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Title: Tunable and Transferable Diamond Membranes for Integrated Quantum Technologies

Journal Article · · Nano Letters
ORCiD logo [1];  [2];  [1];  [1];  [3];  [3]; ORCiD logo [1]; ORCiD logo [4];  [2];  [2]
  1. Pritzker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60615, United States
  2. Pritzker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60615, United States, Center for Molecular Engineering and Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
  3. Department of Physics, University of Chicago, Chicago, Illinois 60615, United States
  4. Pritzker School of Molecular Engineering, University of Chicago, Chicago, Illinois 60615, United States, Center for Molecular Engineering and Materials Science Division, Argonne National Laboratory, Lemont, Illinois 60439, United States, Department of Physics, University of Chicago, Chicago, Illinois 60615, United States

Color centers in diamond are a leading platform in quantum networking and sensing due to their exceptional coherence times, robust spin–photon interfaces, and controllable interactions with local nuclear- and reporter-spin registers. Color centers have been utilized in many landmark experimental demonstrations, including deterministic entanglement, multinode quantum networking, nanoscale NMR spectroscopy, and memory-enhanced quantum key distribution. These advances can be accelerated into scalable technologies with the ability to create high-quality, nanoscale-thick diamond membranes as elements in hybrid devices. Ideally, in the next generation of quantum technology, diamond will simply be another functional layer in heterostructures that can include nonlinear/magnetic/acoustic materials, on-chip detectors, superconductors, nanophotonics, and microfluidics. Such improved integration can increase entanglement efficiency, master control of phonons and photons, enable on-chip frequency conversion, improve interfaces with other quantum systems and sensing targets, and create new opportunities to engineer quantum states. However, the material properties of diamond create fundamental difficulties for heterostructure integration. Specifically, high-quality, single crystal heteroepitaxial growth of diamond thin films remains challenging despite recent progress. In response, a variety of processing and integration schemes have been developed to derive low dimensional structures out of bulk diamond. While promising, a scalable, high-yield approach that enables full heterostructure-like integration of diamond while maintaining bulk-like properties—specifically, crystallinity, surface roughness, and color center coherence—is still lacking. Here, we report the efficient synthesis and manipulation of ultrathin diamond membranes suitable for next-generation applications in quantum information science (QIS). Our membrane fabrication procedure is based on a “smart-cut” technique, in which He+ implantation creates a subsurface graphitized layer that can be electrochemically (EC) etched, in conjuncture with a plasma enhanced chemical vapor deposition (PE-CVD) overgrowth optimized for the synthesis of high-quality, in situ doped, and isotopically purified diamond. The process allows detachment of arbitrarily large diamond membranes with smooth interfaces without relying on reactive-ion-etching (RIE) undercut processes. While previous works have demonstrated the effectiveness of “smart-cut” and overgrowth for diamond membrane creation, our process realizes three critical advancements to the state-of-the-art. First, we demonstrate isotopically controlled and nitrogen δ-doped diamond membrane structures with atomically flat surfaces and high crystal quality showing unprecedentedly narrow Raman line widths. (28,29) Second, we demonstrate a novel dry-transfer technique which enables clean and deterministic membrane placement on arbitrary substrates. Membranes transferred in this way are free from premature detachment and unwieldy curvatures caused by built-in strain between the graphitized and overgrown layers. (30) As such, these membranes can be integrated with other material platforms and functional structures. Third, we report that these structures, even at thickness ≤150 nm, are suitable hosts for germanium vacancy (GeV–) and nitrogen vacancy (NV–) centers created via implantation (in both cases) and overgrowth (NV– only). Specifically, we show that the GeV– centers exhibit stable and coherent emission at 5.4 K, while the NV– centers show bulk-like spin coherence properties at room temperature. Additionally, we demonstrate that doping of other group IV color centers such as silicon-vacancy (SiV–) and tin-vacancy (SnV–) is also viable.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
Grant/Contract Number:
AC02-06CH11357; DMR-2011854; DGE-1746045; ECCS-2025633
OSTI ID:
1835425
Alternate ID(s):
OSTI ID: 1868549
Journal Information:
Nano Letters, Journal Name: Nano Letters Vol. 21 Journal Issue: 24; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

References (56)

