Implementation of the Time-Dependent Complete-Active-Space Self-Consistent-Field Method for Diatomic Molecules.

We present a computational approach that implements the time-dependent complete-active-space self-consistent-field method, as introduced in [Phys. Rev. A 88, 023402 (2013)]. Our implementation addresses the challenge of diatomic molecules subjected to an intense laser pulse by considering the full dimensionality of the problem using prolate spheroidal coordinates. The method incorporates the gauge-invariant frozen-core approximation, boosts the evaluation of the electron-electron interaction term using finite-element discrete-variable representation with Neumann expansion, and utilizes an exponential time differencing scheme tailored for the stable propagation of the stiff nonlinear orbital functions. We have successfully applied this methodology to study high-harmonic generation in diatomic molecules such as H2, LiH, and N2, shedding light on the impact of electron correlations in these systems.

Control of Ion-Photoelectron Entanglement and Coherence Via Rabi Oscillations.

We report a theoretical investigation of photoionization by a pair of coherent, ultrashort, fundamental and second-harmonic extreme-ultraviolet pulses, where the photon energies are selected to yield the same photoelectron energy for ionization of two different subshells. This choice implies that the fundamental energy is equal to the difference in energy of the ionic states and that they are therefore coupled by the fundamental photon. By deriving analytical expressions using the essential-states approach, we show that this Rabi coupling creates coherence between the two photoelectron wave packets, which would otherwise be incoherent. We analyze how the coupling is affected by the parameters, such as relative phase, pulse width, delay between the two pulses, Rabi coupling strength, and photoelectron energy. Our discussion mostly considers Ne 2p and 2s photoionization, but it is generally valid for many other quantum systems where photoionization from two different shells is observed.

Use of Erfgau Potential for Simulations of Multielectron Dynamics in Intense Laser Pulses.

We propose the use of the erfgau potential as a smooth alternative to the pure Coulomb potential between nuclei and electrons in simulating the dynamics of electrons within atoms and molecules driven by high-intensity laser pulses. Even without the sophistication of pseudopotentials, by utilizing a well-designed simple approximate potential, it is possible to make the simulations computationally less demanding while keeping accuracy. By employing the erfgau potential designed for the stationary state of hydrogen-like atoms, we demonstrate that it is possible to simulate not only the high harmonic generation from a hydrogen atom but also that of multielectron systems, including molecules.

Knockdown of optineurin controls C2C12 myoblast differentiation via regulating myogenin and MyoD expressions.

Mutations in optineurin (OPTN) have been identified in a small proportion of sporadic and familial amyotrophic lateral sclerosis (ALS) cases. Recent evidences suggest that OPTN would be involved in not only the pathophysiological mechanisms of motor neuron death of ALS but also myofiber degeneration of sporadic inclusion body myositis. However, the detailed role of OPTN in muscle remains unclear. Initially, we showed that OPTN expression levels were significantly increased in the denervated muscles of mice, suggesting that OPTN may be involved in muscle homeostasis. To reveal the molecular role of OPTN in muscle atrophy, we used cultured C2C12 myotubes treated with tumor necrosis factor-like inducer of apoptosis (TWEAK) as an in vitro model of muscle atrophy. Our data showed that OPTN had no effect on the process of muscle atrophy in this model. On the other hand, we found that myogenic differentiation was affected by OPTN. Immunoblotting analysis showed that OPTN protein levels gradually decreased during C2C12 differentiation. Furthermore, OPTN knockdown inhibited C2C12 differentiation, accompanied by reduction of mRNA and protein expression levels of myogenin and MyoD. These findings suggested that OPTN may have a novel function in muscle homeostasis and play a role in the pathogenesis of neuromuscular diseases.

Time-dependent optimized coupled-cluster method for multielectron dynamics. IV. Approximate consideration of the triple excitation amplitudes.

We present a cost-effective treatment of the triple excitation amplitudes in the time-dependent optimized coupled-cluster (TD-OCC) framework called TD-OCCDT(4) for studying intense laser-driven multielectron dynamics. It considers triple excitation amplitudes correct up to the fourth-order in many-body perturbation theory and achieves a computational scaling of O(N7), with N being the number of active orbital functions. This method is applied to the electron dynamics in Ne and Ar atoms exposed to an intense near-infrared laser pulse with various intensities. We benchmark our results against the TD complete-active-space self-consistent field (TD-CASSCF), TD-OCC with double and triple excitations (TD-OCCDT), TD-OCC with double excitations (TD-OCCD), and TD Hartree-Fock (TDHF) methods to understand how this approximate scheme performs in describing nonperturbatively nonlinear phenomena, such as field-induced ionization and high-harmonic generation. We find that the TD-OCCDT(4) method performs equally well as the TD-OCCDT method, almost perfectly reproducing the results of the fully correlated TD-CASSCF with a more favorable computational scaling.

