Nanoscale imaging of phonon dynamics by electron microscopy

Gadre, Chaitanya A.; Yan, Xingxu; Song, Qichen; Li, Jie; Gu, Lei; Huyan, Huaixun; Aoki, Toshihiro; Lee, Sheng-Wei; Chen, Gang; Wu, Ruqian; Pan, Xiaoqing

doi:10.1038/s41586-022-04736-8

Nanoscale imaging of phonon dynamics by electron microscopy

Journal Article · Wed Jun 08 00:00:00 EDT 2022 · Nature (London)

DOI:https://doi.org/10.1038/s41586-022-04736-8· OSTI ID:1904651

^[1]; ^[2]; ^[3]; ^[2]; Gu, Lei ^[2]; Huyan, Huaixun ^[2]; ^[2]; Lee, Sheng-Wei ^[4]; ^[3]; ^[2]; ^[2]

University of California, Irvine, CA (United States); Univ. of California, Irvine, CA (United States)
University of California, Irvine, CA (United States)
Massachusetts Institute of Technology (MIT), Cambridge, MA (United States)
National Central University, Taoyuan (Taiwan)

Spatially resolved vibrational mapping of nanostructures is indispensable to the development and understanding of thermal nanodevices, modulation of thermal transport and novel nanostructured thermoelectric materials. Through the engineering of complex structures, such as alloys, nanostructures and superlattice interfaces, one can significantly alter the propagation of phonons and suppress material thermal conductivity while maintaining electrical conductivity. There have been no correlative experiments that spatially track the modulation of phonon properties in and around nanostructures due to spatial resolution limitations of conventional optical phonon detection techniques. Here we demonstrate two-dimensional spatial mapping of phonons in a single silicon–germanium (SiGe) quantum dot (QD) using monochromated electron energy loss spectroscopy in the transmission electron microscope. Tracking the variation of the Si optical mode in and around the QD, we observe the nanoscale modification of the composition-induced red shift. We observe non-equilibrium phonons that only exist near the interface and, furthermore, develop a novel technique to differentially map phonon momenta, providing direct evidence that the interplay between diffuse and specular reflection largely depends on the detailed atomistic structure: a major advancement in the field. Our work unveils the non-equilibrium phonon dynamics at nanoscale interfaces and can be used to study actual nanodevices and aid in the understanding of heat dissipation near nanoscale hotspots, which is crucial for future high-performance nanoelectronics.

View Accepted Manuscript (DOE)

Research Organization:: University of California, Irvine, CA (United States)

Sponsoring Organization:: National Energy Research Scientific Computing Center (NERSC); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE)

Grant/Contract Number:: FG02-05ER46237; SC0014430

OSTI ID:: 1904651

Journal Information:: Nature (London), Journal Name: Nature (London) Journal Issue: 7913 Vol. 606; ISSN 0028-0836

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (44)

