Evert-jan Baerends - Academia.edu (original) (raw)
Papers by Evert-jan Baerends
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Journal of Chemical Physics, Aug 8, 1998
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International Journal of Quantum Chemistry, Mar 12, 1988
... LIANGYOU FAN, LOUIS VERSLUIS, and TOM ZIEGLER Department of Chemistry, University of Calgary,... more ... LIANGYOU FAN, LOUIS VERSLUIS, and TOM ZIEGLER Department of Chemistry, University of Calgary, Calgary, Alberta, Canada EVERT JAN BAERENDS and WALTER RAVENEK ... set of linear equations A=M 1 [FTk - E~S,JC~~ = 0 T = l,M A=l The matrix elements FrA are in ...
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Chemical Physics, Nov 1, 1993
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Journal of Physical Chemistry A, Sep 19, 2001
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Chemical Physics, Aug 1, 1976
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In this paper, the history, present status, and future of density-functional theory (DFT) is info... more In this paper, the history, present status, and future of density-functional theory (DFT) is informally reviewed and discussed by 70 workers in the field, including molecular scientists, materials scientists, method developers and practitioners. The format of the paper is that of a roundtable discussion, in which the participants express and exchange views on DFT in the form of 300 individual contributions, formulated as responses to a preset list of 26 questions. Supported by a bibliography of 776 entries, the paper represents a broad snapshot of DFT, anno 2022.
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Physical Chemistry Chemical Physics, 2016
Probabilities of single ionization channels or double and multiple simultaneous ionization can be... more Probabilities of single ionization channels or double and multiple simultaneous ionization can be determined from exact master equations for time-dependent Dyson orbitals.
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The Journal of chemical physics, 2004
We present density functional theory calculations for atomic hydrogen interacting with a stepped ... more We present density functional theory calculations for atomic hydrogen interacting with a stepped surface, the Pt(211) surface. The calculations have been performed at the generalized gradient approximation level, using a slab representation of the surface. This is the state-of-the-art method for calculating the interaction of atoms or molecules with metal surfaces, nevertheless only few studies have used it to study atoms or molecules interacting with stepped surfaces, and none, to the best of our knowledge, have considered hydrogen interacting with stepped platinum surfaces. Our goal has been to initiate a systematic study of this topic. We have calculated the full three-dimensional potential energy surface (PES) for the H/Pt(211) system together with the vibrational band structure and vibrational eigenfunctions of H. A deep global minimum of the PES is found for bridge-bonded hydrogen on the step edge, in agreement with experimental results for the similar H/Pt(533) system. All th...
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ACS Catalysis, 2015
We analyze with DFT calculations the charge effects on the reactivity of the polycationic Compoun... more We analyze with DFT calculations the charge effects on the reactivity of the polycationic Compound I (Cpd I) and Compound II (Cpd II) mimics experimentally investigated by Bell and Groves (Bell, S. R.; Groves, J. T. J. Am. Chem. Soc. 2009, 131, 9640). Specifically, we consider the Cpd I model [(4-THPyP)•+(H2O)FeIV═O]5+ (THPyP = 5,10,15,20-tetrakis(N-hydro-4-pyridinium) porphyrinate), 1H2O, and its Cpd II counterparts [(4-THPyP)FeIV═O]4+, 2, and [(4-THPyP)(H2O)FeIV═O]4+, 2H2O. In gas phase simulations it is found that all positive charges enhance the reactivity. According to a detailed electronic structure analysis in the gas phase of the reactant complexes en route to the transition state, the positive charges stabilize the electron acceptor orbital (EAO) of the catalyst more than the electron donor orbital (EDO) of the substrate, thereby reducing the energy gap between these orbitals and, hence, the H-abstraction barrier. The effect of the peripheral charges residing on the pyridinium groups is dampened ...
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Chemical Physics, 1993
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The Journal of chemical physics, Jan 28, 2015
π-electron conjugation and aromaticity are commonly associated with delocalization and especially... more π-electron conjugation and aromaticity are commonly associated with delocalization and especially high mobility of the π electrons. We investigate if also the electron correlation (pair density) exhibits signatures of the special electronic structure of conjugated systems. To that end the shape and extent of the pair density and derived quantities (exchange-correlation hole, Coulomb hole, and conditional density) are investigated for the prototype systems ethylene, hexatriene, and benzene. The answer is that the effects of π electron conjugation are hardly discernible in the real space representations of the electron correlation. We find the xc hole to be as localized (confined to atomic or diatomic regions) in conjugated systems as in small molecules. This result is relevant for density functional theory (DFT). The potential of the electron exchange-correlation hole is the largest part of vxc, the exchange-correlation Kohn-Sham potential. So the extent of the hole directly affects ...