Time-dependent optimized coupled-cluster method for multielectron dynamics. III. A second-order many-body perturbation approximation.

We report successful implementation of the time-dependent second-order many-body perturbation theory using optimized orthonormal orbital functions called time-dependent optimized second-order many-body perturbation theory to reach out to relatively larger chemical systems for the study of intense-laser-driven multielectron dynamics. We apply this method to strong-field ionization and high-order harmonic generation of Ar. The calculation results are benchmarked against ab initio time-dependent complete-active-space self-consistent field, time-dependent optimized coupled-cluster double, and time-dependent Hartree-Fock methods, as well as a single active electron model to explore the role of electron correlation.

Time-dependent optimized coupled-cluster method for multielectron dynamics. II. A coupled electron-pair approximation.

We report the implementation of a cost-effective approximation method within the framework of the time-dependent optimized coupled-cluster (TD-OCC) method [T. Sato et al., J. Chem. Phys. 148, 051101 (2018)] for real-time simulations of intense laser-driven multielectron dynamics. The method, designated as TD-OCEPA0, is a time-dependent extension of the simplest version of the coupled-electron pair approximation with optimized orbitals [U. Bozkaya and C. D. Sherrill, J. Chem. Phys. 139, 054104 (2013)]. It is size extensive, gauge invariant, and computationally much more efficient than the TD-OCC method with double excitations. We employed this method to simulate the electron dynamics in Ne and Ar atoms exposed to intense near infrared laser pulses with various intensities. The computed results, including high-harmonic generation spectra and ionization yields, are compared with those of various other methods ranging from uncorrelated time-dependent Hartree-Fock to fully correlated (within the active orbital space) time-dependent complete-active-space self-consistent field (TD-CASSCF). The TD-OCEPA0 results show good agreement with TD-CASSCF ones for moderate laser intensities. For higher intensities, however, TD-OCEPA0 tends to overestimate the correlation effect, as occasionally observed for CEPA0 in the ground-state correlation energy calculations.

Complete Characterization of Phase and Amplitude of Bichromatic Extreme Ultraviolet Light.

Intense, mutually coherent beams of multiharmonic extreme ultraviolet light can now be created using seeded free-electron lasers, and the phase difference between harmonics can be tuned with attosecond accuracy. However, the absolute value of the phase is generally not determined. We present a method for determining precisely the absolute phase relationship of a fundamental wavelength and its second harmonic, as well as the amplitude ratio. Only a few easily calculated theoretical parameters are required in addition to the experimental data.

Polarization-Resolved Study of High Harmonics from Bulk Semiconductors.

The polarization property of high harmonics from gallium selenide is investigated using linearly polarized midinfrared laser pulses. With a high electric field, the perpendicular polarization component of the odd harmonics emerges, which is not present with a low electric field and cannot be explained by the perturbative nonlinear optics. A two-dimensional single-band model is developed to show that the anisotropic curvature of an energy band of solids, which is pronounced in an outer part of the Brillouin zone, induces the generation of the perpendicular odd harmonics. This model is validated by three-dimensional quantum mechanical simulations, which reproduce the orientation dependence of the odd-order harmonics. The quantum mechanical simulations also reveal that the odd- and even-order harmonics are produced predominantly by the intraband current and interband polarization, respectively. These experimental and theoretical demonstrations clearly show a strong link between the band structure of a solid and the polarization property of the odd-order harmonics.

Communication: Time-dependent optimized coupled-cluster method for multielectron dynamics.

Time-dependent coupled-cluster method with time-varying orbital functions, called time-dependent optimized coupled-cluster (TD-OCC) method, is formulated for multielectron dynamics in an intense laser field. We have successfully derived the equations of motion for CC amplitudes and orthonormal orbital functions based on the real action functional, and implemented the method including double excitations (TD-OCCD) and double and triple excitations (TD-OCCDT) within the optimized active orbitals. The present method is size extensive and gauge invariant, a polynomial cost-scaling alternative to the time-dependent multiconfiguration self-consistent-field method. The first application of the TD-OCC method of intense-laser driven correlated electron dynamics in Ar atom is reported.

High-Harmonic Generation Enhanced by Dynamical Electron Correlation.

We theoretically study multielectron effects in high-harmonic generation (HHG), using all-electron first-principles simulations for a one-dimensional model atom. In addition to the usual plateau and cutoff (from a cation in the present case, since the neutral is immediately ionized), we find a prominent resonance peak far above the plateau and a second plateau extended beyond the first cutoff. These features originate from the dication response enhanced by orders of magnitude due to the action of the Coulomb force from the rescattering electron, and, hence, are a clear manifestation of electron correlation. Although the present simulations are done in 1D, the physical mechanism underlying the dramatic enhancement is expected to hold also for three-dimensional real systems. This will provide new possibilities to explore dynamical electron correlation in intense laser fields using HHG, which is usually considered to be of single-electron nature in most cases.

