Digital Twin for Corelevel Spectroscopy & real-space KS-DFT

Wednesday, December 7, 2022 - 3:00pm

SpeakerJin Qian, LBL

Program Description:

The concept of Digital Twin originally came from the industry, which was referring to a “digital copy of the physical asset.” We attempt to construct a virtual laboratory infrastructure to solve a variety of technical challenges in data acquisition, control, analysis, and model-driven interpretation, dedicated to X-ray Photon Science with potential applications in chemical conversions. As daunting as it sounds, I will explain the challenges along with the milestones. Specifically, we have come a long way in 1) developing physically accurate quantum chemistry methods that improve the numerical accuracy of XPS binding energy (BE) calculation. 2) realizing that a central piece of chemical reaction network (CRN) is universal and generalizable in the chemical systems of interest (such as heterogeneous catalysis and reactors): the CRN itself is not directly observable, yet the dynamical behaviours of CRN can be probed through advanced characterization (such as APXPS, IR, Raman Spectroscopy ect.) as well as performance experiment (such as the measurement of turn-over-frequency (TOF), tafel slope, overpotential, etc.) 3) sharing a user-friendly, natural chemical language syntax Digital Twin v.01 software package, which we welcome collaboration and feedback in any form.

The second part of my talk acknowledges and addresses the bottleneck in developing and applying Digital Twin, which is the computational limits of conventional KS-DFT with a maximum cell size of a couple hundred atoms. We employed a combination of the real space finite-difference formulation and CheFSI to solve the Kohn–Sham equation and implemented this approach in ab initio Real-space Electronic Structure (ARES) software in a multi-processor, parallel environment. With our special focus in Photon Science, we derived, implemented, and achieved a ~0.15 eV desirable accuracy of ab-initio X-ray Photoelectron Spectroscopy binding energy predictions within the theoretical framework of real-space Kohn–Sham Density Functional Theory (real-space KS-DFT). Our work provides key advantages for calculating accurate core–electron binding energies of exascale systems with >10,000 atoms, hence bridging the knowledge gap between molecules to nanosystems of renewable energy priorities. 



Qian, J. #; Ye, Y. F. #; Yang, H.; Yano, J. *; Crumlin, E. J. *; Goddard, W. A. *, Initial Steps in Forming the Electrode-Electrolyte Interface: H2O Adsorption and Complex Formation on the Ag(111) Surface from Combining Quantum Mechanics Calculations and Ambient Pressure X-ray Photoelectron Spectroscopy. J Am Chem Soc 2019, 141, 6946.

Liu, C. #; Qian, J. #; Ye, Y. F.; Zhou, H.; Sun, C. J.; Sheehan, C.; Zhang, Z. Y.; Wan, G.; Liu, Y. S.; Guo, J. H.; Li, S.; Shin, H.; Hwang, S.; Gunnoe, T. B.; Goddard, W. A. *; Zhang, S. *, Oxygen evolution reaction over catalytic single-site Co in a well-defined brookite TiO2 nanorod surface. Nat Catal 2021, 4, 36.

Xu, Q., Prendergast, D., Qian, J.*, Real-Space Pseudopotential Method for the Calculations of 1s Core-Level Binding Energies. J Chem Theory Comput 2022, 18, 5471.

Qian, J., Crumlin, E.*, Prendergast, D.*, Efficient Basis Sets for Core-Excited States Motivated by Slater’s Rules. Phys Chem Chem Phys 2022, 24, 2243.

Digital Twin for Corelevel Spectroscopy & real-space KS-DFT
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