Human-AI collaborative autonomous synthesis with pulsed laser deposition for remote epitaxy

Fuente: arXiv
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Main Authors: Haque, Asraful, Yimam, Daniel T., Chowdhury, Jawad, Bulanadi, Ralph, Vlassiouk, Ivan, Lasseter, John, Ghosh, Sujoy, Rouleau, Christopher M., Xiao, Kai, Liu, Yongtao, Zarkadoula, Eva, Vasudevan, Rama K., Harris, Sumner B.
Format: Preprint
Published: 2025
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author Haque, Asraful
Yimam, Daniel T.
Chowdhury, Jawad
Bulanadi, Ralph
Vlassiouk, Ivan
Lasseter, John
Ghosh, Sujoy
Rouleau, Christopher M.
Xiao, Kai
Liu, Yongtao
Zarkadoula, Eva
Vasudevan, Rama K.
Harris, Sumner B.
author_facet Haque, Asraful
Yimam, Daniel T.
Chowdhury, Jawad
Bulanadi, Ralph
Vlassiouk, Ivan
Lasseter, John
Ghosh, Sujoy
Rouleau, Christopher M.
Xiao, Kai
Liu, Yongtao
Zarkadoula, Eva
Vasudevan, Rama K.
Harris, Sumner B.
contents Autonomous laboratories typically rely on data-driven decision-making, occasionally with human-in-the-loop oversight to inject domain expertise. Fully leveraging AI agents, however, requires tightly coupled, collaborative workflows spanning hypothesis generation, experimental planning, execution, and interpretation. To address this, we develop and deploy a human-AI collaborative (HAIC) workflow that integrates large language models for hypothesis generation and analysis, with collaborative policy updates driving autonomous pulsed laser deposition (PLD) experiments for remote epitaxy of BaTiO$_3$/graphene. HAIC accelerated the hypothesis formation and experimental design and efficiently mapped the growth space to graphene-damage. In situ Raman spectroscopy reveals that chemistry drives degradation while the highest energy plume components seed defects, identifying a low-O$_2$ pressure low-temperature synthesis window that preserves graphene but is incompatible with optimal BaTiO$_3$ growth. Thus, we show a two-step Ar/O$_2$ deposition is required to exfoliate ferroelectric BaTiO$_3$ while maintaining a monolayer graphene interlayer. HAIC stages human insight with AI reasoning between autonomous batches to drive rapid scientific progress, providing an evolution to many existing human-in-the-loop autonomous workflows.
format Preprint
id arxiv_https___arxiv_org_abs_2511_11558
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle Human-AI collaborative autonomous synthesis with pulsed laser deposition for remote epitaxy
Haque, Asraful
Yimam, Daniel T.
Chowdhury, Jawad
Bulanadi, Ralph
Vlassiouk, Ivan
Lasseter, John
Ghosh, Sujoy
Rouleau, Christopher M.
Xiao, Kai
Liu, Yongtao
Zarkadoula, Eva
Vasudevan, Rama K.
Harris, Sumner B.
Materials Science
Artificial Intelligence
Autonomous laboratories typically rely on data-driven decision-making, occasionally with human-in-the-loop oversight to inject domain expertise. Fully leveraging AI agents, however, requires tightly coupled, collaborative workflows spanning hypothesis generation, experimental planning, execution, and interpretation. To address this, we develop and deploy a human-AI collaborative (HAIC) workflow that integrates large language models for hypothesis generation and analysis, with collaborative policy updates driving autonomous pulsed laser deposition (PLD) experiments for remote epitaxy of BaTiO$_3$/graphene. HAIC accelerated the hypothesis formation and experimental design and efficiently mapped the growth space to graphene-damage. In situ Raman spectroscopy reveals that chemistry drives degradation while the highest energy plume components seed defects, identifying a low-O$_2$ pressure low-temperature synthesis window that preserves graphene but is incompatible with optimal BaTiO$_3$ growth. Thus, we show a two-step Ar/O$_2$ deposition is required to exfoliate ferroelectric BaTiO$_3$ while maintaining a monolayer graphene interlayer. HAIC stages human insight with AI reasoning between autonomous batches to drive rapid scientific progress, providing an evolution to many existing human-in-the-loop autonomous workflows.
title Human-AI collaborative autonomous synthesis with pulsed laser deposition for remote epitaxy
topic Materials Science
Artificial Intelligence
url https://arxiv.org/abs/2511.11558