A fully general time-dependent multiconfiguration self-consistent-field method for the electron-nuclear dynamics.

We present a fully general time-dependent multiconfiguration self-consistent-field method to describe the dynamics of a system consisting of arbitrarily different kinds and numbers of interacting fermions and bosons. The total wave function is expressed as a superposition of different configurations constructed from time-dependent spin-orbitals prepared for each particle kind. We derive equations of motion followed by configuration-interaction (CI) coefficients and spin-orbitals for general, not restricted to full-CI, configuration spaces. The present method provides a flexible framework for the first-principles theoretical study of, e.g., correlated multielectron and multinucleus quantum dynamics in general molecules induced by intense laser fields and attosecond light pulses.

Molecular characterization of cancer reveals interactions between ionizing radiation and chemicals on rat mammary carcinogenesis.

Although various mechanisms have been inferred for combinatorial actions of multiple carcinogens, these mechanisms have not been well demonstrated in experimental carcinogenesis models. We evaluated mammary carcinogenesis initiated by combined exposure to various doses of radiation and chemical carcinogens. Female rats at 7 weeks of age were γ-irradiated (0.2-2 Gy) and/or exposed to 1-methyl-1-nitrosourea (MNU) (20 or 40 mg/kg, single intraperitoneal injection) or 2-amino-1-methyl-6-phenylimidazo[4,5-b]pyridine (PhIP) (40 mg/kg/day by gavage for 10 days) and were observed until 50 weeks of age. The incidence of mammary carcinoma increased steadily as a function of radiation dose in the absence of chemicals; mathematical analysis supported an additive increase when radiation was combined with a chemical carcinogen, irrespective of the chemical species and its dose. Hras mutations were characteristic of carcinomas that developed after chemical carcinogen treatments and were overrepresented in carcinomas induced by the combination of radiation and MNU (but not PhIP), indicating an interaction of radiation and MNU at the level of initiation. The expression profiles of seven classifier genes, previously shown to distinguish two classes of rat mammary carcinomas, categorized almost all examined carcinomas that developed after individual or combined treatments with radiation (1 Gy) and chemicals as belonging to a single class; more comprehensive screening using microarrays and a separate test sample set failed to identify differences in gene expression profiles among these carcinomas. These results suggest that a complex, multilevel interaction underlies the combinatorial action of radiation and chemical carcinogens in the experimental model.

A genotoxic stress-responsive miRNA, miR-574-3p, delays cell growth by suppressing the enhancer of rudimentary homolog gene in vitro.

MicroRNA (miRNA) is a type of non-coding RNA that regulates the expression of its target genes by interacting with the complementary sequence of the target mRNA molecules. Recent evidence has shown that genotoxic stress induces miRNA expression, but the target genes involved and role in cellular responses remain unclear. We examined the role of miRNA in the cellular response to X-ray irradiation by studying the expression profiles of radio-responsive miRNAs and their target genes in cultured human cell lines. We found that expression of miR-574-3p was induced in the lung cancer cell line A549 by X-ray irradiation. Overexpression of miR-574-3p caused delayed growth in A549 cells. A predicted target site was detected in the 3'-untranslated region of the enhancer of the rudimentary homolog (ERH) gene, and transfected cells showed an interaction between the luciferase reporter containing the target sequences and miR-574-3p. Overexpression of miR-574-3p suppressed ERH protein production and delayed cell growth. This delay was confirmed by knockdown of ERH expression. Our study suggests that miR-574-3p may contribute to the regulation of the cell cycle in response to X-ray irradiation via suppression of ERH protein production.

Radio-fluorogenic nanoclay gel dosimeters with reduced linear energy transfer dependence for carbon-ion beam radiotherapy.

PURPOSE: The precise assessment of the dose distribution of high linear energy transfer (LET) radiation remains a challenge, because the signal of most dosimeters will be saturated due to the high ionization density. Such measurements are particularly important for heavy-ion beam cancer therapy. On this basis, the present work examined the high LET effect associated with three-dimensional gel dosimetry based on radiation-induced chemical reactions. The purpose of this study was to create an ion beam radio-fluorogenic gel dosimeter with a reduced effect of LET. METHODS: Nanoclay radio-fluorogenic gel (NC-RFG) dosimeters were prepared, typically containing 100 µM dihydrorhodamine 123 (DHR123) and 2.0 wt% nanoclay together with catalytic additives promoting Fenton or Fenton-like reactions. The radiological properties of NC-RFG dosimeters having different compositions in response to a carbon-ion beam were investigated using a fluorescence gel scanner. RESULTS: An NC-RFG dosimeter capable of generating a fluorescence intensity distribution reflecting the carbon-ion beam dose profile was obtained. It was clarified that the reduction of the unfavorable LET dependence results from an acceleration of the reactions between DHR123 and H2 O2 , which is a molecular radiolysis product. The effects of varying the preparation conditions on the radiological properties of these gels were also examined. The optimum H2 O2 catalyst was determined to include 1 mM Fe3+ ions, and the addition of 100 mM pyridine was also found to increase the sensitivity. CONCLUSIONS: This technique allows the first-ever evaluation of the depth-dose profile of a carbon-ion beam at typical therapeutic levels of several Gy without LET effect.