Materials for thermoelectric refrigeration Rosi, F. D.; Abeles, B.; Jensen, R. V. Journal of Physics and Chemistry of Solids, Vol. 10, Issue 2-3 https://doi.org/10.1016/0022-3697(59)90074-5	journal	July 1959
Unexpected Strong Thermally Induced Phonon Energy Shift for Mapping Local Temperature Yan, Xingxu; Liu, Chengyan; Gadre, Chaitanya A. Nano Letters, Vol. 19, Issue 10 https://doi.org/10.1021/acs.nanolett.9b03307	journal	September 2019
Enhanced thermoelectric performance of rough silicon nanowires Hochbaum, Allon I.; Chen, Renkun; Delgado, Raul Diaz Nature, Vol. 451, Issue 7175, p. 163-167 https://doi.org/10.1038/nature06381	journal	January 2008
Convergence of electronic bands for high performance bulk thermoelectrics Pei, Yanzhong; Shi, Xiaoya; LaLonde, Aaron Nature, Vol. 473, Issue 7345, p. 66-69 https://doi.org/10.1038/nature09996	journal	May 2011
High-performance bulk thermoelectrics with all-scale hierarchical architectures Biswas, Kanishka; He, Jiaqing; Blum, Ivan D. Nature, Vol. 489, Issue 7416, p. 414-418 https://doi.org/10.1038/nature11439	journal	September 2012
Vibrational spectroscopy in the electron microscope Krivanek, Ondrej L.; Lovejoy, Tracy C.; Dellby, Niklas Nature, Vol. 514, Issue 7521 https://doi.org/10.1038/nature13870	journal	October 2014
Mapping vibrational surface and bulk modes in a single nanocube Lagos, Maureen J.; Trügler, Andreas; Hohenester, Ulrich Nature, Vol. 543, Issue 7646 https://doi.org/10.1038/nature21699	journal	March 2017
Precise control of thermal conductivity at the nanoscale through individual phonon-scattering barriers Pernot, G.; Stoffel, M.; Savic, I. Nature Materials, Vol. 9, Issue 6 https://doi.org/10.1038/nmat2752	journal	May 2010
Crossover from incoherent to coherent phonon scattering in epitaxial oxide superlattices Ravichandran, Jayakanth; Yadav, Ajay K.; Cheaito, Ramez Nature Materials, Vol. 13, Issue 2 https://doi.org/10.1038/nmat3826	journal	December 2013
Spectral mapping of thermal conductivity through nanoscale ballistic transport Hu, Yongjie; Zeng, Lingping; Minnich, Austin J. Nature Nanotechnology, Vol. 10, Issue 8 https://doi.org/10.1038/nnano.2015.109	journal	June 2015
Vibrational spectroscopy at atomic resolution with electron impact scattering Venkatraman, Kartik; Levin, Barnaby D. A.; March, Katia Nature Physics, Vol. 15, Issue 12 https://doi.org/10.1038/s41567-019-0675-5	journal	October 2019
Position and momentum mapping of vibrations in graphene nanostructures Senga, Ryosuke; Suenaga, Kazu; Barone, Paolo Nature, Vol. 573, Issue 7773 https://doi.org/10.1038/s41586-019-1477-8	journal	August 2019
Single-defect phonons imaged by electron microscopy Yan, Xingxu; Liu, Chengyan; Gadre, Chaitanya A. Nature, Vol. 589, Issue 7840 https://doi.org/10.1038/s41586-020-03049-y	journal	January 2021
Designer Ge/Si composite quantum dots with enhanced thermoelectric properties Chang, Hung-Tai; Wang, Sih-Yuan; Lee, Sheng-Wei Nanoscale, Vol. 6, Issue 7 https://doi.org/10.1039/C3NR06335F	journal	January 2014
Thermal conductivity of Si–Ge superlattices Lee, S. -M.; Cahill, David G.; Venkatasubramanian, Rama Applied Physics Letters, Vol. 70, Issue 22 https://doi.org/10.1063/1.118755	journal	June 1997
Mechanism of organization of three-dimensional islands in SiGe/Si multilayers Mateeva, E.; Sutter, P.; Bean, J. C. Applied Physics Letters, Vol. 71, Issue 22 https://doi.org/10.1063/1.120300	journal	December 1997
Phonons as probes in self-organized SiGe islands Groenen, J.; Carles, R.; Christiansen, S. Applied Physics Letters, Vol. 71, Issue 26 https://doi.org/10.1063/1.120525	journal	December 1997
Optical and acoustic phonon modes in self-organized Ge quantum dot superlattices Liu, J. L.; Jin, G.; Tang, Y. S. Applied Physics Letters, Vol. 76, Issue 5 https://doi.org/10.1063/1.125825	journal	January 2000
Raman investigation of strain in Si∕SiGe heterostructures: Precise determination of the strain-shift coefficient of Si bands Nakashima, S.; Mitani, T.; Ninomiya, M. Journal of Applied Physics, Vol. 99, Issue 5 https://doi.org/10.1063/1.2178396	journal	March 2006
Measurements of alloy composition and strain in thin Ge_xSi_1−xlayers Tsang, J. C.; Mooney, P. M.; Dacol, F. Journal of Applied Physics, Vol. 75, Issue 12 https://doi.org/10.1063/1.356554	journal	June 1994
Nanoscale thermal transport. II. 2003–2012 Cahill, David G.; Braun, Paul V.; Chen, Gang Applied Physics Reviews, Vol. 1, Issue 1 https://doi.org/10.1063/1.4832615	journal	March 2014
GaAsBi/GaAs multi-quantum well LED grown by molecular beam epitaxy using a two-substrate-temperature technique Patil, Pallavi Kisan; Luna, Esperanza; Matsuda, Teruyoshi Nanotechnology, Vol. 28, Issue 10 https://doi.org/10.1088/1361-6528/aa596c	journal	February 2017
Contrast reversal in atomic-scale phonon spectroscopic imaging Hage, F. S.; Ramasse, Q. M.; Allen, L. J. Physical Review B, Vol. 102, Issue 21 https://doi.org/10.1103/PhysRevB.102.214111	journal	December 2020
