Article
Chemistry, Physical
Jiawei Zhan, Marco Govoni, Giulia Galli
Summary: Electronic structure calculations based on DFT have successfully predicted ground-state properties of molecules and materials. However, the currently used exchange and correlation functionals are often inaccurate for describing the electronic properties of heterogeneous solids. Here, we present a dielectric-dependent range-separated hybrid functional, SE-RSH, which accurately predicts the electronic structure of various nonmetallic interfaces, solids, and nanoparticles.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Subrata Jana, Hemanadhan Myneni, Szymon Smiga, Lucian A. Constantin, Prasanjit Samal
Summary: In this study, the performance of dispersion corrected revised Tao-Mo (revTM) semilocal functionals in various areas such as thermochemistry, different crystal structures, and metal-organic systems is reviewed. It is found that modifications are needed for the revTM function to adapt to the diverse properties of finite and extended systems. The revised revTM+D3 functional provides molecular and solid properties that are closer to experimental findings compared to its predecessor, making it a cost-effective method for simulations.
JOURNAL OF CHEMICAL PHYSICS
(2021)
Article
Chemistry, Physical
Thomas C. Pitts, Sofia Bousiadi, Nikitas I. Gidopoulos, Nektarios N. Lathiotakis
Summary: One way to improve the accuracy of spectral properties in density functional theory is to impose constraints on the effective local potential. This study introduces an effective screening amplitude, f, as a variational quantity, which leads to a more efficient and robust minimization problem. The proposed development is found to be an accurate and robust variant of the constrained effective potential method.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Multidisciplinary
Gang Li, Jiwei Chen, Zhaonan Yan, Shancheng Wang, Yujie Ke, Wei Luo, Huiru Ma, Jianguo Guan, Yi Long
Summary: In this study, a novel physical hydrogel-derived smart window was developed by in situ free radical polymerization of N-isopropylacrylamide (NIPAM) in a glycerol-water (GW) binary solvent system. The resulting noncovalent crosslinked PNIPAM GW solutions exhibited excellent freezing tolerance (approximately -18℃), high luminous transmittance (90%), and modulating ability (60.8% Delta T-sol), along with fast response time (approximately 10 seconds) and good structural integrity before and after phase transition.
MATERIALS HORIZONS
(2023)
Article
Physics, Multidisciplinary
Vivekanand Shukla, Yang Jiao, Jung-Hoon Lee, Elsebeth Schroeder, Jeffrey B. Neaton, Per Hyldgaard
Summary: We introduce a new general-purpose van der Waals density functional, vdW-DF2-ahbr, which combines vdW-DF2 correlation with a screened Fock exchange. It successfully resolves spurious exchange binding and density-driven errors, significantly improving the performance of existing vdW-DFs for molecular problems.
Article
Chemistry, Physical
Wenna Ai, Wei-Hai Fang, Neil Qiang Su
Summary: The short-range corrected reduced density matrix functional omega P22 is developed to utilize the advantages of functionals in KS-DFT and RDMFT without double-counting, outperforming other 1-RDM functionals in tests of thermochemistry, nonbonded interactions, and bond dissociation energy. Omega P22 shows less systematic error for systems involving fractional spins and can accurately predict the energies for different single and multiple bonds, filling a gap left by commonly used KS-DFT and RDMFT functionals.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Renxi Liu, Daye Zheng, Xinyuan Liang, Xinguo Ren, Mohan Chen, Wenfei Li
Summary: Kohn-Sham density functional theory (DFT) is widely used for electronic structure simulations, and meta-GGA functionals improve accuracy and flexibility while maintaining efficiency. The ABACUS package implements meta-GGA functionals with both numerical atomic orbitals and plane wave bases. Validation tests and calculations using SCAN, rSCAN, and r(2)SCAN functionals show satisfactory agreement with previous results and experimental values for various systems.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Alec E. Sigurdarson, Yorick L. A. Schmerwitz, Dagrun K. V. Tveiten, Gianluca Levi, Hannes Jonsson
Summary: In this study, density functional calculations were performed on several molecules to investigate their Rydberg excited states up to high energy. The results show that the generalized gradient approximation (GGA) functional of Perdew, Burke, and Ernzerhof (PBE) can accurately predict the excitation energy when combined with self-interaction correction and complex-valued orbitals. The results from the Tao, Perdew, Staroverov, and Scuseria (TPSS) and r2SCAN meta-GGA functionals did not provide a systematic improvement over the uncorrected PBE functional.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Multidisciplinary Sciences
Alexander Ryabov, Iskander Akhatov, Petr Zhilyaev
Summary: Density functional theory is a primary method for solving the many-body Schrodinger equation, and its accuracy relies on the development of exchange-correlation (XC) functional approximations. The neural network approach offers a unified approach to parametrize the XC functional by interpolating data from higher precision theories. Our developed neural network XC functional converges in the self-consistent cycle and provides reasonable energies for different systems.
