Dr. Polina Lisinetskaya
Post Doc
Room: 00.012
Phone: +49-(0)931-31-80667
Mail: polina.lisinetskaya@uni-wuerzburg.de
Graduation
M. Sc. in Physics (National Academy of Sciences of Belarus) 07/2008
Research Interests
- Methods for the simulation of the optical properties of small metal clusters and their aggregates.
Publication List
9. | Muessig, Jonas; Lisinetskaya, Polina; Dewhurst, Rian; Bertermann, Rüdiger; Thaler, Melanie; Mitrić, Roland; Braunschweig, Holger Tetraiododiborane(4) (B2I4) is a Polymer based on sp3 Boron in the Solid State Journal Article Angew. Chem., 132 , pp. 1-7, 2020. @article{polina19b, title = {Tetraiododiborane(4) (B_{2}I_{4}) is a Polymer based on sp^{3} Boron in the Solid State}, author = {Jonas Muessig and Polina Lisinetskaya and Rian Dewhurst and Rüdiger Bertermann and Melanie Thaler and Roland Mitrić and Holger Braunschweig }, doi = {10.1002/ange.201913590}, year = {2020}, date = {2020-03-27}, journal = {Angew. Chem.}, volume = {132}, pages = {1-7}, keywords = {}, pubstate = {published}, tppubtype = {article} } |
8. | Lisinetskaya, Polina G; Mitric, Roland Collective Response in DNA-Stabilized Silver Cluster Assemblies from First-Principles Simulations Journal Article J. Phys. Chem. Lett., 10 , pp. 7884-7889, 2019. @article{polina19jpcl, title = {Collective Response in DNA-Stabilized Silver Cluster Assemblies from First-Principles Simulations}, author = {Polina G Lisinetskaya and Roland Mitric}, url = {https://pubs.acs.org/doi/10.1021/acs.jpclett.9b03136}, doi = {10.1021/acs.jpclett.9b03136}, year = {2019}, date = {2019-11-27}, journal = {J. Phys. Chem. Lett.}, volume = {10}, pages = {7884-7889}, abstract = {We investigate fluorescence resonant energy transfer and concurrent electron dynamics in a pair of DNA-stabilized silver clusters. For this purpose we introduce a methodology for the simulation of collective opto-electronic properties of coupled molecular aggregates starting from first-principles quantum chemistry, which can be further applied to a broad range of coupled molecular systems to study their electrooptical response. Our simulations reveal the existence of a low-energy coupled excitonic states, which enable ultrafast energy transport between subunits, and give an insight into the origin of the fluorescence signal in coupled DNA-stabilized silver clusters, that have been recently experimentally detected. Hence we demonstrate the possibility to construct an ultrasmall energy transmission lines and optical converters based on these hybrid molecular systems.}, keywords = {}, pubstate = {published}, tppubtype = {article} } We investigate fluorescence resonant energy transfer and concurrent electron dynamics in a pair of DNA-stabilized silver clusters. For this purpose we introduce a methodology for the simulation of collective opto-electronic properties of coupled molecular aggregates starting from first-principles quantum chemistry, which can be further applied to a broad range of coupled molecular systems to study their electrooptical response. Our simulations reveal the existence of a low-energy coupled excitonic states, which enable ultrafast energy transport between subunits, and give an insight into the origin of the fluorescence signal in coupled DNA-stabilized silver clusters, that have been recently experimentally detected. Hence we demonstrate the possibility to construct an ultrasmall energy transmission lines and optical converters based on these hybrid molecular systems. |
7. | Röhr, Merle I S; Lisinetskaya, Polina G; Mitric, Roland. Excitonic Properties of Ordered Metal Nanocluster Arrays: 2D Silver Clusters at Multiporphyrin Templates. Journal Article J. Phys. Chem. A, 120 (26), pp. 4465–4472, 2016, ISSN: 1089-5639. @article{Röhr2016, title = {Excitonic Properties of Ordered Metal Nanocluster Arrays: 2D Silver Clusters at Multiporphyrin Templates.