Article
Materials Science, Multidisciplinary
Francois Damanet, Elliott Mansfield, Megan Briggeman, Patrick Irvin, Jeremy Levy, Andrew J. Daley
Summary: Understanding and controlling the transport properties of interacting fermions is crucial in quantum physics; Different forms of spin-orbit coupling can enhance electron pairing in 1D waveguides; Metal-oxide heterostructures are attractive platforms for controlling the collective spin of electron bound states.
Article
Optics
Shuwei Jin, Jianshun Gao, Karthik Chandrashekara, Christian Goelzhaeuser, Joschka Schoener, Lauriane Chomaz
Summary: We propose a scheme for loading dysprosium atoms into a narrow-line three-dimensional magneto-optical trap (3D MOT) using a two-dimensional MOT on the broad 421-nm line to generate a high-flux slow atoms beam. Efficient loading of the 3D MOT is achieved even without the push beam, and further enhancement is observed by adding push beams at either 421 nm or 626 nm. The best performance is achieved with a red-detuned push beam on the 626-nm line, resulting in an enhancement factor of 3.6.
Article
Physics, Multidisciplinary
Shanshan Ding, G. A. Dominguez-Castro, Aleksi Julku, Arturo Camacho-Guardian, Georg M. Bruun
Summary: This study investigates mobile impurities immersed in a Bose-Einstein condensate in a two-dimensional lattice to understand the interactions and possible bound states of quasiparticles. The results show the emergence of a new type of quasiparticle and the spatial influence of impurity-boson interactions. By deriving an effective Schrodinger equation, it is demonstrated that the attractive interaction between two polarons in the lattice leads to the formation of bound states, known as bipolarons.
Article
Chemistry, Multidisciplinary
Liang Liu, Zezhou Lin, Jifan Hu, Xi Zhang
Summary: Five 2D semiconductors with ferromagnetic properties and their corresponding Curie temperatures were identified using a new method, which showed agreement with experimental results. Systems with low-spin numbers and low anisotropies have higher Curie temperatures. These findings provide excellent candidates for future spintronics applications.
Article
Optics
Yu-Biao Wu, Guang-Can Guo, Zhen Zheng, Xu-Bo Zou
Summary: The proposal introduces a method for synthesizing higher-order topological superfluids that support various Majorana zero modes in ultracold atomic gases. By using a two-dimensional optical superlattice that modulates spin-orbit coupling spatially, different topological phase transitions among trivial superfluids, first-order and second-order topological superfluids are identified with respect to experimentally tunable parameters.
Article
Materials Science, Multidisciplinary
Ying Chen, Ao Wu, Yiming Zhang, Yu Wu, Yujie Xia, Congcong Ma, Heyuan Zhu, Hao Zhang, Zhilai Fang
Summary: This study investigates the exciton macroscopic quantum phases of two-dimensional ultrawide bandgap semiconductors I-Ga2O3 and II-Ga2O3 for the first time, revealing their complex excitonic composition and morphology. It is found that these materials can achieve Bose-Einstein condensation at high temperatures, making them promising for applications in fields such as ultrahigh power photonics and quantum information. These findings expand the material basis for the research of exciton macroscopic quantum phases and will boost their applications in novel optoelectronic devices.
MATERIALS TODAY PHYSICS
(2022)
Article
Chemistry, Physical
Xuanyu Zhu, Marc Riera, Ethan F. Bull-Vulpe, Francesco Paesani
Summary: Using the MB-pol theoretical/computational framework, we have introduced a new family of data-driven many-body potential energy functions (PEFs) for water, named MB-pol(2023). By employing larger training sets and adopting sophisticated machine-learned representations, the MB-pol(2023) PEFs achieve sub-chemical accuracy in modeling hexamer isomers and outperform existing PEFs in describing water clusters in the gas phase. Moreover, the MB-pol(2023) PEFs show remarkable agreement with experimental results for various properties of liquid water, improving upon the original MB-pol PEF and closing the gap with experimental measurements.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Materials Science, Multidisciplinary
Fernando J. Gomez-Ruiz, David Subires, Adolfo del Campo
Summary: The study examines the role of boundary conditions in the statistics of topological defects, finding that the cumulants exhibit universal scaling with the quench rate independent of the boundary conditions for fast and moderate quenches, but an additive term becomes prominent in slow quenches, breaking the power-law behavior.