SCIENTIFIC REPORTS
(2022)
Article
Chemistry, Physical
Robin Grotjahn, Filipp Furche, Martin Kaupp
Summary: For more than a decade, it has been known that the gauge variance of the kinetic energy density tau affects the magnetic orbital rotation Hessian used in linear-response time-dependent density functional theory (TDDFT). This study highlights the pronounced effects of tau-dependent exchange-correlation functionals on excitation energies, especially for the M06-2X functional and some other meta-generalized gradient approximations (mGGAs). Restoring gauge invariance significantly reduces errors in excitation energies obtained with M06-2X, indicating the importance of imposing gauge invariance for different mGGA-based functionals.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Materials Science, Multidisciplinary
C. M. Horowitz, C. R. Proetto, J. M. Pitarke
Summary: This study aims to improve the local-density approximation in density functional theory by constructing a universal exchange enhancement factor Fx. Through jellium-slab exact-exchange self-consistent calculations, we found that such an enhancement factor can be built which satisfies most exact constraints and can be applied to all electron densities.
Article
Materials Science, Multidisciplinary
Xiaofei Shao, Peitao Liu, Cesare Franchini, Yi Xia, Jiangang He
Summary: The exchange-correlation functional is crucial in describing interactions in solids and molecules. The SCAN and its derivatives, rSCAN and r2SCAN, show great promise in accurately describing various properties while maintaining computational efficiency. However, their performance in predicting finite-temperature lattice constants of solids has not been thoroughly assessed yet.
Article
Chemistry, Physical
Briana T. A. Boychuk, Stacey D. Wetmore
Summary: Understanding the structure of metal-nucleic acid systems is important for various applications. This study investigated the ability of 20 density functional theory (DFT) functionals to reproduce the crystal structure geometry of these complexes. The results showed that the reliability of functionals depends on the metal identity, and certain functionals performed well in describing the structure of a range of metal-nucleic acid systems.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Physical
Sicheng Jing, Yu Wang, Wen Chen, Jinghua Pan, Wei Li, Baoan Bian, Bin Liao
Summary: Researchers investigate the performance of 5.1 nm field-effect transistors (FETs) based on two-dimensional (2D) BP using ab initio quantum transport calculations. They use different 2D metal materials to construct van der Waals contacts in the source region, replacing conventional doping sources. The results show that FETs with Boro Delta and T-VTe2 sources with van der Waals contact exhibit superior performance.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Multidisciplinary
Kai Trepte, Johannes Voss
Summary: This paper presents an empirical approach to improve the estimation of surface chemical reaction energetics. By optimizing the exchange-correlation functional with a combination of reference data and physical model constraints, the proposed method achieves accurate predictions not only for surface chemistry simulations but also for gas phase reactions and bulk lattice constants and elastic properties.
JOURNAL OF COMPUTATIONAL CHEMISTRY
(2022)
Article
Chemistry, Physical
Carlos Mora Perez, Dibyajyoti Ghosh, Oleg Prezhdo, Wanyi Nie, Sergei Tretiak, Amanda Neukirch
Summary: This study investigates the impact of defects on the ground state electronic structure of two-dimensional RP halide perovskites. The research reveals that neutral-type point defects have limited influence on the electronic structure, while donor/acceptor defects introduce deep midgap states that can harm the material's electronic performance. Avoiding halide vacancies and interstitial defects is crucial to maintain positive intrinsic properties and improve device performance in 2D halide perovskite-based applications.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Physical
Shahriar N. Khan, Braden M. Weight, Brendan J. Gifford, Sergei Tretiak, Alan Bishop
Summary: The optoelectronic properties of functionalized graphene quantum dots were studied by simulating different shapes and types of functionalization. The results showed that the functionalization position and edge shape played important roles in the optical properties. The isomers with CH2 in the intermediate positions showed higher electronic transition energies and exciton delocalization. Complete passivation of rhombic GQDs resulted in the largest structural deformation and strongest red-shift. The substituents F, CH3, Cl, and Br caused a steady red-shift in the absorption energy, suggesting the dominance of steric effects.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Chemistry, Multidisciplinary
Luo Yan, Jiaojiao Zhu, Bao-Tian Wang, Junjie He, Hai-Zhi Song, Weibin Chu, Sergei Tretiak, Liujiang Zhou
Summary: The study reports the discovery of two-dimensional transition metal oxide materials beyond the MXene family, which exhibit superconducting, semiconducting, and light-harvesting properties. This expands the understanding of emerging phenomena in this field and provides a new platform for optoelectronic and photovoltaic applications.
