nataly kuritz | Tel Aviv University (original) (raw)

Papers by nataly kuritz

Research paper thumbnail of Charge-Transfer-Like πfπ* Excitations in Time-Dependent Density Functional Theory: A Conundrum and Its Solution

fh.huji.ac.il

... Theory Comput. XXXX, XXX, 000-000 ARTICLE pubs.acs.org/JCTC Charge-Transfer-Like πfπ* Excitat... more ... Theory Comput. XXXX, XXX, 000-000 ARTICLE pubs.acs.org/JCTC Charge-Transfer-Like πfπ* Excitations in Time-Dependent Density Functional Theory: A Conundrum and Its Solution Natalia Kuritz, †,§ Tamar Stein, ‡,§ Roi Baer,* ,‡ and Leeor Kronik* ,† ...

Research paper thumbnail of Atomically Wired Molecular Junctions: Connecting a Single Organic Molecule by Chains of Metal Atoms

Nano Letters, 2013

Using a break junction technique, we find a clear signature for the formation of conducting hybri... more Using a break junction technique, we find a clear signature for the formation of conducting hybrid junctions composed of a single organic molecule (benzene, naphthalene or anthracene) connected to chains of platinum atoms. The hybrid junctions exhibit metallic-like conductance (~0.1-1G 0), which is rather insensitive to further elongation by additional atoms. At low bias voltage the hybrid junctions can be elongated significantly beyond the length of the bare atomic chains. Ab initio calculations reveal that benzene based hybrid junctions have a significant binding energy and high structural flexibility that may contribute to the survival of the hybrid junction during the elongation process. The fabrication of hybrid junctions opens the way for combining the different properties of atomic chains and organic molecules to realize a new class of atomic scale interfaces.

Research paper thumbnail of Charge-Transfer-Like π→π* Excitations in Time-Dependent Density Functional Theory: A Conundrum and Its Solution

Journal of Chemical Theory and Computation, 2011

We address the conundrum posed by the well-known failure of time-dependent DFT (TDDFT) with conve... more We address the conundrum posed by the well-known failure of time-dependent DFT (TDDFT) with conventional functionals for "charge-transfer-like" excitations in oligoacenes. We show that this failure is due to a small spatial overlap in orbitals obtained from the underlying single-electron orbitals by means of a unitary transformation. We further show that, as in true chargetransfer excitations, this necessarily results in failure of linear-response TDDFT with standard functionals. Range-separated hybrid functionals have been previously shown to mitigate such errors but at the cost of an empirically adjusted range-separation parameter. Here, we explain why this approach should succeed where conventional functionals fail. Furthermore, we show that optimal tuning of a range-separated hybrid functional, so as to enforce the DFT version of Koopmans' theorem, restores the predictive power of TDDFT even for such difficult cases, without any external reference data and without any adjustable parameters. We demonstrate the success of this approach on the oligoacene series and on related hydrocarbons. This resolves a long-standing question in TDDFT and extends the scope of molecules and systems to which TDDFT can be applied in a predictive manner.

Research paper thumbnail of Charge-Transfer-Like π→π* Excitations in Time-Dependent Density Functional Theory: A Conundrum and Its Solution

Journal of Chemical Theory and Computation, 2011

Research paper thumbnail of Atomically Wired Molecular Junctions: Connecting a Single Organic Molecule by Chains of Metal Atoms

Using a break junction technique, we find a clear signature for the formation of conducting hybri... more Using a break junction technique, we find a clear signature for the formation of conducting hybrid junctions composed of a single organic molecule (benzene, naphthalene, or anthracene) connected to chains of platinum atoms. The hybrid junctions exhibit metallic-like conductance (∼0.1−1G 0 ), which is rather insensitive to further elongation by additional atoms. At low bias voltage the hybrid junctions can be elongated significantly beyond the length of the bare atomic chains. Ab initio calculations reveal that benzene based hybrid junctions have a significant binding energy and high structural flexibility that may contribute to the survival of the hybrid junction during the elongation process. The fabrication of hybrid junctions opens the way for combining the different properties of atomic chains and organic molecules to realize a new class of atomic scale interfaces.

Research paper thumbnail of Charge-Transfer-Like π fπ * Excitations in Time-Dependent Density Functional Theory: A Conundrum and Its Solution

We address the conundrum posed by the well-known failure of time-dependent DFT (TDDFT) with conve... more We address the conundrum posed by the well-known failure of time-dependent DFT (TDDFT) with conventional functionals for "charge-transfer-like" excitations in oligoacenes. We show that this failure is due to a small spatial overlap in orbitals obtained from the underlying single-electron orbitals by means of a unitary transformation. We further show that, as in true chargetransfer excitations, this necessarily results in failure of linear-response TDDFT with standard functionals. Range-separated hybrid functionals have been previously shown to mitigate such errors but at the cost of an empirically adjusted range-separation parameter. Here, we explain why this approach should succeed where conventional functionals fail. Furthermore, we show that optimal tuning of a range-separated hybrid functional, so as to enforce the DFT version of Koopmans' theorem, restores the predictive power of TDDFT even for such difficult cases, without any external reference data and without any adjustable parameters. We demonstrate the success of this approach on the oligoacene series and on related hydrocarbons. This resolves a long-standing question in TDDFT and extends the scope of molecules and systems to which TDDFT can be applied in a predictive manner.

