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Search Results (1,986)

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Keywords = quantum computing

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16 pages, 1639 KiB  
Article
Post-Quantum Delegated Proof of Luck for Blockchain Consensus Algorithm
by Hyunjun Kim, Wonwoong Kim, Yeajun Kang, Hyunji Kim and Hwajeong Seo
Appl. Sci. 2024, 14(18), 8394; https://doi.org/10.3390/app14188394 - 18 Sep 2024
Viewed by 444
Abstract
The advancements in quantum computing and the potential for polynomial-time solutions to traditional public key cryptography (i.e., Rivest–Shamir–Adleman (RSA) and elliptic-curve cryptography (ECC)) using Shor’s algorithm pose a serious threat to the security of pre-quantum blockchain technologies. This paper proposes an efficient quantum-safe [...] Read more.
The advancements in quantum computing and the potential for polynomial-time solutions to traditional public key cryptography (i.e., Rivest–Shamir–Adleman (RSA) and elliptic-curve cryptography (ECC)) using Shor’s algorithm pose a serious threat to the security of pre-quantum blockchain technologies. This paper proposes an efficient quantum-safe blockchain that incorporates new quantum-safe consensus algorithms. We integrate post-quantum signature schemes into the blockchain’s transaction signing and verification processes to enhance resistance against quantum attacks. Specifically, we employ the Falcon signature scheme, which was selected during the NIST post-quantum cryptography (PQC) standardization process. Although the integration of the post-quantum signature scheme results in a reduction in the blockchain’s transactions per second (TPSs), we introduce efficient approaches to mitigate this performance degradation. Our proposed post-quantum delegated proof of luck (PQ-DPoL) combines a proof of luck (PoL) mechanism with a delegated approach, ensuring quantum resistance, energy efficiency, and fairness in block generation. Experimental results demonstrate that while post-quantum cryptographic algorithms like Falcon introduce larger signature sizes and slower processing times, the PQ-DPoL algorithm effectively balances security and performance, providing a viable solution for secure blockchain operations in a post-quantum era. Full article
(This article belongs to the Special Issue Blockchain and Intelligent Networking for Smart Applications)
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16 pages, 755 KiB  
Article
An MLWE-Based Cut-and-Choose Oblivious Transfer Protocol
by Yongli Tang, Menghao Guo, Yachao Huo, Zongqu Zhao, Jinxia Yu and Baodong Qin
Entropy 2024, 26(9), 793; https://doi.org/10.3390/e26090793 - 16 Sep 2024
Viewed by 238
Abstract
The existing lattice-based cut-and-choose oblivious transfer protocol is constructed based on the learning-with-errors (LWE) problem, which generally has the problem of inefficiency. An efficient cut-and-choose oblivious transfer protocol is proposed based on the difficult module-learning-with-errors (MLWE) problem. Compression and decompression techniques are introduced [...] Read more.
The existing lattice-based cut-and-choose oblivious transfer protocol is constructed based on the learning-with-errors (LWE) problem, which generally has the problem of inefficiency. An efficient cut-and-choose oblivious transfer protocol is proposed based on the difficult module-learning-with-errors (MLWE) problem. Compression and decompression techniques are introduced in the LWE-based dual-mode encryption system to improve it to an MLWE-based dual-mode encryption framework, which is applied to the protocol as an intermediate scheme. Subsequently, the security and efficiency of the protocol are analysed, and the security of the protocol can be reduced to the shortest independent vector problem (SIVP) on the lattice, which is resistant to quantum attacks. Since the whole protocol relies on the polynomial ring of elements to perform operations, the efficiency of polynomial modulo multiplication can be improved by using fast Fourier transform (FFT). Finally, this paper compares the protocol with an LWE-based protocol in terms of computational and communication complexities. The analysis results show that the protocol reduces the computation and communication overheads by at least a factor of n while maintaining the optimal number of communication rounds under malicious adversary attacks. Full article
(This article belongs to the Special Issue Information-Theoretic Cryptography and Security)
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19 pages, 7747 KiB  
Article
Modeling UV/Vis Absorption Spectra of Food Colorants in Solution: Anthocyanins and Curcumin as Case Studies
by Sara Gómez, Piero Lafiosca and Tommaso Giovannini
Molecules 2024, 29(18), 4378; https://doi.org/10.3390/molecules29184378 - 14 Sep 2024
Viewed by 284
Abstract
We present a comprehensive computational study of UV/Vis absorption spectra of significant food colorants, specifically anthocyanins and curcumin tautomers, dissolved in polar protic solvents, namely water and ethanol. The absorption spectra are simulated using two fully polarizable quantum mechanical (QM)/molecular mechanics (MM) models [...] Read more.
