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Investigating Layered Topological Magnetic Materials as Efficient Electrocatalysts for the Hydrogen Evolution Reaction under High Current Densities
PublikacjaDespite considerable progress, high-performing durable catalysts operating under large current densities (i.e., >1000 mA/cm2) are still lacking. To discover platinum group metal-free (PGMfree) electrocatalysts for sustainable energy, our research involves investigating layered topological magnetic materials (semiconducting ferromagnets) as highly efficient electrocatalysts for the hydrogen evolution reaction under high current...
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The Ellenbogen's "Matter as Software" Concept for Quantum Computer Implementation: II Bonding Between the C60 and X@C60 Molecules as Available Molecular Building Blocks (MBBs) for Tip-Based Nanofabrication (TBN) of Quantum Computing Devices
PublikacjaThe binding energy, BE of the X@C60-X@C60 homodimer and the X@C60-Y@C60 heterodimer resulting from the bond formation between the occupied X@C60 MBB and the C60 molecule was studied by means of semiempirical PM7 calculations, where X and Y denote atoms from H to Bi, excluding Tc and lanthanides. All possible combinations of N = 68 guest atoms were considered, which resulted in K = 2346 of different calculated dimers of (X@C60-Y@C60)...
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Necessary and Sufficient Condition for State-Independent Contextual Measurement Scenarios
PublikacjaThe problem of identifying measurement scenarios capable of revealing state-independent contextuality in a given Hilbert space dimension is considered. We begin by showing that for any given dimension d and any measurement scenario consisting of projective measurements, (i) the measure of contextuality of a quantum state is entirely determined by its spectrum, so that pure and maximally mixed states represent the two extremes...
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Realistic noise-tolerant randomness amplification using finite number of devices
PublikacjaRandomness is a fundamental concept, with implications from security of modern data systems, to fundamental laws of nature and even the philosophy of science. Randomness is called certified if it describes events that cannot be pre-determined by an external adversary. It is known that weak certified randomness can be amplified to nearly ideal randomness using quantum-mechanical systems. However, so far, it was unclear whether randomness amplification...
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Site-selective magnetic order of neptunium inNp2Ni17
PublikacjaWe present the results obtained by superconducting quantum interference device (SQUID) magnetometry, specific heat, and Mossbauer spectroscopy measurements carried out on Np2Ni17 polycrystalline samples. We show that long-range magnetic order, with a moment mu((2b)) similar to 2.25 mu(B), occurs below T-N = 17.5 K on the Np (2b) sites. A nontrivial situation is observed in that the other Np sites (2d) do not take part to the order...
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Redundant information encoding in QED during decoherence
PublikacjaBroadly understood decoherence processes in quantum electrodynamics, induced by neglecting either the radiation [L. Landau, Z. Phys. 45, 430 (1927)] or the charged matter [N. Bohr and L. Rosenfeld, K. Danske Vidensk. Selsk, Math.-Fys. Medd. XII, 8 (1933)], have been studied from the dawn of the theory. However, what happens in between, when a part of the radiation may be observed, as is the case in many real-life situations, has...
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Formation of carbon monoxide by radiative association: a quantum dynamical study
PublikacjaRate coefficients for the formation of carbon monoxide (CO) by radiative association of carbon and oxygen atoms are computed using quantum dynamical simulations. At temperatures above 10 K CO radiative association is dominated by C(3P) and O(3P) approaching on the A1Π potential energy curve. The rate coefficient is estimated as k=A(T/300 K)αexp−β/T with A= 1.39 × 10−18 cm3 s−1, α=−0.016 and β= 92.2 for temperatures between 6 and...
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Elemental and tight monogamy relations in nonsignaling theories
PublikacjaPhysical principles constrain the way nonlocal correlations can be distributed among distant parties. These constraints are usually expressed by monogamy relations that bound the amount of Bell inequality violation observed among a set of parties by the violation observed by a different set of parties. We prove here that much stronger monogamy relations are possible for nonsignaling correlations by showing how nonlocal correlations...
