elangovan, A.; Arivazhagan, G.

2017-05-01

Dielectric studies using Time Domain Reflectometry method has been carried out on the binary solution of Ethyl acetate (EA) with Chlorobenzene (CBZ) over the entire composition range. Spectroscopic (FTIR and 13C NMR) signatures of neat EA, CBZ and their equimolar binary solution have also been recorded. The results of the spectroscopic studies favour the presence of (CBZ) Csbnd H ⋯ Odbnd C (EA), (EA) methylene Csbnd H ⋯ π electrons (CBZ) and (EA) methyl Csbnd H ⋯ Cl (CBZ) contacts which have been validated using quantum chemical calculations. Dimerization of CBZ has been identified. Presence of β-clusters has been identified in all the solutions. Although EA and CBZ molecules have nearly equal molar volumes, CBZ molecules experience larger hindrance for the rotation than EA molecules. Very small excess dielectric constant (εE) values may be correlated with weak heteromolecular forces and/or closed heteromolecular association.

Semiempirical Quantum Chemical Calculations Accelerated on a Hybrid Multicore CPU-GPU Computing Platform.

PubMed

Wu, Xin; Koslowski, Axel; Thiel, Walter

2012-07-10

In this work, we demonstrate that semiempirical quantum chemical calculations can be accelerated significantly by leveraging the graphics processing unit (GPU) as a coprocessor on a hybrid multicore CPU-GPU computing platform. Semiempirical calculations using the MNDO, AM1, PM3, OM1, OM2, and OM3 model Hamiltonians were systematically profiled for three types of test systems (fullerenes, water clusters, and solvated crambin) to identify the most time-consuming sections of the code. The corresponding routines were ported to the GPU and optimized employing both existing library functions and a GPU kernel that carries out a sequence of noniterative Jacobi transformations during pseudodiagonalization. The overall computation times for single-point energy calculations and geometry optimizations of large molecules were reduced by one order of magnitude for all methods, as compared to runs on a single CPU core.

Pentachlorophenol radical cations generated on Fe(III)-montmorillonite initiate octachlorodibenzo-p-dioxin formation in clays: DFT and FTIR studies

PubMed Central

Gu, Cheng; Liu, Cun; Johnston, Cliff T.; Teppen, Brian J.; Li, Hui; Boyd, Stephen A.

2011-01-01

Octachlorodibenzodioxin (OCDD) forms spontaneously from pentachlorophenol (PCP) on the surfaces of Fe(III)-saturated smectite clay (1). Here, we used in situ FTIR methods and quantum mechanical calculations to determine the mechanism by which this reaction is initiated. As the clay was dehydrated, vibrational spectra showed new peaks that grew and then reversibly disappeared as the clay rehydrated. First principle DFT calculations of hydrated Fe-PCP clusters reproduced these transient FTIR peaks when inner-sphere complexation and concomitant electron transfer produced Fe(II) and PCP radical cations. Thus, our experimental (FTIR) and theoretical (quantum mechanical) results mutually support the hypothesis that OCDD formation on Fe-smectite surfaces is initiated by the reversible formation of metastable PCP radical cations via single electron transfer from PCP to Fe(III). The negatively charged clay surface apparently selects for this reaction mechanism by stabilizing PCP radical cations. PMID:21254769

Size dependence in tunneling spectra of PbSe quantum-dot arrays.

PubMed

Ou, Y C; Cheng, S F; Jian, W B

2009-07-15

Interdot Coulomb interactions and collective Coulomb blockade were theoretically argued to be a newly important topic, and experimentally identified in semiconductor quantum dots, formed in the gate confined two-dimensional electron gas system. Developments of cluster science and colloidal synthesis accelerated the studies of electron transport in colloidal nanocrystal or quantum-dot solids. To study the interdot coupling, various sizes of two-dimensional arrays of colloidal PbSe quantum dots are self-assembled on flat gold surfaces for scanning tunneling microscopy and scanning tunneling spectroscopy measurements at both room and liquid-nitrogen temperatures. The tip-to-array, array-to-substrate, and interdot capacitances are evaluated and the tunneling spectra of quantum-dot arrays are analyzed by the theory of collective Coulomb blockade. The current-voltage of PbSe quantum-dot arrays conforms properly to a scaling power law function. In this study, the dependence of tunneling spectra on the sizes (numbers of quantum dots) of arrays is reported and the capacitive coupling between quantum dots in the arrays is explored.

Entanglement Concentration for Arbitrary Four-Photon Cluster State Assisted with Single Photons

NASA Astrophysics Data System (ADS)

Zhao, Sheng-Yang; Cai, Chun; Liu, Jiong; Zhou, Lan; Sheng, Yu-Bo

2016-02-01

We present an entanglement concentration protocol (ECP) to concentrate arbitrary four-photon less-entangled cluster state into maximally entangled cluster state. Different from other ECPs for cluster state, we only exploit the single photon as auxiliary, which makes this protocol feasible and economic. In our ECP, the concentrated maximally entangled state can be retained for further application and the discarded state can be reused for a higher success probability. This ECP works with the help of cross-Kerr nonlinearity and conventional photon detectors. This ECP may be useful in future one-way quantum computation.

Teleportation of Three-Qubit State via Six-qubit Cluster State

NASA Astrophysics Data System (ADS)

Yu, Li-zhi; Sun, Shao-xin

2015-05-01

A scheme of probabilistic teleportation was proposed. In this scheme, we took a six-qubit nonmaximally cluster state as the quantum channel to teleport an unknown three-qubit entangled state. Based on Bob's three times Bell state measurement (BSM) results, the receiver Bob can by introducing an auxiliary particle and the appropriate transformation to reconstruct the initial state with a certain probability. We found that, the successful transmission probability depend on the absolute value of coefficients of two of six particle cluster state minimum.

Conjugate-gradient optimization method for orbital-free density functional calculations.

PubMed

Jiang, Hong; Yang, Weitao

2004-08-01

Orbital-free density functional theory as an extension of traditional Thomas-Fermi theory has attracted a lot of interest in the past decade because of developments in both more accurate kinetic energy functionals and highly efficient numerical methodology. In this paper, we developed a conjugate-gradient method for the numerical solution of spin-dependent extended Thomas-Fermi equation by incorporating techniques previously used in Kohn-Sham calculations. The key ingredient of the method is an approximate line-search scheme and a collective treatment of two spin densities in the case of spin-dependent extended Thomas-Fermi problem. Test calculations for a quartic two-dimensional quantum dot system and a three-dimensional sodium cluster Na216 with a local pseudopotential demonstrate that the method is accurate and efficient. (c) 2004 American Institute of Physics.

Efficient Remote Preparation of Four-Qubit Cluster-Type Entangled States with Multi-Party Over Partially Entangled Channels

NASA Astrophysics Data System (ADS)

Wang, Dong; Hoehn, Ross D.; Ye, Liu; Kais, Sabre

2016-07-01

We present a strategy for realizing multiparty-controlled remote state preparation (MCRSP) for a family of four-qubit cluster-type states by taking a pair of partial entanglements as the quantum channels. In this scenario, the encoded information is transmitted from the sender to a spatially separated receiver with control of the transmission by multiple parties. Predicated on the collaboration of all participants, the desired state can be faithfully restored at the receiver's location with high success probability by application of additional appropriate local operations and necessary classical communication. Moreover, this proposal for MCRSP can be faithfully achieved with unit total success probability when the quantum channels are distilled to maximally entangled ones.

Investigating the significance of zero-point motion in small molecular clusters of sulphuric acid and water

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stinson, Jake L.; Kathmann, Shawn M.; Ford, Ian J.

2014-01-14

The nucleation of particles from trace gases in the atmosphere is an important source of cloud condensation nuclei (CCN), and these are vital for the formation of clouds in view of the high supersaturations required for homogeneous water droplet nucleation. The methods of quantum chemistry have increasingly been employed to model nucleation due to their high accuracy and efficiency in calculating configurational energies; and nucleation rates can be obtained from the associated free energies of particle formation. However, even in such advanced approaches, it is typically assumed that the nuclei have a classical nature, which is questionable for some systems.more » The importance of zero-point motion (also known as quantum nuclear dynamics) in modelling small clusters of sulphuric acid and water is tested here using the path integral molecular dynamics (PIMD) method at the density functional theory (DFT) level of theory. We observe a small zero-point effect on the the equilibrium structures of certain clusters. One configuration is found to display a bimodal behaviour at 300 K in contrast to the stable ionised state suggested from a zero temperature classical geometry optimisation. The general effect of zero-point motion is to promote the extent of proton transfer with respect to classical behaviour. We thank Prof. Angelos Michaelides and his group in University College London (UCL) for practical advice and helpful discussions. This work benefited from interactions with the Thomas Young Centre through seminar and discussions involving the PIMD method. SMK was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. JLS and IJF were supported by the IMPACT scheme at UCL and by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences. We are grateful for use of the UCL Legion High Performance Computing Facility and the resources of the National Energy Research Scientific Computing Center (NERSC), which is supported by the U.S. Department of Energy, Office of Science of the under Contract No. DE-AC02-05CH11231.« less

Energetics of charged metal clusters containing vacancies

NASA Astrophysics Data System (ADS)

Pogosov, Valentin V.; Reva, Vitalii I.

2018-01-01

We study theoretically large metal clusters containing vacancies. We propose an approach, which combines the Kohn-Sham results for monovacancy in a bulk of metal and analytical expansions in small parameters cv (relative concentration of vacancies) and RN,v -1, RN ,v being cluster radii. We obtain expressions of the ionization potential and electron affinity in the form of corrections to electron work function, which require only the characteristics of 3D defect-free metal. The Kohn-Sham method is used to calculate the electron profiles, ionization potential, electron affinity, electrical capacitance; dissociation, cohesion, and monovacancy-formation energies of the small perfect clusters NaN, MgN, AlN (N ≤ 270) and the clusters containing a monovacancy (N ≥ 12) in the stabilized-jellium model. The quantum-sized dependences for monovacancy-formation energies are calculated for the Schottky scenario and the "bubble blowing" scenario, and their asymptotic behavior is also determined. It is shown that the asymptotical behaviors of size dependences for these two mechanisms differ from each other and weakly depend on the number of atoms in the cluster. The contribution of monovacancy to energetics of charged clusters and the size dependences of their characteristics and asymptotics are discussed. It is shown that the difference between the characteristics for the neutral and charged clusters is entirely determined by size dependences of ionization potential and electron affinity. Obtained analytical dependences may be useful for the analysis of the results of photoionization experiments and for the estimation of the size dependences of the vacancy concentration including the vicinity of the melting point.

Hydration of a Large Anionic Charge Distribution - Naphthalene-Water Cluster Anions

NASA Astrophysics Data System (ADS)

Weber, J. Mathias; Adams, Christopher L.

2010-06-01

We report the infrared spectra of anionic clusters of naphthalene with up to three water molecules. Comparison of the experimental infrared spectra with theoretically predicted spectra from quantum chemistry calculations allow conclusions regarding the structures of the clusters under study. The first water molecule forms two hydrogen bonds with the π electron system of the naphthalene moiety. Subsequent water ligands interact with both the naphthalene and the other water ligands to form hydrogen bonded networks, similar to other hydrated anion clusters. Naphthalene-water anion clusters illustrate how water interacts with negative charge delocalized over a large π electron system. The clusters are interesting model systems that are discussed in the context of wetting of graphene surfaces and polyaromatic hydrocarbons.

Advances in molecular quantum chemistry contained in the Q-Chem 4 program package

NASA Astrophysics Data System (ADS)

Shao, Yihan; Gan, Zhengting; Epifanovsky, Evgeny; Gilbert, Andrew T. B.; Wormit, Michael; Kussmann, Joerg; Lange, Adrian W.; Behn, Andrew; Deng, Jia; Feng, Xintian; Ghosh, Debashree; Goldey, Matthew; Horn, Paul R.; Jacobson, Leif D.; Kaliman, Ilya; Khaliullin, Rustam Z.; Kuś, Tomasz; Landau, Arie; Liu, Jie; Proynov, Emil I.; Rhee, Young Min; Richard, Ryan M.; Rohrdanz, Mary A.; Steele, Ryan P.; Sundstrom, Eric J.; Woodcock, H. Lee, III; Zimmerman, Paul M.; Zuev, Dmitry; Albrecht, Ben; Alguire, Ethan; Austin, Brian; Beran, Gregory J. O.; Bernard, Yves A.; Berquist, Eric; Brandhorst, Kai; Bravaya, Ksenia B.; Brown, Shawn T.; Casanova, David; Chang, Chun-Min; Chen, Yunqing; Chien, Siu Hung; Closser, Kristina D.; Crittenden, Deborah L.; Diedenhofen, Michael; DiStasio, Robert A., Jr.; Do, Hainam; Dutoi, Anthony D.; Edgar, Richard G.; Fatehi, Shervin; Fusti-Molnar, Laszlo; Ghysels, An; Golubeva-Zadorozhnaya, Anna; Gomes, Joseph; Hanson-Heine, Magnus W. D.; Harbach, Philipp H. P.; Hauser, Andreas W.; Hohenstein, Edward G.; Holden, Zachary C.; Jagau, Thomas-C.; Ji, Hyunjun; Kaduk, Benjamin; Khistyaev, Kirill; Kim, Jaehoon; Kim, Jihan; King, Rollin A.; Klunzinger, Phil; Kosenkov, Dmytro; Kowalczyk, Tim; Krauter, Caroline M.; Lao, Ka Un; Laurent, Adèle D.; Lawler, Keith V.; Levchenko, Sergey V.; Lin, Ching Yeh; Liu, Fenglai; Livshits, Ester; Lochan, Rohini C.; Luenser, Arne; Manohar, Prashant; Manzer, Samuel F.; Mao, Shan-Ping; Mardirossian, Narbe; Marenich, Aleksandr V.; Maurer, Simon A.; Mayhall, Nicholas J.; Neuscamman, Eric; Oana, C. Melania; Olivares-Amaya, Roberto; O'Neill, Darragh P.; Parkhill, John A.; Perrine, Trilisa M.; Peverati, Roberto; Prociuk, Alexander; Rehn, Dirk R.; Rosta, Edina; Russ, Nicholas J.; Sharada, Shaama M.; Sharma, Sandeep; Small, David W.; Sodt, Alexander; Stein, Tamar; Stück, David; Su, Yu-Chuan; Thom, Alex J. W.; Tsuchimochi, Takashi; Vanovschi, Vitalii; Vogt, Leslie; Vydrov, Oleg; Wang, Tao; Watson, Mark A.; Wenzel, Jan; White, Alec; Williams, Christopher F.; Yang, Jun; Yeganeh, Sina; Yost, Shane R.; You, Zhi-Qiang; Zhang, Igor Ying; Zhang, Xing; Zhao, Yan; Brooks, Bernard R.; Chan, Garnet K. L.; Chipman, Daniel M.; Cramer, Christopher J.; Goddard, William A., III; Gordon, Mark S.; Hehre, Warren J.; Klamt, Andreas; Schaefer, Henry F., III; Schmidt, Michael W.; Sherrill, C. David; Truhlar, Donald G.; Warshel, Arieh; Xu, Xin; Aspuru-Guzik, Alán; Baer, Roi; Bell, Alexis T.; Besley, Nicholas A.; Chai, Jeng-Da; Dreuw, Andreas; Dunietz, Barry D.; Furlani, Thomas R.; Gwaltney, Steven R.; Hsu, Chao-Ping; Jung, Yousung; Kong, Jing; Lambrecht, Daniel S.; Liang, WanZhen; Ochsenfeld, Christian; Rassolov, Vitaly A.; Slipchenko, Lyudmila V.; Subotnik, Joseph E.; Van Voorhis, Troy; Herbert, John M.; Krylov, Anna I.; Gill, Peter M. W.; Head-Gordon, Martin

2015-01-01

A summary of the technical advances that are incorporated in the fourth major release of the Q-Chem quantum chemistry program is provided, covering approximately the last seven years. These include developments in density functional theory methods and algorithms, nuclear magnetic resonance (NMR) property evaluation, coupled cluster and perturbation theories, methods for electronically excited and open-shell species, tools for treating extended environments, algorithms for walking on potential surfaces, analysis tools, energy and electron transfer modelling, parallel computing capabilities, and graphical user interfaces. In addition, a selection of example case studies that illustrate these capabilities is given. These include extensive benchmarks of the comparative accuracy of modern density functionals for bonded and non-bonded interactions, tests of attenuated second order Møller-Plesset (MP2) methods for intermolecular interactions, a variety of parallel performance benchmarks, and tests of the accuracy of implicit solvation models. Some specific chemical examples include calculations on the strongly correlated Cr2 dimer, exploring zeolite-catalysed ethane dehydrogenation, energy decomposition analysis of a charged ter-molecular complex arising from glycerol photoionisation, and natural transition orbitals for a Frenkel exciton state in a nine-unit model of a self-assembling nanotube.

The Importance of Electron Correlation on Stacking Interaction of Adenine-Thymine Base-Pair Step in B-DNA: A Quantum Monte Carlo Study.

PubMed

Hongo, Kenta; Cuong, Nguyen Thanh; Maezono, Ryo

2013-02-12

We report fixed-node diffusion Monte Carlo (DMC) calculations of stacking interaction energy between two adenine(A)-thymine(T) base pairs in B-DNA (AA:TT), for which reference data are available, obtained from a complete basis set estimate of CCSD(T) (coupled-cluster with singles, doubles, and perturbative triples). We consider four sets of nodal surfaces obtained from self-consistent field calculations and examine how the different nodal surfaces affect the DMC potential energy curves of the AA:TT molecule and the resulting stacking energies. We find that the DMC potential energy curves using the different nodes look similar to each other as a whole. We also benchmark the performance of various quantum chemistry methods, including Hartree-Fock (HF) theory, second-order Møller-Plesset perturbation theory (MP2), and density functional theory (DFT). The DMC and recently developed DFT results of the stacking energy reasonably agree with the reference, while the HF, MP2, and conventional DFT methods give unsatisfactory results.

Measurement-based quantum teleportation on finite AKLT chains

NASA Astrophysics Data System (ADS)

Fujii, Akihiko; Feder, David

In the measurement-based model of quantum computation, universal quantum operations are effected by making repeated local measurements on resource states which contain suitable entanglement. Resource states include two-dimensional cluster states and the ground state of the Affleck-Kennedy-Lieb-Tasaki (AKLT) state on the honeycomb lattice. Recent studies suggest that measurements on one-dimensional systems in the Haldane phase teleport perfect single-qubit gates in the correlation space, protected by the underlying symmetry. As laboratory realizations of symmetry-protected states will necessarily be finite, we investigate the potential for quantum gate teleportation in finite chains of a bilinear-biquadratic Hamiltonian which is a generalization of the AKLT model representing the full Haldane phase.

Improving the Teleportation Scheme of Three-Qubit State with a Four-Qubit Quantum Channel

NASA Astrophysics Data System (ADS)

Cai, Tao; Jiang, Min

2018-01-01

Recently, Zhao-Hui Wei et al. (Int. J. Theor. Phys. 55, 4687, 2016) proposed an improved quantum teleportation scheme for one three-qubit unknown state with a four-qubit quantum channel based on the original one proposed by Binayak S. Choudhury and Arpan Dhara (Int. J. Theor. Phys. 55, 3393, 2016). According to their schemes, the three-qubit entangled state could be teleported with one four-qubit cluster state and five-qubit joint measurements or four-qubit joint measurements. In this paper, we present an improved protocol only with single-qubit measurements and the same four-qubit quantum channel, lessening the difficulty and intensity of necessary operations.

Composite Reinforcement using Boron Nitride Nanotubes

DTIC Science & Technology

2014-05-09

while retaining the nanotube structure. This project involves the use of computational quantum chemistry to study interactions of aluminium (Al...small clusters of 1–4 metal atoms. The effect of varying the radius of the nanotubes and the size of aluminium and titanium clusters was considered...15. SUBJECT TERMS Boron Nitride Nanotubes, composite materials, Aluminum Alloys , Titanium Alloy , Theoretical Chemistry 16. SECURITY

Poly(vinylpyrrolidone) supported copper nanoclusters: glutathione enhanced blue photoluminescence for application in phosphor converted light emitting devices

NASA Astrophysics Data System (ADS)

Wang, Zhenguang; Susha, Andrei S.; Chen, Bingkun; Reckmeier, Claas; Tomanec, Ondrej; Zboril, Radek; Zhong, Haizheng; Rogach, Andrey L.

