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NASA NTRS2007

Two-photon or higher-order absorbing optical materials for generation of reactive species

Disclosed are highly efficient multiphoton absorbing compounds and methods of their use. The compounds generally include a bridge of pi-conjugated bonds connecting electron donating groups or electron accepting groups. The bridge may be substituted with a variety of substituents as well. Solubility, lipophilicity, absorption maxima and other characteristics of the compounds may be tailored by changing the electron donating groups or electron accepting groups, the substituents attached to or the length of the pi-conjugated bridge. Numerous photophysical and photochemical methods are enabled by converting these compounds to electronically excited states upon simultaneous absorption of at least two photons of radiation. The compounds have large two-photon or higher-order absorptivities such that upon absorption, one or more Lewis acidic species, Lewis basic species, radical species or ionic species are formed.

Cumpston, Brian↗

NASA NTRS2013

Two-Photon or Higher-Order Absorbing Optical Materials for Generation of Reactive Species

Cumpston, Brian↗

DOE OSTI2022

Fock-Space Schrieffer–Wolff Transformation: Classically-Assisted Rank-Reduced Quantum Phase Estimation Algorithm

We present an extension of many-body downfolding methods to reduce the resources required in the quantum phase estimation (QPE) algorithm. In this paper, we focus on the Schrieffer–Wolff (SW) transformation of the electronic Hamiltonians for molecular systems that provides significant simplifications of quantum circuits for simulations of quantum dynamics. We demonstrate that by employing Fock-space variants of the SW transformation (or rank-reducing similarity transformations (RRST)) one can significantly increase the locality of the qubit-mapped similarity-transformed Hamiltonians. The practical utilization of the SW-RRST formalism is associated with a series of approximations discussed in the manuscript. In particular, amplitudes that define RRST can be evaluated using conventional computers and then encoded on quantum computers. The SW-RRST QPE quantum algorithms can also be viewed as an extension of the standard state-specific coupled-cluster downfolding methods to provide a robust alternative to the traditional QPE algorithms to identify the ground and excited states for systems with various numbers of electrons using the same Fock-space representations of the downfolded Hamiltonian. The RRST formalism serves as a design principle for developing new classes of approximate schemes that reduce the complexity of quantum circuits.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2022

Development of the multi-purpose Cologne Compact Differential Plunger (CoCoDiff) for the measurement of nuclear level lifetimes with the Recoil Distance Doppler-shift method

Here, a new 3-foil plunger device, the Cologne Compact Differential (CoCoDiff) plunger has been built and commissioned. Due to its compact size, it can be used together with many different spectrometers and auxiliary detectors. As a commissioning experiment, level lifetimes of the $2^{+}_{1}$ and the $4^{+}_{1}$ excited states of 50 Cr have been measured, using the Differential Decay Curve method (DDCM). A derivation is given on how this method can be applied to a differential plunger measurement, in order to measure distances for lifetimes from two different regions of sensitivity at the same time. The commissioning experiment took place at the Cologne FN tandem accelerator, using the reaction 24 Mg( 32 S,4p2n) 50 Cr. Lifetimes, deduced from this measurement, agree well with literature values from earlier measurements.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2022

Ultrafast infrared transient absorption spectroscopy of gas-phase Ni(CO) 4 photodissociation at 261 nm

Here, we employ ultrafast mid-infrared transient absorption spectroscopy to probe the rapid loss of carbonyl ligands from gas-phase nickel tetracarbonyl following ultraviolet photoexcitation at 261 nm. Here, nickel tetracarbonyl undergoes prompt dissociation to produce nickel tricarbonyl in a singlet excited state; this electronically excited tricarbonyl loses another CO group over tens of picoseconds. Our results also suggest the presence of a parallel, concerted dissociation mechanism to produce nickel dicarbonyl in a triplet excited state, which likely dissociates to nickel monocarbonyl. Mechanisms for the formation of these photoproducts in multiple electronic excited states are theoretically predicted with one-dimensional cuts through the potential energy surfaces and computation of spin–orbit coupling constants using equation of motion coupled cluster methods (EOM-CC) and coupled cluster theory with single and double excitations (CCSD). Bond dissociation energies are calculated with CCSD, and anharmonic frequencies of ground and excited state species are computed using density functional theory (DFT) and time-dependent density functional theory (TD-DFT).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1993