}, author = {Merle I S Röhr and Polina G Lisinetskaya and Roland. Mitric}, doi = {10.1021/acs.jpca.6b04243}, issn = {1089-5639}, year = {2016}, date = {2016-01-01}, journal = {J. Phys. Chem. A}, volume = {120}, number = {26}, pages = {4465--4472}, publisher = {American Chemical Society}, abstract = {The design of ordered arrays of metal nanoclusters such as, for example, two-dimensional cluster-org. frameworks might open a new route toward the development of materials with tailored optical properties. Such systems could serve as plasmonically enhanced light-harvesting materials, sensors, or catalysts. The authors present here a theor. approach for the simulation of the optical properties of ordered arrays of metal clusters that is based on the ab initio parametrized Frenkel exciton model. Small atomically precise Ag clusters can be assembled in 1- and two-dimensional arrays on suitably designed porphyrin templates exhibiting remarkable optical properties. By employing explicit time-dependent d. functional theory calcns. on smaller homologs, the intrinsic optical properties of metal clusters are largely preserved but undergo J- and H-type excitonic coupling that results in controllable splitting of their excited states. Also, ab initio parametrized Frenkel exciton model calcns. allow the authors to predict an energetic splitting of up to 0.77 eV in extended two-dimensional square arrays and 0.79 eV in tilted square aggregates contg. up to 25 cluster-porphyrin subunits. [on SciFinder(R)]}, keywords = {}, pubstate = {published}, tppubtype = {article} } The design of ordered arrays of metal nanoclusters such as, for example, two-dimensional cluster-org. frameworks might open a new route toward the development of materials with tailored optical properties. Such systems could serve as plasmonically enhanced light-harvesting materials, sensors, or catalysts. The authors present here a theor. approach for the simulation of the optical properties of ordered arrays of metal clusters that is based on the ab initio parametrized Frenkel exciton model. Small atomically precise Ag clusters can be assembled in 1- and two-dimensional arrays on suitably designed porphyrin templates exhibiting remarkable optical properties. By employing explicit time-dependent d. functional theory calcns. on smaller homologs, the intrinsic optical properties of metal clusters are largely preserved but undergo J- and H-type excitonic coupling that results in controllable splitting of their excited states. Also, ab initio parametrized Frenkel exciton model calcns. allow the authors to predict an energetic splitting of up to 0.77 eV in extended two-dimensional square arrays and 0.79 eV in tilted square aggregates contg. up to 25 cluster-porphyrin subunits. [on SciFinder(R)] |
6. | Lisinetskaya, Polina G; Röhr, Merle I S; Mitric, Roland. First-principles simulation of light propagation and exciton dynamics in metal cluster nanostructures. Journal Article Applied Physics B: Lasers and Optics, 122 (6), pp. 1–12, 2016, ISSN: 0946-2171. @article{Lisinetskaya2016, title = {First-principles simulation of light propagation and exciton dynamics in metal cluster nanostructures.}, author = {Polina G Lisinetskaya and Merle I S Röhr and Roland. Mitric}, doi = {10.1007/s00340-016-6436-6}, issn = {0946-2171}, year = {2016}, date = {2016-01-01}, journal = {Applied Physics B: Lasers and Optics}, volume = {122}, number = {6}, pages = {1--12}, publisher = {Springer}, abstract = {We present a theor. approach for the simulation of the elec. field and exciton propagation in ordered arrays constructed of mol.-sized noble metal clusters bound to org. polymer templates. In order to describe the electronic coupling between individual constituents of the nanostructure we use the ab initio parameterized transition charge method which is more accurate than the usual dipole-dipole coupling. The electronic population dynamics in the nanostructure under an external laser pulse excitation is simulated by numerical integration of the time-dependent Schrodinger equation employing the fully coupled Hamiltonian. The soln. of the TDSE gives rise to time-dependent partial point charges for each subunit of the nanostructure, and the spatio-temporal elec. field distribution is evaluated by means of classical electrodynamics methods. The time-dependent partial charges are detd. based on the stationary partial and transition charges obtained in the framework of the TDDFT. In order to treat large plasmonic nanostructures constructed of many constituents, the approx. self-consistent iterative approach presented in (Lisinetskaya and Mitric in Phys Rev B 89:035433, 2014) is modified to include the transition-charge-based interaction. The developed methods are used to study the optical response and exciton dynamics of Ag+3 and porphyrin-Ag4 dimers. Subsequently, the spatio-temporal elec. field distribution in a ring constructed of ten porphyrin-Ag4 subunits under the action of circularly polarized laser pulse is simulated. The presented methodol. provides a theor. basis for the investigation of coupled light-exciton propagation in nanoarchitectures built from mol. size metal nanoclusters in which quantum confinement effects are important. [on SciFinder(R)]}, keywords = {}, pubstate = {published}, tppubtype = {article} } We present a theor. approach for the simulation of the elec. field and exciton propagation in ordered arrays constructed of mol.