A Perspective on Phase Space Electronic Structure Theory : From Its Surface Hopping Origins Through To Its Future Promise
Abstract
We trace the history of phase space electronic structure theory (PSEST), high- lighting how this powerful approach emerged from fundamental questions in semi- classical surface hopping dynamics and evolved into an alternative to standard Born- Oppenheimer based electronic structure theory (with moving instead of frozen nuclei). Our goal herein is not to recapitulate the mathematical details of phase space electronic structure calculations, and few equations are presented so as to maximize readability. Instead, our goal is to provide intuition for those new to the field both (i) regarding the physics present when solving the Schrodinger equation in a non-inertial frame as well as (ii) regarding why PSEST is a necessary step forward towards understanding chemical problems involving spin (with limited practical alternatives). We further high- light some of the many open questions in this fast developing area, which will hopefully inspire new practitioners in this field. This intuitive perspective lacks many equations and is meant to complement (rather than replace) the more technical review given in Bian et al, Chem. Phys. Rev. 7, 011303 (2026)
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BibTeX
@misc{subotnik2026perspective,
title = {{A Perspective on Phase Space Electronic Structure Theory : From Its Surface Hopping Origins Through To Its Future Promise}},
author = {Joseph E. Subotnik and Ethan Alguire and Nicole Bellonzi and Xuezhi Bian and Mansi Bhati and Nadine Bradbury and D. Vale Cofer-Shabica and Ben Curlee and Titouan Duston and Shervin Fatehi and Gaohan Miao and Zheng Pei and Linqing Peng and Tian Qiu and Zhen Tao and Hung-Hsuan Teh and Xinchun Wu and Yanze Wu and Zain Zaidi and Yihan Shao and Jonathan Rawlinson and Neil Shenvi and Robert Littlejohn},
howpublished = {arXiv},
year = {2026},
month = sep,
doi = {10.48550/arxiv.2608.11448},
eprint = {2608.11448},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2608.11448},
}
RIS
TY - UNPB
TI - A Perspective on Phase Space Electronic Structure Theory : From Its Surface Hopping Origins Through To Its Future Promise
AU - Joseph E. Subotnik
AU - Ethan Alguire
AU - Nicole Bellonzi
AU - Xuezhi Bian
AU - Mansi Bhati
AU - Nadine Bradbury
AU - D. Vale Cofer-Shabica
AU - Ben Curlee
AU - Titouan Duston
AU - Shervin Fatehi
AU - Gaohan Miao
AU - Zheng Pei
AU - Linqing Peng
AU - Tian Qiu
AU - Zhen Tao
AU - Hung-Hsuan Teh
AU - Xinchun Wu
AU - Yanze Wu
AU - Zain Zaidi
AU - Yihan Shao
AU - Jonathan Rawlinson
AU - Neil Shenvi
AU - Robert Littlejohn
PY - 2026
DA - 2026/09/20
PB - arXiv
DO - 10.48550/arxiv.2608.11448
UR - https://arxiv.org/abs/2608.11448
AB - We trace the history of phase space electronic structure theory (PSEST), high- lighting how this powerful approach emerged from fundamental questions in semi- classical surface hopping dynamics and evolved into an alternative to standard Born- Oppenheimer based electronic structure theory (with moving instead of frozen nuclei). Our goal herein is not to recapitulate the mathematical details of phase space electronic structure calculations, and few equations are presented so as to maximize readability. Instead, our goal is to provide intuition for those new to the field both (i) regarding the physics present when solving the Schrodinger equation in a non-inertial frame as well as (ii) regarding why PSEST is a necessary step forward towards understanding chemical problems involving spin (with limited practical alternatives). We further high- light some of the many open questions in this fast developing area, which will hopefully inspire new practitioners in this field. This intuitive perspective lacks many equations and is meant to complement (rather than replace) the more technical review given in Bian et al, Chem. Phys. Rev. 7, 011303 (2026)
ER -