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We propose a protocol for the preparation of high-fidelity entangled cat states with composite pulses. The physical model contains two Kerr-nonlinear resonators and a cavity. By properly designing the parameters, each Kerr-nonlinear resonator is confined in the cat-state subspace and the entangled cat states can be generated efficiently. We introduce composite two-photon drives with multiple amplitudes and frequencies to improve the fidelity of the entangled cat states in the presence of parameter errors. The performance of the protocol is estimated by taking into account the parametric errors and decoherence. Numerical simulation results show that the protocol is insensitive to timing error and detuning error, and has strong robustness to decoherence. We hope the protocol may provide a method for preparing stable entangled cat states., Comment: 9 pages, 7 figures, comments are welcome

It is well known that in the quantum Rabi model, a three-photon resonance occurs when the cavity field bare frequency is about 1/3 of the atomic transition frequency. In this manuscript, we show that the resonance can also be generated in the absence of the 1/3 condition by employing an artificial atom with tunable transition frequency. To realize the protocol, the modulation frequency should be comparable to the cavity frequency in order to induce a counter-rotating interaction in the effective Hamiltonian. In this way, three-photon Rabi oscillations can be observed in a small-detuning regime, thus avoiding the excitation of high-energy states. We derive an effective Hamiltonian (equivalent to the anisotropic Rabi model Hamiltonian) to determine the magnitude of the energy splitting and the resonance position. Numerical simulations results show that the protocol not only generates a three-photon resonance, but also has a detectable output photon flux. We hope the protocol can be exploited for the realization of Fock-state sources and the generation of multiparticle entanglement., Comment: 10 pages, 10 figures, comments are welcome

Cat-state qubits formed by photonic coherent states are a promising candidate for realizing fault-tolerant quantum computing. Such logic qubits have a biased noise channel that the bit-flip error dominates over all the other errors. In this manuscript, we propose an optimally robust protocol using the control method of shortcuts to adiabaticity to realize a nearly perfect population inversion in a cat-state qubit. We construct a shortcut based on the Lewis-Riesenfeld invariant and examine the stability versus different types of perturbations for the fast and robust population inversion. Numerical simulations demonstrate that the population inversion can be mostly insensitive to systematic errors in our protocol. Even when the parameter imperfection rate for bit-flip control is $20\%$, the final population of the target state can still reach $\geq 99\%$. The optimally robust control provides a feasible method for fault-tolerant and scalable quantum computation., Comment: 9 pages, 8 figures, comments are welcome

We describe the implementation details of periodic local coupled-cluster theory with single and double excitations (CCSD) and perturbative triple excitations [CCSD(T)] using local natural orbitals (LNOs) and $k$-point symmetry. We discuss and compare several choices for orbital localization, fragmentation, and LNO construction. By studying diamond and lithium, we demonstrate that periodic LNO-CC theory can be applied with equal success to both insulators and metals, achieving speedups of two to three orders of magnitude even for moderately sized $k$-point meshes. Our final predictions of the equilibrium cohesive energy, lattice constant, and bulk modulus for diamond and lithium are in good agreement with previous theoretical predictions and experimental results., Comment: 11 pages, 9 figures, 2 tables

In this work, we introduce a differentiable implementation of the local natural orbital coupled cluster (LNOCC) method within the automatic differentiation framework of the PySCFAD package. The implementation is comprehensively tuned for enhanced performance, which enables the calculation of first-order static response properties on medium-sized molecular systems using coupled cluster theory with single, double, and perturbative triple excitations [CCSD(T)]. We evaluate the accuracy of our method by benchmarking it against the canonical CCSD(T) reference for nuclear gradients, dipole moments, and geometry optimizations. In addition, we demonstrate the possibility of property calculations for chemically interesting systems through the computation of bond orders and M\"ossbauer spectroscopy parameters for a [NiFe]-hydrogenase active site model, along with the simulation of infrared (IR) spectra via ab initio LNO-CC molecular dynamics for a protonated water hexamer.

