The prediction of material properties based on density-functional theory has become routinely common, thanks, in part, to the steady increase in the number and robustness of available simulation packages. This plurality of codes and methods is both a boon and a burden. While providing great opportunities for cross-verification, these packages adopt...
S.P. Huber, E. Bosoni, M. Bercx, et al. Common workflows for computing material properties using different quantum engines. npj Comput Mater 7, 136 (2021).
© 2021, The Author(s)
The Open Databases Integration for Materials Design (OPTIMADE) consortium has designed a universal application programming interface (API) to make materials databases accessible and interoperable. We outline the first stable release of the specification, v1.0, which is already supported by many leading databases and several software packages....
C.W.Andersen, R. Armiento, E. Blokhin et al. OPTIMADE, an API for exchanging materials data. Sci Data 8, 217 (2021).
© 2021, The Author(s)
Layered materials (LMs), such as graphite, hexagonal boron nitride, and transition-metal dichalcogenides, are at the center of an ever-increasing research effort, due to their scientific and technological relevance. Raman and infrared spectroscopies are accurate, non-destructive approaches to determine a wide range of properties, including the numb...
G. Pizzi, S. Milana, A. C. Ferrari, N. Marzari, and M. Gibertini. Shear and Breathing Modes of Layered Materials. ACS Nano 2021, 15, 8, 12509–12534
© 2021 The Authors
Spontaneous condensation of excitons is a long-sought phenomenon analogous to the condensation of Cooper pairs in a superconductor. It is expected to occur in a semiconductor at thermodynamic equilibrium if the binding energy of the excitons—electron (e) and hole (h) pairs interacting by Coulomb force—overcomes the band gap, giving rise to a new ph...
S. S. Ataei, D. Varsano, E. Molinari, and M. Rontani. Evidence of ideal excitonic insulator in bulk MoS2 under pressure. PNAS March 30, 2021 118 (13) e2010110118
Cloud platforms allow users to execute tasks directly from their web browser and are a key enabling technology not only for commerce but also for computational science. Research software is often developed by scientists with limited experience in (and time for) user interface design, which can make research software...
A.V. Yakutovic, K. Eimre, O. Schütt, L. Talirz, C.S. Adorf, C.W. Andersen, E. Ditler, D. Du, D. Passerone, B. Smit, N. Marzari, G. Pizzi and C.A. Pignedoli, AiiDAlab – an ecosystem for developing, executing, and sharing scientific workflows, Computational Materials Science 188, 110165 (2021)
© 2020 The Authors
Even the best quality 2D materials have non‐negligible concentrations of vacancies and impurities. It is critical to understand and quantify how defects change intrinsic properties, and use this knowledge to generate functionality. This challenge can be addressed by employing many‐body perturbation theory to obtain the optical...
P. M. M. C. de Melo, Z. Zanolli and M.J. Verstraete, Optical Signatures of Defect Centers in Transition Metal Dichalcogenide Monolayers, Advanced Quantum Technologies, 202000118 (2020)
© The Authors
The structures of the ion-pairs formed in aqueous NaOH and LiOH solutions are elucidated by combining Raman multivariate curve resolution (Raman-MCR) experiments and ab initio molecular dynamics (AIMD) simulations. The results extend prior findings to reveal that the initially formed ion-pairs are predominantly water-shared, with the hydroxide ion ...
D. Mendes de Oliveira, A. J. Bredt, T. C. Miller, S. A. Corcelli, and D. Ben-Amotz. Spectroscopic and Structural Characterization of Water-Shared Ion-Pairs in Aqueous Sodium and Lithium Hydroxide. The Journal of Physical Chemistry B 2021 125 (5), 1439-1446
© 2021 American Chemical Society
Vibrational sum-frequency generation (vSFG) spectroscopy allows the study of the structure and dynamics of interfacial systems. In the present work, we provide a simple recipe, based on a narrowband IR pump and broadband vSFG probe technique, to computationally obtain the two-dimensional vSFG spectrum of water molecules at the air–water interface. ...
D. Ojha, T.D. Kühne. Hydrogen bond dynamics of interfacial water molecules revealed from two-dimensional vibrational sum-frequency generation spectroscopy. Sci Rep 11, 2456 (2021)
© The Authors
We investigate a well defined heterostructure constituted by magnetic Fe layers sandwiched between graphene (Gr) and Ir(111). The challenging task to avoid Fe-C solubility and Fe-Ir intermixing has been achieved with atomic controlled Fe intercalation at moderate temperature below 500 K...
C. Cardoso, G. Avvisati, P. Gargiani, M. Sbroscia, M.S. Jagadeesh, C. Mariani, D.A. Leon Valido, D. Varsano, A. Ferretti, and M.G. Betti, Magnetic response and electronic states of well defined Graphene/Fe/Ir(111) heterostructure, Phys. Rev. Materials 5, 014405 (2020)
©2020 American Physical Society
A moiré superlattice formed by stacking two lattice mismatched transition metal dichalcogenide monolayers, functions as a diffusion barrier that affects the energy transport and dynamics of interlayer excitons (electron and hole spatially concentrated in different monolayers). In this work, we experimentally quantify the diffusion barrier experienc...
Z. Li, X. Lu, D. F. Cordovilla Leon, Z. Lyu, H. Xie, J. Hou, Y. Lu, X. Guo, A. Kaczmarek, T. Taniguchi, K. Watanabe, L. Zhao, L. Yang, and P. B. Deotare. Interlayer Exciton Transport in MoSe2/WSe2 Heterostructures. ACS Nano 2021 15 (1), 1539-1547
© 2021 American Chemical Society
The discovery of building blocks offers new opportunities to develop and control properties of extended solids. Compounds with fluorite-type Bi2O2 blocks host various properties including lead-free ferroelectrics and photocatalysts. In this study, we show that triple-layered Bi2MO4 blocks (M = Bi, La, Y) in Bi2MO4Cl allow, unlike double-layered Bi2...
