Quantum Chemistry Research Institute

Mushrooms from Pleurotus genus produce unique two-component pore-forming toxins consisting of a lipid-binding aegerolysin protein and a membrane-attack complex/perforin (MACPF) domain-containing protein, pleurotolysin B (PlyB). Here, we investigated the interaction between a well-characterized aegerolysin, ostreolysin A6 (OlyA6), and PlyB on membranes composed of ceramide phosphoethanolamine (CPE) and cholesterol (Chol). The binding of PlyB to OlyA6 induced its oligomerization and the formation of porous structures on the membrane. However, the efficiency of oligomerization depended strongly on the density of membrane-bound OlyA6. High OlyA6 density hindered the oligomerization process, resulting predominantly in arc-shaped oligomers rather than ring-shaped structures. This crowding also impaired the pore formation process. Our results suggest that the association of PlyB with OlyA6 occurs on the membrane surface, and the subsequent oligomerization and pore formation are highly regulated by the OlyA6/PlyB molar ratio, consistent with previous observations of inefficient pore formation at high OlyA6/PlyB molar ratios.

The δN formalism has been the major computational tool to study the superhorizon evolution of the scalar type perturbation sourced by scalar fields. Recently, this formalism was generalized to compute an arbitrary scalar, vector, and tensor type perturbations, including the gravitational waves (GWs), sourced by an arbitrary bosonic fields. In this paper, we explain how to use the generalized δN formalism (the gδN formalism), considering a model with U(1) gauge fields as a concrete example. Several new findings on this model and prospects on future gravitational wave experiments are also discussed, including the condition for the two linear polarizations of GWs to have different amplitudes. This paper provides a detailed explanation of our previous paper published in Physical Review Letters. We also discuss the Weinberg's adiabatic mode for an anisotropic background, showing a qualitative difference from the one for the FLRW background.

Global urbanisation is leading to the degradation of living soils, with substantial and direct impacts on climate, biodiversity, food security, and human health. Urban land use policies are beginning to address soil protection. However, they rarely address the depollution and remediation of urban soils and the revitalisation of the agricultural socio-economic fabric, both essential to recover and maintain healthy soils. Instead polluted soils are often managed through further soil sealing (i.e. covering with a plastic ‘geotextile’ layer to isolate it and adding new soil on top). As alternatives, emerging urban communities of practice are currently experimenting with integrated and holistic practices of soil care, such as sourcing urban organic waste streams (food waste, leaves, grass clippings, waste from breweries, ecological paperboard packaging, etc.) for topsoil regeneration or using nature-based approaches (e.g. bioremediation) for the depollution of topsoils. Such practices urgently need enabling and adequate policy frameworks to be mainstreamed and aligned with related policies regarding climate action, green/blue infrastructure and urban food policy plans.

The interaction of light and matter at the single-photon level is of central importance in various fields of physics, including, e.g., condensed matter physics, astronomy, quantum optics, and quantum information. Amplification of such quantum light-matter interaction can be highly beneficial to, e.g., improve device performance, explore novel phenomena, and understand fundamental physics, and has therefore been a long-standing goal. Furthermore, simulation of light-matter interaction in the regime of ultrastrong coupling, where the interaction strength is comparable to the bare frequencies of the uncoupled systems, has also become a hot research topic, and considerable progress has been made both theoretically and experimentally in the past decade. In this review, we provide a detailed introduction of recent advances in amplification of quantum light-matter interaction and simulation of ultrastrong light-matter interaction, particularly in cavity and circuit quantum electrodynamics and in cavity optomechanics.

The potential energy curves (PECs) of the low-lying five 1Σ+ and 1Π states (X1Σ+, C1Σ+, 31Σ+, A1Π, and D1Π states) of a CH+ molecule, an important interstellar molecule, were calculated by the free complement (FC) - local Schrödinger equation (LSE) theory with the direct local sampling scheme. The FC wave functions were constructed based on the chemical formula theory (CFT), whose local characters correspond to the covalent dissociations: C+(2P°(s2p))) + H(2S) of the X1Σ+ and A1Π states and the ionic dissociations: C(1D(s2p2)) + H+ of the C1Σ+ and D1Π states. All the calculated PECs were obtained with satisfying the chemical accuracy, i.e., error less than 1 kcal/mol, as absolute total energy of the Schrödinger equation without any energy shift. The spectroscopic data calculated from the PECs agreed well with both experimental and other accurate theoretical references. We also analyzed the wave functions using the inverse overlap weights proposed by Gallup et al. with the CFT configurations. For the X1Σ+ and A1Π states, the covalent C+(sp2) and C+(p3) configurations played important roles for bond formation. In the small internuclear distances of the C1Σ+, D1Π, and 31Σ+ states, the covalent character was also dominant as a result of the electron charge transfer from C to H+. Thus, the present FC-LSE results not only are accurate but also can provide chemical understanding according to the CFT.

We propose a general approach to implement ultrafast nonadiabatic geometric single- and two-qubit gates by employing counter-rotating effects. This protocol is compatible with most optimal control methods used in previous rotating-wave approximation (RWA) protocols; thus, it is as robust as (or even more robust than) the RWA protocols. Using counter-rotating effects allows us to apply strong drives. Therefore, we can improve the gate speed by 5--10 times compared to the RWA counterpart for implementing high-fidelity ($\ensuremath{\ge}\phantom{\rule{0.2em}{0ex}}99.99\mathrm{%}$) gates. Such an ultrafast evolution (nanoseconds, even picoseconds) significantly reduces the influence of decoherence (e.g., the qubit dissipation and dephasing). Moreover, because the counter-rotating effects no longer induce a gate infidelity (in both the weak and strong driving regimes), we can achieve a higher fidelity compared to the RWA protocols. Therefore, in the presence of decoherence, one can implement ultrafast geometric quantum gates with $\ensuremath{\ge}\phantom{\rule{0.2em}{0ex}}99\mathrm{%}$ fidelities.