Article
Multidisciplinary Sciences
Yu Zheng, Yulun Han, Braden M. Weight, Zhiwei Lin, Brendan J. Gifford, Ming Zheng, Dmitri Kilin, Svetlana Kilina, Stephen K. Doorn, Han Htoon, Sergei Tretiak
Summary: By controlling the morphology of the emitting sites, spin-selective photochemistry diversifies the tunability of carbon nanotube emission.
NATURE COMMUNICATIONS
(2022)
Article
Quantum Science & Technology
Yu Zhang, Lukasz Cincio, Christian F. A. Negre, Piotr Czarnik, Patrick J. Coles, Petr M. Anisimov, Susan M. Mniszewski, Sergei Tretiak, Pavel A. Dub
Summary: This study presents an approach to reduce quantum circuit complexity for electronic structure calculations. The method divides the qubit space into clusters and connects them using a new dressed Hamiltonian, enabling accurate simulation with fewer resources.
NPJ QUANTUM INFORMATION
(2022)
Article
Chemistry, Multidisciplinary
Hsinhan Tsai, Dibyajyoti Ghosh, Eli Kinigstein, Bogdan Dryzhakov, Honora Driscoll, Magdalena Owczarek, Bin Hu, Xiaoyi Zhang, Sergei Tretiak, Wanyi Nie
Summary: The dynamic structure changes in metal halide perovskite lattice upon photoexcitation and its impact on carrier transport properties in Ruddlesden-Popper phase perovskite thin films are reported in this study. Time-resolved X-ray scattering technique reveals rapid lattice expansion and slow relaxation over 100 ns after photoexcitation. The expansion is attributed to lattice thermal fluctuations caused by photon energy deposition. High laser powers induce strong local structural disorder, increasing the charge dissociation activation energy and leading to localized transport.
Article
Mechanics
M. Serrano, K. Larkin, M. Ghommem, S. Tretiak, A. Abdelkefi
Summary: A multi-purpose energy harvesting microgyroscope system based on piezoelectric materials is proposed for small devices in remote areas. Numerical analysis shows that a system with a non-symmetric beam design is suitable for broadband energy harvesting. The nonlinear softening effects create a broadband frequency response with high voltage output, but careful selection of DC and AC voltages is necessary to avoid dynamic pull-in.
EUROPEAN JOURNAL OF MECHANICS A-SOLIDS
(2023)
Article
Mechanics
M. Serrano, K. Larkin, S. Tretiak, A. Abdelkefi
Summary: Most microelectromechanical systems (MEMS) are made from brittle materials that are prone to cracking. Understanding the potential influences cracks in MEMS is necessary for the longevity of these systems. This study developed an electromechanical model to capture the impacts of cracks on the performance of a damaged energy harvesting microgyroscope, and numerical methods were used to approximate the damage associated with distributed crack networks. The study revealed that cracks can significantly affect the static and dynamic behaviors of the microgyroscope energy harvester.
