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Title: Imaging material functionality through three-dimensional nanoscale tracking of energy flow

Abstract

The ability of energy carriers to move between atoms and molecules underlies biochemical and material function. Understanding and controlling energy flow, however, requires observing it on ultrasmall and ultrafast spatio-temporal scales, where energetic and structural roadblocks dictate the fate of energy carriers. Here, we developed a non-invasive optical scheme that leverages non-resonant interferometric scattering to track tiny changes in material polarizability created by energy carriers. We thus map evolving energy carrier distributions in four dimensions of spacetime with few-nanometre lateral precision and directly correlate them with material morphology. We visualize exciton, charge and heat transport in polyacene, silicon and perovskite semiconductors and elucidate how disorder affects energy flow in three dimensions. For example, we show that morphological boundaries in polycrystalline metal halide perovskites possess lateral- and depth-dependent resistivities, blocking lateral transport for surface but not bulk carriers. We also reveal strategies for interpreting energy transport in disordered environments that will direct the design of defect-tolerant materials for the semiconductor industry of tomorrow.

Authors:
 [1]; ORCiD logo [2];  [2]; ORCiD logo [3]
+ Show Author Affiliations
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
  2. Univ. of California, Berkeley, CA (United States). Dept. of Physics
  3. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry, Dept. of Physics; Kavli Energy NanoSciences Inst., Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division, Molecular Biophysics and Integrated Bioimaging Division
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Photonics at Thermodynamic Limits (PTL); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1572854
Grant/Contract Number:  
AC02-05CH11231; SC0019140
Resource Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 19; Journal Issue: 1; Journal ID: ISSN 1476-1122
Publisher:
Springer Nature - Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Delor, Milan, Weaver, Hannah L., Yu, QinQin, and Ginsberg, Naomi S. Imaging material functionality through three-dimensional nanoscale tracking of energy flow. United States: N. p., 2019. Web. doi:10.1038/s41563-019-0498-x.
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Delor, Milan, Weaver, Hannah L., Yu, QinQin, & Ginsberg, Naomi S. Imaging material functionality through three-dimensional nanoscale tracking of energy flow. United States. https://doi.org/10.1038/s41563-019-0498-x
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Delor, Milan, Weaver, Hannah L., Yu, QinQin, and Ginsberg, Naomi S. Mon . "Imaging material functionality through three-dimensional nanoscale tracking of energy flow". United States. https://doi.org/10.1038/s41563-019-0498-x. https://www.osti.gov/servlets/purl/1572854.
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@article{osti_1572854,
title = {Imaging material functionality through three-dimensional nanoscale tracking of energy flow},
author = {Delor, Milan and Weaver, Hannah L. and Yu, QinQin and Ginsberg, Naomi S.},
abstractNote = {The ability of energy carriers to move between atoms and molecules underlies biochemical and material function. Understanding and controlling energy flow, however, requires observing it on ultrasmall and ultrafast spatio-temporal scales, where energetic and structural roadblocks dictate the fate of energy carriers. Here, we developed a non-invasive optical scheme that leverages non-resonant interferometric scattering to track tiny changes in material polarizability created by energy carriers. We thus map evolving energy carrier distributions in four dimensions of spacetime with few-nanometre lateral precision and directly correlate them with material morphology. We visualize exciton, charge and heat transport in polyacene, silicon and perovskite semiconductors and elucidate how disorder affects energy flow in three dimensions. For example, we show that morphological boundaries in polycrystalline metal halide perovskites possess lateral- and depth-dependent resistivities, blocking lateral transport for surface but not bulk carriers. We also reveal strategies for interpreting energy transport in disordered environments that will direct the design of defect-tolerant materials for the semiconductor industry of tomorrow.},
doi = {10.1038/s41563-019-0498-x},
journal = {Nature Materials},
number = 1,
volume = 19,
place = {United States},
year = {Mon Oct 07 00:00:00 EDT 2019},
month = {Mon Oct 07 00:00:00 EDT 2019}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41563-019-0498-x
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Cited by: 62 works
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Figures / Tables:

Figure 1 Figure 1: Visualizing semiconductor exciton, charge and heat transport across four orders of magnitude in space and time. (a) stroboSCAT setup. A confocal pump (306 nm diameter, λ = 440 nm) and widefield probe (8 µm diameter, λ = 635 nm) are overlapped in the sample. Both probe light scatteredmore » by the sample and reflected at the sample-substrate interface are imaged on the camera (CMOS). Full details in Supplementary Sections 1-6. (b) Example stroboSCAT dataset for a MAPbBr3 single crystal, showing charge carriers diffusing as a function of pump-probe time delay. The peak pump-injected carrier density is 2 x 1018 cm-3 and the probe is spectrally far from the band edge (570 nm). The peak power densities at the sample are on the order of 0.2 MW/cm2, far below the onset of nonlinear optical effects. All stroboSCAT plots are generated by taking the difference between pumpON and pumpOFF raw images, normalized to the raw pumpOFF image. Scale bar 1 µm. The spatiotemporal population distribution along the horizontal spatial axis is plotted in c, along with 1D Gaussian profiles extracted at 0 and 1 ns pump-probe delay. (d) Charge, exciton, or heat distributions vs time measured for a range of semiconductors (Supplementary Section 7). Error bars represent the 95% confidence intervals from Gaussian fits. All experiments are performed in a linear excitation regime, as confirmed by a lack of power dependence to extracted diffusivities. (e) Diffusivities extracted from linear fits of the data in (d).« less
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    Heat current fluctuations and anomalous transport in low-dimensional carbon lattices
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