2016-03-01

Poly(vinylpyrrolidone) supported Cu nanoclusters were synthesized by reduction of Cu(ii) ions with ascorbic acid in water, and initially showed blue photoluminescence with a quantum yield of 8%. An enhancement of the emission quantum yield has been achieved by treatment of Cu clusters with different electron-rich ligands, with the most pronounced effect (photoluminescence quantum yield of 27%) achieved with glutathione. The bright blue emission of glutathione treated Cu NCs is fully preserved in the solid state powder, which has been combined with commercial green and red phosphors to fabricate down-conversion white light emitting diodes with a high colour rendering index of 92.Poly(vinylpyrrolidone) supported Cu nanoclusters were synthesized by reduction of Cu(ii) ions with ascorbic acid in water, and initially showed blue photoluminescence with a quantum yield of 8%. An enhancement of the emission quantum yield has been achieved by treatment of Cu clusters with different electron-rich ligands, with the most pronounced effect (photoluminescence quantum yield of 27%) achieved with glutathione. The bright blue emission of glutathione treated Cu NCs is fully preserved in the solid state powder, which has been combined with commercial green and red phosphors to fabricate down-conversion white light emitting diodes with a high colour rendering index of 92. Electronic supplementary information (ESI) available: The optical spectra of control experiments for Cu NC synthesis, optimization of the reaction conditions, and spectra for LEDs chips and blue LEDs. See DOI: 10.1039/c6nr00806b

Structural transition of (InSb)n clusters at n = 6-10

NASA Astrophysics Data System (ADS)

Lu, Qi Liang; Luo, Qi Quan; Huang, Shou Guo; Li, Yi De

2016-10-01

An optimization strategy combining global semi-empirical quantum mechanical search with all-electron density functional theory was adopted to determine the lowest energy structure of (InSb)n clusters with n = 6-10. A new structural growth pattern of the clusters was observed. The lowest energy structures of (InSb)6 and (InSb)8 were different from that of previously reported results. Competition existed between core-shell and cage-like structures of (InSb)8. The structural transition of (InSb)n clusters occurred at size n = 8-9. For (InSb)9 and (InSb)10 clusters, core-shell structure were more energetically favorable than the cage. The corresponding electronic properties were investigated.

Quantum tunneling of magnetization and related phenomena in molecular materials.

PubMed

Gatteschi, Dante; Sessoli, Roberta

2003-01-20

Molecules comprising a large number of coupled paramagnetic centers are attracting much interest because they may show properties which are intermediate between those of simple paramagnets and classical bulk magnets and provide unambiguous evidence of quantum size effects in magnets. To date, two cluster families, usually referred to as Mn12 and Fe8, have been used to test theories. However, it is reasonable to predict that other classes of molecules will be discovered which have similar or superior properties. To do this it is necessary that synthetic chemists have a good understanding of the correlation between the structure and properties of the molecules, for this it is necessary that concepts such as quantum tunneling, quantum coherence, quantum oscillations are understood. The goal of this article is to review the fundamental concepts needed to understand quantum size effects in molecular magnets and to critically report what has been done in the field to date.

Experimental realization of a one-way quantum computer algorithm solving Simon's problem.

PubMed

Tame, M S; Bell, B A; Di Franco, C; Wadsworth, W J; Rarity, J G

2014-11-14

We report an experimental demonstration of a one-way implementation of a quantum algorithm solving Simon's problem-a black-box period-finding problem that has an exponential gap between the classical and quantum runtime. Using an all-optical setup and modifying the bases of single-qubit measurements on a five-qubit cluster state, key representative functions of the logical two-qubit version's black box can be queried and solved. To the best of our knowledge, this work represents the first experimental realization of the quantum algorithm solving Simon's problem. The experimental results are in excellent agreement with the theoretical model, demonstrating the successful performance of the algorithm. With a view to scaling up to larger numbers of qubits, we analyze the resource requirements for an n-qubit version. This work helps highlight how one-way quantum computing provides a practical route to experimentally investigating the quantum-classical gap in the query complexity model.

Cooperative effects in the structuring of fluoride water clusters: Ab initio hybrid quantum mechanical/molecular mechanical model incorporating polarizable fluctuating charge solvent

NASA Astrophysics Data System (ADS)

Bryce, Richard A.; Vincent, Mark A.; Malcolm, Nathaniel O. J.; Hillier, Ian H.; Burton, Neil A.

1998-08-01

A new hybrid quantum mechanical/molecular mechanical model of solvation is developed and used to describe the structure and dynamics of small fluoride/water clusters, using an ab initio wave function to model the ion and a fluctuating charge potential to model the waters. Appropriate parameters for the water-water and fluoride-water interactions are derived, with the fluoride anion being described by density functional theory and a large Gaussian basis. The role of solvent polarization in determining the structure and energetics of F(H2O)4- clusters is investigated, predicting a slightly greater stability of the interior compared to the surface structure, in agreement with ab initio studies. An extended Lagrangian treatment of the polarizable water, in which the water atomic charges fluctuate dynamically, is used to study the dynamics of F(H2O)4- cluster. A simulation using a fixed solvent charge distribution indicates principally interior, solvated states for the cluster. However, a preponderance of trisolvated configurations is observed using the polarizable model at 300 K, which involves only three direct fluoride-water hydrogen bonds. Ab initio calculations confirm this trisolvated species as a thermally accessible state at room temperature, in addition to the tetrasolvated interior and surface structures. Extension of this polarizable water model to fluoride clusters with five and six waters gave less satisfactory agreement with experimental energies and with ab initio geometries. However, our results do suggest that a quantitative model of solvent polarization is fundamental for an accurate understanding of the properties of anionic water clusters.

Enhanced positron trapping by Ag nanoclusters at low temperatures: A challenge of positron sensitivity to quantum dots

NASA Astrophysics Data System (ADS)

Zou, B.; Qi, N.; Liu, Z. W.; Chen, Z. Q.; Liu, H. Q.; Yi, D. Q.; Tang, Z.

2017-03-01

Microstructure evolution of three Al-Ag alloys with different Ag contents (1 wt. % Ag, 5 wt. % Ag, and 15 wt. % Ag) was studied by positron annihilation spectroscopy during the aging process. In situ measurements of the positron lifetime and Doppler broadening of annihilation radiation indicate the fast formation of Ag-rich clusters during natural aging of the alloys. The formation of Ag-rich clusters was further confirmed by coincidence Doppler broadening measurements. The Ag signal reflected by the Coincidence Doppler broadening spectrum increases with increasing Ag content and is further enhanced after subsequent artificial aging at 140 °C. This might be due to the increase in the size of Ag clusters. The temperature dependence of the Doppler broadening spectra between 10 K and 290 K was measured for the Al-Ag alloys after natural and artificial aging. Detrapping of positrons from Ag clusters with increasing temperature was observed for all the three Al-Ag alloys after natural aging and for the Al-1 wt. % Ag after artificial aging. This indicates that Ag clusters act as shallow positron trapping centers. The thermal detrapping of positrons becomes ambiguous with increasing Ag content in the alloy and is nearly invisible in the artificially aged Al-5 wt. % Ag and Al-15 wt. % Ag. The positron binding energy of the Ag cluster is roughly estimated to be about 18.8 meV and 50 meV in the Al-1 wt. % Ag sample after natural aging and artificial aging at 140 °C, respectively, which suggests that the confinement of positrons in the quantum-dot like state depends on the size or chemical composition of clusters. Theoretical calculations confirm positron trapping by Ag nanoclusters, and the confinement of positrons is enhanced with increasing Ag cluster size.

Role of a Water Network around the Mn4CaO5 Cluster in Photosynthetic Water Oxidation: A Fourier Transform Infrared Spectroscopy and Quantum Mechanics/Molecular Mechanics Calculation Study.

PubMed

Nakamura, Shin; Ota, Kai; Shibuya, Yuichi; Noguchi, Takumi

2016-01-26

Photosynthetic water oxidation takes place at the Mn4CaO5 cluster in photosystem II. Around the Mn4CaO5 cluster, a hydrogen bond network is formed by several water molecules, including four water ligands. To clarify the role of this water network in the mechanism of water oxidation, we investigated the effects of the removal of Ca(2+) and substitution with metal ions on the vibrations of water molecules coupled to the Mn4CaO5 cluster by means of Fourier transform infrared (FTIR) difference spectroscopy and quantum mechanics/molecular mechanics (QM/MM) calculations. The OH stretching vibrations of nine water molecules forming a network between D1-D61 and YZ were calculated using the QM/MM method. On the the calculated normal modes, a broad positive feature at 3200-2500 cm(-1) in an S2-minus-S1 FTIR spectrum was attributed to the vibrations of strongly hydrogen-bonded OH bonds of water involving the vibrations of water ligands to a Mn ion and the in-phase coupled vibration of a water network connected to YZ, while bands in the 3700-3500 cm(-1) region were assigned to the coupled vibrations of weakly hydrogen-bonded OH bonds of water. All the water bands were lost upon Ca(2+) depletion and Ba(2+) substitution, which inhibit the S2 → S3 transition, indicating that a solid water network was broken by these treatments. By contrast, Sr(2+) substitution slightly altered the water bands around 3600 cm(-1), reflecting minor modification in water interactions, consistent with the retention of water oxidation activity with a decreased efficiency. These results suggest that the water network around the Mn4CaO5 cluster plays an essential role in the water oxidation mechanism particularly in a concerted process of proton transfer and water insertion during the S2 → S3 transition.

Quantum dynamics of small H2 and D2 clusters in the large cage of structure II clathrate hydrate: Energetics, occupancy, and vibrationally averaged cluster structures

NASA Astrophysics Data System (ADS)

Sebastianelli, Francesco; Xu, Minzhong; Bačić, Zlatko

2008-12-01

We report diffusion Monte Carlo (DMC) calculations of the quantum translation-rotation (T-R) dynamics of one to five para-H2 (p-H2) and ortho-D2 (o-D2) molecules inside the large hexakaidecahedral (51264) cage of the structure II clathrate hydrate, which was taken to be rigid. These calculations provide a quantitative description of the size evolution of the ground-state properties, energetics, and the vibrationally averaged geometries, of small (p-H2)n and (o-D2)n clusters, n=1-5, in nanoconfinement. The zero-point energy (ZPE) of the T-R motions rises steeply with the cluster size, reaching 74% of the potential well depth for the caged (p-H2)4. At low temperatures, the rapid increase of the cluster ZPE as a function of n is the main factor that limits the occupancy of the large cage to at most four H2 or D2 molecules, in agreement with experiments. Our DMC results concerning the vibrationally averaged spatial distribution of four D2 molecules, their mean distance from the cage center, the D2-D2 separation, and the specific orientation and localization of the tetrahedral (D2)4 cluster relative to the framework of the large cage, agree very well with the low-temperature neutron diffraction experiments involving the large cage with the quadruple D2 occupancy.

Quantum dynamics of small H2 and D2 clusters in the large cage of structure II clathrate hydrate: energetics, occupancy, and vibrationally averaged cluster structures.

PubMed

Sebastianelli, Francesco; Xu, Minzhong; Bacić, Zlatko

2008-12-28

We report diffusion Monte Carlo (DMC) calculations of the quantum translation-rotation (T-R) dynamics of one to five para-H(2) (p-H(2)) and ortho-D(2) (o-D(2)) molecules inside the large hexakaidecahedral (5(12)6(4)) cage of the structure II clathrate hydrate, which was taken to be rigid. These calculations provide a quantitative description of the size evolution of the ground-state properties, energetics, and the vibrationally averaged geometries, of small (p-H(2))(n) and (o-D(2))(n) clusters, n=1-5, in nanoconfinement. The zero-point energy (ZPE) of the T-R motions rises steeply with the cluster size, reaching 74% of the potential well depth for the caged (p-H(2))(4). At low temperatures, the rapid increase of the cluster ZPE as a function of n is the main factor that limits the occupancy of the large cage to at most four H(2) or D(2) molecules, in agreement with experiments. Our DMC results concerning the vibrationally averaged spatial distribution of four D(2) molecules, their mean distance from the cage center, the D(2)-D(2) separation, and the specific orientation and localization of the tetrahedral (D(2))(4) cluster relative to the framework of the large cage, agree very well with the low-temperature neutron diffraction experiments involving the large cage with the quadruple D(2) occupancy.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lafata, K; Ren, L; Wu, Q

Purpose: To develop a data-mining methodology based on quantum clustering and machine learning to predict expected dosimetric endpoints for lung SBRT applications based on patient-specific anatomic features. Methods: Ninety-three patients who received lung SBRT at our clinic from 2011–2013 were retrospectively identified. Planning information was acquired for each patient, from which various features were extracted using in-house semi-automatic software. Anatomic features included tumor-to-OAR distances, tumor location, total-lung-volume, GTV and ITV. Dosimetric endpoints were adopted from RTOG-0195 recommendations, and consisted of various OAR-specific partial-volume doses and maximum point-doses. First, PCA analysis and unsupervised quantum-clustering was used to explore the feature-space tomore » identify potentially strong classifiers. Secondly, a multi-class logistic regression algorithm was developed and trained to predict dose-volume endpoints based on patient-specific anatomic features. Classes were defined by discretizing the dose-volume data, and the feature-space was zero-mean normalized. Fitting parameters were determined by minimizing a regularized cost function, and optimization was performed via gradient descent. As a pilot study, the model was tested on two esophageal dosimetric planning endpoints (maximum point-dose, dose-to-5cc), and its generalizability was evaluated with leave-one-out cross-validation. Results: Quantum-Clustering demonstrated a strong separation of feature-space at 15Gy across the first-and-second Principle Components of the data when the dosimetric endpoints were retrospectively identified. Maximum point dose prediction to the esophagus demonstrated a cross-validation accuracy of 87%, and the maximum dose to 5cc demonstrated a respective value of 79%. The largest optimized weighting factor was placed on GTV-to-esophagus distance (a factor of 10 greater than the second largest weighting factor), indicating an intuitively strong correlation between this feature and both endpoints. Conclusion: This pilot study shows that it is feasible to predict dose-volume endpoints based on patient-specific anatomic features. The developed methodology can potentially help to identify patients at risk for higher OAR doses, thus improving the efficiency of treatment planning. R01-184173.« less

Hybrid Quantum Mechanics/Molecular Mechanics Solvation Scheme for Computing Free Energies of Reactions at Metal-Water Interfaces.

PubMed

Faheem, Muhammad; Heyden, Andreas

2014-08-12

We report the development of a quantum mechanics/molecular mechanics free energy perturbation (QM/MM-FEP) method for modeling chemical reactions at metal-water interfaces. This novel solvation scheme combines planewave density function theory (DFT), periodic electrostatic embedded cluster method (PEECM) calculations using Gaussian-type orbitals, and classical molecular dynamics (MD) simulations to obtain a free energy description of a complex metal-water system. We derive a potential of mean force (PMF) of the reaction system within the QM/MM framework. A fixed-size, finite ensemble of MM conformations is used to permit precise evaluation of the PMF of QM coordinates and its gradient defined within this ensemble. Local conformations of adsorbed reaction moieties are optimized using sequential MD-sampling and QM-optimization steps. An approximate reaction coordinate is constructed using a number of interpolated states and the free energy difference between adjacent states is calculated using the QM/MM-FEP method. By avoiding on-the-fly QM calculations and by circumventing the challenges associated with statistical averaging during MD sampling, a computational speedup of multiple orders of magnitude is realized. The method is systematically validated against the results of ab initio QM calculations and demonstrated for C-C cleavage in double-dehydrogenated ethylene glycol on a Pt (111) model surface.

Quantum electron tunneling in respiratory complex I.

PubMed

Hayashi, Tomoyuki; Stuchebrukhov, Alexei A

2011-05-12

We have simulated the atomistic details of electronic wiring of all Fe/S clusters in complex I, a key enzyme in the respiratory electron transport chain. The tunneling current theory of many-electron systems is applied to the broken-symmetry (BS) states of the protein at the ZINDO level. While the one-electron tunneling approximation is found to hold in electron tunneling between the antiferromagnetic binuclear and tetranuclear Fe/S clusters without major orbital or spin rearrangement of the core electrons, induced polarization of the core electrons contributes significantly to decrease the electron transfer rates to 19-56 %. Calculated tunneling energy is about 3 eV higher than Fermi level in the band gap of the protein, which supports that the mechanism of electron transfer is quantum mechanical tunneling, as in the rest of the electron transport chain. Resulting electron tunneling pathways consist of up to three key contributing protein residues between neighboring Fe/S clusters. A signature of the wave properties of electrons is observed as distinct quantum interferences when multiple tunneling pathways exist. In N6a-N6b, electron tunnels along different pathways depending on the involved BS states, suggesting possible fluctuations of the tunneling pathways driven by the local protein environment. The calculated distance dependence of the electron transfer rates with internal water molecules included is in good agreement with a reported phenomenological relation.

Magnetic field induced quantum dot brightening in liquid crystal synergized magnetic and semiconducting nanoparticle composite assemblies

DOE PAGES

Amaral, Jose Jussi; Wan, Jacky; Rodarte, Andrea L.; ...

2014-10-22

The design and development of multifunctional composite materials from artificial nano-constituents is one of the most compelling current research areas. This drive to improve over nature and produce ‘meta-materials’ has met with some success, but results have proven limited with regards to both the demonstration of synergistic functionalities and in the ability to manipulate the material properties post-fabrication and in situ. Here, magnetic nanoparticles (MNPs) and semiconducting quantum dots (QDs) are co-assembled in a nematic liquid crystalline (LC) matrix, forming composite structures in which the emission intensity of the quantum dots is systematically and reversibly controlled with a small appliedmore » magnetic field (<100 mT). This magnetic field-driven brightening, ranging between a two- to three-fold peak intensity increase, is a truly cooperative effect: the LC phase transition creates the co-assemblies, the clustering of the MNPs produces LC re-orientation at atypical low external field, and this re-arrangement produces compaction of the clusters, resulting in the detection of increased QD emission. These results demonstrate a synergistic, reversible, and an all-optical process to detect magnetic fields and additionally, as the clusters are self-assembled in a fluid medium, they offer the possibility for these sensors to be used in broad ranging fluid-based applications.« less

Transition mechanism of the reaction interface of the thermal decomposition of calcite

NASA Astrophysics Data System (ADS)

Li, Zhi; Zhao, Zhen; Wang, Qi; Wang, Guocheng

2018-06-01

Even the reaction layer (excited state CaCO3) is so thin that it is difficult to detect, it is significantly restrict the orientation of the solid product (excited state CaO) of the thermal decomposition of calcite. Quantum chemical calculation with GGA-PW91 functional reveals that the ground-state (CaCO3)m clusters are more stable than the hybrid objects (CaCO3)m-(CaO)n clusters. The lowest-energy (CaCO3)m clusters are more kinetically stable than that of (CaCO3)m-n(CaO)n clusters and then than that of (CaO)n clusters except (CaCO3)(CaO)3 clusters from the HOMO-LUMO gaps. (CaCO3)2 clusters should co-exist at room temperature and they prefer to decompose with the temperature increasing.

Quantum chemical analysis of thermodynamics of 2D cluster formation of alkanes at the water/vapor interface in the presence of aliphatic alcohols.

PubMed

Vysotsky, Yu B; Kartashynska, E S; Belyaeva, E A; Fainerman, V B; Vollhardt, D; Miller, R

2015-11-21

Using the quantum chemical semi-empirical PM3 method it is shown that aliphatic alcohols favor the spontaneous clusterization of vaporous alkanes at the water surface due to the change of adsorption from the barrier to non-barrier mechanism. A theoretical model of the non-barrier mechanism for monolayer formation is developed. In the framework of this model alcohols (or any other surfactants) act as 'floats', which interact with alkane molecules of the vapor phase using their hydrophobic part, whereas the hydrophilic part is immersed into the water phase. This results in a significant increase of contact effectiveness of alkanes with the interface during the adsorption and film formation. The obtained results are in good agreement with the existing experimental data. To test the model the thermodynamic and structural parameters of formation and clusterization are calculated for vaporous alkanes C(n)H(2n+2) (n(CH3) = 6-16) at the water surface in the presence of aliphatic alcohols C(n)H(2n+1)OH (n(OH) = 8-16) at 298 K. It is shown that the values of clusterization enthalpy, entropy and Gibbs' energy per one monomer of the cluster depend on the chain lengths of corresponding alcohols and alkanes, the alcohol molar fraction in the monolayers formed, and the shift of the alkane molecules with respect to the alcohol molecules Δn. Two possible competitive structures of mixed 2D film alkane-alcohol are considered: 2D films 1 with single alcohol molecules enclosed by alkane molecules (the alcohols do not form domains) and 2D films 2 that contain alcohol domains enclosed by alkane molecules. The formation of the alkane films of the first type is nearly independent of the surfactant type present at the interface, but depends on their molar fraction in the monolayer formed and the chain length of the compounds participating in the clusterization, whereas for the formation of the films of the second type the interaction between the hydrophilic parts of the surfactant is essential and different for various types of amphiphilic compounds. The energetic preference of the film formation of both types depends significantly on the chain length of compounds. The surfactant concentration (in the range of X = 0-10%) exerts a slight influence on the process of film formation.

Quantum-Size Dependence of the Energy for Vacancy Formation in Charged Small Metal Clusters. Drop Model

NASA Astrophysics Data System (ADS)

Pogosov, V. V.; Reva, V. I.

2018-04-01

Self-consistent computations of the monovacancy formation energy are performed for Na N , Mg N , and Al N (12 < N ≤ 168) spherical clusters in the drop model for stable jelly. Scenarios of the Schottky vacancy formation and "bubble vacancy blowing" are considered. It is shown that the asymptotic behavior of the size dependences of the energy for the vacancy formation by these two mechanisms is different and the difference between the characteristics of a charged and neutral cluster is entirely determined by the difference between the ionization potentials of clusters and the energies of electron attachment to them.

Generalized clustering conditions of Jack polynomials at negative Jack parameter {alpha}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bernevig, B. Andrei; Department of Physics, Princeton University, Princeton, New Jersey 08544; Haldane, F. D. M.

