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Decomposition of contributions from core-levels exhibiting spin-orbit splitting in XUV core-level spectroscopy

Chang, Hung-Tzu and Zuerch, Michael W. and Kraus, Peter and Kaplan, Christopher and Borja, Lauren J. and Cushing, Scott and Neumark, Daniel M. and Leone, Stephen R. (2017) Decomposition of contributions from core-levels exhibiting spin-orbit splitting in XUV core-level spectroscopy. In: 253rd American Chemical Society National Meeting & Exposition, April 2-6, 2017, San Francisco, CA.

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Attosecond transient absorption spectroscopy (ATAS) is a versatile technique that allows observing ultrafast charge dynamics in solid-state samples. In ATAS, the transient absorption of a core-level excitation in the extreme UV (XUV) is measured following optical excitation of the sample. The lack of spin-selectivity in the XUV pulse results in overlapping XUV absorption spectra from spin-orbit split core-levels and leads to difficulty in disentangling the spectral signatures. Here, we demonstrate the successful retrieval of the contribution of a single spin-orbit level on the XUV transient absorption signal. Under the approxn. that the spin-orbit split levels yield identical absorption spectra which are energetically shifted and weighted by the degeneracy of the spin-orbit states, the contribution of one single spin-orbit state can be retrieved by the Fourier transform of the measured signal. In this case the energy shift of the spectra from the spin-orbit split states becomes a phase shift. By dividing out this phase factor and taking the inverse Fourier transform, the underlying signal referenced to a single spin-orbit level can be retrieved. We apply this method to an ATAS measurement at the germanium M_(4,5)-edge (30 eV), where the spin-orbit energy splitting (0.57 eV) is comparable to the germanium band gap (0.66 eV). The successful decompn. of the transient absorption signals yields clear, spectrally-resolved signatures of electrons and holes such that carrier dynamics can be simultaneously measured and characterized. The presented method allows decompg. contributions of spin-orbit split core-levels in a transient absorption spectrum. This allows clearer assignment of spectroscopic features and reveals weak signal contributions not visible in the exptl. raw data. In the presented case of germanium M-edge spectroscopy, a clear assignment of features assocd. with electrons, holes and the bandgap becomes possible only after applying this method.

Item Type:Conference or Workshop Item (Paper)
Related URLs:
URLURL TypeDescription Archive
Chang, Hung-Tzu0000-0001-7378-8212
Kaplan, Christopher0000-0002-5873-9487
Cushing, Scott0000-0003-3538-2259
Neumark, Daniel M.0000-0002-3762-9473
Leone, Stephen R.0000-0003-1819-1338
Additional Information:© 2017 American Chemical Society.
Record Number:CaltechAUTHORS:20180627-100741086
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:87384
Deposited By: Tony Diaz
Deposited On:27 Jun 2018 17:14
Last Modified:09 Mar 2020 13:19

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