We introduce a multireference version of the driven similarity renormalization group (DSRG) approach [Evangelista, F. A. J. Chem. Phys. 2014, 141, 054109] based on generalized reference wave function and operator normal ordering [Kutzelnigg, W.; Mukherjee, D. 1997, 107, 432]. perform perturbative analysis corresponding equations at second order derive novel perturbation theory, termed DSRG-MRPT2. The DSRG-MRPT2 energy equation can be written in simple compact form solved via noniterative...

Supramolecular coordination is an efficient strategy to construct supramolecular frameworks with predesigned structures, assembled shapes, and specific function. In this work, we report the synthesis, structural characterization, photophysical property of two tetraphenylethene-based 1a 1b formed from 1,1,2,2-tetrakis(4-(pyridin-4-yl)phenyl)ethene (2a) or 1,1,2,2-tetrakis(4-((E)-2-(pyridin-4-yl)vinyl)phenyl)ethene (2b) a linear difunctional platinum(II) ligand (3a) via coordination-driven...

Abstract Planar-chiral cyclophanes have gained considerable concerns for drug discovery due to their unique conformational strain and 3D structure. However, the enantioselective synthesis of planar-chiral is a long-standing challenge synthetic community. We herein describe an N-heterocyclic carbene (NHC)-catalyzed asymmetric construction cyclophanes. This transformation occurs through dynamic kinetic resolution (DKR) process convert racemic substrates into macrocycle scaffolds in good high...

An N-heterocyclic carbene (NHC)-catalyzed atroposelective macrolactonization has been disclosed. This approach affords planar-chiral macrocycles in high yields with excellent enantioselectivities over a broad substrate scope. Controlled experiments suggest that the enantioselectivity might arise from cation–n interaction between acyl azolium and electron-rich moiety substrate. mechanism is supported by density functional theory calculations, which also an important π–π stabilizing transition state.

We have combined our adaptive configuration interaction (ACI) [J. B. Schriber and F. A. Evangelista, J. Chem. Phys. 2016, 144, 161106] with a density-fitted implementation of the second-order perturbative multireference-driven similarity renormalization group (DSRG-MRPT2) [K. P. Hannon, C. Li, 204111]. use ACI reference wave functions to recover static correlation for active spaces larger than conventional limit 18 orbitals. The dynamical is computed using DSRG-MRPT2 method yield complete...

A quantum unitary downfolding formalism that works on noisy and fault-tolerant hardware is proposed tested several challenging chemical problems, offering a viable approach for estimating molecular properties with accuracy.

A third-order multireference perturbation theory based on the driven similarity renormalization group approach (DSRG-MRPT3) is presented. The DSRG-MRPT3 method has several appealing features: a) it intruder free, b) size consistent, c) leads to a non-iterative algorithm with ${\cal O}(N^6)$ scaling, and d) includes reference relaxation effects. scheme benchmarked potential energy curves of F$_2$, H$_2$O$_2$, C$_2$H$_6$, N$_2$ along F-F, O-O, C-C, N-N bond dissociation coordinates,...

We report an efficient implementation of a second-order multireference perturbation theory based on the driven similarity renormalization group (DSRG-MRPT2) [C. Li and F. A. Evangelista, J. Chem. Theory Comput. 11, 2097 (2015)]. Our employs factorized two-electron integrals to avoid storage large four-index intermediates. It also exploits block structure reference density matrices reduce computational cost that Møller-Plesset theory. new DSRG-MRPT2 is benchmarked ten naphthyne isomers using...

Abstract Developing efficient cyan‐green phosphors and ultrathin phosphor‐glass composites (PGCs) with remarkable chemical thermal stability is important for fabricating full‐visible‐spectrum white light‐emitting diodes (LEDs). In this study, a garnet‐structured phosphor, known as Y 3 Sc 2 Ga O 12 :Ce (YSGG:Ce), synthesized, exhibiting an intense excitation peak at 420 nm broad‐emission band centered 507 nm. Theoretical analysis indicates that phonon characteristic energy of 90 meV...

This publisher's note contains a correction to Opt. Lett.49, 6928 (2024)10.1364/OL.544994.

An unprecedented catalytic kinetic resolution of 2-substituted 3-nitro-2H-chromenes via Rh-catalyzed asymmetric hydrogenation has been developed to simultaneously produce a variety syn-chiral 3-nitro-2H-chromanes containing vicinal stereogenic centers with excellent diastero- and enantioselectivities [diastereomeric ratio (dr) >99:1 up 99.9% enantiomeric excess (ee)] recovered chiral 90–99.9% ee in high yields, respectively, achieving selectivity factors 1057. Moreover, addition...