We present a comprehensive computational study of UV/Vis absorption spectra of significant food colorants, specifically anthocyanins and curcumin tautomers, dissolved in polar protic solvents, namely water and ethanol. The absorption spectra are simulated using two fully polarizable quantum mechanical (QM)/molecular mechanics (MM) models based on the fluctuating charge (FQ) and fluctuating charge and dipoles (FQFμ) force fields. To accurately capture the dynamical aspects of the solvation phenomenon, atomistic approaches are combined with configurational sampling obtained through classical molecular dynamics (MD) simulations. The calculated QM/FQ and QM/FQFμ spectra are then compared with experiments. Our findings demonstrate that a precise reproduction of the UV/Vis spectra of the studied pigments can be achieved by adequately accounting for configurational sampling, polarization effects, and hydrogen bonding interactions. Full article
(This article belongs to the Special Issue Exclusive Feature Papers in Physical Chemistry, 2nd Edition)
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10 pages, 1762 KiB  
Article
Evanescent Electron Wave-Spin
by Ju Gao and Fang Shen
Entropy 2024, 26(9), 789; https://doi.org/10.3390/e26090789 - 14 Sep 2024
Viewed by 213
Abstract
This study demonstrates the existence of an evanescent electron wave outside both finite and infinite quantum wells by solving the Dirac equation and ensuring the continuity of the spinor wavefunction at the boundaries. We show that this evanescent wave shares the spin characteristics [...] Read more.
This study demonstrates the existence of an evanescent electron wave outside both finite and infinite quantum wells by solving the Dirac equation and ensuring the continuity of the spinor wavefunction at the boundaries. We show that this evanescent wave shares the spin characteristics of the wave confined within the well, as indicated by analytical expressions for the current density across all regions. Our findings suggest that the electron cannot be confined to a mathematical singularity and that quantum information, or quantum entropy, can leak through any quantum confinement. These results emphasize that the electron wave, fully characterized by Lorentz-invariant charge and current densities, should be considered the true and sole entity of the electron. Full article
(This article belongs to the Section Quantum Information)
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57 pages, 2935 KiB  
Article
Quantum Tensor DBMS and Quantum Gantt Charts: Towards Exponentially Faster Earth Data Engineering
by Ramon Antonio Rodriges Zalipynis
Earth 2024, 5(3), 491-547; https://doi.org/10.3390/earth5030027 - 14 Sep 2024
Viewed by 252
Abstract
Earth data is essential for global environmental studies. Many Earth data types are naturally modeled by multidimensional arrays (tensors). Array (Tensor) DBMSs strive to be the best systems for tensor-related workloads and can be especially helpful for Earth data engineering, which takes up [...] Read more.