Article
Chemistry, Physical
Jin-Wei Hu, Yong-Chang Han
Summary: This paper presents a method for calculating the thermally averaged population by simulating thermal ensembles with random phases, and compares it with two other methods. It is found that method A is more efficient in inducing molecular field-free alignment, showing higher computational efficiency at higher temperatures.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Quantum Science & Technology
Dominik Kiesenhofer, Helene Hainzer, Artem Zhdanov, Philip C. Holz, Matthias Bock, Tuomas Ollikainen, Christian F. Roos
Summary: This paper presents experiments with planar Coulomb crystals of up to 105 40Ca+ ions in a novel monolithic rf trap, laying the groundwork for quantum simulations of two-dimensional spin models with single-particle control. The trapping potential is characterized through analysis of crystal images and comparison with numerical simulations. Stable confinement of large crystals free of structural configuration changes is demonstrated, and it is found that rf heating of the crystal is not an obstacle for future quantum simulation experiments. Finally, the out-of-plane motional modes of planar crystals consisting of up to 105 ions are prepared close to their ground state through electromagnetically induced transparency cooling, an important prerequisite for implementing long-range entangling interactions.
Article
Chemistry, Physical
Tomislav Begusic, Jiri Vanicek
Summary: An exact finite-temperature expression for vibrational dynamics is derived using the concept of thermo-field dynamics, allowing for an intuitive wavepacket-based interpretation. The new method combines this exact approach with the thawed Gaussian approximation to compute finite-temperature two-dimensional spectra efficiently, providing insight into symmetry breaking and deviation from traditional models in the signal.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2021)
Article
Optics
Samrit Mainali, Fabien Gatti, Osman Atabek
Summary: The control strategies inspired by interference and kicks were applied to pyrazine to achieve the maximum population deposition in the acceptor state.
CHINESE OPTICS LETTERS
(2022)
Article
Mechanics
Juan Jose Mendoza-Arenas
Summary: This study investigates the emergence of dynamical quantum phase transitions in the extended Fermi-Hubbard model using tensor network simulations. The researchers identify various sudden interaction quenches that lead to DQPTs and establish clear connections to specific properties of observables.
JOURNAL OF STATISTICAL MECHANICS-THEORY AND EXPERIMENT
(2022)
Article
Chemistry, Physical
Xiaoren Zhang, Zhaojun Zhang, Fabien Gatti, Dong H. Zhang
Summary: This study presents a full-dimensional quantum dynamical investigation of bimolecular reactions of hydrogen molecules with amino radicals for different isotopologues. The effects of different vibrational mode excitations of the reagents on the reactivities are studied, along with thorough physical explanations about the isotope effects.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Physics, Fluids & Plasmas
Jae Dong Noh
Summary: We investigate the eigenstate thermalization properties of the spin-1/2 XXZ model in two-dimensional rectangular lattices. The numerical analysis supports that the model follows the eigenstate thermalization hypothesis, and this hypothesis is still valid within each subspace where the total spin is a good quantum number.