Hyperon decays present a promising alternative for extracting $\vert V_{us} \vert$ from lattice QCD combined with experimental measurements. Currently $\vert V_{us} \vert$ is determined from the kaon decay widths and a lattice calculation of the associated form factor. In this proceeding, I will present preliminary work on a lattice determination of the hyperon mass spectrum. I will additionally summarize future goals in which we will calculate the hyperon transition matrix elements, which will provide an alternative means for accessing $\vert V_{us} \vert$. This work is based on a particular formulation of SU(2) chiral perturbation theory for hyperons; determining the extent to which this effective field theory converges is instrumental in understanding the limits of its predictive power, especially since some hyperonic observables are difficult to calculate near the physical pion mass (e.g., hyperon-to-nucleon form factors), and thus the use of heavier than physical pion masses is likely to yield more precise results when combined with extrapolations to the physical point.

High performance global exploration of isomers and isomerization channels on the quantum chemical potential energy surface (PES) is performed for H5 C2 NO2 by using the scaled hypersphere search-anharmonic downward distortion following (SHS-ADDF) method. A multi-node operation, NeoGRRM, has achieved high performance exploration calculations for the large system by submitting SHS-ADDF sub-jobs into many cores in parallel and unifying the results of sub-jobs into the total lists of the main-job. Global exploration of equilibrium (EQ) and transition-state structures at the level of B3LYP/6-31G(d) gave 3210 EQs and 23278 TSs. Nine compounds were found in the low energy regions of 0-100 kJ/mol; the lowest energy compound is N-methylcarbamic acid, the second is methyl carbamate, and the third is glycine (the most fundamental amino acid). Interconversion pathways between the conformers of each of the low energy compounds were surveyed. Isomerization channels around glycine were explored in detail. The lowest energy barriers around some of the EQs turned to be negative after zero-point energy corrections. This indicates that those structures cannot exist as independent structures because they spontaneously collapse into more stable structures. The global PES search showed various interesting dissociating channels which indicate synthon reaction pathways in the reverse directions.

A variational theory called free-complement (FC) ${s}_{ij}$ theory for solving the Schr\odinger equation of atoms and molecules using only one- and two-electron integrals over Slater or Gaussian functions is proposed. It is derived from the scaled Schr\odinger equation [Phys Rev. Lett. 93, 030403 (2004)] by replacing the two-electron part ${r}_{ij}$ of the scaling $g$ operator with ${s}_{ij}={r}_{ij}^{2}$, both of which solve the divergence difficulty inherent to the original Schr\odinger equation by avoiding the interelectron collisions. The ${s}_{ij}$ function can be rewritten with only one-electron functions so that when the initial wave function of the FC theory is composed of only one-electron functions, the FC wave function including ${s}_{ij}$ can be rewritten with only one-electron functions. Therefore, the variational calculations of the FC ${s}_{ij}$ theory can be performed with only one- and two-electron integrals. However, in comparison with the ${r}_{ij}$ function, the ${s}_{ij}$ function behaves less efficiently when two electrons come close to each other: the electron-electron cusp condition is not satisfied with the FC ${s}_{ij}$ theory, though the wave function has explicit ${r}_{ij}$ dependence. On the other hand, the electron-nuclear cusp condition is satisfied, even with the Gaussian functions, for the presence of the electron-nuclear function ${r}_{iA}$ in the $g$ operator. Test applications of the FC ${s}_{ij}$ theory were done to He, Li, and the $^{5}S^{\mathrm{o}} {\mathit{sp}}^{3}$ state of carbon atom and to hydrogen molecule using the local-molecular orbital (MO)- and valence bond (VB)-type initial functions. We examined both Slater and Gaussian functions. As the order of the FC theory increased, the wave functions were improved and the energies approached from a few kcal/mol to less than 1 kcal/mol accuracies relative to the known exact values. Thus, with the FC ${s}_{ij}$ theory, the Schr\odinger equation was solved to less than 1 kcal/mol accuracy for all the systems examined. The costs for the ${s}_{ij}$ calculations were much smaller than those of the ${r}_{ij}$ theory. However, for the $^{5}S^{\mathrm{o}} {\mathit{sp}}^{3}$ state of the carbon atom, we observed that the convergence rate became slow when the calculation came close to $\ensuremath{\sim}1$ kcal/mol accuracy. This suggests that for the FC ${s}_{ij}$ theory, the calculations would become easier if the required accuracy is within a few kcal/mol for the absolute energy. Actually, what we need in chemical studies are mostly related to the difference energy, whose accuracy could be better than that of the absolute energy with the robust variational method. Two lines of future studies were suggested.

The possibility to manipulate quantum coherence and interference, apart from its fundamental interest in quantum mechanics, is essential for controlling nonlinear optical processes such as high harmonic generation, multiphoton absorption, and stimulated Raman scattering. We show, analytically and numerically, how a nonlinear optical process via resonance Raman scattering (RRS) can be manipulated in a four-level double-Λ system by using pulsed laser fields. We find that two simultaneously excited RRS paths involved in the system can generate an ultimately destructive interference in the broad-bandwidth-limit regime. This, in turn, reduces the four-level system to an equivalent three-level system in a V configuration capable of naturally vanishing RRS effects. We further show that this counterintuitive phenomenon, i.e., the RRS vanishing, can be prevented by transferring a modulated phase of the laser pulse to the system at resonance frequencies. This work demonstrates a clear signature of both quantum destructive and constructive interference by actively controlling resonant multiphoton processes in multilevel quantum systems, and it therefore has potential applications in nonlinear optics, quantum control, and quantum information science.