Earth data is essential for global environmental studies. Many Earth data types are naturally modeled by multidimensional arrays (tensors). Array (Tensor) DBMSs strive to be the best systems for tensor-related workloads and can be especially helpful for Earth data engineering, which takes up to 80% of Earth data science. We present a new quantum Array (Tensor) DBMS data model and new quantum approaches that rely on the upcoming quantum memory and demonstrate exponential speedups when applied to many toughest Array (Tensor) DBMS challenges stipulated by classical computing and real-world Earth data use-cases. We also propose new types of charts: Quantum Gantt (QGantt) Charts and Quantum Network Diagrams (QND). QGantt charts clearly illustrate how multiple operations occur simultaneously across different data items and what are the input/output data dependencies between these operations. Unlike traditional Gantt charts, which typically track project timelines and resources, QGantt charts integrate specific data items and operations over time. A Quantum Network Diagram combines several QGantt charts to show dependencies between multistage operations, including their inputs/outputs. By using a static format, QGantt charts and Quantum Network Diagrams allow users to explore complex processes at their own pace, which can be beneficial for educational and R&D purposes. Full article
26 pages, 2913 KiB  
Review
Overview of Startups Developing Artificial Intelligence for the Energy Sector
by Naiyer Mohammadi Lanbaran, Darius Naujokaitis, Gediminas Kairaitis, Gabrielė Jenciūtė and Neringa Radziukynienė
Appl. Sci. 2024, 14(18), 8294; https://doi.org/10.3390/app14188294 - 14 Sep 2024
Viewed by 654
Abstract
The energy industry is experiencing a major change due to fast progress in artificial intelligence (AI). Startup companies in this revolution use AI technologies like Machine Learning (ML), predictive analytics, and optimization algorithms to improve energy efficiency, optimize grid management, and incorporate renewable [...] Read more.
The energy industry is experiencing a major change due to fast progress in artificial intelligence (AI). Startup companies in this revolution use AI technologies like Machine Learning (ML), predictive analytics, and optimization algorithms to improve energy efficiency, optimize grid management, and incorporate renewable energy sources. AI-powered solutions allow for a more accurate prediction of demand, immediate monitoring, and automated decision-making processes, significantly enhancing operational efficiency and sustainability. Through promoting a more effective energy system, these advancements play a vital role in the worldwide battle against climate change and carbon dioxide emissions. Adding to the progress of AI, quantum computing (QC) shows great potential despite being a nascent area. The collaboration of AI and QC is poised to transform the energy industry by offering unmatched computational capabilities. This blend of technologies can tackle intricate energy obstacles like enhancing power grids and enhancing battery storage, which traditional computers cannot currently handle. Combining QC with AI speeds up innovation, providing advanced solutions that improve the resilience and efficiency of energy networks. This paper discusses the latest advancements, possible effects, and upcoming paths of new companies leading in AI and QC innovations within the energy industry. Their joint responsibility is highlighted in advancing a sustainable and intelligent energy future, as well as tackling crucial environmental issues and lessening the impact of climate change. Full article
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17 pages, 707 KiB  
Article
PyRAMD Scheme: A Protocol for Computing the Infrared Spectra of Polyatomic Molecules Using ab Initio Molecular Dynamics
by Denis S. Tikhonov
Spectrosc. J. 2024, 2(3), 171-187; https://doi.org/10.3390/spectroscj2030012 - 13 Sep 2024
Viewed by 215
Abstract
Here, we present a general framework for computing the infrared anharmonic vibrational spectra of polyatomic molecules using Born–Oppenheimer molecular dynamics (BOMD) with PyRAMD software. To account for nuclear quantum effects, we suggest using a simplified Wigner sampling (SWS) approach simultaneously coupled with Andersen [...] Read more.
