arXiv subjects

Takao Kobayashi

Publications and source records attributed to Takao Kobayashi.

12 recordsLinked to original sources

arXiv2026

Quantum Simulations for Extreme Ultraviolet Photolithography

A key challenge of extreme ultraviolet (EUV) lithography in semiconductor fabrication is the line edge roughness or "blur" produced by the electron cascades following absorption of a high-energy photon. Here we present quantum algorithms to compute EUV absorption and photoelectron emission spectra, which are key to predicting blur. The first is a time-domain algorithm resolving absorption at a given frequency; the second is a first-quantized plane-wave algorithm computing the photoemission spectrum via real-time dynamics that treats bound and continuum states on equal footing. For a model photoresist monomer IMePh, 92 eV absorption requires $200$ logical qubits and $10^{9}$ non-Clifford gates per circuit with $10^3$ shots, while the photoemission spectrum needs $\geq 10^{14}$ gates, $10^4$ shots, and several thousand logical qubits. These results establish high-fidelity quantum simulations as a key component to parameterize the multi-scale macroscopic models required to overcome the electron blur bottleneck in semiconductor miniaturization.

quant-ph↗

arXiv2026

Auger Spectroscopy via Generative Quantum Eigensolver: A Quantum Approach to Molecular Excitations

Auger electron spectroscopy, a way of characterizing electronic structure through core-level decay processes, is widely used in materials characterization; however direct calculation from molecular geometry requires accurate treatment of many excited states, posing a challenge for classical methods. We present a hybrid quantum-classical workflow for calculating Auger spectra that combines the generative quantum eigensolver (GQE) for ground-state preparation, the quantum self-consistent equation-of-motion method for excited-state calculations, and the one-centre approximation for Auger transition rates. GQE uses a GPT-2 model to generate quantum circuits for ground-state optimization, allowing our workflow to benefit from HPC parallelization and GPU-acceleration for favourable scaling with system size. We demonstrate the validity of our workflow by calculating the Auger spectrum of water with the STO-3G basis set and demonstrating qualitative and quantitative agreement with spectra obtained using completely classical full configuration interaction calculations, from the computational literature, and from the experimental literature. We also find that for water, substituting the variational quantum eigensolver (VQE) for GQE results in near-identical spectra, but that the ground state estimator generated by GQE contains about half the total gate count as that generated by VQE.

quant-ph↗

arXiv2025

Tensor-based quantum phase difference estimation for large-scale demonstration

We develop an energy calculation algorithm leveraging quantum phase difference estimation (QPDE) scheme and a tensor-network-based unitary compression method in the preparation of superposition states and time-evolution gates. Alongside its efficient implementation, this algorithm reduces depolarization noise affections exponentially. We demonstrated energy gap calculations for one-dimensional Hubbard models on IBM superconducting devices using circuits up to 32-system (plus one-ancilla) qubits, a five-fold increase over previous QPE demonstrations, at the 7242 controlled-Z gate level of standard transpilation, utilizing a Q-CTRL error suppression module. Additionally, we propose a technique towards molecular executions using spatial orbital localization and index sorting, verified linear polyene simulations up to 21 qubits. Since QPDE can handle the same objectives as QPE, our algorithm represents a leap forward in quantum computing on real devices.

quant-ph↗

arXiv2024

Trajectory Planning Using Tire Thermodynamics for Automated Drifting

Automated vehicles need to estimate tire-road friction information, as it plays a key role in safe trajectory planning and vehicle dynamics control. Notably, friction is not solely dependent on road surface conditions, but also varies significantly depending on the tire temperature. However, tire parameters such as the friction coefficient have been conventionally treated as constant values in automated vehicle motion planning. This paper develops a simple thermodynamic model that captures tire friction temperature variation. To verify the model, it is implemented into trajectory planning for automated drifting - a challenging application that requires leveraging an unstable, drifting equilibrium at the friction limits. The proposed method which captures the hidden tire dynamics provides a dynamically feasible trajectory, leading to more precise tracking during experiments with an LQR (Linear Quadratic Regulator) controller.

eess.SY↗

arXiv2024

Quantum computing quantum Monte Carlo with hybrid tensor network for electronic structure calculations

Quantum computers have a potential for solving quantum chemistry problems with higher accuracy than classical computers. Quantum computing quantum Monte Carlo (QC-QMC) is a QMC with a trial state prepared in quantum circuit, which is employed to obtain the ground state with higher accuracy than QMC alone. We propose an algorithm combining QC-QMC with a hybrid tensor network to extend the applicability of QC-QMC beyond a single quantum device size. In a two-layer quantum-quantum tree tensor, our algorithm for the larger trial wave function can be executed than preparable wave function in a device. Our algorithm is evaluated on the Heisenberg chain model, graphite-based Hubbard model, hydrogen plane model, and MonoArylBiImidazole using full configuration interaction QMC. Our algorithm can achieve energy accuracy (specifically, variance) several orders of magnitude higher than QMC, and the hybrid tensor version of QMC gives the same energy accuracy as QC-QMC when the system is appropriately decomposed. Moreover, we develop a pseudo-Hadamard test technique that enables efficient overlap calculations between a trial wave function and an orthonormal basis state. In a real device experiment by using the technique, we obtained almost the same accuracy as the statevector simulator, indicating the noise robustness of our algorithm. These results suggests that the present approach will pave the way to electronic structure calculation for large systems with high accuracy on current quantum devices.

