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Physics of Neutral-to-Ionic Phase Transition in Organic Charge Transfer Semiconducting Compounds

100%
Cailleau H., Lemée-Cailleau M. H., Le Cointe M., Luty T.
Acta Physica Polonica A
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1997
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vol. 92
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issue 4
597-608
EN
An uncommon excitonic instability takes place in some exotic semiconducting compounds. Indeed, the equilibrium neutral-to-ionic (N-I) phase transition, as well as the non-equilibrium photo-induced phase transformation, observed in some organic charge-transfer complexes, originate from intra- and inter-chain cooperative effects between structurally relaxed charge-transfer excitations. This electronic-structural phase transition manifests itself by a change of the degree of charge-transfer and a dimerization distortion with the formation of donor-acceptor pairs along the stacking axis in the I phase. Thermal charge-transfer excitations associated with the formation of I strings along N chains are at the heart of the mechanism of this phase transition. These relaxed electronic excitations, which are an intrinsic feature of low-dimensional systems with strong electron-phonon coupling, can be described in terms of self-trapping and self-multiplication of charge-transfer excitons. Precise structural studies on the prototype compound, tetrathiafulvalene-p-chloranil allow to highlight the respective role taken by the ionicity and the dimerization. Symmetry and thermodynamics analysis of the N-I transition, based on recent determination of the pressure-temperature phase diagram, make possible to present a consistent picture of this phase transition. Supported by theoretical considerations taking into account the interplay between quantum and thermal effects, the experimental observations show that the N-I transition results from the condensation and the ordering (crystallization) of charge-transfer excitations, following a phase diagram analogous to the solid-liquid-gas one.
2
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Domain h Type Collective Dimerization of Graphite and Possible sp^2 rightarrow sp^3 Transition Induced by Inter h Layer Charge Transfer Excitations in the Visible Region

88%
Radosinski L., Ostasiewicz K., Luty T., Radosz A., Nasu K.
Acta Physica Polonica A
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2010
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vol. 118
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issue 3
500-506
EN
We theoretically study possible domain-type collective dimerizations of graphite induced by inter-layer charge transfer excitations in the visible region. Using the semiempirical Brenner theory, we have calculated the adiabatic energy along the path that starts from original two distant graphite layers, but finally reaches the dimerized domain which consists of about 100 carbons with inter-layer σ-bonds. The energy barrier between this new domain and the starting graphite is shown to be of the order of 1 eV, being easily overcome by applying a few visible photons. We have also shown the optimal path of transformation via step by step increase of the domain size.
3
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Photoinduced Conversion of Hybridization in Graphite

76%
Radosinski L., Luty T., Nasu K., Ohnishi H., Nishioka K., Radosz A., Wójt D.
Acta Physica Polonica A
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2012
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vol. 121
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issue 2
359-368
EN
Recent experiments indicate that a photostimulated graphite with a femtosecond laser pulse results in the formation of a stable domain with sp^3 like interlayer bonds. By means of the energy barrier minimization and molecular dynamics using the empirical Brenner potential we study a geometrical structure of the new phase. We clarify proliferation of the initial domain and prove that the overall process is a multiphoton one. Furthermore, we present a model describing the initial transformation - an interlayer charge transfer resulting in the localization of an exciton-like state. The local density approximation electronic structure analysis reveals that the electronic state of the new phase is an insulator immersed in semimetal. We study by means of the long-range carbon bond order potential the effect of the existence of the new phase on the surrounding graphite and propose a new mid step structure on the path of a photoinduced graphite-diamond conversion.
4
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PIPT from the Beginning to Future

76%
Cailleau H., Luty T., Koshihara S., Servol M., Lorenc M., Buron-Le Cointe M., Collet E.
Acta Physica Polonica A
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2012
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vol. 121
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issue 2
297-306
EN
The birth of the field of photoinduced phase transitions was strongly influenced by the conceptual viewpoint expressed by Professor Y. Toyozawa on the condensation of relaxed excitons. Since this first period, twenty years ago, this young field has been expanding rapidly along a diversity of directions. Nowadays, it goes hand in hand with the challenges of today's science: emergence, nonlinearity, coherence, far away from equilibrium, for example. The control of the functionality of a material via photoexcited states poses many new fundamental questions. Some of them will be overviewed: (i) the nature of the control parameters and the nature of the relevant collective variables, especially the order parameters, which characterize the evolution of the system, (ii) the difference between photoinduced transformations under continuous light irradiation and those resulting from an ultrashort laser pulse, (iii) the physical mechanisms of ultrafast photoinduced phase transitions from the formation and proliferation of phototransformed entities to the softening of a collective mode.
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