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The Journal of Physical Chemistry A, 1999
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Physical Review Letters, 2001
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Journal of Organometallic Chemistry, 1987
... is usually described in a qualitative fashion in terms of the DewarChattDuncanson model [1]. ... more ... is usually described in a qualitative fashion in terms of the DewarChattDuncanson model [1]. in which there are two synergic alkenemetal bonding interactions: ligandtometal odona tion (Fig. ... 713 00601 (1,1 324 18 12 2 93 98 97 84 93 2 7,, i4 6a 3h, 3h1 11)2 a 70 are don h)i ...
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The Journal of Chemical Physics, 2011
We demonstrate and advocate the use of observable quantities derived from the two-electron reduce... more We demonstrate and advocate the use of observable quantities derived from the two-electron reduced density matrix - pair densities, conditional densities, and exchange-correlation holes--as signatures of the type of electron correlation in a chemical bond. The prototype cases of the lowest (1)Σ(u)(+) and (1)Σ(g)(+) states of H(2), which exhibit large variation in types of bonding, ranging from strongly ionic to covalent, are discussed. Both the excited (1)Σ(g)(+) and (1)Σ(u)(+) states have been interpreted as essentially consisting of (natural) orbital configurations with an inner electron in a contracted 1sσ(g) orbital and an outer electron in a diffuse (united atom type, Rydberg) orbital. We show that nevertheless totally different correlation behavior is encountered in various states when comparing them at a common internuclear distance. Also when following one state along the internuclear distance coordinate, strong variation in correlation behavior is observed, as expected. Switches between ionic to covalent character of a state occur till very large distances (40 bohrs for states approaching the 1s3[script-l] asymptotic limit, and 282 bohrs for states approaching the 1s4[script-l] limit).
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The Journal of Chemical Physics, 2003
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Inorganic Chemistry, 1999
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Journal of Chemical Physics, Aug 8, 1998
Bookmarks Related papers MentionsView impact
International Journal of Quantum Chemistry, Mar 12, 1988
... LIANGYOU FAN, LOUIS VERSLUIS, and TOM ZIEGLER Department of Chemistry, University of Calgary,... more ... LIANGYOU FAN, LOUIS VERSLUIS, and TOM ZIEGLER Department of Chemistry, University of Calgary, Calgary, Alberta, Canada EVERT JAN BAERENDS and WALTER RAVENEK ... set of linear equations A=M 1 [FTk - E~S,JC~~ = 0 T = l,M A=l The matrix elements FrA are in ...
Bookmarks Related papers MentionsView impact
Chemical Physics, Nov 1, 1993
Bookmarks Related papers MentionsView impact
Journal of Physical Chemistry A, Sep 19, 2001
Bookmarks Related papers MentionsView impact
Chemical Physics, Aug 1, 1976
Bookmarks Related papers MentionsView impact
In this paper, the history, present status, and future of density-functional theory (DFT) is info... more In this paper, the history, present status, and future of density-functional theory (DFT) is informally reviewed and discussed by 70 workers in the field, including molecular scientists, materials scientists, method developers and practitioners. The format of the paper is that of a roundtable discussion, in which the participants express and exchange views on DFT in the form of 300 individual contributions, formulated as responses to a preset list of 26 questions. Supported by a bibliography of 776 entries, the paper represents a broad snapshot of DFT, anno 2022.
Bookmarks Related papers MentionsView impact
Bookmarks Related papers MentionsView impact
Physical Chemistry Chemical Physics, 2016
Probabilities of single ionization channels or double and multiple simultaneous ionization can be... more Probabilities of single ionization channels or double and multiple simultaneous ionization can be determined from exact master equations for time-dependent Dyson orbitals.
Bookmarks Related papers MentionsView impact
The Journal of chemical physics, 2004
We present density functional theory calculations for atomic hydrogen interacting with a stepped ... more We present density functional theory calculations for atomic hydrogen interacting with a stepped surface, the Pt(211) surface. The calculations have been performed at the generalized gradient approximation level, using a slab representation of the surface. This is the state-of-the-art method for calculating the interaction of atoms or molecules with metal surfaces, nevertheless only few studies have used it to study atoms or molecules interacting with stepped surfaces, and none, to the best of our knowledge, have considered hydrogen interacting with stepped platinum surfaces. Our goal has been to initiate a systematic study of this topic. We have calculated the full three-dimensional potential energy surface (PES) for the H/Pt(211) system together with the vibrational band structure and vibrational eigenfunctions of H. A deep global minimum of the PES is found for bridge-bonded hydrogen on the step edge, in agreement with experimental results for the similar H/Pt(533) system. All th...