The quantum dynamics of electronically nonadiabatic chemical reactions

Considerable progress was achieved on the quantum mechanical treatment of electronically nonadiabatic collisions involving energy transfer and chemical reaction in the collision of an electronically excited atom with a molecule. In the first step, a new diabatic representation for the coupled potential energy surfaces was created. A two-state diabatic representation was developed which was designed to realistically reproduce the two lowest adiabatic states of the valence bond model and also to have the following three desirable features: (1) it is more economical to evaluate; (2) it is more portable; and (3) all spline fits are replaced by analytic functions. The new representation consists of a set of two coupled diabatic potential energy surfaces plus a coupling surface. It is suitable for dynamics calculations on both the electronic quenching and reaction processes in collisions of Na(3p2p) with H2. The new two-state representation was obtained by a three-step process from a modified eight-state diatomics-in-molecules (DIM) representation of Blais. The second step required the development of new dynamical methods. A formalism was developed for treating reactions with very general basis functions including electronically excited states. Our formalism is based on the generalized Newton, scattered wave, and outgoing wave variational principles that were used previously for reactive collisions on a single potential energy surface, and it incorporates three new features: (1) the basis functions include electronic degrees of freedom, as required to treat reactions involving electronic excitation and two or more coupled potential energy surfaces; (2) the primitive electronic basis is assumed to be diabatic, and it is not assumed that it diagonalizes the electronic Hamiltonian even asymptotically; and (3) contracted basis functions for vibrational-rotational-orbital degrees of freedom are included in a very general way, similar to previous prescriptions for locally adiabatic functions in various quantum scattering algorithms.

Truhlar, Donald G.↗

DOE OSTI2020

An ab initio exciton model for singlet fission

Here we present an ab initio exciton model that extends the Frenkel exciton model and includes valence, charge-transfer, and multiexcitonic excited states. It serves as a general, parameter-free, yet computationally efficient and scalable approach for simulation of singlet fission processes in multichromophoric systems. A comparison with multiconfigurational methods confirms that our exciton model predicts consistent energies and couplings for the pentacene dimer and captures the correct physics. Calculations of larger pentacene clusters demonstrate the computational scalability of the exciton model and suggest that the mixing between local and charge-transfer excitations narrows the gap between singlet and multiexcitonic states. Local vibrations of pentacene molecules are found to facilitate singlet–multiexcitonic state-crossing and hence are important for understanding singlet fission. The exciton model developed in this work also sets the stage for further implementation of the nuclear gradients and nonadiabatic couplings needed for first principles nonadiabatic quantum molecular dynamics simulations of singlet fission.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1990

Direct simulation Monte Carlo with ionization and radiation

Improvements in the modeling of radiation in low density shock waves with Direct Simulation Monte Carlo (DSMC) are the subject of this study. The physical processes which determine the amount of radiation in a shock wave were investigated and the way in which they were modeled with DSMC was evaluated. Three physical processes were identified for which an improvement in the modeling technique could result in improved radiation predictions. New physical modeling schemes are introduced in this report for the three processes. First a method for determining the electric field and its effect on the flow is introduced. Second, a two step reaction process for electron impact ionization reactions is evaluated. Finally, a new scheme to determine the relaxation collision numbers for excitation of electronic states is proposed. Each new scheme attempts to move the DSMC method toward more accurate physics or more reliance on experimental data. The new schemes are all compared to the current modeling techniques and the differences in the results are evaluated. In all cases the results agree with the available data as well as, or better than the results from earlier schemes.

Carlson, Ann B.↗

DOE OSTI2020

Accurate and efficient description of interacting carriers in quantum nanostructures by selected configuration interaction and perturbation theory

In this paper, we present a method to accurately and efficiently calculate many-body states of interacting carriers in quantum nanostructures based on a combination of iterative selection of configurations and perturbation theory. This method enables investigations of large excitonic complexes and multielectron systems with near full configuration interaction accuracy, even though only a small subspace of the full many-body Hilbert space is sampled, thus saving orders of magnitudes in computational resources. Important advantages of this method are that the convergence is controlled by a single parameter, the threshold, and that ground and excited states can be treated on an equal footing. On the example of InAsP nanowire quantum dots described using a million-atom tight-binding approach, we demonstrate the extreme efficiency of the method by numerical studies of large excitonic complexes filling up to the fourth electronic shell. We find that the method generally converges fast as a function of the threshold, profiting from a significant acceleration due to the perturbative corrections. The role of the choice of single-particle basis states is discussed. It is found that the algorithm converges faster in the Hartree-Fock basis only for highly charged systems, where Coulomb repulsion dominates. Finally, based on the observation that second-order perturbative energy corrections only depend on off-diagonal elements of the many-body Hamiltonian, we present a way to accurately calculate many-body states that requires only a relatively small number of Coulomb matrix elements.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Predicting nucleon-nucleus scattering observables using nuclear structure theory

