journal article·2023-10-10Open access

Detecting, Distinguishing, and Spatiotemporally Tracking Photogenerated Charge and Heat at the Nanoscale

Hannah L. Weaver, Cora M. Went, Joeson Wong, Dipti Jasrasaria, Eran Rabani, Harry A. Atwater, Naomi S. Ginsberg

ACS Nano· Volume 17· Issue 19

Abstract

High Resolution Image Download MS PowerPoint Slide Since dissipative processes are ubiquitous in semiconductors, characterizing how electronic and thermal energy transduce and transport at the nanoscale is vital for understanding and leveraging their fundamental properties. For example, in low-dimensional transition metal dichalcogenides (TMDCs), excess heat generation upon photoexcitation is difficult to avoid since even with modest injected exciton densities exciton–exciton annihilation still occurs. Both heat and photoexcited electronic species imprint transient changes in the optical response of a semiconductor, yet the distinct signatures of each are difficult to disentangle in typical spectra due to overlapping resonances. In response, we employ stroboscopic optical scattering microscopy (stroboSCAT) to simultaneously map both heat and exciton populations in few-layer MoS 2 on relevant nanometer and picosecond length- and time scales and with 100-mK temperature sensitivity. We discern excitonic contributions to the signal from heat by combining observations close to and far from exciton resonances, characterizing the photoinduced dynamics for each. Our approach is general and can be applied to any electronic material, including thermoelectrics, where heat and electronic observables spatially interplay, and it will enable direct and quantitative discernment of different types of coexisting energy without recourse to complex models or underlying assumptions.
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Research context

OpenAlex topics: 2D Materials and Applications · Thermal properties of materials · Advanced Thermoelectric Materials and Devices

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Physics, University of California, Berkeley, California 94720, United States

Department of Physics, California Institute of Technology, Pasadena, California 91125, United States

Department of Applied Physics and Materials Science, California Institute of Technology, Pasadena, California 91125, United States

Department of Chemistry, University of California, Berkeley, California 94720, United States

Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States

The Sackler Center for Computational Molecular and Materials Science, Tel Aviv University, Tel Aviv, 69978, Israel

Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States

Kavli Energy NanoScience Institute, Berkeley, California 94720, United States

Funding

Energy Frontier Research Centers · Basic Energy Sciences · Division of Graduate Education · Alfred P. Sloan Foundation · Camille and Henry Dreyfus Foundation · David and Lucile Packard Foundation · U.S. Department of Energy · Division of Materials Research

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