A. Nakada, D. Kato, R. Nelson, H. Takahira, M. Yabuuchi, M. Higashi, H. Suzuki, M. Kirsanova, N. Kakudou, C. Tassel, T. Yamamoto, C. M. Brown, R. Dronskowski, A. Saeki, A. Abakumov, H. Kageyama, and R. Abe. Conduction Band Control of Oxyhalides with a Triple-Fluorite Layer for Visible Light Photocatalysis. Journal of the American Chemical Society 2021 143 (6), 2491-2499
© 2021 American Chemical Society
The physical and chemical properties of MXenes are strongly dependent on surface terminations; thus, the tailoring of surface functional groups in two-dimensional transition-metal carbides (MXenes) may extend the applicability of these compelling materials to a wider set of fields. In this work, we demonstrate the chemical modification of Ti3C2Tx M...
H. Jing, H. Yeo, B. Lyu, J. Ryou, S. Choi, J-H Park, B. Hun Lee, Y-H Kim, and S. Lee. Modulation of the Electronic Properties of MXene (Ti3C2Tx) via Surface-Covalent Functionalization with Diazonium. ACS Nano 2021 15 (1), 1388-1396
© 2021 American Chemical Society
Using accurate dissipative DFT-NEGF atomistic-simulation techniques within the Wannier-Function formalism, we give a fresh look at the possibility of sub-10-nm scaling for high-performance complementary metal oxide semiconductor (CMOS) applications. We show that a combination of good electrostatic control together with high mobility is paramount to...
A. Afzalian. Ab initio perspective of ultra-scaled CMOS from 2D-material fundamentals to dynamically doped transistors. npj 2D Mater Appl 5, 5 (2021)
© The Authors
PbS quantum dots and nanoplatelets (NPLs) are of enormous interest in the development of optoelectronic devices. However, some important aspects of their nature remain unclear. Recent studies have revealed that colloidal PbS NPLs may depart from the rock-salt crystal structure of bulk and form an orthorhombic (Pnma) modification instead. To gain in...
D. F. Macias-Pinilla, C. Echeverría-Arrondo, A. F. Gualdrón Reyes, S. Agouram, V. Muñoz-Sanjosé, J. Planelles, I. Mora-Seró, and J. I. Climente. Morphology and Band Structure of Orthorhombic PbS Nanoplatelets: An Indirect Band Gap Material. Chemistry of Materials 2021 33 (1), 420-429
© 2021 American Chemical Society
We calculate the time evolution of the transient reflection signal in an MoS2 monolayer on a SiO2/Si substrate using first-principles out-of-equilibrium real-time methods. Our simulations provide a simple and intuitive physical picture for the delayed, yet ultrafast, evolution of the signal whose rise...
V. Smejkal, F. Libisch, A. Molina-Sanchez, L. Wirtz, and A. Marini. Time-dependent screening explains the ultrafast excitonic signal rise in 2D semiconductors. ACS Nano 15, 1, 1179–1185 (2021)
© 2020 American Chemical Society
We implement the Bogoliubov-de Gennes (BdG) equation in real-space using the screened Korringa-Kohn-Rostoker (KKR) method. This allows us to solve, self-consistently, the superconducting state for 3D crystals including substitutional impurities with a full normal-state DFT band structure. We apply...
T.G. Saunderson, Z. Győrgypál, J.F. Annett, G. Csire, B. Újfalussy, and M. Gradhand. Real-space multiple scattering theory for superconductors with impurities. Phys. Rev. B 102, 245106 (2020)
©2020 American Physical Society
We propose a computationally efficient Kerker mixing scheme for robust and rapidly converging self-consistent-field calculations using all-electron first-principles electronic structure methods based on the muffin-tin partitioning of space. The mixing scheme is composed of the Kerker preconditioner...
M. Winkelmann, E. Di Napoli, D. Wortmann, and S. Blügel. Kerker mixing scheme for self-consistent muffin-tin based all-electron electronic structure calculations. Phys. Rev. B 102, 195138 (2020)
©2020 American Physical Society
Over the last two decades, the field of computational science has seen a dramatic shift towards incorporating high-throughput computation and big-data analysis as fundamental pillars of the scientific discovery process. This has necessitated the development of tools and techniques to deal with the generation, storage...
M. Uhrin, S. P. Huber, J. Yu, N. Marzari, G. Pizzi. Workflows in AiiDA: Engineering a high-throughput, event-based engine for robust and modular computational workflows. Computational Materials Science, 187 (2021)
© 1969, Elsevier
Thouless’ quantization of adiabatic particle transport permits one to associate an integer topological charge with each atom of an electronically gapped material. If these charges are additive and independent of atomic positions, they provide a rigorous definition of atomic oxidation states and atoms...
P. Pegolo, F. Grasselli and S. Baroni. Oxidation States, Thouless’ Pumps, and Nontrivial Ionic Transport in Nonstoichiometric Electrolytes. Phys. Rev. X 10, 041031 (2020)
©2020 American Physical Society
The power consumption of supercomputers is a major challenge for system owners, users, and society. It limits the capacity of system installations, it requires large cooling infrastructures, and it is the cause of a large carbon footprint. Reducing power during application execution without changing...