Developing a predictive capability for inelastic scattering will find applications in multiple areas. Experimental data for neutron-nucleus inelastic scattering is limited and thus one needs a robust theoretical framework to complement it. Charged-particle inelastic scattering can be used as a surrogate for ( n, γ ) reactions to predict capture cross sections for unstable nuclei. Our work uses microscopic nuclear structure calculations for spherical nuclei to obtain nucleon-nucleus scattering potentials and calculate cross sections for these processes. We implement the Jeukenne, Lejeune, Mahaux (JLM) semi-microscopic folding approach, where the medium effects on nuclear interaction are parameterized in nuclear matter to obtain the nucleon-nucleon ( NN ) interaction in a medium at positive energies. We solve for the nuclear ground state using the Hartree-Fock-Bogliubov (HFB) many-body method, assuming the nucleons within the nucleus interact via the Gogny-D1M potential. The vibrational excited states of the target nucleus are calculated using the quasi-particle random phase approximation (QRPA). We demonstrate our approach for spherical nuclei in the medium-mass region, showing scattering results for the 90 Zr nucleus.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

NASA NTRS1999

Optical model methods of predicting nuclide production cross sections from heavy ion fragmentation

Quantum mechanical optical potential methods for calculating inclusive isotope and element production cross sections from the fragmenting of heavy nuclei by intermediate- and high-energy protons and heavy ions are presented based upon a modified abrasion-ablation-FSI (frictional spectator interaction) collision model. The abrasion stage is treated as a quantum mechanical knockout process that leaves the residual prefragment in an excited state. Prefragment excitation energies are estimated using a combined liquid drop and FSI method. In ablation the prefragment deexcites by particle and photon emission to produce the final fragment. Contributions from electromagnetic dissociation to single nucleon removal cross sections are incorporated using a Weiszacker-Williams theory that includes electric dipole and electric quadrupole interactions. Estimates of elemental and isotopic production cross sections are in good agreement with published cross section measurements for a variety of projectile-target-beam energy combinations.

NASA Discipline Radiation Health↗

DOE OSTI2020

Coupled-cluster techniques for computational chemistry: The CFOUR program package

An up-to-date overview of the CFOUR program system is given. After providing a brief outline of the evolution of the program since its inception in 1989, a comprehensive presentation is given of its well-known capabilities for high-level coupled-cluster theory and its application to molecular properties. Subsequent to this generally well-known background information, much of the remaining content focuses on lesser-known capabilities of CFOUR, most of which have become available to the public only recently or will become available in the near future. Each of these new features is illustrated by a representative example, with additional discussion targeted to educating users as to classes of applications that are now enabled by these capabilities. Lastly, some speculation about future directions is given, and the mode of distribution and support for CFOUR are outlined in the appendix.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Evolution of collectivity in 118 Xe

A recoil-distance Doppler shift experiment has been performed using the Pd 102 ( F 19 , p 2 n ) reaction at a beam energy of 73 MeV to measure the lifetime of excited states in Xe 118 . Additionally, the differential decay-curve method using γ γ coincidences and a gating procedure that allows to extract the lifetime without feeding assumptions has been employed. The lifetimes obtained for the yrast states up to spin-parity 8 + are compared with interacting boson model calculations and Xe 118 can be classified as a transitional nucleus between the spherical and a deformed shape. Systematics of the B ( E 2 ) values for the 2 + → 0 + and 4 + → 2 + transitions in the isotopic chains of tin, tellurium and xenon are presented. It is proposed that a “critical point” exists at which the B ( E 2 ; 4 + → 2 + ) / B ( E 2 ; 2 + → 0 + ) ratio drops to unity for lower neutron numbers within the isotopic chain. The position of the “critical point” varies with proton number, i.e., it is presumed to be located at the same mass number A = 114 in the Sn, Te, and Xe isotopes.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2024

A Bottom-Up Approach to Rational Design of Crystalline Materials: Investigation of Vibronic Coherences Underlying Exciton Dynamics in Semiconductors