Role of ionization in imaging and spectroscopy utilizing fast electrons that have excited phonons Barthel, Juri; Allen, Leslie J. Physical Review B, Vol. 104, Issue 10 https://doi.org/10.1103/PhysRevB.104.104108	journal	September 2021
Raman spectra of c - Si 1 − x Ge x alloys Alonso, M. I.; Winer, K. Physical Review B, Vol. 39, Issue 14 https://doi.org/10.1103/PhysRevB.39.10056	journal	May 1989
Projector augmented-wave method Blöchl, P. E. Physical Review B, Vol. 50, Issue 24, p. 17953-17979 https://doi.org/10.1103/PhysRevB.50.17953	journal	December 1994
Dynamical matrices, Born effective charges, dielectric permittivity tensors, and interatomic force constants from density-functional perturbation theory Gonze, Xavier; Lee, Changyol Physical Review B, Vol. 55, Issue 16 https://doi.org/10.1103/PhysRevB.55.10355	journal	April 1997
Thermal conductivity and ballistic-phonon transport in the cross-plane direction of superlattices Chen, G. Physical Review B, Vol. 57, Issue 23, p. 14958-14973 https://doi.org/10.1103/PhysRevB.57.14958	journal	June 1998
From ultrasoft pseudopotentials to the projector augmented-wave method Kresse, G.; Joubert, D. Physical Review B, Vol. 59, Issue 3, p. 1758-1775 https://doi.org/10.1103/PhysRevB.59.1758	journal	January 1999
Multiple layers of self-asssembled Ge/Si islands: Photoluminescence, strain fields, material interdiffusion, and island formation Schmidt, O. G.; Eberl, K. Physical Review B, Vol. 61, Issue 20 https://doi.org/10.1103/PhysRevB.61.13721	journal	May 2000
Role of Disorder and Anharmonicity in the Thermal Conductivity of Silicon-Germanium Alloys: A First-Principles Study Garg, Jivtesh; Bonini, Nicola; Kozinsky, Boris Physical Review Letters, Vol. 106, Issue 4 https://doi.org/10.1103/PhysRevLett.106.045901	journal	January 2011
Significant Reduction of Lattice Thermal Conductivity by the Electron-Phonon Interaction in Silicon with High Carrier Concentrations: A First-Principles Study Liao, Bolin; Qiu, Bo; Zhou, Jiawei Physical Review Letters, Vol. 114, Issue 11 https://doi.org/10.1103/PhysRevLett.114.115901	journal	March 2015
Temperature Measurement by a Nanoscale Electron Probe Using Energy Gain and Loss Spectroscopy Idrobo, Juan Carlos; Lupini, Andrew R.; Feng, Tianli Physical Review Letters, Vol. 120, Issue 9 https://doi.org/10.1103/PhysRevLett.120.095901	journal	March 2018
Phonon Spectroscopy at Atomic Resolution Hage, F. S.; Kepaptsoglou, D. M.; Ramasse, Q. M. Physical Review Letters, Vol. 122, Issue 1 https://doi.org/10.1103/PhysRevLett.122.016103	journal	January 2019
Generalized Gradient Approximation Made Simple Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868 https://doi.org/10.1103/PhysRevLett.77.3865	journal	October 1996
Thermal Conductivity Reduction and Thermoelectric Figure of Merit Increase by Embedding Nanoparticles in Crystalline Semiconductors Kim, Woochul; Zide, Joshua; Gossard, Arthur Physical Review Letters, Vol. 96, Issue 4 https://doi.org/10.1103/PhysRevLett.96.045901	journal	February 2006
Thermal boundary resistance Swartz, E. T.; Pohl, R. O. Reviews of Modern Physics, Vol. 61, Issue 3, p. 605-668 https://doi.org/10.1103/RevModPhys.61.605	journal	July 1989
Nanoscale momentum-resolved vibrational spectroscopy Hage, Fredrik S.; Nicholls, Rebecca J.; Yates, Jonathan R. Science Advances, Vol. 4, Issue 6 https://doi.org/10.1126/sciadv.aar7495	journal	June 2018
High-Thermoelectric Performance of Nanostructured Bismuth Antimony Telluride Bulk Alloys Poudel, B.; Hao, Q.; Ma, Y. Science, Vol. 320, Issue 5876, p. 634-638 https://doi.org/10.1126/science.1156446	journal	May 2008
Coherent Phonon Heat Conduction in Superlattices Luckyanova, M. N.; Garg, J.; Esfarjani, K. Science, Vol. 338, Issue 6109 https://doi.org/10.1126/science.1225549	journal	November 2012
Advances in thermoelectric materials research: Looking back and moving forward He, Jian; Tritt, Terry M. Science, Vol. 357, Issue 6358 https://doi.org/10.1126/science.aak9997	journal	September 2017
Single-atom vibrational spectroscopy in the scanning transmission electron microscope Hage, F. S.; Radtke, G.; Kepaptsoglou, D. M. Science, Vol. 367, Issue 6482 https://doi.org/10.1126/science.aba1136	journal	March 2020
Anisotropic Thermal Conductivity of Ge Quantum-Dot and Symmetrically Strained Si/Ge Superlattices Liu, W. L.; Borca-Tasciuc, T.; Chen, G. Journal of Nanoscience and Nanotechnology, Vol. 1, Issue 1 https://doi.org/10.1166/jnn.2001.013	journal	March 2001
Si/SiGe Heterointerfaces in One-, Two-, and Three-Dimensional Nanostructures: Their Impact on SiGe Light Emission Lockwood, David J.; Wu, Xiaohua; Baribeau, Jean-Marc Frontiers in Materials, Vol. 3 https://doi.org/10.3389/fmats.2016.00012	journal	March 2016

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36 MATERIALS SCIENCE
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Nanoscale imaging of phonon dynamics by electron microscopy

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