D. Cesarini, A. Bartolini, A. Borghesi, C. Cavazzoni, M. Luisier and L. Benini, Countdown Slack: A Run-Time Library to Reduce Energy Footprint in Large-Scale MPI Applications. IEEE Transactions on Parallel and Distributed Systems 31, 11 (2020)
© 2020 IEEE
We combine density functional theory and many body perturbation theory to investigate the electronic properties of Si(100) and Ge(100) surfaces terminated with halogen atoms (–I, –Br, –Cl, –F) and other chemical functionalizations (–H, –OH, –CH3) addressing the absolute values of their work function...
I. Marri, M. Amato, M. Bertocchi, A. Ferretti, D. Varsano and S. Ossicini. Surface chemistry effects on work function, ionization potential and electronic affinity of Si(100), Ge(100) surfaces and SiGe heterostructure. Phys. Chem. Chem. Phys. 22 (2020)
© the Owner Societies 2020
Chemical reactions that convert sp2 to sp3 hybridization have been demonstrated to be a fascinating yet challenging route to functionalize graphene. So far it has not been possible to precisely control the reaction sites nor their lateral order at the atomic/molecular scale...
Yu, M., Chen, C., Liu, Q. et al. Long-range ordered and atomic-scale control of graphene hybridization by photocycloaddition. Nat. Chem. 12 (2020)
© 2020, The Author(s), under exclusive licence to Springer Nature Limit
Mixtures of cations or halides with FAPbI3 (where FA is formamidinium) lead to high efficiency in perovskite solar cells (PSCs) but also to blue-shifted absorption and long-term stability issues caused by loss of volatile methylammonium (MA) and phase segregation. We report a deposition method using MA thiocyanate (MASCN)...
H. Lu, Y. Liu, P. Ahlawat, A. Mishra, W. R. Tress, F. T. Eickemeyer, Y. Yang, F. Fu, Z. Wang, C. E. Avalos, B. I. Carlsen, A. Agarwalla, X. Zhang, X. Li, Y. Zhan, S. M. Zakeeruddin, L. Emsley, U. Rothlisberger, L. Zheng, A. Hagfeldt, M. Grätzel. Vapor-assisted deposition of highly efficient, stable black-phase FAPbI3 perovskite solar cells. Science 370, 6512 (2020)
© 2020 The Authors
We present a real-time ab initio description of optical orientation in bulk GaAs due to the coupling with an ultrashort circularly polarized laser source. The injection of spin-polarized electrons in the conduction band is correctly reproduced, and a nonvanishing spin polarization P parallel to the direction of...
M. D'Alessandro and D. Sangalli. Real-time modeling of optical orientation in GaAs: Generation and decay of the degree of spin polarization. Phys. Rev. B 102, 10 (2020)
©2020 American Physical Society
Antiferromagnetically coupled magnetic skyrmions are considered ideal candidates for high-density information carriers. This is due to the suppressed skyrmion Hall effect compared to conventional skyrmions and a smaller size due to the cancellation of some contributions to the magnetostatic dipolar fields...
H. Jia, B. Zimmermann, M. Hoffmann, M. Sallermann, G. Bihlmayer, and S. Blügel. Material systems for FM-/AFM-coupled skyrmions in Co/Pt-based multilayers. Phys. Rev. Materials 4, 094407 (2020)
©2020 American Physical Society
The ever-growing availability of computing power and the sustained development of advanced computational methods have contributed much to recent scientific progress. These developments present new challenges driven by the sheer amount of calculations and data to manage. Next-generation exascale supercomputers will harden these challenges, such that...
S. P. Huber, S. Zoupanos, M. Uhrin, L. Talirz, L. Kahle, R. Häuselmann, D. Gresch, T. Müller, A. V. Yakutovich, C. W. Andersen, F. F. Ramirez, C. S. Adorf, F. Gargiulo, S. Kumbhar, E. Passaro, C. Johnston, A. Merkys, A. Cepellotti, N. Mounet, N. Marzari, B. Kozinsky, and G. Pizzi. AiiDA 1.0, a scalable computational infrastructure for automated reproducible workflows and data provenance. Sci Data 7, 300 (2020)
© 2020, The Author(s)
https://doi.org/10.1038/s41597-020-00638-4
Materials Cloud is a platform designed to enable open and seamless sharing of resources for computational science, driven by applications in materials modelling. It hosts (1) archival and dissemination services for raw and curated data, together with their provenance graph, (2) modelling services and virtual machines, (3) tools for data analytics, ...
L. Talirz, .l Kumbhar, E. Passaro, A. V. Yakutovich, V. Granata, F. Gargiulo, M. Borelli, M. Uhrin, S. P. Huber, S. Zoupanos, C. S. Adorf, C. W. Andersen, O. Schütt, C. A. Pignedoli, D. Passerone, J. VandeVondele, T.C. Schulthess, B. Smit, G. Pizzi, and N. Marzari. Materials Cloud, a platform for open computational science. Sci Data 7, 299 (2020)
© 2020, The Author(s)
https://doi.org/10.1038/s41597-020-00637-5
Electrosorption of solvated species at metal electrodes is a most fundamental class of processes in interfacial electrochemistry. Here, we use its sensitive dependence on the electric double layer to assess the performance of ab initio thermodynamics approaches increasingly used for the first-principles description of electrocatalysis. We show anal...
N.G. Hörmann, N. Marzari, N. and K. Reuter. Electrosorption at metal surfaces from first principles. npj Comput Mater 6, 136 (2020).