A novel two-photon upconversion luminescence process was reported in Yb³⁺/Tm³⁺ co-doped LuAG transparent ceramics. Systematic photoluminescence measurements as a function of Tm³⁺ concentration reveal that an optimal doping level of...

The multireference driven similarity renormalization group (MRDSRG) approach [C. Li and F. A. Evangelista, J. Chem. Theory Comput. 11, 2097 (2015)] is generalized to treat quasi-degenerate electronic excited states. new scheme, termed state-averaged (SA) MRDSRG, a state-universal that considers an ensemble of states on equal footing. Using the SA-MRDSRG framework, we implement second- (SA-DSRG-PT2) third-order (SA-DSRG-PT3) perturbation theories. These theories can manifold near-degenerate...

The first nonperturbative version of the multireference driven similarity renormalization group (MR-DSRG) theory [C. Li and F. A. Evangelista, J. Chem. Theory Comput. 11, 2097 (2015)] is introduced. structure MR-DSRG equations ensures numerical robustness avoidance intruder-state problem, while connected nature amplitude energy guarantees size consistency extensivity. We approximate by keeping only one- two-body operators using a linearized recursive commutator approximation...

The driven similarity renormalization group (DSRG) provides an alternative way to address the intruder state problem in quantum chemistry. In this review, we discuss recent developments of multireference methods based on DSRG. We provide a pedagogical introduction DSRG and its various extensions formal properties great detail. addition, report several illustrative applications molecular systems.

Lead sulfide (PbS) quantum dots (QDs) have shown promising performance as a sensitizer in infrared-to-visible photon upconversion systems. To investigate the key design rules, we compare three PbS-sensitized systems using mediator molecules with same tetracene triplet acceptor at different distances from QD. Using transient absorption spectroscopy, directly measure energy-transfer rates and efficiencies QD to emitter. With increasing distance between PbS QD, efficiency of first energy...

Abstract This study presents photonic vertical cavities consisting of nonlinear materials embedded in crystals (PhCs) for resonantly enhancing second harmonic generation (SHG). Previous attempts at SHG such structures have been limited to efficiencies 10 −7 −5 , but a high efficiency 0.28% by constructing cavity with lithium niobate membrane placed between two PhCs is demonstrated, which exhibits high‐quality resonances. The results open up new possibilities compact laser frequency...

We report a spin-free formulation of the multireference (MR) driven similarity renormalization group (DSRG) based on ensemble normal ordering Mukherjee and Kutzelnigg [J. Chem. Phys. 107, 432 (1997)]. This averages over all microstates given total spin quantum number, therefore, it is invariant with respect to SU(2) transformations. As such, equations may be reformulated in terms quantities they closely resemble those spin-adapted closed-shell coupled cluster (CC) theory. The current...

We introduce two new approaches to compute near-degenerate electronic states based on the driven similarity renormalization group (DSRG) framework. The first approach is a unitary multi-state formalism DSRG (MS-DSRG), whereby an effective Hamiltonian built from set of state-specific solutions. second employs dynamic weighting parameter smoothly interpolate between and state-averaged schemes. resulting dynamically weighted (DW-DSRG) theory incorporates most desirable features both (ability...

This study examines several techniques to improve the efficiency of linearized multireference driven similarity renormalization group truncated one- and two-body operators [MR-LDSRG(2)]. We propose a sequential MR-LDSRG(2) [sq-MR-LDSRG(2)] scheme, in which one-body substitutions are folded exactly into Hamiltonian. new approach is combined with density fitting (DF) reduce storage cost two-electron integrals. To further avoid large four-index intermediates, we noninteracting virtual orbital...

Quantum embedding schemes are a promising way to extend multireference computations large molecules with strong correlation effects localized on small number of atoms. This work introduces second-order active-space theory [ASET(2)] which improves upon mean-field frozen by treating fragment-environment interactions via an approximate canonical transformation. The transformation employed in ASET(2) is formulated using the driven similarity renormalization group. scheme benchmarked N═N bond...

Left figure shows PL spectra of phosphors with and without Ca 2+ ion. The central images present the photos PiG under illumination sunlight UV light. Right figures give EL LED encapsulated different phosphors.