Article
Chemistry, Physical
Ethan F. Bull-Vulpe, Marc Riera, Sigbjorn L. Bore, Francesco Paesani
Summary: This study presents a generalization of the many-body energy framework, which can be used to develop data-driven potential energy functions for molecules with covalent bonds. By defining monomers as building blocks and using permutationally invariant polynomials to represent the energy, complex molecular systems can be simulated with arbitrary quantum mechanical accuracy.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Chemistry, Physical
Debbie Zhuang, Marc Riera, Ruihan Zhou, Alexander Deary, Francesco Paesani
Summary: The study systematically investigated the hydration structure of Na+ and K+ ions in solution by progressively including many-body effects derived from the many-body expansion of the energy. It found that MB-nrg potential energy functions achieved nearly quantitative agreement with the experimental EXAFS spectra, providing accurate models for predicting properties of ionic aqueous systems from gas to liquid phase.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Physical
Alessandro Caruso, Xuanyu Zhu, John L. Fulton, Francesco Paesani
Summary: Ion-water interactions are crucial for determining the properties of aqueous systems, but the evolution of ion hydration from small clusters to bulk solutions and interfaces remains unclear. In this study, the authors introduce a data-driven many-body energy potential energy function that accurately predicts bromide-water and iodide-water interactions. Molecular dynamics simulations using this potential energy function successfully reproduce experimental spectra, allowing for characterization of the hydration structure of these ions.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Physical
Yaoguang Zhai, Alessandro Caruso, Sigbjorn Loland Bore, Zhishang Luo, Francesco Paesani
Summary: Deep neural network (DNN) potentials have gained popularity in computer simulations of molecular systems. This study combines the computational efficiency of the DeePMD framework and the accuracy of the MB-pol potential to train a DNN potential for large-scale simulations of water. The DNN potential can reproduce MB-pol results for liquid water but lacks accuracy for vapor-liquid equilibrium properties. Attempts to include many-body effects result in a new DNN potential that accurately reproduces vapor-liquid equilibrium properties but loses accuracy in liquid properties.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Raja Ghosh, Francesco Paesani
Summary: Photoactive organic and hybrid organic-inorganic materials exhibit interesting photophysical properties upon interaction with light. A theoretical model that accurately describes the structure-photophysics-property relationships is crucial for understanding these materials. This perspective introduces a unified theoretical framework and discusses excitonic and polaronic photophysical signatures in different materials using the Multiparticle Holstein Formalism. The integration of advanced computational methods with the Multiparticle Holstein Formalism is expected to identify new design strategies for next-generation energy materials.
Article
Biochemistry & Molecular Biology
Brodie L. Ranzau, Kartik L. Rallapalli, Mallory Evanoff, Francesco Paesani, Alexis C. Komor
Summary: Base editors are genome editing tools that modify nucleobases in DNA to enable precise base conversions. Adenine base editors convert A.T base pairs to G.C base pairs by using an adenosine deaminase enzyme. Previous experiments showed that the wild-type TadA enzyme had no activity on DNA, but we demonstrated that it can perform base editing in both bacterial and mammalian cells.
Article
Chemistry, Physical
Xuanyu Zhu, Marc Riera, Ethan F. Bull-Vulpe, Francesco Paesani
Summary: Using the MB-pol theoretical/computational framework, we have introduced a new family of data-driven many-body potential energy functions (PEFs) for water, named MB-pol(2023). By employing larger training sets and adopting sophisticated machine-learned representations, the MB-pol(2023) PEFs achieve sub-chemical accuracy in modeling hexamer isomers and outperform existing PEFs in describing water clusters in the gas phase. Moreover, the MB-pol(2023) PEFs show remarkable agreement with experimental results for various properties of liquid water, improving upon the original MB-pol PEF and closing the gap with experimental measurements.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Multidisciplinary
Thomas M. Rayder, Filip Formalik, Simon M. Vornholt, Hilliary Frank, Seryeong Lee, Maytham Alzayer, Zhihengyu Chen, Debabrata Sengupta, Timur Islamoglu, Francesco Paesani, Karena W. Chapman, Randall Q. Snurr, Omar K. Farha
Summary: Carbon capture, storage, and utilization (CCSU) is an opportunity to reduce carbon emissions and combat global climate change. Metal-organic frameworks (MOFs) have shown great potential as effective CO2 sorbents in CCSU through gas adsorption. Understanding the properties of MOF pores and their dynamic behavior during sorption can lead to the development of more efficient CCSU materials.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Multidisciplinary Sciences
Sigbjrn Lland Bore, Francesco Paesani
Summary: Since the early 1900s, scientists have been trying to understand the stability of ice polymorphs in water's phase diagram. This study combines the MB-pol data-driven many-body potential for water with advanced enhanced-sampling algorithms to simulate water's phase diagram with a high level of realism. The study provides insights into the role of enthalpic, entropic, and nuclear quantum effects in shaping the free-energy landscape of water and bridges the gap between experiments and simulations.