-sized noble metal clusters bound to org. polymer templates. In order to describe the electronic coupling between individual constituents of the nanostructure we use the ab initio parameterized transition charge method which is more accurate than the usual dipole-dipole coupling. The electronic population dynamics in the nanostructure under an external laser pulse excitation is simulated by numerical integration of the time-dependent Schrodinger equation employing the fully coupled Hamiltonian. The soln. of the TDSE gives rise to time-dependent partial point charges for each subunit of the nanostructure, and the spatio-temporal elec. field distribution is evaluated by means of classical electrodynamics methods. The time-dependent partial charges are detd. based on the stationary partial and transition charges obtained in the framework of the TDDFT. In order to treat large plasmonic nanostructures constructed of many constituents, the approx. self-consistent iterative approach presented in (Lisinetskaya and Mitric in Phys Rev B 89:035433, 2014) is modified to include the transition-charge-based interaction. The developed methods are used to study the optical response and exciton dynamics of Ag+3 and porphyrin-Ag4 dimers. Subsequently, the spatio-temporal elec. field distribution in a ring constructed of ten porphyrin-Ag4 subunits under the action of circularly polarized laser pulse is simulated. The presented methodol. provides a theor. basis for the investigation of coupled light-exciton propagation in nanoarchitectures built from mol. size metal nanoclusters in which quantum confinement effects are important. [on SciFinder(R)] |
5. | Lisinetskaya, Polina G; Braun, Christian; Proch, Sebastian; Kim, Young Dok; Gantefoer, Gerd; Mitric, Roland. Excited state nonadiabatic dynamics of bare and hydrated anionic gold clusters Au3-[H2O]n (n = 0-2). Journal Article Physical Chemistry Chemical Physics, 18 (9), pp. 6411–6419, 2016, ISSN: 1463-9076. @article{Lisinetskaya2016a, title = {Excited state nonadiabatic dynamics of bare and hydrated anionic gold clusters Au3-[H2O]n (n = 0-2).}, author = {Polina G Lisinetskaya and Christian Braun and Sebastian Proch and Young Dok Kim and Gerd Gantefoer and Roland. Mitric}, doi = {10.1039/C5CP04297F}, issn = {1463-9076}, year = {2016}, date = {2016-01-01}, journal = {Physical Chemistry Chemical Physics}, volume = {18}, number = {9}, pages = {6411--6419}, publisher = {Royal Society of Chemistry}, abstract = {We present a joint theor. and exptl. study of excited state dynamics in pure and hydrated anionic gold clusters Au3-[H2O]n (n = 0-2). We employ mixed quantum-classical dynamics combined with femtosecond time-resolved photoelectron spectroscopy in order to investigate the influence of hydration on excited state lifetimes and photo-dissocn. dynamics. A gradual decrease of the excited state lifetime with the no. of adsorbed water mols. as well as gold cluster fragmentation quenching by two or more water mols. are obsd. both in expt. and in simulations. Nonradiative relaxation and dissocn. in excited states are found to be responsible for the excited state population depletion. Time consts. of these two processes strongly depend on the no. of water mols. leading to the possibility to modulate excited state dynamics and fragmentation of the anionic cluster by adsorption of water mols. [on SciFinder(R)]}, keywords = {}, pubstate = {published}, tppubtype = {article} } We present a joint theor. and exptl. study of excited state dynamics in pure and hydrated anionic gold clusters Au3-[H2O]n (n = 0-2). We employ mixed quantum-classical dynamics combined with femtosecond time-resolved photoelectron spectroscopy in order to investigate the influence of hydration on excited state lifetimes and photo-dissocn. dynamics. A gradual decrease of the excited state lifetime with the no. of adsorbed water mols. as well as gold cluster fragmentation quenching by two or more water mols. are obsd. both in expt. and in simulations. Nonradiative relaxation and dissocn. in excited states are found to be responsible for the excited state population depletion. Time consts. of these two processes strongly depend on the no. of water mols. leading to the possibility to modulate excited state dynamics and fragmentation of the anionic cluster by adsorption of water mols. [on SciFinder(R)] |
