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Electronic Structure Theory for Electronic Excitation and Dynamics: Materials and Condensed Phase Systems
The overarching theme of our research is to develop a predictive understanding of electronic excitation and dynamical phenomena that emerge from the complex interplay between electrons and atomic nuclei, particularly in condensed phases and other extended systems. We focus on the development and application of computational methods grounded in first-principles electronic structure theory to gain new molecular-level insights into these processes. Our research program is inherently interdisciplinary, integrating concepts and techniques from chemistry, condensed matter physics, and materials science, and drawing upon applied mathematics and computer science for methodological and computational advances.
Current Research Areas
Electronic structure methods for condensed-phase matter
We aim to advance computational methodologies based on first-principles electronic structure theory, with a particular emphasis on large-scale, massively parallel computing, to explore new frontiers in condensed matter science. In recent years, our development efforts have focused primarily on real-time time-dependent density functional theory (RT-TDDFT) for investigating nonequilibrium electron dynamics in extended systems. This work is also closely integrated with our development of the nuclear–electronic orbital (NEO) method, enabling the study of coupled quantum dynamics of protons and electrons in heterogeneous environments. Another major direction of our research is the development of all-electron, numeric atom-centered orbital approaches to first-principles Green’s function theories—such as the GW approximation and Bethe–Salpeter equation (BSE) methods—for probing electronic excitation properties of extended systems.
Read recent publications in this area:
Constrained nuclear-electronic orbital method for periodic density functional theory:Application to H2 chemisorption on Si(001)surfaces
S. Liu, J. Xu, Y. Kanai
J. Chem. Phys., 163, 084110 (2025) - Annabella Selloni Festschrift
All-electron BSE@GW method with Nnumeric Atom-Centered Orbitals for Extended Periodic Systems
R. Zhou, Y. Yao, V. Blum, X. Ren, Y. Kanai
J. Chem. Theory. Comput., 21, 291 (2025)
Machine-Learning Electron Dynamics with Moment Propagation Theory: Application to Optical Absorption Spectrum Computation using Real-Time TDDFT
N. Boyer, C. Shepard, R. Zhou, J. Xu, Y. Kanai
J. Chem. Theory. Comput., 21, 114 (2025)
Lagrangian Formulation of Nuclear-Electronic Orbital Ehrenfest Dynamics with Real-Time TDDFT for Extended Periodic Systems
J. Xu, R. Zhou, T. E. Li, S. Hammes-Schiffer, Y. Kanai
J. Chem. Phys., 161, 194109 (2024)
BSE@GW Prediction of Charge Transfer Exciton in Molecular Complexes: Assessment of Self-energy and Exchange-Correlation Dependence
S. Bhattacharya, J. Li, W. Yang, and Y. Kanai
J. Phys. Chem. A, 128, 6072 (2024) - Rodney J. Bartlett Festschrift issue
Efficient Exact Exchange using Wannier Functions and Other Related Developments in Planewave-Pseudopotential Implementation of RT-TDDFT
C. Shepard, R. Zhou, T. E. Carney, J. Bost, Y. Yao, Y. Kanai
J. Chem. Phys. 161, 024111 (2024)
Real-Time TDDFT for Simulating Nonequilibrium Electron Dynamics
J. Xu, T. E. Carney, R. Zhou, C. Shepard, Y. Kanai
J. Am. Chem. Soc. 146, 5011 (2024) - Invited Perspective
Efficient Exact Exchange using Wannier Functions and Other Related Developments in Planewave-Pseudopotential Implementation of RT-TDDFT
C. Shepard, R. Zhou, T. E. Carney, J. Bost, Y. Yao, Y. Kanai
J. Chem. Phys. 161, 024111 (2024)
Theory of Moment Propagation for Quantum Dynamics in Single-Particle Description
N. Boyer, C. Shepard, R. Zhou, J. Xu, Y. Kanai
J. Chem. Phys. 160, 064113 (2024)
First-Principles Approach for Coupled Quantum Dynamics of Electrons and Protons in Heterogeneous Systems
J. Xu, R. Zhou, V. Blum, T. E. Li, S. Hammes-Schiffer, Y. Kanai
Phys. Rev. Lett. 131, 238002 (2023) Editors' Suggestion
All-electron BSE@GW method for K-edge Core Electron Excitation Energies
Y. Yao, D. Golze, P. RInke, V. Blum, Y. Kanai
J. Chem. Theor. Comp. 18, 1569 (2022)
Nuclear-Electronic Orbital Approach to Quantization of Protons in Periodic Electronic Structure Calculations
J. Xu, R. Zhou, Z. Tao, C. Malbon, V. Blum, S. Hammes-Schiffer, Y. Kanai
J. Chem. Phys. 156, 224111 (2022)
Simulating Electronic Excitation and Dynamics with Real-time Propagation Approach to TDDFT within Plane-wave Pseudopotential Formulation (Perspective)
C. Shepard, R. Zhou, D. C. Yost, Y. Yao, Y. Kanai
J. Chem. Phys. 155, 100901 (2021)