NATURE COMMUNICATIONS
(2023)
Article
Chemistry, Multidisciplinary
Ching-Hwa Ho, Mason L. L. Valentine, Zhijie Chen, Haomiao Xie, Omar Farha, Wei Xiong, Francesco Paesani
Summary: This study investigates the water adsorption mechanism in the hydrophilic metal-organic framework NU-1500-Cr using molecular dynamics simulations and infrared spectroscopy. It is found that water initially adsorbs at the open Cr3+ sites and then forms water chains that gradually fill the framework. The insights gained from this study can contribute to the design of efficient water harvesting materials.
COMMUNICATIONS CHEMISTRY
(2023)
Article
Chemistry, Physical
Yuanhui Pan, Ching-Hwa Ho, Francesco Paesani, Raja Ghosh
Summary: Covalent organic frameworks (COFs) are 2D organic materials with unique electronic and transport properties. In this study, the impact of interlayer stacking arrangements on the electronic structure and coherence of polarons in donor-acceptor COFs was investigated through density functional theory and multiparticle Holstein formalism simulations. It was found that the stacking arrangement significantly influences the transport properties, with varying behavior from metallic to highly localized states. The extent of charge delocalization is sensitive to the type and precise arrangement of interlayer stacking and donor-acceptor fragments in the COF structure. The results suggest that interlayer interactions can aid in enhancing charge delocalization and guide the design of new COF structures for potential applications in organic electronics.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Physical
Marc Riera, Christopher Knight, Ethan F. Bull-Vulpe, Xuanyu Zhu, Henry Agnew, Daniel G. A. C. Smith, Andrew Simmonett, Francesco Paesani
Summary: MBX is a C++ library that implements many-body potential energy functions (PEFs) within the many-body energy (MB-nrg) formalism. MB-nrg PEFs integrate an underlying polarizable model with explicit machine-learned representations of many-body interactions to achieve chemical accuracy from the gas to the condensed phases. MBX can be used as a standalone package or integrated with other molecular simulation software as an energy/force engine. It allows for classical and quantum molecular simulations with MB-nrg PEFs, as well as hybrid simulations combining conventional force fields and MB-nrg PEFs for diverse systems.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Ruihan Zhou, Marc Riera, Francesco Paesani
Summary: We introduce a data-driven many-body energy potential energy function (MB-nrg PEF) to accurately describe the energetics and structural properties of N-methylacetamide (NMA), as well as the NMA-water interactions. The results show that the MB-nrg PEF is able to accurately represent many-body effects in both gas and liquid phases, making it a promising molecular model for predictive simulations of biomolecular systems.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Materials Science, Multidisciplinary
Zhihengyu Chen, Ching-Hwa Ho, Xiaoliang Wang, Simon M. Vornholt, Thomas M. Rayder, Timur Islamoglu, Omar K. Farha, Francesco Paesani, Karena W. Chapman
Summary: CALF-20, a metal-organic framework, shows selective CO2 physisorption. This study reveals that CALF-20 undergoes a structure transformation when exposed to humid environments, resulting in a new polymorph. The transformation is reversible, and the original structure can be regenerated. Computational evaluation indicates that the new polymorph has a higher CO2 heat of adsorption, potentially leading to improved CO2 sorption selectivity at low partial pressures.
ACS MATERIALS LETTERS
(2023)
Article
Materials Science, Multidisciplinary
Jierui Zhang, Francesco Paesani, Martina Lessio
Summary: Studies have shown that incorporating hydrophilic functional groups into the UiO-66 metal-organic framework (MOF) can improve its water uptake ability at low relative humidity (RH). This computational study provides insights into the adsorption mechanism of water in UiO-66 and its functionalized derivatives, revealing the preferential interaction sites and the formation of localized water clusters inside the octahedral pores. The presence of functional groups allows water to cluster in the pores at lower RH, making the MOF a more efficient water harvester.
JOURNAL OF MATERIALS CHEMISTRY C
(2023)