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At least 253 records · Page 14

Spectrum of end of the world branes in holographic BCFTs

We study overlaps between two regularized boundary states in conformal field theories. Regularized boundary states are dual to end of the world branes in an AdS black hole via the AdS/BCFT. Thus they can be regarded as microstates of a single sided black hole. Owing to the open-closed duality, such an overlap between two different regularized boundary states is exponentially suppressed as $\langle$ψ a |ψ b $\rangle$~e -O (h$^{(min)}_{ab}$) , where h$^{(min)}_{ab}$ is the lowest energy of open strings which connect two different boundaries a and b. Our gravity dual analysis leads to h$^{(min)}_{ab}$ = c/24 for a pure AdS 3 gravity. This shows that a holographic boundary state is a random vector among all left-right symmetric states, whose number is given by a square root of the number of all black hole microstates. We also perform a similar computation in higher dimensions, and find that h$^{(min)}_{ab}$ depends on the tensions of the branes. In our analysis of holographic boundary states, the off diagonal elements of the inner products can be computed directly from on-shell gravity actions, as opposed to earlier calculations of inner products of microstates in two dimensional gravity.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

A tale of two saddles

We find a new on-shell replica wormhole in a computation of the generating functional of JT gravity coupled to matter. We show that this saddle has lower action than the disconnected one, and that it is stable under restriction to real Lorentzian sections, but can be unstable otherwise. The behavior of the classical generating functional thus may be strongly dependent on the signature of allowed perturbations. As part of our analysis, we give an LM-style construction for computing the on-shell action of replicated manifolds even as the number of boundaries approaches zero, including a type of one-step replica symmetry breaking that is necessary to capture the contribution of the new saddle. Our results are robust against quantum corrections; in fact, we find evidence that such corrections may sometimes stabilize this new saddle.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Excited State Orbital Optimization via Minimizing the Square of the Gradient: General Approach and Application to Singly and Doubly Excited States via Density Functional Theory

We present a general approach to converge excited state solutions to any quantum chemistry orbital optimization process, without the risk of variational collapse. The resulting square gradient minimization (SGM) approach only requires analytic energy/Lagrangian orbital gradients and merely costs 3 times as much as ground state orbital optimization (per iteration), when implemented via a finite difference approach. SGM is applied to both single determinant ΔSCF and spin-purified restricted open-shell Kohn-Sham (ROKS) approaches to study the accuracy of orbital optimized DFT excited states. It is found that SGM can converge challenging states where the maximum overlap method (MOM) or analogues either collapse to the ground state or fail to converge. We also report that ΔSCF/ROKS predict highly accurate excitation energies for doubly excited states (which are inaccessible via TDDFT). Singly excited states obtained via ROKS are also found to be quite accurate, especially for Rydberg states that frustrate (semi)local TDDFT. Our results suggest that orbital optimized excited state DFT methods can be used to push past the limitations of TDDFT to doubly excited, charge-transfer, or Rydberg states, making them a useful tool for the practical quantum chemist's toolbox for studying excited states in large systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Condensed Phase Water Molecular Multipole Moments from Deep Neural Network Models Trained on Ab Initio Simulation Data

Ionic solvation phenomena in liquids involve intense interactions in the inner solvation shell. For interactions beyond the first shell, the ion–solvent interaction energies result from the sum of many smaller-magnitude contributions that can still include polarization effects. Deep neural network (DNN) methods have recently found wide application in developing efficient molecular models that maintain near-quantum accuracy. In this work, we extend the DeePMD-kit code to produce accurate molecular multipole moments in the bulk and near interfaces. The new method is validated by comparing the DNN moments with those generated by ab initio simulations. The moments are used to compute the electrostatic potential at the center of a molecular-sized hydrophobic cavity in water. The results show that the fields produced by the DNN models are in quantitative agreement with the AIMD-derived values. These efficient methods will open the door to more accurate solvation models for large solutes such as proteins.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Compositionally Tuning Electron Transfer from Photoexcited Core/Shell Quantum Dots via Cation Exchange

It is critical to find methods to control the thermodynamic driving force for photoexcited charge transfer from quantum dots (QDs) and explore how this affects charge transfer rates, since the efficiency of QD-based photovoltaic and photocatalysis technologies depends on both this rate and the associated energetic losses. In this work, we introduce a single-pot shell growth and Cu-catalyzed cation exchange method to synthesize Cd x Zn 1-x Se/Cd y Zn 1-y S QDs with tunable driving forces for electron transfer. Functionalizing them with two molecular electron acceptors—naphthalenediimide (NDI) and anthraquinone (AQ)—allowed us to probe nearly 1 eV of driving forces. For AQ, at lower driving forces, we find that higher Zn content results in a 130-fold increase of electron transfer rate constants. However, at higher driving forces electron transfer dynamics are unaltered. Here, the data are understood using an Auger-assisted electron transfer model and analyzed with computational work to determine approximate binding geometries of these electron acceptors. Our work provides a method to tune QD reducing power and produces useful metrics for optimizing QD charge transfer systems that maximize rates of electron transfer while minimizing energetic losses.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