Research paper thumbnail of Charge-Transfer-Like πfπ* Excitations in Time-Dependent Density Functional Theory: A Conundrum and Its Solution

fh.huji.ac.il

... Theory Comput. XXXX, XXX, 000-000 ARTICLE pubs.acs.org/JCTC Charge-Transfer-Like πfπ* Excitat... more ... Theory Comput. XXXX, XXX, 000-000 ARTICLE pubs.acs.org/JCTC Charge-Transfer-Like πfπ* Excitations in Time-Dependent Density Functional Theory: A Conundrum and Its Solution Natalia Kuritz, †,§ Tamar Stein, ‡,§ Roi Baer,* ,‡ and Leeor Kronik* ,† ...

Research paper thumbnail of Atomically Wired Molecular Junctions: Connecting a Single Organic Molecule by Chains of Metal Atoms

Nano Letters, 2013

Using a break junction technique, we find a clear signature for the formation of conducting hybri... more Using a break junction technique, we find a clear signature for the formation of conducting hybrid junctions composed of a single organic molecule (benzene, naphthalene or anthracene) connected to chains of platinum atoms. The hybrid junctions exhibit metallic-like conductance (~0.1-1G 0), which is rather insensitive to further elongation by additional atoms. At low bias voltage the hybrid junctions can be elongated significantly beyond the length of the bare atomic chains. Ab initio calculations reveal that benzene based hybrid junctions have a significant binding energy and high structural flexibility that may contribute to the survival of the hybrid junction during the elongation process. The fabrication of hybrid junctions opens the way for combining the different properties of atomic chains and organic molecules to realize a new class of atomic scale interfaces.

Research paper thumbnail of Charge-Transfer-Like π→π* Excitations in Time-Dependent Density Functional Theory: A Conundrum and Its Solution

Journal of Chemical Theory and Computation, 2011

We address the conundrum posed by the well-known failure of time-dependent DFT (TDDFT) with conve... more We address the conundrum posed by the well-known failure of time-dependent DFT (TDDFT) with conventional functionals for "charge-transfer-like" excitations in oligoacenes. We show that this failure is due to a small spatial overlap in orbitals obtained from the underlying single-electron orbitals by means of a unitary transformation. We further show that, as in true chargetransfer excitations, this necessarily results in failure of linear-response TDDFT with standard functionals. Range-separated hybrid functionals have been previously shown to mitigate such errors but at the cost of an empirically adjusted range-separation parameter. Here, we explain why this approach should succeed where conventional functionals fail. Furthermore, we show that optimal tuning of a range-separated hybrid functional, so as to enforce the DFT version of Koopmans' theorem, restores the predictive power of TDDFT even for such difficult cases, without any external reference data and without any adjustable parameters. We demonstrate the success of this approach on the oligoacene series and on related hydrocarbons. This resolves a long-standing question in TDDFT and extends the scope of molecules and systems to which TDDFT can be applied in a predictive manner.

Research paper thumbnail of Charge-Transfer-Like π→π* Excitations in Time-Dependent Density Functional Theory: A Conundrum and Its Solution

Journal of Chemical Theory and Computation, 2011

Research paper thumbnail of Atomically Wired Molecular Junctions: Connecting a Single Organic Molecule by Chains of Metal Atoms

Using a break junction technique, we find a clear signature for the formation of conducting hybri... more Using a break junction technique, we find a clear signature for the formation of conducting hybrid junctions composed of a single organic molecule (benzene, naphthalene, or anthracene) connected to chains of platinum atoms. The hybrid junctions exhibit metallic-like conductance (∼0.1−1G 0 ), which is rather insensitive to further elongation by additional atoms. At low bias voltage the hybrid junctions can be elongated significantly beyond the length of the bare atomic chains. Ab initio calculations reveal that benzene based hybrid junctions have a significant binding energy and high structural flexibility that may contribute to the survival of the hybrid junction during the elongation process. The fabrication of hybrid junctions opens the way for combining the different properties of atomic chains and organic molecules to realize a new class of atomic scale interfaces.

Research paper thumbnail of Charge-Transfer-Like π fπ * Excitations in Time-Dependent Density Functional Theory: A Conundrum and Its Solution

We address the conundrum posed by the well-known failure of time-dependent DFT (TDDFT) with conve... more We address the conundrum posed by the well-known failure of time-dependent DFT (TDDFT) with conventional functionals for "charge-transfer-like" excitations in oligoacenes. We show that this failure is due to a small spatial overlap in orbitals obtained from the underlying single-electron orbitals by means of a unitary transformation. We further show that, as in true chargetransfer excitations, this necessarily results in failure of linear-response TDDFT with standard functionals. Range-separated hybrid functionals have been previously shown to mitigate such errors but at the cost of an empirically adjusted range-separation parameter. Here, we explain why this approach should succeed where conventional functionals fail. Furthermore, we show that optimal tuning of a range-separated hybrid functional, so as to enforce the DFT version of Koopmans' theorem, restores the predictive power of TDDFT even for such difficult cases, without any external reference data and without any adjustable parameters. We demonstrate the success of this approach on the oligoacene series and on related hydrocarbons. This resolves a long-standing question in TDDFT and extends the scope of molecules and systems to which TDDFT can be applied in a predictive manner.