Research
Subtask 1: "Digital Twin" for Core Level Spectroscopy
The fascinating concept of "Digital Twin" originated from the industry, which was referring to a "digital copy of the physical asset". For example, in its industrial settings, such asset can refer to a turbine, where we could use the data collected during the digital twin's simulated operations to minimize failure rates, to shorten development cycle, and to ensure that the product can be built. In other contexts, we could imagine having a digital twin of the organization, which facilitates the comprehensive planning of the processes in a business. "Digital Twin" is a broad concept that is applicable to a wide range of different fields. Embracing and moving into the digital era, our grand vision is to build a digital entity, that faithfully outputs the precise experimental outcomes such as measurable spectra, materials characterization data, performances cycle, etc., with a current special focus on core-level spectroscopy. The pillar stones for the success of our "Digital Twin" are a) the correct physics captured in electronic structure theory (Subtask 2), as well as b) accurate description of the thermodynamics and kinetics (Subtask 3).
Subtask 2: Physics-Driven Electronic Structure Theory Development
Upon bombarding of a photon (either with tunable photon energy from a synchrotron source or a monochromatic tabletop source) to a given sample of interest, a pair of core-hole are created. This excited electron can further be ejected to the vacuum level (as in the case of X-ray Photoelectron Spectroscopy or XPS), or to the valence band (as in the case of X-ray Adsorption Spectroscopy or XAS), or to the valence band and then subsequently filling the empty core states (as in the case of Resonant inelastic X-ray scattering or RIXS). As one may naturally expect, physically and numerically accurate description of such core-excited processes demand more than routine ground state setups. We develop electronic structure code and efficient algorithms specialized for the description of core excitation in isolated molecular systems, condensed matter systems, as well as large-scale systems. These computational tools are actively helping out the interpretation of experimentally observed X-ray spectra in various scenarios.
Subtask 3: Thermodynamics and Kinetics in Chemical Transformations
Chemical transformations and conversions plays a significant role in almost every aspect of modern society, such as transportation, utility, agriculture, and the manufacturing of a variety of consumer products. Chemical transformations involved in the realistic systems are orders of magnitude more complex than the clean electronic/atomic picture described above in Subtask 2, yet we may be able to approximate these complex systems as a collection and network of fundamental chemical reactions dominated by thermodynamics and kinetics principles that control chemical reactivity in their pristine environment. Coupling the thermodynamics/kinetics aspects with the electronic structure aspects, we aim to uncover new insights in more complex environments, such as clusters, and nanoparticle surfaces which are frequently utilized in renewable energy applications.
APXPS_15min_Jin Qian_subtitle.mp4Jin's 15-mins talk at 7th International Ambient Pressure X-ray Photoemission Spectroscopy Workshop, December 2020
An updated list of published works can be found at google scholar.
Jana, A., Qian, J.*, Crumlin, E. J.*, Impact of surface defects on the design of energy-efficient metal nanoparticle/ligand-based catalysts for electrochemical CO2 reduction. Submitted 2024.
Liu, L., Cunha, L., Xu, Q., Xin, H., Head-Gordon, M., Qian, J.*, Real-Space Pseudopotential Method for the Calculation of Third-Row Elements X-ray Photoelectron Spectroscopic (XPS) Signatures. In preparation 2024.
Shan, Y., Zhao, X., Guzman, M. F., Jana, A., Chen, S., Yu, S., Ng, K., Roh, I., Chen, H., Altoe, V., Corder, S. G., Bechtel, H., Qian, J., Salmeron, M.*, Yang, P.*, Nanometre-resolved observation of electrochemical microenvironment formation at the nanoparticle–ligand interface. Nat Catal 2024, in press.
Glenna, D. M., Jana, A., Xu, Q., Wang, Y., Meng, Y., Yang Y., Neupane M., Wang, L., Zhao, H.*, Qian J.*, Snyder, S. W.*, Carbon Capture: Theoretical Guidelines for Activated Carbon-based CO2 Adsorption Material Evaluation. J Phys Chem Lett 2023, 14, 10693.
Devlin, S., Jamnuch, S., Xu, Q., Chen, A., Qian, J.*, Pascal, T. A.*, Saykally, R.*, Agglomeration Drives the Reversed Fractionation of Aqueous Carbonate and Bicarbonate at the Air-water Interface. J Am Chem Soc 2023, 145, 22384
Jana, A., Snyder, S., Crumlin, E. J.*, Qian, J.*, Integrated Carbon Capture and Conversion: A Review on C2+ Product Mechanisms and Mechanism-guided Strategies. Frontiers in Chemistry 2023, 11,1135829
Aydogan Gokturk, P., Sujanani, R., Qian, J., Wang, Y., Katz, L. E., Freeman, B., Crumlin, E. J.*, The Donnan Potential Revealed. Nat Commun 2022, 13, 5880
Lu, W., Zhang, E., Qian, J., Weeraratna, C., Jackson, M., Zhu, C., Long, J., Ahmed, M.*, Probing Growth of Metal–Organic Frameworks with X-Ray Scattering and Vibrational Spectroscopy. Phys Chem Chem Phys 2022, 24, 26102
Hao, H. #, Pestana L. #, Liu M., Qian, J. #, Xu, Q., Head-Gordon T. *, Chemical Transformation and Transport Properties at Interfaces. Wiley Interdiscip Rev Comput Mol Sci 2022, 1639.