$T\overline{T}$ deformations of supersymmetric quantum mechanics

We define a manifestly supersymmetric version of the $T\overline{T}$ deformation appropriate for a class of (0 + 1)-dimensional theories with $\mathcal{N}$ = 1 or $\mathcal{N}$ = 2 supersymmetry, including one presentation of the super-Schwarzian theory which is dual to JT supergravity. These deformations are written in terms of Noether currents associated with translations in superspace, so we refer to them collectively as f($\mathcal{Q}$) deformations. We provide evidence that the f($\mathcal{Q}$) deformations of $\mathcal{N}$ = 1 and $\mathcal{N}$ = 2 theories are on-shell equivalent to the dimensionally reduced supercurrent-squared deformations of 2d theories with $\mathcal{N}$ = (0, 1) and $\mathcal{N}$ = (1, 1)supersymmetry, respectively. In the $\mathcal{N}$ = 1 case, we present two forms of the f($\mathcal{Q}$) deformation which drive the same flow, and clarify their equivalence by studying the analogous equivalent deformations in the non-supersymmetric setting.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Hetero-site Double Core Ionization Energies with Sub-electronvolt Accuracy from Delta-Coupled-Cluster Calculations

Benchmark scalar-relativistic delta-coupled-cluster calculations of hetero-site double core ionization energies of small molecules containing second-row elements are reported. The present study has focused on the high-spin triplet components of two-site double core-ionized states, which are single reference in character and consistent with the use of standard coupledcluster methods. Contributions to computed double core ionization energies from electron-correlation and basis-set effects as well as corrections to the core-valence separation approximation have been analyzed. Furthermore, on the basis of systematic convergence of computational results with respect to these effects, delta-coupled-cluster calculations have been shown to be capable of providing accurate double core ionization energies with remaining errors estimated to be below 0.3 eV, and thus they are recommended for use to facilitate experimental studies of two-site double core-ionized states that are involved in X-ray pump/X-ray probe studies of electronic and molecular dynamics following inner shell ionization or excitation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Low-threshold laser medium utilizing semiconductor nanoshell quantum dots

Colloidal semiconductor nanocrystals (NCs) represent a promising class of nanomaterials for lasing applications. Currently, one of the key challenges facing the development of high-performance NC optical gain media lies in enhancing the lifetime of biexciton populations. This usually requires the employment of charge-delocalizing particle architectures, such as core/shell NCs, nanorods, and nanoplatelets. Here, we report on a two-dimensional nanoshell quantum dot (QD) morphology that enables a strong delocalization of photoinduced charges, leading to enhanced biexciton lifetimes and low lasing thresholds. A unique combination of a large exciton volume and a smoothed potential gradient across interfaces of the reported CdS bulk /CdSe/CdS shell (core/shell/shell) nanoshell QDs results in strong suppression of Auger processes, which was manifested in this work though the observation of stable amplified stimulated emission (ASE) at low pump fluences. An extensive charge delocalization in nanoshell QDs was confirmed by transient absorption measurements, showing that the presence of a bulk-size core in CdS bulk /CdSe/CdS shell QDs reduces exciton–exciton interactions. Altogether, present findings demonstrate unique advantages of the nanoshell QD architecture as a promising optical gain medium in solid-state lighting and lasing applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Evaluation of two-particle properties within finite-temperature self-consistent one-particle Green’s function methods: Theory and application to GW and GF2

One-particle Green’s function methods can model molecular and solid spectra at zero or non-zero temperatures. One-particle Green’s functions directly provide electronic energies and one-particle properties, such as dipole moment. However, the evaluation of two-particle properties, such as $\langle$S 2 $\rangle$ and $\langle$N 2 $\rangle$, can be challenging because they require a solution of the computationally expensive Bethe–Salpeter equation to find two-particle Green’s functions. We demonstrate that the solution of the Bethe–Salpeter equation can be completely avoided. Applying the thermodynamic Hellmann–Feynman theorem to self-consistent one-particle Green’s function methods, we derive expressions for two-particle density matrices in a general case and provide explicit expressions for GF2 and GW methods. Such density matrices can be decomposed into an antisymmetrized product of correlated one-electron density matrices and the two-particle electronic cumulant of the density matrix. Cumulant expressions reveal a deviation from ensemble representability for GW, explaining its known deficiencies. We analyze the temperature dependence of $\langle$S 2 $\rangle$ and $\langle$N 2 $\rangle$ for a set of small closed-shell systems. Interestingly, both GF2 and GW show a non-zero spin contamination and a non-zero fluctuation of the number of particles for closed-shell systems at the zero-temperature limit.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Search for an s -wave resonance in Li 7 just above the proton-decay threshold