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Calculation of Vibrational Resonance Raman Spectra of Molecules Using Quantum Chemistry Methods
PublikacjaThe understanding and interpretation of experimental resonance Raman (RR) spectra can strongly benefit from theoretical simulations. These can be achieved by combining quantum chemistry (QC) methods to calculate the electronic and vibrational molecular properties, together with appropriate models and approximations to compute the Raman intensities. This chapter presents the main and most commonly employed approaches to calculate...
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Fluorescence of nanodiamond cocktails: pH-induced effects through interactions with comestible liquids
PublikacjaFluorescent nanodiamonds with nitrogen-vacancy centers have become important nanoscale probes for sensing and imaging. The surface chemistry of the nanodiamonds influences their emission, interactions, and quantum properties. In this work, we propose to utilize fluorescent nanodiamonds as photostable markers for investigation of comestible liquids. We prepared nanodiamond/comestibles suspensions/cocktails with a wide range of pH...
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Spontaneous electron emission vs dissociation in internally hot silver dimer anions
PublikacjaReferring to a recent experiment, we theoretically study the process of a two-channel decay of the diatomic silver anion (Ag2-), namely the spontaneous electron ejection giving Ag2 + e- and the dissociation leading to Ag- + Ag. The ground state potential energy curves of the silver molecules of diatomic neutral and negative ion were calculated using proper pseudo-potentials and atomic basis sets. We also estimated the non-adiabatic...
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Evaluating experimental molecular physics studies of radiation damage in DNA*
PublikacjaThe field of Atomic and Molecular Physics (AMP) is a mature field exploring the spectroscopy, excitation, ionisation of atoms and molecules in all three phases. Understanding of the spectroscopy and collisional dynamics of AMP has been fundamental to the development and application of quantum mechanics and is applied across a broad range of disparate disciplines including atmospheric sciences, astrochemistry, combustion and environmental...
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Theoretical study of the photoelectron spectrum of ethyl formate: Ab initio and density functional theory investigation
PublikacjaThe first ionization energy and associated photoelectron spectrum of ethyl formate are investigated with quantum chemistry calculations. The geometries, harmonic vibrational frequencies and first ionization energy are computed at the Hartree-Fock (HF) and at the second order Moller-Plesset perturbation theory (MP2). Moreover, accurate ionization energies are obtained with the Coupled-Cluster theory including singles and doubles...
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Hydroperoxyl radical and formic acid formation from common DNA stabilizers upon low energy electron attachment
Publikacja2-Amino-2-(hydroxymethyl)-1,3-propanediol (TRIS) and ethylenediaminetetraacetic acid (EDTA) are key components of biological buffers and are frequently used as DNA stabilizers in irradiation studies. Such surface or liquid phase studies are done with the aim to understand the fundamental mechanisms of DNA radiation damage and to improve cancer radiotherapy. When ionizing radiation is used, abundant secondary electrons are formed...
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The LaPdIn 4 indide and elementary properties of the LaTIn 4 ( T = Ni, Pd, Pt) materials family
PublikacjaThe indium-rich intermetallic compound LaPdIn4 is reported, prepared by arc-melting and annealing at 600 C. Single crystal X-ray diffraction found the material to be orthorhombic, space group Cmcm (No. 63), with lattice parameters a ¼ 4.5462(3) Å, b ¼ 16.9208(10) Å, and c ¼ 7.3100(5) Å. This previously unreported indide is isostructural with LaNiIn4 and LaPtIn4. It is demonstrated that all three compounds in the LaTIn4 (T ¼ Ni,...
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(CsX)Cu5O2(PO4)2 (X = Cl, Br, I): A Family of Cu2+ S = 1/2 Compounds with Capped-Kagomé Networks Composed of OCu4 Units
PublikacjaThree new salt inclusion compounds (CsX)Cu5O2(PO4)2 (X = Cl, Br, I), phosphate analogues of the kagomé mineral averievite, are reported. Their crystal structures are composed of trigonal networks of corner-sharing OCu4 anion-centered tetrahedra, forming capped-kagomé planes, which can also be regarded as two-dimensional slices along the [111] direction of a pyrochlore lattice. Magnetization and heat capacity measurements reveal...