Here, we present a general framework for computing the infrared anharmonic vibrational spectra of polyatomic molecules using Born–Oppenheimer molecular dynamics (BOMD) with PyRAMD software. To account for nuclear quantum effects, we suggest using a simplified Wigner sampling (SWS) approach simultaneously coupled with Andersen and Berendsen thermostats. We propose a new criterion for selecting the parameter of the SWS based on the molecules’ harmonic vibrational frequencies and usage of the large-time-step blue shift correction, allowing for a decrease in computational expenses. For the Fourier transform of the dipole moment autocorrelation function, we propose using the regularized least-squares analysis, which allows us to obtain higher-frequency resolution than with the direct application of fast Fourier transform. Finally, we suggest the usage of the pre-parameterized scaling factors for the IR spectra from BOMD, also providing the scaling factors for the spectra at the BLYP-D3(BJ)/6-31G, PBE-D3(BJ)/6-31G, and PBEh-3c levels of theory. Full article
(This article belongs to the Special Issue Feature Papers in Spectroscopy Journal)
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28 pages, 1121 KiB  
Article
Comparing Analytic and Numerical Studies of Tensor Perturbations in Loop Quantum Cosmology
by Guillermo A. Mena Marugán, Antonio Vicente-Becerril and Jesús Yébana Carrilero
Viewed by 269
Abstract
We investigate the implications of different quantization approaches in Loop Quantum Cosmology for the primordial power spectrum of tensor modes. Specifically, we consider the hybrid and dressed metric approaches to derive the effective mass that governs the evolution of the tensor modes. Our [...] Read more.
We investigate the implications of different quantization approaches in Loop Quantum Cosmology for the primordial power spectrum of tensor modes. Specifically, we consider the hybrid and dressed metric approaches to derive the effective mass that governs the evolution of the tensor modes. Our study comprehensively examines the two resulting effective masses and how to estimate them in order to obtain approximated analytic solutions to the tensor perturbation equations. Since Loop Quantum Cosmology incorporates preinflationary effects in the dynamics of the perturbations, we do not have at our disposal a standard choice of privileged vacuum, like the Bunch–Davies state in quasi-de Sitter inflation. We then select the vacuum state by a recently proposed criterion which removes unwanted oscillations in the power spectrum and guarantees an asymptotic diagonalization of the Hamiltonian in the ultraviolet. This vacuum is usually called the NO-AHD (from the initials of Non-Oscillating with Asymptotic Hamiltonian Diagonalization) vacuum. Consequently, we compute the power spectrum by using our analytic approximations and by introducing a suitable numerical procedure, adopting in both cases an NO-AHD vacuum. With this information, we compare the different spectra obtained from the hybrid and the dressed metric approaches, as well as from the analytic and numerical procedures. In particular, this proves the remarkable accuracy of our approximations. Full article
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9 pages, 242 KiB  
Article
Improving Quantum Optimization Algorithms by Constraint Relaxation
by Tomasz Pecyna and Rafał Różycki
Appl. Sci. 2024, 14(18), 8099; https://doi.org/10.3390/app14188099 - 10 Sep 2024
Viewed by 466
Abstract
Quantum optimization is a significant area of quantum computing research with anticipated near-term quantum advantages. Current quantum optimization algorithms, most of which are hybrid variational-Hamiltonian-based algorithms, struggle to present quantum devices due to noise and decoherence. Existing techniques attempt to mitigate these issues [...] Read more.
Quantum optimization is a significant area of quantum computing research with anticipated near-term quantum advantages. Current quantum optimization algorithms, most of which are hybrid variational-Hamiltonian-based algorithms, struggle to present quantum devices due to noise and decoherence. Existing techniques attempt to mitigate these issues through employing different Hamiltonian encodings or Hamiltonian clause pruning, but they often rely on optimistic assumptions rather than a deep analysis of the problem structure. We demonstrate how to formulate the problem Hamiltonian for a quantum approximate optimization algorithm that satisfies all the requirements to correctly describe the considered tactical aircraft deconfliction problem, achieving higher probabilities for finding solutions compared to previous works. Our results indicate that constructing Hamiltonians from an unconventional, quantum-specific perspective with a high degree of entanglement results in a linear instead of exponential number of entanglement gates instead and superior performance compared to standard formulations. Specifically, we achieve a higher probability of finding feasible solutions: finding solutions in nine out of nine instances compared to standard Hamiltonian formulations and quadratic programming formulations known from quantum annealers, which only found solutions in seven out of nine instances. These findings suggest that there is substantial potential for further research in quantum Hamiltonian design and that gate-based approaches may offer superior optimization performance over quantum annealers in the future. Full article
(This article belongs to the Section Quantum Science and Technology)
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11 pages, 4793 KiB  
Proceeding Paper
The Physicochemical Characterisation and Computational Studies of Tilapia Fish Scales as a Green Inhibitor for Steel Corrosion
by Ntiyiso Faith Nyambi, Kasturie Premlall and Krishna Kuben Govender
Viewed by 104
Abstract
The effect of increased corrosion in re-enforcement structures has led to the need to identify and develop more inexpensive, non-toxic, eco-friendly and readily available inhibitors from natural resources. Extensive research and development have led to the discovery of new classes of green corrosion [...] Read more.
