Bulletin of the American Physical Society
APS March Meeting 2023
Volume 68, Number 3
Las Vegas, Nevada (March 510)
Virtual (March 2022); Time Zone: Pacific Time
Session K17: Density Functional Theory in Chemical Physics IVFocus

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Sponsoring Units: DCP Chair: Adam Wasserman, Purdue University Room: Room 209 
Tuesday, March 7, 2023 3:00PM  3:36PM 
K17.00001: Realtime TDDFT for complex systems and dynamics Invited Speaker: Yosuke Kanai Realtime propagation approach to timedependent density functional theory (RTTDDFT) is a powerful firstprinciples method for simulating nonequilibrium electron dynamics. I will start by discussing our method development effort, particularly how massivelyparallel computers are used to investigate electron dynamics in large complex systems like DNA solvated in water under ion irradiation. I will then discuss the need for advanced hybrid exchangecorrelation approximations in the context of RTTDDFT and how the unitary transformation of timedependent orbitals is used to mitigate their prohibitively large cost for condensed matter systems. I will finish the talk by discussing our new effort on using nuclearelectronic orbital (NEO) paradigm for expanding the realm of RTTDDFT by treating protons quantummechanically in heterogeneous systems. Competing kinetics between electronic excitation dynamics and quantummechanical proton transfer is discussed as an example of how such new multicomponent DFT formulation can expand the application of RTTDDFT. 
Tuesday, March 7, 2023 3:36PM  3:48PM 
K17.00002: Exchangecorrelation functionals for noncollinear spin density functional theory Nicolas TancogneDejean, Carsten A Ullrich We present new semilocal exchange and correlation energy functionals for spin density functional theory (SDFT). These exchange and correlation functionals are directly derived for noncollinear magnetism, in order to preserve gauge invariance, and give rise to nonvanishing exchange correlation torques. We further propose generalization of selfinteraction corrections to the noncollinear case, which also give rise to nonvanishing exchangecorrelation torques. These functionals are tested for frustrated antiferromagnetic clusters and are shown to perform favorably compared to the far more expensive optimized effective potential for exact exchange. This provides a path forward for functional development in noncollinear SDFT and the ab initio study of magnetic materials in and out of equilibrium. 
Tuesday, March 7, 2023 3:48PM  4:00PM 
K17.00003: Approximate exchangecorrelation energy from model Green's functions Steven Crisostomo, Kieron Burke Density functional theory (DFT) and Green’s function (GF) methods are frequently used together to 
Tuesday, March 7, 2023 4:00PM  4:12PM 
K17.00004: A DFT analysis of a covalent organic donoracceptorradical molecule used for quantum teleportation Pedro U Medina Gonzalez, Rajendra R Zope, Mark R Pederson, Tunna Baruah Radical ion pairs (RIPs) have been used to demonstrate quantum teleportation in molecular systems for applications in quantum information science. Covalent organic donoracceptor (DA) molecules can produce RIPs through photoinduced charge transfer and an additional radical (R) molecule makes quantum teleportation possible. We present the electronic structure and analyze charge transfer excited states of a recently studied[1] DAR molecular system using density functional theory. The distances between donoracceptor and donorradical are about 12.9 Å and 21.9 Å, respectively. The excitation energies are calculated using the perturbative deltaSCF method and agree with other conventional excitedstate methods and experimental reference values. Charge transfer energies change with solvent polarity, but we find that due to the ionic nature of triad, even low polarity solvents make a significant change in energies. We discuss the spin ordering energies and the Heisenberg exchange coupling parameters for this DAR system. 
Tuesday, March 7, 2023 4:12PM  4:24PM 
K17.00005: TDDFTas(p): a series of high accuracy semiempirical TDDFT model using minimal auxiliary basis. ZEHAO ZHOU, Shane M Parker, Fabio D Sala We report a general strategy to efficiently approximate TimeDependent Density Functional Theory (TDDFT) calculations of molecular response properties such as UV absorption spectra. This strategy leads to a series of highly accurate semiempirical TDDFT models: TDDFTas(p). In our benchmarking on 39 small to medium sized molecules, TDDFTas has an energy error of 0.06 eV, 25% of currently best method sTDDFT with an energy error of 0.24 eV. The advantage of our approach is that we can improve the TDDFTas model by adding one more p function per atom, which makes the TDDFTasp model with an energy error of 0.04 eV. Moreover, TDDFTas(p) needs a nearly trivial implementation and is naturally ready for existing quantum chemistry softwares such as Turbomole. 
