Martin Head‐Gordon
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View article: Gold-Standard Chemical Database 137 (GSCDB137): A Diverse Set of Accurate Energy Differences for Assessing and Developing Density Functionals
Gold-Standard Chemical Database 137 (GSCDB137): A Diverse Set of Accurate Energy Differences for Assessing and Developing Density Functionals Open
We present GSCDB137, a rigorously curated benchmark library of 137 data sets (8377 entries) covering main-group and transition-metal reaction energies and barrier heights, (intra- and intermolecular) noncovalent interactions, dipole moment…
View article: Structural Evidence of Interanionic Hydrogen Bonding in Phosphoric Acid Solutions
Structural Evidence of Interanionic Hydrogen Bonding in Phosphoric Acid Solutions Open
Interanionic hydrogen bonding (IAHB) is a noncovalent interaction between like-charged ions that challenges conventional electrostatic understanding. This study provides direct structural evidence of IAHB in concentrated aqueous phosphoric…
View article: Can Charge Transfer Across C─H⋅⋅⋅O Hydrogen Bonds Stabilize Oil Droplets in Water?
Can Charge Transfer Across C─H⋅⋅⋅O Hydrogen Bonds Stabilize Oil Droplets in Water? Open
Oil–water emulsions resist aggregation due to the presence of negative charges at their surface that leads to mutual repulsion between droplets, but the molecular origin of oil charge is currently under debate. Although much evidence has s…
View article: More numerical precision for less compute cost: Optimizing a local correlation algorithm for second order Møller-Plesset theory and comparing against pair natural orbital methods
More numerical precision for less compute cost: Optimizing a local correlation algorithm for second order Møller-Plesset theory and comparing against pair natural orbital methods Open
Correlations associated with dynamical fluctuations of electrons in molecules can be spatially localized, which offers the promise of reducing the compute complexity of many-body quantum chemical methods such as second-order Møller-Plesset…
View article: X-ray Thermometry Reveals that Glycerol Aerosols Spontaneously form Glasses
X-ray Thermometry Reveals that Glycerol Aerosols Spontaneously form Glasses Open
Our lack of knowledge about molecular-level structure within atmospheric aerosols hinders understanding of the chemical reactivity and light-matter interactions therein, contributing to the outsized contribution of aerosols to the error in…
View article: Gold-Standard Chemical Database 137 (GSCDB137): A diverse set of accurate energy differences for assessing and developing density functionals
Gold-Standard Chemical Database 137 (GSCDB137): A diverse set of accurate energy differences for assessing and developing density functionals Open
We present GSCDB137, a rigorously curated benchmark library of 137 data sets (8377 entries) covering main-group and transition-metal reaction energies and barrier heights, (intramolecular) non-covalent interactions, dipole moments, polariz…
View article: Mechanistic Studies of Oxidative Degradation in Diamine-Appended Metal–Organic Frameworks Exhibiting Cooperative CO<sub>2</sub> Capture
Mechanistic Studies of Oxidative Degradation in Diamine-Appended Metal–Organic Frameworks Exhibiting Cooperative CO<sub>2</sub> Capture Open
Understanding the impact of O2 during a carbon capture process is vital for designing robust, cost-effective materials for carrying it out. However, mechanistic studies of the O2-induced degradation of materials are n…
View article: A Perspective on Quantum Computing Applications in Quantum Chemistry using 25--100 Logical Qubits
A Perspective on Quantum Computing Applications in Quantum Chemistry using 25--100 Logical Qubits Open
The intersection of quantum computing and quantum chemistry represents a promising frontier for achieving quantum utility in domains of both scientific and societal relevance. Owing to the exponential growth of classical resource requireme…
View article: The approximate second order coupled-cluster method based on a size-consistent Brillouin-Wigner partitioning
The approximate second order coupled-cluster method based on a size-consistent Brillouin-Wigner partitioning Open
We present a variant of the approximate second order coupled-cluster method (CC2) with a two parameter size- consistent Brillouin-Wigner (BW-s) partitioning instead of a Møller-Plesset (MP) partitioning for the unperturbed Hamiltonian, whi…
View article: Optimized auxiliary functions for robust mitigation of finite-size errors in periodic hybrid density functional theory
Optimized auxiliary functions for robust mitigation of finite-size errors in periodic hybrid density functional theory Open