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Constructing genuinely entangled multipartite states with applications to local hidden variables and local hidden states models
PublikacjaBuilding upon the results of R. Augusiak et al. [Phys. Rev. Lett. 115, 030404 (2015)] we develop a general approach to the generation of genuinely entangled multipartite states of any number of parties from genuinely entangled states of a fixed number of parties, in particular, the bipartite entangled ones. In our approach, certain isometries whose output subspaces are either symmetric or genuinely entangled in some multipartite...
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Wavepacket of the Universe and its Spreading
PublikacjaWavepackets in quantum mechanics spread and the Universe in cosmology expands. We discuss a formalism where the two effects can be unified. The basic assumption is that the Universe is determined by a unitarily evolving wavepacket defined on space-time. Space-time is static but the Universe is dynamic. Spreading analogous to expansion known from observational cosmology is obtained if one regards time evolution as a dynamical process...
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Mechanism of hopping conduction in Be–Fe–Al–Te–O semiconducting glasses and glass–ceramics
PublikacjaElectrical properties of beryllium-alumino-tellurite glasses and glass–ceramics doped with iron ions were studied using impedance spectroscopy. The conductivity was measured over a wide frequency range from 10 mHz to 1 MHz and the temperature range from 213 to 473 K. The D.C. conductivity values showed a correlation with the Fe-ion concentration and ratio of iron ions on different valence states in the samples. On the basis of...
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Quantifying Contextuality
PublikacjaContextuality is central to both the foundations of quantum theory and to the novel information processing tasks. Despite some recent proposals, it still faces a fundamental problem: how to quantify its presence? In this work, we provide a universal framework for quantifying contextuality. We conduct two complementary approaches: (i) the bottom-up approach, where we introduce a communication game, which grasps the phenomenon of...
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The Ellenbogen’s “Matter as Software” Concept for Quantum Computer Implementation: IV. The X@C60 Molecular Building Blocks (MBBs) and Computing System Lifetime Estimation
PublikacjaThe problem of approximate lifetimes of individual X@C60 MBBs and tip-based nanofabricated quantum computing device systems is discussed under the conservative assumption of single-point failure. A single chemical transformation of the C60 cage into high-energy opened o-C60 isomer which forms the communication canal for the low energy transfer of an X atom from X@C60 MBB to the outside environment was studied. According to the...
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Electron-Induced Decomposition of 5-Bromo-4-thiouracil and 5-Bromo-4-thio-2′-deoxyuridine: The Effect of the Deoxyribose Moiety on Dissociative Electron Attachment
PublikacjaWhen modified uridine derivatives are incorporated into DNA, radical species may form that cause DNA damage. This category of molecules has been proposed as radiosensitizers and is currently being researched. Here, we study electron attachment to 5-bromo-4-thiouracil (BrSU), a uracil derivative, and 5-bromo-4-thio-20 -deoxyuridine (BrSdU), with an attached deoxyribose moiety via the N-glycosidic (N1-C) bond. Quadrupole mass spectrometry...
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Extending loophole-free nonlocal correlations to arbitrarily large distances
PublikacjaQuantum theory allows spatially separated observers to share nonlocal correlations, which enable them to accomplish classically inconceivable information processing and cryptographic feats. However, the distances over which nonlocal correlations can be realized remain severely limited due to their high fragility to noise and high threshold detection efficiencies. To enable loophole- free nonlocality across large distances, we introduce...
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Crossover from charge density wave stabilized antiferromagnetism to superconductivity in Nd1−xLaxNiC2 compounds
PublikacjaThe path from the charge density wave antiferromagnet NdNiC2 to the noncentrosymmetric superconductor LaNiC2 is studied by gradual replacement of Nd by La ions. The evolution of physical properties is explored by structural, magnetic, transport, magnetoresistance, and specific heat measurements. With the substitution of La for Nd, the Peierls temperature is gradually suppressed, which falls within the BCS mean-field relation for...
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Electron-Induced Decomposition of Uracil-5-yl O-(N,N-dimethylsulfamate): Role of Methylation in Molecular Stability
PublikacjaThe incorporation of modified uracil derivatives into DNA leads to the formation of radical species that induce DNA damage. Molecules of this class have been suggested as radiosensitizers and are still under investigation. In this study, we present the results of dissociative electron attachment to uracil-5-yl O-(N,N-dimethylsulfamate) in the gas phase. We observed the formation of 10 fragment anions in the studied range of electron...
