Nonlinearity in the Dynamics of Photoinduced Nucleation Process

Ishida, Kunio; Nasu, Keiichirō

doi:10.1103/physrevlett.100.116403

Cited by 35 publications

(33 citation statements)

References 21 publications

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“…This is fundamentally different from the Debye-Waller effect and thermal diffuse scattering which result from thermally excited incoherent phonons. In addition, in case of localized molecular excitations in solid state coherent nucleation and growth processes can take place [24]. These different dynamics are no more stochastic as at thermal equilibrium but instead become deterministic and ultrafast.…”

Section: Coherencementioning

confidence: 99%

“…These phototransformed entities may cooperatively interact with the atoms/molecules in the surroundings. This may trigger coherent nucleation and growth [24,51] and coherent phonons [52,53]. This may even lead to the spontaneous formation of a macroscopic domain in a second stage, with a new long range electronic and structural order.…”

Section: Nanodomains Vs Softeningmentioning

confidence: 99%

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PIPT from the Beginning to Future

et al. 2012

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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. 78.47.D- Flash-backThis paper is dedicated in memoriam of Professor Yutaka Toyozawa, a founding father of the field of photoinduced phase transitions (PIPT). After the pioneering experimental work of Koshihara on the observation of the photoinduced neutral-to-ionic instability [1], the paper of Prof. Y. Toyozawa, "Condensation of relaxed excitons in static and dynamic phase transitions" [2], is the fingerprint of his inspiring contribution. He brought out some conceptual keys which strongly influenced our research and that of many of our colleagues. In the conclusion of this paper he emphasizes "the usefulness of the global view-point . . . considering the crossover of the excited and the ground electronic states and correlating static and dynamic phase transitions through the motion of (spontaneously or optically) condensed elementary excitations".A second step was the Taniguchi symposium in 1996 "Relaxations of excited states and photoinduced phase transitions" chaired by Prof. Nasu [3]. The aim of this symposium was to discuss the new problem of unconventionally photoactive materials. In these materials the relaxation of optically excited states result in collective motions or drastic structural changes, involving a large number of atoms and electrons. Actually, in a way this symposium was the precursor of the PIPT conferences. The extension of the physics of self-trapped excitons, which Toyozawa has largely contributed to [4], to systems with electron-spin-lattice cooperative interactions was discussed from the viewpoint of both material science and solid state spectroscopy. * corresponding author; e-mail:herve.cailleau@univ-rennes1.frThroughout this first period different theoretical papers were published, developing this approach to establish some backgrounds in the understanding of photoinduced phase transitions [3,5,6]. At the same period, different approaches of photoinduced phase transitions were introduced [7], in particular to t...

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Section: Coherencementioning

confidence: 99%

Section: Nanodomains Vs Softeningmentioning

confidence: 99%

PIPT from the Beginning to Future

et al. 2012

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“…We focus on the deterministic solution of the time-dependent Schrödinger equation in order to clarify and understand the nonlinear nature of the photoinduced cooperativity. In our previous paper [12], we showed that the the dynamics of pattern formation and the nonlinear dependence of the conversion ratio are understood with the above-mentioned model. We present our calculated results on the initial dynamics of the pattern formation in photoinduced nucleation process in detail.…”

Section: Introductionmentioning

confidence: 85%

“…As we discussed in our previous papers [11,12], nonadiabatic transitions between quantized states are important to study the dynamical aspects of photoinduced cooperative phenomena.…”

Section: Models and Methodsmentioning

confidence: 97%

“…These photoinduced cooperative phenomena in condensed matter have brought us fruitful theoretical and experimental problems with nonequilibrium dynamics of excited states, and many studies have been presented to clarify their mechanism[8, 9,10,11,12,13]. In particular, coherent dynamics of the photoinduced cooperative phenomena is relevant to control such cooperativity by designed optical pulses.…”

Section: Introductionmentioning

confidence: 99%

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Quantum pattern formation dynamics of photoinduced nucleation

Ishida

Nasu

2008

Phys. Rev. B

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We study the dynamics of quantum pattern formation processes in molecular crystals which is a concomitant with photoinduced nucleation. Since the nucleation process in coherent regime is driven by the nonadiabatic transition in each molecule followed by the propagation of phonons, it is necessary to take into account the quantum nature of both electrons and phonons in order to pursue the dynamics of the system. Therefore, we employ a model of localized electrons coupled with a quantized phonon mode and solved the time-dependent Schrödinger equation numerically.We found that there is a minimal size of clusters of excited molecules which triggers the photoinduced nucleation process, i.e., nucleation does not take place unless sufficient photoexcitation energy is concentrated within a narrow area of the system. We show that this result means that the spatial distribution of photoexcited molecules plays 1 an important role in the nonlinearity of the dynamics and also of the optical properties observed in experiments. We calculated the conversion ratio, the nucleation rate, and correlation functions to reveal the dynamical properties of the pattern formation process, and the initial dynamics of the photoinduced structural change is discussed from the viewpoint of pattern formation.

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Coherent Control of Nonadiabatic Dynamics of Electron-Phonon Systems by Quantized Light Field

Ishida

2020

Topics in Applied Physics

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Nonlinearity in the Dynamics of Photoinduced Nucleation Process

Cited by 35 publications

References 21 publications

PIPT from the Beginning to Future

PIPT from the Beginning to Future

Quantum pattern formation dynamics of photoinduced nucleation

Coherent Control of Nonadiabatic Dynamics of Electron-Phonon Systems by Quantized Light Field

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