The effect of increased corrosion in re-enforcement structures has led to the need to identify and develop more inexpensive, non-toxic, eco-friendly and readily available inhibitors from natural resources. Extensive research and development have led to the discovery of new classes of green corrosion inhibitors. In this work, Tilapia fish scales (FSs) were used as a green corrosion inhibitor as they are abundant in both organic components, such as collagen (C12H19N3O5), and inorganic components, such as hydroxyapatite (Ca10(PO4)6(OH)2). The FSs were subjected to a maceration process to extract all the inorganic and organic compounds. The FS extract was then characterised using an X-ray diffractometer (XRD), a scanning electron microscope (SEM) and Fourier transform infra-red (FTIR). Quantum computational studies were conducted in order to determine parameters such as the energy of the highest occupied molecular orbital (EHOMO) and the energy of the lowest occupied molecular orbital (ELUMO). The Gaussian 09 program density functional theory at the 6-311++(d,p) basis set was used to investigate the interaction between the organic and inorganic molecules, therefore examining both interaction energies. The XRD results confirmed that a large amount of hydroxyapatite was present in the extract, with a high diffractive peak at 32θ and small amounts of collagen picked up between 13θ and 25θ. SEM results showed the percentage weight of atoms, such as carbon (19.8%), calcium (27%), oxygen (41.3%) and phosphate (11.9%), which were found to be present in both the organic and inorganic part of the FS sample. FTIR results confirmed the presence of hydroxyl (3200–3500 cm−1), carbonate (1620–1700 cm−1) and phosphate groups (1200–800 cm−1). The computation studies showed that hydroxyapatite was the most reactive molecule, as it had the highest EHOMO of −0.2076 eV compared with that of collagen at −0.2470 eV. The interaction energy of the FS molecule was −615 kJ/mol. Full article
(This article belongs to the Proceedings of The 3rd International Electronic Conference on Processes)
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12 pages, 4784 KiB  
Article
Optimal Computational Modeling and Simulation of QCA Reversible Gates for Information Reliability in Nano-Quantum Circuits
by Jun-Cheol Jeon
Nanomaterials 2024, 14(17), 1460; https://doi.org/10.3390/nano14171460 - 8 Sep 2024
Viewed by 361
Abstract
As the relationship between energy and information loss and reversible gates was revealed, much interest in reversible gate design arose, and as quantum-dot cellular automata (QCA) gained attention as a next-generation nano circuit design technology, various reversible gates based on QCA emerged. The [...] Read more.