Near-threshold resonances play an important role in nucleosynthesis and applied nuclear science. The study of nuclei removed from stability has greatly extended the list of resonances close to decay thresholds. The no core shell model with continuum (NCSMC) recently predicted an s-wave resonance just above the proton-decay threshold of 7 Li at an excitation energy of 10.2 MeV. This potential case of a near-threshold resonance is dependent on the quantum mechanics of the p + 6 He fragments extended into the continuum. Further, the 6 He(d,n) 7 Li* reaction was employed in an attempt to populate this resonance and search for its proton decay via the invariant-mass method. No evidence of this resonance was found. However, the data collected in this search led to better constraints on the energy and width of the isobaric analog state (IAS) with (J π ,T) = (3/2 - , 3/2) and revealed a new weak resonance just above the IAS in energy, predicted by the NCSMC as a (J π , T ) = (3/2 – , 1/2) state and potentially a part of the antianalog structure.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Bright Infrared‐to‐Ultraviolet/Visible Upconversion in Small Alkaline Earth‐Based Nanoparticles with Biocompatible CaF 2 Shells

Abstract Upconverting nanoparticles (UCNPs) are promising candidates for photon‐driven reactions, including light‐triggered drug delivery, photodynamic therapy, and photocatalysis. Herein, we investigate the NIR‐to‐UV/visible emission of sub‐15 nm alkaline‐earth rare‐earth fluoride UCNPs (M 1− x Ln x F 2+ x , MLnF) with a CaF 2 shell. We synthesize 8 alkaline‐earth host materials doped with Yb 3+ and Tm 3+ , with alkaline‐earth (M) spanning Ca, Sr, and Ba, MgSr, CaSr, CaBa, SrBa, and CaSrBa. We explore UCNP composition, size, and lanthanide doping‐dependent emission, focusing on upconversion quantum yield (UCQY) and UV emission. UCQY values of 2.46 % at 250 W cm −2 are achieved with 14.5 nm SrLuF@CaF 2 particles, with 7.3 % of total emission in the UV. In 10.9 nm SrYbF:1 %Tm 3+ @CaF 2 particles, UV emission increased to 9.9 % with UCQY at 1.14 %. We demonstrate dye degradation under NIR illumination using SrYbF:1 %Tm 3+ @CaF 2 , highlighting the efficiency of these UCNPs and their ability to trigger photoprocesses.

Fischer, Stefan↗

Bright Infrared‐to‐Ultraviolet/Visible Upconversion in Small Alkaline Earth‐Based Nanoparticles with Biocompatible CaF 2 Shells

Abstract Upconverting nanoparticles (UCNPs) are promising candidates for photon‐driven reactions, including light‐triggered drug delivery, photodynamic therapy, and photocatalysis. Herein, we investigate the NIR‐to‐UV/visible emission of sub‐15 nm alkaline‐earth rare‐earth fluoride UCNPs (M 1− x Ln x F 2+ x , MLnF) with a CaF 2 shell. We synthesize 8 alkaline‐earth host materials doped with Yb 3+ and Tm 3+ , with alkaline‐earth (M) spanning Ca, Sr, and Ba, MgSr, CaSr, CaBa, SrBa, and CaSrBa. We explore UCNP composition, size, and lanthanide doping‐dependent emission, focusing on upconversion quantum yield (UCQY) and UV emission. UCQY values of 2.46 % at 250 W cm −2 are achieved with 14.5 nm SrLuF@CaF 2 particles, with 7.3 % of total emission in the UV. In 10.9 nm SrYbF:1 %Tm 3+ @CaF 2 particles, UV emission increased to 9.9 % with UCQY at 1.14 %. We demonstrate dye degradation under NIR illumination using SrYbF:1 %Tm 3+ @CaF 2 , highlighting the efficiency of these UCNPs and their ability to trigger photoprocesses.