4. | Lisinetskaya, Polina G; Mitric, Roland. Optimal control of light propagation and exciton transfer in arrays of molecular-like noble-metal clusters. Journal Article Physical Review B: Condensed Matter and Materials Physics, 91 (12), pp. 125436/1–125436/8, 2015, ISSN: 1098-0121. @article{Lisinetskaya2015, title = {Optimal control of light propagation and exciton transfer in arrays of molecular-like noble-metal clusters.}, author = {Polina G Lisinetskaya and Roland. Mitric}, doi = {10.1103/PhysRevB.91.125436}, issn = {1098-0121}, year = {2015}, date = {2015-01-01}, journal = {Physical Review B: Condensed Matter and Materials Physics}, volume = {91}, number = {12}, pages = {125436/1--125436/8}, publisher = {American Physical Society}, abstract = {We demonstrate theor. the possibility of optimal control of light propagation and exciton transfer in arrays constructed of subnanometer sized noble-metal clusters by using phase-shaped laser pulses and analyze the mechanism underlying this process. The theor. approach for simulation of light propagation in the arrays is based on the numerical soln. of the coupled time-dependent Schrodinger equation and the classical elec. field propagation in an iterative self-consistent manner. The electronic eigenstates of individual clusters and the dipole couplings are obtained from ab initio TDDFT calcns. The total elec. field is propagated along the array by coupling an external excitation elec. field with the elec. fields produced by all clusters. A genetic algorithm is used to det. optimal pulse shapes which drive the excitation in a desired direction. The described theor. approach is applied to control the light propagation and exciton transfer dynamics into a T-shaped structure built of seven Ag8 clusters. We demonstrate that a selective switching of light localization is possible in ∼5 nm sized cluster arrays which might serve as a building block for plasmonic devices with an ultrafast operation regime. [on SciFinder(R)]}, keywords = {}, pubstate = {published}, tppubtype = {article} } We demonstrate theor. the possibility of optimal control of light propagation and exciton transfer in arrays constructed of subnanometer sized noble-metal clusters by using phase-shaped laser pulses and analyze the mechanism underlying this process. The theor. approach for simulation of light propagation in the arrays is based on the numerical soln. of the coupled time-dependent Schrodinger equation and the classical elec. field propagation in an iterative self-consistent manner. The electronic eigenstates of individual clusters and the dipole couplings are obtained from ab initio TDDFT calcns. The total elec. field is propagated along the array by coupling an external excitation elec. field with the elec. fields produced by all clusters. A genetic algorithm is used to det. optimal pulse shapes which drive the excitation in a desired direction. The described theor. approach is applied to control the light propagation and exciton transfer dynamics into a T-shaped structure built of seven Ag8 clusters. We demonstrate that a selective switching of light localization is possible in ∼5 nm sized cluster arrays which might serve as a building block for plasmonic devices with an ultrafast operation regime. [on SciFinder(R)] |
3. | Lisinetskaya, Polina G; Mitric, Roland. Ab initio simulations of light propagation in silver cluster nanostructures. Journal Article Physical Review B: Condensed Matter and Materials Physics, 89 (3), pp. 035433/1–035433/13, 2014, ISSN: 1098-0121. @article{Lisinetskaya2014, title = {Ab initio simulations of light propagation in silver cluster nanostructures.}, author = {Polina G Lisinetskaya and Roland. Mitric}, doi = {10.1103/PhysRevB.89.035433}, issn = {1098-0121}, year = {2014}, date = {2014-01-01}, journal = {Physical Review B: Condensed Matter and Materials Physics}, volume = {89}, number = {3}, pages = {035433/1--035433/13}, publisher = {American Physical Society}, abstract = {We present a theor. approach for the simulation of the optical response and light propagation in aggregates and in ordered arrays of small noble-metal clusters with discrete electronic structure. We construct the Hamiltonian for the aggregate system based on the time-dependent d. functional theory electronic states of the individual subunits and describe the interaction between