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Title: V x In (2–x) S 3 Intermediate Band Absorbers Deposited by Atomic Layer Deposition

Substitutional alloys of several thin film semiconductors have been proposed as intermediate band (IB) materials for use in next-generation photovoltaics, which aim to utilize a larger fraction of the solar spectrum without sacrificing significant photovoltage. Here, we demonstrate a novel approach to IB material growth, namely atomic layer deposition (ALD), to enable unique control over substitutional-dopant location and density. Two new ALD processes for vanadium sulfide incorporation are introduced, one of which incorporates a vanadium (III) amidinate previously untested for ALD. We synthesize the first thin film V xIn (2-x)S 3 intermediate band semiconductors, using this process, and further demonstrate that the V:In ratio, and therefore intraband gap density of states, can be finely tuned according to the ALD dosing schedule. Deposition on a crystalline In 2S 3 underlayer promotes the growth of a tetragonal β-In 2S 3-like phase V xIn (2-x)S 3, which exhibits a distinct sub-band gap absorption peak with onset near 1.1 eV in agreement with computational predictions. But, the V xIn (2-x)S 3 films lack the lower energy transition predicted for a partially filled IB, and photoelectrochemical devices reveal a photocurrent response only from illumination with energy sufficient to span the parent band-gap.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [1]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division; Illinois Inst. of Technology, Chicago, IL (United States). Dept. of Biological and Chemical Sciences
  3. Univ. of Illinois, Urbana-Champaign, IL (United States). Frederick Seitz Materials Research Lab.
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Nanoscience and Technology Division
  5. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division; Illinois Inst. of Technology, Chicago, IL (United States). Dept. of Biological and Chemical Sciences
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 28; Journal Issue: 7; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1352646