Electrochemical Control of the Ultrafast Lattice Response of a Layered Semimetal

Felipe A de Quesada; Philipp K Muscher; Eliana S Krakovsky; Aditya Sood; Andrey D Poletayev; Edbert J Sie; Clara M Nyby; Sara J Irvine; Marc E Zajac; Duan Luo; Xiaozhe Shen; Matthias C Hoffmann; Patrick L Kramer; R Joel England; Alexander H Reid; Stephen P Weathersby; Leora E Dresselhaus-Marais; Daniel A Rehn; William C Chueh; Aaron M Lindenberg

doi:10.1002/advs.202411344

Electrochemical Control of the Ultrafast Lattice Response of a Layered Semimetal

Adv Sci (Weinh). 2024 Dec 16:e2411344. doi: 10.1002/advs.202411344. Online ahead of print.

Authors

Felipe A de Quesada^{1

2}, Philipp K Muscher^{1

2}, Eliana S Krakovsky^{1

3}, Aditya Sood^{4

5}, Andrey D Poletayev^{1

2

6}, Edbert J Sie^{1

2}, Clara M Nyby^{1

2}, Sara J Irvine^{1

2}, Marc E Zajac^{1

2}, Duan Luo^{1

2}, Xiaozhe Shen⁷, Matthias C Hoffmann⁷, Patrick L Kramer⁷, R Joel England⁷, Alexander H Reid⁷, Stephen P Weathersby⁷, Leora E Dresselhaus-Marais^{1

2

8}, Daniel A Rehn³, William C Chueh^{1

2}, Aaron M Lindenberg^{1

2

8}

Affiliations

¹ Department of Materials Science and Engineering, Stanford University, Stanford, CA, 94305, USA.
² Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
³ Computational Physics Division, Los Alamos National Laboratory, Los Alamos, NM, 87545, USA.
⁴ Department of Mechanical and Aerospace Engineering, Princeton University, Princeton, NJ, 08544, USA.
⁵ Princeton Materials Institute, Princeton University, Princeton, NJ, 08540, USA.
⁶ Department of Materials, University of Oxford, Oxford, OX1 3PH, UK.
⁷ SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.
⁸ Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, CA, 94025, USA.

PMID: 39686650
DOI: 10.1002/advs.202411344

Abstract

The unique layer-stacking in two-dimensional (2D) van der Waals materials facilitates the formation of nearly degenerate phases of matter and opens novel routes for the design of low-power, reconfigurable functional materials. Electrochemical ion intercalation between stacked layers offers a promising approach to stabilize bulk metastable phases and to explore the effects of extreme carrier doping and strain. However, in situ characterization methods to study the structural evolution and dynamical functional properties of these intercalated materials remains limited. Here a novel experimental platform is presented capable of simultaneously performing electrochemical lithium-ion intercalation and multimodal ultrafast characterization of the lattice using both electron diffraction and nonlinear optical techniques. Using the layered semimetal WTe₂ as a model system, the interlayer shear phonon mode that modulates stacking between 2Dlayers is probed, showing that small amounts of lithiation enhance the amplitude and lifetime of the phonon, contrary to expectations. This results from the dynamically fluctuating and anharmonic structure between nearly degenerate phases at room temperature, which can be stabilized by electronic carriers accompanying the inserted lithium ions. At high lithiation, the T_d' structure emerges and quenches the phonon response. This work defines new approaches for using electrochemistry to engineer the dynamic structure of 2D materials.

Keywords: WTe2; electrochemical lithiation; in‐operando; phase control; ultrafast electron diffraction.

Abstract

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