skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Cross-plane coherent acoustic phonons in two-dimensional organic-inorganic hybrid perovskites

Journal Article · · Nature Communications
 [1]; ORCiD logo [2];  [2];  [1];  [2];  [1];  [2];  [3]
  1. Argonne National Lab. (ANL), Lemont, IL (United States)
  2. Northwestern Univ., Evanston, IL (United States)
  3. Argonne National Lab. (ANL), Lemont, IL (United States); Northwestern Univ., Evanston, IL (United States)

Two-dimensional, Ruddlesden-Popper organic-inorganic hybrid layered perovskites (2D-RPs) are solution-grown semiconductors with prospective applications in next-generation optoelectronics. The heat-carrying, low-energy acoustic vibrations of 2D-RPs, which are important for heat management of 2D-RP-based devices, have remained unexplored. Here we report on the propagation of coherent longitudinal acoustic phonons along the cross-plane direction of 2D-RPs, following separate characterizations of below-bandgap refractive index for each 2D-RP. Through experiments on crystals of systematically varied perovskite layer thickness, we demonstrate significant reduction in both group velocity and propagation length of acoustic phonons in 2D-RPs as compared to the three-dimensional methylammonium lead iodide. As borne out by a minimal coarse-grained model, these vibrational properties arise from a large acoustic impedance mismatch between the alternating layers of perovskite sheets and bulky organic cations. Furthermore, our results inform on thermal transport in highly impedance-mismatched crystal sub-lattices and provide insights towards design of materials that exhibit highly anisotropic thermal dissipation properties.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1461512
Journal Information:
Nature Communications, Vol. 9, Issue 1; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 53 works
Citation information provided by
Web of Science

References (65)