© 2020, The Author(s)
Bottom-up approaches exploiting on-surface synthesis reactions allow atomic-scale precision in the fabrication of graphene nanoribbons (GNRs); this is essential for their technological applications since their unique electronic and optical properties are largely controlled by the specific edge structure. By means of a combined experimental-theoreti...
N. Cavani, M. De Corato, A. Ruini, D. Prezzi, E. Molinari, A. Lodi Rizzini, A. Rosi, R. Biagi, V. Corradini, X.-Y. Wang, X. Feng, A. Narita, K. Muellen, and V. De Renzi. Vibrational signature of the graphene nanoribbon edge structure from high-resolution electron energy-loss spectroscopy. Nanoscale 12 (2020)
© The Royal Society of Chemistry 2020
https://doi.org/10.1039/D0NR05763K
Electron-phonon interactions are key to understanding the dynamics of electrons in materials and can be modeled accurately from first principles. However, when electrons and holes form Coulomb-bound states (excitons), quantifying their interactions and scattering processes with phonons remains an open challenge. Here we show a rigorous approach for...
H. Chen, D. Sangalli, M. Bernardi. Exciton-Phonon Interaction and Relaxation Times from First Principles. Phys. Rev. Lett. 125, 107401 (2020)
© 2020 American Physical Society
https://doi.org/10.1103/PhysRevLett.125.107401
Understanding the electronic energy landscape in metal halide perovskites is essential for further improvements in their promising performance in thin-film photovoltaics. Here, we uncover the presence of above-bandgap oscillatory features in the absorption spectra of formamidinium lead triiodide thin films. We attribute these discrete features to i...
A.D. Wright, G. Volonakis, J. Borchert, et al. Intrinsic quantum confinement in formamidinium lead triiodide perovskite. Nat. Mater. 19, 1201–1206 (2020).
© 2020, The Author(s)
https://doi.org/10.1038/s41563-020-0774-9
The nonequilibrium excitonic insulator (NEQ-EI) is an excited state of matter characterized by a finite density of coherent excitons and a time-dependent macroscopic polarization. The stability of this exciton superfluid as the density grows is jeopardized by the increased screening efficiency of the looser excitons. In this work we put forward a H...
E. Perfetto, A. Marini, G. Stefanucci. Self-consistent screening enhances stability of the nonequilibrium excitonic insulator phase. Phys. Rev. B 102, 085203 (2020)
©2020 American Physical Society
https://doi.org/10.1103/PhysRevB.102.085203
Time-resolved soft-x-ray photoemission spectroscopy is used to simultaneously measure the ultrafast dynamics of core-level spectral functions and excited states upon excitation of excitons in WSe2. We present a many-body approximation for the Green’s function, which excellently describes the transient core-hole spectral function. The relative dynam...
M. Dendzik, R. P. Xian, E. Perfetto, D. Sangalli, D. Kutnyakhov, S. Dong, S. Beaulieu, T. Pincelli, F. Pressacco, D. Curcio, S. Y. Agustsson, M. Heber, J. Hauer, W. Wurth, G. Brenner, Y. Acremann, P. Hofmann, M. Wolf, A. Marini, G. Stefanucci, L. Rettig, and R. Ernstorfer. Observation of an Excitonic Mott Transition through Ultrafast Core-cum-Conduction Photoemission Spectroscopy. Phys. Rev. B 102, 085203 (2020)
© 2020 The Authors
https://doi.org/10.1103/PhysRevB.102.085203
We present an ab initio computational approach for the calculation of resonant Raman intensities, including both excitonic and nonadiabatic effects. Our diagrammatic approach, which we apply to two prototype, semiconducting layered materials, allows a detailed analysis of the impact of phonon-mediated exciton-exciton scattering on the intensities. ...
S. Reichardt and L. Wirtz. Nonadiabatic exciton-phonon coupling in Raman spectroscopy of layered materials. Science Advances 6 eabb5915 (2020)
© 2020 The Authors
https://doi.org/10.1126/sciadv.abb5915
The implementation of ultrasoft pseudopotentials into time-dependent density-functional perturbation theory is detailed for both the Sternheimer approach and the Liouville-Lanczos (LL) method, and equations are presented in the scalar relativistic approximation for periodic solids with finite momentum transfer q. The LL method is applied to calcula...
O. Motornyi, N. Vast, I. Timrov, O. Baseggio, S. Baroni, and A. Dal Corso. Electron energy loss spectroscopy of bulk gold with ultrasoft pseudopotentials and the Liouville-Lanczos method. Phys. Rev. B 102, 3 (2020)
©2020 American Physical Society
The impact of the inner structure and thermal history of planets on their observable features, such as luminosity or magnetic field, crucially depends on the poorly known heat and charge transport properties of their internal layers. The thermal and electric conductivities of dif- ferent phases of water (liquid, solid, and super-ionic) occurring in...
F. Grasselli, L. Stixrude, and S. Baroni. Heat and charge transport in H2O at ice-giant conditions from ab initio MD simulations. Nat Commun 11, 3605 (2020)
© 2020, The Author(s)
https://doi.org/10.1038/s41467-020-17275-5
Suppressing coke deposition over reduced oxygen carriers, the key to breaking competing effects between oxygen supply and methane-to-syngas selectivity, is an important but challenging task for chemical looping partial oxidation technology. We report that A-site engineering of La1–xSrxFe0.8Al0.2O3 oxides significantly adjusts the oxygen capacity, w...