Cat-state qubits formed by photonic cat states have a biased noise channel, i.e., one type of error dominates over all the others. We demonstrate that such biased-noise qubits are also promising for error-tolerant simulations of the quantum Rabi model (and its varieties) by coupling a cat-state qubit to an optical cavity. Using the cat-state qubit can effectively enhance the counter-rotating coupling, allowing us to explore several fascinating quantum phenomena relying on the counter-rotating interaction. Moreover, another benefit from biased-noise cat qubits is that the two main error channels (frequency and amplitude mismatches) are both exponentially suppressed. Therefore, the simulation protocols are robust against parameter errors of the parametric drive which determines the projection subspace. We analyze three examples: (i) collapse and revivals of quantum states; (ii) hidden symmetry and tunneling dynamics; and (iii) pair-cat-code computation., Comment: 7 pages, 7 figures

The adsorption of CO on the surface of MgO has long been a model problem in surface chemistry. Here, we report periodic Gaussian-based calculations for this problem using second-order perturbation theory (MP2) and coupled-cluster theory with single and double excitations (CCSD) and perturbative triple excitations [CCSD(T)], with the latter two performed using a recently developed extension of the local natural orbital approximation to problems with periodic boundary conditions. The low cost of periodic local correlation calculations allows us to calculate the full CCSD(T) binding curve of CO approaching the surface of MgO (and thus the adsorption energy) and the two-dimensional potential energy surface (PES) as a function of the distance from the surface and the CO stretching coordinate. From the PES, we obtain the fundamental vibrational frequency of CO on MgO, whose shift from the gas phase value is a common experimental probe of surface adsorption. We find that CCSD(T) correctly predicts a positive frequency shift upon adsorption of $+14.7~\textrm{cm}^{-1}$, in excellent agreement with the experimental shift of $+14.3~\textrm{cm}^{-1}$. We use our CCSD(T) results to assess the accuracy of MP2, CCSD, and several density functional theory (DFT) approximations, including exchange correlation functionals and dispersion corrections. We find that MP2 and CCSD yield reasonable binding energies and frequency shifts, whereas many DFT calculations overestimate the magnitude of the adsorption energy by $5$ -- $15$~kJ/mol and predict a negative frequency shift of about $-20~\textrm{cm}^{-1}$, which we attribute to self-interaction-induced delocalization errors that are mildly ameliorated with hybrid functionals. Our findings highlight the accuracy and computational efficiency of the periodic local correlation for the simulation of surface chemistry with accurate wavefunction methods., Comment: 6 pages, 3 figures, 1 tables (excluding references and SI)

First-principles calculations are a cornerstone of modern surface science and heterogeneous catalysis. However, accurate reaction energies and barrier heights are frequently inaccessible due to the approximations demanded by the large number of atoms. Here we combine developments in local correlation and periodic correlated wavefunction theory to solve the many-electron Schr\"odinger equation for molecules on surfaces with chemical accuracy, commonly defined as 1~kcal/mol. As a demonstration, we study water on the surface of \ce{Al2O3} and \ce{TiO2}, two prototypical and industrially important metal oxides for which we obtain converged energies at the level of coupled-cluster theory with single, double, and perturbative triple excitations [CCSD(T)], commonly known as the "gold-standard" in molecular quantum chemistry. We definitively resolve the energetics associated with water adsorption and dissociation, enabling us to address recent experiments and to analyze the errors of more commonly used approximate theories., Comment: 6 pages (w/o SI), 3 figures

We develop a local correlation variant of auxiliary field quantum Monte Carlo (AFQMC) that is based on local natural orbitals (LNO-AFQMC). In LNO-AFQMC, independent AFQMC calculations are performed for each localized occupied orbital using a truncated set of tailored orbitals. Because the size of this space does not grow with system size for a target accuracy, the method has linear scaling. Applying LNO AFQMC to molecular problems containing a few hundred to a thousand orbitals, we demonstrate convergence of total energies with significantly reduced costs. The savings are more significant for larger systems and larger basis sets. However, even for our smallest system studied, we find that LNO-AFQMC is cheaper than canonical AFQMC, in contrast with many other reduced-scaling methods. Perhaps most significantly, we show that energy differences converge much more quickly than total energies, making the method ideal for applications in chemistry and material science. Our work paves the way for linear scaling AFQMC calculations of strongly correlated systems, which would have a transformative effect on ab initio quantum chemistry., Comment: 9 pages, 2 figures

In this work, we develop a supervised learning model for implementing robust quantum control in composite-pulse systems, where the training parameters can be either phases, detunings, or Rabi frequencies. This model exhibits great resistance to all kinds of systematic errors, including single, multiple, and time-varying errors. We propose a modified gradient descent algorithm for adapting the training of phase parameters, and show that different sampling methods result in different robust performances. In particular, there is a trade-off between high fidelity and robustness for a given number of training parameters, and both can be simultaneously enhanced by increasing the number of training parameters (pulses). For its applications, we demonstrate that the current model can be used for achieving high-fidelity arbitrary superposition states and universal quantum gates in a robust manner. This work provides a highly efficient learning model for fault-tolerant quantum computation by training various physical parameters., Comment: 19 pages, comments welcome!