Tuesday, March 7, 2023 4:24PM  4:36PM 
K17.00006: Hubbard clusters as testing grounds for noncollinear spins in (TD)DFT Daniel M Hill, Carsten A Ullrich, Justin Shotton Commonly used DFT approximations for noncollinear magnetism, most notably the LSDA, are based on reference systems with collinear spins; this neglects exchangecorrelation (xc) torque effects. In order to test when these xc torques are important it is helpful to have a fully solvable model to compare to DFT approximations. Finite sized Hubbard models are an ideal testing ground for DFT, but the most common systems in use, the dimer and trimer, are too small to model extended Hubbard interactions, which are necessary for nontrivial exchange torques to arise. We advocate for the use of a halffilled 5site Hubbard cluster in DFT testing of orbitaldependent xc functionals, including spinorbit coupling induced geometric frustrations. We find that xc torques make a significant contribution to the noncollinear spin dynamics, especially in the vicinity of boundaries between different phases of frustration. 
Tuesday, March 7, 2023 4:36PM  5:12PM 
K17.00007: Description of the interaction of light and matter using the timedependent density functional theory Invited Speaker: Kalman Varga In this talk, I present our recent work on the interaction of light and 
Tuesday, March 7, 2023 5:12PM  5:24PM 
K17.00008: Modern exact twocomponent Hamiltonians for relativistic quantum chemistry and physics: Twoelectron picturechange corrections made simple Michal Repisky, Stefan Knecht, Hans Jørgen Aagaard Jensen, Trond Saue, Lukas Konecny Based on atomic meanfield (amf) SCF quantities, we present two simple, yet computationally efficient and numerically accurate matrix approaches to correct scalarrelativistic and spinorbit twoelectron picturechange corrections (PCs) arising within an exact twocomponent (X2C) Hamiltonian framework.[1] Both approaches, dubbed amfX2C and eamfX2C, allow us to uniquely tailor PCs to meanfield models, viz. Hartree–Fock or Kohn–Sham DFT, in the latter case also avoiding the need of a pointwise calculation of exchange–correlation PCs. We assess the numerical performance of these Hamiltonians on spinor energies of closedshell and openshell molecules, achieving a consistent 10^{5} Hartree accuracy compared to reference fourcomponent (4c) data. Excellent agreements with reference data are also observed for molecular properties sensitive to relativistic effects such as EPR or Xray absorption energies.[2] We believe that our (e)amfX2C Hamiltonians constitute a fundamental milestone towards a universal and reliable relativistic 2c approach for quantum chemistry and physics, maintaining the accuracy of the parent 4c one at a fraction of its computational cost. 
Tuesday, March 7, 2023 5:24PM  5:36PM 
K17.00009: Quantum Model of Propagating Plexcitons in TwoDimensional Semiconducting Materials Martin A Mosquera, Juan M MarmolejoTejada, Nicholas Borys Hybrid quantum states emerge upon the strong interaction of surface plasmon waves and excitonic species in 2D semiconducting materials. This gives rise to the socalled "plexcitons", which are a special class of polaritonic states that can attain quantum properties that are not possible in either of the decoupled states. In this work, we present a quantum model of the coupling between 2D mobile excitons and mobile surface plasmon polaritons, where both physical states are treated quantum mechanically. Our model shows the emergence of the propagating plexciton states, reflecting a strong coupling between the individual species. The application to a hypothetical device (composed of a gold surface, a spacer, the 2D material, and a capping dielectric) we propose also shows scenarios in which the lower polariton (plexciton) quasiparticle dominates the dynamics of the system upon the injection of surface plasmons to the system. We then discuss opportunities for future work, from both theoretical and experimental perspectives. 
Tuesday, March 7, 2023 5:36PM  5:48PM 
K17.00010: Plasmons and excitons in Pddoped Ag nanoparticles from an ab initio GWBSE approach Emma Simmerman, Aaron R Altman, Supavit Pokawanvit, Felipe H da Jornada Combining transitionmetal catalyst materials with plasmonic metals can enhance photocatalytic reaction rates, selectivity, and open nonequilibrium reaction paths. These effects are initiated by surface plasmon resonances (SPRs) in the plasmonic metal, and direct electronhole (eh) interactions can also significantly alter the landscape of excited states and affect SPR evolution. However, ab initio calculations in realistic metallic nanoparticle systems have mostly either neglected eh interactions or been limited to very small (<25 atom) clusters that display zerodimensionallike excitation spectrum due to strong confinement effects. Here, we study Pddoped Ag nanoparticles of up to 147 atoms with varying dopant levels, including eh interactions, through the firstprinciples GW plus BetheSalpeter equation (BSE) approach. Applying new lowrank approximations and spectral folding techniques to accelerate these calculations, we can directly obtain excited states of nanoparticles capturing both plasmonic and excitonic effects. For small systems, we observe strong eh interactions that redshift the spectrum by up to ~2 eV, demonstrating the importance of excitonic effects for spatially confined metallic systems. We also analyze the excitonic and plasmonic character of the excitations as a function of size and doping, and the impact of manybody interactions for reactions involving excitedstate potentialenergy surfaces. 
Tuesday, March 7, 2023 5:48PM  6:00PM 
K17.00011: Modeling ultrafast photoinduced dynamics of adsorbates on metals with machine learning potentials Ivor Loncaric I will present theoretical approaches for modeling the dynamics of molecules on metal surfaces induced by short laser pulses. 
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