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Quantum and carbon dots conjugated molecularly imprinted polymers as advanced nanomaterials for selective recognition of analytes in environmental, food and biomedical applications
PublikacjaSamples with complex matrix analyzed during explanation of pathogenesis of various diseases and food or environmental monitoring request advanced analytical and instrumental devices. Among the materials used for described purposes, quantum (QDs) or carbon dots (CDs) layered by molecularly imprinted polymer (MIP) shells have gained widespread attention. Unique optical and physicochemical properties of QDs/CDs together with high...
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Determination of aminoglycoside antibiotics: current status and future trends
PublikacjaThe use of aminoglycoside antibiotics is prevalent in medicine and agriculture. Their overuse increases their mobility in the environment, resulting in a need for reliable methods for their determination in a variety of matrices. However, the properties of aminoglycosides, in particular their high polarity, make the development of such methods a non-trivial task, inciting researchers to tackle this complex issue from different...
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Spinon excitations in the quasi-one-dimensional S=12 chain compound Cs4CuSb2Cl12
PublikacjaThe spin−1/2 Heisenberg antiferromagnetic chain is ideal for realizing one of the simplest gapless quantum spin liquids (QSLs), supporting a many-body ground state whose elementary excitations are fractional fermionic excitations called spinons. Here we report the discovery of such a one-dimensional (1D) QSL in Cs4CuSb2Cl12. Compared to previously reported S=1/2 1D chains, this material possesses a wider temperature range over...
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Beyond the helium buffer: 12C−2 rotational cooling in cold traps with H2 as a partner gas: interaction forces and quantum dynamics
Publikacjaabstract = { The scattering cross-sections and corresponding rate coefficients for rotationally inelastic collisions of $^{12}$C$_2$^-$ ($^2 \Sigma_g^+$) with H$_2$ ($^1 \Sigma_g^+$) are presented over a broad range of cold-trap temperatures. They have been calculated using quantum scattering theory that employs a new ab initio potential energy surface. The rate coefficients for the inelastic processes in the anionic partner are...
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General solution of quantum mechanical equations of motion with time-dependent Hamiltonians: A Lie algebraic approach
PublikacjaThe unitary operators U(t), describing the quantum time evolution of systems with a time-dependent Hamiltonian, can be constructed in an explicit manner using the method of time-dependent invariants. We clarify the role of Lie-algebraic techniques in this context and elaborate the theory for SU(2) and SU(1,1). In these cases we give explicit formulae for obtaining general solutions from special ones. We show that the constructions...
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Highly Visible-Light-Photoactive Heterojunction Based on TiO2 Nanotubes Decorated by Pt Nanoparticles and Bi2S3 Quantum Dots
PublikacjaA heterojunction with excellent visible light response and stability based on titanium dioxide nanotubes (TiO2 NTs), bismuth sulfide quantum dots (Bi2S3 QDs), and platinum nanoparticles (Pt NPs) is proposed. Both Pt NPs (3.0 ± 0.2 nm) and Bi2S3 QDs (3.50 ± 0.20 nm) are well distributed on the (i) top parts, (ii) inner walls, and (iii) outer walls of the TiO2 NTs. Visible-light-induced photoreaction was initialized by excitation...
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Distributed Representations Based on Geometric Algebra: the Continuous Model
PublikacjaAuthors revise the concept of a distributed representation of data as well as two previously developed models: Holographic Reduced Representation (HRR) and Binary Spatter Codes (BSC). A Geometric Analogue (GAc - ''c'' stands for continuous as opposed to its discrete version) of HRR is introduced - it employs role-filler binding based on geometric products. Atomic objects are real-valued vectors in n-dimensional Euclidean space...
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Why Are Left-Handed G-Quadruplexes Scarce?
PublikacjaG-quadruplexes (G4s) are nucleic acid structures crucial for the regulation of gene expression and genome maintenance. While they hold promise as nanodevice components, achieving desired G4 folds requires understanding the interplay between stability and structural properties, like helicity. Although right-handed G4 structures dominate the experimental data, the molecular basis for this preference over left-handed helicity is unclear....