Achieving kJ/mol accuracy in the cohesive energy of molecular crystals, as necessary for crystal structure prediction and the resolution of polymorphism, is an ongoing challenge in computational materials science. Here, we evaluate the performance of second-order M{\o}ller-Plesset perturbation theory (MP2), including its spin-component scaled models, by calculating the cohesive energies of the 23 molecular crystals contained in the X23 dataset. Our calculations are performed with periodic boundary conditions and Brillouin zone sampling, and we converge results to the thermodynamic limit and the complete basis set limit to an accuracy of about 1 kJ/mol (0.25 kcal/mol), which is rarely achieved in previous MP2 calculations of molecular crystals. Comparing to experimental cohesive energies, we find that MP2 has a mean absolute error of 12.9 kJ/mol, which is comparable to that of DFT using the PBE functional and TS dispersion correction. Separate scaling of the opposite-spin and same-spin components of the correlation energy, with parameters previously determined for molecular interactions, reduces the mean absolute error to 9.5 kJ/mol, and reoptimizing the spin-component scaling parameters for the X23 set further reduces the mean absolute error to 7.5 kJ/mol.

Using a systematic ab initio quantum many-body approach that goes beyond low-energy models, we directly compute the superconducting pairing order of several doped cuprate materials and structures. We find that we can correctly capture two well-known trends: the pressure effect, where pairing order increases with intra-layer pressure, and the layer effect, where the pairing order varies with the number of copper-oxygen layers. From these calculations, we observe that the strength of superexchange and the covalency at optimal doping are the best descriptors of the maximal pairing order. Our microscopic analysis further identifies short-range copper spin fluctuations, together with multi-orbital charge fluctuations, as central to the pairing trends. Our work illustrates the possibility of a quantitative computational understanding of unconventional high-temperature superconducting materials., Comment: 10 pages, 5 figures, with supplementary materials

Obtaining the atomistic structure and dynamics of disordered condensed phase systems from first principles remains one of the forefront challenges of chemical theory. Here we exploit recent advances in periodic electronic structure to show that, by leveraging transfer learning starting from lower tier electronic structure methods, one can obtain machine learned potential energy surfaces for liquid water from the higher tier AFQMC, CCSD, and CCSD(T) approaches using $\le$200 energies. By performing both classical and path integral molecular dynamics simulations on these machine learned potential energy surfaces we uncover the interplay of dynamical electron correlation and nuclear quantum effects across the entire liquid range of water while providing a general strategy for efficiently utilizing periodic correlated electronic structure methods to explore disordered condensed phase systems.

Spin squeezing is one of the most attractive methods for realizing high-precision metrology. In this paper, we propose a protocol for generating spin squeezing in an atomic ensemble via a fully quantum degenerate parametric amplifier. We discuss the properties of generating spin squeezing with and without driving the pump cavity. Numerical simulation results show that the generated spin squeezing strength is sizable, and is able to be comparable to that obtained using a two-axis twisting (TAT) model. Moreover, we demonstrate that the protocol is experimentally feasible by introducing the corresponding experimental parameters. Therefore, the proposed protocol provides a promising approach to realize spin squeezing in photon-spin coupling systems.

Light-sheet fluorescence microscopy (LSFM) makes use of a thin plane of light to optically section and image transparent tissues or organisms {\it{in vivo}}, which has the advantages of fast imaging speed and low phototoxicity. In this paper, we have employed light-sheet microscopy to investigate the polarization effects on fluorescence emission of zebrafish neurons via modifying the electric oscillation orientation of the excitation light. The intensity of the fluorescence emission from the excited zebrafish larvae follows a cosine square function with respect to the polarization state of the excitation light and reveals a 40$\%$ higher fluorescence emission when the polarization orientation is orthogonal to the illumination and detection axes. Through registration and subtraction of fluorescence images under different polarization states, we have demonstrated that most of the enhanced fluorescence signals are from the nerve cells rather than the extracellular substance. This provides us a way to distinguish the cell boundaries and observe the organism structures with improved contrast and resolution.