In this project we uncovered structure-function relationships of donor-acceptor co-crystals used to develop next-generation optoelectronic devices. Unraveling the photodynamics of molecular crystalline materials poses many challenges for spectroscopy due to broad, overlapping features representing numerous underlying dynamical processes. This leads researchers to make many assumptions about the dynamics of a system in choosing an appropriate kinetic fitting model. Computationally, electronic structure methods are either prohibitively expensive or underdeveloped for computing the excited state structure of molecular materials, especially states that exhibit charge transfer. Researchers must therefore perform calculations of excited electronic states using truncated models of molecular materials. Here we present a joint experimental-theoretical approach to bridging the gap between the photodynamics of a molecular material and its constituent molecules. We focus our efforts on quantifying the timescales and mechanisms of photoexcitation in donor-acceptor co-crystals and donor-acceptor dimers where the lowest-lying excited state is characterized by charge transfer from the donor to the acceptor. We employ ultrafast UV pump, UV-Vis probe transient absorption spectroscopy to unravel the time-resolved spectroscopic signatures of the photodynamics in both the crystalline material and donor-acceptor dimers in solution. We perform electronic structure and excited state dynamics calculations of the dimers to inform kinetic fitting models and assign the spectral features. The photodynamics of the crystal vs. dimer systems have many similarities, enabling unprecedented insights into the formation and evolution of charge transfer excitons in the crystalline systems.

36 MATERIALS SCIENCE↗

NASA NTRS1972

Stabilities of nitrogen containing heterocyclic radicals and geometrical influences on non-radiative processes in organic molecules

Stabilities of nitrogen containing heterocyclic radicals were studied to detect radicals of the type R-N-R, and to theoretically rationalize their electronic structure. The computation of simple potential energy surfaces for ground and excited states is discussed along with the photophysical properties of indolizine. Methods of calculation and problems associated with the calculations are presented. Results, tables, diagrams, discussions, and references are included.

Evleth, E. M.↗

NASA NTRS2003

Stochastic Optimal Control via Bellman's Principle

This paper presents a method for finding optimal controls of nonlinear systems subject to random excitations. The method is capable to generate global control solutions when state and control constraints are present. The solution is global in the sense that controls for all initial conditions in a region of the state space are obtained. The approach is based on Bellman's Principle of optimality, the Gaussian closure and the Short-time Gaussian approximation. Examples include a system with a state-dependent diffusion term, a system in which the infinite hierarchy of moment equations cannot be analytically closed, and an impact system with a elastic boundary. The uncontrolled and controlled dynamics are studied by creating a Markov chain with a control dependent transition probability matrix via the Generalized Cell Mapping method. In this fashion, both the transient and stationary controlled responses are evaluated. The results show excellent control performances.

Crespo, Luis G.↗

DOE OSTI2022

Excited state lifetime modulation in semiconductor nanocrystals for super-resolution imaging

Abstract We report on proof of principle measurements of a concept for a super-resolution imaging method that is based on excitation field density-dependent lifetime modulation of semiconductor nanocrystals. The prerequisite of the technique is access to semiconductor nanocrystals with emission lifetimes that depend on the excitation intensity. Experimentally, the method requires a confocal microscope with fluorescence-lifetime measurement capability that makes it easily accessible to a broad optical imaging community. We demonstrate with single particle imaging that the method allows one to achieve a spatial resolution of the order of several tens of nanometers at moderate fluorescence excitation intensity.

36 MATERIALS SCIENCE↗

DOE OSTI2024

coh3

CoH3 (CoH ver.3) is an optical model, exciton pre-equilibrium, and Hauser-Feshbach statistical model code, which calculates nuclear reaction cross sections for medium to heavy targets in the keV to MeV energy region. This program is written in standard C++, divided into approximately 200 source and header files. CoH solves the Schroedinger equation for optical potentials defined in the code, and calculates differential elastic scattering, reaction, and total cross sections, for neutron, proton, deuteron, triton, 3He, and alpha-particle. Deformed optical potentials are solved with the coupled-channels method, in which the ground state rotational band members, or vibrational phonon states are coupled. The optical model gives particle transmission coefficients that are fed into the statistical model calculations. CoH includes the pre-equilibrium model (exciton model), the direct/semidirect capture model, and the multi-stage Hauser-Feshbach statistical decay with width fluctuation correction based on the Gaussian orthogonal ensemble. For weakly coupled levels, the DWBA (distorted wave Born approximation) method is used to calculate the direct inelastic scattering process to the excited states.

Kawano, Toshihiko↗