We present several conjectures on the behavior and clustering properties of Jack polynomials at a negative parameter {alpha}=-(k+1/r-1), with partitions that violate the (k,r,N)- admissibility rule of [Feigin et al. [Int. Math. Res. Notices 23, 1223 (2002)]. We find that the ''highest weight'' Jack polynomials of specific partitions represent the minimum degree polynomials in N variables that vanish when s distinct clusters of k+1 particles are formed, where s and k are positive integers. Explicit counting formulas are conjectured. The generalized clustering conditions are useful in a forthcoming description of fractional quantum Hall quasiparticles.

Surface enhanced Raman scattering activity of dual-functional Fe3O4/Au composites

NASA Astrophysics Data System (ADS)

Wang, Li-Ping; Huang, Yu-Bin; Lai, Ying-Huang

2018-03-01

There is a high demand for multifunctional materials that can integrate sample collection and sensing. In this study, magnetic Fe3O4 clusters were fabricated using a simple solvent-thermal method. The effect of the reductant (sodium citrate, SC) on the structure and morphology of Fe3O4 was examined by the variation in the reagent amount. The resulting Fe3O4 clusters were functionalized with 3-aminopropyltriethoxysilane (APTES) to anchor Au nanoparticles to its surface. The fabricated composites were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), and a superconducting quantum interference device (SQUID) magnetometer. Dual-functional Fe3O4/Au clusters were obtained, effectively combining magnetic and plasmonic optical properties. The magnetic Fe3O4 cluster cores permitted the adsorption of the probe molecules, while sample concentration and collection were carried out under an external magnetic field. In addition, 4-nitrothiophenol (4-NTP) was chosen as the probe molecule to examine the analyte concentration ability and surface-enhanced Raman scattering (SERS) activity of the Fe3O4/Au composites. The results indicated that the Fe3O4/Au clusters exhibit a prominent SERS effect. The best 4-NTP detection limit obtained was 1 × 10-8 M, with a corresponding SERS analytical enhancement factor (AEF) exceeding 2 × 105.

Hierarchical Controlled Remote State Preparation by Using a Four-Qubit Cluster State

NASA Astrophysics Data System (ADS)

Ma, Peng-Cheng; Chen, Gui-Bin; Li, Xiao-Wei; Zhan, You-Bang

2018-06-01

We propose a scheme for hierarchical controlled remote preparation of an arbitrary single-qubit state via a four-qubit cluster state as the quantum channel. In this scheme, a sender wishes to help three agents to remotely prepare a quantum state, respectively. The three agents are divided into two grades, that is, an agent is in the upper grade and other two agents are in the lower grade. In this process of remote state preparation, the agent of the upper grade only needs the assistance of any one of the other two agents for recovering the sender's original state, while an agent of the lower grade needs the collaboration of all the other two agents. In other words, the agents of two grades have different authorities to reconstruct sender's original state.

Core Ion Structures and Solvation Effects in Gas Phase [Sn(CO_{2})_{n}]^{-} Clusters

NASA Astrophysics Data System (ADS)

Thompson, Michael C.; Weber, J. Mathias

2017-06-01

We report infrared photodissociation spectra of [Sn(CO_{2})_{n}] (n=2-6) clusters. We explore core ion geometries through quantum chemical calculations and assign our experimental spectra through comparison with calculated vibrational frequencies. We discuss our results in the context of heterogeneous catalytic reduction of CO_{2}, and compare our results with previous work on other post-transition metal species.

Efficient and accurate treatment of electron correlations with correlation matrix renormalization theory

DOE PAGES

Yao, Y. X.; Liu, J.; Liu, C.; ...

2015-08-28

We present an efficient method for calculating the electronic structure and total energy of strongly correlated electron systems. The method extends the traditional Gutzwiller approximation for one-particle operators to the evaluation of the expectation values of two particle operators in the many-electron Hamiltonian. The method is free of adjustable Coulomb parameters, and has no double counting issues in the calculation of total energy, and has the correct atomic limit. We demonstrate that the method describes well the bonding and dissociation behaviors of the hydrogen and nitrogen clusters, as well as the ammonia composed of hydrogen and nitrogen atoms. We alsomore » show that the method can satisfactorily tackle great challenging problems faced by the density functional theory recently discussed in the literature. The computational workload of our method is similar to the Hartree-Fock approach while the results are comparable to high-level quantum chemistry calculations.« less

Many-body optimization using an ab initio monte carlo method.

PubMed

Haubein, Ned C; McMillan, Scott A; Broadbelt, Linda J

2003-01-01

Advances in computing power have made it possible to study solvated molecules using ab initio quantum chemistry. Inclusion of discrete solvent molecules is required to determine geometric information about solute/solvent clusters. Monte Carlo methods are well suited to finding minima in many-body systems, and ab initio methods are applicable to the widest range of systems. A first principles Monte Carlo (FPMC) method was developed to find minima in many-body systems, and emphasis was placed on implementing moves that increase the likelihood of finding minimum energy structures. Partial optimization and molecular interchange moves aid in finding minima and overcome the incomplete sampling that is unavoidable when using ab initio methods. FPMC was validated by studying the boron trifluoride-water system, and then the method was used to examine the methyl carbenium ion in water to demonstrate its application to solvation problems.

Multimode entanglement in reconfigurable graph states using optical frequency combs

PubMed Central

Cai, Y.; Roslund, J.; Ferrini, G.; Arzani, F.; Xu, X.; Fabre, C.; Treps, N.

2017-01-01

Multimode entanglement is an essential resource for quantum information processing and quantum metrology. However, multimode entangled states are generally constructed by targeting a specific graph configuration. This yields to a fixed experimental setup that therefore exhibits reduced versatility and scalability. Here we demonstrate an optical on-demand, reconfigurable multimode entangled state, using an intrinsically multimode quantum resource and a homodyne detection apparatus. Without altering either the initial squeezing source or experimental architecture, we realize the construction of thirteen cluster states of various sizes and connectivities as well as the implementation of a secret sharing protocol. In particular, this system enables the interrogation of quantum correlations and fluctuations for any multimode Gaussian state. This initiates an avenue for implementing on-demand quantum information processing by only adapting the measurement process and not the experimental layout. PMID:28585530

Diffusion doping in quantum dots: bond strength and diffusivity.

PubMed

Saha, Avijit; Makkar, Mahima; Shetty, Amitha; Gahlot, Kushagra; A R, Pavan; Viswanatha, Ranjani

2017-02-23

Semiconducting materials uniformly doped with optical or magnetic impurities have been useful in a number of potential applications. However, clustering or phase separation during synthesis has made this job challenging. Recently the "inside out" diffusion doping was proposed to be successful in obtaining large sized quantum dots (QDs) uniformly doped with a dilute percentage of dopant atoms. Herein, we demonstrate the use of basic physical chemistry of diffusion to control the size and concentration of the dopants within the QDs for a given transition metal ion. We have studied three parameters; the bond strength of the core molecules and the diffusion coefficient of the diffusing metal ion are found to be important while the ease of cation exchange was not highly influential in the control of size and concentration of the single domain dilute magnetic semiconductor quantum dots (DMSQDs) with diverse dopant ions M 2+ (Fe 2+ , Ni 2+ , Co 2+ , Mn 2+ ). Steady state optical emission spectra reveal that the dopants are incorporated inside the semiconducting CdS and the emission can be tuned during shell growth. We have shown that this method enables control over doping percentage and the QDs show a superior ferromagnetic response at room temperature as compared to previously reported systems.

How To Identify Plasmons from the Optical Response of Nanostructures

PubMed Central

2017-01-01

A promising trend in plasmonics involves shrinking the size of plasmon-supporting structures down to a few nanometers, thus enabling control over light–matter interaction at extreme-subwavelength scales. In this limit, quantum mechanical effects, such as nonlocal screening and size quantization, strongly affect the plasmonic response, rendering it substantially different from classical predictions. For very small clusters and molecules, collective plasmonic modes are hard to distinguish from other excitations such as single-electron transitions. Using rigorous quantum mechanical computational techniques for a wide variety of physical systems, we describe how an optical resonance of a nanostructure can be classified as either plasmonic or nonplasmonic. More precisely, we define a universal metric for such classification, the generalized plasmonicity index (GPI), which can be straightforwardly implemented in any computational electronic-structure method or classical electromagnetic approach to discriminate plasmons from single-particle excitations and photonic modes. Using the GPI, we investigate the plasmonicity of optical resonances in a wide range of systems including: the emergence of plasmonic behavior in small jellium spheres as the size and the number of electrons increase; atomic-scale metallic clusters as a function of the number of atoms; and nanostructured graphene as a function of size and doping down to the molecular plasmons in polycyclic aromatic hydrocarbons. Our study provides a rigorous foundation for the further development of ultrasmall nanostructures based on molecular plasmonics. PMID:28651057

Quantum mechanics/molecular mechanics simulation of the ligand vibrations of the water-oxidizing Mn4CaO5 cluster in photosystem II.

PubMed

Nakamura, Shin; Noguchi, Takumi

2016-10-11

During photosynthesis, the light-driven oxidation of water performed by photosystem II (PSII) provides electrons necessary to fix CO 2 , in turn supporting life on Earth by liberating molecular oxygen. Recent high-resolution X-ray images of PSII show that the water-oxidizing center (WOC) is composed of an Mn 4 CaO 5 cluster with six carboxylate, one imidazole, and four water ligands. FTIR difference spectroscopy has shown significant structural changes of the WOC during the S-state cycle of water oxidation, especially within carboxylate groups. However, the roles that these carboxylate groups play in water oxidation as well as how they should be properly assigned in spectra are unresolved. In this study, we performed a normal mode analysis of the WOC using the quantum mechanics/molecular mechanics (QM/MM) method to simulate FTIR difference spectra on the S 1 to S 2 transition in the carboxylate stretching region. By evaluating WOC models with different oxidation and protonation states, we determined that models of high-oxidation states, Mn(III) 2 Mn(IV) 2 , satisfactorily reproduced experimental spectra from intact and Ca-depleted PSII compared with low-oxidation models. It is further suggested that the carboxylate groups bridging Ca and Mn ions within this center tune the reactivity of water ligands bound to Ca by shifting charge via their π conjugation.

First-principles calculations of 17O nuclear magnetic resonance chemical shielding in Pb(Zr(1/2)Ti(1/2))O3 and Pb(Mg(1/3)Nb(2/3))O3: linear dependence on transition-metal/oxygen bond lengths.

PubMed

Pechkis, Daniel L; Walter, Eric J; Krakauer, Henry

2011-09-21

First-principles density functional theory oxygen chemical shift tensors were calculated for A(B,B')O(3) perovskite alloys Pb(Zr(1/2)Ti(1/2))O(3) (PZT) and Pb(Mg(1/3)Nb(2/3))O(3) (PMN). Quantum chemistry methods for embedded clusters and the gauge including projector augmented waves (GIPAW) method [C. J. Pickard and F. Mauri, Phys. Rev. B 63, 245101 (2001)] for periodic boundary conditions were used. Results from both methods are in good agreement for PZT and prototypical perovskites. PMN results were obtained using only GIPAW. Both isotropic δ(iso) and axial δ(ax) chemical shifts were found to vary approximately linearly as a function of the nearest-distance transition-metal/oxygen bond length, r(s). Using these results, we argue against Ti clustering in PZT, as conjectured from recent (17)O NMR magic-angle-spinning measurements. Our findings indicate that (17)O NMR measurements, coupled with first-principles calculations, can be an important probe of local structure in complex perovskite solid solutions.

First-principles calculations of 17O nuclear magnetic resonance chemical shielding in Pb(Zr1/2Ti1/2)O3 and Pb(Mg1/3Nb2/3)O3: Linear dependence on transition-metal/oxygen bond lengths

NASA Astrophysics Data System (ADS)

Pechkis, Daniel L.; Walter, Eric J.; Krakauer, Henry

2011-09-01

First-principles density functional theory oxygen chemical shift tensors were calculated for A(B,B')O3 perovskite alloys Pb(Zr1/2Ti1/2)O3 (PZT) and Pb(Mg1/3Nb2/3)O3 (PMN). Quantum chemistry methods for embedded clusters and the gauge including projector augmented waves (GIPAW) method [C. J. Pickard and F. Mauri, Phys. Rev. B 63, 245101 (2001)], 10.1103/PhysRevB.63.245101 for periodic boundary conditions were used. Results from both methods are in good agreement for PZT and prototypical perovskites. PMN results were obtained using only GIPAW. Both isotropic δiso and axial δax chemical shifts were found to vary approximately linearly as a function of the nearest-distance transition-metal/oxygen bond length, rs. Using these results, we argue against Ti clustering in PZT, as conjectured from recent 17O NMR magic-angle-spinning measurements. Our findings indicate that 17O NMR measurements, coupled with first-principles calculations, can be an important probe of local structure in complex perovskite solid solutions.

Convergence of the Light-Front Coupled-Cluster Method in Scalar Yukawa Theory

NASA Astrophysics Data System (ADS)

Usselman, Austin

We use Fock-state expansions and the Light-Front Coupled-Cluster (LFCC) method to study mass eigenvalue problems in quantum field theory. Specifically, we study convergence of the method in scalar Yukawa theory. In this theory, a single charged particle is surrounded by a cloud of neutral particles. The charged particle can create or annihilate neutral particles, causing the n-particle state to depend on the n + 1 and n - 1-particle state. Fock state expansion leads to an infinite set of coupled equations where truncation is required. The wave functions for the particle states are expanded in a basis of symmetric polynomials and a generalized eigenvalue problem is solved for the mass eigenvalue. The mass eigenvalue problem is solved for multiple values for the coupling strength while the number of particle states and polynomial basis order are increased. Convergence of the mass eigenvalue solutions is then obtained. Three mass ratios between the charged particle and neutral particles were studied. This includes a massive charged particle, equal masses and massive neutral particles. Relative probability between states can also be explored for more detailed understanding of the process of convergence with respect to the number of Fock sectors. The reliance on higher order particle states depended on how large the mass of the charge particle was. The higher the mass of the charged particle, the more the system depended on higher order particle states. The LFCC method solves this same mass eigenvalue problem using an exponential operator. This exponential operator can then be truncated instead to form a finite system of equations that can be solved using a built in system solver provided in most computational environments, such as MatLab and Mathematica. First approximation in the LFCC method allows for only one particle to be created by the new operator and proved to be not powerful enough to match the Fock state expansion. The second order approximation allowed one and two particles to be created by the new operator and converged to the Fock state expansion results. This showed the LFCC method to be a reliable replacement method for solving quantum field theory problems.

Parallel scalability of Hartree-Fock calculations

NASA Astrophysics Data System (ADS)

Chow, Edmond; Liu, Xing; Smelyanskiy, Mikhail; Hammond, Jeff R.

2015-03-01

Quantum chemistry is increasingly performed using large cluster computers consisting of multiple interconnected nodes. For a fixed molecular problem, the efficiency of a calculation usually decreases as more nodes are used, due to the cost of communication between the nodes. This paper empirically investigates the parallel scalability of Hartree-Fock calculations. The construction of the Fock matrix and the density matrix calculation are analyzed separately. For the former, we use a parallelization of Fock matrix construction based on a static partitioning of work followed by a work stealing phase. For the latter, we use density matrix purification from the linear scaling methods literature, but without using sparsity. When using large numbers of nodes for moderately sized problems, density matrix computations are network-bandwidth bound, making purification methods potentially faster than eigendecomposition methods.

Aspects of perturbation theory in quantum mechanics: The BenderWuMATHEMATICA® package

NASA Astrophysics Data System (ADS)

Sulejmanpasic, Tin; Ünsal, Mithat

2018-07-01

We discuss a general setup which allows the study of the perturbation theory of an arbitrary, locally harmonic 1D quantum mechanical potential as well as its multi-variable (many-body) generalization. The latter may form a prototype for regularized quantum field theory. We first generalize the method of Bender-Wu,and derive exact recursion relations which allow the determination of the perturbative wave-function and energy corrections to an arbitrary order, at least in principle. For 1D systems, we implement these equations in an easy to use MATHEMATICA® package we call BenderWu. Our package enables quick home-computer computation of high orders of perturbation theory (about 100 orders in 10-30 s, and 250 orders in 1-2 h) and enables practical study of a large class of problems in Quantum Mechanics. We have two hopes concerning the BenderWu package. One is that due to resurgence, large amount of non-perturbative information, such as non-perturbative energies and wave-functions (e.g. WKB wave functions), can in principle be extracted from the perturbative data. We also hope that the package may be used as a teaching tool, providing an effective bridge between perturbation theory and non-perturbative physics in textbooks. Finally, we show that for the multi-variable case, the recursion relation acquires a geometric character, and has a structure which allows parallelization to computer clusters.

Fault-tolerant quantum computation with nondeterministic entangling gates

NASA Astrophysics Data System (ADS)

Auger, James M.; Anwar, Hussain; Gimeno-Segovia, Mercedes; Stace, Thomas M.; Browne, Dan E.

2018-03-01

Performing entangling gates between physical qubits is necessary for building a large-scale universal quantum computer, but in some physical implementations—for example, those that are based on linear optics or networks of ion traps—entangling gates can only be implemented probabilistically. In this work, we study the fault-tolerant performance of a topological cluster state scheme with local nondeterministic entanglement generation, where failed entangling gates (which correspond to bonds on the lattice representation of the cluster state) lead to a defective three-dimensional lattice with missing bonds. We present two approaches for dealing with missing bonds; the first is a nonadaptive scheme that requires no additional quantum processing, and the second is an adaptive scheme in which qubits can be measured in an alternative basis to effectively remove them from the lattice, hence eliminating their damaging effect and leading to better threshold performance. We find that a fault-tolerance threshold can still be observed with a bond-loss rate of 6.5% for the nonadaptive scheme, and a bond-loss rate as high as 14.5% for the adaptive scheme.

BSA Au clusters as a probe for enhanced fluorescence detection using multipulse excitation scheme.

PubMed

Raut, Sangram L; Rich, Ryan; Fudala, Rafal; Kokate, R; Kimball, J D; Borejdo, Julian; Vishwanatha, Jamboor K; Gryczynski, Zygmunt; Gryczynski, Ignacy

2014-01-01

Although BSA Au clusters fluoresce in red region (λmax: 650 nm), they are of limited use due to low fluorescence quantum yield (~6%). Here we report an enhanced fluorescence imaging application of fluorescent bio-nano probe BSA Au clusters using multipulse excitation scheme. Multipulse excitation takes advantage of long fluorescence lifetime (> 1 µs) of BSA Au clusters and enhances its fluorescence intensity 15 times over short lived cellular auto-fluorescence. Moreover we have also shown that by using time gated detection strategy signal (fluorescence of BSA Au clusters) to noise (auto-fluorescence) ratio can be increased by 30 fold. Thereby with multipulse excitation long lifetime probes can be used to develop biochemical assays and perform optical imaging with zero background.

A Comparison of Quantum and Molecular Mechanical Methods to Estimate Strain Energy in Druglike Fragments.

PubMed

Sellers, Benjamin D; James, Natalie C; Gobbi, Alberto

2017-06-26

Reducing internal strain energy in small molecules is critical for designing potent drugs. Quantum mechanical (QM) and molecular mechanical (MM) methods are often used to estimate these energies. In an effort to determine which methods offer an optimal balance in accuracy and performance, we have carried out torsion scan analyses on 62 fragments. We compared nine QM and four MM methods to reference energies calculated at a higher level of theory: CCSD(T)/CBS single point energies (coupled cluster with single, double, and perturbative triple excitations at the complete basis set limit) calculated on optimized geometries using MP2/6-311+G**. The results show that both the more recent MP2.X perturbation method as well as MP2/CBS perform quite well. In addition, combining a Hartree-Fock geometry optimization with a MP2/CBS single point energy calculation offers a fast and accurate compromise when dispersion is not a key energy component. Among MM methods, the OPLS3 force field accurately reproduces CCSD(T)/CBS torsion energies on more test cases than the MMFF94s or Amber12:EHT force fields, which struggle with aryl-amide and aryl-aryl torsions. Using experimental conformations from the Cambridge Structural Database, we highlight three example structures for which OPLS3 significantly overestimates the strain. The energies and conformations presented should enable scientists to estimate the expected error for the methods described and we hope will spur further research into QM and MM methods.

Quantum mechanical force field for water with explicit electronic polarization.

PubMed

Han, Jaebeom; Mazack, Michael J M; Zhang, Peng; Truhlar, Donald G; Gao, Jiali

2013-08-07

A quantum mechanical force field (QMFF) for water is described. Unlike traditional approaches that use quantum mechanical results and experimental data to parameterize empirical potential energy functions, the present QMFF uses a quantum mechanical framework to represent intramolecular and intermolecular interactions in an entire condensed-phase system. In particular, the internal energy terms used in molecular mechanics are replaced by a quantum mechanical formalism that naturally includes electronic polarization due to intermolecular interactions and its effects on the force constants of the intramolecular force field. As a quantum mechanical force field, both intermolecular interactions and the Hamiltonian describing the individual molecular fragments can be parameterized to strive for accuracy and computational efficiency. In this work, we introduce a polarizable molecular orbital model Hamiltonian for water and for oxygen- and hydrogen-containing compounds, whereas the electrostatic potential responsible for intermolecular interactions in the liquid and in solution is modeled by a three-point charge representation that realistically reproduces the total molecular dipole moment and the local hybridization contributions. The present QMFF for water, which is called the XP3P (explicit polarization with three-point-charge potential) model, is suitable for modeling both gas-phase clusters and liquid water. The paper demonstrates the performance of the XP3P model for water and proton clusters and the properties of the pure liquid from about 900 × 10(6) self-consistent-field calculations on a periodic system consisting of 267 water molecules. The unusual dipole derivative behavior of water, which is incorrectly modeled in molecular mechanics, is naturally reproduced as a result of an electronic structural treatment of chemical bonding by XP3P. We anticipate that the XP3P model will be useful for studying proton transport in solution and solid phases as well as across biological ion channels through membranes.

