Computational methods for the one-particle green's function

Niessen, W. von; Schirmer, J.; Cederbaum, Lorenz S.

doi:10.1016/0167-7977(84)90002-9

Cited by 1,092 publications

(671 citation statements)

References 116 publications

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“…Still, for clarity, we should note that, in the present terminology, the method of ref. 29 coincides with that labeled "2nd-order pole" here, as it corresponds to the second-order correction in the the electron-electron interaction to the electronic self-energy 21,22 . So, the results labeled "MP2-based" and "2nd-order pole" in Table 8 should coincide.…”

Section: Comparison With Results Of Previously Utilized Manybody Methodsmentioning

confidence: 53%

“…(iii) The outer valence Green's function (OVGF) method 22,33 represents the most elaborate quantum chemical approach based on a single-particle picture. To the best of our knowledge, the OVFG approach has not yet been utilized in molecular transport studies.…”

Section: Methodsmentioning

confidence: 99%

“…Details can be found in ref. 22,33 . As explained below, this method is superior to the MP2-like approximation used recently 20 (see sec.…”

Section: Methodsmentioning

confidence: 99%

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A quantum chemical study from a molecular transport perspective: ionization and electron attachment energies for species often used to fabricate single-molecule junctions

Bâldea

2014

Faraday Discuss.

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Abstract:The accurate determination of the lowest electron attachment (EA) and ionization (IP) energies for molecules embedded in molecular junctions is important for correctly estimating, e.g., the magnitude of the currents (I) or the biases (V ) where an I −V -curve exhibits a significant non-Ohmic behavior. Benchmark calculations for the lowest electron attachment and ionization energies of several typical molecules utilized to fabricate single-molecule junctions characterized by n-type conduction (4,4'-bipyridine, 1,4-dicyanobenzene, and 4,4'-dicyano-1,1'-biphenyl) and p-type conduction (benzenedithiol, biphenyldithiol, hexanemonothiol, and hexanedithiol] based on the EOM-CCSD (equation-of-motion coupled-cluster singles and doubles) state-of-the-art method of quantum chemistry are presented. They indicate significant differences from the results obtained within current approaches to molecular transport. The present study emphasizes that, in addition to a reliable quantum chemical method, basis sets much better than the ubiquitous double-zeta set employed for transport calculations are needed. The latter is a particularly critical issue for correctly determining EA's, which is impossible without including sufficient diffuse basis functions. The spatial distribution of the dominant molecular orbitals (MO's) is another important issue, on which the present study draws attention, because it sensitively affects the MO-energy shifts Φ due to image charges formed in electrodes. The present results cannot substantiate the common assumption of a point-like MO midway between electrodes, which substantially affects the actual Φ-values.

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Section: Comparison With Results Of Previously Utilized Manybody Methodsmentioning

confidence: 53%

Section: Methodsmentioning

confidence: 99%

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A quantum chemical study from a molecular transport perspective: ionization and electron attachment energies for species often used to fabricate single-molecule junctions

Bâldea

2014

Faraday Discuss.

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“…We shall particularly concentrate hereafter on the third order, ADC(3), approximation, 6,17,18 but most considerations apply equally well to higher order schemes. In ADC(3) four classes of ionic configurations appear: one-hole (1h) and two-hole-one-particle (2h1p) for the N 2 1-electron configurations, one-particle (1p) and two-particle-one-hole (2p1h) for the N 1 1-electron configurations.…”

Section: The Adc(3) Schemementioning

confidence: 99%

“…The secular matrix is conveniently partitioned as shown in Figure 1 and its matrix elements are reported and discussed at length in, for example, ref. 17. The upper-left block (main block) represents the interaction over the 1p and 1h configurations and includes the energy-independent part of the selfenergy, S(1).…”

Section: The Adc(3) Schemementioning

confidence: 99%

Implementation and use of a direct, partially integral‐driven non‐Dyson propagator method for molecular ionization

2008

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The Green's function ADC(3) scheme has been for many years a successful method to predict theoretically the ionization (and electron affinity) spectrum of molecules. However, a dramatic enhancement of the method's power has come only recently, with the development of an approximation method to the one-particle Green's function which does not make direct use of the Dyson equation. In the present work, we present an efficient computer implementation of this novel approach, with first comparative tests demonstrating its enormous computational advantage over the conventional approach.

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Comparison of perturbative and multiconfigurational electron propagator methods

Zakrzewski

Ortiz

Nichols

et al. 1996

Int. J. Quantum Chem.

212

150

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Ionization energies below 20 eV of 10 molecules calculated with electron propagator techniques employing Hartree-Fock orbitals and multiconfigurational self-consistent field orbitals are compared. Diagonal and nondiagonal self-energy approximations are used in the perturbative formalism. Three diagonal methods based on second-and third-order self-energy terms, all known as the outer valence Green's function, are discussed. A procedure for selecting the most reliable of these three versions for a given calculation is tested. Results with a polarized, triple < basis produce root mean square errors with respect to experiment of approximately 0.3 eV. Use of the selection procedure has a slight influence on the quality of the results. A related, nondiagonal method, known as ADC(3), performs infinite-order summations on several types of self-energy contributions, is complete through third-order, and produces similar accuracy. These results are compared to ionization energies calculated with the multiconfigurational spin-tensor electron propagator method. Complete active space wave functions or close approximations constitute the reference states. Simple field operators and transfer operators pertaining to the active space define the operator manifold. With the same basis sets, these methods produce ionization energies with accuracy that is comparable to that of the perturbative techniques.

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Computational methods for the one-particle green's function

Cited by 1,092 publications

References 116 publications

A quantum chemical study from a molecular transport perspective: ionization and electron attachment energies for species often used to fabricate single-molecule junctions

A quantum chemical study from a molecular transport perspective: ionization and electron attachment energies for species often used to fabricate single-molecule junctions

Implementation and use of a direct, partially integral‐driven non‐Dyson propagator method for molecular ionization

Comparison of perturbative and multiconfigurational electron propagator methods

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