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. J. *; Prendergast, D. *, Efficient Basis Sets for Core-excited States Motivated by Slater's Rules. Phys Chem Chem Phys 2022, 24, 2243.
Peng, T. #; Zhuang, T. T. #; Yuan, Y. #; Qian, J. #; Dick, G. R.; Bueren, J. B.; Hung S. F.; Zhang, Y; Wang, Z. Y.; Wicks, J.; Arquer, F. P.; Abed, J.; Wang, N.; Rasouli, A. S.; Lee, G. H.; Wang, M.; He, D. P.; Wang, Z.; Liang, Z. X.; Song, L.; Wang, X.; Chen, B.; Ozden, A.; Lum, Y.W.; Leow, W. R.; Luo, M. C.; Meira, D. M.; Ip, A. H.; Luterbacher, J. S. *; Zhao, W. *; Sargent, E. H. *, Ternary Alloys Enable Efficient Production of Methoxylated Chemicals via Selective Electrocatalytic Hydrogenation of Lignin Monomers. J Am Chem Soc 2021, 143, 17226.
Esmaeilirad, M. #; Baskin, A. #; Kondori, A.; Matias, A. S.; Qian, J.; Song, B. B.; Kucuk, K.; Belmonte, A. R.; Delgado, P. N. M.; Park, J. W.; Azari, R.; Segre, C. U.; Shahbazian-Yassar, R.; Prendergast, D. *; Asadi, M. *, Gold-Like Activity, Copper-Like Selectivity of Heteroatomic Transition Metal Carbides (M2C) for Electrocatalytic Carbon Dioxide Reduction Reaction. Nat Commun 2021, 12, 5067.
Wang, Y. X.; Qian, J.; Fang, Z. T.; Kunz, M. R.; Yablonsky, G.; Fortunelli, A.; Goddard, W. A. *; Fushimi, R. R. *, Understanding Reaction Networks through Artificial Equilibrium Experiments using Transient Methods. J Am Chem Soc 2021, 143, 10998.
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.
Qian, J.; Baskin, A.; Liu, Z.; Prendergast, D. *; Crumlin, E. J. *, Addressing the Sensitivity of Signals from Solid/Liquid Ambient Pressure XPS (APXPS) Measurement. J Chem Phys 2020, 153, 044709.
Ye, Y. F. #; Qian, J. #; Yang, H. #; Su, H. Y.; Lee, K. J.; Etxebarria, A.; Cheng, T.; Xiao, H.; Yano, J. K. *; Goddard, W. A. *; Crumlin, E. J. *, Synergy between a Silver-Copper Surface Alloy Composition and Carbon Dioxide Adsorption and Activation. Acs Appl Mater Inter 2020, 12, 25374.
Ye, Y. F. #; Yang, H. #; Qian, J. #; Su, H. Y.; Lee, K. J.; Cheng, T.; Xiao, H.; Yano, J. *; Goddard, W. A. *; Crumlin, E. J. *, Dramatic Differences in Carbon Dioxide Adsorption and Initial Steps of Reduction between Silver and Copper. Nat Commun 2019, 10, 1875.
Qian, J.; Fortunelli, A.; Goddard, W. A. *, Effect of Co Doping on Mechanism and Kinetics of Ammonia Synthesis on Fe(111) Surface. J Catal 2019, 370, 364.
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.
Qian, J.; An, Q.; Fortunelli, A.; Nielsen, R. J.; Goddard, W. A. *, Reaction Mechanism and Kinetics for Ammonia Synthesis on the Fe(111) Surface. J Am Chem Soc 2018, 140, 6288.
An, Q.; Reddy, K. M.; Qian, J.; Hemker, K. J.; Chen, M. W.; Goddard, W. A. *, Nucleation of Amorphous Shear Bands at Nanotwins in Boron Suboxide. Nat Commun 2016, 7, 11001.
An, Q.; Qian, J.; Nielsen, R. R.; Sementa, L.; Barcaro, G.; Negreiros, F. R.; Fortunelli, A.; Goddard, W. A. *, The Quantum Mechanics Derived Atomistic Mechanism Underlying the Acceleration of Catalytic CO Oxidation on Pt(110) by Surface Acoustic Waves. J Mater Chem A 2016, 4, 12036.