Understanding the HIV-1 protease reactivity with DFT: what do we gain from recent functionals?

PubMed

Garrec, J; Sautet, P; Fleurat-Lessard, P

2011-07-07

The modeling of HIV-1 plays a crucial role in the understanding of its reactivity and its interactions with specific drugs. In this work, we propose a medium sized model to test the ability of a variety of quantum chemistry approaches to provide reasonable geometric parameters and energetics for this system. Although our model is large enough to include the main polarizing groups of the active site, it is small enough to be used within full quantum studies up to the second order Møller-Plesset (MP2) level with extrapolations to coupled cluster CCSD(T) level. These high level calculations are used as reference to assess the ability of electronic structure methods (semiempirical and DFT) to provide accurate geometries and energies for the HIV-1 protease reaction. All semiempirical methods fail to describe the geometry of the protease active site. Within DFT, pure generalized gradient approximation (GGA) functionals have difficulty in reproducing the reaction energy and underestimate the barrier. Hybrid and/or meta GGA approaches do not yield a consistent improvement. The best results are obtained with hybrid GGA B3LYP or X3LYP and with hybrid meta GGA functionals with a fraction of exact exchange around 30-40%, such as M06, B1B95, or BMK functionals. On the basis of these results, we propose an accurate and computationally efficient strategy, employing quantum chemistry methods. This is applied here to study the protonation state of the reaction intermediate and could be easily used in further QM/MM studies.

In-gap corner states in core-shell polygonal quantum rings.

PubMed

Sitek, Anna; Ţolea, Mugurel; Niţă, Marian; Serra, Llorenç; Gudmundsson, Vidar; Manolescu, Andrei

2017-01-10

We study Coulomb interacting electrons confined in polygonal quantum rings. We focus on the interplay of localization at the polygon corners and Coulomb repulsion. Remarkably, the Coulomb repulsion allows the formation of in-gap states, i.e., corner-localized states of electron pairs or clusters shifted to energies that were forbidden for non-interacting electrons, but below the energies of corner-side-localized states. We specify conditions allowing optical excitation to those states.

In-gap corner states in core-shell polygonal quantum rings

NASA Astrophysics Data System (ADS)

Sitek, Anna; Ţolea, Mugurel; Niţă, Marian; Serra, Llorenç; Gudmundsson, Vidar; Manolescu, Andrei

2017-01-01

We study Coulomb interacting electrons confined in polygonal quantum rings. We focus on the interplay of localization at the polygon corners and Coulomb repulsion. Remarkably, the Coulomb repulsion allows the formation of in-gap states, i.e., corner-localized states of electron pairs or clusters shifted to energies that were forbidden for non-interacting electrons, but below the energies of corner-side-localized states. We specify conditions allowing optical excitation to those states.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gobrecht, David; Cristallo, Sergio; Piersanti, Luciano

Silicon carbide (SiC) grains are a major dust component in carbon-rich asymptotic giant branch stars. However, the formation pathways of these grains are not fully understood. We calculate ground states and energetically low-lying structures of (SiC){sub n}, n = 1, 16 clusters by means of simulated annealing and Monte Carlo simulations of seed structures and subsequent quantum-mechanical calculations on the density functional level of theory. We derive the infrared (IR) spectra of these clusters and compare the IR signatures to observational and laboratory data. According to energetic considerations, we evaluate the viability of SiC cluster growth at several densities andmore » temperatures, characterizing various locations and evolutionary states in circumstellar envelopes. We discover new, energetically low-lying structures for Si{sub 4}C{sub 4}, Si{sub 5}C{sub 5}, Si{sub 15}C{sub 15}, and Si{sub 16}C{sub 16} and new ground states for Si{sub 10}C{sub 10} and Si{sub 15}C{sub 15}. The clusters with carbon-segregated substructures tend to be more stable by 4–9 eV than their bulk-like isomers with alternating Si–C bonds. However, we find ground states with cage geometries resembling buckminsterfullerens (“bucky-like”) for Si{sub 12}C{sub 12} and Si{sub 16}C{sub 16} and low-lying stable cage structures for n ≥ 12. The latter findings thus indicate a regime of cluster sizes that differ from small clusters as well as from large-scale crystals. Thus—and owing to their stability and geometry—the latter clusters may mark a transition from a quantum-confined cluster regime to a crystalline, solid bulk-material. The calculated vibrational IR spectra of the ground-state SiC clusters show significant emission. They include the 10–13 μ m wavelength range and the 11.3 μm feature inferred from laboratory measurements and observations, respectively, although the overall intensities are rather low.« less

Analysis of the Structures and Properties of (GaSb)n (n = 4-9) Clusters through Density Functional Theory.

PubMed

Lu, Qi Liang; Luo, Qi Quan; Huang, Shou Guo; Li, Yi De; Wan, Jian Guo

2016-07-07

An optimization strategy combining global semiempirical quantum mechanical search with all-electron density functional theory was adopted to determine the lowest energy structure of (GaSb)n clusters up to n = 9. The growth pattern of the clusters differed from those of previously reported group III-V binary clusters. A cagelike configuration was found for cluster sizes n ≤ 7. The structure of (GaSb)6 deviated from that of other III-V clusters. Competition existed between core-shell and hollow cage structures of (GaSb)7. Novel noncagelike structures were energetically preferred over the cages for the (GaSb)8 and (GaSb)9 clusters. Electronic properties, such as vertical ionization potential, adiabatic electron affinities, HOMO-LUMO gaps, and average on-site charges on Ga or Sb atoms, as well as binding energies, were computed.

Comparing the accuracy of high-dimensional neural network potentials and the systematic molecular fragmentation method: A benchmark study for all-trans alkanes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gastegger, Michael; Kauffmann, Clemens; Marquetand, Philipp, E-mail: philipp.marquetand@univie.ac.at

Many approaches, which have been developed to express the potential energy of large systems, exploit the locality of the atomic interactions. A prominent example is the fragmentation methods in which the quantum chemical calculations are carried out for overlapping small fragments of a given molecule that are then combined in a second step to yield the system’s total energy. Here we compare the accuracy of the systematic molecular fragmentation approach with the performance of high-dimensional neural network (HDNN) potentials introduced by Behler and Parrinello. HDNN potentials are similar in spirit to the fragmentation approach in that the total energy ismore » constructed as a sum of environment-dependent atomic energies, which are derived indirectly from electronic structure calculations. As a benchmark set, we use all-trans alkanes containing up to eleven carbon atoms at the coupled cluster level of theory. These molecules have been chosen because they allow to extrapolate reliable reference energies for very long chains, enabling an assessment of the energies obtained by both methods for alkanes including up to 10 000 carbon atoms. We find that both methods predict high-quality energies with the HDNN potentials yielding smaller errors with respect to the coupled cluster reference.« less

Atomistic Simulations of High-intensity XFEL Pulses on Diffractive Imaging of Nano-sized System Dynamics

NASA Astrophysics Data System (ADS)

Ho, Phay; Knight, Christopher; Bostedt, Christoph; Young, Linda; Tegze, Miklos; Faigel, Gyula

2016-05-01

We have developed a large-scale atomistic computational method based on a combined Monte Carlo and Molecular Dynamics (MC/MD) method to simulate XFEL-induced radiation damage dynamics of complex materials. The MD algorithm is used to propagate the trajectories of electrons, ions and atoms forward in time and the quantum nature of interactions with an XFEL pulse is accounted for by a MC method to calculate probabilities of electronic transitions. Our code has good scalability with MPI/OpenMP parallelization, and it has been run on Mira, a petascale system at the Argonne Leardership Computing Facility, with particle number >50 million. Using this code, we have examined the impact of high-intensity 8-keV XFEL pulses on the x-ray diffraction patterns of argon clusters. The obtained patterns show strong pulse parameter dependence, providing evidence of significant lattice rearrangement and diffuse scattering. Real-space electronic reconstruction was performed using phase retrieval methods. We found that the structure of the argon cluster can be recovered with atomic resolution even in the presence of considerable radiation damage. This work was supported by the US Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division.

First-principles energetics of water clusters and ice: A many-body analysis

NASA Astrophysics Data System (ADS)

Gillan, M. J.; Alfè, D.; Bartók, A. P.; Csányi, G.

2013-12-01

Standard forms of density-functional theory (DFT) have good predictive power for many materials, but are not yet fully satisfactory for cluster, solid, and liquid forms of water. Recent work has stressed the importance of DFT errors in describing dispersion, but we note that errors in other parts of the energy may also contribute. We obtain information about the nature of DFT errors by using a many-body separation of the total energy into its 1-body, 2-body, and beyond-2-body components to analyze the deficiencies of the popular PBE and BLYP approximations for the energetics of water clusters and ice structures. The errors of these approximations are computed by using accurate benchmark energies from the coupled-cluster technique of molecular quantum chemistry and from quantum Monte Carlo calculations. The systems studied are isomers of the water hexamer cluster, the crystal structures Ih, II, XV, and VIII of ice, and two clusters extracted from ice VIII. For the binding energies of these systems, we use the machine-learning technique of Gaussian Approximation Potentials to correct successively for 1-body and 2-body errors of the DFT approximations. We find that even after correction for these errors, substantial beyond-2-body errors remain. The characteristics of the 2-body and beyond-2-body errors of PBE are completely different from those of BLYP, but the errors of both approximations disfavor the close approach of non-hydrogen-bonded monomers. We note the possible relevance of our findings to the understanding of liquid water.

Entanglement enhancement through multirail noise reduction for continuous-variable measurement-based quantum-information processing

NASA Astrophysics Data System (ADS)

Su, Yung-Chao; Wu, Shin-Tza

2017-09-01

We study theoretically the teleportation of a controlled-phase (cz) gate through measurement-based quantum-information processing for continuous-variable systems. We examine the degree of entanglement in the output modes of the teleported cz-gate for two classes of resource states: the canonical cluster states that are constructed via direct implementations of two-mode squeezing operations and the linear-optical version of cluster states which are built from linear-optical networks of beam splitters and phase shifters. In order to reduce the excess noise arising from finite-squeezed resource states, teleportation through resource states with different multirail designs will be considered and the enhancement of entanglement in the teleported cz gates will be analyzed. For multirail cluster with an arbitrary number of rails, we obtain analytical expressions for the entanglement in the output modes and analyze in detail the results for both classes of resource states. At the same time, we also show that for uniformly squeezed clusters the multirail noise reduction can be optimized when the excess noise is allocated uniformly to the rails. To facilitate the analysis, we develop a trick with manipulations of quadrature operators that can reveal rather efficiently the measurement sequence and corrective operations needed for the measurement-based gate teleportation, which will also be explained in detail.

Quasichemical analysis of the cluster-pair approximation for the thermodynamics of proton hydration

DOE Office of Scientific and Technical Information (OSTI.GOV)

Pollard, Travis; Beck, Thomas L.; Department of Physics, University of Cincinnati, Cincinnati, Ohio 45221

2014-06-14

A theoretical analysis of the cluster-pair approximation (CPA) is presented based on the quasichemical theory of solutions. The sought single-ion hydration free energy of the proton includes an interfacial potential contribution by definition. It is shown, however, that the CPA involves an extra-thermodynamic assumption that does not guarantee uniform convergence to a bulk free energy value with increasing cluster size. A numerical test of the CPA is performed using the classical polarizable AMOEBA force field and supporting quantum chemical calculations. The enthalpy and free energy differences are computed for the kosmotropic Na{sup +}/F{sup −} ion pair in water clusters ofmore » size n = 5, 25, 105. Additional calculations are performed for the chaotropic Rb{sup +}/I{sup −} ion pair. A small shift in the proton hydration free energy and a larger shift in the hydration enthalpy, relative to the CPA values, are predicted based on the n = 105 simulations. The shifts arise from a combination of sequential hydration and interfacial potential effects. The AMOEBA and quantum chemical results suggest an electrochemical surface potential of water in the range −0.4 to −0.5 V. The physical content of single-ion free energies and implications for ion-water force field development are also discussed.« less

Exploiting the spatial locality of electron correlation within the parametric two-electron reduced-density-matrix method

NASA Astrophysics Data System (ADS)

DePrince, A. Eugene; Mazziotti, David A.

2010-01-01

The parametric variational two-electron reduced-density-matrix (2-RDM) method is applied to computing electronic correlation energies of medium-to-large molecular systems by exploiting the spatial locality of electron correlation within the framework of the cluster-in-molecule (CIM) approximation [S. Li et al., J. Comput. Chem. 23, 238 (2002); J. Chem. Phys. 125, 074109 (2006)]. The 2-RDMs of individual molecular fragments within a molecule are determined, and selected portions of these 2-RDMs are recombined to yield an accurate approximation to the correlation energy of the entire molecule. In addition to extending CIM to the parametric 2-RDM method, we (i) suggest a more systematic selection of atomic-orbital domains than that presented in previous CIM studies and (ii) generalize the CIM method for open-shell quantum systems. The resulting method is tested with a series of polyacetylene molecules, water clusters, and diazobenzene derivatives in minimal and nonminimal basis sets. Calculations show that the computational cost of the method scales linearly with system size. We also compute hydrogen-abstraction energies for a series of hydroxyurea derivatives. Abstraction of hydrogen from hydroxyurea is thought to be a key step in its treatment of sickle cell anemia; the design of hydroxyurea derivatives that oxidize more rapidly is one approach to devising more effective treatments.

Enhanced light extraction in tunnel junction-enabled top emitting UV LEDs

DOE PAGES

Zhang, Yuewei; Allerman, Andrew A.; Krishnamoorthy, Sriram; ...

2016-04-11

The efficiency of ultra violet LEDs has been critically limited by the absorption losses in p-type and metal layers. In this work, surface roughening based light extraction structures are combined with tunneling based p-contacts to realize highly efficient top-side light extraction efficiency in UV LEDs. Surface roughening of the top n-type AlGaN contact layer is demonstrated using self-assembled Ni nano-clusters as etch mask. The top surface roughened LEDs were found to enhance external quantum efficiency by over 40% for UV LEDs with a peak emission wavelength of 326 nm. The method described here can enable highly efficient UV LEDs withoutmore » the need for complex manufacturing methods such as flip chip bonding.« less

High-fidelity cluster state generation for ultracold atoms in an optical lattice.

PubMed

Inaba, Kensuke; Tokunaga, Yuuki; Tamaki, Kiyoshi; Igeta, Kazuhiro; Yamashita, Makoto

2014-03-21

We propose a method for generating high-fidelity multipartite spin entanglement of ultracold atoms in an optical lattice in a short operation time with a scalable manner, which is suitable for measurement-based quantum computation. To perform the desired operations based on the perturbative spin-spin interactions, we propose to actively utilize the extra degrees of freedom (DOFs) usually neglected in the perturbative treatment but included in the Hubbard Hamiltonian of atoms, such as, (pseudo-)charge and orbital DOFs. Our method simultaneously achieves high fidelity, short operation time, and scalability by overcoming the following fundamental problem: enhancing the interaction strength for shortening the operation time breaks the perturbative condition of the interaction and inevitably induces unwanted correlations among the spin and extra DOFs.

Fermi liquid, clustering, and structure factor in dilute warm nuclear matter

NASA Astrophysics Data System (ADS)

Röpke, G.; Voskresensky, D. N.; Kryukov, I. A.; Blaschke, D.

2018-02-01

Properties of nuclear systems at subsaturation densities can be obtained from different approaches. We demonstrate the use of the density autocorrelation function which is related to the isothermal compressibility and, after integration, to the equation of state. This way we connect the Landau Fermi liquid theory well elaborated in nuclear physics with the approaches to dilute nuclear matter describing cluster formation. A quantum statistical approach is presented, based on the cluster decomposition of the polarization function. The fundamental quantity to be calculated is the dynamic structure factor. Comparing with the Landau Fermi liquid theory which is reproduced in lowest approximation, the account of bound state formation and continuum correlations gives the correct low-density result as described by the second virial coefficient and by the mass action law (nuclear statistical equilibrium). Going to higher densities, the inclusion of medium effects is more involved compared with other quantum statistical approaches, but the relation to the Landau Fermi liquid theory gives a promising approach to describe not only thermodynamic but also collective excitations and non-equilibrium properties of nuclear systems in a wide region of the phase diagram.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yu, Chongqi; Harbich, Wolfgang; Sementa, Luca

Ligand-protected Au clusters are non-bleaching fluorescence markers in bio- and medical applications. We show that their fluorescence is an intrinsic property of the Au cluster itself. We find a very intense and sharp fluorescence peak located at λ =739.2 nm (1.68 eV) for Au20 clusters in a Ne matrix held at 6 K. The fluorescence reflects the HOMO-LUMO diabatic bandgap of the cluster. The cluster shows a very rich absorption fine structure reminiscent of well defined molecule-like quantum levels. These levels are resolved since Au20 has only one stable isomer (tetrahedral), therefore our sample is mono-disperse in cluster size andmore » conformation. Density-functional theory (DFT) and time-dependent DFT calculations clarify the nature of optical absorptionand predict both main absorption peaks and intrinsic fluorescence in good agreement with experiment.« less

Photonic multipartite entanglement conversion using nonlocal operations

NASA Astrophysics Data System (ADS)

Tashima, T.; Tame, M. S.; Özdemir, Ş. K.; Nori, F.; Koashi, M.; Weinfurter, H.

2016-11-01

We propose a simple setup for the conversion of multipartite entangled states in a quantum network with restricted access. The scheme uses nonlocal operations to enable the preparation of states that are inequivalent under local operations and classical communication, but most importantly does not require full access to the states. It is based on a flexible linear optical conversion gate that uses photons, which are ideally suited for distributed quantum computation and quantum communication in extended networks. In order to show the basic working principles of the gate, we focus on converting a four-qubit entangled cluster state to other locally inequivalent four-qubit states, such as the Greenberger-Horne-Zeilinger and symmetric Dicke states. We also show how the gate can be incorporated into extended graph state networks and can be used to generate variable entanglement and quantum correlations without entanglement but nonvanishing quantum discord.

Hall effect in quantum critical charge-cluster glass

DOE PAGES

Bozovic, Ivan; Wu, Jie; Bollinger, Anthony T.; ...

2016-04-04

Upon doping, cuprates undergo a quantum phase transition from an insulator to a d-wave superconductor. The nature of this transition and of the insulating state is vividly debated. Here, we study the Hall effect in La 2-xSr xCuO 4 (LSCO) samples doped near the quantum critical point at x ≈ 0.06. Dramatic fluctuations in the Hall resistance appear below T CG ≈ 1.5 K and increase as the sample is cooled down further, signaling quantum critical behavior. We explore the doping dependence of this effect in detail, by studying a combinatorial LSCO library in which the Sr content is variedmore » in extremely fine steps, Δx ≈ 0.00008. Furthermore, we observe that quantum charge fluctuations wash out when superconductivity emerges but can be restored when the latter is suppressed by applying a magnetic field, showing that the two instabilities compete for the ground state.« less

Hall effect in quantum critical charge-cluster glass

PubMed Central

Wu, Jie; Bollinger, Anthony T.; Sun, Yujie; Božović, Ivan

2016-01-01

Upon doping, cuprates undergo a quantum phase transition from an insulator to a d-wave superconductor. The nature of this transition and of the insulating state is vividly debated. Here, we study the Hall effect in La2-xSrxCuO4 (LSCO) samples doped near the quantum critical point at x ∼ 0.06. Dramatic fluctuations in the Hall resistance appear below TCG ∼ 1.5 K and increase as the sample is cooled down further, signaling quantum critical behavior. We explore the doping dependence of this effect in detail, by studying a combinatorial LSCO library in which the Sr content is varied in extremely fine steps, Δx ∼ 0.00008. We observe that quantum charge fluctuations wash out when superconductivity emerges but can be restored when the latter is suppressed by applying a magnetic field, showing that the two instabilities compete for the ground state. PMID:27044081

Hall effect in quantum critical charge-cluster glass.

PubMed

Wu, Jie; Bollinger, Anthony T; Sun, Yujie; Božović, Ivan

2016-04-19

Upon doping, cuprates undergo a quantum phase transition from an insulator to a d-wave superconductor. The nature of this transition and of the insulating state is vividly debated. Here, we study the Hall effect in La2-xSrxCuO4(LSCO) samples doped near the quantum critical point atx∼ 0.06. Dramatic fluctuations in the Hall resistance appear belowTCG∼ 1.5 K and increase as the sample is cooled down further, signaling quantum critical behavior. We explore the doping dependence of this effect in detail, by studying a combinatorial LSCO library in which the Sr content is varied in extremely fine steps,Δx∼ 0.00008. We observe that quantum charge fluctuations wash out when superconductivity emerges but can be restored when the latter is suppressed by applying a magnetic field, showing that the two instabilities compete for the ground state.

