Abstract

Employing a two-orbital extended Peierls–Hubbard model, we demonstrate the photomanipulation of mixed-valent states in platinum-halide ladder compounds. There are two types of interchain valence arrangements, namely in-phase and out-of-phase types. The conversion of the in-phase structure to the out-of-phase structure is induced by photoirradiation, which is accelerated with increasing light intensity, while the reverse process hardly occurs. The out-of-phase arrangement is highly stabilized in the photoexcited states by the interchain electron transfer.

Highlights

  • We investigate the competition between in phase (IP) CDW and OP CDW in the ground and photoexcited states with particular emphasis on the effects of the lattice geometry

  • We focus on the IP-CDW and OP-CDW ground states in the vicinity of the phase boundaries, and reveal whether and how IP CDW and OP CDW are manipulated by photoirradiation

  • We have investigated photomanipulation of the IP-CDW and OP-CDW states in platinum-halide

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Summary

Introduction

We can tune the electronic structures by replacing constituent metals, halogens, and ligands Applying pressure is another way of controlling electronic properties [13,14,15]. In the diplatinum-halide chain compounds [16,17,18], the pressure-induced phase transition between the charge-density-wave (CDW) state [· · · X − −Pt3+ Pt3+. The platinum-halide ladder compound, which consists of two PtX chains connected with each other by interchain ligands (Figure 1), is a good model compound for the study of the interplay between photoinduced electron–phonon dynamics and lattice geometry. Valence-alternating ground states [27,28], where the interchain arrangement is in phase (IP) in the μ-bpym compounds, whereas it is out of phase (OP) in the bpy compounds These competing CDWs can be optically distinguished from each other.

Modeling
MX q k k
Competing Mixed-Valent States and Their Optical Properties
Photoexcitation and Following Lattice Relaxation
Real-Time Dynamics
Variational Calculation
Summary and Discussion

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