All-electron real-time and imaginary-time time-dependent density functional theory within a numeric atom-centered basis function framework
J. Hekele, Y. Yao, Y. Kanai, V. Blum, P. Kratzer
J. Chem. Phys. 155, 154801 (2021)
Dynamical Transition Orbitals: A Particle-Hole Description in Real-time TDDFT Dynamics
R. Zhou and Y. Kanai
J. Chem. Phys. 154, 054107 (2021)
All-electron Ab Initio Bethe-Salpeter Equation Approach to Neutral Excitations in Molecules with Numeric Atom-Centered Orbitals
C. Liu, J. Kloppernburg, Y. Yao, X. Ren, H. Appel, Y. Kanai, V. Blum
J. Chem. Phys. 152, 044105 (2020)
Propagation of Maximally Localized Wannier Functions in Real-Time TDDFT
D. Yost, Y. Yao, Y. Kanai
J. Chem. Phys. 150, 194113 (2019)
Quantum Dynamics Simulation of Electrons in Materials on High-Performance Computers
A. Schleife, E. Draeger, V. Anisimov, A. Correa, Y. Kanai
Electronic excitation and transport
A major effort in this thrust is devoted to investigating electronic stopping dynamics, which describes the nonlinear energy transfer from energetic charged particles (e.g., protons and alpha particles) to materials via electronic excitation. Understanding this nonequilibrium process at the atomistic scale in condensed matter systems is fundamental to a wide range of technological applications, including aerospace electronics and proton beam therapy. Another key direction involves exploring novel electron transport phenomena in extended systems. For instance, we have been studying Floquet topological phases in molecular systems using first-principles theory.
Read recent publications in this area:
Robustness of the Floquet Topological Phase at Room Temperature: a First-Principles Dynamics Study
R. Zhou and Y. Kanai
Phys. Chem. Chem. Phys., 27, 14410 (2025)
Hot Carrier Transfer from Plasmon Decay in Ag20 at H-Si(111) Surface: Real-Time TDDFT Simulation in Wannier Gauge
J. Bost, C. Shepard and Y. Kanai
Ion Type Dependence of DNA Electronic Excitation in Water under Proton, Alpha-particle, and Carbon Ion Irradiation: A First-Principles Simulation Study
C. Shepard and Y. Kanai
J. Phys. Chem. B, 127, 10700 (2023)
Molecular Control of Floquet Topological Phase in Non-adiabatic Thouless Pumping
R. Zhou and Y. Kanai
J. Phys. Chem. Lett. 14, 8205 (2023)
Electronic Excitation Response of DNA to High-Energy Proton Radiation in Water
C. Shepard, D. C. Yost, Y. Kanai
Phys. Rev. Lett. 130, 118401 (2023) Editors' Suggestion and Featured in Physics magazine
Nonlinear Electronic Excitation in Water under Proton Irradiation : A First Principles Study
C. Shepard and Y. Kanai
Physical Chemistry Chemical Physics, 24, 5598 (2022)
First-Principles Demonstration of Nonadiabatic Thouless Pumping of Electrons in a Molecular System
R. Zhou, D. C. Yost, and Y. Kanai
J. Phys. Chem. Lett. 12, 4496 (2021)
First-Principles Modeling of Electronic Stopping in Complex Matter under Ion Irradiation
D. C. Yost, Y. Yao, Y. Kanai
J. Phys. Chem. Lett. 11, 229 (2020)
K-shell Core Electronic Excitation in Electronic Stopping of Protons in Water from First Principles
Y. Yao, D. Yost, Y. Kanai
Phys. Rev. Lett., 123, 066401 (2019)
Electronic Excitation Dynamics in DNA under Proton and Alpha-particle Irradiation
D. Yost and Y. Kanai
J. Am. Chem. Soc., 141, 5241 (2019)
Examining Real-time TDDFT Non-equilibrium Simulation for the Calculation of Electronic Stopping Power
D. Yost, Y. Yao, and Y. Kanai
Phys. Rev. B, 96, 115134 (2017)
Electronic Excitation Dynamics in Liquid Water under Proton Irradiation
K. G. Reeves and Y. Kanai
Scientific Reports, 7, 40379 (2017)
Electronic Stopping Power for Protons and Alpha-particles from First Principles Electron Dynamics: The case of silicon carbide
D. C. Yost and Y. Kanai
Phys. Rev. B, 94, 115107 (2016)
Electronic Stopping Power in Liquid Water for Protons and Alpha-particles from First Principles
K. G. Reeves, Y. Yao, Y. Kanai
Phys. Rev. B (Rapid Comm.), 94, 041108(R) (2016)
Accurate Atomistic First-Principles Calculations of Electronic Stopping
A. Schleife, Y. Kanai, A. Correa
Phys. Rev. B, 91, 014306 (2015)
Novel material properties and dynamics
Using first-principles electronic structure methods, we also investigate novel materials and their emergent properties, often in close collaboration with experimental groups. Our research spans technologically promising systems such as two-dimensional organic–inorganic hybrid perovskites and molecule–semiconductor interfaces. Modern quantum-mechanical simulations enable us to explore these materials at the atomistic level, uncovering their fundamental behavior and assessing their potential for technological applications.