Application of the symbolic regression program AI-Feynman to psychology.

The discovery of hidden laws in data is the core challenge in many fields, from the natural sciences to the social sciences. However, this task has historically relied on human intuition and experience in many areas, including psychology. Therefore, discovering laws using artificial intelligence (AI) has two significant advantages. First, it makes it possible to detect laws that humans cannot discover. Second, it will help construct more accurate theories. An AI called AI-Feynman was released in a very different field, and it performed impressively. Although AI-Feynman was initially designed to discover laws in physics, it can also work well in psychology. This research aims to examine whether AI-Feynman can be a new data analysis method for inter-temporal choice experiments by testing whether it can discover the hyperbolic discount model as a discount function. An inter-temporal choice experiment was conducted to accomplish these objectives, and the data were input into AI-Feynman. As a result, seven discount function candidates were proposed by AI-Feynman. One candidate was the hyperbolic discount model, which is currently considered the most accurate. The three functions of the root-mean-squared errors were superior to the hyperbolic discount model. Moreover, one of the three candidates was more "hyperbolic" than the standard hyperbolic discount function. These results indicate two things. One is that AI-Feynman can be a new data analysis method for inter-temporal choice experiments. The other is that AI-Feynman can discover discount functions that humans cannot find.

Reversible Brain Atrophy in Cryptogenic New-onset Refractory Status Epilepticus.

Cryptogenic new-onset refractory status epilepticus (C-NORSE) is a neurologic emergency condition characterized by refractory status epilepticus (RSE) of unknown cause. Brain atrophy in a setting of C-NORSE is usually irreversible. A 33-year-old woman who was highly suspected of C-NORSE once showed mild frontotemporal atrophy on brain magnetic resonance imaging (MRI), but follow-up MRI revealed recovery of the brain atrophy. Her cognitive function also gradually improved, with a reduction in seizure frequency. Early initiation of intensive immunotherapy with anti-seizure medications may have minimized irreversible brain damage associated with RSE, resulting in a relatively good outcome.

Resolving vibrational wave-packet dynamics of D2(+) using multicolor probe pulses.

We demonstrate the generation and real-time observation of the vibrational wave packet of D(2)(+) by using a sub-10-fs extreme UV high-harmonic pump pulse and a three-color probe laser pulse whose wavelength ranges from near-IR to vacuum UV. This multicolor pump-probe scheme can provide us with a powerful experimental tool for investigating a variety of wave packets evolving with a time scale of ~20 fs.

Competition of resonant and nonresonant paths in resonance-enhanced two-photon single ionization of He by an ultrashort extreme-ultraviolet pulse.

We theoretically study the pulse-width dependence of the photoelectron angular distribution (PAD) from the resonance-enhanced two-photon single ionization of He by femtosecond (≲20 fs) extreme-ultraviolet pulses, based on the time-dependent perturbation theory and simulations with the full time-dependent Schrödinger equation. In particular, we focus on the competition between resonant and nonresonant ionization paths, which leads to the relative phase δ between the S and D wave packets distinct from the corresponding scattering phase shift difference. When the spectrally broadened pulse is resonant with an excited level, the competition varies with pulse width, and, therefore, δ and the PAD also change with it. On the other hand, when the Rydberg manifold is excited, δ and the PAD do not much vary with the pulse width, except for the very short-pulse regime.

Amplitude and phase reconstruction of electron wave packets for probing ultrafast photoionization dynamics.

Ultrafast atomic processes, such as excitation and ionization occurring on the femtosecond or shorter time scale, were explored by employing attosecond high-harmonic pulses. With the absorption of a suitable high-harmonic photon a He atom was ionized, or resonantly excited with further ionization by absorbing a number of infrared photons. The electron wave packets liberated by the two processes generated an interference containing the information on ultrafast atomic dynamics. The attosecond electron wave packet, including the phase, from the ground state was reconstructed first and, subsequently, that from the 1s3p state was retrieved by applying the holographic technique to the photoelectron spectra comprising the interference between the two ionization paths. The reconstructed electron wave packet revealed details of the ultrafast photoionization dynamics, such as the instantaneous two-photon ionization rate.