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Effect of copper and silver modification of NH2-MIL-125(Ti) on the photoreduction of carbon dioxide to formic acid over this framework under visible-light irradiation
PublikacjaCu and Ag enhance the photocatalytic activities of metal–organic frameworks (MOFs) toward CO2 conversion because of their CO2 adsorption capacities and effects on the lowest unoccupied molecular orbital (LUMO) overpotentials of MOFs. However, to date, targeted introduction of metals into MOFs to achieve visible (Vis)- light-active photocatalysts for CO2 photoconversion has not been realized. Herein, a series of aminefunctionalized...
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Visible light photocatalytic activity of ionic liquid-TiO2 spheres: effect of the ionic liquid's anion structure
PublikacjaThe effect of the ionic liquid’s (IL) anion type ([BIMIM][X], where X= [Br], [PF6] or [OctSO4]) and content on the morphology, surface properties and photoactivity of TiO2 obtained by solvothermal method has been systematically investigated. Our results revealed that the presence of [Br], [OctSO4] anions favors formation of anatase phase, while presence of [PF6] anion causes formation of mixture of anatase and Ti(OH)PO4 phases....
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Comparison of simplified sum-over-state expressions to calculate resonance Raman intensities including Franck-Condon and Herzberg-Teller effects
PublikacjaSum-over-state (SOS) expressions to simulate absorption spectroscopy and resonance Raman (RR) scattering including Franck-Condon (FC) and Herzberg-Teller (HT) effects are described. Starting from the general SOS method, several simplified SOS formulae are derived. In particular, within the so-called independent mode displaced harmonic oscillator model, it is shown that including the vibronic structure in the absorption and RR spectra...
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The Role of Electrostatics in Enzymes: Do Biomolecular Force Fields Reflect Protein Electric Fields?
PublikacjaPreorganization of large, directionally oriented, electric fields inside protein active sites has been proposed as a crucial contributor to catalytic mechanism in many enzymes, and it may be efficiently investigated at the atomistic level with molecular dynamics simulations. Here, we evaluate the ability of the AMOEBA polarizable force field, as well as the additive Amber ff14SB and Charmm C36m models, to describe the electric...
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Soft X-ray Induced Production of Neutral Fragments in High-Rydberg States at the O 1s Ionization Threshold of the Water Molecule
PublikacjaDissociation of water molecules after soft X-ray absorption can yield neutral fragments in high-Rydberg (HR) states. We have studied the production of such fragments by field ionization and ion time-of-flight (TOF) spectrometry. Neutral HR fragments are created at all resonances below the O 1s ionization potential (IP) and particularly within 1 eV above the O 1s IP. The latter effect is due to the recapture of the O 1s photoelectrons...
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Theoretical and Experimental Studies on the Visible Light Activity of TiO2 Modified with Halide-Based Ionic Liquids
PublikacjaFormation of a surface complex between organic molecules and TiO2 is one of the possible strategies for the development of visible light-induced TiO2 photoactivity. Herein, three ionic liquids (ILs) with the same cation and dierent anions (1-butylpirydynium chloride/bromide/iodide) have been applied for the surface modification of TiO2 and to understand the role of anions in visible light-induced activity of ILs-TiO2 systems. Photocatalytic...
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Mechanism of reaction of RNA-dependent RNA polymerase from SARS-CoV-2
PublikacjaWe combine molecular dynamics, statistical mechanics, and hybrid quantum mechanics/molecular mechanics simulations to describe mechanistically the severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) RNA-dependent RNA polymerase (RdRp). Our study analyzes the binding mode of both natural triphosphate substrates as well as remdesivir triphosphate (the active form of drug), which is bound preferentially over ATP by RdRp while...
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Principles of target DNA cleavage and the role of Mg2+ in the catalysis of CRISPR–Cas9
PublikacjaAt the core of the CRISPR–Cas9 genome-editing technology, the endonuclease Cas9 introduces site-specific breaks in DNA. However, precise mechanistic information to ameliorate Cas9 function is still missing. Here, multimicrosecond molecular dynamics, free energy and multiscale simulations are combined with solution NMR and DNA cleavage experiments to resolve the catalytic mechanism of target DNA cleavage. We show that the conformation...