EUROPEAN JOURNAL OF MECHANICS A-SOLIDS
(2023)
Article
Chemistry, Physical
Hassiel Negrin-Yuvero, Victor M. Freixas, Dianelys Ondarse-Alvarez, Ana E. Ledesma, Sergei Tretiak, Sebastian Fernandez-Alberti
Summary: The photoexcitation, energy relaxation, and redistribution of a recently synthesized zigzag carbon nanobelt were studied using molecular dynamics simulations. The transition dipole moments and electronic transition density were found to gradually change during the internal conversion process. The electronic relaxation involved long-lived states with large energy gaps and changes in symmetry. These results provide insights into the excited-state properties of the zigzag nanobelt and can inspire the design of tailored nanobelts for specific nanoelectronic and photonic applications.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Chintam Hanmandlu, Rohan Paste, Hsinhan Tsai, Shyam Narayan Singh Yadav, Kuan-Wen Lai, Yen-Yu Wang, Chandra Shekar Gantepogu, Chen-Hung Hou, Jing-Jong Shyue, Yu-Jung Lu, Tushar Sanjay Jadhav, Jian-Ming Liao, Hsien-Hsin Chou, Hui Qi Wong, Chao-Sung Lai, Dibyajyoti Ghosh, Sergei Tretiak, Ta-Jen Yen, Hung-Ju Yen, Chih-Wei Chu
Summary: This study used a holistic interface strategy to enhance the efficiency and stability of perovskite solar cells by decreasing the number of interfacial defect states. The researchers utilized three-dimensional triphenylamine-based nanographene precursors to form a bridge between the perovskite film and the hole transport layer, resulting in improved performance characteristics.
Article
Chemistry, Physical
Hassiel Negrin-Yuvero, Victor M. Freixas, Dianelys Ondarse-Alvarez, Ana E. Ledesma, Sergei Tretiak, Sebastian Fernandez-Alberti
Summary: Progress in the synthesis of new carbon nanorings and nanobelts broadens the library of materials with unique structural and optical properties that can be attractive for further potential applications in host-guest chemistry, nanoelectronics, and photonics. In this study, we investigate the photoexcitation and subsequent energy relaxation and redistribution of a recently synthesized zigzag carbon nanobelt using nonadiabatic excited state molecular dynamics simulations. Our results reveal the excited-state dynamical properties of the zigzag-type nanobelt that differentiate this molecule from other nanobelts, providing insights for further designs tailored for specific nanoelectronic and photonic applications.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Multidisciplinary Sciences
Guoqing Zhou, Nicholas Lubbers, Kipton Barros, Sergei Tretiak, Benjamin Nebgen
Summary: Conventional machine learning models in computational chemistry predict molecular properties using quantum chemistry, but their accuracy degrades on larger or newer chemical systems. Incorporating quantum chemistry frameworks into machine learning models improves accuracy. This study demonstrates accurate prediction of various molecular properties on larger chemical systems by using machine-learned dynamic values in semiempirical quantum mechanics.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2022)
Article
Chemistry, Physical
Laura Alfonso Hernandez, Victor M. Freixas, Beatriz Rodriguez-Hernandez, Sergei Tretiak, Sebastian Fernandez-Alberti, Nicolas Oldani
Summary: The effect of introducing a satellite tetraphenyl substitution on the structural and dynamical properties of cycloparaphenylene is studied. The results show that the substitution accelerates the electronic relaxation and induces efficient inter-band energy transfer and exciton self-trapping.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Aaron Forde, Victor M. Freixas, Sebastian Fernandez-Alberti, Amanda J. Neukirch, Sergei Tretiak
Summary: This article investigates a novel donor-acceptor molecular complex with dual fluorescence properties for charge transfer. Using time-dependent density functional theory, the alignment of excitonic and charge-transfer states is characterized, and the results are in agreement with experimental observations. This work is important for understanding and utilizing charge transfer processes.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Materials Science, Multidisciplinary
Dibyajyoti Ghosh, Carlos Mora Perez, Oleg Prezhdo, Wanyi Nie, Sergei Tretiak, Amanda J. Neukirch
Summary: Mixed A-cation halide perovskites have shown great potential for next-generation optoelectronic applications due to their attractive charge carrier transport properties and enhanced stability. In this study, we investigate the influence of A-cation mixing on the relaxation processes of hot charge carriers in FA(1-x)Cs(x)PbI(3) materials using nonadiabatic molecular dynamics and time-domain density functional theory methods. Our results demonstrate that the partial substitution of organic FA species with inorganic Cs cations significantly extends the relaxation times of hot electrons and hot holes. The understanding of the relationship between the dynamic structure and carrier relaxation allows us to propose rational design principles for enhancing the hot carrier lifetimes in photoactive materials.
JOURNAL OF MATERIALS CHEMISTRY C
(2022)