L. Zhang, W. Xu, J. Wu, Y. Hu, C. Huang, Y. Zhu, M. Tian, Y. Kang, X. Pan, Y. Su, J. Wang, X. Wang. Identifying the Role of A-Site Cations in Modulating Oxygen Capacity of Iron-Based Perovskite for Enhanced Chemical Looping Methane-to-Syngas Conversion. ACS Catal. 10, 16 (2020)
© 2020 American Chemical Society
https://doi.org/10.1021/acscatal.0c01811
Conversion-type transition-metal phosphide anode materials with high theoretical capacity usually suffer from low-rate capability and severe capacity decay, which are mainly caused by their inferior electronic conductivities and large volumetric variations together with the poor reversibility of discharge product (Li3P), impeding their practical ap...
Z.M. Zheng, H.H. Wu, H.D. Liu, Q.B. Zhang, X. He, S.C. Yu, V. Petrova, J. Feng, R. Kostecki, P. Liu, D.L. Peng, M.L. Liu, M.S. Wang. Achieving Fast and Durable Lithium Storage through Amorphous FeP Nanoparticles Encapsulated in Ultrathin 3D P-Doped Porous Carbon Nanosheets. ACS Nano, 14, 8, 9545–9561 (2020)
© 2020 American Chemical Society
https://doi.org/10.1021/acsnano.9b08575
The methanol-to-hydrocarbon process is known to proceed autocatalytically in H-ZSM-5 after an induction period where framework methoxy species are formed. In this work, we provide mechanistic insight into the framework methylation within H-ZSM-5 at high methanol loadings and varying acid site densities by means of first-principles molecular dynamic...
S. A. F. Nastase, P. Cnudde, L. Vanduyfhuys, K. De Wispelaere, V. Van Speybroeck, C. R. A. Catlow, and A. J. Logsdail. Mechanistic Insight into the Framework Methylation of H-ZSM-5 for Varying Methanol Loadings and Si/Al Ratios Using First-Principles Molecular Dynamics Simulations. ACS Catalysis 10, 15 (2020)
© 2020 American Chemical Society
https://doi.org/10.1021/acscatal.0c01454
Interlayer interaction could substantially affect the electrical transport in transition metal dichalcogenides, serving as an effective way to control the device performance. However, it is still challenging to utilize interlayer interaction in weakly interlayer-coupled materials such as pristine MoS2 to realize layer-dependent tunable transport be...
L. Zhang, G. Wang, Y. Zhang, Z. Cao, Y. Wang, T. Cao, C. Wang, B. Cheng, W. Zhang, X. Wan, J. Lin, S.-J. Liang, and F. Miao. Tuning Electrical Conductance in Bilayer MoS2 through Defect-Mediated Interlayer Chemical Bonding. ACS Nano 14, 8 (2020)
© 2020 American Chemical Society
https://doi.org/10.1021/acsnano.0c03665
We present the theory and the application of a first-principle transport model employing a basis set obtained directly from the ab initio Bloch functions. We use a plane-wave density functional theory Hamiltonian and show that a judicious choice of the reduced basis set can effectively suppress the potentially thorny problem of the unphysical solut...
M. G. Pala, P. Giannozzi, and D. Esseni. Unit cell restricted Bloch functions basis for first-principle transport models: Theory and application. Phys. Rev. B 102, 045410 (2020)
©2020 American Physical Society
https://doi.org/10.1103/PhysRevB.102.045410
Grain boundaries (GBs) are ubiquitous in solids and have been of central importance in understanding the nature of polycrystals. In addition to their classical roles, topological insulators (TIs) offer a chance to realize GBs hosting distinct topological states that can be controlled by their crystal symmetries. However, such roles of crystalline s...
H. W. Kim, S.-H. Kang, H.-J. Kim, K. Chae, S. Cho, W. Ko, S. Jeon, S. Hwang Kang, H. Yang, S. Wng Kim, S. Park, S. Hwang, Y.-K. Kwon, and Y.-W. Son. Symmetry Dictated Grain Boundary State in a Two-Dimensional Topological Insulator. Nano Letters 20, 8 (2020)
© 2020 American Chemical Society
While the Landauer viewpoint constitutes a modern basis to understand nanoscale electronic transport and to realize first‐principles implementations of the nonequilibrium Green's function (NEGF) formalism, seeking an alternative picture can be beneficial for the fundamental understanding and practical calculations of quantum transport processes. He...
J. Lee, H. Seul Kim, Y.‐H. Kim Multi‐Space Excitation as an Alternative to the Landauer Picture for Nonequilibrium Quantum Transport. Advanced Science 7, 16 (2020)
© 2020 The Authors
https://doi.org/10.1002/advs.202001038
Routine applications of electronic structure theory to molecules and periodic systems need to compute the electron density from given Hamiltonian and, in case of non-orthogonal basis sets, overlap matrices. System sizes can range from few to thousands or, in some examples, millions of atoms. Different discretization schemes (basis sets) and differe...
V. Wen-zhe Yu, C. Campos, W. Dawson, A. García, V. Havu, B. Hourahine, W. P Huhn, M. Jacquelin, W. Jia, M. Keçeli, R. Laasner, Y. Li, Lin Lin, J. Lu, J. Moussa, J. E Roman, Á. Vázquez-Mayagoitia, C. Yang, V. Blum. ELSI -- An Open Infrastructure for Electronic Structure Solvers. Comp. Phys. Comm. 256 (2020)
© 2020 Elsevier B.V. All rights reserved.
https://doi.org/10.1016/j.cpc.2020.107459
Charge density waves have been intensely studied in inorganic materials such as transition metal dichalcogenides; however their counterpart in organic materials has yet to be explored in detail. Here we report the finding of robust two-dimensional charge density waves in molecular layers formed by α-(BEDT-TTF)2–I3 on a Ag(111) surface. Low-temperat...