quant-ph↗

arXiv2023

A combined quantum-classical method applied to material design: optimization and discovery of photochromic materials for photopharmacology applications

Integration of quantum chemistry simulations, machine learning techniques, and optimization calculations is expected to accelerate material discovery by making large chemical spaces amenable to computational study; a challenging task for classical computers. In this work, we develop a combined quantum-classical computing scheme involving the computational-basis Variational Quantum Deflation (cVQD) method for calculating excited states of a general classical Hamiltonian, such as Ising Hamiltonian. We apply this scheme to the practical use case of generating photochromic diarylethene (DAE) derivatives for photopharmacology applications. Using a data set of 384 DAE derivatives quantum chemistry calculation results, we show that a factorization-machine-based model can construct an Ising Hamiltonian to accurately predict the wavelength of maximum absorbance of the derivatives, $λ_{\rm max}$, for a larger set of 4096 DAE derivatives. A 12-qubit cVQD calculation for the constructed Ising Hamiltonian provides the ground and first four excited states corresponding to five DAE candidates possessing large $λ_{\rm max}$. On a quantum simulator, results are found to be in excellent agreement with those obtained by an exact eigensolver. Utilizing error suppression and mitigation techniques, cVQD on a real quantum device produces results with accuracy comparable to the ideal calculations on a simulator. Finally, we show that quantum chemistry calculations for the five DAE candidates provides a path to achieving large $λ_{\rm max}$ and oscillator strengths by molecular engineering of DAE derivatives. These findings pave the way for future work on applying hybrid quantum-classical approaches to large system optimization and the discovery of novel materials.

quant-ph↗

arXiv2022

Excited state calculations using variational quantum eigensolver with spin-restricted ansätze and automatically-adjusted constraints

The ground and excited state calculations at key geometries, such as the Frank-Condon (FC) and the conical intersection (CI) geometries, are essential for understanding photophysical properties. To compute these geometries on noisy intermediate-scale quantum devices, we proposed a strategy that combined a chemistry-inspired spin-restricted ansatz and a new excited state calculation method called the variational quantum eigensolver under automatically-adjusted constraints (VQE/AC). Unlike the conventional excited state calculation method, called the variational quantum deflation, the VQE/AC does not require the pre-determination of constraint weights and has the potential to describe smooth potential energy surfaces. To validate this strategy, we performed the excited state calculations at the FC and CI geometries of ethylene and phenol blue at the complete active space self-consistent field (CASSCF) level of theory, and found that the energy errors were at most 2 kcal mol$^{-1}$ even on the ibm_kawasaki device.

quant-ph↗

arXiv2022

Analytical energy gradient for state-averaged orbital-optimized variational quantum eigensolvers and its application to a photochemical reaction

Elucidating photochemical reactions is vital to understand various biochemical phenomena and develop functional materials such as artificial photosynthesis and organic solar cells, albeit its notorious difficulty by both experiments and theories. The best theoretical way so far to analyze photochemical reactions at the level of ab initio electronic structure is the state-averaged multi-configurational self-consistent field (SA-MCSCF) method. However, the exponential computational cost of classical computers with the increasing number of molecular orbitals hinders applications of SA-MCSCF for large systems we are interested in. Utilizing quantum computers was recently proposed as a promising approach to overcome such computational cost, dubbed as state-averaged orbital-optimized variational quantum eigensolver (SA-OO-VQE). Here we extend a theory of SA-OO-VQE so that analytical gradients of energy can be evaluated by standard techniques that are feasible with near-term quantum computers. The analytical gradients, known only for the state-specific OO-VQE in previous studies, allow us to determine various characteristics of photochemical reactions such as the conical intersection (CI) points. We perform a proof-of-principle calculation of our methods by applying it to the photochemical cis-trans isomerization of 1,3,3,3-tetrafluoropropene. Numerical simulations of quantum circuits and measurements can correctly capture the photochemical reaction pathway of this model system, including the CI points. Our results illustrate the possibility of leveraging quantum computers for studying photochemical reactions.

physics.chem-ph↗

arXiv2021

Quantum-Classical Computational Molecular Design of Deuterated High-Efficiency OLED Emitters