Fischer, Stefan↗

Controlled Formation of Stacked Si Quantum Dots in Vertical SiGe Nanowires

In this work, we demonstrate the ability to fabricate vertically stacked Si quantum dots (QDs) within SiGe nanowires with QD diameters down to 2 nm. These QDs are formed during high-temperature dry oxidation of Si/SiGe heterostructure pillars, during which Ge diffuses along the pillars’ sidewalls and encapsulates the Si layers. Continued oxidation results in QDs with sizes dependent on oxidation time. The formation of a Ge-rich shell that encapsulates the Si QDs is observed, a configuration which is confirmed to be thermodynamically favorable with molecular dynamics and density functional theory. The type-II band alignment of the Si dot/SiGe pillar suggests that charge trapping on the Si QDs is possible, and electron energy loss spectra show that a conduction band offset of at least 200 meV is maintained for even the smallest Si QDs. Our approach is compatible with current Si-based manufacturing processes, offering a new avenue for realizing Si QD devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Quinonoid versus Aromatic π-Conjugated Oligomers and Polymers and Their Diradical Characters

Quinonoid elements in π-conjugated oligomers and polymers have promising characteristics by providing unique structures and electronic properties, including varying degrees of ground state open shell diradical character and small band gaps. So far, quinonoid ground state polymers were rarely identified, and one of the goals of this work was to expand the portfolio of such systems in which over 17 different repeat units were considered, about half preferred a quinonoid and half preferred aromatic structures plus several with the alternating A-Q composition were also included. The dependency of the diradical character as a function of size and composition opens a rich space to discover trends affecting the aromaticity and diradical character. Herein, we show that the diradical character is a useful parameter to classify a wide variety of polymers based on their ground states in a systematic study of a large number of homo- and heterosystems. Homo-polymers with quinonoid ground states show a high diradical character, while those with the aromatic ground state behave as closed-shell systems with no or a very small diradical character. The diradical character of quinonoid systems depends strongly on the size, which increases with the size of the oligomer. Here, we found a correlation between the diradical character and the interring C–C distance as well as the singlet–triplet energy gaps. In alternating copolymers mixing quinonoid and aromatic subunits, we found open-shell hetero-polymers with moderate to high diradical characters.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Connected three-body terms in single-reference unitary many-body theories: Iterative and perturbative approximations

This work introduces various approaches to include connected three-body terms in unitary many-body theories, focusing on the driven similarity renormalization group (DSRG). Starting from the least approximate method—the linearized DSRG truncated to one-, two-, and three-body operators [LDSRG(3)]—we develop several approximate LDSRG(3) models with reduced computational cost. Through a perturbative analysis, we motivate a family of iterative LDSRG(3)-n and -n' (n = 1, 2, 3, 4) methods that contain a subset of the LDSRG(3) diagrams. Among these variants, the LDSRG(3)-2 scheme has the same computational complexity of coupled cluster theory with singles, doubles, and triples (CCSDT), but it outperforms CCSDT in the accuracy of the predicted correlation energies. We also propose and implement two perturbative triples corrections based on the linearized DSRG truncated to one- and two-body operators augmented with recursive semi-quadratic commutators [qDSRG(2)]. Overall, the resulting qDSRG(2)+(T) approach matches the accuracy of the “gold-standard” coupled cluster theory with singles, doubles, and perturbative triples model on the energetics of twenty-eight closed-shell atoms and small molecules.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Description for N = 126 Isotones 210 Po and 212 Rn with Particle-Hole Excited Nucleon-Pair Approximation and Realistic Effective Interaction

In this paper, we study yrast states of two N=126 isotones 210 Po and 212 Rn using the nucleon-pair approximation with particle–hole excitations and using a low-momentum interaction V low–k renormalized from the free CD-Bonn NN potential. An overall good agreement with experimental level structures, B(E2)s, and B(E3)s, is achieved. We also calculate the probabilities of neutron particle–hole excitations in these yrast states, with a focus on negative-parity states, which reflect the roles played by the neutron negative-parity configurations of one-particle-one-hole excitations across the N=126 shell gap and the negative-parity configurations of valence proton particles involving the 0i 13/2 orbit. The N=126 shell gap is discussed in terms of energies of neutron one-particle-one-hole excitations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Angular distribution of Auger electrons due to 3d-shell ionization of krypton

Cross sections for electron impact ionization of krypton due to ejection of a 3rd shell electron have been calculated using screened hydrogenic and Hartree-Slater wave functions for target atom. While the total ionization cross sections in the two approximations are within 10% of each other, the Auger electron angular distribution, related to cross sections for specific magnetic quantum numbers of the 3rd electrons, is widely different in the two approximations. The angular distribution due to Hartree-Slater approximation is in excellent agreement with measurement. The physical reason for the discrepancies in the two approximations is explained.

Omidvar, K.↗