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Theory versus experiment for vacuum Rabi oscillations in lossy cavities. II. Direct test of uniqueness of vacuum
PublikacjaThe paper continues the analysis of vacuum Rabi oscillations we started in part I [Phys. Rev. A 79, 033836 (2009)]. Here we concentrate on experimental consequences for cavity QED of two different classes of representations of harmonic-oscillator Lie algebras. The zero-temperature master equation, derived in part I for irreducible representations of the algebra, is reformulated in a reducible representation that models electromagnetic...
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Self-healing mechanism of metallopolymers investigated by QM/MM simulations and Raman spectroscopy
PublikacjaThe thermally induced self-healing mechanisms in metallopolymers based on bisterpyridine complexes of iron(II) sulfate and cadmium(II) bromide, respectively, were studied by means of combined quantum mechanical/molecular mechanical (QM/MM) simulations and Raman spectroscopy. Two possible healing schemes, one based on a decomplexation of the cross-linking complexes and a second one relying on the dissociation of ionic clusters,...
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Numerical modeling of quantum dynamical processes
PublikacjaIn this dissertation I present a high-precision (15, 18 or 33 decimal places) C++ implementation of quantum dynamics time propagation algorithms for both time-independent and time-dependent Hamiltonian with an inhomogeneous source term. Moreover I present an extension of both algorithms for time propagation to handle arbitrary number of coupled electronic levels. I have performed a careful validation of these implementations comparing...
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Experimental and DFT insights into an eco-friendly photocatalytic system toward environmental remediation and hydrogen generation based on AgInS2 quantum dots embedded on Bi2WO6
PublikacjaBismuth tungstate (Bi2WO6) can work as a photocatalyst but suffers from rapid recombination of photogenerated charge carriers. Herein, density functional theory (DFT) simulations revealed that the formation of a thermodynamically stable AgInS2(112)/Bi2WO6(010) heterojunction could promote charge separation and enhance the photoactivity of Bi2WO6. To confirm these theoretical predictions, a new type of photocatalysts in the form...
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Calculating the Partition Coefficients of Organic Solvents in Octanol/Water and Octanol/Air
PublikacjaPartition coefficients define how a solute is distributed between two immiscible phases at equilibrium. The experimental estimation of partition coefficients in a complex system can be an expensive, difficult, and time-consuming process. Here a computational strategy to predict the distributions of a set of solutes in two relevant phase equilibria is presented. The octanol/water and octanol/air partition coefficients are predicted...
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Guanosine Dianions Hydrated by One to Four Water Molecules
PublikacjaIntermolecular interactions such as those present in molecule···water complexes may profoundly influence the physicochemical properties of molecules. Here, we carried out an experimental–computational study on doubly deprotonated guanosine monophosphate···water clusters, [dGMP – 2H]2–·nH2O (n = 1–4), using a combination of negative anion photoelectron spectroscopy (NIPES) with molecular dynamics (MD) and quantum chemical (QM) calculations....
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Non-Perfect Propagation of Information to a Noisy Environment with Self-Evolution
PublikacjaWe study the non-perfect propagation of information for evolving a low-dimensional environment that includes self-evolution as well as noisy initial states and analyse the interrelations between the degree of objectivization and environment parameters. In particular, we consider an analytical model of three interacting qubits and derive its objectivity parameters. The numerical analysis shows that the quality of the spectrum broadcast...
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New Screening Protocol for Effective Green Solvents Selection of Benzamide, Salicylamide and Ethenzamide
PublikacjaNew protocol for screening efficient and environmentally friendly solvents was proposed and experimentally verified. The guidance for solvent selection comes from computed solubility via COSMO-RS approach. Furthermore, solute-solvent affinities computed using advanced quantum chemistry level were used as a rationale for observed solvents ranking. The screening protocol pointed out that 4-formylomorpholine (4FM) is an attractive...
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Waterborne polyesters partially based on renewable resources
PublikacjaA new experimental approach for preparing biobased, water-soluble polyesters via titanium(IV) n-butoxide-catalyzed bulk polycondensation is presented. In the described method polymers were obtained from isosorbide, maleic anhydride and poly(ethylene glycol). The chemical structure of the synthesized polyesters was confirmed using 2D NMR spectroscopy and by titration methods. Careful analysis of 2D NMR spectra viz. Correlation Spectra...