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Rushi Gong

Publications and source records attributed to Rushi Gong.

11 recordsLinked to original sources

Clifford-efficient sparse state preparation for molecular wavefunctions

Sparse quantum state preparation concerns an $n$-qubit target state that is a superposition of only $d \ll 2^n$ computational basis states. Existing approaches exploit this sparsity by compressing these $d$ basis states and their amplitudes onto a smaller set of qubits, called the dense register, before expanding the prepared state to the full register. Rather than relying on the permutation-based compression used in prior work, we exploit affine relationships among the binary configurations over the finite field $\operatorname{GF}(2)$ to reduce both the non-Clifford gate count and the ancillary qubit count. Invertible affine transformations over $\operatorname{GF}(2)$, comprising Gaussian elimination and all-ones-row removal, first reduce the dense register from $n$ to the rank $r$ using only Clifford gates and no ancillary qubits. An optional binary encoding stage then trades additional Toffoli gates and ancillary qubits for further compression to the minimum $\lceil\log_2 d\rceil$ dense qubits needed to represent $d$ distinct configurations. For chemically relevant wavefunctions, such as those obtained from selected configuration interaction calculations, shared electronic excitation patterns produce many of these affine relationships, enabling substantial Clifford-only compression before binary encoding. Across the molecular benchmarks, our method requires the fewest ancillary qubits among the evaluated sparse state preparation methods while maintaining comparable non-Clifford gate counts when using binary encoding.

quant-ph

QDK/Chemistry: A Modular Toolkit for Quantum Chemistry Applications

We present QDK/Chemistry, a software toolkit for quantum chemistry workflows targeting quantum computers. The toolkit addresses a key challenge in the field: while quantum algorithms for chemistry have matured considerably, the infrastructure connecting classical electronic structure calculations to quantum circuit execution remains fragmented. QDK/Chemistry provides this infrastructure through a modular architecture that separates data representations from computational methods, enabling researchers to compose workflows from interchangeable components. In addition to providing native implementations of targeted algorithms in the quantum-classical pipeline, the toolkit builds upon and integrates with widely used open-source quantum chemistry packages and quantum computing frameworks through a plugin system, allowing users to combine methods from different sources without modifying workflow logic. This paper describes the design philosophy, current capabilities, and role of QDK/Chemistry as a foundation for reproducible quantum chemistry experiments.

quant-ph

Achieving accurate entropy and melting point by ab initio molecular dynamics and zentropy theory: Application to fluoride and chloride molten salts

We have recently developed a breakthrough methodology for rapidly computing entropy in both solids and liquids by integrating a multiscale entropy approach (known as zentropy theory) with molecular dynamics (MD) simulations. This approach enables entropy estimation from a single MD trajectory by analyzing the probabilities of local structural configurations and atomic distributions, effectively addressing the long-standing challenge of capturing configurational entropy. Here, we demonstrate the power of this method by predicting entropies, enthalpies, and melting points for 25 binary and ternary chlorite- and fluoride-based molten salts using ab initio MD (AIMD) simulations. The strong agreement between our predictions and experimental data underscores the potential of this approach to transform computational thermodynamics, offering accurate, efficient, and direct predictions of thermodynamic properties across both solid and liquid phases.

cond-mat.mtrl-sci

Thermodynamic modeling of the LiCl-KCl-LaCl$_3$ system with Bayesian model selection and uncertainty quantification

Chloride molten salts are increasingly used in pyroprocessing techniques for the separation of lanthanides. Understanding thermodynamic properties of these salts is essential to predict their critical characteristics and optimize the separation process. Several thermodynamic models, including the associate model, the two-sublattice ionic model, and the modified quasichemical model with quadruplet approximation (MQMQA), have been utilized in the literature to capture the complexity of molten salts. In the present work, the Bayes factor is used to guide the model selection process for thermodynamic modeling of the KCl-LaCl3 system and provide statistical comparison of various models. The results indicate that the MQMQA model is the most favorable one based on available data. The LiCl-KCl-LaCl3 system has been further modelled with uncertainty quantification (UQ) using MQMQA with the thermodynamic properties of compounds in KCl-LaCl3 predicted by the quasiharmonic approach in terms of first-principles phonon calculations as a function of temperature. The calculated phase stability shows excellent agreement with experimental data, indicating that an appropriate thermodynamic model is important for accurately predicting critical characteristics of complex molten salts.

cond-mat.mtrl-sci

Molecular interaction volume model of mixing enthalpy for molten salt system: An integrated calorimetry-model case study of LaCl$_3$-(LiCl-KCl)