Quantum trilogy: discrete Toda, Y-system and chaos

NASA Astrophysics Data System (ADS)

Yamazaki, Masahito

2018-02-01

We discuss a discretization of the quantum Toda field theory associated with a semisimple finite-dimensional Lie algebra or a tamely-laced infinite-dimensional Kac-Moody algebra G, generalizing the previous construction of discrete quantum Liouville theory for the case G  =  A 1. The model is defined on a discrete two-dimensional lattice, whose spatial direction is of length L. In addition we also find a ‘discretized extra dimension’ whose width is given by the rank r of G, which decompactifies in the large r limit. For the case of G  =  A N or AN-1(1) , we find a symmetry exchanging L and N under appropriate spatial boundary conditions. The dynamical time evolution rule of the model is quantizations of the so-called Y-system, and the theory can be well described by the quantum cluster algebra. We discuss possible implications for recent discussions of quantum chaos, and comment on the relation with the quantum higher Teichmüller theory of type A N .

Quantum pattern recognition with multi-neuron interactions

NASA Astrophysics Data System (ADS)

Fard, E. Rezaei; Aghayar, K.; Amniat-Talab, M.

2018-03-01

We present a quantum neural network with multi-neuron interactions for pattern recognition tasks by a combination of extended classic Hopfield network and adiabatic quantum computation. This scheme can be used as an associative memory to retrieve partial patterns with any number of unknown bits. Also, we propose a preprocessing approach to classifying the pattern space S to suppress spurious patterns. The results of pattern clustering show that for pattern association, the number of weights (η ) should equal the numbers of unknown bits in the input pattern ( d). It is also remarkable that associative memory function depends on the location of unknown bits apart from the d and load parameter α.

Understanding the many-body expansion for large systems. I. Precision considerations

NASA Astrophysics Data System (ADS)

Richard, Ryan M.; Lao, Ka Un; Herbert, John M.

2014-07-01

Electronic structure methods based on low-order "n-body" expansions are an increasingly popular means to defeat the highly nonlinear scaling of ab initio quantum chemistry calculations, taking advantage of the inherently distributable nature of the numerous subsystem calculations. Here, we examine how the finite precision of these subsystem calculations manifests in applications to large systems, in this case, a sequence of water clusters ranging in size up to (H_2O)_{47}. Using two different computer implementations of the n-body expansion, one fully integrated into a quantum chemistry program and the other written as a separate driver routine for the same program, we examine the reproducibility of total binding energies as a function of cluster size. The combinatorial nature of the n-body expansion amplifies subtle differences between the two implementations, especially for n ⩾ 4, leading to total energies that differ by as much as several kcal/mol between two implementations of what is ostensibly the same method. This behavior can be understood based on a propagation-of-errors analysis applied to a closed-form expression for the n-body expansion, which is derived here for the first time. Discrepancies between the two implementations arise primarily from the Coulomb self-energy correction that is required when electrostatic embedding charges are implemented by means of an external driver program. For reliable results in large systems, our analysis suggests that script- or driver-based implementations should read binary output files from an electronic structure program, in full double precision, or better yet be fully integrated in a way that avoids the need to compute the aforementioned self-energy. Moreover, four-body and higher-order expansions may be too sensitive to numerical thresholds to be of practical use in large systems.

Understanding the many-body expansion for large systems. I. Precision considerations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Richard, Ryan M.; Lao, Ka Un; Herbert, John M., E-mail: herbert@chemistry.ohio-state.edu

2014-07-07

Electronic structure methods based on low-order “n-body” expansions are an increasingly popular means to defeat the highly nonlinear scaling of ab initio quantum chemistry calculations, taking advantage of the inherently distributable nature of the numerous subsystem calculations. Here, we examine how the finite precision of these subsystem calculations manifests in applications to large systems, in this case, a sequence of water clusters ranging in size up to (H{sub 2}O){sub 47}. Using two different computer implementations of the n-body expansion, one fully integrated into a quantum chemistry program and the other written as a separate driver routine for the same program,more » we examine the reproducibility of total binding energies as a function of cluster size. The combinatorial nature of the n-body expansion amplifies subtle differences between the two implementations, especially for n ⩾ 4, leading to total energies that differ by as much as several kcal/mol between two implementations of what is ostensibly the same method. This behavior can be understood based on a propagation-of-errors analysis applied to a closed-form expression for the n-body expansion, which is derived here for the first time. Discrepancies between the two implementations arise primarily from the Coulomb self-energy correction that is required when electrostatic embedding charges are implemented by means of an external driver program. For reliable results in large systems, our analysis suggests that script- or driver-based implementations should read binary output files from an electronic structure program, in full double precision, or better yet be fully integrated in a way that avoids the need to compute the aforementioned self-energy. Moreover, four-body and higher-order expansions may be too sensitive to numerical thresholds to be of practical use in large systems.« less

Computational Thermochemistry of Jet Fuels and Rocket Propellants

NASA Technical Reports Server (NTRS)

Crawford, T. Daniel

2002-01-01

The design of new high-energy density molecules as candidates for jet and rocket fuels is an important goal of modern chemical thermodynamics. The NASA Glenn Research Center is home to a database of thermodynamic data for over 2000 compounds related to this goal, in the form of least-squares fits of heat capacities, enthalpies, and entropies as functions of temperature over the range of 300 - 6000 K. The chemical equilibrium with applications (CEA) program written and maintained by researchers at NASA Glenn over the last fifty years, makes use of this database for modeling the performance of potential rocket propellants. During its long history, the NASA Glenn database has been developed based on experimental results and data published in the scientific literature such as the standard JANAF tables. The recent development of efficient computational techniques based on quantum chemical methods provides an alternative source of information for expansion of such databases. For example, it is now possible to model dissociation or combustion reactions of small molecules to high accuracy using techniques such as coupled cluster theory or density functional theory. Unfortunately, the current applicability of reliable computational models is limited to relatively small molecules containing only around a dozen (non-hydrogen) atoms. We propose to extend the applicability of coupled cluster theory- often referred to as the 'gold standard' of quantum chemical methods- to molecules containing 30-50 non-hydrogen atoms. The centerpiece of this work is the concept of local correlation, in which the description of the electron interactions- known as electron correlation effects- are reduced to only their most important localized components. Such an advance has the potential to greatly expand the current reach of computational thermochemistry and thus to have a significant impact on the theoretical study of jet and rocket propellants.

A quantum mechanical strategy to investigate the structure of liquids: the cases of acetonitrile, formamide, and their mixture.

PubMed

Mennucci, Benedetta; da Silva, Clarissa O

2008-06-05

A computational strategy based on quantum mechanical (QM) calculations and continuum solvation models is used to investigate the structure of liquids (either neat liquids or mixtures). The strategy is based on the comparison of calculated and experimental spectroscopic properties (IR-Raman vibrational frequencies and Raman intensities). In particular, neat formamide, neat acetonitrile, and their equimolar mixture are studied comparing isolated and solvated clusters of different nature and size. In all cases, the study seems to indicate that liquids, even when strongly associated, can be effectively modeled in terms of a shell-like system in which clusters of strongly interacting molecules (the microenvironments) are solvated by a polarizable macroenvironment represented by the rest of the molecules. Only taking into proper account both these effects can a correct picture of the liquid structure be achieved.

Acidity in DMSO from the embedded cluster integral equation quantum solvation model.

PubMed

Heil, Jochen; Tomazic, Daniel; Egbers, Simon; Kast, Stefan M

2014-04-01

The embedded cluster reference interaction site model (EC-RISM) is applied to the prediction of acidity constants of organic molecules in dimethyl sulfoxide (DMSO) solution. EC-RISM is based on a self-consistent treatment of the solute's electronic structure and the solvent's structure by coupling quantum-chemical calculations with three-dimensional (3D) RISM integral equation theory. We compare available DMSO force fields with reference calculations obtained using the polarizable continuum model (PCM). The results are evaluated statistically using two different approaches to eliminating the proton contribution: a linear regression model and an analysis of pK(a) shifts for compound pairs. Suitable levels of theory for the integral equation methodology are benchmarked. The results are further analyzed and illustrated by visualizing solvent site distribution functions and comparing them with an aqueous environment.

Ultracold few fermionic atoms in needle-shaped double wells: spin chains and resonating spin clusters from microscopic Hamiltonians emulated via antiferromagnetic Heisenberg and t-J models

NASA Astrophysics Data System (ADS)

Yannouleas, Constantine; Brandt, Benedikt B.; Landman, Uzi

2016-07-01

Advances with trapped ultracold atoms intensified interest in simulating complex physical phenomena, including quantum magnetism and transitions from itinerant to non-itinerant behavior. Here we show formation of antiferromagnetic ground states of few ultracold fermionic atoms in single and double well (DW) traps, through microscopic Hamiltonian exact diagonalization for two DW arrangements: (i) two linearly oriented one-dimensional, 1D, wells, and (ii) two coupled parallel wells, forming a trap of two-dimensional, 2D, nature. The spectra and spin-resolved conditional probabilities reveal for both cases, under strong repulsion, atomic spatial localization at extemporaneously created sites, forming quantum molecular magnetic structures with non-itinerant character. These findings usher future theoretical and experimental explorations into the highly correlated behavior of ultracold strongly repelling fermionic atoms in higher dimensions, beyond the fermionization physics that is strictly applicable only in the 1D case. The results for four atoms are well described with finite Heisenberg spin-chain and cluster models. The numerical simulations of three fermionic atoms in symmetric DWs reveal the emergent appearance of coupled resonating 2D Heisenberg clusters, whose emulation requires the use of a t-J-like model, akin to that used in investigations of high T c superconductivity. The highly entangled states discovered in the microscopic and model calculations of controllably detuned, asymmetric, DWs suggest three-cold-atom DW quantum computing qubits.

Antiferromagnetic exchange coupling measurements on single Co clusters

NASA Astrophysics Data System (ADS)

Wernsdorfer, W.; Leroy, D.; Portemont, C.; Brenac, A.; Morel, R.; Notin, L.; Mailly, D.

2009-03-01

We report on single-cluster measurements of the angular dependence of the low-temperature ferromagnetic core magnetization switching field in exchange-coupled Co/CoO core-shell clusters (4 nm) using a micro-bridge DC superconducting quantum interference device (μ-SQUID). It is observed that the coupling with the antiferromagnetic shell induces modification in the switching field for clusters with intrinsic uniaxial anisotropy depending on the direction of the magnetic field applied during the cooling. Using a modified Stoner-Wohlfarth model, it is shown that the core interacts with two weakly coupled and asymmetrical antiferromagnetic sublattices. Ref.: C. Portemont, R. Morel, W. Wernsdorfer, D. Mailly, A. Brenac, and L. Notin, Phys. Rev. B 78, 144415 (2008)

Relay entanglement and clusters of correlated spins

NASA Astrophysics Data System (ADS)

Doronin, S. I.; Zenchuk, A. I.

2018-06-01

Considering a spin-1/2 chain, we suppose that the entanglement passes from a given pair of particles to another one, thus establishing the relay transfer of entanglement along the chain. Therefore, we introduce the relay entanglement as a sum of all pairwise entanglements in a spin chain. For more detailed studying the effects of remote pairwise entanglements, we use the partial sums collecting entanglements between the spins separated by up to a certain number of nodes. The problem of entangled cluster formation is considered, and the geometric mean entanglement is introduced as a characteristic of quantum correlations in a cluster. Generally, the lifetime of a cluster decreases with an increase in its size.

Theory of complicated liquids. Investigation of liquids, solvents and solvent effects with modern theoretical methods

NASA Astrophysics Data System (ADS)

Kirchner, Barbara

2007-03-01

It is the aim of this work to elucidate the usefulness and feasibility of the first-principles approach and to extend it to the regime of liquid molecular substances of complex structure. Physical and thermodynamic properties of complicated liquids are investigated by means of Car-Parrinello molecular dynamics (CPMD) and also with static quantum chemical methods. The connection between the dynamic and static approach is given by the quantum cluster equilibrium (QCE) theory. Since the QCE theory is not yet well established, a new implementation in the MD post-processing program P EACEMAKER is presented. It can be shown that it is by far more important to include cooperative effects rather than to concentrate the effort on the inclusion of weak dispersion forces not present in current density functionals. Traditionally, investigations of complicated liquids were also undertaken with the tools of simple liquids, because for some problems the size of the system does not allow for a more accurate description. Although linear-scaling techniques are simplifications from the point of view of quantum chemistry, they might be severe improvements when compared to traditional molecular dynamics simulations. For the interpretation of the liquid state the introduction of local properties is inevitable. New methods are presented for the calculation of local dipole moments and for the estimation of hydrogen bond energies in quantum mechanically nondecomposable systems. The latter also allows for the detection of hydrogen bonds in simulations through a wavefunction-based criterion instead of one which is solely grounded on the geometric structure of the atomic nuclei involved. The article then discusses prominent liquids which show properties that are not yet understood. Another part of the work analyzes the effect of solvent molecules on solutes and their reactions in the solvent. Finaly, neoteric solvents, such as ionic liquids are discussed.

Massively parallel quantum computer simulator

NASA Astrophysics Data System (ADS)

De Raedt, K.; Michielsen, K.; De Raedt, H.; Trieu, B.; Arnold, G.; Richter, M.; Lippert, Th.; Watanabe, H.; Ito, N.

2007-01-01

We describe portable software to simulate universal quantum computers on massive parallel computers. We illustrate the use of the simulation software by running various quantum algorithms on different computer architectures, such as a IBM BlueGene/L, a IBM Regatta p690+, a Hitachi SR11000/J1, a Cray X1E, a SGI Altix 3700 and clusters of PCs running Windows XP. We study the performance of the software by simulating quantum computers containing up to 36 qubits, using up to 4096 processors and up to 1 TB of memory. Our results demonstrate that the simulator exhibits nearly ideal scaling as a function of the number of processors and suggest that the simulation software described in this paper may also serve as benchmark for testing high-end parallel computers.

Barrierless association of CF2 and dissociation of C2F4 by variational transition-state theory and system-specific quantum Rice–Ramsperger–Kassel theory

PubMed Central

Bao, Junwei Lucas; Zhang, Xin

2016-01-01

Bond dissociation is a fundamental chemical reaction, and the first principles modeling of the kinetics of dissociation reactions with a monotonically increasing potential energy along the dissociation coordinate presents a challenge not only for modern electronic structure methods but also for kinetics theory. In this work, we use multifaceted variable-reaction-coordinate variational transition-state theory (VRC-VTST) to compute the high-pressure limit dissociation rate constant of tetrafluoroethylene (C2F4), in which the potential energies are computed by direct dynamics with the M08-HX exchange correlation functional. To treat the pressure dependence of the unimolecular rate constants, we use the recently developed system-specific quantum Rice–Ramsperger–Kassel theory. The calculations are carried out by direct dynamics using an exchange correlation functional validated against calculations that go beyond coupled-cluster theory with single, double, and triple excitations. Our computed dissociation rate constants agree well with the recent experimental measurements. PMID:27834727

Barrierless association of CF2 and dissociation of C2F4 by variational transition-state theory and system-specific quantum Rice-Ramsperger-Kassel theory.

PubMed

Bao, Junwei Lucas; Zhang, Xin; Truhlar, Donald G

2016-11-29

Bond dissociation is a fundamental chemical reaction, and the first principles modeling of the kinetics of dissociation reactions with a monotonically increasing potential energy along the dissociation coordinate presents a challenge not only for modern electronic structure methods but also for kinetics theory. In this work, we use multifaceted variable-reaction-coordinate variational transition-state theory (VRC-VTST) to compute the high-pressure limit dissociation rate constant of tetrafluoroethylene (C 2 F 4 ), in which the potential energies are computed by direct dynamics with the M08-HX exchange correlation functional. To treat the pressure dependence of the unimolecular rate constants, we use the recently developed system-specific quantum Rice-Ramsperger-Kassel theory. The calculations are carried out by direct dynamics using an exchange correlation functional validated against calculations that go beyond coupled-cluster theory with single, double, and triple excitations. Our computed dissociation rate constants agree well with the recent experimental measurements.

In-gap corner states in core-shell polygonal quantum rings

PubMed Central

Sitek, Anna; Ţolea, Mugurel; Niţă, Marian; Serra, Llorenç; Gudmundsson, Vidar; Manolescu, Andrei

2017-01-01

We study Coulomb interacting electrons confined in polygonal quantum rings. We focus on the interplay of localization at the polygon corners and Coulomb repulsion. Remarkably, the Coulomb repulsion allows the formation of in-gap states, i.e., corner-localized states of electron pairs or clusters shifted to energies that were forbidden for non-interacting electrons, but below the energies of corner-side-localized states. We specify conditions allowing optical excitation to those states. PMID:28071750

Optically Generated 2-Dimensional Photonic Cluster State from Coupled Quantum Dots

DTIC Science & Technology

2010-03-12

coupled quantum dots 5a. CONTRACT NUMBER 5b. GRANT NUMBER 5c. PROGRAM ELEMENT NUMBER 6. AUTHOR( S ) 5d. PROJECT NUMBER 5e. TASK NUMBER 5f. WORK UNIT...NUMBER 7. PERFORMING ORGANIZATION NAME( S ) AND ADDRESS(ES) Naval Research Laboratory,,Washington,DC,20375 8. PERFORMING ORGANIZATION REPORT NUMBER...9. SPONSORING/MONITORING AGENCY NAME( S ) AND ADDRESS(ES) 10. SPONSOR/MONITOR’S ACRONYM( S ) 11. SPONSOR/MONITOR’S REPORT NUMBER( S ) 12. DISTRIBUTION

A Molecular–Structure Hypothesis

PubMed Central

Boeyens, Jan C. A.

2010-01-01

The self-similar symmetry that occurs between atomic nuclei, biological growth structures, the solar system, globular clusters and spiral galaxies suggests that a similar pattern should characterize atomic and molecular structures. This possibility is explored in terms of the current molecular structure-hypothesis and its extension into four-dimensional space-time. It is concluded that a quantum molecule only has structure in four dimensions and that classical (Newtonian) structure, which occurs in three dimensions, cannot be simulated by quantum-chemical computation. PMID:21151437

QDENSITY—A Mathematica quantum computer simulation

NASA Astrophysics Data System (ADS)

Juliá-Díaz, Bruno; Burdis, Joseph M.; Tabakin, Frank

2009-03-01

This Mathematica 6.0 package is a simulation of a Quantum Computer. The program provides a modular, instructive approach for generating the basic elements that make up a quantum circuit. The main emphasis is on using the density matrix, although an approach using state vectors is also implemented in the package. The package commands are defined in Qdensity.m which contains the tools needed in quantum circuits, e.g., multiqubit kets, projectors, gates, etc. New version program summaryProgram title: QDENSITY 2.0 Catalogue identifier: ADXH_v2_0 Program summary URL:http://cpc.cs.qub.ac.uk/summaries/ADXH_v2_0.html Program obtainable from: CPC Program Library, Queen's University, Belfast, N. Ireland Licensing provisions: Standard CPC licence, http://cpc.cs.qub.ac.uk/licence/licence.html No. of lines in distributed program, including test data, etc.: 26 055 No. of bytes in distributed program, including test data, etc.: 227 540 Distribution format: tar.gz Programming language: Mathematica 6.0 Operating system: Any which supports Mathematica; tested under Microsoft Windows XP, Macintosh OS X, and Linux FC4 Catalogue identifier of previous version: ADXH_v1_0 Journal reference of previous version: Comput. Phys. Comm. 174 (2006) 914 Classification: 4.15 Does the new version supersede the previous version?: Offers an alternative, more up to date, implementation Nature of problem: Analysis and design of quantum circuits, quantum algorithms and quantum clusters. Solution method: A Mathematica package is provided which contains commands to create and analyze quantum circuits. Several Mathematica notebooks containing relevant examples: Teleportation, Shor's Algorithm and Grover's search are explained in detail. A tutorial, Tutorial.nb is also enclosed. Reasons for new version: The package has been updated to make it fully compatible with Mathematica 6.0 Summary of revisions: The package has been updated to make it fully compatible with Mathematica 6.0 Running time: Most examples included in the package, e.g., the tutorial, Shor's examples, Teleportation examples and Grover's search, run in less than a minute on a Pentium 4 processor (2.6 GHz). The running time for a quantum computation depends crucially on the number of qubits employed.

Facile synthesis of CsPbBr3/PbSe composite clusters

PubMed Central

Nguyen, Thang Phan; Ozturk, Abdullah; Park, Jongee; Sohn, Woonbae; Lee, Tae Hyung; Jang, Ho Won; Kim, Soo Young

2018-01-01

Abstract In this work, CsPbBr3 and PbSe nanocomposites were synthesized to protect perovskite material from self-enlargement during reaction. UV absorption and photoluminescence (PL) spectra indicate that the addition of Se into CsPbBr3 quantum dots modified the electronic structure of CsPbBr3, increasing the band gap from 2.38 to 2.48 eV as the Cs:Se ratio increased to 1:3. Thus, the emission color of CsPbBr3 perovskite quantum dots was modified from green to blue by increasing the Se ratio in composites. According to X-ray diffraction patterns, the structure of CsPbBr3 quantum dots changed from cubic to orthorhombic due to the introduction of PbSe at the surface. Transmission electron microscopy and X-ray photoemission spectroscopy confirmed that the atomic distribution in CsPbBr3/PbSe composite clusters is uniform and the composite materials were well formed. The PL intensity of a CsPbBr3/PbSe sample with a 1:1 Cs:Se ratio maintained 50% of its initial intensity after keeping the sample for 81 h in air, while the PL intensity of CsPbBr3 reduced to 20% of its initial intensity. Therefore, it is considered that low amounts of Se could improve the stability of CsPbBr3 quantum dots. PMID:29296127

Nuclear quantum effects on the structure and the dynamics of [H2O]8 at low temperatures.