K. Zin Latt, J. A. Schlueter, P. Darancet, and S.-W. Hla. Two-Dimensional Molecular Charge Density Waves in Single-Layer-Thick Islands of a Dirac Fermion System. ACS Nano 14, 7 (2020)
© 2020 American Chemical Society
Liquid ammonia is unusual in its capacity to host electrons in stable solution, with vivid blue and bronze colors signifying the low- and high-concentration regimes, respectively. Buttersack et al. used photoelectron spectroscopy and accompanying theoretical simulations to track the precise energetic changes that ensued as steadily rising quantitie...
T. Buttersack, P.E. Mason, R.S. McMullen, H.C. Schewe, T. Martinek, K. Brezina, M. Crhan, A. Gomez, D. Hein, G. Wartner, R. Seidel, H. Ali, S. Thürmer, O. Marsalek, B. Winter, S.E. Bradforth, P. Jungwirth. Photoelectron spectra of alkali metal–ammonia microjets: From blue electrolyte to bronze metal Science 368 (2020)
© 2020 The Authors
Two-dimensional van der Waals heterojunctions (2D-vdWHs) stacked from atomically thick 2D materials are predicted to be a diverse class of electronic materials with unique electronic properties. These properties can be further tuned by sandwiching monolayers of planar organic molecules between 2D materials to form molecular 2D-vdWHs (M-2D-vdWHs), i...
S. Zhao, Q. Wu, J. Pi, J. Liu, J. Zheng, S. Hou, J. Wei, R. Li, H. Sadeghi, Y. Yang, J. Shi, Z. Chen, Z. Xiao, C. Lambert, W. Hong. Cross-plane transport in a single-molecule two-dimensional van der Waals heterojunction. Science Advances 6, 22 (2020)
© 2020 The Authors
https://doi.org/10.1126/sciadv.aba6714
Current polymeric transfer methods of 2D materials often bring about the presence of wrinkles, cracks, and polymer residue, limiting the quality of the transferred materials and performance of devices. Herein, we report a transfer approach combining pretreatment by liquid nitrogen and lithium ion intercalation with polymer composite of small molecu...
P. Wang, S. Song, A. Najafi, C. Huai, P. Zhang, Y. Hou, S. Huang, and H. Zeng. High-Fidelity Transfer of Chemical Vapor Deposition Grown 2D Transition Metal Dichalcogenides via Substrate Decoupling and Polymer/Small Molecule Composite. ACS Nano 14, 6 (2020)
© 2020 American Chemical Society
Chromium trihalides (CrI3, CrBr3 and CrCl3) form a prominent family of isostructural insulating layered materials in which ferromagnetic order has been observed down to the monolayer. Here we provide a comprehensive computational study of magneto-optical properties that are used as probes for the monolayer ferromagnetic order: magnetic circular dic...
A. Molina-Sánchez, G. Catarina, J. Fernández-Rossier. Magneto-optical response of chromium trihalide monolayers: chemical trends. J. Mater. Chem. C, 8 (2020)
© The Royal Society of Chemistry 2020
https://doi.org/10.1039/D0TC01322F
We report on the structural and transport properties of the smallest dislocation loop in graphene, known as a flower defect. First, by means of advanced experimental imaging techniques, we deduce how flower defects are formed during recrystallization of chemical vapor deposited graphene. We propose that the flower defects arise from a bulge type me...
Hotspot engineering has the potential to transform the field of surface-enhanced Raman spectroscopy (SERS) by enabling ultrasensitive and reproducible detection of analytes. However, the ability to controllably generate SERS hotspots, with desired location and geometry, over large-area substrates, has remained elusive. In this study, we sculpt arti...
R. Rani, A. Yoshimura, S. Das, M. R. Sahoo, A. Kundu, K. K. Sahu, V. Meunier, S. K. Nayak, N. Koratkar, and K. S. Hazra. Sculpting Artificial Edges in Monolayer MoS2 for Controlled Formation of Surface-Enhanced Raman Hotspots. ACS Nano 14, 5 (2020)
© 2020 American Chemical Society
The formation of the soluble polysulfides (Na2Sn, 4 ≤ n ≤ 8) causes poor cycling performance for room temperature sodium–sulfur (RT Na–S) batteries. Moreover, the formation of insoluble polysulfides (Na2Sn, 2 ≤ n < 4) can slow down the reaction kinetics and terminate the discharge reaction before it reaches the final product. In this work, coffee r...
Q. Guo, S. Li, X. Liu, H. Lu, X. Chang, H. Zhang, X. Zhu, Q. Xia, C. Yan, H. Xia. Ultrastable Sodium–Sulfur Batteries without Polysulfides Formation Using Slit Ultramicropore Carbon Carrier. Adv. Sci. 7, 1903246 (2020)
© 2020 The Authors
Materials with layered crystal structures and high in-plane anisotropy, such as black phosphorus, present unique properties and thus promise for applications in electronic and photonic devices. Recently, the layered structures of GeS2 and GeSe2 were utilized for high-performance polarization-sensitive photodetection in the short wavelength region d...
X. Wang, J. Tan, C. Han, J-J Wang, L. Lu, H. Du, C.-L. Jia, V. L. Deringer, J. Zhou and W. Zhang. Sub-Angstrom Characterization of the Structural Origin for High In-Plane Anisotropy in 2D GeS2. ACS Nano 14, 4 (2020)
© 2020 American Chemical Society
The spliceosome, a protein-directed metallo-ribozyme, catalyzes premature mRNA splicing via two transesterification reactions. The atomic-level details of the splicing mechanism and the role of the entwined protein-RNA environment during catalysis remain unresolved. Here, quantum-classical molecular dynamics simulations along with thermodynamic int...
