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Establishing the phase diagram of hydrogen is a major challenge for experimental and theoretical physics. Experiment alone cannot establish the atomic structure of solid hydrogen at high pressure, because hydrogen scatters X-rays only…

The crystal structure of high-pressure solid hydrogen remains a fundamental open problem. Although the research frontier has mostly shifted toward ultra-high pressure phases above 400 GPa, we show that even the broken symmetry phase…

Strongly Correlated Electrons · Physics 2025-12-30 Shengdu Chai , Chen Lin , Xinyang Dong , Yuqiang Li , Wanli Ouyang , Lei Wang , X. C. Xie

The study of the high pressure phase diagram of hydrogen has continued with renewed effort for about one century as it remains a fundamental challenge for experimental and theoretical techniques. Here we employ an efficient molecular…

Chemical Physics · Physics 2014-04-23 Guglielmo Mazzola , Seiji Yunoki , Sandro Sorella

The high-pressure II-III phase transition in solid hydrogen is investigated using the random phase approximation and diffusion Monte Carlo. Good agreement between the methods is found confirming that an accurate treatment of exchange and…

Materials Science · Physics 2024-10-08 Maria Hellgren , Damian Contant , Thomas Pitts , Michele Casula

The interplay between electron correlation and nuclear quantum effects makes our understanding of elemental hydrogen a formidable challenge. Here, we present the phase diagram of hydrogen and deuterium at low temperatures and high-pressure…

Materials Science · Physics 2023-06-28 Lorenzo Monacelli , Michele Casula , Kosuke Nakano , Sandro Sorella , Francesco Mauri

Experimental progress finally reached the metallic solid hydrogen phase, which was predicted by Wigner and Huntington over 80 years ago. However, the different structures in the phase diagram are still been debated due to the difficulty of…

Materials Science · Physics 2022-01-03 Tom Ichibha , Yunwei Zhang , Kenta Hongo , Ryo Maezono , Fernando A. Reboredo

We have studied solid hydrogen up to pressures of 300 GPa and temperatures of 350 K using density functional theory methods and have found "mixed structures" that are more stable than those predicted earlier. Mixed structures consist of…

Materials Science · Physics 2012-06-20 Chris J. Pickard , Miguel Martinez-Canales , Richard J. Needs

The high-pressure phases of solid hydrogen are of fundamental interest and relevant to the interior of giant planets; however, knowledge of these phases is far from complete. Particle swarm optimization (PSO) techniques were applied to a…

Materials Science · Physics 2012-05-09 Hanyu Liu , Hui Wang , Yanming Ma

We use the diffusion quantum Monte Carlo to revisit the enthalpy-pressure phase diagram of the various products from the different proposed decompositions of H$_2$S at pressures above 150~GPa. Our results entails a revision of the…

Materials Science · Physics 2017-03-03 Sam Azadi , Thomas D. Kühne

We study the structural and electronic properties of phase III of solid hydrogen using accurate many-electron theories and compare to state-of-the-art experimental findings. The atomic structures of phase III modelled by C2/c-24 crystals…

Materials Science · Physics 2021-02-24 Ke Liao , Tong Shen , Xin-Zheng Li , Ali Alavi , Andreas Grüneis

We reassess the phase diagram of high-pressure solid hydrogen using mean-field and many-body wave function based approaches to determine the nature of phase III of solid hydrogen. To discover the best candidates for phase III, density…

Other Condensed Matter · Physics 2019-10-09 Sam Azadi , T. D. Kuehne

A theoretical study is reported of the molecular-to-atomic transition in solid hydrogen at high pressure. We use the diffusion quantum Monte Carlo method to calculate the static lattice energies of the competing phases and a…

Materials Science · Physics 2014-04-23 Sam Azadi , Bartomeu Monserrat , W. M. C. Foulkes , R. J. Needs

We use the diffusion quantum Monte Carlo (DMC) method to calculate the ground state phase diagram of solid molecular hydrogen and examine the stability of the most important insulating phases relative to metallic crystalline molecular…

Materials Science · Physics 2015-06-16 S. Azadi , W. M. C. Foulkes , T. D. Kuehne

We use coupled-cluster quantum chemical methods to calculate the energetics of molecular clusters cut out of periodic molecular hydrogen structures that model observed phases of solid hydrogen. The hydrogen structures are obtained from…

Materials Science · Physics 2017-03-15 J. R. Trail , P. López Ríos , R. J. Needs

We survey the phase diagram of high-pressure molecular hydrogen with path integral molecular dynamics using a machine-learned interatomic potential trained with Quantum Monte Carlo forces and energies. Besides the HCP and C2/c-24 phases, we…

Materials Science · Physics 2023-02-22 Hongwei Niu , Yubo Yang , Scott Jensen , Markus Holzmann , Carlo Pierleoni , David M. Ceperley

The stability of high-pressure phases of hydrogen remains a central question in condensed matter physics, where both experimental observations and theoretical predictions are highly sensitive to methodological choices. Here, we revisit the…

Materials Science · Physics 2025-10-03 Stefano Racioppi , Eva Zurek

We present extensive molecular dynamics (MD) simulations investigating numerous candidate crystal structures for hydrogen in conditions around the present experimental frontier (400GPa). Spontaneous phase transitions in the simulations…

Materials Science · Physics 2015-11-18 Ioan B. Magdau , Graeme J. Ackland

Ab initio molecular dynamic method within the framework of density functional theory is applied to analyze the structural and electronic properties of crystalline molecular hydrogen at temperature 100\,K. Pressure, pair correlation function…

Materials Science · Physics 2022-01-12 I. Saitov

We present a study of hydrogen at pressures higher than molecular dissociation using the Coupled Electron-Ion Monte Carlo method. These calculations use the accurate Reptation Quantum Monte Carlo method to estimate the electronic energy and…

Materials Science · Physics 2013-05-29 Miguel A. Morales , Carlo Pierleoni , David Ceperley

We introduce an efficient scheme for the molecular dynamics of electronic systems by means of quantum Monte Carlo. The evaluation of the (Born-Oppenheimer) forces acting on the ionic positions is achieved by two main ingredients: i) the…

Strongly Correlated Electrons · Physics 2009-11-13 Claudio Attaccalite , Sandro Sorella
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