PubMed

Videla, Pablo E; Rossky, Peter J; Laria, D

2013-11-07

We use ring-polymer-molecular-dynamics (RPMD) techniques and the semi-empirical q-TIP4P/F water model to investigate the relationship between hydrogen bond connectivity and the characteristics of nuclear position fluctuations, including explicit incorporation of quantum effects, for the energetically low lying isomers of the prototype cluster [H2O]8 at T = 50 K and at 150 K. Our results reveal that tunneling and zero-point energy effects lead to sensible increments in the magnitudes of the fluctuations of intra and intermolecular distances. The degree of proton spatial delocalization is found to map logically with the hydrogen-bond connectivity pattern of the cluster. Dangling hydrogen bonds exhibit the largest extent of spatial delocalization and participate in shorter intramolecular O-H bonds. Combined effects from quantum and polarization fluctuations on the resulting individual dipole moments are also examined. From the dynamical side, we analyze the characteristics of the infrared absorption spectrum. The incorporation of nuclear quantum fluctuations promotes red shifts and sensible broadening relative to the classical profile, bringing the simulation results in much more satisfactory agreement with direct experimental information in the mid and high frequency range of the stretching band. While RPMD predictions overestimate the peak position of the low frequency shoulder, the overall agreement with that reported using an accurate, parameterized, many-body potential is reasonable, and far superior to that one obtains by implementing a partially adiabatic centroid molecular dynamics approach. Quantum effects on the collective dynamics, as reported by instantaneous normal modes, are also discussed.

Complex quantum network geometries: Evolution and phase transitions

NASA Astrophysics Data System (ADS)

Bianconi, Ginestra; Rahmede, Christoph; Wu, Zhihao

2015-08-01

Networks are topological and geometric structures used to describe systems as different as the Internet, the brain, or the quantum structure of space-time. Here we define complex quantum network geometries, describing the underlying structure of growing simplicial 2-complexes, i.e., simplicial complexes formed by triangles. These networks are geometric networks with energies of the links that grow according to a nonequilibrium dynamics. The evolution in time of the geometric networks is a classical evolution describing a given path of a path integral defining the evolution of quantum network states. The quantum network states are characterized by quantum occupation numbers that can be mapped, respectively, to the nodes, links, and triangles incident to each link of the network. We call the geometric networks describing the evolution of quantum network states the quantum geometric networks. The quantum geometric networks have many properties common to complex networks, including small-world property, high clustering coefficient, high modularity, and scale-free degree distribution. Moreover, they can be distinguished between the Fermi-Dirac network and the Bose-Einstein network obeying, respectively, the Fermi-Dirac and Bose-Einstein statistics. We show that these networks can undergo structural phase transitions where the geometrical properties of the networks change drastically. Finally, we comment on the relation between quantum complex network geometries, spin networks, and triangulations.

Complex quantum network geometries: Evolution and phase transitions.

PubMed

Bianconi, Ginestra; Rahmede, Christoph; Wu, Zhihao

2015-08-01

Networks are topological and geometric structures used to describe systems as different as the Internet, the brain, or the quantum structure of space-time. Here we define complex quantum network geometries, describing the underlying structure of growing simplicial 2-complexes, i.e., simplicial complexes formed by triangles. These networks are geometric networks with energies of the links that grow according to a nonequilibrium dynamics. The evolution in time of the geometric networks is a classical evolution describing a given path of a path integral defining the evolution of quantum network states. The quantum network states are characterized by quantum occupation numbers that can be mapped, respectively, to the nodes, links, and triangles incident to each link of the network. We call the geometric networks describing the evolution of quantum network states the quantum geometric networks. The quantum geometric networks have many properties common to complex networks, including small-world property, high clustering coefficient, high modularity, and scale-free degree distribution. Moreover, they can be distinguished between the Fermi-Dirac network and the Bose-Einstein network obeying, respectively, the Fermi-Dirac and Bose-Einstein statistics. We show that these networks can undergo structural phase transitions where the geometrical properties of the networks change drastically. Finally, we comment on the relation between quantum complex network geometries, spin networks, and triangulations.

Anamorphic quasiperiodic universes in modified and Einstein gravity with loop quantum gravity corrections

NASA Astrophysics Data System (ADS)

Amaral, Marcelo M.; Aschheim, Raymond; Bubuianu, Laurenţiu; Irwin, Klee; Vacaru, Sergiu I.; Woolridge, Daniel

2017-09-01

The goal of this work is to elaborate on new geometric methods of constructing exact and parametric quasiperiodic solutions for anamorphic cosmology models in modified gravity theories, MGTs, and general relativity, GR. There exist previously studied generic off-diagonal and diagonalizable cosmological metrics encoding gravitational and matter fields with quasicrystal like structures, QC, and holonomy corrections from loop quantum gravity, LQG. We apply the anholonomic frame deformation method, AFDM, in order to decouple the (modified) gravitational and matter field equations in general form. This allows us to find integral varieties of cosmological solutions determined by generating functions, effective sources, integration functions and constants. The coefficients of metrics and connections for such cosmological configurations depend, in general, on all spacetime coordinates and can be chosen to generate observable (quasi)-periodic/aperiodic/fractal/stochastic/(super) cluster/filament/polymer like (continuous, stochastic, fractal and/or discrete structures) in MGTs and/or GR. In this work, we study new classes of solutions for anamorphic cosmology with LQG holonomy corrections. Such solutions are characterized by nonlinear symmetries of generating functions for generic off-diagonal cosmological metrics and generalized connections, with possible nonholonomic constraints to Levi-Civita configurations and diagonalizable metrics depending only on a time like coordinate. We argue that anamorphic quasiperiodic cosmological models integrate the concept of quantum discrete spacetime, with certain gravitational QC-like vacuum and nonvacuum structures. And, that of a contracting universe that homogenizes, isotropizes and flattens without introducing initial conditions or multiverse problems.

Spectroscopy and Chemistry of Cold Molecules

NASA Astrophysics Data System (ADS)

Momose, Takamasa

2012-06-01

Molecules at low temperatures are expected to behave quite differently from those at high temperatures because pronounced quantum effects emerge from thermal averages. Even at 10 K, a significant enhancement of reaction cross section is expected due to tunneling and resonance effects. Chemistry at this temperature is very important in order to understand chemical reactions in interstellar molecular clouds. At temperatures lower than 1 K, collisions and intermolecular interactions become qualitatively different from those at high temperatures because of the large thermal de Broglie wavelength of molecules. Collisions at these temperatures must be treated as the interference of molecular matter waves, but not as hard sphere collisions. A Bose-Einstein condensate is a significant state of matter as a result of coherent matter wave interaction. Especially, dense para-H_2 molecules are predicted to become a condensate even around 1 K. A convenient method to investigate molecules around 1 K is to dope molecules in cold matrices. Among various matrices, quantum hosts such as solid para-H_2 and superfluid He nano-droplets have been proven to be an excellent host for high-resolution spectroscopy. Rovibrational motion of molecules in these quantum hosts is well quantized on account of the weak interactions and the softness of quantum environment. The linewidths of infrared spectra of molecules in the quantum hosts are extremely narrow compared with those in other matrices. The sharp linewidths allow us to resolve fine spectral structures originated in subtle interactions between guest and host molecules. In this talk, I will describe how the splitting and lineshape of high-resolution spectra of molecules in quantum hosts give us new information on the static and dynamical interactions of molecules in quantum medium. The topics include dynamical response of superfluid environment upon rotational excitation, and possible superfluid phase of para-H_2 clusters. I will also describe our current efforts to make free cold molecules for the study of cold chemistry.

Full-dimensional quantum dynamics of rovibrationally inelastic scattering between CN and H2

NASA Astrophysics Data System (ADS)

Yang, Benhui; Wang, X. H.; Stancil, P. C.; Bowman, J. M.; Balakrishnan, N.; Forrey, R. C.

2016-12-01

We report six-dimensional (6D) potential energy surface (PES) and rovibrational scattering calculations for the CN-H2 collision system. The PES was computed using the high-level ab initio spin-restricted coupled-cluster with single, double, and perturbative triple excitations-F12B method and fitted to an analytic function using an invariant polynomial method in 6D. Quantum close-coupling calculations are reported for rotational transitions in CN by H2 and D2 collisions in 6D as well as four-dimensional (4D) within a rigid rotor model for collision energies of 1.0-1500 cm-1. Comparisons with experimental data and previous 4D calculations are presented for CN rotational levels j1 = 4 and 11. For the first time, rovibrational quenching cross sections and rate coefficients of CN (v1 = 1,j1 = 0) in collisions with para- and ortho-H2 are also reported in full-dimension. Agreement for pure rotational transitions is found to be good, but no experimental data on rovibrational collisional quenching for CN-H2 are available. Applications of the current rotational and rovibrational rate coefficients in astrophysical modeling are briefly discussed.

Transition from one revolving cluster to two revolving clusters in the ground-state rotational bands of nuclei in the lanthanon region.

PubMed

Pauling, L

1991-02-01

Whereas 234(92)U142 and other actinon nuclei have ground-state bands that indicate that each nucleus consists of a sphere and a single revolving cluster with constant composition and with only a steady increase in the moment of inertia with increase in J, the angular-momentum quantum number, many of the lanthanon ground-state bands show discontinuities, usually with an initial slightly or strongly curved segment followed by one or two nearly straight segments. The transition to nearly straight segments is interpreted as a change in structure from one revolving cluster to two revolving clusters. The proton-neutron compositions of the clusters and the central sphere are assigned, leading to values of the radius of revolution. The approximation of the two-cluster sequences to linearity is attributed to the very small values of the quadrupole polarizability of the central sphere. Values of the nucleon numbers of clusters and spheres, of the radius of revolution, and of promotion energy are discussed.

Ab initio investigation of structure, stability, thermal behavior, bonding, and infrared spectra of ionized water cluster (H2O)6+

NASA Astrophysics Data System (ADS)

Liu, Lei; Hu, Cui-E.; Tang, Mei; Chen, Xiang-Rong; Cai, Ling-Cang

2016-10-01

The low-lying isomers of cationic water cluster (H2O)6+ have been globally explored by using particle swarm optimization algorithm in conjunction with quantum chemical calculations. Compared with previous results, our searching method covers a wide range of structural isomers of (H2O)6+ and therefore turns out to be more effective. With these local minima, geometry optimization and vibrational analysis are performed for the most interesting clusters at second-order Møller-Plesset (MP2)/aug-cc-pVDZ level, and their energies are further refined at MP2/aug-cc-pVTZ and coupled-cluster theory with single, double, and perturbative triple excitations/aug-cc-pVDZ level. The interaction energies using the complete basis set limits at MP2 level are also reported. The relationships between their structure arrangement and their energies are discussed. Based on the results of thermal simulation, structural change from a four-numbered ring to a tree-like structure occurs at T ≈ 45 K, and the relative population of six lowest-free-energy isomers is found to exceed 4% at some point within the studied temperature range. Studies reveal that, among these six isomers, two new-found isomers constitute 10% of isomer population at 180 K, and the experimental spectra can be better explained with inclusions of the two isomers. The molecular orbitals for six representative cationic water clusters are also studied. Through topological and reduced density gradient analysis, we investigated the structural characteristics and the bonding strengths of these water cluster radical cations.

Interaction energies for the purine inhibitor roscovitine with cyclin-dependent kinase 2: correlated ab initio quantum-chemical, DFT and empirical calculations.

PubMed

Dobes, Petr; Otyepka, Michal; Strnad, Miroslav; Hobza, Pavel

2006-05-24

The interaction between roscovitine and cyclin-dependent kinase 2 (cdk2) was investigated by performing correlated ab initio quantum-chemical calculations. The whole protein was fragmented into smaller systems consisting of one or a few amino acids, and the interaction energies of these fragments with roscovitine were determined by using the MP2 method with the extended aug-cc-pVDZ basis set. For selected complexes, the complete basis set limit MP2 interaction energies, as well as the coupled-cluster corrections with inclusion of single, double and noninteractive triples contributions [CCSD(T)], were also evaluated. The energies of interaction between roscovitine and small fragments and between roscovitine and substantial sections of protein (722 atoms) were also computed by using density-functional tight-binding methods covering dispersion energy (DFTB-D) and the Cornell empirical potential. Total stabilisation energy originates predominantly from dispersion energy and methods that do not account for the dispersion energy cannot, therefore, be recommended for the study of protein-inhibitor interactions. The Cornell empirical potential describes reasonably well the interaction between roscovitine and protein; therefore, this method can be applied in future thermodynamic calculations. A limited number of amino acid residues contribute significantly to the binding of roscovitine and cdk2, whereas a rather large number of amino acids make a negligible contribution.

Theoretical Study of Sodium Effect on the Gasification of Carbonaceous Materials with Carbon Dioxide.

PubMed

Calderón, Lucas A; Garza, Jorge; Espinal, Juan F

2015-12-24

The effect of sodium on the thermodynamics and kinetics of carbon gasification with carbon dioxide was studied by using quantum chemistry methods. Specifically, in the density functional context, two exchange-correlation functionals were used: B3LYP and M06. Some results obtained by these exchange-correlation functionals were contrasted with those obtained by the CCSD(T) method. It was found that density functional theory gives similar conclusions with respect to the coupled-cluster method. As one important conclusion we can mention that the thermodynamics of carbon monoxide desorption is not favored by the sodium presence. However, the presence of this metal induces: (a) an easier formation of one semiquinone group, (b) the dissociation of carbon dioxide, and (c) an increment on the CO desorption rate for one of the proposed pathways.

Stochastic multi-reference perturbation theory with application to the linearized coupled cluster method

NASA Astrophysics Data System (ADS)

Jeanmairet, Guillaume; Sharma, Sandeep; Alavi, Ali

2017-01-01

In this article we report a stochastic evaluation of the recently proposed multireference linearized coupled cluster theory [S. Sharma and A. Alavi, J. Chem. Phys. 143, 102815 (2015)]. In this method, both the zeroth-order and first-order wavefunctions are sampled stochastically by propagating simultaneously two populations of signed walkers. The sampling of the zeroth-order wavefunction follows a set of stochastic processes identical to the one used in the full configuration interaction quantum Monte Carlo (FCIQMC) method. To sample the first-order wavefunction, the usual FCIQMC algorithm is augmented with a source term that spawns walkers in the sampled first-order wavefunction from the zeroth-order wavefunction. The second-order energy is also computed stochastically but requires no additional overhead outside of the added cost of sampling the first-order wavefunction. This fully stochastic method opens up the possibility of simultaneously treating large active spaces to account for static correlation and recovering the dynamical correlation using perturbation theory. The method is used to study a few benchmark systems including the carbon dimer and aromatic molecules. We have computed the singlet-triplet gaps of benzene and m-xylylene. For m-xylylene, which has proved difficult for standard complete active space self consistent field theory with perturbative correction, we find the singlet-triplet gap to be in good agreement with the experimental values.

New developments in theoretical thermochemistry and electronic structure applications in supramolecular chemistry and cluster science

NASA Astrophysics Data System (ADS)

Ramabhadran, Raghunath Ozhapakkam

In a concise display of the power and diversity of electronic structure theory (EST), the work presented herein involves the development of new computational methods to advance the practical utility of quantum chemistry, as well as solving different types of challenging chemical problems by applying existing EST tools. The research presented is highly interdisciplinary in nature and features synergistic collaborations to solve real-life problems such as regulating toxic chemicals and generating alternative sources of energy. In the first chapter of this dissertation, the solution to a long-standing problem in theoretical thermochemistry is accomplished by the development of the automated, chemically intuitive and generalized thermochemical hierarchy, Connectivity-Based Hierarchy (CBH) to accurately predict the thermochemical properties of organic molecules. The extension of the hierarchy to predict the enthalpies of formations of biomonomers such as amino acids is also presented. The development of a computationally efficient protocol to accurately extrapolate to high CCSD(T) energies based on MP2 and DFT energies using CBH is presented in the second chapter, thus merging theoretical thermochemistry with fragment-based methods in quantum chemistry. This merger drastically reduces the computational cost involved in a CCSD(T) calculation, while retaining the impeccable accuracy it offers. The practical utility of the CH hydrogen bond, commonly thought as being too weak to be used in supramolecular applications has been demonstrated by DFT calculations (along with experimental results from the Flood group) in the third chapter. This is accomplished by systematically studying the binding of monoatomic chloride, diatomic and toxic cyanide and the polyatomic bi-fluoride anions for the first time using only CH hydrogen bonds within a triazolophane macrocycle. The fourth chapter contains the introduction of the concept of fluxionality in the chemical reactions of transition metal oxide clusters. This is useful to develop a systematic paradigm for discussing the mechanisms in the reactions of larger transition metal oxide clusters with small molecules. Additionally, DFT calculations (along with experimental results from the C. C. Jarrold group) are shown to be useful to provide new insights on hydrogen liberation from water, thus aiding in the generation of alternative sources of energy.

Theory of the vortex-clustering transition in a confined two-dimensional quantum fluid

NASA Astrophysics Data System (ADS)

Yu, Xiaoquan; Billam, Thomas P.; Nian, Jun; Reeves, Matthew T.; Bradley, Ashton S.

2016-08-01

Clustering of like-sign vortices in a planar bounded domain is known to occur at negative temperature, a phenomenon that Onsager demonstrated to be a consequence of bounded phase space. In a confined superfluid, quantized vortices can support such an ordered phase, provided they evolve as an almost isolated subsystem containing sufficient energy. A detailed theoretical understanding of the statistical mechanics of such states thus requires a microcanonical approach. Here we develop an analytical theory of the vortex clustering transition in a neutral system of quantum vortices confined to a two-dimensional disk geometry, within the microcanonical ensemble. The choice of ensemble is essential for identifying the correct thermodynamic limit of the system, enabling a rigorous description of clustering in the language of critical phenomena. As the system energy increases above a critical value, the system develops global order via the emergence of a macroscopic dipole structure from the homogeneous phase of vortices, spontaneously breaking the Z2 symmetry associated with invariance under vortex circulation exchange, and the rotational SO (2 ) symmetry due to the disk geometry. The dipole structure emerges characterized by the continuous growth of the macroscopic dipole moment which serves as a global order parameter, resembling a continuous phase transition. The critical temperature of the transition, and the critical exponent associated with the dipole moment, are obtained exactly within mean-field theory. The clustering transition is shown to be distinct from the final state reached at high energy, known as supercondensation. The dipole moment develops via two macroscopic vortex clusters and the cluster locations are found analytically, both near the clustering transition and in the supercondensation limit. The microcanonical theory shows excellent agreement with Monte Carlo simulations, and signatures of the transition are apparent even for a modest system of 100 vortices, accessible in current Bose-Einstein condensate experiments.

Quantum model of a solid-state spin qubit: Ni cluster on a silicon surface by the generalized spin Hamiltonian and X-ray absorption spectroscopy investigations

NASA Astrophysics Data System (ADS)

Farberovich, Oleg V.; Mazalova, Victoria L.; Soldatov, Alexander V.

2015-11-01

We present here the quantum model of a Ni solid-state electron spin qubit on a silicon surface with the use of a density-functional scheme for the calculation of the exchange integrals in the non-collinear spin configurations in the generalized spin Hamiltonian (GSH) with the anisotropic exchange coupling parameters linking the nickel ions with a silicon substrate. In this model the interaction of a spin qubit with substrate is considered in GSH at the calculation of exchange integrals Jij of the nanosystem Ni7-Si in the one-electron approach taking into account chemical bonds of all Si-atoms of a substrate (environment) with atoms of the Ni7-cluster. The energy pattern was found from the effective GSH Hamiltonian acting in the restricted spin space of the Ni ions by the application of the irreducible tensor operators (ITO) technique. In this paper we offer the model of the quantum solid-state N-spin qubit based on the studying of the spin structure and the spin-dynamics simulations of the 3d-metal Ni clusters on the silicon surface. The solution of the problem of the entanglement between spin states in the N-spin systems is becoming more interesting when considering clusters or molecules with a spectral gap in their density of states. For quantifying the distribution of the entanglement between the individual spin eigenvalues (modes) in the spin structure of the N-spin system we use the density of entanglement (DOE). In this study we have developed and used the advanced high-precision numerical techniques to accurately assess the details of the decoherence process governing the dynamics of the N-spin qubits interacting with a silicon surface. We have studied the Rabi oscillations to evaluate the N-spin qubits system as a function of the time and the magnetic field. We have observed the stabilized Rabi oscillations and have stabilized the quantum dynamical qubit state and Rabi driving after a fixed time (0.327 μs). The comparison of the energy pattern with the anisotropic exchange models conventionally used for the analysis of this system and, with the results of the experimental XANES spectra, shows that our complex investigations provide a good description of the pattern of the spin levels and the spin structures of the nanomagnetic Ni7 qubit. The results are discussed in the view of the general problem of the solid-state spin qubits and the spin structure of the Ni cluster.

