Ultrafast hot-hole injection modifies hot-electron dynamics in Au/p-GaN heterostructures

Tagliabue, Giulia; DuChene, Joseph S.; Abdellah, Mohamed; Habib, Adela; Gosztola, David J.; Hattori, Yocefu; Cheng, Wen-Hui; Zheng, Kaibo; Canton, Sophie E.; Sundararaman, Ravishankar; Sá, Jacinto; Atwater, Harry A.

doi:10.1038/s41563-020-0737-1

Title: Ultrafast hot-hole injection modifies hot-electron dynamics in Au/p-GaN heterostructures

Journal Article · Mon Jul 27 00:00:00 EDT 2020 · Nature Materials

DOI:https://doi.org/10.1038/s41563-020-0737-1· OSTI ID:1764850

^[1]; DuChene, Joseph S. ^[1]; Abdellah, Mohamed ^[2]; Habib, Adela ^[3];

^[4]; Hattori, Yocefu ^[5];

^[1]; Zheng, Kaibo ^[6];

^[7]; Sundararaman, Ravishankar ^[3];

^[8];

^[1]

California Institute of Technology (CalTech), Pasadena, CA (United States)
Uppsala Univ. (Sweden); South Valley Univ., Qena (Egypt)
Rensselaer Polytechnic Inst., Troy, NY (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Uppsala Univ. (Sweden)
Technical Univ. of Denmark, Lyngby (Denmark); Lund Univ. (Sweden)
ELI-HU Non-Profit Ltd., Szeged (Hungary); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
Uppsala Univ. (Sweden); Polish Academy of Sciences (PAS), Warsaw (Poland)

A fundamental understanding of hot-carrier dynamics in photo-excited metal nanostructures is needed to unlock their potential for photodetection and photocatalysis. Despite numerous studies on the ultrafast dynamics of hot electrons, so far, the temporal evolution of hot holes in metal-semiconductor heterostructures remains unknown. Here, we report ultrafast (t < 200 fs) hot-hole injection from Au nanoparticles into the valence band of p-type GaN. The removal of hot holes from below the Au Fermi level is observed to substantially alter the thermalization dynamics of hot electrons, reducing the peak electronic temperature and the electron-phonon coupling time of the Au nanoparticles. First-principles calculations reveal that hot-hole injection modifies the relaxation dynamics of hot electrons in Au nanoparticles by modulating the electronic structure of the metal on timescales commensurate with electron-electron scattering. Overall, these results advance our understanding of hot-hole dynamics in metal-semiconductor heterostructures and offer additional strategies for manipulating the dynamics of hot carriers on ultrafast timescales. Photo-excited gold nanoparticles are shown to provide ultrafast and efficient hot-hole injection to the valence band of p-type GaN, substantially altering hot-electron dynamics in the nanoparticles and forming a basis to design hot-hole-based optoelectronics.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC); Swiss National Science Foundation (SNSF)

Grant/Contract Number:: AC02-06CH11357; SC0004993; P2EZP2_159101; P300P2_171417

OSTI ID:: 1764850

Journal Information:: Nature Materials, Vol. 19, Issue 12; ISSN 1476-1122

Publisher:: Springer Nature - Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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