As the relationship between energy and information loss and reversible gates was revealed, much interest in reversible gate design arose, and as quantum-dot cellular automata (QCA) gained attention as a next-generation nano circuit design technology, various reversible gates based on QCA emerged. The proposed study optimizes the performance and design costs of existing QCA-based reversible gates including TR, RUG, PQR, and URG. According to most indicators, the proposed circuits showed significant improvement rates and outperformed existing studies. In particular, the proposed optimal TR, RUG, PQR, and URG showed performance improvements of 266%, 265%, 300%, and 144% in CostAD, respectively, compared with the best existing circuit. This shows outstanding improvement and superiority in terms of area and delay, which are the most important factors in the performance of nano-scale circuits that are becoming extremely miniaturized. Additionally, the exceptionally high-output polarization of the proposed circuits is an important indicator of the circuit’s expansion and connection and increases the circuit’s reliability. Full article
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15 pages, 6481 KiB  
Article
Impact of Channel Thickness and Doping Concentration for Normally-Off Operation in Sn-Doped β-Ga2O3 Phototransistors
by Youngbin Yoon, Yongki Kim and Myunghun Shin
Sensors 2024, 24(17), 5822; https://doi.org/10.3390/s24175822 - 7 Sep 2024
Viewed by 386
Abstract
We demonstrate a Sn-doped monoclinic gallium oxide (β-Ga2O3)-based deep ultraviolet (DUV) phototransistor with high area coverage and manufacturing efficiency. The threshold voltage (VT) switches between negative and positive depending on the β-Ga2 [...] Read more.
We demonstrate a Sn-doped monoclinic gallium oxide (β-Ga2O3)-based deep ultraviolet (DUV) phototransistor with high area coverage and manufacturing efficiency. The threshold voltage (VT) switches between negative and positive depending on the β-Ga2O3 channel thickness and doping concentration. Channel depletion and Ga diffusion during manufacturing significantly influence device characteristics, as validated through computer-aided design (TCAD) simulations, which agree with the experimental results. We achieved enhancement-mode (e-mode) operation in <10 nm-thick channels, enabling a zero VG to achieve a low dark current (1.84 pA) in a fully depleted equilibrium. Quantum confinement in thin β-Ga2O3 layers enhances UV detection (down to 210 nm) by widening the band gap. Compared with bulk materials, dimensionally constrained optical absorption reduces electron–phonon interactions and phonon scattering, leading to faster optical responses. Decreasing β-Ga2O3 channel thickness reduces VT and VG, enhancing power efficiency, dark current, and the photo-to-dark current ratio under dark and illuminated conditions. These results can guide the fabrication of tailored Ga2O3-based DUV phototransistors. Full article
(This article belongs to the Section Electronic Sensors)
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11 pages, 284 KiB  
Article
The Planck Computer Is the Quantum Gravity Computer: We Live inside a Gigantic Computer, the Hubble Sphere Computer?
by Espen Gaarder Haug
Quantum Rep. 2024, 6(3), 482-492; https://doi.org/10.3390/quantum6030032 - 7 Sep 2024
Viewed by 889
Abstract
Recent developments in the quantization of general relativity theory provide a new perspective on matter and even the whole universe. Already, in 1922, Eddington suggested that a future quantum gravity theory had to be linked to Planck length. This is today the main [...] Read more.
Recent developments in the quantization of general relativity theory provide a new perspective on matter and even the whole universe. Already, in 1922, Eddington suggested that a future quantum gravity theory had to be linked to Planck length. This is today the main view among many working with quantum gravity. Recently, it has been demonstrated how Planck length, the Planck time, can be extracted from gravity observations with no knowledge of G, , or even c. Rooted in this, both general relativity theory and multiple other gravity theories can be quantized and linked to the Planck scale. A revelation from this is that matter seems to be ticking at the reduced Compton frequency, where each tick can be seen as one bit, and one bit corresponds to a Planck mass event. This new speculative way of looking at gravity can also potentially tell us considerably about what quantum gravity computers are and what they potentially can do. We will conjecture that that all quantum gravity and quantum gravity computers are directly linked to the Planck scale and the Compton frequency in matter, something we will discuss in this paper. Quantum gravity computers, we will see, in many ways, are nature’s own designed computers with enormous capacity to 3D “print” real time. So, somewhat speculatively, we suggest we live inside a gigantic quantum gravity computer known as the Hubble sphere, and we even are quantum gravity computers. The observable universe is based on this model, basically a quantum gravity computer that calculates approximately 10104 bits per second (bps). Full article
10 pages, 448 KiB  
Article
Random Generation Topology Coding Technique in Asymmetric Topology Encryption
by Jing Su and Bing Yao
Mathematics 2024, 12(17), 2768; https://doi.org/10.3390/math12172768 - 6 Sep 2024
Viewed by 485
Abstract
The security of traditional public key cryptography algorithms depends on the difficulty of the underlying mathematical problems. Asymmetric topological encryption is a graph-dependent encryption algorithm produced to resist attacks by quantum computers on these mathematical problems. The security of this encryption algorithm depends [...] Read more.