When calculating properties of periodic systems at the thermodynamic limit (TDL), the dominant source of finite size error (FSE) arises from the long-range Coulomb interaction, and can manifest as a slowly converging quadrature error when …
View article: Extending orbital-optimized density functional theory to L-edge XPS and beyond: Spin-orbit coupling via non-orthogonal quasi-degenerate perturbation theory
Extending orbital-optimized density functional theory to L-edge XPS and beyond: Spin-orbit coupling via non-orthogonal quasi-degenerate perturbation theory Open
Quantum mechanical calculations of core electron binding energies (CEBEs) leading to 2p hole states are relevant to interpreting L-edge x-ray photo-electron spectroscopy (XPS), as well as higher edges. Orbital-optimized density functional …
View article: Beyond real: Alternative unitary cluster Jastrow models for molecular electronic structure calculations on near-term quantum computers
Beyond real: Alternative unitary cluster Jastrow models for molecular electronic structure calculations on near-term quantum computers Open
Near-term quantum devices require wavefunction ansätze that are expressive while also of shallow circuit depth in order to both accurately and efficiently simulate molecular electronic structure. While unitary coupled cluster (e.g., UCCSD)…
View article: Mechanistic Studies of Oxidative Degradation in Diamine-Appended Metal–Organic Frameworks Exhibiting Cooperative CO2 Capture
Mechanistic Studies of Oxidative Degradation in Diamine-Appended Metal–Organic Frameworks Exhibiting Cooperative CO2 Capture Open
Understanding the impact of O2 during a carbon capture process is vital for designing robust, cost-effective materials for carrying it out. However, mechanistic studies of the O2-induced degradation of materials are not easily undertaken o…
View article: The conundrum of diffuse basis sets: A blessing for accuracy yet a curse for sparsity
The conundrum of diffuse basis sets: A blessing for accuracy yet a curse for sparsity Open
Diffuse atomic orbital basis sets have proven to be essential to obtain accurate interaction energies, especially in regard to non-covalent interactions. However, they also have a detrimental impact on the sparsity of the one-particle dens…
View article: An Error Mitigated Non-Orthogonal Quantum Eigensolver via Shadow Tomography
An Error Mitigated Non-Orthogonal Quantum Eigensolver via Shadow Tomography Open
We present a shadow-tomography-enhanced Non-Orthogonal Quantum Eigensolver (NOQE) for more efficient and accurate electronic structure calculations on near-term quantum devices. By integrating shadow tomography into the NOQE, the measureme…
View article: Coupled-cluster pairing models for radicals with strong correlations
Coupled-cluster pairing models for radicals with strong correlations Open
The pairing hierarchy of perfect pairing (PP), perfect quadruples (PQ) and perfect hextuples (PH) are sparsified coupled cluster models that are exact in a pairing active space for 2, 4, and 6 electron clusters, respectively. We describe a…
View article: Foundation Models for Atomistic Simulation of Chemistry and Materials
Foundation Models for Atomistic Simulation of Chemistry and Materials Open
Given the power of large language and large vision models, it is of profound and fundamental interest to ask if a foundational model based on data and parameter scaling laws and pre-training strategies is possible for learned simulations o…
View article: The Conundrum of Diffuse Basis Sets: A Blessing for Accuracy yet a Curse for Sparsity
The Conundrum of Diffuse Basis Sets: A Blessing for Accuracy yet a Curse for Sparsity Open
Diffuse atomic orbital basis sets have proven to be essential to obtain accurate interaction energies, especially in regard to non-covalent interactions. However, they also have a detrimental impact on the sparsity of the one-particle dens…
View article: Repartitioning the Hamiltonian in many-body second-order Brillouin–Wigner perturbation theory: Uncovering new size-consistent models
Repartitioning the Hamiltonian in many-body second-order Brillouin–Wigner perturbation theory: Uncovering new size-consistent models Open
Second-order Møller–Plesset perturbation theory is well-known as a computationally inexpensive approach to the electron correlation problem that is size-consistent with a size-consistent reference but fails to be regular. On the other hand…
View article: Programmable simulations of molecules and materials with reconfigurable quantum processors
Programmable simulations of molecules and materials with reconfigurable quantum processors Open