This study describes a hybrid quantum-classical computational approach for designing synthesizable deuterated $Alq_3$ emitters possessing desirable emission quantum efficiencies (QEs). This design process has been performed on the tris(8-hydroxyquinolinato) ligands typically bound to aluminum in $Alq_3$. It involves a multi-pronged approach which first utilizes classical quantum chemistry to predict the emission QEs of the $Alq_3$ ligands. These initial results were then used as a machine learning dataset for a factorization machine-based model which was applied to construct an Ising Hamiltonian to predict emission quantum efficiencies on a classical computer. We show that such a factorization machine-based approach can yield accurate property predictions for all 64 deuterated $Alq_3$ emitters with 13 training values. Moreover, another Ising Hamiltonian could be constructed by including synthetic constraints which could be used to perform optimizations on a quantum simulator and device using the variational quantum eigensolver (VQE) and quantum approximate optimization algorithm (QAOA) to discover a molecule possessing the optimal QE and synthetic cost. We observe that both VQE and QAOA calculations can predict the optimal molecule with greater than 0.95 probability on quantum simulators. These probabilities decrease to 0.83 and 0.075 for simulations with VQE and QAOA, respectively, on a quantum device, but these can be improved to 0.90 and 0.084 by mitigating readout error. Application of a binary search routine on quantum devices improves these results to a probability of 0.97 for simulations involving VQE and QAOA.

quant-ph↗

arXiv2021

Calculating transition amplitudes by variational quantum deflation

Variational quantum eigensolver (VQE) is an appealing candidate for the application of near-term quantum computers. A technique introduced in [Higgot et al., Quantum 3, 156 (2019)], which is named variational quantum deflation (VQD), has extended the ability of the VQE framework for finding excited states of a Hamiltonian. However, no method to evaluate transition amplitudes between the eigenstates found by the VQD without using any costly Hadamard-test-like circuit has been proposed despite its importance for computing properties of the system such as oscillator strengths of molecules. Here we propose a method to evaluate transition amplitudes between the eigenstates obtained by the VQD avoiding any Hadamard-test-like circuit. Our method relies only on the ability to estimate overlap between two states, so it does not restrict to the VQD eigenstates and applies for general situations. To support the significance of our method, we provide a comprehensive comparison of three previously proposed methods to find excited states with numerical simulation of three molecules (lithium hydride, diazene, and azobenzene) in a noiseless situation and find that the VQD method exhibits the best performance among the three methods. Finally, we demonstrate the validity of our method by calculating the oscillator strength of lithium hydride, comparing results from numerical simulations and real-hardware experiments on the cloud enabled quantum computer IBMQ Rome. Our results illustrate the superiority of the VQD to find excited states and widen its applicability to various quantum systems.

quant-ph↗

arXiv2020

Comet 12P/Pons-Brooks: Identification with Comets C/1385 U1 and C/1457 A1

Comet 12P/Pons-Brooks is an intermediate-period comet (orbital period around 71 years) comparable to 1P/Halley. The comet was seen first in 1812, and then again in 1883 and 1954. The comet was recovered in 2020 an will pass its perihelion passage 2024. We report the unambiguous identification of this comet with the historic comets C/1385 U1 and C/1457 A1; we were able to link both historic apparitions with 12P. The link is also supported by the historic descriptions of its appearance and brightness. Further, we discuss other historical comets for possible relationships with 12P and identify a comet seen in 245 as a probable earliest recorded sighting of 12P/Pons-Brooks.

astro-ph.EP↗

arXiv2020

Applications of Quantum Computing for Investigations of Electronic Transitions in Phenylsulfonyl-carbazole TADF Emitters

A quantum chemistry study of the first singlet (S1) and triplet (T1) excited states of phenylsulfonyl-carbazole compounds, proposed as useful thermally activated delayed fluorescence (TADF) emitters for organic light emitting diode (OLED) applications, was performed with the quantum Equation-Of-Motion Variational Quantum Eigensolver (qEOM-VQE) and Variational Quantum Deflation (VQD) algorithms on quantum simulators and devices. These quantum simulations were performed with double zeta quality basis sets on an active space comprising the highest occupied and lowest unoccupied molecular orbitals (HOMO, LUMO) of the TADF molecules. The differences in energy separations between S1 and T1 ($ΔE_{st}$) predicted by calculations on quantum simulators were found to be in excellent agreement with experimental data. Differences of 16 and 88 mHa with respect to exact energies were found for excited states by using the qEOM-VQE and VQD algorithms, respectively, to perform simulations on quantum devices without error mitigation. By utilizing error mitigation by state tomography to purify the quantum states and correct energy values, the large errors found for unmitigated results could be improved to differences of, at most, 3 mHa with respect to exact values. Consequently, excellent agreement could be found between values of $ΔE_{st}$ predicted by quantum simulations and those found in experiments.

quant-ph↗