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.
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This work was supported by STROBE, A National Science Foundation Science and Technology Center under grant no. DMR 1548924. The manuscript revision was also supported by the Photonics at Thermodynamic Limits Energy Frontier Research Center, funded by the US Department of Energy Office of Science Basic Energy Sciences Program, under award no. DE-SC0019140. Q.Y. and H.L.W. acknowledge National Science Foundation Graduate Research Fellowship DGE 1106400. N.S.G. acknowledges an Alfred P. Sloan Research Fellowship, a David and Lucile Packard Foundation Fellowship for Science and Engineering, and a Camille and Henry Dreyfus Teacher-Scholar Award.
The authors declare no competing interests.
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Detailed description of the stroboSCAT set-up, stroboSCAT contrast mechanism, data analysis, sample preparation, current system resolution, distinguishing scattering from normal reflection, supporting experimental data, in situ spectral interferometry on MAPbI3(Cl) films, simulations of depth-dependent carrier diffusion in polycrystalline films using the finite element method, Figs. 1–24 and refs. 1–54.
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Delor, M., Weaver, H.L., Yu, Q. et al. Imaging material functionality through three-dimensional nanoscale tracking of energy flow. Nat. Mater. 19, 56–62 (2020). https://doi.org/10.1038/s41563-019-0498-x
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