As part of the NSF Designing Materials to Revolutionize and Engineer our Future (DMREF) program, we investigate the material properties of hybrid organic–inorganic perovskites (HOIPs). These materials offer exceptional tunability of their optoelectronic properties due to their unique heterogeneous molecular and inorganic components. HOIPs exhibit a range of remarkable phenomena, including spin splitting induced by spin–orbit coupling and temperature-dependent superradiance. Our goal is to understand and design these novel properties at the atomistic scale through first-principles modeling.
Within the DOE Energy Innovation Hub, Center for Hybrid Approaches in Solar Energy to Liquid Fuels (CHASE), we study charge transfer dynamics and protonation steps at catalyst–semiconductor interfaces relevant to CO₂ reduction. We employ a combination of first-principles Green’s function theory and the real-time nuclear–electronic orbital time-dependent density functional theory (RT-NEO-TDDFT) approach, in which proton quantization is explicitly treated. Through this collaborative effort, we bring state-of-the-art computational methodologies to address key scientific challenges in solar energy conversion and catalysis.
Read recent publications in this area:
Predicting dynamic spin splitting in 2D hybrid organic-inorganic perovskites via machine learning model
S. Bhattacharya, A. J. Thomas, Y. Kanai
First-Principles Approach for Coupled Quantum Dynamics of Electrons and Protons in Heterogeneous Systems
J. Xu, R. Zhou, V. Blum, T. E. Li, S. Hammes-Schiffer, Y. Kanai
Phys. Rev. Lett. 131, 238002 (2023) Editors' Suggestion
Structure and electronic tunability of acene alkylamine based layered hybrid organic-inorganic perovskites from first principles
R. Song, C. Liu, Y. Kanai, D. B. Mitzi, V. Blum
Phys. Rev. Materials, 7, 084601 (2023)
Spin-orbit-coupling-induced band splitting in two-dimensional hybrid organic-inorganic perovskites: Importance of Organic Cations
S. Bhattacharya and Y. Kanai
Phys. Rev. Materials, 7, 055001 (2023)
Nuclear Quantum Effect and Its Temperature Dependence in Liquid Water from Random Phase Approximation via Artificial Neural Network
Y. Yao and Y. Kanai
J. Phys. Chem. Lett. 12, 6354 (2021)
Temperature Dependence of Nuclear Quantum Effects on Liquid Water via Artificial Neural Network Model based on SCAN meta-GGA Functional
Y. Yao and Y. Kanai
J. Chem. Phys. 153, 044114 (2020)
Tunable Semiconductors: Control over Carrier States and Excitations in Layered Hybrid Organic-Inorganic Perovskites
C. Liu, W. Huhn, K. Du, A. Vazquez-Mayagoitia, D. Dirkes, W. You, Y. Kanai, D. B. Mitzi, V. Blum
Phys. Rev. Lett., 121, 146401 (2018)
Diffusion Quantum Monte Carlo Study of Martensitic Phase Transition Energetics: The Case of Phosphorene
K. G. Reeves, Y. Yao, and Y. Kanai
J. Chem. Phys., 145, 124705 (2016)
Communication: Modeling of Concentration Dependent Water Diffusivity in Ionic Solutions: Role of Intermolecular Charge Transfer
Y. Yao, M. L. Berkowitz, Y. Kanai
J. Chem. Phys. (Comm.) 143, 241101 (2015)
We are a part of NSF-DMREF team and DOE-Energy Innovation Hub, CHASE, which offer exciting opportunities to collaborate with other research groups.
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