J. Borišek and A. Magistrato. All-Atom Simulations Decrypt the Molecular Terms of RNA Catalysis in the Exon-Ligation Step of the Spliceosome. ACS Catal. 10, 9 (2020)
© 2020 American Chemical Society
https://doi.org/10.1021/acscatal.0c00390
We present a transient absorption setup combining broadband detection over the visible–UV range with high temporal resolution (∼20 fs) which is ideally suited to trigger and detect vibrational coherences in different classes of materials. We generate and detect coherent phonons (CPs) in single-layer (1L)-MoS2, as a representative semiconducting 1L-...
C.Trovatello, H.P.C. Miranda, A. Molina-Sánchez, R. Borrego-Varillas, C. Manzoni, L. Moretti, L. Ganzer, M. Maiuri, J. Wang, D. Dumcenco, A. Kis, L. Wirtz, A. Marini, G. Soavi, A.C. Ferrari, G. Cerullo, D. Sangalli, and S. Dal Conte. Strongly Coupled Coherent Phonons in Single-Layer MoS2. ACS Nano 14, 5 (2020)
© 2020 American Chemical Society
Doping lies at the heart of modern semiconductor technologies. Therefore, for two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs), the significance of controlled doping is no exception. Recent studies have indicated that, by substitutionally doping 2D TMDs with a judicious selection of dopants, their electrical, optical, mag...
T.Y. Zhang, K. Fujisawa, F. Zhang, M.Z. Liu, M.C. Lucking, R.N. Gontijo, Y. Lei, H. Liu, K. Crust, T. Granzier-Nakajima, H. Terrones, A.L. Elias, M. Terrones. Universal In Situ Substitutional Doping of Transition Metal Dichalcogenides by Liquid-Phase Precursor-Assisted Synthesis. ACS Nano 2020, 14, 4, 4326–4335
© 2020 American Chemical Society
Different dispersion near the electronic band edge of a semiconductor can have great influence on its transport, thermoelectric, and optical properties. Using first‐principles calculations, it is demonstrated that a new phase of group‐IV monochalcogenides (γ‐MX, M = Ge, Sn; X = S, Se, or Te) can be stabilized in monolayer limit. γ‐MXs are shown to ...
N. Luo, W. Duan, B.I. Yakobson, X. Zou. Excitons and Electron–Hole Liquid State in 2D γ‐Phase Group‐IV Monochalcogenides. Adv. Funct. Mater. 30, 2000533 (2020)
© 2020 WILEY-VCH
https://doi.org/10.1002/adfm.202000533
Monolayer transition-metal dichalcogenides in the T′ phase could enable the realization of the quantum spin Hall effect at room temperature, because they exhibit a prominent spin–orbit gap between inverted bands in the bulk. Here we show that the binding energy of electron–hole pairs excited through this gap is larger than the gap itself in the par...
D. Varsano, M. Palummo, E. Molinari, and M. Rontani. A monolayer transition-metal dichalcogenide as a topological excitonic insulator. Nature Nanotechnology, 15 (2020)
© The Author(s)
https://doi.org/10.1038/s41565-020-0650-4
Alkanol dehydration on Lewis acid–base pairs of transition metal oxide catalysts is a reaction of importance in oxygen removal from biomass-derived feedstocks and their conversion to chemicals in general. However, catalysts with a high degree of structural heterogeneity, such as commercial TiO2 powders, are not well-suited to establish rigorous str...
F. Lin, Y. Chen, L. Zhang, D. Mei, L. Kovarik, B. Sudduth, H. Wang, F. Gao, and Y. Wang. Single-Facet Dominant Anatase TiO2 (101) and (001) Model Catalysts to Elucidate the Active Sites for Alkanol Dehydration. ACS Catalysis 10, 7 (2020)
© 2020 American Chemical Society
https://doi.org/10.1021/acscatal.9b04654
Graphene nanoribbons (GNRs) have attracted much interest due to their largely modifiable electronic properties. Manifestation of these properties requires atomically precise GNRs which can be achieved through a bottom–up synthesis approach. This has recently been applied to the synthesis of width‐modulated GNRs hosting topological electronic quantu...
Q. Sun, O. Gröning. J. Overbeck, O. Braun, M.L. Perrin, G. Borin Barin, M. El Abbassi, K. Eimre, E. Ditler, C. Daniels, V. Meunier, C.A. Pignedoli, M. Calame, R. Fasel, and P. Ruffieux. Massive Dirac Fermion Behavior in a Low Bandgap Graphene Nanoribbon Near a Topological Phase Boundary. Adv. Mater. 32, 1906054 (2020)
© 2020 WILEY‐VCH
https://doi.org/10.1002/adma.201906054
Gold-supported ceria nanoparticles (CeOx/Au), constituting an inverse system with respect to the more commonly studied ceria-supported gold nanoparticles, were previously identified as an excellent catalyst for water–gas shift reaction, CO oxidation, and steam reforming of methanol. However, the electronic structure and reactivity of such inverse c...