Strain engineering of the silicon-vacancy center in diamond journal May 2018
Large-scale integration of artificial atoms in hybrid photonic circuits journal July 2020
Quantum Engineering With Hybrid Magnonic Systems and Materials (Invited Paper) journal January 2021
A cavity-based optical antenna for color centers in diamond journal August 2021
Increasing the coherence time of single electron spins in diamond by high temperature annealing journal December 2010
Germanium-Vacancy Single Color Centers in Diamond journal August 2015
Measuring magnetic field texture in correlated electron systems under extreme conditions journal December 2019
Coherent acoustic control of a single silicon vacancy spin in diamond journal January 2020
Scalable Fabrication of Integrated Nanophotonic Circuits on Arrays of Thin Single Crystal Diamond Membrane Windows journal April 2016
Homoepitaxial Growth of Single Crystal Diamond Membranes for Quantum Information Processing journal January 2012
Cavity-Enhanced Photon Emission from a Single Germanium-Vacancy Center in a Diamond Membrane journal June 2020
Growth, stress, and defects of heteroepitaxial diamond on Ir/YSZ/Si(111) journal June 2018
Brillouin and Raman scattering in natural and isotopically controlled diamond journal August 1996
Thermal Curing of Hydrogen Silsesquioxane journal January 2000
Characterization of optical and spin properties of single tin-vacancy centers in diamond nanopillars journal May 2019
Electrical Tuning of Tin-Vacancy Centers in Diamond journal June 2021
Silicon-Vacancy Spin Qubit in Diamond: A Quantum Memory Exceeding 10 ms with Single-Shot State Readout journal November 2017
Magnetic Resonance Detection of Individual Proton Spins Using Quantum Reporters journal November 2014
Engineered Micro- and Nanoscale Diamonds as Mobile Probes for High-Resolution Sensing in Fluid journal August 2014
High- Q Nanophotonic Resonators on Diamond Membranes using Templated Atomic Layer Deposition of TiO 2 journal May 2020
SRIM – The stopping and range of ions in matter (2010)
  • Ziegler, James F.; Ziegler, M. D.; Biersack, J. P.
  • Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 268, Issue 11-12 https://doi.org/10.1016/j.nimb.2010.02.091
journal June 2010
Observation of an environmentally insensitive solid-state spin defect in diamond journal July 2018
Engineering Electron–Phonon Coupling of Quantum Defects to a Semiconfocal Acoustic Resonator journal September 2019
Spectral Alignment of Single-Photon Emitters in Diamond using Strain Gradient journal August 2018
Experimental demonstration of memory-enhanced quantum communication journal March 2020
Predicted strong coupling of solid-state spins via a single magnon mode journal December 2020
Engineering shallow spins in diamond with nitrogen delta-doping journal August 2012
Optically Coherent Nitrogen-Vacancy Centers in Micrometer-Thin Etched Diamond Membranes journal April 2019
Strongly coupled diamond spin qubits by molecular nitrogen implantation journal November 2013
Nanoscale NMR spectroscopy and imaging of multiple nuclear species journal January 2015
All-Optical Initialization, Readout, and Coherent Preparation of Single Silicon-Vacancy Spins in Diamond journal December 2014
Optical and microwave control of germanium-vacancy center spins in diamond journal August 2017
Planar fabrication of arrays of ion-exfoliated single-crystal-diamond membranes with nitrogen-vacancy color centers journal January 2013
Deterministic delivery of remote entanglement on a quantum network journal June 2018
Reproducible fabrication and characterization of diamond membranes for photonic crystal cavities: Reproducible fabrication and characterization of diamond membranes journal September 2016
Engineering quantum-coherent defects: The role of substrate miscut in chemical vapor deposition diamond growth journal November 2020
Sensitivity optimization for NV-diamond magnetometry journal March 2020
In situ study of annealing-induced strain relaxation in diamond nanoparticles using Bragg coherent diffraction imaging journal February 2017
Origins of Diamond Surface Noise Probed by Correlating Single-Spin Measurements with Surface Spectroscopy journal September 2019
Quantum entanglement between an optical photon and a solid-state spin qubit journal August 2010
Free-Standing Mechanical and Photonic Nanostructures in Single-Crystal Diamond journal February 2012
Ion bombardment induced buried lateral growth: the key mechanism for the synthesis of single crystal diamond wafers journal March 2017
Fast pick up technique for high quality heterostructures of bilayer graphene and hexagonal boron nitride journal July 2014
Realization of a multinode quantum network of remote solid-state qubits journal April 2021
Opportunities for wavelength conversion with on-chip diamond ring resonators journal October 2012
Single Crystal Diamond Membranes and Photonic Resonators Containing Germanium Vacancy Color Centers journal November 2018
Fabrication of thin, luminescent, single-crystal diamond membranes journal August 2011
Quantum technologies with hybrid systems journal March 2015
High-fidelity projective read-out of a solid-state spin quantum register journal September 2011
Etching and micro-optics fabrication in diamond using chlorine-based inductively-coupled plasma journal July 2008
Opportunities for Long-Range Magnon-Mediated Entanglement of Spin Qubits via On- and Off-Resonant Coupling journal October 2021
Probing Surface Noise with Depth-Calibrated Spins in Diamond journal July 2014
Initialization and Readout of Nuclear Spins via a Negatively Charged Silicon-Vacancy Center in Diamond journal May 2019
Optical magnetic imaging of living cells journal April 2013
Quantum Nonlinear Optics with a Germanium-Vacancy Color Center in a Nanoscale Diamond Waveguide journal May 2017
Fabrication of thin diamond membranes for photonic applications journal March 2013