The security of traditional public key cryptography algorithms depends on the difficulty of the underlying mathematical problems. Asymmetric topological encryption is a graph-dependent encryption algorithm produced to resist attacks by quantum computers on these mathematical problems. The security of this encryption algorithm depends on two types of NP-complete problems: subgraph isomorphism and graph coloring. Topological coding technology refers to the technology of generating key strings or topology signature strings through topological coding graphs. We take odd-graceful labeling and set-ordered odd-graceful labeling as limiting functions, and propose two kinds of topological coding generation technique, which we call the random leaf-adding operation and randomly adding edge-removing operation. Through these two techniques, graphs of the same scale and larger scales can be generated with the same type of labeling so as to derive more number strings, expand the key space, and analyze the topology and property of the generated graphs. Full article
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18 pages, 6059 KiB  
Article
Computational and Experimental Comparison of Molecularly Imprinted Polymers Prepared by Different Functional Monomers—Quantitative Parameters Defined Based on Molecular Dynamics Simulation
by Jing Yuan, Ying Gao, Xinzhuo Tian, Wenhao Su, Yuxin Su, Shengli Niu, Xiangying Meng, Tong Jia, Ronghuan Yin and Jianmin Hu
Molecules 2024, 29(17), 4236; https://doi.org/10.3390/molecules29174236 - 6 Sep 2024
Viewed by 396
Abstract
Background: In recent years, the advancement of computational chemistry has offered new insights into the rational design of molecularly imprinted polymers (MIPs). From this aspect, our study tried to give quantitative parameters for evaluating imprinting efficiency and exploring the formation mechanism of MIPs [...] Read more.
Background: In recent years, the advancement of computational chemistry has offered new insights into the rational design of molecularly imprinted polymers (MIPs). From this aspect, our study tried to give quantitative parameters for evaluating imprinting efficiency and exploring the formation mechanism of MIPs by combining simulation and experiments. Methods: The pre-polymerization system of sulfadimethoxine (SDM) was investigated using a combination of quantum chemical (QC) calculations and molecular dynamics (MD) simulations. MIPs were prepared on the surface of silica gel by a surface-initiated supplemental activator and reducing agent atom transfer radical polymerization (SI-SARA ATRP). Results: The results of the QC calculations showed that carboxylic monomers exhibited higher bonding energies with template molecules than carboxylic ester monomers. MD simulations confirmed the hydrogen bonding sites predicted by QC calculations. Furthermore, it was observed that only two molecules of monomers could bind up to one molecule of SDM, even when the functional monomer ratio was up to 10. Two quantitative parameters, namely, the effective binding number (EBN) and the maximum hydrogen bond number (HBNMax), were defined. Higher values of EBN and HBNMax indicated a higher effective binding efficiency. Hydrogen bond occupancies and RDF analysis were performed to analyze the hydrogen bond formation between the template and the monomer from different perspectives. Furthermore, under the influence of the EBN and collision probability of the template and the monomers, the experimental results show that the optimal molar ratio of template to monomer is 1:3. Conclusions: The method of monomer screening presented in this study can be extended to future investigations of pre-polymerization systems involving different templates and monomers. Full article
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