Synthesis and Formation Mechanism of All-Organic Block Copolymer-Directed Templating of Laser-Induced Crystalline Silicon Nanostructures

Kwan Wee Tan; Jörg G. Werner; Matthew D. Goodman; Ha Seong Kim; Byungki Jung; Hiroaki Sai; Paul V. Braun; Michael O. Thompson; Ulrich Wiesner

doi:10.1021/acsami.8b12706

Synthesis and Formation Mechanism of All-Organic Block Copolymer-Directed Templating of Laser-Induced Crystalline Silicon Nanostructures

Kwan Wee Tan
, Jörg G. Werner
, Matthew D. Goodman
, Ha Seong Kim
, Byungki Jung
, Hiroaki Sai
, Paul V. Braun
, Michael O. Thompson
, Ulrich Wiesner

Research output: Contribution to journal › Article › peer-review

16 Scopus citations

Abstract

This report describes the generation of three-dimensional (3D) crystalline silicon continuous network nanostructures by coupling all-organic block copolymer self-assembly-directed resin templates with lowerature silicon chemical vapor deposition and pulsed excimer laser annealing. Organic 3D mesoporous continuous-network resin templates were synthesized from the all-organic self-assembly of an ABC triblock terpolymer and resorcinol-formaldehyde resols. Nanosecond pulsed excimer laser irradiation induced the transient melt transformation of amorphous silicon precursors backfilled in the organic template into complementary 3D mesoporous crystalline silicon nanostructures with high pattern fidelity. Mechanistic studies on laser-induced crystalline silicon nanostructure formation revealed that the resin template was carbonized during transient laser-induced heating on the milli- to nanosecond timescales, thereby imparting enhanced thermal and structural stability to support the silicon melt-crystallization process at temperatures above 1250 °C. Photoablation of the resin material under pulsed excimer laser irradiation was mitigated by depositing an amorphous silicon overlayer on the resin template. This approach represents a potential pathway from organic block copolymer self-assembly to alternative functional hard materials with well-ordered 3D morphologies for potential hybrid photovoltaics, photonic, and energy storage applications.

Original language	English
Pages (from-to)	42777-42785
Number of pages	9
Journal	ACS Applied Materials and Interfaces
Volume	10
Issue number	49
DOIs	https://doi.org/10.1021/acsami.8b12706
State	Published - Dec 12 2018
Externally published	Yes

Funding

This work was supported by the National Science Foundation (NSF) Single Investigator Award (DMR-1707836). This work made use of research facilities at Cornell Center for Materials Research with support from the NSF Materials Research Science and Engineering Centers program (DMR-1719875); Cornell NanoScale Science & Technology Facility, a member of the National Nanotechnology Coordinated Infrastructure, which is supported by the NSF (Grant ECCS-1542081); and Cornell High Energy Synchrotron Source supported by the National Science Foundation under award DMR-1332208. The work at the University of Illinois was supported by Air Force Office of Scientific Research MURI FA9550-12-1-0471. K.W.T. acknowledges the Singapore Ministry of Education AcRF Tier 1 grant (2018-T1-001-084) and a startup grant from Nanyang Technological University, Singapore. The authors gratefully acknowledge Prof. L. Estroff, Dr. M. Weathers, Dr. R. Bell, and Dr. A. Jacobs of Cornell University for their kind experimental assistance and helpful discussions.

Keywords

3D silicon nanostructure
block copolymers
laser heating
self-assembly
templating

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10.1021/acsami.8b12706

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title = "Synthesis and Formation Mechanism of All-Organic Block Copolymer-Directed Templating of Laser-Induced Crystalline Silicon Nanostructures",

abstract = "This report describes the generation of three-dimensional (3D) crystalline silicon continuous network nanostructures by coupling all-organic block copolymer self-assembly-directed resin templates with lowerature silicon chemical vapor deposition and pulsed excimer laser annealing. Organic 3D mesoporous continuous-network resin templates were synthesized from the all-organic self-assembly of an ABC triblock terpolymer and resorcinol-formaldehyde resols. Nanosecond pulsed excimer laser irradiation induced the transient melt transformation of amorphous silicon precursors backfilled in the organic template into complementary 3D mesoporous crystalline silicon nanostructures with high pattern fidelity. Mechanistic studies on laser-induced crystalline silicon nanostructure formation revealed that the resin template was carbonized during transient laser-induced heating on the milli- to nanosecond timescales, thereby imparting enhanced thermal and structural stability to support the silicon melt-crystallization process at temperatures above 1250 °C. Photoablation of the resin material under pulsed excimer laser irradiation was mitigated by depositing an amorphous silicon overlayer on the resin template. This approach represents a potential pathway from organic block copolymer self-assembly to alternative functional hard materials with well-ordered 3D morphologies for potential hybrid photovoltaics, photonic, and energy storage applications.",

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author = "Tan, \{Kwan Wee\} and Werner, \{J{\"o}rg G.\} and Goodman, \{Matthew D.\} and Kim, \{Ha Seong\} and Byungki Jung and Hiroaki Sai and Braun, \{Paul V.\} and Thompson, \{Michael O.\} and Ulrich Wiesner",

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AU - Kim, Ha Seong

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AU - Sai, Hiroaki

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AU - Thompson, Michael O.

AU - Wiesner, Ulrich

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AB - This report describes the generation of three-dimensional (3D) crystalline silicon continuous network nanostructures by coupling all-organic block copolymer self-assembly-directed resin templates with lowerature silicon chemical vapor deposition and pulsed excimer laser annealing. Organic 3D mesoporous continuous-network resin templates were synthesized from the all-organic self-assembly of an ABC triblock terpolymer and resorcinol-formaldehyde resols. Nanosecond pulsed excimer laser irradiation induced the transient melt transformation of amorphous silicon precursors backfilled in the organic template into complementary 3D mesoporous crystalline silicon nanostructures with high pattern fidelity. Mechanistic studies on laser-induced crystalline silicon nanostructure formation revealed that the resin template was carbonized during transient laser-induced heating on the milli- to nanosecond timescales, thereby imparting enhanced thermal and structural stability to support the silicon melt-crystallization process at temperatures above 1250 °C. Photoablation of the resin material under pulsed excimer laser irradiation was mitigated by depositing an amorphous silicon overlayer on the resin template. This approach represents a potential pathway from organic block copolymer self-assembly to alternative functional hard materials with well-ordered 3D morphologies for potential hybrid photovoltaics, photonic, and energy storage applications.

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Synthesis and Formation Mechanism of All-Organic Block Copolymer-Directed Templating of Laser-Induced Crystalline Silicon Nanostructures

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