Higher-order equation-of-motion coupled-cluster methods for ionization processes.

PubMed

Kamiya, Muneaki; Hirata, So

2006-08-21

Compact algebraic equations defining the equation-of-motion coupled-cluster (EOM-CC) methods for ionization potentials (IP-EOM-CC) have been derived and computer implemented by virtue of a symbolic algebra system largely automating these processes. Models with connected cluster excitation operators truncated after double, triple, or quadruple level and with linear ionization operators truncated after two-hole-one-particle (2h1p), three-hole-two-particle (3h2p), or four-hole-three-particle (4h3p) level (abbreviated as IP-EOM-CCSD, CCSDT, and CCSDTQ, respectively) have been realized into parallel algorithms taking advantage of spin, spatial, and permutation symmetries with optimal size dependence of the computational costs. They are based on spin-orbital formalisms and can describe both alpha and beta ionizations from open-shell (doublet, triplet, etc.) reference states into ionized states with various spin magnetic quantum numbers. The application of these methods to Koopmans and satellite ionizations of N2 and CO (with the ambiguity due to finite basis sets eliminated by extrapolation) has shown that IP-EOM-CCSD frequently accounts for orbital relaxation inadequately and displays errors exceeding a couple of eV. However, these errors can be systematically reduced to tenths or even hundredths of an eV by IP-EOM-CCSDT or CCSDTQ. Comparison of spectroscopic parameters of the FH+ and NH+ radicals between IP-EOM-CC and experiments has also underscored the importance of higher-order IP-EOM-CC treatments. For instance, the harmonic frequencies of the A 2Sigma- state of NH+ are predicted to be 1285, 1723, and 1705 cm(-1) by IP-EOM-CCSD, CCSDT, and CCSDTQ, respectively, as compared to the observed value of 1707 cm(-1). The small adiabatic energy separation (observed 0.04 eV) between the X 2Pi and a 4Sigma- states of NH+ also requires IP-EOM-CCSDTQ for a quantitative prediction (0.06 eV) when the a 4Sigma- state has the low-spin magnetic quantum number (s(z) = 1/2). When the state with s(z) = 3/2 is sought, the energy separations converge much more rapidly with the IP-EOM-CCSD value (0.03 eV) already being close to the observed (0.04 eV).

Collective Flows of 16O+16O Collisions with α-Clustering Configurations

NASA Astrophysics Data System (ADS)

Guo, Chen-Chen; He, Wan-Bing; Ma, Yu-Gang

2017-08-01

The main purpose of the present paper is to discuss whether or not the collective flows in heavy-ion collision at Fermi energy can be taken as a tool to investigate the cluster configuration in light nuclei. In practice, within an Extended Quantum Molecular Dynamics model, four $\\alpha$-clustering (linear chain, kite, square, and tetrahedron) configurations of $^{16}$O are employed in the initialization, $^{16}$O+$^{16}$O around Fermi energy (40 - 60 MeV$/$nucleon) with impact parameter 1 - 3 fm are simulated, the directed and elliptic flows are analyzed. It is found that collective flows are influenced by the different $\\alpha$-clustering configurations, and the directed flow of free protons is more sensitive to the initial cluster configuration than the elliptic flow. Nuclear reaction at Fermi energy can be taken a useful way to study cluster configuration in light nuclei.

Condensed Matter Theories - Volume 22

NASA Astrophysics Data System (ADS)

Reinholz, Heidi; Röpke, Gerd; de Llano, Manuel

2007-09-01

pt. A. Fermi liquids. Pressure comparison between the spherical cellular model and the Thomas-Fermi model / G.A. Baker, Jr. Pair excitations and vertex corrections in Fermi fluids and the dynamic structure function of two-dimension 3He / H.M. Böhm, H. Godfrin, E. Krotscheck, H.J. Lauter, M. Meschke and M. Panholzer. Condensation of helium in wedges / E.S. Hernádez ... [et al.]. Non-Fermi liquid behavior from the Fermi-liquid approach / V.A. Khodel ... [et al.]. Theory of third sound and stability of thin 3He-4He superfluid films / E. Krotscheck and M.D. Miller. Pairing in asymmetrical Fermi systems / K.F. Quader and R. Liao. Ground-state properties of small 3He drops from quantum Monte Carlo simulations / E. Sola, J. Casulleras and J. Boronat. Ground-state energy and compressibility of a disordered two-dimensional electron gas / Tanatar ... [et al.]. Quasiexcitons in photoluminescence of incompressible quantum liquids / A. Wójs, A.G ladysiewicz and J.J. Quinn -- pt. B. Bose liquids. Quantum Boltzmann liquids / K.A. Gernoth, M L. Ristig and T. Lindenau. Condensate fraction in the dynamic structure function of Bose fluids / M. Saarela, F. Mazzanti and V. Apaja -- pt. C. Strongly-correlated electronic systems. Electron gas in high-field nanoscopic transport: metallic carbon nanotubes / F. Green and D. Neilson. Evolution and destruction of the Kondo effect in a capacitively coupled double dot system / D.E. Logan and M.R. Galpin. The method of increments-a wavefunction-based Ab-Initio correlation method for solids / B. Paulus. Fractionally charged excitations on frustrated lattices / E. Runge, F. Pollmann and P. Fulde. 5f Electrons in actinides: dual nature and photoemission spectra / G. Zwicknagl -- pt. D. Magnetism. Magnetism in disordered two-dimensional Kondo-Necklace / W. Brenig. On the de Haas-can Alphen oscillation in 2D / S. Fujita and D.L. Morabito. Dynamics in one-dimensional spin systems-density matrix reformalization group study / S. Nishimoto and M. Arikawa. Frustrated quantum antiferromagnets: application of high-order coupled cluster method / J. Richter ... [et al.]. Vorticity and antivorticity in submicron ferromagnetic films / H. Wang, M. Yan and C.E. Campbell -- pt. E. Conductivity. D-wave checkerboard bose condensate of mobile bipolarons / A.S. Alexandrov. Five possible reasons why high-Tc superconductivity is stalled / M. Grether and M. de Llano. Multistability and Multi 2[Pie symbol]-Kinks in the Frenkel-Kontorova model: an application to arrays of Josephson junctions / K.E. Kürten and C. Krattenthaler. Lowering of Boson-Fermion system energy with a gapped cooper resonant-pair dispersion relation / T.A. Mamedov and M. de Llano. The concept of correlated density and its application / K. Morawetz ... [et al.]. Competing local and non-local phase correlations in Fermionic systems with resonant pairing: the Boson-Fermion scenario / J. Ranninger. Superconducting order parameters in the extended Hubbard model: a simple mean-field study / J.S. Thakur and M.P. Das -- pt. F. Nuclear systems. Distribution of maxima of the antisymmetized wave function for the nucleons of a closed-shell and for the nucleons of all closed-shells in a nucleus / G.S. Anagnostatos. Pairing of strongly correlated nucleons / W.H. Dickhoff. Short range correlations in relativistic nuclear models / P.K. Panda, C. Providência and J. da Providência. Quartetting in attractive Fermi-systems and alpha particle condensation in nuclear systems / P. Schuck ... [et al.]. Alpha-alpha and Alpha-nucleus potentials: an energy-density fucntional approach / Z.F. Shehadeh ... [et al.]. -- pt. G. Density functional theory and MD simulations. Dynamics of metal clusters in rare gas clusters / M. Baer ... [et al.]. Reinhard and E. Suraud. Kohn-Sham calculations combined with an average pair-density functional theory / P. Gori-Giorgi and A. Savin. Correlations, collision frequency and optical properties in laser excited clusters / H. Reinholz, T. Raitza and G. Röpke -- pt. H. Biophysics. Condensed matter physics of biomolecule systems in a differential geometric framework / H. Bohr, J.I. Ipsen and S. Markvorsen. The brain's view of the natural world in motion: computing structure from function using directional Fourier transformations / B.K. Dellen, J.W. Clark and R. Wessel -- pt. I. Quantum information. Control and error prevention in condensed matter quantum computing devices / M.S. Byrd and L.A. Wu. Maxent approaches to qubits / C.M. Sarris, A.N. Proto and F B. Malik -- pt. J. New formalisms. Thermal coherent states, a broader class of mixed coherent states, and generalized thermo-field dynamics / R.F. Bishop and A. Vourdas. Ergodic condition and magnetic models / M. Howard Lee. From thermodynamics to Maxent / A. Plastino and E. M.F. Curado. Recent progress in the density-matrix renormalization group / U. Schollwöck.

Quantum many-body theory for electron spin decoherence in nanoscale nuclear spin baths.

PubMed

Yang, Wen; Ma, Wen-Long; Liu, Ren-Bao

2017-01-01

Decoherence of electron spins in nanoscale systems is important to quantum technologies such as quantum information processing and magnetometry. It is also an ideal model problem for studying the crossover between quantum and classical phenomena. At low temperatures or in light-element materials where the spin-orbit coupling is weak, the phonon scattering in nanostructures is less important and the fluctuations of nuclear spins become the dominant decoherence mechanism for electron spins. Since the 1950s, semi-classical noise theories have been developed for understanding electron spin decoherence. In spin-based solid-state quantum technologies, the relevant systems are in the nanometer scale and nuclear spin baths are quantum objects which require a quantum description. Recently, quantum pictures have been established to understand the decoherence and quantum many-body theories have been developed to quantitatively describe this phenomenon. Anomalous quantum effects have been predicted and some have been experimentally confirmed. A systematically truncated cluster-correlation expansion theory has been developed to account for the many-body correlations in nanoscale nuclear spin baths that are built up during electron spin decoherence. The theory has successfully predicted and explained a number of experimental results in a wide range of physical systems. In this review, we will cover this recent progress. The limitations of the present quantum many-body theories and possible directions for future development will also be discussed.

A Framework for Load Balancing of Tensor Contraction Expressions via Dynamic Task Partitioning

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lai, Pai-Wei; Stock, Kevin; Rajbhandari, Samyam

In this paper, we introduce the Dynamic Load-balanced Tensor Contractions (DLTC), a domain-specific library for efficient task parallel execution of tensor contraction expressions, a class of computation encountered in quantum chemistry and physics. Our framework decomposes each contraction into smaller unit of tasks, represented by an abstraction referred to as iterators. We exploit an extra level of parallelism by having tasks across independent contractions executed concurrently through a dynamic load balancing run- time. We demonstrate the improved performance, scalability, and flexibility for the computation of tensor contraction expressions on parallel computers using examples from coupled cluster methods.

Spin and Magnetism: Two Transfer Matrix Formulations of a Classical Heisenberg Ring in a Magnetic Field.

DTIC Science & Technology

1998-06-01

determination of the partition function could be attempted. According to Gatteschi et al, however, [Ref. 15] when commenting on the quantum mechanical...1995 15. Gatteschi , D. et al, "Large Clusters of Metal Ions: The Transition from Molecular to Bulk Magnets" Science vol. 265, pp. 1054-1058, August... Gatteschi , D. et al, "Spin Dynamics in Mesoscopic Size Magnetic Systems... ", Phys. Rev. B, vol. 55, no. 21, 01 June, 1997 18. Tejeda, J. etal, "Quantum

A multi-hop teleportation protocol of arbitrary four-qubit states through intermediate nodes

NASA Astrophysics Data System (ADS)

Choudhury, Binayak S.; Samanta, Soumen

Teleportation processes over long distances become affected by the almost inevitable existence of noise which interferes with the entangled quantum channels. In view of this, intermediate nodes are introduced in the scheme. These nodes are connected in series through quantum entanglement. In this paper, we present a protocol for transferring an entangled four-particle cluster-type state in an integrated manner through the intermediate nodes. Its efficiency and advantage over the corresponding part by part teleportation process is discussed.

Multipartite quantum correlations in the extended J1-J2 Heisenberg model

NASA Astrophysics Data System (ADS)

Batle, J.; Tarawneh, O.; Nagata, Koji; Nakamura, Tadao; Abdalla, S.; Farouk, Ahmed

2017-11-01

Multipartite entanglement and the maximum violation of Bell inequalities are studied in finite clusters of spins in an extended J1-J2 Heisenberg model at zero temperature. The ensuing highly frustrated states will unveil a rich structure for different values of the corresponding spin-spin interaction strengths. The interplay between nearest-neighbors, next-nearest neighbors and further couplings will be explored using multipartite correlations. The model is relevant to certain quantum annealing computation architectures where an all-to-all connectivity is considered.

[{(Mo)Mo5O21(H2O)3(SO4)}12(VO)30(H2O)20]36-: a molecular quantum spin icosidodecahedron.

PubMed

Botar, Bogdan; Kögerler, Paul; Hill, Craig L

2005-07-07

Self-assembly of aqueous solutions of molybdate and vanadate under reducing, mildly acidic conditions results in a polyoxomolybdate-based {Mo72V30} cluster compound Na8K16(VO)(H2O)5[K10 subset{(Mo)Mo5O21(H2O)3(SO4)}12(VO)30(H2O)20].150H2O, 1, a quantum spin-based Keplerate structure.

Fractional charge revealed in computer simulations of resonant tunneling in the fractional quantum Hall regime.

PubMed

Tsiper, E V

2006-08-18

The concept of fractional charge is central to the theory of the fractional quantum Hall effect. Here I use exact diagonalization as well as configuration space renormalization to study finite clusters which are large enough to contain two independent edges. I analyze the conditions of resonant tunneling between the two edges. The "computer experiment" reveals a periodic sequence of resonant tunneling events consistent with the experimentally observed fractional quantization of electric charge in units of e/3 and e/5.

Polarization entangled cluster state generation in a lithium niobate chip

NASA Astrophysics Data System (ADS)

Szep, Attila; Kim, Richard; Shin, Eunsung; Fanto, Michael L.; Osman, Joseph; Alsing, Paul M.

2016-10-01

We present a design of a quantum information processing C-phase (Controlled-phase) gate applicable for generating cluster states that has a form of integrated photonic circuits assembled with cascaded directional couplers on a Ti in-diffused Lithium Niobate (Ti-LN) platform where directional couplers as the integrated optical analogue of bulk beam splitters are used as fundamental building blocks. Based on experimentally optimized fabrication parameters of Ti-LN optical waveguides operating at an 810nm wavelength, an integrated Ti-LN quantum C-phase gate is designed and simulated. Our proposed C-phase gate consists of three tunable directional couplers cascaded together with having different weighted switching ratios for providing a tool of routing vertically- and horizontally-polarized photons independently. Its operation mechanism relies on selectively controlling the optical coupling of orthogonally polarized modes via the change in the index of refraction, and its operation is confirmed by the BPM simulation.

Structural, Chemical and Physical Properties of Mn12

NASA Astrophysics Data System (ADS)

Sessoli, Roberta

1997-03-01

Recent investigations on the physical properties of the first molecular nanomagnet, Mn12ac, will be reported. Among them very high field EPR spectra (up to 25 T) (A. L. Barra, D. Gatteschi, R. Sessoli Phys. Rev. B. submitted) have provided precise information on the spin hamiltonian up to the fourth order terms. These new findings justify the irregularities in the step separations in the quantum hysteresis that we have observed performing the measurements on a single crystal (L. Thomas et al, Nature.383, 145 (1996)), and confirm that we are observing resonant quantum tunneling of the magnetization. The magnetic hysteresis has been also optically detected in collaboration with Prof. A. Thomson of the University of East Anglia, UK. Possible modifications to the Mn12 cluster as well as an iron cluster showing MQT of the magnetization (C. Sangregorio, T. Ohm, C. Paulsen, R. Sessoli, D. Gatteschi, submitted) will be briefly presented.

PEG-phospholipid-encapsulated bismuth sulfide and CdSe/ZnS quantum dot core-shell nanoparticle and its computed tomography/fluorescence performance

NASA Astrophysics Data System (ADS)

Chen, Jun; Yang, Xiao-Quan; Qin, Meng-Yao; Zhang, Xiao-Shuai; Xuan, Yang; Zhao, Yuan-Di

2015-11-01

In this paper, polyethylene glycol-phospholipid structure is used to synthesize hybrid cluster of 40-50 nm diameter that contains hydrophobic bismuth sulfide nanoparticles and CdSe/ZnS quantum dots. The composite probe's toxicity, CT imaging, and fluorescence imaging performance are also studied. Experimental results show that the nanocomposite hybrid cluster has obvious CT contrast enhancement and fluorescence imaging capability in vitro even after cellular uptake. It gives a CT number of 700 (Hounsfield units) at 15 mg/mL, higher than that of the current iobitridol CT contrast agent. 3-(4,5-dimethyl-2-thiazolyl)-2,5-diphenyl-2-H-tetrazolium bromide experiment reveals that it has low cytotoxicity at concentration up to of 3.14 mg/mL of Bi, indicating the composite probe has potential ability for CT and fluorescence bimodal imaging.

Quantum mechanical calculations related to ionization and charge transfer in DNA

NASA Astrophysics Data System (ADS)

Cauët, E.; Valiev, M.; Weare, J. H.; Liévin, J.

2012-07-01

Ionization and charge migration in DNA play crucial roles in mechanisms of DNA damage caused by ionizing radiation, oxidizing agents and photo-irradiation. Therefore, an evaluation of the ionization properties of the DNA bases is central to the full interpretation and understanding of the elementary reactive processes that occur at the molecular level during the initial exposure and afterwards. Ab initio quantum mechanical (QM) methods have been successful in providing highly accurate evaluations of key parameters, such as ionization energies (IE) of DNA bases. Hence, in this study, we performed high-level QM calculations to characterize the molecular energy levels and potential energy surfaces, which shed light on ionization and charge migration between DNA bases. In particular, we examined the IEs of guanine, the most easily oxidized base, isolated and embedded in base clusters, and investigated the mechanism of charge migration over two and three stacked guanines. The IE of guanine in the human telomere sequence has also been evaluated. We report a simple molecular orbital analysis to explain how modifications in the base sequence are expected to change the efficiency of the sequence as a hole trap. Finally, the application of a hybrid approach combining quantum mechanics with molecular mechanics brings an interesting discussion as to how the native aqueous DNA environment affects the IE threshold of nucleobases.

Using experimental data to test an n -body dynamical model coupled with an energy-based clusterization algorithm at low incident energies

NASA Astrophysics Data System (ADS)

Kumar, Rohit; Puri, Rajeev K.

2018-03-01

Employing the quantum molecular dynamics (QMD) approach for nucleus-nucleus collisions, we test the predictive power of the energy-based clusterization algorithm, i.e., the simulating annealing clusterization algorithm (SACA), to describe the experimental data of charge distribution and various event-by-event correlations among fragments. The calculations are constrained into the Fermi-energy domain and/or mildly excited nuclear matter. Our detailed study spans over different system masses, and system-mass asymmetries of colliding partners show the importance of the energy-based clusterization algorithm for understanding multifragmentation. The present calculations are also compared with the other available calculations, which use one-body models, statistical models, and/or hybrid models.

Verifying genuine high-order entanglement.

PubMed

Li, Che-Ming; Chen, Kai; Reingruber, Andreas; Chen, Yueh-Nan; Pan, Jian-Wei

2010-11-19

High-order entanglement embedded in multipartite multilevel quantum systems (qudits) with many degrees of freedom (DOFs) plays an important role in quantum foundation and quantum engineering. Verifying high-order entanglement without the restriction of system complexity is a critical need in any experiments on general entanglement. Here, we introduce a scheme to efficiently detect genuine high-order entanglement, such as states close to genuine qudit Bell, Greenberger-Horne-Zeilinger, and cluster states as well as multilevel multi-DOF hyperentanglement. All of them can be identified with two local measurement settings per DOF regardless of the qudit or DOF number. The proposed verifications together with further utilities such as fidelity estimation could pave the way for experiments by reducing dramatically the measurement overhead.

Origin of matter and space-time in the big bang

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mathews, G. J.; Kajino, T.; Yamazaki, D.

We review the case for and against a bulk cosmic motion resulting from the quantum entanglement of our universe with the multiverse beyond our horizon. Within the current theory for the selection of the initial state of the universe from the landscape multiverse there is a generic prediction that pre-inflation quantum entanglement with other universes should give rise to a cosmic bulk flow with a correlation length of order horizon size and a velocity field relative to the expansion frame of the universe. Indeed, the parameters of this motion are are tightly constrained. A robust prediction can be deduced indicatingmore » that there should be an overall motion of of about 800 km/s relative to the background space time as defined by the cosmic microwave background (CMB). This talk will summarize the underlying theoretical motivation for this hypothesis. Of course our motion relative to the background space time (CMB dipole) has been known for decades and is generally attributed to the gravitational pull of the local super cluster. However, this cosmic peculiar velocity field has been recently deduced out to very large distances well beyond that of the local super cluster by using X-ray galaxy clusters as tracers of matter motion. This is achieved via the kinematic component of the Sunyaev-Zeldovich (KSZ) effect produced by Compton scattering of cosmic microwave background photons from the local hot intracluster gas. As such, this method measures peculiar velocity directly in the frame of the cluster. Similar attempts by our group and others have attempted to independently assess this bulk flow via Type la supernova redshifts. In this talk we will review the observation case for and against the existence of this bulk flow based upon the observations and predictions of the theory. If this interpretation is correct it has profound implications in that we may be observing for the first time both the physics that occurred before the big bang and the existence of the multiverse beyond our horizon.« less

The gravitational-optical methods for examination of the hypothesis about galaxies and antigalaxies in the Universe

NASA Astrophysics Data System (ADS)

Gribov, I. A.; Trigger, S. A.