We study the performance of spin-component-scaled second-order M{\o}ller-Plesset perturbation theory (SCS-MP2) for the prediction of the lattice constant, bulk modulus, and cohesive energy of 12 simple, three-dimensional, covalent and ionic semiconductors and insulators. We find that SCS-MP2 and the simpler scaled opposite-spin MP2 (SOS-MP2) yield predictions that are significantly improved over the already good performance of MP2. Specifically, when compared to experimental values with zero-point vibrational corrections, SCS-MP2 (SOS-MP2) yields mean absolute errors of 0.015 (0.017) {\AA} for the lattice constant, 3.8 (3.7) GPa for the bulk modulus, and 0.06 (0.08) eV for the cohesive energy, which are smaller than those of leading density functionals by about a factor of two or more. We consider a reparameterization of the spin scaling parameters and find that the optimal parameters for these solids are very similar to those already in common use in molecular quantum chemistry, suggesting good transferability and reliable future applications to surface chemistry on insulators., Comment: 7 pages, 4 figures

The experimental observation of quantum phase transitions predicted by the quantum Rabi model in quantum critical systems is usually challenging due to the lack of signature experimental observables associated with them. Here, we describe a method to identify the dynamical critical phenomenon in the quantum Rabi model consisting of a three-level atom and a cavity at the quantum phase transition. Such a critical phenomenon manifests itself as a sudden change of steady-state output photons in the system driven by two classical fields, when both the atom and the cavity are initially unexcited. The process occurs as the high-frequency pump field is converted into the low-frequency Stokes field and multiple cavity photons in the normal phase, while this conversion cannot occur in the superradiant phase. The sudden change of steady-state output photons is an experimentally accessible measure to probe quantum phase transitions, as it does not require preparing the equilibrium state., Comment: has been published in Communcations Physics as a regular article

Superradiant phase transitions (SPTs) are important for understanding light-matter interactions at the quantum level, and play a central role in criticality-enhanced quantum sensing. So far, SPTs have been observed in driven-dissipative systems, but the emergent light fields did not show any nonclassical characteristic due to the presence of strong dissipation. Here we report an experimental demonstration of the SPT featuring the emergence of a highly nonclassical photonic field, realized with a resonator coupled to a superconducting qubit, implementing the quantum Rabi model. We fully characterize the light-matter state by Wigner matrix tomography. The measured matrix elements exhibit quantum interference intrinsic of a photonic mesoscopic superposition, and reveal light-matter entanglement, Comment: 20 pages, 19 figures, 2 tables

We present an algorithm and implementation of integral-direct, density-fitted Hartree-Fock (HF) and second-order M{\o}ller-Plesset perturbation theory (MP2) for periodic systems. The new code eliminates the formerly prohibitive storage requirements and allows us to study systems one order of magnitude larger than before at the periodic MP2 level. We demonstrate the significance of the development by studying the benzene crystal in both the thermodynamic limit and the complete basis set limit, for which we predict an MP2 cohesive energy of $-72.8$ kJ/mol, which is about $10$--$15$ kJ/mol larger in magnitude than all previously reported MP2 calculations. Compared to the best theoretical estimate from literature, several modified MP2 models approach chemical accuracy in the predicted cohesive energy of the benzene crystal and hence may be promising cost-effective choices for future applications on molecular crystals., Comment: 5 pages (w/o refs or SI), 3 figures, 1 table

Metallic solids are a challenging target for wavefunction-based electronic structure theories and have not been studied in great detail by such methods. Here, we use coupled-cluster theory with single and double excitations (CCSD) to study the structure of solid lithium and aluminum using optimized Gaussian basis sets. We calculate the equilibrium lattice constant, bulk modulus, and cohesive energy and compare them to experimental values, finding accuracy comparable to common density functionals. Because the quantum chemical "gold standard" CCSD(T) (CCSD with perturbative triple excitations) is inapplicable to metals in the thermodynamic limit, we test two approximate improvements to CCSD, which are found to improve the predicted cohesive energies.