Calorimetric determination of enthalpies of mixing ($Δ$H$_{\rm mix}$) of multicomponent molten salts often employs empirical models that lack parameters with clear physical interpretation (e.g., coordination numbers, molar volumes, and pair potentials). Although such physics informed models are not always needed, a thermodynamic understanding of the relationships between excess energies of mixing and local to intermediate solvation structures is particularly important for pyrochemical separation, as is the case for lanthanides (Ln), which are common neutron poisons and critical industrial elements found in spent nuclear fuels. Here we implement the molecular interaction volume model (MIVM) to synthesize information from experimentally measured $Δ$H$_{\rm mix}$ (using high temperature melt drop calorimetry) and the distribution of solvation structures from ab initio molecular dynamics (AIMD) simulations. This was demonstrated by a case study of molten salt system consisted of LaCl$_3$ mixing with a eutectic LiCl-KCl (58mol% to 42mol%) at 873 K and 1133 K. The parameters modelled from MIVM were used to extrapolate excess Gibbs energy ($Δ$G$_{\rm mix}$), and compositional dependence of La$^{3+}$ activity in the LaCl$_3$-(LiCl-KCl) system. In contrast, by AIMD or polarizable ion model (PIM) simulations, a significant deviation regarding the predicted $Δ$H$_{\rm mix}$ was seen if computed directly from the molecular dynamic trajectories. The integrated experimental and simulation data within the MIVM formalism are generalizable to a wide variety of molten salts and demonstrate a significant improvement over currently employed methods to study molten salts for nuclear and separations sciences.

cond-mat.mtrl-sci

Revisiting first-principles thermodynamics by quasiharmonic approach: Application to study thermal expansion of additively-manufactured Inconel 625

An innovative method is developed for accurate determination of thermodynamic properties as a function of temperature by revisiting the density functional theory (DFT) based quasiharmonic approach (QHA). The present methodology individually evaluates the contributions from static total energy, phonon, and thermal electron to free energy for increased efficiency and accuracy. The Akaike information criterion with a correction (AICc) is used to select models and model parameters for fitting each contribution as a function of volume. Using the additively manufactured Inconel alloy 625 (IN625) as an example, predicted temperature-dependent linear coefficient of thermal expansion (CTE) agrees well with dilatometer measurements and values in the literature. Sensitivity and uncertainty are also analyzed for the predicted IN625 CTE due to different structural configurations used by DFT, and hence different equilibrium properties determined.

cond-mat.mtrl-sci

Revisiting thermodynamics in (LiF, NaF, KF, CrF2)-CrF3 by first-principles calculations and CALPHAD modeling

The thermodynamic description of the (LiF, NaF, KF, CrF2)-CrF3 systems has been revisited, aiming for a better understanding of the effects of Cr on the FLiNaK molten salt. First-principles calculations based on density functional theory (DFT) were performed to determine the electronic and structural properties of each compound, including the formation enthalpy, volume, and bulk modulus. DFT-based phonon calculations were carried out to determine the thermodynamic properties of compounds, for example, enthalpy, entropy, and heat capacity as functions of temperature. Phonon-based thermodynamic properties show a good agreement with experimental data of binary compounds LiF, NaF, KF, CrF3, and CrF2, establishing a solid foundation to determine thermodynamic properties of ternary compounds as well as to verify results estimated by the Neumann-Kopp rule. Additionally, DFT-based ab initio molecular dynamics (AIMD) simulations were employed to predict the mixing enthalpies of liquid salts. Using DFT-based results and experimental data in the literature, the (LiF, NaF, KF, CrF2)-CrF3 system has been remodeled in terms of the CALculation of PHAse Diagrams (CALPHAD) approach using the modified quasichemical model with quadruplet approximation (MQMQA) for liquid. Calculated phase stability in the present work shows an excellent agreement with experiments, indicating the effectiveness of combining DFT-based total energy, phonon, and AIMD calculations, and CALPHAD modeling to provide the thermodynamic description in complex molten salt systems.

cond-mat.mtrl-sci

Thermodynamic modeling with uncertainty quantification in the Nb-Ni system using the upgraded PyCalphad and ESPEI