Effect of reduced dimensionality on the optical band gap of SrTiO 3 journal March 2013
Ultralow Self-Doping in Two-dimensional Hybrid Perovskite Single Crystals journal June 2017
Ultralow Thermal Conductivity in Disordered, Layered WSe2 Crystals journal January 2007
Polar Fluctuations in Metal Halide Perovskites Uncovered by Acoustic Phonon Anomalies journal September 2017
Phonon wave interference and thermal bandgap materials journal June 2015
Structures, Phase Transitions and Tricritical Behavior of the Hybrid Perovskite Methyl Ammonium Lead Iodide journal October 2016
Elastic Constants, Optical Phonons, and Molecular Relaxations in the High Temperature Plastic Phase of the CH 3 NH 3 PbBr 3 Hybrid Perovskite journal September 2016
Metal halide perovskites for energy applications journal May 2016
Heat Capacities, Speeds of Sound, and Isothermal Compressibilities of Some n -Amines and Tri- n -amines at 298.15 K journal January 2002
Elastic Moduli of Organic Electronic Materials by the Buckling Method journal September 2009
QUANTUM ESPRESSO: a modular and open-source software project for quantum simulations of materials journal September 2009
Self-Assembled Monolayers of Thiolates on Metals as a Form of Nanotechnology journal April 2005
Atomically thin two-dimensional organic-inorganic hybrid perovskites journal September 2015
Bright light-emitting diodes based on organometal halide perovskite journal August 2014
Phonon Speed, Not Scattering, Differentiates Thermal Transport in Lead Halide Perovskites journal August 2017
Ruddlesden–Popper Hybrid Lead Iodide Perovskite 2D Homologous Semiconductors journal April 2016
Exceptional elastic anisotropy of hybrid organic-inorganic perovskite CH 3 NH 3 PbBr 3 measured by laser ultrasonic technique journal July 2016
Thermal properties of AlAs/GaAs superlattices journal November 1987
Screening in crystalline liquids protects energetic carriers in hybrid perovskites journal September 2016
Experimental and theoretical optical properties of methylammonium lead halide perovskites journal January 2016
Phonon Dynamics at Surfaces and Interfaces and Its Implications in Energy Transport in Nanostructured Materials—An opinion Paper journal April 2015
Organic-Inorganic Hybrid Materials as Semiconducting Channels in Thin-Film Field-Effect Transistors journal October 1999
White-Light Emission and Structural Distortion in New Corrugated Two-Dimensional Lead Bromide Perovskites journal March 2017
Orientational order controls crystalline and amorphous thermal transport in superatomic crystals journal September 2016
High-efficiency two-dimensional Ruddlesden–Popper perovskite solar cells journal July 2016
Electron–Phonon Scattering in Atomically Thin 2D Perovskites journal October 2016
Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites journal March 2017
Mechanism for Broadband White-Light Emission from Two-Dimensional (110) Hybrid Perovskites journal May 2016
Surface chemistry mediates thermal transport in three-dimensional nanocrystal arrays journal March 2013
Direct–indirect character of the bandgap in methylammonium lead iodide perovskite journal October 2016
Coherent Phonon Heat Conduction in Superlattices journal November 2012
Electron–acoustic phonon coupling in single crystal CH3NH3PbI3 perovskites revealed by coherent acoustic phonons journal February 2017
Thermal conductivity of Si–Ge superlattices journal June 1997
Van der Waals heterostructures journal July 2013
Acoustic-phonon propagation in superlattices journal July 1988
Ultra-Low Thermal Conductivity in Organic–Inorganic Hybrid Perovskite CH 3 NH 3 PbI 3 journal July 2014
25th Anniversary Article: MXenes: A New Family of Two-Dimensional Materials journal December 2013
Charge-Carrier Dynamics in Organic-Inorganic Metal Halide Perovskites journal May 2016
Relations between the Refractive Index and Energy Gap of Semiconductors journal October 1985
Effects of chemical bonding on heat transport across interfaces journal April 2012
Physical mechanisms of coherent acoustic phonons generation by ultrafast laser action journal February 2015
Atomic and molecular layer deposition: off the beaten track journal January 2017
Targeted Magnetic Nanoparticles for Remote Magnetothermal Disruption of Amyloid-β Aggregates journal August 2015
High Members of the 2D Ruddlesden-Popper Halide Perovskites: Synthesis, Optical Properties, and Solar Cells of (CH 3 (CH 2 ) 3 NH 3 ) 2 (CH 3 NH 3 ) 4 Pb 5 I 16 journal March 2017
Crossover from incoherent to coherent phonon scattering in epitaxial oxide superlattices journal December 2013
Tailoring the Energy Landscape in Quasi-2D Halide Perovskites Enables Efficient Green-Light Emission journal May 2017
Low-Dimensional-Networked Metal Halide Perovskites: The Next Big Thing journal March 2017
Size and Interface Effects on Thermal Conductivity of Superlattices and Periodic Thin-Film Structures journal May 1997
Role of Organic Counterion in Lead- and Tin-Based Two-Dimensional Semiconducting Iodide Perovskites and Application in Planar Solar Cells journal October 2016
An overview of molecular layer deposition for organic and organic–inorganic hybrid materials: mechanisms, growth characteristics, and promising applications journal January 2017
Chemically diverse and multifunctional hybrid organic–inorganic perovskites journal February 2017
Direct Observation of Electron–Phonon Coupling and Slow Vibrational Relaxation in Organic–Inorganic Hybrid Perovskites journal October 2016
Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy journal April 2017
Selective enhancement of optical nonlinearity in two-dimensional organic-inorganic lead iodide perovskites journal September 2017
Acoustic-optical phonon up-conversion and hot-phonon bottleneck in lead-halide perovskites journal January 2017
Near infrared two photon imaging using a bright cationic Yb( iii ) bioprobe spontaneously internalized into live cells journal January 2017
Self-Assembled Monolayers of Thiolates on Metals as a Form of Nanotechnology journal August 2005
Lattice thermal transport in two-dimensional alloys and fractal heterostructures journal January 2021
Direct-indirect character of the bandgap in methylammonium lead iodide perovskite. text January 2017
Local polar fluctuations in lead halide perovskite crystals text January 2016
Three- and low-dimensional inorganic semiconductors journal January 1997
Directed assembly of layered perovskite heterostructures as single crystals journal September 2021
Ultrasonic study of liquid crystals journal August 1975
Surface generation and detection of phonons by picosecond light pulses journal September 1986
Van der Waals heterostructures text January 2013

Cited By (8)

Merits and Challenges of Ruddlesden-Popper Soft Halide Perovskites in Electro-Optics and Optoelectronics journal October 2018
Edge Effect on the Population of Free Carriers and Excitons in Single‐Crystal CH 3 NH 3 PbBr 3 Perovskite Nanomaterials journal May 2019
Self-Assembled 2D Perovskite Layers for Efficient Printable Solar Cells journal December 2018
Infrared-pump electronic-probe of methylammonium lead iodide reveals electronically decoupled organic and inorganic sublattices journal January 2019
Hot carrier solar cells and the potential of perovskites for breaking the Shockley–Queisser limit journal January 2019
Superlattices based on van der Waals 2D materials journal January 2019
Optical deformation potential and self-trapped excitons in 2D hybrid perovskites journal January 2019
Broadband white-light emission from supramolecular piperazinium-based lead halide perovskites linked by hydrogen bonds journal January 2019