2018-01-01

The optical-gravitational methods for distinction between photons and antiphotons (galaxies, emitting photons and antigalaxies, emitting antiphotons) in the proposed hypothesis of totally gravitationally neutral (TGN)-Universe are considered. These methods are based on the extension of the earlier proposed the gravitationally neutral Universe concept, including now gravitational neutrality of vacuum. This concept contains (i) enlarged unbroken baryon-like, charge, parity and time and full ±M gr gravitational symmetries between all massive elementary particles-antiparticles, including (ia) ordinary matter (OM)-ordinary antimatter (OAM), (ib) dark matter (DM)-dark antimatter (DAM) and (ii) the resulting gravitational repulsion between equally presented (OM+DM)-galactic and (OAM+DAM)-antigalactic clusters, what spatially isolates and preserves their mutual annihilations in the large-scale TGN-Universe. It is assumed the gravitational balance not only between positive and negative gravitational masses of elementary particles and antiparticles, but also between all massless fields of the quantum field theory (QFT), including the opposite gravitational properties of photons and antiphotons, etc, realizing the totally gravitationally neutral vacuum in the QFT. These photons and antiphotons could be distinguishable optically-gravitationally, if one can observe a massive, deviating OM-star or a deviating (OM+DM)-galaxy from our galactic group, moving fast enough on the heavenly sphere, crossing the line directed to spatially separated far-remote galactic clusters (with the visible OM-markers, emitting photons) or antigalactic cluster (with the visible OAM-markers, emitting antiphotons). The deviations and gravitational microlensing with temporarily increased or decreased brightness of their OM and OAM rays will be opposite, indicating the galaxies and antigalaxies in the Universe.

Computational Studies on the Anharmonic Dynamics of Molecular Clusters

NASA Astrophysics Data System (ADS)

Mancini, John S.

Molecular nanoclusters present ideal systems to probe the physical forces and dynamics that drive the behavior of larger bulk systems. At the nanocluster limit the first instances of several phenomena can be observed including the breaking of hydrogen and molecular bonds. Advancements in experimental and theoretical techniques have made it possible to explore these phenomena in great detail. The most fruitful of these studies have involved the use of both experimental and theoretical techniques to leverage to strengths of the two approaches. This dissertation seeks to explore several important phenomena of molecular clusters using new and existing theoretical methodologies. Three specific systems are considered, hydrogen chloride clusters, mixed water and hydrogen chloride clusters and the first cluster where hydrogen chloride autoionization occurs. The focus of these studies remain as close as possible to experimentally observable phenomena with the intention of validating, simulating and expanding on experimental work. Specifically, the properties of interested are those related to the vibrational ground and excited state dynamics of these systems. Studies are performed using full and reduced dimensional potential energy surface alongside advanced quantum mechanical methods including diffusion Monte Carlo, vibrational configuration interaction theory and quasi-classical molecular dynamics. The insight gained from these studies are great and varied. A new on-they-fly ab initio method for studying molecular clusters is validated for (HCl)1--6. A landmark study of the dissociation energy and predissociation mechanism of (HCl)3 is reported. The ground states of mixed (HCl)n(H2O)m are found to be highly delocalized across multiple stationary point configurations. Furthermore, it is identified that the consideration of this delocalization is required in vibrational excited state calculations to achieve agreement with experimental measurements. Finally, the theoretical infrared spectra for the first case of HCl ionization in (H 2O)m is reported, H+(H2O) 3Cl--. The calculation indicates that the ionized cluster's spectra is much more complex than any pervious harmonic predictions, with a large number of the system's infrared active peaks resulting from overtones of lower frequency molecular motions.

Molecular Dynamics Simulations of the [2Fe-2S] Cluster-Binding Domain of NEET Proteins Reveal Key Molecular Determinants That Induce Their Cluster Transfer/Release.

PubMed

Pesce, Luca; Calandrini, Vania; Marjault, Henri-Baptiste; Lipper, Colin H; Rossetti, Gulia; Mittler, Ron; Jennings, Patricia A; Bauer, Andreas; Nechushtai, Rachel; Carloni, Paolo

2017-11-30

The NEET proteins are a novel family of iron-sulfur proteins characterized by an unusual three cysteine and one histidine coordinated [2Fe-2S] cluster. Aberrant cluster release, facilitated by the breakage of the Fe-N bond, is implicated in a variety of human diseases, including cancer. Here, the molecular dynamics in the multi-microsecond timescale, along with quantum chemical calculations, on two representative members of the family (the human NAF-1 and mitoNEET proteins), show that the loss of the cluster is associated with a dramatic decrease in secondary and tertiary structure. In addition, the calculations provide a mechanism for cluster release and clarify, for the first time, crucial differences existing between the two proteins, which are reflected in the experimentally observed difference in the pH-dependent cluster reactivity. The reliability of our conclusions is established by an extensive comparison with the NMR data of the solution proteins, in part measured in this work.

From bismuth oxide/hydroxide precursor clusters towards stable oxides: Proton transfer reactions and structural reorganization govern the stability of [Bi18O13(OH)10]-nitrate clusters

NASA Astrophysics Data System (ADS)

Walther, M.; Zahn, D.

2018-01-01

Structural relaxation and stability of a Bi18-cluster as obtained from association of [Bi6O4(OH)4](NO3)6 precursor clusters in DMSO solution is investigated from a combination of quantum chemical calculations and μs-scale molecular dynamics simulations using empirical interaction potentials. The Bi18-cluster undergoes a OH⋯OH proton transfer reaction, followed by considerable structural relaxation. While the aggregation of the Bi18-cluster is induced by the dissociation of a single nitrate ion leading to [Bi6O4(OH)4](NO3)5+ as an activated precursor species that can bind two more Bi6-clusters, we find the [Bi18O13(OH)10](NO3)18-x+x species (explored for x = 1-6) rather inert against either nitrate dissociation, collision with Bi6-precursors or combinations thereof.

Primordial Particles; Collisions of Inelastic Particles

NASA Astrophysics Data System (ADS)

Sagi, George

2011-03-01

Three-dimensional matter is not defined by Euclidian or Cartesian geometries. Newton's and Einstein's laws are related to the motions of elastic masses. The study of collisions of inelastic particles opens up new vistas in physics. The present article reveals how such particles create clusters composed of various numbers of particles. The Probability of each formation, duplets, triplets, etc. can be calculated. The particles are held together by a binding force, and depending upon the angles of collisions they may also rotate around their center of geometry. Because of these unique properties such inelastic particles are referred to as primordial particles, Pp. When a given density of Pp per cubic space is given, then random collisions create a field. The calculation of the properties of such primordial field is very complex and beyond the present study. However, the angles of collisions are infinite in principle, but the probabilities of various cluster sizes are quantum dependent. Consequently, field calculations will require new complex mathematical methods to be discovered yet.

Water-chromophore electron transfer determines the photochemistry of cytosine and cytidine.

PubMed

Szabla, Rafał; Kruse, Holger; Šponer, Jiří; Góra, Robert W

2017-07-21

Many of the UV-induced phenomena observed experimentally for aqueous cytidine were lacking the mechanistic interpretation for decades. These processes include the substantial population of the puzzling long-lived dark state, photohydration, cytidine to uridine conversion and oxazolidinone formation. Here, we present quantum-chemical simulations of excited-state spectra and potential energy surfaces of N1-methylcytosine clustered with two water molecules using the second-order approximate coupled cluster (CC2), complete active space with second-order perturbation theory (CASPT2), and multireference configuration interaction with single and double excitation (MR-CISD) methods. We argue that the assignment of the long-lived dark state to a singlet nπ* excitation involving water-chromophore electron transfer might serve as an explanation for the numerous experimental observations. While our simulated spectra for the state are in excellent agreement with experimentally acquired data, the electron-driven proton transfer process occurring on the surface may initiate the subsequent damage in the vibrationally hot ground state of the chromophore.

NMR study of spin dynamics in mesoscopic molecular clusters

NASA Astrophysics Data System (ADS)

Borsa, Ferdinando

1998-03-01

Recent published and umpublished work regarding the magnetic properties and the spin dynamics of molecules containing rings of 6,8 and 10 spins and of molecules containing clusters of 8 and 12 spins are reviewed. The 1H nuclear spin-lattice relaxation rate (NSLR) and the Muon Spin Resonance relaxation in Mn12 (A.Lascialfari, D.Gatteschi, F.Borsa, A.Shastri, Z.H.Jang and P.Carretta, Phys.Rev. B 1 January 1998) and Fe8 clusters are presented and discussed with regards to the high temperature spin dynamics of the Mn (Fe) magnetic moments and with regards to the low temperature superparamagnetic behavior. 1H and 63Cu NMR results are presented for two "quantum" spin rings : Cu6 and Cu8. The Cu6 is a weakly coupled (J/k=60K) ferromagnetic S=1/2 spin ring while Cu8 is a strongly coupled (J/k greater than 400K) antiferromagnetic S=1/2 spin ring.The dependence of the NSRL from temperature and from applied magnetic field are analyzed in terms of the calculated magnetic energy levels of the magnetic ring. The values of the energy gap between the ground state and the first excited state are extracted from the exponential decrease of the NSLR as the temperature is lowered. The results in the Cu ( S=1/2) "quantum" rings are compared with the results in "quantum" chains and ladders and with the results in "classical" Fe (S=5/2) antiferromagnetic rings : Fe6 and Fe10 (A.Lascialfari, D.Gatteschi, F.Borsa and A.Cornia , Phys.Rev. 55B,14341,1997) ).

[Effects of different rootstocks on the weak light tolerance ability of summer black grape based on 4 photo-response models].

PubMed

Han, Xiao; Wang, Hai Bo; Wang, Xiao di; Shi, Xiang Bin; Wang, Bao Liang; Zheng, Xiao Cui; Wang, Zhi Qiang; Liu, Feng Zhi

2017-10-01

The photo response curves of 11 rootstock-scion combinations including summer black/Beta, summer black/1103P, summer black/101-14, summer black/3309C, summer black/140Ru, summer black/5C, summer black/5BB, summer black/420A, summer black/SO4, summer black/Kangzhen No.1, summer black/Huapu No.1 were fitted by rectangular hyperbola mo-del, non-rectangular hyperbola model, modified rectangular hyperbola model and exponential model respectively, and the differences of imitative effects were analyzed by determination coefficiency, light compensation point, light saturation point, initial quantum efficiency, maximum photosynthetic rate and dark respiration rate. The result showed that the fit coefficients of all four models were above 0.98, and there was no obvious difference on the fitted values of light compensation point among the four models. The modified rectangular hyperbola model fitted best on light saturation point, apparent quantum yield, maximum photosynthetic rate and dark respiration rate, and had the minimum AIC value based on the akaike information criterion, therefore, the modified rectangular hyperbola model was the best one. The clustering analysis indicated that summer black/SO4 and summer black/420A combinations had low light compensation point, high apparent quantum yield and low dark respiration rate among 11 rootstock-scion combinations, suggesting that these two combinations could use weak light more efficiently due to their less respiratory consumption and higher weak light tolerance. The Topsis comparison method ranked summer black/SO4 and summer black/420A combinations as No. 1 and No. 2 respectively in weak light tolerance ability, which was consistent with cluster analysis. Consequently, summer black has the highest weak light tolerance in case grafted on 420A or SO4, which could be the most suitable rootstock-scion combinations for protected cultivation.

Atomically precise arrays of fluorescent silver clusters: a modular approach for metal cluster photonics on DNA nanostructures.

PubMed

Copp, Stacy M; Schultz, Danielle E; Swasey, Steven; Gwinn, Elisabeth G

2015-03-24

The remarkable precision that DNA scaffolds provide for arraying nanoscale optical elements enables optical phenomena that arise from interactions of metal nanoparticles, dye molecules, and quantum dots placed at nanoscale separations. However, control of ensemble optical properties has been limited by the difficulty of achieving uniform particle sizes and shapes. Ligand-stabilized metal clusters offer a route to atomically precise arrays that combine desirable attributes of both metals and molecules. Exploiting the unique advantages of the cluster regime requires techniques to realize controlled nanoscale placement of select cluster structures. Here we show that atomically monodisperse arrays of fluorescent, DNA-stabilized silver clusters can be realized on a prototypical scaffold, a DNA nanotube, with attachment sites separated by <10 nm. Cluster attachment is mediated by designed DNA linkers that enable isolation of specific clusters prior to assembly on nanotubes and preserve cluster structure and spectral purity after assembly. The modularity of this approach generalizes to silver clusters of diverse sizes and DNA scaffolds of many types. Thus, these silver cluster nano-optical elements, which themselves have colors selected by their particular DNA templating oligomer, bring unique dimensions of control and flexibility to the rapidly expanding field of nano-optics.

Thermodynamics of Small Alkali Metal Halide Cluster Ions: Comparison of Classical Molecular Simulations with Experiment and Quantum Chemistry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vlcek, Lukas; Uhlik, Filip; Moucka, Filip

We evaluate the ability of selected classical molecular models to describe the thermodynamic and structural aspects of gas-phase hydration of alkali halide ions and the formation of small water clusters. To understand the effect of many-body interactions (polarization) and charge penetration effects on the accuracy of a force field, we perform Monte Carlo simulations with three rigid water models using different functional forms to account for these effects: (i) point charge non-polarizable SPC/E, (ii) Drude point charge polarizable SWM4- DP, and (iii) Drude Gaussian charge polarizable BK3. Model predictions are compared with experimental Gibbs free energies and enthalpies of ionmore » hydration, and with microscopic structural properties obtained from quantum DFT calculations. We find that all three models provide comparable predictions for pure water clusters and cation hydration, but differ significantly in their description of anion hydration. None of the investigated classical force fields can consistently and quantitatively reproduce the experimental gas phase hydration thermodynamics. The outcome of this study highlights the relation between the functional form that describes the effective intermolecular interactions and the accuracy of the resulting ion hydration properties.« less

High-resolution electron spectroscopy of lanthanide (Ce, Pr, and Nd) complexes of cyclooctatetraene: the role of 4f electrons.

PubMed

Kumari, Sudesh; Roudjane, Mourad; Hewage, Dilrukshi; Liu, Yang; Yang, Dong-Sheng

2013-04-28

Cerium, praseodymium, and neodymium complexes of 1,3,5,7-cyclooctatetraene (COT) complexes were produced in a laser-vaporization metal cluster source and studied by pulsed-field ionization zero electron kinetic energy spectroscopy and quantum chemical calculations. The computations included the second-order Møller-Plesset perturbation theory, the coupled cluster method with single, double, and perturbative triple excitations, and the state-average complete active space self-consistent field method. The spectrum of each complex exhibits multiple band systems and is assigned to ionization of several low-energy electronic states of the neutral complex. This observation is different from previous studies of M(COT) (M = Sc, Y, La, and Gd), for which a single band system was observed. The presence of the multiple low-energy electronic states is caused by the splitting of the partially filled lanthanide 4f orbitals in the ligand field, and the number of the low-energy states increases rapidly with increasing number of the metal 4f electrons. On the other hand, the 4f electrons have a small effect on the geometries and vibrational frequencies of these lanthanide complexes.

Vindication of Yb2Ti2O7 as a model exchange quantum spin ice.

PubMed

Applegate, R; Hayre, N R; Singh, R R P; Lin, T; Day, A G R; Gingras, M J P

2012-08-31

We use numerical linked-cluster expansions to compute the specific heat C(T) and entropy S(T) of a quantum spin ice Hamiltonian for Yb2Ti2O7 using anisotropic exchange interactions, recently determined from inelastic neutron scattering measurements, and find good agreement with experimental calorimetric data. This vindicates Yb2Ti2O7 as a model quantum spin ice. We find that in the perturbative weak quantum regime, such a system has a ferrimagnetic ordered ground state, with two peaks in C(T): a Schottky anomaly signaling the paramagnetic to spin ice crossover, followed at a lower temperature by a sharp peak accompanying a first-order phase transition to the ordered state. We suggest that the two C(T) features observed in Yb2Ti2O7 are associated with the same physics. Spin excitations in this regime consist of weakly confined spinon-antispinon pairs. We anticipate that the conventional ground state with exotic quantum dynamics will prove a prevalent characteristic of many real quantum spin ice materials.

Interaction of scandium and titanium atoms with a carbon surface containing five- and seven-membered rings

DOE Office of Scientific and Technical Information (OSTI.GOV)

Krasnov, P. O., E-mail: kpo1980@gmail.com; Eliseeva, N. S.; Kuzubov, A. A., E-mail: alex_xx@rambler.ru

2012-01-15

The use of carbon nanotubes coated by atoms of transition metals to store molecular hydrogen is associated with the problem of the aggregation of these atoms, which leads to the formation of metal clusters. The quantum-chemical simulation of cluster models of the carbon surface of a graphene type with scandium and titanium atoms has been performed. It has been shown that the presence of five- and seven-membered rings, in addition to six-membered rings, in these structures makes it possible to strongly suppress the processes of the migration of metal atoms over the surface, preventing their clustering.

Albumin-stabilized fluorescent silver nanodots

NASA Astrophysics Data System (ADS)

Sych, Tomash; Polyanichko, Alexander; Kononov, Alexei

2017-07-01

Ligand-stabilized Ag nanoclusters (NCs) possess many attractive features including high fluorescence quantum yield, large absorption cross-section, good photostability, large Stokes shift and two-photon absorption cross sections. While plenty of fluorescent clusters have been synthesized on various polymer templates, only a few studies have been reported on the fluorescent Ag clusters on peptides and proteins. We study silver NCs synthesized on different protein matrices, including bovine serum albumin, human serum albumin, egg albumin, equine serum albumin, and lysozyme. Our results show that red-emitting Ag NCs can effectively be stabilized by the disulfide bonds in proteins and that the looser structure of the denatured protein favors formation of the clusters.

Correlated signals of cluster superfluorescence under two-and three-photon excitation of CdSe/CdS nanostructures

NASA Astrophysics Data System (ADS)

Samartsev, Vitaly; Mitrofanova, Tatiana

2017-10-01

The possibility and conditions for generation of the correlated signals of cluster superfluorescence (CSF) under two and three-quantum excitation of nanostructured samples CdSe/CdS by two crossed at the angle of 60° femtosecond beams of the Ti:Sapphire laser radiation are investigated. It is shown that intensity of the CSF signals is proportional to the cube of the number of clusters and that these collective signals are generated in mutually opposite directions k1 - k2 and k2 - k1, where k1, k2 are the wavevectors of the exciting pulses.

Ge14 Br8 (PEt3 )4 : A Subhalide Cluster of Germanium.

PubMed

Kunz, Tanja; Schrenk, Claudio; Schnepf, Andreas

2018-04-03

Heating a metastable solution of Ge I Br to room temperature led to the first structurally characterized metalloid subhalide cluster Ge 14 Br 8 (PEt 3 ) 4 (1). Furthermore 1 can be seen as the first isolated binary halide cluster on the way from Ge I Br to elemental germanium, giving insight into the complex reaction mechanism of its disproportionation reaction. Quantum chemical calculations further indicate that a classical bonding situation is realized within 1 and that the last step of the formation of 1 might include the trapping of GeBr 2 units. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Coherent exciton transport in dendrimers and continuous-time quantum walks

NASA Astrophysics Data System (ADS)

Mülken, Oliver; Bierbaum, Veronika; Blumen, Alexander

2006-03-01

We model coherent exciton transport in dendrimers by continuous-time quantum walks. For dendrimers up to the second generation the coherent transport shows perfect recurrences when the initial excitation starts at the central node. For larger dendrimers, the recurrence ceases to be perfect, a fact which resembles results for discrete quantum carpets. Moreover, depending on the initial excitation site, we find that the coherent transport to certain nodes of the dendrimer has a very low probability. When the initial excitation starts from the central node, the problem can be mapped onto a line which simplifies the computational effort. Furthermore, the long time average of the quantum mechanical transition probabilities between pairs of nodes shows characteristic patterns and allows us to classify the nodes into clusters with identical limiting probabilities. For the (space) average of the quantum mechanical probability to be still or to be again at the initial site, we obtain, based on the Cauchy-Schwarz inequality, a simple lower bound which depends only on the eigenvalue spectrum of the Hamiltonian.

Gröbner bases for finite-temperature quantum computing and their complexity

NASA Astrophysics Data System (ADS)

Crompton, P. R.

2011-11-01

Following the recent approach of using order domains to construct Gröbner bases from general projective varieties, we examine the parity and time-reversal arguments relating to the Wightman axioms of quantum field theory and propose that the definition of associativity in these axioms should be introduced a posteriori to the cluster property in order to generalize the anyon conjecture for quantum computing to indefinite metrics. We then show that this modification, which we define via ideal quotients, does not admit a faithful representation of the Braid group, because the generalized twisted inner automorphisms that we use to reintroduce associativity are only parity invariant for the prime spectra of the exterior algebra. We then use a coordinate prescription for the quantum deformations of toric varieties to show how a faithful representation of the Braid group can be reconstructed and argue that for a degree reverse lexicographic (monomial) ordered Gröbner basis, the complexity class of this problem is bounded quantum polynomial.