Seunghoon Lee

Due to intense interest in the potential applications of quantum computing, it is critical to understand the basis for potential exponential quantum advantage in quantum chemistry. Here we gather the evidence for this case in the most common task in quantum chemistry, namely, ground-state energy estimation, for generic chemical problems where heuristic quantum state preparation might be assumed to be efficient. The availability of exponential quantum advantage then centers on whether features of

The use of the mixed reference (MR) reduced density matrix, which combines reduced density matrices of the <i>M</i>_<i>S</i> = +1 and -1 triplet-ground states, is proposed in the context of the collinear spin-flip-time-dependent density functional theory (SF-TDDFT) methodology. The time-dependent Kohn-Sham equation with the mixed state is solved by the use of spinor-like open-shell orbitals within the linear response formalism, which enables to generate additional configurations in the

Analytic energy gradients of individual singlet and triplet states with respect to nuclear coordinates are derived and implemented for the collinear mixed-reference spin-flip time-dependent density functional theory (MRSF-TDDFT), which eliminates the problematic spin-contamination of SF-TDDFT. Dimensional-transformation matrices for the singlet and triplet response spaces are introduced, simplifying the subsequent derivations. These matrices enable the general forms of MRSF-TDDFT equations to be

The mixed-reference spin-flip time-dependent density functional theory (MRSF-TD-DFT) method eliminates the erroneous spin contamination of the SF-TD-DFT methodology, while retaining the conceptual and practical simplicity of the latter. The availability of the analytic gradient of the energy of the MRSF-TD-DFT response states enables automatic geometry optimization of the targeted states. Here, we apply the new method to optimize the geometry of several S₁/S₀ conical inters

The density functional theory (DFT) and linear response (LR) time-dependent (TD)-DFT are of the utmost importance for routine computations. However, the single reference formulation of DFT suffers in the description of open-shell singlet systems such as diradicals and bond-breaking. LR-TDDFT, on the other hand, finds difficulties in the modeling of conical intersections, doubly excited states, and core-level excitations. In this Perspective, we demonstrate that many of these limitations can be o

Fast overlap integral algorithms for the spin-flip time-dependent density functional theory (SF-TDDFT) and the linear response (LR)-TDDFT were proposed on the basis of determinant factorization (DF) and the truncated Leibnitz formula (TLF). These in turn allow efficient computation of nonadiabatic coupling terms (NACTs) in nonadiabatic molecular dynamics simulations. The TLF(0), TLF(1), and TLF(2) were proposed according to the truncation order. The DF and TLF(1) or TLF(2) provide a four order c

We present a fast and accurate numerical algorithm for computing the first-order nonadiabatic coupling matrix element (NACME). The algorithm employs the truncated Leibniz formula (TLF) approximation within the finite-difference method, which makes it easily applicable in connection with any wave function-based methodology. In this work, we used the algorithm in connection with the recently developed mixed-reference spin-flip time-dependent density functional theory (MRSF-TDDFT, MRSF for brevity)

Abstract The formulations and performances of spin ‐ restricted ensemble ‐ referenced KS and mixed‐reference spin‐flip time‐dependent density functional theory incorporating strong correlations into density functional theories are documented. As a result of balanced dynamic and nondynamic correlation, they are capable of describing strongly correlated challenging systems including diradicals, bond dissociation, conical intersections, doubly excited states, and so on, overcoming the limitations o

Analog beamforming technology is being used to overcome various technical drawbacks of mm-wave wireless communications systems. However, the errors caused by circuit implementations, quantized control, and imperfect isolation between antenna elements result in radiation pattern (RP) distortion and performance deterioration. In particular, the quantization error and mutual coupling cause the active reflection coefficient (ARC) of each antenna element to vary with respect to the main beam directio

ConspectusWhile traditional quantum chemical theories have long been central to research, they encounter limitations when applied to complex situations. Two of the most widely used quantum chemical approaches, Density Functional Theory (DFT) and Time-Dependent Density Functional Theory (TDDFT), perform well in cases with relatively weak electron correlation, such as the ground-state minima of closed-shell systems (Franck-Condon region). However, their applicability diminishes in more demanding s

Relativistic mixed-reference spin-flip (MRSF)-TDDFT is developed considering the spin-orbit coupling (SOC) within the mean-field approximation. The resulting SOC-MRSF faithfully reproduces the experiments with very high accuracy, which is also consistent with the values by four-component (4c) relativistic CASSCF and 4c-CASPT2 in the spin-orbit-energy splitting calculations of the C, Si, and Ge atoms. Even for the fifth-row element Sn, the SOC-MRSF yielded accurate splittings (∼ 3 % error). In th

It is demonstrated that significant accuracy improvements in MRSF-TDDFT can be achieved by introducing two different exchange-correlation (XC) functionals for the reference Kohn-Sham DFT and the response part of the calculations, respectively. Accordingly, two new XC functionals of doubly tuned Coulomb attenuated method-vertical excitation energy (DTCAM-VEE) and DTCAM-AEE were developed on the basis of the "adaptive exact exchange (AEE)" concept in the framework of the Coulomb-attenuating XC fun

As machine learning (ML) has been proven effective in solving various problems, researchers in the real-time systems (RT) community have recently paid increasing attention to ML. While most of them focused on timing issues for ML applications (i.e., RT for ML), only a little has been done on the use of ML for solving fundamental RT problems. In this paper, we aim at utilizing ML to solve a fundamental RT problem of priority assignment for global fixed-priority preemptive (gFP) scheduling on a mu

We describe an ab initio approach to simulate L-edge X-ray absorption (XAS) and 2p3d resonant inelastic X-ray scattering (RIXS) spectroscopies. We model the strongly correlated electronic structure within a restricted active space and employ a correction vector formulation instead of sum-over-state expressions for the spectra, thus eliminating the need to calculate a large number of intermediate and final electronic states. We present benchmark simulations of the XAS and RIXS spectra of the iron

A new current reused quadrature voltage controlled oscillator (QVCO) is proposed and implemented using UMC 0.18 μm CMOS 1P6M process. The proposed circuit topology is made up two low voltage LC-tank VCOs, where the QVCO is obtained using the transformer coupling and current reuse technique. At 1.8 V supply voltage, the phase noise of the VCO is -117.13 dBc/Hz at 1 MHz offset frequency from the carrier frequency of 2.18GHz, the core power consumption is 4.14mW, the total power consumption is 6.48