Simulations of quantum chemistry and quantum materials are believed to be among the most important applications of quantum information processors. However, realizing practical quantum advantage for such problems is challenging because of t…
View article: Completely Multipolar Model for Many-Body Water–Ion and Ion–Ion Interactions
Completely Multipolar Model for Many-Body Water–Ion and Ion–Ion Interactions Open
This work constructs an advanced force field, the Completely Multipolar Model (CMM), to quantitatively reproduce each term of an energy decomposition analysis (EDA) for aqueous solvated alkali metal cations and halide anions and their ion …
View article: Regioisomeric Engineering for Multicharge and Spin Stabilization in Two-Electron Organic Catholytes
Regioisomeric Engineering for Multicharge and Spin Stabilization in Two-Electron Organic Catholytes Open
Developing multicharge and spin stabilization strategies is fundamental to enhancing the lifetime of functional organic materials, particularly for long-term energy storage in multiredox organic redox flow batteries. Current approaches are…
View article: An improved guess for the variational calculation of charge-transfer excitations in large systems
An improved guess for the variational calculation of charge-transfer excitations in large systems Open
The variational calculation of charge-transfer excitations with methods based on density functional theory greatly benefits from guess refinement strategies. We develop such a method that enables accurate calculations for large systems.
View article: Beyond real: alternative unitary cluster Jastrow models for molecular electronic structure calculations on near-term quantum computers
Beyond real: alternative unitary cluster Jastrow models for molecular electronic structure calculations on near-term quantum computers Open
Im-uCJ and g-uCJ ansätze extend orbital rotations into complex space. Implemented exactly via generalized Givens rotations, these ansätze achieve higher accuracy and more robust optimization than the currently available Re-uCJ.
View article: Computational Optimization of Room Temperature Usable Capacity for Hydrogen Storage in MFU-4-Type Metal–Organic Frameworks via Pairwise Metal Substitutions
Computational Optimization of Room Temperature Usable Capacity for Hydrogen Storage in MFU-4-Type Metal–Organic Frameworks via Pairwise Metal Substitutions Open
The efficient storage of hydrogen is a critical challenge in the quest for sustainable energy solutions. Current adsorbent-based methods achieve satisfactory storage densities predominantly under cryogenic temperatures and/or high pressure…
View article: Hydrogen ejection from hydrocarbons: Characterization and relevance in soot formation and interstellar chemistry
Hydrogen ejection from hydrocarbons: Characterization and relevance in soot formation and interstellar chemistry Open
Polycyclic aromatic hydrocarbons (PAHs) play a major role in the chemistry of combustion, pyrolysis, and the interstellar medium. Production (or activation) of radical PAHs and propagation of their resulting reactions require efficient deh…
View article: Characterizing the interplay of 'σ-hole’ and ‘σ*' interactions in chalcogen bonding
Characterizing the interplay of 'σ-hole’ and ‘σ*' interactions in chalcogen bonding Open
Intermolecular non-covalent interactions, such as hydrogen, halogen and chalcogen bonds, are crucial in gas phase and condensed phase chemistry. Here we investigate and challenge the conflicting ‘σ-hole’ and ‘σ*’ paradigms commonly used fo…
View article: High-temperature carbon dioxide capture in a porous material with terminal zinc hydride sites
High-temperature carbon dioxide capture in a porous material with terminal zinc hydride sites Open
Carbon capture can mitigate point-source carbon dioxide (CO 2 ) emissions, but hurdles remain that impede the widespread adoption of amine-based technologies. Capturing CO 2 at temperatures closer to those of many industrial exhaust stream…
View article: Real-time propagation of adaptive sampling selected configuration interaction wave function
Real-time propagation of adaptive sampling selected configuration interaction wave function Open
We have developed a new time propagation method, time-dependent adaptive sampling configuration interaction (TD-ASCI), to describe the dynamics of a strongly correlated system. We employ the short iterative Lanczos (SIL) method as the time…
View article: A static quantum embedding scheme based on coupled cluster theory
A static quantum embedding scheme based on coupled cluster theory Open
We develop a static quantum embedding scheme that utilizes different levels of approximations to coupled cluster (CC) theory for an active fragment region and its environment. To reduce the computational cost, we solve the local fragment p…