them using the dipole approxn. The time evolution of the aggregate under the influence of the external elec. field is obtained from the numerical soln. of the time-dependent Schroedinger equation with the coupled excitonic Hamiltonian. For each subunit, the time-dependent dipole moment is calcd. using the reduced d. matrix formalism. Such quantum-mech. detd. dipole moments are used to simulate the spatiotemporal distribution of the elec. field produced by the array. Addnl., we introduce an approx. self-consistent iterative approach to treat arrays consisting of many subunits which are of interest in the context of nanoplasmonics, nano-optical applications, and development of light-harvesting materials. The developed methodol. is illustrated 1st on the example of Ag2 and Ag8 cluster pairs. Subsequently, light propagation in a triangular-shaped array consisting of six Ag8 clusters is simulated. [on SciFinder(R)]}, keywords = {}, pubstate = {published}, tppubtype = {article} } We present a theor. approach for the simulation of the optical response and light propagation in aggregates and in ordered arrays of small noble-metal clusters with discrete electronic structure. We construct the Hamiltonian for the aggregate system based on the time-dependent d. functional theory electronic states of the individual subunits and describe the interaction between them using the dipole approxn. The time evolution of the aggregate under the influence of the external elec. field is obtained from the numerical soln. of the time-dependent Schroedinger equation with the coupled excitonic Hamiltonian. For each subunit, the time-dependent dipole moment is calcd. using the reduced d. matrix formalism. Such quantum-mech. detd. dipole moments are used to simulate the spatiotemporal distribution of the elec. field produced by the array. Addnl., we introduce an approx. self-consistent iterative approach to treat arrays consisting of many subunits which are of interest in the context of nanoplasmonics, nano-optical applications, and development of light-harvesting materials. The developed methodol. is illustrated 1st on the example of Ag2 and Ag8 cluster pairs. Subsequently, light propagation in a triangular-shaped array consisting of six Ag8 clusters is simulated. [on SciFinder(R)] |
2. | Stanzel, Joerg; Neeb, Matthias; Eberhardt, Wolfgang; Lisinetskaya, Polina G; Petersen, Jens; Mitric, Roland. Switching from molecular to bulk-like dynamics in electronic relaxation of a small gold cluster. Journal Article Physical Review A: Atomic, Molecular, and Optical Physics, 85 (1-A), pp. 013201/1–013201/6, 2012, ISSN: 1050-2947. @article{Stanzel2012, title = {Switching from molecular to bulk-like dynamics in electronic relaxation of a small gold cluster.}, author = {Joerg Stanzel and Matthias Neeb and Wolfgang Eberhardt and Polina G Lisinetskaya and Jens Petersen and Roland. Mitric}, doi = {10.1103/PhysRevA.85.013201}, issn = {1050-2947}, year = {2012}, date = {2012-01-01}, journal = {Physical Review A: Atomic, Molecular, and Optical Physics}, volume = {85}, number = {1-A}, pages = {013201/1--013201/6}, publisher = {American Physical Society}, abstract = {We have investigated the ultrafast electronic relaxation of Au7- using time-resolved photoelectron spectroscopy combined with first-principles simulations of the excited-state dynamics. Unlike previous findings, which have demonstrated molecularlike excited-state relaxation in Au7- at low excitation energy (1.56 eV), we show here that excitation with 3.12 eV leads to bulklike electronic relaxation without a considerable change of geometry. The exptl. findings are fully supported by theor. simulations, which reveal a bulklike electron-hole relaxation mechanism in a far band-gap cluster. Our findings demonstrate that small gold clusters in the sub-nm size range can exhibit either molecularlike or bulklike properties, depending on the excitation energy. [on SciFinder(R)]}, keywords = {}, pubstate = {published}, tppubtype = {article} } We have investigated the ultrafast electronic relaxation of Au7- using time-resolved photoelectron spectroscopy combined with first-principles simulations of the excited-state dynamics. Unlike previous findings, which have demonstrated molecularlike excited-state relaxation in Au7- at low excitation energy (1.56 eV), we show here that excitation with 3.12 eV leads to bulklike electronic relaxation without a considerable change of geometry. The exptl. findings are fully supported by theor. simulations, which reveal a bulklike electron-hole relaxation mechanism in a far band-gap cluster. Our findings demonstrate that small gold clusters in the sub-nm size range can exhibit either molecularlike or bulklike properties, depending on the excitation energy. [on SciFinder(R)] |
