Beyond the molecular movie: Dynamics of bands and bonds during a photoinduced phase transition

被引：88

作者：

Nicholson, C. W. ^{[1
,3
]}

Luecke, A. ^{[2
]}

Schmidt, W. G. ^{[2
]}

Puppin, M. ^{[1
]}

Rettig, L. ^{[1
]}

Ernstorfer, R. ^{[1
]}

Wolf, M. ^{[1
]}

机构：

[1] Max Planck Gesell, Fritz Haber Inst, Dept Phys Chem, Faradayweg 4-6, D-14195 Berlin, Germany

[2] Univ Paderborn, Dept Phys, Warburger Str 100, D-33098 Paderborn, Germany

[3] Univ Fribourg, Dept Phys, Chemin Musee 3, CH-1700 Fribourg, Switzerland

来源：

SCIENCE | 2018年 / 362卷 / 6416期

关键词：

CHARGE-DENSITY-WAVE; ELECTRONIC-STRUCTURE; ATOMIC WIRES; PHOTOEMISSION; INSTABILITY; SOLIDS; SYSTEM; MOTION; CHAINS;

D O I：

10.1126/science.aar4183

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Ultrafast nonequilibrium dynamics offer a route to study the microscopic interactions that govern macroscopic behavior. In particular, photoinduced phase transitions (PIPTs) in solids provide a test case for how forces, and the resulting atomic motion along a reaction coordinate, originate from a nonequilibrium population of excited electronic states. Using femtosecond photoemission, we obtain access to the transient electronic structure during an ultrafast PIPT in a model system: indium nanowires on a silicon(111) surface. We uncover a detailed reaction pathway, allowing a direct comparison with the dynamics predicted by ab initio simulations. This further reveals the crucial role played by localized photoholes in shaping the potential energy landscape and enables a combined momentum-and real-space description of PIPTs, including the ultrafast formation of chemical bonds.

引用

页码：821 / +

页数：22

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