Bookmarks Related papers MentionsView impact
ACS Catalysis, 2015
We analyze with DFT calculations the charge effects on the reactivity of the polycationic Compoun... more We analyze with DFT calculations the charge effects on the reactivity of the polycationic Compound I (Cpd I) and Compound II (Cpd II) mimics experimentally investigated by Bell and Groves (Bell, S. R.; Groves, J. T. J. Am. Chem. Soc. 2009, 131, 9640). Specifically, we consider the Cpd I model [(4-THPyP)•+(H2O)FeIV═O]5+ (THPyP = 5,10,15,20-tetrakis(N-hydro-4-pyridinium) porphyrinate), 1H2O, and its Cpd II counterparts [(4-THPyP)FeIV═O]4+, 2, and [(4-THPyP)(H2O)FeIV═O]4+, 2H2O. In gas phase simulations it is found that all positive charges enhance the reactivity. According to a detailed electronic structure analysis in the gas phase of the reactant complexes en route to the transition state, the positive charges stabilize the electron acceptor orbital (EAO) of the catalyst more than the electron donor orbital (EDO) of the substrate, thereby reducing the energy gap between these orbitals and, hence, the H-abstraction barrier. The effect of the peripheral charges residing on the pyridinium groups is dampened ...
Bookmarks Related papers MentionsView impact
Chemical Physics, 1993
Bookmarks Related papers MentionsView impact
Bookmarks Related papers MentionsView impact
The Journal of chemical physics, Jan 28, 2015
π-electron conjugation and aromaticity are commonly associated with delocalization and especially... more π-electron conjugation and aromaticity are commonly associated with delocalization and especially high mobility of the π electrons. We investigate if also the electron correlation (pair density) exhibits signatures of the special electronic structure of conjugated systems. To that end the shape and extent of the pair density and derived quantities (exchange-correlation hole, Coulomb hole, and conditional density) are investigated for the prototype systems ethylene, hexatriene, and benzene. The answer is that the effects of π electron conjugation are hardly discernible in the real space representations of the electron correlation. We find the xc hole to be as localized (confined to atomic or diatomic regions) in conjugated systems as in small molecules. This result is relevant for density functional theory (DFT). The potential of the electron exchange-correlation hole is the largest part of vxc, the exchange-correlation Kohn-Sham potential. So the extent of the hole directly affects ...
Bookmarks Related papers MentionsView impact
The Journal of Physical Chemistry A, 1999
Bookmarks Related papers MentionsView impact
Physical Review Letters, 2001
Bookmarks Related papers MentionsView impact
Journal of Organometallic Chemistry, 1987
... is usually described in a qualitative fashion in terms of the DewarChattDuncanson model [1]. ... more ... is usually described in a qualitative fashion in terms of the DewarChattDuncanson model [1]. in which there are two synergic alkenemetal bonding interactions: ligandtometal odona tion (Fig. ... 713 00601 (1,1 324 18 12 2 93 98 97 84 93 2 7,, i4 6a 3h, 3h1 11)2 a 70 are don h)i ...
Bookmarks Related papers MentionsView impact
The Journal of Chemical Physics, 2011
We demonstrate and advocate the use of observable quantities derived from the two-electron reduce... more We demonstrate and advocate the use of observable quantities derived from the two-electron reduced density matrix - pair densities, conditional densities, and exchange-correlation holes--as signatures of the type of electron correlation in a chemical bond. The prototype cases of the lowest (1)Σ(u)(+) and (1)Σ(g)(+) states of H(2), which exhibit large variation in types of bonding, ranging from strongly ionic to covalent, are discussed. Both the excited (1)Σ(g)(+) and (1)Σ(u)(+) states have been interpreted as essentially consisting of (natural) orbital configurations with an inner electron in a contracted 1sσ(g) orbital and an outer electron in a diffuse (united atom type, Rydberg) orbital. We show that nevertheless totally different correlation behavior is encountered in various states when comparing them at a common internuclear distance. Also when following one state along the internuclear distance coordinate, strong variation in correlation behavior is observed, as expected. Switches between ionic to covalent character of a state occur till very large distances (40 bohrs for states approaching the 1s3[script-l] asymptotic limit, and 282 bohrs for states approaching the 1s4[script-l] limit).
Bookmarks Related papers MentionsView impact
The Journal of Chemical Physics, 2003
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Inorganic Chemistry, 1999
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