Y. Li, S. Li, M. Bäumer, E. A. Ivanova-Shor, and L. V. Moskaleva. What Changes on the Inverse Catalyst? Insights from CO Oxidation on Au-Supported Ceria Nanoparticles Using Ab Initio Molecular Dynamics. ACS Catalysis 10, 5 (2020)
© 2020 American Chemical Society
https://doi.org/10.1021/acscatal.9b05175
The electronic properties of graphene nanoribbons (GNRs) can be precisely tuned by chemical doping. Here we demonstrate that amino (NH2) functional groups attached at the edges of chiral GNRs (chGNRs) can efficiently gate the chGNRs and lead to the valence band (VB) depopulation on a metallic surface. The NH2-doped chGNRs are grown by on-surface sy...
J. Li, P. Brandimarte, M. Vilas-Varela, N. Merino-Díez, C. Moreno, A. Mugarza, J. Sáez Mollejo, D. Sánchez-Portal, D. Garcia de Oteyza, M. Corso, A. Garcia-Lekue, D. Peña, and J. I. Pascual. Band Depopulation of Graphene Nanoribbons Induced by Chemical Gating with Amino Groups. ACS Nano 14, 2 (2020)
© 2020 American Chemical Society
The commercial Haber-Bosch process for NH3 production not only requires large amounts of energy and hydrogen supply but also generates tremendous greenhouse CO2 emission. To mitigate energy and environmental challenges, renewable ammonia production technologies based on electrochemical and photochemical methods, in particular, photocatalytic nitrog...
J. Li, P. Liu, Y. Tang, H. Huang, H. Cui, D. Mei, and C. Zhong. Single-Atom Pt–N3 Sites on the Stable Covalent Triazine Framework Nanosheets for Photocatalytic N2 Fixation. ACS Catalysis 10, 4 (2020)
© 2020 American Chemical Society
We extensively characterize the electronic structure of ultranarrow graphene nanoribbons (GNRs) with armchair edges and zigzag termini that have five carbon atoms across their width (5-AGNRs), as synthesized on Au(111). Scanning tunneling spectroscopy measurements on the ribbons, recorded on both the metallic substrate and a decoupling NaCl layer, ...
J. Lawrence, P. Brandimarte, A. Berdonces-Layunta, M. S. G. Mohammed, A. Grewal, C. C. Leon, D. Sánchez-Portal, and D. G. de Oteyza. Probing the Magnetism of Topological End States in 5-Armchair Graphene Nanoribbons. ACS Nano 14, 4 (2020)
© 2020 American Chemical Society
Catalyst discovery is increasingly relying on computational chemistry, and many of the computational tools are currently being automated. The state of this automation and the degree to which it may contribute to speeding up development of catalysts are the subject of this Perspective. We also consider the main challenges associated with automated c...
M. Foscato and V. R. Jensen. Automated in Silico Design of Homogeneous Catalysts. ACS Catal. 10, 3 (2020)
© 2020 American Chemical Society
https://doi.org/10.1021/acscatal.9b04952
Perovskite solar cells are among the most exciting photovoltaic systems as they combine low recombination losses, ease of fabrication, and high spectral tunability. The Achilles heel of this technology is the device stability due to the ionic nature of the perovskite crystal, rendering it highly hygroscopic, and the extensive diffusion of ions espe...
- C. M. Wolff, L. Canil, C. Rehermann, N. N. Linh, F. Zu, M. Ralaiarisoa, P. Caprioglio, L. Fiedler, M. Stolterfoht, S..Kogikoski Jr., I. Bald, N. Koch, E. L. Unger, T. Dittrich, A. Abate, and D. Neher. Perfluorinated Self-Assembled Monolayers Enhance the Stability and Efficiency of Inverted Perovskite Solar Cells. ACS Nano, 14, 2, 1445–1456 (2020)
© 2020 American Chemical Society
The lithium ion conductivity of lithium argyrodite can be improved by introducing Cl to tailor the S/Cl disorder in the structure. An ultrafast room temperature lithium ion conductivity of up to 6.4 mS/cm was achieved for Li5.7PS4.7Cl1.3. The synthesis parameters for Li7-xPS6-xClx (x = 1.0, 1.1, 1.2, 1.3, 1.4, 1.5, 1.6, 1.7, 1.8, 1.9) are systemati...
C. Yu, Y. Li, M. Willans, Y. Zhao, K.R. Adair, F. Zhao, W. Li, S. Deng, J. Liang, M. N. Banis, R. Li, H. Huang, L. Zhang, R. Yang, S. Lu, Y. Huang, X. Sun. Superionic conductivity in lithium argyrodite solid-state electrolyte by controlled Cl-doping. Nano Energy 69, 104396 (2020)
© 2019 Elsevier Ltd. All rights reserved.
https://doi.org/10.1016/j.nanoen.2019.104396
The chemical versatility of carbon imparts manifold properties to organic compounds, where magnetism remains one of the most desirable but elusive. Polycyclic aromatic hydrocarbons, also referred to as nanographenes, show a critical dependence of electronic structure on the topologies of the edges and the π-electron network, which makes them model ...
S. Mishra, D. Beyer, K. Eimre et al. Topological frustration induces unconventional magnetism in a nanographene. Nat. Nanotechnol. 15 (2020)
© 2020 The Authors
https://doi.org/10.1038/s41565-019-0577-9
Platinum (Pt)-based materials are important components of microelectronic sensors, anticancer drugs, automotive catalytic converters and electrochemical energy conversion devices1. Pt is currently the most common catalyst used for the oxygen reduction reaction (ORR) in devices such as fuel cells and metal–air batteries2,3, although a scalable use i
Y. Yuan, J. Wang, S. Adimi et al. Zirconium nitride catalysts surpass platinum for oxygen reduction. Nat. Mater. 19, 282–286 (2020).
© 2019 The Author(s)
https://doi.org/10.1038/s41563-019-0535-9