The Nb-Ni system has been remodeled with uncertainty quantification (UQ) by using the presently upgraded software tools of PyCalphad and ESPEI that contain the new capability to model site occupancy of Wyckoff position for the phases of interest. Specifically, the five- and three-sublattice models are used to model the topologically close pack (TCP) phases of μ-Nb7Ni6 and δ-NbNi3, respectively, according to exactly their Wyckoff positions; where the inputs for CALPHAD-based modeling include the presently predicted thermochemical data as a function of temperature by density functional theory (DFT) based first-principles and phonon calculations together with both phase equilibrium and site occupancy data in the literature. Besides phase diagram and thermodynamic properties, the present CALPHAD predictions of site occupancies are also agreed well with experimental data such as the measured Nb sites in μ-Nb7Ni6. In addition, the predicted UQ values using the Markov Chain Monte Carlo (MCMC) method as implemented in ESPEI make it possible to quantify uncertainties in the Nb-Ni system, such as site occupancies in μ-Nb7Ni6 and enthalpy of mixing in liquid.

cond-mat.mtrl-sci

Thermodynamic modeling with uncertainty quantification using the modified quasichemical model in quadruplet approximation: Implementation into PyCalphad and ESPEI

The modified quasichemical model in the quadruplet approximation (MQMQA) considers the first- and the second-nearest-neighbor coordination and interactions, particularly useful in describing short-range ordering in complex liquids such as molten salts, slag in metal processing, and electrolytic solutions. The present work implements the MQMQA into the Python based open-source software PyCalphad for thermodynamic calculations. This endeavor facilitates the development of MQMQA-based thermodynamic database with uncertainty quantification (UQ) using the open-source software ESPEI. A new database structure based on Extensible Markup Language (XML) is proposed for ESPEI evaluation of MQMQA model parameters. Using the KF-NiF2 system as an example, we demonstrate the successful implementation of MQMQA in PyCalphad through thermodynamic calculations of Gibbs energy, equilibrium quadruplet fractions, and phase diagram, as well as database development with UQ using ESPEI. The present implementation offers an open-source capability for performing CALPHAD modeling for complex liquids with short-range ordering using MQMQA.

physics.comp-ph

Thermodynamic modeling of the Pd-Zn system with uncertainty quantification and its implication to tailor catalysts

Pd-Zn intermetallic catalysts show encouraging combinations of activity and selectivity on well-defined active site ensembles. Thermodynamic description of the Pd-Zn system, delineating phase boundaries, and enumerating site occupancies within intermediate alloy phases, are essential to determining the ensembles of Pd-Zn atoms as a function of composition and temperature. Combining the present extensive first-principles calculations based on density functional theory (DFT) and available experimental data, the Pd-Zn system was remodeled using the CALculation of PHAse Diagrams (CALPHAD) approach. High throughput modeling tools with uncertainty quantification, i.e., ESPEI and PyCalphad, were incorporated in the phase analysis. The site occupancies across the γ-phase composition region were given special attention. A four-sublattice model was used for the γ-phase owing to its four Wyckoff positions, i.e., the outer tetrahedral (OT) site 8c, the inner tetrahedral (IT) site 8c, the octahedral (OH) 12e, and the cuboctahedral (CO) site 24g. The site fractions of Pd and Zn calculated from the present thermodynamic model show the occupancy preference of Pd in the OT and OH sublattices in agreement with experimental observations. The force constants obtained from DFT-based phonon calculations further supports the tendency of Pd occupying the OH sublattice compared with the IT and CO sublattice. The catalytic assembles changing from Pd monomers (Pd1) to trimers (Pd3) on the surface of the γ-phase is attributed to the increase of Pd occupancy in the OH sublattice.

cond-mat.mtrl-sci

Anisotropic Bi2O2Se(Te) Monolayer: Realizing Ultra-High Carrier Mobility and Giant Electric Polarization in Two-Dimension

Here, we have identified the monolayer phase of Bi2O2Se as a promising two-dimensional semiconductor with ultra-high carrier mobility and giant electric polarization. Due to the strong reconstruction originated from the interlayer electrostatic force, we have applied structure prediction algorithms to explore the crystalline geometry of Bi2O2Se monolayer with the lowest total energy. Considering Se and Te belong to the same group, Bi2O2Te monolayer is also investigated based on a similar scheme. Further calculations suggest that the high carrier mobility is maintained in the monolayer phase and the moderate band gap will lead to the strong optical absorption in the visible light region. In particular, the electron mobility in Bi2O2Te can reach as high as 3610 cm2V-1s-1 at room temperature, which is almost ten times of conventional transition metal dichalcogenides (TMD) family. Because of the strong structural anisotropy, a remarkable spontaneous in-plane and out-of-plane electric polarization is additionally revealed along with significant piezoelectric properties, endowing them as promising candidates in the area of photovoltaic solar cells, optoelectronic materials and field effect transistors.

cond-mat.mtrl-sci