Title: Atomic Layer Deposition of Metal Sulfide Materials

Abstract

The field of nanoscience is delivering increasingly intricate yet elegant geometric structures incorporating an ever-expanding palette of materials. Atomic layer deposition (ALD) is a powerful driver of this field, providing exceptionally conformal coatings spanning the periodic table and atomic-scale precision independent of substrate geometry. This versatility is intrinsic to ALD and results from sequential and self-limiting surface reactions. This characteristic facilitates digital synthesis, in which the film grows linearly with the number of reaction cycles. While the majority of ALD processes identified to date produce metal oxides, novel applications in areas such as energy storage, catalysis, and nanophotonics are motivating interest in sulfide materials. Recent progress in ALD of sulfides has expanded the diversity of accessible materials as well as a more complete understanding of the unique chalcogenide surface chemistry. ALD of sulfide materials typically uses metalorganic precursors and hydrogen sulfide (H₂S). As in oxide ALD, the precursor chemistry is critical to controlling both the film growth and properties including roughness, crystallinity, and impurity levels. By modification of the precursor sequence, multicomponent sulfides have been deposited, although challenges remain because of the higher propensity for cation exchange reactions, greater diffusion rates, and unintentional annealing of this more labile class ofmore » materials. A deeper understanding of these surface chemical reactions has been achieved through a combination of in situ studies and quantum-chemical calculations. As this understanding matures, so does our ability to deterministically tailor film properties to new applications and more sophisticated devices. This Account highlights the attributes of ALD chemistry that are unique to metal sulfides and surveys recent applications of these materials in photovoltaics, energy storage, and photonics. Within each application space, the benefits and challenges of novel ALD processes are emphasized and common trends are summarized. We conclude with a perspective on potential future directions for metal chalcogenide ALD as well as untapped opportunities. As a result, we consider challenges that must be addressed prior to implementing ALD metal sulfides into future device architectures.« less

Authors:

Dasgupta, Neil P. ^[1]; Meng, Xiangbo ^[2]; Elam, Jeffrey W. ^[2]; Martinson, Alex B. F. ^[3]

---

+ Show Author Affiliations

1. Department of Mechanical Engineering, University of Michigan, Ann Arbor, Michigan 41809, United States
2. Energy Systems Division, Argonne National Laboratory, Argonne, Illinois 60439, United States
3. Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, United States

Publication Date:

2015-01-12

Research Org.:

Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:

1168427

Alternate Identifier(s):

OSTI ID: 1210267; OSTI ID: 1224204

Grant/Contract Number:  

AC02-06CH11357; SC0001059

Resource Type:

Published Article

Journal Name:

Accounts of Chemical Research

Additional Journal Information:

Journal Name: Accounts of Chemical Research Journal Volume: 48 Journal Issue: 2; Journal ID: ISSN 0001-4842

Publisher:

American Chemical Society

Country of Publication:

United States

Language:

English

Subject:

25 ENERGY STORAGE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; energy storage (including batteries and capacitors); charge transport; materials and chemistry by design; synthesis (novel materials); 77 NANOSCIENCE AND NANOTECHNOLOGY