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Ultrasensitive Photothermal Spectroscopy: Harnessing the Seebeck Effect for Attogram-Level Detection

  • Yaoli Zhao
    Yaoli Zhao
    Chemical and Biological Engineering, University at Buffalo, Buffalo, New York 14260, United States
    More by Yaoli Zhao
  • Patatri Chakraborty
    Patatri Chakraborty
    Chemical and Biological Engineering, University at Buffalo, Buffalo, New York 14260, United States
  • Ali Passian
    Ali Passian
    Quantum Computing and Sensing Group, Computational Sciences and Engineering Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    More by Ali Passian
  • , and 
  • Thomas Thundat*
    Thomas Thundat
    Chemical and Biological Engineering, University at Buffalo, Buffalo, New York 14260, United States
    *Email: [email protected]
Cite this: Nano Lett. 2023, 23, 17, 7883–7889
Publication Date (Web):August 14, 2023
https://doi.org/10.1021/acs.nanolett.3c01710
Copyright © 2023 American Chemical Society

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    Abstract

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    Molecular-level spectroscopy is crucial for sensing and imaging applications, yet detecting and quantifying minuscule quantities of chemicals remain a challenge, especially when they surface adsorb in low numbers. Here, we introduce a photothermal spectroscopic technique that enables the high selectivity sensing of adsorbates with an attogram detection limit. Our approach utilizes the Seebeck effect in a microfabricated nanoscale thermocouple junction, incorporated into the apex of a microcantilever. We observe minimal thermal mass exhibited by the sensor, which maintains exceptional thermal insulation. The temperature variation driving the thermoelectric junction arises from the nonradiative decay of molecular adsorbates’ vibrational states on the tip. We demonstrate the detection of photothermal spectra of physisorbed trinitrotoluene (TNT) and dimethyl methylphosphonate (DMMP) molecules, as well as representative polymers, with an estimated mass of 10–18 g.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.nanolett.3c01710.

    • Additional details on the nanothermal probe, TAPS experimental arrangement, photothermal spectroscopy, the comparison of performance between the bimaterial cantilever and nanothermal probe, a detailed analysis of experimental data on another set of nanoprobes, QCL power profile, calculations of adsorbed mass on the nanoprobe, and the computational model (PDF)

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