1. | Lisinetskaya, Polina G; Mitric, Roland. Simulation of laser-induced coupled electron-nuclear dynamics and time-resolved harmonic spectra in complex systems. Journal Article Physical Review A: Atomic, Molecular, and Optical Physics, 83 (3, Pt. B), pp. 033408/1–033408/13, 2011, ISSN: 1050-2947. @article{Lisinetskaya2011, title = {Simulation of laser-induced coupled electron-nuclear dynamics and time-resolved harmonic spectra in complex systems.}, author = {Polina G Lisinetskaya and Roland. Mitric}, doi = {10.1103/PhysRevA.83.033408}, issn = {1050-2947}, year = {2011}, date = {2011-01-01}, journal = {Physical Review A: Atomic, Molecular, and Optical Physics}, volume = {83}, number = {3, Pt. B}, pages = {033408/1--033408/13}, publisher = {American Physical Society}, abstract = {The authors present a theor. approach for the simulation of time-resolved harmonic spectra, including the effect of nuclear dynamics, which is applicable to complex systems involving many nuclear degrees of freedom. The method is based on the combination of semiclassical field-induced surface hopping approach for the treatment of laser-induced nuclear dynamics with the time-dependent d. functional theory for electron dynamics. The authors apply method to the simulation of ultrafast nonadiabatic dynamics and time-resolved harmonic spectra in small Ag clusters (Ag2 and Ag8), which exhibit discrete molecularlike electronic transitions. The harmonic signal is highly sensitive to the nuclear dynamics and thus can be used as a probe of coupled electron-nuclear dynamics, which is complementary to common pump-probe methods such as time-resolved photoelectron spectroscopy. Simulations allowed one also to det. the mechanism and the time scale of nonradiative relaxation in the magic Ag8 cluster and provided a fundamental insight into ultrafast dynamics of metal nanoclusters in the size regime where each atom counts. The excited-state dynamics of Ag8 involves an isomerization process from the initial structure with Td symmetry to the quadratic antiprism structure with D4d symmetry which takes place on a time scale of ∼600 fs and is clearly identified in a time-resolved harmonic signal. Theor. approach is generally applicable for the prediction of time-resolved harmonic spectra in complex systems with many nuclear degrees freedom and should serve to stimulate new ultrafast expts. using harmonic signals as a probe for nonadiabatic processes in mol. systems. [on SciFinder(R)]}, keywords = {}, pubstate = {published}, tppubtype = {article} } The authors present a theor. approach for the simulation of time-resolved harmonic spectra, including the effect of nuclear dynamics, which is applicable to complex systems involving many nuclear degrees of freedom. The method is based on the combination of semiclassical field-induced surface hopping approach for the treatment of laser-induced nuclear dynamics with the time-dependent d. functional theory for electron dynamics. The authors apply method to the simulation of ultrafast nonadiabatic dynamics and time-resolved harmonic spectra in small Ag clusters (Ag2 and Ag8), which exhibit discrete molecularlike electronic transitions. The harmonic signal is highly sensitive to the nuclear dynamics and thus can be used as a probe of coupled electron-nuclear dynamics, which is complementary to common pump-probe methods such as time-resolved photoelectron spectroscopy. Simulations allowed one also to det. the mechanism and the time scale of nonradiative relaxation in the magic Ag8 cluster and provided a fundamental insight into ultrafast dynamics of metal nanoclusters in the size regime where each atom counts. The excited-state dynamics of Ag8 involves an isomerization process from the initial structure with Td symmetry to the quadratic antiprism structure with D4d symmetry which takes place on a time scale of ∼600 fs and is clearly identified in a time-resolved harmonic signal. Theor. approach is generally applicable for the prediction of time-resolved harmonic spectra in complex systems with many nuclear degrees freedom and should serve to stimulate new ultrafast expts. using harmonic signals as a probe for nonadiabatic processes in mol. systems. [on SciFinder(R)] |